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Aluminum air batteries have great potential as a state-of-the-art energy storage device due to their high capacity, energy density and fascinating safety. However, the disturbing hydrogen evolution reaction (HER) of the Al anode increase the gap between practical application and theoretical level. Electrolyte engineering with organic additives has been the spotlight to address the problem of HER. The polar functional group of organic molecules could bound with the water via the hydrogen bond to drop the activity of water. Unfortunately, the basic physicochemical properties of electrolyte would be deteriorated due to the organic matter, which has a negative impact on the electrochemical performance of batteries. Herein, an inorganic additive was adopted to regulate the hydrogen bond network and anode interface. The activity of H 2 O could be obviously suppressed by the stronger three-center-four-electron hydrogen bonds bridged by fluoride ions. And the water molecules are kept away from the anode surface due to the protective layer caused by the adsorption of fluoride ions. The HER could be greatly inhibited by both pathways, which reaches an inhibition efficiency of 55% in the electrolyte with 5 M KF. Correspondingly, the Al air battery exhibits a high discharge specific capacity of 1552.8 mAh g−1 and an energy density of 1829.51 Wh kg−1 at a current density of 25 mA cm−2. This work showcases a promising inorganic additive to suppress the HER for high-performance Al air battery. [Display omitted] • An inorganic additive was adopted to regulate hydrogen bond network. • The 3c4e hydrogen bond bridged by fluoride ion decreases the activity of H 2 O. • The fluoride ions constructure a protective layer for anode. • Al air battery exhibits high discharge capacity of 1552.8 mAh g−1 at 25 mA cm−2. [ABSTRACT FROM AUTHOR]

This paper proposes a molecular model of covalent grafting of azobenzene derivatives with graphite-like carbon nitride based on hydrogen bond regulation to improve the azobenzene photothermal energy storage density. The enthalpy of isomerization (Δ H) of azobenzene molecular cis - trans isomers is calculated using density functional theory, and the magnitude of Δ H is used to evaluate the photothermal storage performance of the azobenzene graphite-like carbon nitride model. The results showed that the molecular Δ H value increased by 0.105–0.243 eV after the azobenzene derivatives were covalently grafted to the graphitic carbon nitride template. In addition, when the donator group replaced the active benzene ring ortho-site of azobenzene, its value was 0.069–0.295 eV higher than that of the electron-withdrawing groups. Moreover, intramolecular hydrogen bonds can stabilize cis - trans isomers and increase the energy of azobenzene. Compared with unsubstituted azobenzene, the energy of azobenzene Δ H containing one intramolecular hydrogen bond increased by 0.295 eV, while the energy of azobenzene Δ H containing multiple intramolecular hydrogen bonds increased by 0.775 eV. [Display omitted] • A molecular model for covalent grafting of azobenzene onto g-C 3 N 4 with hydrogen bond was developed. • The energy conversion density of azobenzene synthetic was determined using density functional theory. • The grafting effect was evaluated by considering intramolecular hydrogen bond, substitution location, and electron group. [ABSTRACT FROM AUTHOR]

Polybenzimidazole (PBI) doped with phosphoric acid (PA) exhibits fast proton conduction in the range of 120–180 °C. However, PA loss during high temperature fuel cells (HT-PEMFCs) operation and plasticization after PA doping are the main obstacles to PBI membrane application. In this work, the properties of PA-doped PBI membranes were improved by branching polyurethane side chains onto the PBI backbone via N-substitution reaction. The urea and amide-ester bonds between the polyurethane side chains form a rich hydrogen bonding network. The hydrogen bonding network together with Ce–O coordination bonding enhance the mechanical properties of PBI membranes. Long branched chains increase the spacing between the molecular chains, and the additional unbonded groups in the polyurethane side chains can also form hydrogen bonding interactions with the PA, which increase the adsorption and retention capacity of the PA. The proton conductivity of polyurethane grafting PBI reached 0.104 S cm −1, while the conductivity of the pristine PBI membrane was only 0.026 S cm −1 under the same conditions. The PBI membrane grafted with polyurethane side chains showed a proton conductivity of up to 0.104 S cm −1 at 160 °C in anhydrous conditions, whereas the pristine PBI membrane showed a conductivity of only 0.026 S cm −1 under the same conditions. During single-cell testing, polyurethane-grafted PBI membrane peak power densities of 408 mW cm −2 could be achieved. In addition, the polyurethane grafted membrane has excellent durability with a voltage decay of only 245 μV h −1 in a 120 h test. Formation of a rich hydrogen bonding network in the polybenzimidazole membrane after grafting polyurethanes promotes rapid proton transfer. [Display omitted] • Rich hydrogen bonding network. • Ce-O coordination bonds enhance the mechanical properties of membranes. • Excellent durability. [ABSTRACT FROM AUTHOR]

Hydrogels have broad application prospects in drug delivery due to their biocompatibility, high water content and three-dimensional structure. However, the regulation of drug release from hydrogels is an important issue in medical applications. At the same time, water also has an important impact on drug release. In this study, a hydrogel with hydrogen bond and ion dipole interaction (PAHDP) was prepared by introducing catechol group into polymer to regulate drug release. Ten model drugs were selected to explore the relationship and mechanism of action among polymer, drug and water. The results showed that PAHDP had excellent adhesion and safety. Drug release test showed that 10 kinds of drugs had different drug release trends, and the release amount was negatively correlated with drug polarizability and LogP. In addition, in vitro transdermal test and pharmacokinetic results showed that the hydrogel based on PAHDP achieved increased or decreased blood drug concentration, and the area under the concentration-time curve (AUC) of >1.5 times showed its potential to regulate drug release. The mechanism study showed that the hydrogen bond and ion dipole interaction between polymer and drug were affected by drug polarizability and LogP, and the distribution of water in different states was changed. Hydrogen bond and ion dipole interactions synergistically control drug release. Therefore, the mussel inspired PAHDP hydrogel has the potential to become a controllable drug delivery system. [Display omitted] [ABSTRACT FROM AUTHOR]

The Japanese traditional pot-distilled spirit shochu has various tastes that are produced by variations in the manufacturing processes. In this study, an alcohol-stimulative taste was organoleptically evaluated using shochu samples, and the chemical components and proton nuclear magnetic resonance (1H NMR) spectra were measured. In some shochu samples, the alcohol-stimulative taste was weaker than that of the standard 15% (v/v) EtOH–H 2 O mixture, and the water–ethanol hydrogen-bonding structure was stronger compared to a water–ethanol solution. However, some shochu samples filtered with ion-exchange resin had a strong alcohol-stimulative taste comparable to that of the standard 15% (v/v) EtOH–H 2 O mixture, and the hydrogen-bonding structure was found to be similar to that of the water–ethanol solution. We also investigated the effect of MgCl 2 on reducing the alcohol-stimulative taste, and it was observed most strongly with in shochu samples filtered with ion-exchange resin. The change in chemical shift values of the 1H NMR spectra was also the largest in ion-exchange resin filtered shochu samples. The sensory reduction in the alcohol-stimulative taste could be enhanced by the strengthening of the water–ethanol hydrogen-bonding structure. Shochu samples contained many components in larger quantities compared to vodkas. It was found that MgCl 2 could reduce the alcohol-stimulative taste of shochu samples. Some salts, such as MgCl 2 , can be introduced into spirits through the water used to dilute the ethanol content before bottling the products. Our results indicated that some components, such as MgCl 2 , present in water used can reduce the alcohol-stimulative taste of different spirits produced worldwide. • The alcohol-stimulative taste of Japanese spirit "shochu" was investigated. • Shochu filtered with ion-exchange resin had a strong alcohol-stimulative taste. • MgCl 2 reduced the alcohol-stimulative taste of shochu. • MgCl 2 strengthened the water–ethanol hydrogen-bonding structure of shochu. • Components in water can reduce the alcohol-stimulative taste of spirits worldwide. [ABSTRACT FROM AUTHOR]

Photocatalysis is a prospective technology to solve the current environment and energy crisis. The exploitation of 2D photocatalyst materials is a research hotspot owing to their large specific surface area, intrinsic defect and abundant active sites. Particularly, 2D/2D heterojunctions own intimate interfaces with expanded contact areas, which is beneficial to facilitate the separation and transportation of electron-hole pairs and further improve the photocatalytic activity. Currently, most studies focus on the band structure alignment in the design of 2D/2D heterojunctions, while the importance of interfacial binding forces is often ignored. This review aims at highlighting the critical role of interfacial binding forces in the photocatalytic activity of 2D/2D heterojunctions for the first time. First, we classify the types of interfacial forces, including electrostatic force, van der Waals force, covalent bond, hydrogen bond. Then we summarize several typical strategies for constructing 2D/2D heterojunctions with corresponding structural features. Importantly, the photocatalytic mechanism is discussed based on interfacial composition, charge transfer path and modification of active sites, and various photocatalytic applications are summarized. Finally, we outline the challenges and future development in this prospective research field. It is expected to fill the existing knowledge gap on interfacial binding forces for designing efficient 2D/2D heterojunctions rationally. • The types of different interfacial binding forces are introduced. • The construction strategies of different interfacial binding forces are reviewed. • The key role of interfacial binding forces of 2D/2D heterojunctions is summarized. • Prospects of 2D hybrids in energy and environment photocatalysis are discussed. [ABSTRACT FROM AUTHOR]

The notion of asymmetrical Hydrogen Bond (O:H-O) Cooperativity and Polarizability (HBCP) has enabled exploration of the core physics behind irregularities of water and ice, particularly, the evolution of mass density, phase stability, energy exchange, and their transition velocity under perturbation. We humbly share the initiatives of the quasisolidity presented between Liquid and Ice, the supersolidity pertained to polarization by electrification or molecular undercoordination, and the H ↔ H and O: ⇔ :O repulsivity owing to the respective injection of excessive protons and lone pairs to the liquid by solvation. The O—O repulsivity forms the key that drives the O:H-O bond to cooperatively relax its segmental length, cohesive energy, vibration frequency, and specific heat upon perturbation, which establishes an efficient set of parameters to feature the bonding and electronic dynamics in the frequency–space–time domains. An interplay of the segmental specific heats defines the mass densities, phase boundaries, and the exotic quasisolid (QS) phase that exhibits negative thermal expansivity through H-O contracting less than the scale of O:H expansion upon cooling. However, the H-O bond undergoes cooling elongation in the Liquid and the Ice-I phase and remains silent in the XI phase. H-O bond absorbs energy by contraction and does it inverse at expansion. The O:H nonbond always relaxes more than the H-O bond does in contrasting direction. Mechanical compression symmetrizes the O:H-O segmental length associated with polarization, which disperses inwardly the QS phase boundary to lower the T m for melting but raise the temperature T N for ice nucleation and the T V for evaporation, resulting in the phenomena of ice regelation and instant-ice formation. Polarization, however, has the contrast effect to compression on the hydrogen bond relaxation and phase transition. The polarization converts the pristine water into the gel-like, hydrophobic, and viscoelastic supersolid which is less-dense and thermally more diffusive and stable, entitling surface premelting, superheating at T m , and supercooling at T N and T V. Polarization enhances the dielectrics of water and widens the bandgap of ice. The supersolidity ensures the 120 K superelasticity of ice microfibers and the 330 K stability of the electrified water bridge crossing the rims of infilled containers. The high elasticity of the softer O:H nonbond and the interface electrostatic repulsivity secure the slipperiness of ice and the superfluidity of water traveling in fine channels. The skin supersolidity and the O:H-O bond memorability uniquely foster the Mpemba effect — warm water cools more quickly. The H ↔ H or O: ⇔ :O repulsivity modifies the bonding network and solution properties through solvent H-O bond elongation, solute H-O bond contraction, and polarization. The HBCP premise has thus correlated the irregularity of water and ice to the O:H-O bonding and electronic dynamics under perturbation. Further extension of the HBCP to aqueous and molecular assemblies involved with electron lone pairs and coupling interactions could be even more fascinating and profoundly promising. [Display omitted] • O—O repulsive coupling interaction entitles the irregularity of water and ice. • O:H-O bond cooperativity and polarizability revolutionizes the parameter space. • Perturbations drive the quasisolidity, supersolidity, H ↔ H and O: ⇔ :O repulsivity. • Specific-heat disparity resolves water's density anomalies and phase boundaries. • The T m and T N /T V vary respectively with the H-O and the O:H binding energy. • (e; ± ;H 3 O + ;HO −) ⋅ 4H 2 O:6H 2 O hydration revises solution's network and properties. [ABSTRACT FROM AUTHOR]

Primary quasi-solid Al-air batteries using hydrogels have attracted increasing research attention owing to their high energy density, good handling, safety and reliability. However, it is still difficult to develop hydrogel electrolytes with high ionic conductivity and water retention owing to limited capacity of single material hydrogels. Herein, we report a hydrogel electrolyte of poly (acrylic acid) (PAA) is modified by κ-carrageenan (KC) for solid-state Al-air batteries. The result suggests that the hydrogels not only exhibit outstanding water retention but also high ionic conductivity, which is attributed to the amorphous phase and hydrophilic group of the KC. Additionally, the lifespan of solid-state Al-air battery is extended at a current density of 5 mA cm−2 owing to adding KC. Further, the lifetime of open Al-air batteries is improved by self-corrosion inhibition of Al anode. [ABSTRACT FROM AUTHOR]

An ideal biomedical hydrogel should imitate natural tissues with high water absorption, high toughness and superior biocompatibility. However, hydrogels constructed from biomolecules such as polysaccharides have low mechanical strength and limited applications. Based on carboxymethyl chitosan (CMCS) and polyacrylamide (PAM), a facile process is presented for preparing double network hydrogels (CMCS/PAM) with improved mechanical properties. According to the systematic characterization, carboxymethyl chitosan and polyacrylamide form a double network hydrogel through hydrogen bonding. The introduction of carboxymethyl chitosan alters the microscopic structure of PAM hydrogel, resulting in a consistent porosity pattern. Hydrogels with double networks exhibit high tensile properties, high stiffness, and good energy dissipation. Furthermore, the hydrogel exhibits effective adhesion to other hydrophilic surfaces. The CMCS/PAM network hydrogels possess excellent properties such as high swelling capacity, injectability, and cellular biocompatibility, making them potentially valuable for biomedical applications. [Display omitted] [ABSTRACT FROM AUTHOR]

Hydrogen bonds (H-bonds), usually mainchain amide H-bonds, have been well recognized to play important roles in modulating the properties of polyimides (PIs) by strengthening macromolecular interaction. While the structure-properties relationships of symmetric mainchain amide H-bonded PIs have been extensively researched, the asymmetric H-bonded PIs, particularly those containing rigid-flexible backbone structure, and sidechain-involving H-bonds, have been rarely explored. Herein, starting from designed synthesis of diamine monomers, we present two series of asymmetric PIs containing rigid amide and flexible ether linkages that form mainchain amide-amide and amide-imide H-bonds, lacking or bearing pendent trifluoromethyls (-CF 3) that form sidechain-involving amide-CF 3 H-bonds. The presence of these three types of H-bonds were revealed by RDF simulation and confirmed by FTIR. Mainchain H-bonded PIs (PI-A x) show higher T g than sidechain-involving H-bonded PIs (PI-T x), while PI-T x series exhibit higher optical transparency and hydrophobicity, lower dielectric constant (ε′) and better mechanical properties than PI-A x. The general researches on the PIs' solubility, WAXD spectra, thermal properties, fluorescence emission and optical transparency, the dihedral angles (φ), fractional free volume (FFV), theoretical gas transport properties, chain geometry optimization and HOMO-LUMO energy gap (Δ E) values have been comprehensively carried out from the aspects of both experiments and theoretical calculation. Mainchain and sidechain-involving H-bonded asymmetric polyimides containing rigid amide and flexible ether linkages were comprehensively studied, with particular emphasis on investigating the effects of mainchain-mainchain H-bonds and mainchain-sidechain H-bonds to the properties of asymmetric polyimides. [Display omitted] • Two asymmetric diamines containing rigid amide and flexible ether linkages were synthesized and showed satisfactory copolymerization reactivity. • Two types of mainchain H-bonds and one type of sidechain-involving H-bonds were revealed by RDF simulations and IR spectra. • Mainchain H-bonded PIs showhigher T g while sidechain-involving H-bonded PIs exhibit better mechanical properties, higher optical transparency and hydrophobicity, lower dielectric constant (ε ′). • "Structure-properties" relationships of asymmetric H-bonded PAIs were comprehensively explored from both experimental and theoretical aspects. [ABSTRACT FROM AUTHOR]

• Dielectric spectra of aqueous DK reveal three relaxation processes: EP, normal (n) and alpha (α) relaxation. • Stokes relation fails to hold strictly to K+ cation in aqueous solutions of DK. • Violation of Stokes law results from the ion's electric field interaction with the solvent's dielectric relaxation. • DK's ionic diffusion in water isn't governed by chain motion but by local segmental motion. • The average number of H-bond formations between solute and solvent remains constant. Diclofenac potassium (DK) is a salt and undergoes ionization in an aqueous environment. The detailed information about the molecular structure and interactions of such aqueous ionic solutions holds substantial significance in the field of pharmaceutics. This comprehension facilitates the enhancement of pharmaceutical formulations, leading to improved bioavailability, stability, and therapeutic efficacy. It also contributes to the optimization of drug delivery systems. Molecular interactions in the aqueous solutions of DK were studied using dielectric relaxation spectroscopy (DRS) and molecular dynamic (MD) simulation. In DRS, complex dielectric permittivity, ε ∗ (f) for aqueous solutions of DK of varying concentrations were measured in the frequency range of 20 Hz to 2 MHz at five different temperatures ranging from 303.15 K to 323.15 K. Complex ac conductivity, σ ∗ (f) and dc conductivity (σ d c) were determined from the complex dielectric permittivity. The effect of concentration and temperature on complex permittivity and allied parameters are discussed. The dielectric spectra of aqueous DK reveal dual relaxation processes i.e., normal (n) relaxation and alpha (α) relaxation. The dielectric strength is predominant for α-process and n-process in the low (0 < X ≤ 0.0299) and high (0.029 < X ≤ 0.0822) concentration range respectively. Moreover, Stoke's relation between dielectric relaxation time, ion mobility and viscosity of the aqueous solutions is discussed. MD simulation at 303.15 K temperature has also been conducted to get additional information on molecular interactions between DK and/or H 2 O molecules through hydrogen bonding (HB). [ABSTRACT FROM AUTHOR]

Lignin, a biopolymer derived from plant biomass, is recognized as a highly promising substance for developing self-healing polymers owing to its dynamic linkages and functional groups. This paper provides a thorough review of lignin-based self-healing polymer, from the process of extracting lignin, chemical modification, synthesis techniques such as via reversible addition-fragmentation chain transfer (RAFT) polymerization, crosslinking with polymers like polyvinyl alcohol (PVA) and chitosan, and reactions with isocyanates to create lignin-based networks with reversible interactions. This work also summarizes the optimization of self-healing ability, such as including dynamic copolymers, encapsulating healing agents like dicyclopentadiene and polycaprolactone (PCL), and chain extenders with disulfide or Diels-Alder (DA) moieties. The material's characterization focuses on its capacity to recover via hydrogen bonding and dynamic re-associations, improved mechanical properties from lignin's rigid structure, and enhanced temperature resistance. Primary obstacles involve the optimization of lignin extraction, enhancement of polymer compatibility, and the establishment of efficient procedures for synthesis and characterization. Overall, lignin shows great potential as a renewable component of self-healing polymers, with plenty of opportunities for further development. • Lignin in self-healing polymers utilizes its aromatic nature and diverse functional groups • Adding reactive groups to lignin's backbone is a popular method in self-healing synthesis • Lignin and its derivatives' hydrogen bond are key to its self-healing ability • Optimizing self-healing polymers with copolymer, healing agents, or extenders is crucial • Lignin's UV absorption and antibacterial properties enhance polymer performance [ABSTRACT FROM AUTHOR]

Cellulose-based aerogels offer exceptional promise for oily wastewater treatment, but the challenge of low mechanical strength and limited application functions persists. Inspired by the graded porous structures in the animal skeleton and bamboo stem, we firstly report here a stepwise solvent diffusion-induced phase separation approach for constructing the gradient pore-density three-dimensional (3D) cellulose scaffold (GPDS). Benefiting from the regulation of competitive hydrogen bonding between the anti-solvents and the ionic liquid (IL) in cellulose solution, GPDS exhibits the decreased major channels size and increased minor pores amount gradually along the solvent diffusion direction. These endow GPDS with the characteristics of low density (0.019 g/cm) and super strength (high up to 870 KPa). The application of GPDS in the field of oil-water separation has achieved remarkable results, including oil/organic solvent absorption (13–25 g/g GPDS), immiscible oil-water mixture separation (high efficiency up to 99.8 %, flux > 2000 L/m2·h), and surfactant-stabilized oil-in-water emulsion (efficiency up to 97.7 %). Moreover, a simple hydrophobic treatment further realizes the efficient separation of water-in-oil emulsion (98.5 % efficiency). The as-fabricated GPDS accordingly achieves the multifunctional application in oil-water separation field. Thus, a new avenue is opened to construct 3D cellulose porous scaffold as adsorbent materials in oily wastewater treatment. [Display omitted] [ABSTRACT FROM AUTHOR]

Curcumin (Cur) as a natural food additive and photosensitizer has been widely applied on photodynamic sterilization and preservation for food, but the poor aqueous solubility and light stability restrict its extensive application. In this study, we report a Cur nanocapsules (Cur-CDs) made by carbon dots (CDs). Attributing to the hydrogen bonds formed between Cur and CDs, Cur-CDs exhibits excellent Cur aqueous solubility each to 9286.98 ng/mL (enhanced by 246.27 times) and light stability (enhanced by 1.51 times). The photogenerated electron transmission from Cur to CDs in addition resulted in >1.23 and 1.60 times generation of •O 2 − and •OH, compared to that of bare Cur. Accordingly, 5.73 × 103 CFU L. monocytogenes , and 5.43 × 103 CFU S. aureus were killed by 0.06 mg/mL Cur-CDs within 20 mins of blue light, showing the promising potential in the development and application of safe and environmentally friendly non-thermal sterilization technology based on Cur-CDs. [Display omitted] • The aqueous solubility of Cur is enhanced up to 9286.98 ng/mL. • Hydrogen bonds formed between Cur and CDs improved the light and thermal stability. • Electron transfers from Cur to CDs lead to enhanced photogenerating ROS. • L. monocytogenes is sensitive to the photodynamic treatment of Cur-CDs. • Cur-CDs cause ROS destruction to bacteria cellular membrane under blue light. [ABSTRACT FROM AUTHOR]

[Display omitted] • A VO 2 @CC self-supporting electrode was designed for aqueous ammonium ion batteries. • The battery capacity surpasses that of other ammonium storage electrode materials. • The as-prepared VO 2 @CC shows excellent rate capability. • The insertion and extraction mechanism of NH 4 + in VO 2 was revealed. Among these aqueous (non-)metal ion battery systems, ammonium ions are drawing increasing attention due to its unique advantages including small molar mass, abundant reserves and nontoxicity. However, suitable NH 4 + hosting materials with rational structure design are still in high demand to build high performance ammonium ion batteries (AIB). Herein, a graphene-like vanadium dioxide (VO 2) vertically growing on carbon cloth (CC) is reported as self-supporting electrode for AIB. The three-dimensional conductive carbon fiber substrate and the warped graphene-like VO 2 lead to enhanced NH 4 + transport and shortened diffusion length. As a result, the as-prepared VO 2 @CC displays an initial specific capacity up to 250.1 mAh g−1 at the current density of 1 A g−1. After 1000 cycles, it still maintains a capacity of 60.4 m Ah g−1. A series of ex-situ characterizations provides firm evidence that the insertion and extraction of NH 4 + in VO 2 are realized through the formation and breakage of hydrogen bonds. When combined with activated carbon (AC) to form a hybrid battery VO 2 @CC//AC, an initial discharge capacity of 74.98 mAh g−1 with the capacity retention of 43.64 % after 200 cycles is achieved, while the efficiency is maintained at about 92 %, surpassing other reported vanadium-based materials. [ABSTRACT FROM AUTHOR]

[Display omitted] • The renewed and corrected interpretations of experimental vibrational spectra and hydrogen bonds in the L- and D- iso ascorbic acids. • The d(OO) = f(γ(OH)) correlation is a tool for verification of the dissimilarity between the resonance-assisted hydrogen bond (RAHB) and the charge assisted hydrogen bond (CAHB). • The difference between the bridged proton dynamics of the intramolecular and intermolecular hydrogen bonds in ascorbic acids shown by CPMD and DFT calculations. The studies of two isomers of ascorbic acid and their deuteroanalogues, presented in the paper, have been accomplished by vibrational spectroscopy methods and quantum-chemical simulations. The spectroscopic research of L-ascorbic and D-isoascorbic acids have been carried out by the infrared (IR) and Raman (R) techniques. On the basis of the obtained results the spectral interpretation of the hydrogen bonded groups of ascorbic acids has been performed. Car-Parrinello Molecular Dynamics (CPMD) and Density Functional Theory (DFT) have been employed to support spectroscopic experimental findings and shed light onto the bridged proton dynamics in the L- and D- isomers of ascorbic acids. The accurate assignments of the hydrogen bond modes have been accomplished with the application of deuterosubstitution, CPMD-solid state simulations and Potential Energy Distribution (PED) analysis. The spectral and structural results have shown that dependency ν(OH) = f(γ(OH)) is the most common for the OHO hydrogen bond, whereas dependency d(OO) = f(γ(OH)) differs as for the ionic and resonance assisted hydrogen bonds. [ABSTRACT FROM AUTHOR]

Constructing hydrogen bonds through the heterojunction is expected be a successful tactic for achieving efficient charge separation. Here, we presented a heterojunction between 1,3,6,8-Tetra(4-carboxyphenyl) pyrene (T) and carbon nitride (CN), named T/CN. Hydrogen bonds formed between carboxyl groups of T and pyridine N in CN through the heterojunction. T/CN exhibited improved visible light absorption and enhanced charge carrier separation. The yield of CH 4 over T/CN reached up to 17.8 μmol·g−1·h−1, ∼7 times higher than that of CN (2.55 μmol·g−1·h−1). This work improved the photocatalytic performance of carbon nitride by synthesizing heterojunction catalysts containing hydrogen bonds, which provided a scheme for the diversified development of heterojunction catalysts. [Display omitted] • The heterojunction between 1,3,6,8-Tetra(4-carboxyphenyl) pyrene and carbon nitride (T/CN) was constructed. • Hydrogen bonds were formed through the heterojunction. • The yield of CH 4 over T/CN reached 17.8 μmol·g−1·h−1 under stimulated sunlight. [ABSTRACT FROM AUTHOR]

The objective of this research was to fabricate pH-responsive and active films based on gellan gum (GG) and pullulan (PL) with extracts of Broussonetia papyrifera fruits (BPFE) and leaves (BPLE) by a casting method. Results indicated that the extracts had good compatibility with GG and PL, which were uniformly distributed throughout the matrix. The incorporation of BPFE and BPLE increased the thickness, UV–vis barrier property, mechanical strength, thermal stability and moisture content of the films, while decreasing the water contact angle. Notably, the films exhibited enhanced antioxidant properties, with maximum radical scavenging rates of 77.45 % using 2,2 Diphenyl-1-picrylhydrazyl and 66.21 % using 2,2′-azino-bis (3-ethylbenzothiazoline-6-sulfonic acid). The antibacterial capability of the films also increased significantly after adding BPLE and BPFE. The results of XRD and FTIR showed that BPFE was bound to GG and PL by hydrogen bond. The release behavior of BPFE from the films agreed best with the first-level kinetic model. Furthermore, the films displayed obvious color responses to ammonia gas and different pH environments. Simultaneously, the films were applied to monitor the freshness of Pelteobagrus fulvidraco fish. The color parameters of the films demonstrated high correlations with the freshness indexes measured through standard laboratory procedures. • The extracts of Broussonetia papyrifera were incorporated into intelligent films. • Anthocyanin could interact with GG/PL chains through hydrogen bonds. • The film could be used to monitor the freshness of fish. • Intelligent films containing anthocyanin showed pH-sensitive and ammonia-response properties. [ABSTRACT FROM AUTHOR]

• A fully physically crosslinked, strong and tough polyion complex (PIC) hydrogel adhesive PNaSS/P(DAC- co -VDT) was fabricated. • The Hofmeister effect was taken advantage of to further enhance the mechanical properties of PNaSS/P(DAC- co -VDT). • The mechanical data of PNaSS/P(DAC- co -VDT) was analyzed using Mooney-Rivlin model and Creton's viscoelastic model. • The influence of polymer entanglement on the PIC hydrogel network structure was explored. Polyion complex (PIC) hydrogels possess excellent strength and toughness due to the dynamic and synergetic energy dissipation mechanism associated with the co-existence of both strong and weak bonds, ionic and hydrogen, in their networks. On the other hand, PIC hydrogels usually exhibit poor wet adhesion properties. Furthermore, the role such dynamic energy dissipation mechanism plays in determining interfacial binding is unknown. To address these challenges, here, we report the fabrication of an adhesive PIC hydrogel, poly(sodium p -styrenesulfonate) (NaSS)/poly(acryloyloxyethyltrimethyl ammonium chloride (DAC)– co -2-vinyl-4,6-diamino-1,3,5-triazine (VDT), i.e. PNaSS/P(DAC -co- VDT), by introducing a multi-hydrogen bonding capacity functional co-monomer, VDT, and solvent-induced gel phase separation into the fabrication process. The resulting hydrogel exhibited as high as 174 kPa adhesion strength, with retained high mechanical properties, typically 1.2 MPa tensile strength, 2.12 MPa Young's modulus, and 452% strain. The mechanical properties of PNaSS/P(DAC -co- VDT) were tunable by adjusting the content of VDT and of the total monomer concentration in hydrogel precursor solutions (C m), as well as by taking advantage of the Hofmeister effect. The dynamic modulus spectra of PNaSS/P(DAC -co- VDT) hydrogels at different C m 's in extended frequency windows with time–temperature superposition method (TTS) were acquired and analyzed to explore the influence of polymer entanglement on the hydrogel network structure. The microscopic structure-macroscopic mechanical property relationship of PNaSS/P(DAC -co- VDT) hydrogels at different C m 's and immersed in different salt solutions was further studied using the Mooney-Rivlin equation and by fitting the tensile data to Creton's viscoelastic model. This study may provide new insights into designing and constructing strong and tough PIC hydrogel-based adhesives. [ABSTRACT FROM AUTHOR]

• Provided a new strategy that combines biomimetics with microstructure control. • PCL-HBU3 exhibits excellent mechanical and self-healing properties. • First imitation of connective tissue for self-healing material construction. • Developed multifunctional self-healing conductive composites. Achieving a balance between mechanical strength and self-healing efficiency in self-healing materials is challenging yet crucial. This work introduces PCL-HBU, a polyurethane material designed for the first time to mimic collagen fibers, elastic fibers, and vascular networks of connective tissue, with excellent mechanical properties and self-healing efficiency. Meanwhile, by adjusting the 2-ureido-4-[1H]-pyrimidinone (UPy) and N,N-bis(2-hydroxyethyl)oxamide (BHO) ratio, this work creatively developed PCL-HBU3 with three distinct phase structures: amorphous region, soft segment crystallisation, and hard segment crystallisation, which approach confers excellent mechanical properties to the material. PCL-HBU3 exhibits a tensile strength of 70.0 MPa and elongation at break of 1500 %. It can recover from 600 % elongation within 20 s, achieving 100 % elongation at break self-healing efficiency. Furthermore, the composite conductive material fabricated using PCL-HBU3 as the matrix showcases self-healing abilities and holds promise in motion detection and sound recognition applications. [ABSTRACT FROM AUTHOR]

Enrofloxacin (ENR) residues in animal-derived food and water threaten human health. Simple, low-cost and on-site detection methods are urgently needed. Blue emitting carbon quantum dots (CQDs) and orange rhodamine B (RhB) were used as recognition and reference signals, respectively, to construct a ratiometric fluorescence sensor. After the addition of ENR, the color of the sensor changed from orange to blue because hydrogen bonding induced a considerable increase in CQDs fluorescence. Based on this mechanism, a simple and low cost on-site portable sensing platform was constructed, which integrated a stable UV light strip and a smartphone with voice-controlled phototaking function and an RGB app. The t -test results of spiked ENR recoveries for diluted milk, honey and drinking water revealed no significant differences between the ratiometric fluorescent sensor and portable sensing platform. Thus, this portable sensing platform provides a novel strategy for on-site quantification of quinolone antibiotics in foodstuffs and environmental water. • Fast synthesis of a novel carbon quantum dots with blue luminescence. • Sensitive ratiometric fluorescent sensor was constructed based on hydrogen bonding induction. • Portable sensing platform for ENR detection in diluted milk with high accuracy and low detection limit as 7.16 nM. [ABSTRACT FROM AUTHOR]

The constant-temperature θ(t) thermal decay discriminates the performance of the quasisolid water from that of the saturated NaCl supersolid solution, unveiling the respective O:H–O bond relaxation dynamics. [Display omitted] • O:H–O bond specific-heats disparity entitles the quasisolidity of negative thermal expansivity. • The H–O contracts ∼10 % in the supersolid phase owing to electrification and undercoordination. • Polarization drives the supersolid phase with the ω H shifting from 3200 to 3450 cm−1. • The viscoelastic, hydrophobic supersolid is less dense, more thermally diffusive, and stabler. This work features the recent findings of the quasisolid (QS, or quasi-liquid) in the temperature domain and supersolid due to electric polarization or molecular undercoordination, which are beyond the scope of the P-T phase diagram. The cooperativity of the coupling O:H–O bond in its segmental length, energy, specific heat, and associated polarization derive these abnormal phases. The specific-heat disparity defines structure phases varying from XI to Vapor and mass density evolution under ambient pressure. Possessing negative thermal expansivity (NTE), the QS phase transfers the liquid to the solid phase, which fosters ice buoyancy. The supersolid phase presents in the skin of water, ice, and droplets, and the ionic hydration cells and volumetric water with a current flow or under ∼106 eV/cm electric bias. The H–O bond of the supersolid phase is 8 ∼ 10 % shorter and vibrating at frequencies 7.3 % higher than that of the standard pristine water (0.1 nm in length and 3250 cm−1 in frequency). The supersolid has extraordinary elasticity, mechanical strength, optical reflectivity, structure order, thermal stability and diffusivity, catalytic capability, and chemical reactivity but 25 % lower mass density. The gel-like supersolidity endows ice and water with high hydrophobicity, viscoelasticity, catalytic and hydro-voltaic capability, and thermal diffusivity. The H–O bond contracts and absorbs energy during the Liquid-QS-Ice phase transition while doing contrastingly in the supersolid phase of the saturated NaCl solution under 254 K temperature. [ABSTRACT FROM AUTHOR]

Urea and barbiturates are bioactive compounds with diverse applications, ranging from pharmaceuticals to industrial processes. In reference to their biological relevance, it is essential to detect and quantify urea and barbiturates with high selectivity and sensitivity. The development of synthetic receptors for their recognition is a topic of research in supramolecular chemistry. This review highlights the progress in the development of synthetic receptors in last four decades for the selective recognition of urea and barbiturates. [Display omitted] • Synthetic receptors for urea recognition. • Synthetic receptors for barbiturates. • Macrocyclic and acyclic receptors. • Comprehensive review work on urea and barbiturate recognitions. Urea and barbiturates are bioactive compounds with diverse applications, ranging from pharmaceuticals to industrial processes. Urea functionality and barbiturates are present in various bioactive substances, including several clinically approved drugs. For analytic, diagnostic, and therapeutic applications, it is essential to detect and quantify urea and barbiturates with high selectivity and sensitivity. The development of the synthetic receptors for urea and barbiturates recognition involves the incorporation of specific functional groups and structural motifs to create binding sites that can interact selectively with urea and barbiturates. Consequently, a myriad of receptors for selective recognition and sensing of urea and barbiturates have been reported to date. The binding affinity, selectivity as well as supramolecular host–guest interactions of these receptors were studied by various methods, including UV–vis, fluorescence, 1H NMR titration, and single crystal X-ray diffraction analysis. These receptors offer valuable tools for detecting and quantifying urea and barbiturates in complex biological and environmental samples, leading to advancements in various fields and facilitating the development of novel diagnostic and therapeutic strategies. This review highlights the progress in the development of synthetic receptors for the selective recognition of urea and barbiturates. [ABSTRACT FROM AUTHOR]

Breaking hydrogen bond in metal free carbon nitride (CN) to increase peroxymonosulfate (PMS) adsorption for surface-mediated electron transfer has been challenging. Herein, we incorporated N−C N monomer into CN to break hydrogen bond by the introduction of polyvinylpyrrolidone (PVP). The developed nonradical oxidation system achieved selective decomposition of highly hydrophilic contaminants and efficient removal of chemical oxygen demand (58.0%), total phosphorus (88.1%), ammonia nitrogen (100.0%) and total nitrogen (67.8%) from the secondary effluent in a continuous flow reactor. This was attributed to that the breakage of hydrogen bond accelerated the redistribution of electron densities at C and N sites, leading to an increase in the adsorption energy of N site to PMS. This promoted the formation of PVP/CN-PMS* complex for the selective and efficient removal of organics and inorganics. This work provided a new perspective for the selective and long-term treatment of practical wastewater. [Display omitted] • Surface-mediated electron transfer system was constructed by breaking hydrogen bond. • The effect of hydrogen bond in carbon nitride on PMS activation pathway was revealed. • PVP/CN/PMS/vis system selectively remove highly hydrophilic contaminants. • The efficient and continuous flow treatment of practical wastewater was achieved. [ABSTRACT FROM AUTHOR]

Self-healing bitumen can significantly enhance the durability and service life of bituminous pavement, thereby reducing the need for frequent maintenance and repairs. In this study, isophorone diisocyanate (IPDI), hexamethylene diisocyanate (HDI), and isophorone diamine (IPDA) were utilized to design asymmetric dynamic hard segments, imparting self-healing properties to polyurethane even at room temperature. Particular emphasis was placed on hydrogen bonding, as its reversible formation serves as a primary mechanism for the self-healing characteristics of the material. During the synthesis of polyurethane (PU), two different composition ratios were employed to produce two types of PU with distinct chemical structures, molecular weights, and dynamic crosslink densities, which were characterized using NMR, FTIR, GPC, and DMA, respectively. Furthermore, these two PU types exhibited varying mechanical properties and glass transition temperatures, leading to differences in the rheological properties of the corresponding PU-modified bitumen. Dynamic frequency sweep test results indicated that bitumen modified with PU exhibiting higher molecular weight and narrower molecular weight distribution had superior rutting resistance and enhanced room-temperature self-healing capabilities. The underlying reasons for this improvement can be attributed to the hydrogen bonding present in the PU as well as the phase separation structure between the PU and bitumen. • Self-healing polyurethane (PU) was synthesized with a strategy of asymmetric dynamic hard segments. • PU with close ratio of hard/soft segments had higher hydrogen bonding content. • Dynamic crosslink density is much higher for PU with high molecular weight and narrow molecular weight distribution. • Rutting resistance of PU modified bitumen is enhanced by high crosslink density. • More hydrogen bonds in the PU leads to stronger self-healing ability in corresponding PU modified bitumen. [ABSTRACT FROM AUTHOR]

Hydrogel materials with hydrophilic cross-linked network exhibit remarkable super-wettability, enabling their widespread application in oily wastewater treatment. However, the single and loose structure lacks sufficient strength and porosity to resist long-term degradation. Herein, a structural synergistic molecular strategy was reported to introduce reinforcing phase structures and interfacial active sites into the polymer networks for long-term oil-water emulsion separation. The carbon skeleton was uniformly interspersed through the strongly hydrogen-bonded polymer chains via covalent bonds, resulting in a hydrogel network with high mechanical strength and exceptional flow conductivity, which maintained a separation flux of 1233 L m−2 h−1 after 20 separation cycles under gravitational force. Dense negative charges on the surface disrupted the internal charge stability of the oil-water emulsion, leading to remarkable demulsification with a separation efficiency exceeding 99 %. Simultaneously, the strong redox reaction of the photoheterojunction effectively removed organic dyes under visible light, enhancing the overall antifouling performance. This study provided a feasible strategy at the molecular level for optimizing the suitability of hydrogels for oil-water emulsion separation. [Display omitted] • Dual-network membranes are prepared by a freeze-assisted hydrothermal strategy. • The interfacial active sites formed by pyrolysis chains enhances the separation efficiency of oil-in-water emulsions. • Photocatalytic heterojunction of the membrane enables the degradation of organic dyes under natural light. • The transport effect of fibers endows gravity-driven separation. • The stable hydrogel layer provides exceptional antifouling properties. [ABSTRACT FROM AUTHOR]

Regional water scarcity is among the most urgent challenges of global climate change. Atmospheric water harvesting is a promising method to mitigate these challenges, and the atmospheric water generator (AWG) is already an established technology. Although this method can produce over 10,000 L of water per day, the water's quality has not been studied in depth. Air pollutants, especially volatile organic compounds (VOCs), are potential contaminants of water produced from air. We evaluated the chemical and physical parameters of different VOCs that might influence their ability to be transferred from air to AWG water. Our findings strongly suggest that the ability to form hydrogen bonds is a key factor in this transfer. Henry's law constant, polarity, and intrinsic solubility were the main predictors of a VOC's transfer to AWG water. Hence, aliphatic or aromatic compounds (such as benzene or octane) were not found at significant concentrations in AWG water (e.g. above WHO guidelines), whereas ammonia and alcohol compounds were. This should be taken into consideration when analyzing potential contaminants in harvested atmospheric water. The condensation process itself was also found to enhance the transfer of VOCs into water droplets, and higher relative humidity (%RH) also increased VOC transfer. Gas-phase infrared spectrum analysis of VOCs at different %RH revealed possible interactions between water vapor and specific VOCs in the air. However, our main conclusion from this study is that VOC transfer from the air into AWG water occurs predominantly via dissolution in the condensed droplets, and strongly depends on their chemical properties of polarity and hydrogen-bond formation. [Display omitted] • The transfer of VOCs into harvested atmospheric water is significantly influenced by their polarity and Henry's constant. • Hydrogen-bond formation is a key factor in VOC transfer to harvested water. • Droplet condensation enhances VOC transfer to harvested water, primarily through the dissolution of VOCs on water droplets. • High relative humidity increases the presence of airborne VOCs in harvested water. [ABSTRACT FROM AUTHOR]

• Enhanced adsorption on coal dust surfaces following fluorocarbon treatment. • Immersion wetting more discernible than collision contact and adsorption wetting. • PFPA and PFTA exhibit superior low-concentration immersion wetting capabilities. • Structural among fluorocarbon molecules influence adsorption, immersion wetting. To explore methods for enhancing the wetting performance of coal dust to mitigate its hazards, this study selected four different structures of non-ionic fluorocarbon solutions: perfluorinated propyl acrylate (PFPA), perfluorooctyl acrylate (PFTA), perfluorooctyl sulfonyl phenyloxy ethyl methylacrylate (PPM), and perfluoro propanoic acid (PFA). The dynamic wetting performance and mechanisms of these solutions on coal dust were measured and analyzed through kinetic calculations. The results indicate that all four fluorocarbon solutions achieve optimal wetting performance at a concentration of 0.3 %. Comprehensive analysis shows that their wetting ability follows the order PFPA > PFTA > PPM > PFA. Further analysis reveals that coal dust treated with PFPA shows an increase in structures such as COOH and C O. The relative concentration distribution indicates partial overlap between the fluorocarbon solution and water, with an overlap range of 8.2 Å. Additionally, the maximum diffusion coefficient is 0.577 Å/ps, and the system's adsorption energy is the highest at −5757.25 kcal/mol. [ABSTRACT FROM AUTHOR]

• Four oxygen atoms actively participated in forming hydrogen bonds and water bridges. • C atoms of the D and E rings form hydrophobic interactions more than other C atoms. • N7 atom was mainly involved in the formation of cation-π interactions. • The number of π-π interaction depends on the content of aromatic residues. • ΔG_Lipo and ΔG_vdW were two important forces driving protein-berberine interaction. Structural modification on berberine has garnered considerable attention among medicinal chemists as a means to enhance its therapeutic potential. The dissection of macrobiomolecule-berberine interactions is pivotal for guiding such modifications. In this study, four diverse crystal complexes of protein-berberine were selected, and simulated by molecular dynamics, in which each complex was conducted five times. Subsequently, the interactions of protein-berberine were collected, and analyzed by in-house scripts. Our findings indicated that the four oxygen atoms, namely O15, O16, O17, and O18, actively participated in the formation of hydrogen bonds and water bridges; the carbon atoms within the D and E rings were able to form hydrophobic interactions more than other carbon atoms; the positively charged N7 atom predominantly participated in the formation of cation-π interactions; π-π interactions were prevalent in the A, B, and D rings, with their frequency influenced by the presence of the residues Trp, Tyr, His, and Phe in the binding pocket. In the free energy decomposition analysis, the terms ΔG_Lipo and ΔG_vdW emerged as the most significant contributors to the overall energy, with ΔG_vdW accounting for over 50% of the energy contribution. Notably, the contribution of ΔG_Packing to the free energy was substantially greater than that of ΔG_Hbond, which contributed less than 1%. These insights into molecular interactions provide valuable guidance for the structural modification of berberine, such as site selection of structural modification, group optimization with the improvement of van der Waals and hydrophobic interactions, and the trade-off between hydrogen bonding and π-packing interactions in terms of interaction weights. [ABSTRACT FROM AUTHOR]

Understanding the solvation process requires an understanding of how the solvent affects the molecular cluster configurations. The current study examined the impact of solvents on the structures of the hydrated Cu 2 + cation, as well as the temperature dependence, and the energetics of the hydrated Cu 2 + cation clusters from sizes n = 1 from n = 10 (Cu 2 + (H 2 O) n = 1 − 10). The potential energy surfaces (PESs) in the solvent phase (represented by a dielectric continuum medium) at the MP2/6-31++G(d,p) level of computation have been comprehensively investigated. We employed the integral equation formalism polarized continuum model (IEF-PCM) to describe the dielectric continuum medium. It is pointed out that changes in PESs of hydrated copper dication isomers and structural morphologies occur in the continuum medium. Thus, the relative energies are smallest at T=0 K and for the cluster populations of Cu 2 + (H 2 O) n = 1 − 10 are modified. Thus, in the solvent phase, the competition between the conformers is more severe than in the gas phase. Furthermore, highly coordinated conformers are more favorable, and favored conformers in the gas phase are disfavored in the solvent phase. The structural investigations are validated by the analysis of Wiberg Bond Index (WBI) at 300 K. In the solvent phase, the WBIs of the most stable isomers are the smallest and the WBIs of axial bonds are lower than those of equatorial bonds. Concerning the energy analysis, the binding energies were predicted for enormous sizes (at saturation) using a fit function. Thus, the new values of the binding energies obtained are -5467.8 and ▪ in the gas and solvent phases respectively. All these observed differences are due to the effects of the implicit solvent. • The Cu2+ ion is hexa- and penta-hydrated in Cu2+(H 2 O) n=1-10 clusters in solvent phase. • The dative bonds are shorter in solvent phase than in gas phase. • The structural investigations are validated by the analysis of WBI at 300 K. • New values of the binding energies per water molecule at n = ∞ are predicted by fitting the data with a fit function. • The binding energies were predicted for enormous sizes (at saturation) using a fit function. [ABSTRACT FROM AUTHOR]

[Display omitted] • Reversible phase transition of 1-nitropyrazole was observed at 2.2 GPa. • Ab initio calculations were used to explain changes in molecular arrangements and hydrogen-bonded networks. • Hirshfeld surfaces and fingerprint plots were used to compare packing patterns. • Phase transition was likely caused by the distortion of hydrogen-bonded networks. The study investigated the behavior of N-nitropyrazole (1-NP, C 3 H 3 N 3 O 2) under high pressure using a diamond anvil cell, Raman spectroscopy, and simulation calculations. The pressure–volume relationship of the sample, molecular interactions, and changes in optical Raman were analyzed. The Raman experiments revealed abnormal vibration intensities and a discontinuity in peak position at 2.2 GPa. For instance, the C-H stretching vibration produces a new vibration peak under pressure, and the NO 2 torsion mode continues to red shift beyond 2.2 GPa. These observations suggest that the crystal's phase transition results from the distortion of its hydrogen-bonded network structure. The pressure relief experiment confirms the reversibility of the phase transition. [ABSTRACT FROM AUTHOR]

Cr(VI) is a representative heavy metal which has significant toxicity to biological organisms. Ion-imprinted polymers (IIPs) have been recognized as effective adsorbents to remove Cr(VI) from environment. Among them, imidazole derivatives are expected to serve as potential monomers for Cr(VI)-IIPs, but the binding mechanisms of monomers with Cr(VI) remain unclear, which makes Cr(VI)-IIPs design having rare sound theory to be guideline. In this work, the suitable functional monomer of Cr 2 O 7 2--IIPs was screened among five imidazole derivatives (adenine, cytosine, uric acid, l-histidine, 1-methacryloyl imidazole) with a target-monomer binding affinity guide strategy, and the optimal self-assembling conditions were investigated using theoretical calculations and experimental methods. Adenine exhibited the highest potential among the five candidate monomers, followed by cytosine. The optimal ratio of target and monomer was determined to be 2:3. Furthermore, a 5:5 mixture of ethanol and cyclohexane was identified as the most suitable solvent for the pre-polymerization environment, while epichlorohydrin acted as the most appropriate crosslinker. Additionally, the binding nature of non-covalent interaction between target and monomer was identified to be electrostatic-dominated hydrogen bonding. These mechanistic insights provide valuable theoretical support for the rational design of Cr 2 O 7 2--IIPs, which are significant for IIPs development as adsorbents for contaminants detection and removal from environment. • Adenine was a potential functional monomer of Cr 2 O 7 2- IIPs among imidazole derivatives. • The binding interactions between Cr 2 O 7 2- and adenine/cytosine was hydrogen bond. • Self-assembling conditions of IIPs can be obtained under template-monomer binding affinity guide strategy. • Sovent ethanol-cyclohexane mixture and crosslinker epichlorohydrin are optimal for Cr 2 O 7 2- IIPs preparation. [ABSTRACT FROM AUTHOR]

The biochar after long-term application will inevitably undergo ageing, thus promoting or inhibiting its remediation efficiency for antibiotics due to the differences in feedstocks and ageing process. To elucidate the adsorption performance and mechanisms of norfloxacin (NOR) by the different aged biochars, a batch of fresh biochars (BCs) prepared from Platanus orientalis Linn. leaf at 400 and 700 ℃ were aged by H 2 O 2 (HBCs) and KMnO 4 (MBCs) to simulate the natural ageing process. Compared with BCs, HBCs and MBCs showed larger specific surface area, richer micropores and O-containing functional groups. The maximum adsorption capacities of MBCs (43.96–49.32 mg g−1) and HBCs (18.38–19.79 mg g−1) were generally greater than those of BCs (16.44–20.01 mg g−1), which was resulted from the enhanced pore filling and hydrogen bonds. Furthermore, MBCs introduced with MnO x showed higher adsorption performances than those of HBCs, mainly due to the surface complexation. Na+ and Ca2+ inhibited the NOR adsorption by all the aged biochars. Humic acid and citric acid enhanced NOR adsorption at pH 3.0 but weakened the adsorption at pH 7.0. Furthermore, the NOR removal efficiency of BCs and aged biochars in the natural waters were reduced by 20–25 % and 6–17 %, respectively, showing the excellent sorption performance of the aged biochars. Our findings clarified the enhanced adsorption capacities of NOR by the aged biochar and the potential adsorption mechanism, providing the evidence for predicting the environmental fate of antibiotics in water environment and designing the functional biochars for controlling antibiotic pollution. • Aged biochars had more micropores and O-containing functional groups. • Oxidation of biochars enhanced norfloxacin (NOR) sorption. • Enhanced pore filling and H-bond contributed to the improved adsorption. • Surface complexation contributed to enhanced sorption of KMnO 4 -aged biochars. [ABSTRACT FROM AUTHOR]

The depletion of natural resources for precious metals is occurring as the economy expands, and conventional recovery techniques often involve the use of hazardous reagents. We have successfully developed a novel deep eutectic solvent, choline chloride/sulfamide, which exhibits exceptional efficiency in forming a highly effective deep eutectic dissolution reagent with dibromohydantoin for the efficient recovery of precious metals. The acidity provided by sulfamide and the oxygen negative ions generated by choline chloride jointly initiate an attack on the N-Br bond in dibromohydantoin. Bromine radicals and Br 2 together promote the oxidation of precious metals. The Cl- and Br- ions form complexes to generate AuCl 2 Br 2 -, which effectively stabilizes the Au3+ species in solution. Under optimal reaction conditions, Au0 can be completely dissolved within 25 minutes. The average rate of gold dissolution in this DES dissolution reagent was 10,235.9 mg Au/(h·mol DBD), which is more than 200 times the average rate of gold dissolution in conventional cyanide. Moreover, DES dissolution reagent allows for recycling of the precious metal up to 6 times with dissolution rates consistently above 95 %. By adding it into an oxalic acid solution, the gold complex can be reduced to Au0 to achieve recycling of precious metals. [Display omitted] • A novel deep eutectic solvent where choline chloride is synthesized with sulfamide in various molar ratios. • A new precious metal dissolvent generated from dibromohydantoin with a deep eutectic solvent. • A novel system for the dissolution of precious metals enabling multiple recycling cycles. [ABSTRACT FROM AUTHOR]

[Display omitted] • Synthesized quaternized polyamine-based DES for enhanced CO 2 capture. • Employed FT-IR, DSC, and 2D 1H/1H NOESY for comprehensive DES characterization. • DES with MEA and EDA show superior CO 2 absorption due to lower viscosity. • Water additives enhance CO 2 absorption efficiency by creating additional voids. • Low-viscosity DES have potential for various industrial applications in CO 2 capture. This study explores the synthesis and characterization of deep eutectic solvents (DES) for efficient CO 2 capture, focusing on the hydrogen bonding strength between hydrogen bond acceptors (HBA) and donors (HBD). Tetraethylenepentamine (TEPA) was quaternized with hydrochloric acid (HCl) to produce HBAs, which were then combined with various HBDs, including monoethanolamine (MEA), diethanolamine (DEA), N-methyldiethanolamine (MDEA), ethylenediamine (EDA), triethylenetetramine (TETA), and TEPA. The DES were synthesized and their structures confirmed using FT-IR for functional group analysis and DSC for thermal behavior assessment. The molecular structure of DES was further elucidated through 2D 1H/1H NOESY, revealing significant effects of the HBA accepting site on physicochemical properties. Our results indicate that DES exhibit two distinct behaviors when water is used as an additive, creating additional voids during semicrystalline transitions and enhancing CO 2 absorption efficiency. DES composed of MEA and EDA demonstrated superior absorption performance due to their lower viscosity. Polyamine-based DES showed increased CO 2 capacity per mole of DES but reduced efficiency per mole of amine, attributed to increased viscosity from carboxylate formation. This research provides a detailed analysis of the hydrogen-bond network within DES and its impact on CO 2 absorption. By optimizing the selection of HBA and HBD, we developed low-viscosity DES, suitable for applications in porous material impregnation, membrane impregnation, and porous liquids. This study provides new insights into the role of free volume and hydrogen bonding in enhancing gas diffusivity and reaction kinetics. The findings contribute significantly to the development of advanced DES for industrial applications, offering a promising solution for mitigating greenhouse gas emissions and promoting a sustainable, low-carbon future. [ABSTRACT FROM AUTHOR]

[Display omitted] • The synergistic system of tartaric acid and isopropanol regulated hydrogen bond. • High yield of diosgenin was reached within the green and recyclable system. • The integrated technological process exhibited fine prospect of industrialization. • Porous carbon material could be prepared by the upgrading of the residual solid. Herein, a renewable system consisted of tartaric acid and isopropanol was developed to produce diosgenin efficiently from Dioscorea zingiberensis rhizomes. The yield of diosgenin reached 4.15% comparable to the highest value reported in previous researches. The combination of experiment and DFT calculation revealed that the acid-alcohol system could regulate the hydrogen bond interaction of each component in the rhizomes to disassemble the connection network and promote the release of saponin. Meanwhile, the intramolecular hydrogen bond of tartaric acid and the steric hindrance effect of isopropanol could prevent the esterification reaction and maintain the strong acidity of the system for the high yield of diosgenin. The scale-up experiment with a 100-fold feeding capacity was also conducted successfully. Furthermore, the technological process integrated with purification of diosgenin, recovery of organic acid and solvent and upgrading of residual solid to porous carbon materials has been established systematically to verify the prospective of industrialization. [ABSTRACT FROM AUTHOR]

• A new wurster-type twisted covalent organic framework (TN COF) was synthesized and characterized. • TN COF in 1,4-dioxane exhibits a highly selective and sensitive "turn-off" fluorescent and colorimetric sensing ability towards HSO 4 ˉ. • DFT calculation proved that the TN COF formed complex with HSO 4 ˉ via the hydrogen bonding. • TN COF has high recovery in the detection of HSO 4 ˉ in the practical water sample and serum. A novel wurster-type twisted covalent organic framework (TN COF) composed of N, N, N', N' -tetrakis(4-aminophenyl)-1,4-benzenediamine and 2,6-naphthalenedicarbaldehyde was synthesized and characterized. TN COF exhibits exceptional crystallinity, as well as remarkable thermal and chemical stability. TN COF in 1,4-dioxane exhibits highly selective and sensitive "on-off" fluorescent and colorimetric sensing ability towards HSO 4 ˉ over the other anions with fast response time. The fluorescence color of TN COF suspension changes from pink to blue under the 365 nm UV lamp. Meanwhile, the color also changes under day light from grapefruit color to colorless. Both the fluorescence intensity at 597 nm and absorbance at 255 nm are linear relationship against the concentration of HSO 4 ˉ over a broad range, with lower limits at the micromolar level. The XPS, FTIR spectra and DFT calculation prove that TN COF forms complex with HSO 4 ˉ via the hydrogen bonding. TN COF demonstrates high recovery for detecting HSO 4 ˉ in practical water samples and serum, making it a suitable chemosensor for the identification and detection of HSO 4 ˉ. [Display omitted] [ABSTRACT FROM AUTHOR]

[Display omitted] • IL pretreatment reduce pyrolysis temperature, achieve carbon reduction. • Fe ions enhances ionic liquid swelling and pyrolysis capacity of coal. • Study ionic liquids effect on coal physical and chemical structure by simulation. Investigate the effects of Ionic Liquid and metal ions on the swelling and pyrolysis characteristics. The simulation results show that IL can weaken intermolecular hydrogen bond of coal, Magnetic Ionic Liquid has a stronger modification effect after adding Fe ions, and hydrogen bond weakening leads to the improvement of coal swelling degree. After [Bmim]Cl modification, the swelling degree is increased by 17.37% compared with raw coal, and after [Bmim]FeCl 4 treatment, the swelling degree is further improved. Ionic liquid swelling also has a better effect on subsequent pyrolysis of coal samples, the modification effect of [Bmim]FeCl 4 is more significant, which increases by 6.77%. The swelling of MIL significantly reduces the pyrolysis activation energy of coal and thermochemical reaction temperature. On the one hand, the content of heavy groups in pyrolysis products is reduced, and on the other hand, the target of carbon emission reduction can be achieved. [ABSTRACT FROM AUTHOR]

[Display omitted] • Pb(II) ions strongly activate NaCl flotation but show negligible effects on KCl flotation. • This activation is observed forPb(II) only, not for Ca2+, Mg2+, Ba2+ and Cu2+. • Sodium/potassium laurate collectors aggregate into collector colloids on air bubbles. • Pb(II) ions alter the surface of collector colloids via ion substitution. • Hydrogen bonds between Pb(II) in colloids and hydrated NaCl surfaces promote flotation. In the flotation of water-soluble minerals (e.g., NaCl and KCl crystals), the high ionic-strength environments alter the typical interfacial interactions and challenge the applicability of conventional flotation theories. Here, we report an intriguing effect of Pb(II) ions on the flotation of NaCl and KCl crystals in brines using sodium/potassium laurate as collectors. We revealed contrary effects of Pb(II) ions on flotation recoveries of NaCl crystals and KCl crystals. Pb(II) ions strongly enhance the NaCl crystals recovery but show no considerable effect on KCl crystals recovery. Interestingly, such activation is observed exclusively for Pb(II), not for Ca2+, Mg2+, Ba2+, and Cu2+. Our analysis using XPS and XRD rules out the adsorption of lead on crystal surfaces but reveals a significant presence of lead on the collector colloids via ion substitution. In particular, we unveil a crucial role of interfacial hydrogen bonding between Pb(II) ions in the collector colloids and the outward-pointing OH groups of surface-bound water on NaCl crystals. These hydrogen bonds sustain a strong bubble-particle attraction for high recovery of NaCl crystals. No similar hydrogen bonding is possible for KCl crystals which causes a poor recovery of this salt. These insights provide hints to tailoring the flotation conditions to enable efficient separation of water-soluble minerals, which is the core interest of the potash industry. [ABSTRACT FROM AUTHOR]

The high vaporization enthalpy of water attributed to the strong hydrogen bonds between water molecules is limiting the performance of solar evaporators. This work demonstrates a deliberate attempt to significantly reduce the vaporization enthalpy of water through the introduction of weak water-amine hydrogen bond interactions in hydrogel evaporators. In this article, bio-based chitosan-agarose/multiwalled carbon nanotube hydrogel film evaporators (CAMFEs) exhibit larger vaporization enthalpy reduction with the presence of primary amine groups in chitosan. An interplay between vaporization enthalpy reduction and water diffusivity leads to an optimal ratio of chitosan to agarose = 7:1 (CAMFE7) showing an impressive evaporation rate of 4.13 kg m−2 h−1 under 1 sun irradiation. CAMFE7 also exhibits excellent salt resistance, with a stable water evaporation rate, using brine water of up to 10 % salinity under continuous 1 sun irradiation. The high mechanical robustness together with its scalability makes CAMFE7 a highly promising material for practical drinking water production. [Display omitted] [ABSTRACT FROM AUTHOR]

To verfy their difference from isolated fatty acids, the absolute kinetics of peroxidation was studied for seven triglyceride-based oils of olive (OLI-1, OLI-2), high-oleic sunflower (SUN-HO), high-oleic and high-linoleic safflower (SAF-HO, SAF-HL) grapeseed (GRA) and borage (BOR), by oxygen uptake monitoring, using 2,6-di- tert -butyl-4-methoxyphenol and 2,2,5,7,8-pentamethyl-6-chromanol as reference inhibitors. Propagation constants (k p /M−1 s−1 at 303 K in PhCl) were respectively 34.8 ± 2.3, 35.1 ± 1.8, 40.6 ± 5.5, 36.0 ± 7.7, 160.8 ± 5.1, 145.1 ± 24.5, 275.1 ± 63.8, while oxidizability responded to empirical equation k p (2 k t)-½/M-½s-½ = 1.63 × 10−3[allyl >CH 2 /M] + 1.82 × 10−2[bisallyl >CH 2 /M], based on fatty acids residues assessed by GC–MS. Peroxidation kinetics was markedly different from that of isolated fatty acids. The H-bond basicity of all oils was measured by FT-IR affording Abraham's βH 2 values in the range 0.55 ± 0.03. H-bonding explained the protection of oils measured for seven reference phenolic antioxidants, except for the catechols quercetin and caffeic acid phenethyl ester, which were 2-to-4-folds more effective than expected, supporting a proposed different mechanism. • k p and 2 k t constants for triglycerides differ from those of their main fatty acids. • MUFA-rich triglycerides oxidize 40-folds faster than their isolated MUFAs. • A linear empirical equation predicted oxidizability from FAME analysis (r 2 = 0.992). • Protection and k i nh for antioxidants were explained by H-bonding to triglycerides. • Catechols quercetin and CAPE gave exceptional protection via different mechanisms. [ABSTRACT FROM AUTHOR]

Poly(vinylidene fluoride-hexafluoropropylene) (PVDF-HFP)-based solid electrolytes with wide electrochemical windows and high thermal stabilities are promising candidates for use in solid-state lithium batteries. However, the practical applications of these electrolytes are currently hindered by their low room-temperature ionic conductivity, limited Li+ transfer number, and the poor stability of the lithium/electrolyte interface. This study proposes a 'one stone, three birds' modification method, wherein a small amount of lithium carboxymethylcellulose (CMC-Li) containing rich hydroxyl groups is added to form abundant hydrogen bonds with numerous electronegative C–F groups in the PVDF-HFP molecular chain and lithium bistrifluoromethane sulfonimide (LiTFSI). The strong connections formed between CMC-Li and PVDF-HFP or TFSI− significantly reduced the crystallinity of PVDF-HFP, promoted the dissociation of LiTFSI, and anchored TFSI−, achieving a synchronous improvement in the ionic conductivity and Li+ transfer number. The hydrogen bonds drove the densification of the membrane surface, improving the lithium/electrolyte compatibility at the interface. The ionic conductivity of the modified electrolytes was 5.1 × 10−4 S cm−1 and the Li + transfer number was 0.72 at room temperature. A Li||Li symmetric cell demonstrated stable cycling over 1000 h at 0.2 mA cm−2, where the initial discharge capacity of an all-solid-state cell was enhanced to 165.1 mAh g−1, with steady cycling for 400 runs. Thus, this study provides a novel and effective method for promoting the practical application of solid-state electrolytes. [Display omitted] • CMC-Li produce hydrogen-bonds with PVDF-HFP and LiTFSI as O–H⋯F. • The crystallinity of PVDF-HFP was reduced and ion conductivity was improved. • Li + transfer number was enhanced through restraining the TFSI− by Hydrogen-bonds. • Achieving synchronous improvement in the ionic conductivity and Li + transfer number. • A Li.||Li symmetric cell demonstrated stable cycling over 1000 h at 0.2 mA cm−2. [ABSTRACT FROM AUTHOR]

[Display omitted] • Two isomers of the 2-(trifluoromethyl)acrylic acid–water complex are observed by rotational spectroscopy complemented by quantum chemical calculations. • The structures, populations, and non-covalent interactions of the two isomers are determined. • The fluorination effect is proved to only enhance the energy of O-H···O w hydrogen bond by compared the energies of the corresponding hydrogen bonds formed in similar complexes. This study explores the effects of the −CF 3 group on non-covalent interactions through a comprehensive rotational investigation of the 2-(trifluoromethyl)acrylic acid–water complex. Employing Fourier transform microwave spectroscopy complemented by quantum chemical calculations, two isomers, i.e., s-cis and s-trans structures, have been observed in the pulsed jet. Based on relative intensity measurements, the s-cis to the s-trans population ratio was experimentally estimated to be ∼ 1:1.2. Subsequently, a comparison of the non-covalent interactions was carried out between the three similar complexes, acrylic acid–water, methacrylic acid–water, and 2-(trifluoromethyl)acrylic acid–water, offering quantitative insights into fluorination affecting the strength of the formed hydrogen bonds important, e.g., in molecular recognition. [ABSTRACT FROM AUTHOR]

• The thixotropic gel YSL synthesized by AM, SMA, TA, KA and LAP showed good shear thinning behavior, thixotropic behavior, viscoelasticity and adhesion performance. • The shear thixotropic mechanism of gel YSL depends on the physical cross-linking of hydrophobic monomers and clay particles in the gel: hydrogen bonding, hydrophobic association and electrostatic interaction. • TA in the gel improves its adhesion ability in the leakage channels (TA and the rock surface will produce non-covalent bonding: metal coordination and cation-π). • Gel YSL can be used as a lost circulation material in the drilling field, plugging mechanism of gel YSL was explained. Gel-based plugging materials have become commonplace in addressing lost circulation wells. However, traditional gels are associated with challenges such as difficulties in injection, irreversible structural damage under high shear stress, poor retention capacity within leakage channels, resulting in diminished pressure-bearing capabilities, subpar sealing efficacy, and prolonged non-production periods. In this study, a plugging gel, denoted as YSL, was synthesized via free-radical aqueous solution polymerization using AM, hydrophobic monomer SMA, and TA as raw materials, with KA and LAP as inorganic additives. The physicochemical properties were characterized using FT-IR, TGA, and SEM. Additionally, the rheological properties, thixotropic behavior, viscoelasticity, adhesion performance, and plugging performance of the YSL gel were systematically investigated. The results indicate that increasing the hydrophobic monomer and inorganic clay particles can enhance the viscosity, thixotropic ability, and storage modulus of the gel, although excessive non-covalent interactions diminish the adhesion capability of TA in the gel. Compared to commercial polymer gels and bridging plugging materials, YSL exhibits superior pressure-bearing plugging capability. Additionally, plugging mechanism of the gel in leakage channels was analyzed. The findings suggest significant potential applications of YSL in drilling leakage prevention and plugging in the oil and gas industry. [ABSTRACT FROM AUTHOR]

[Display omitted] • Two novel DESs (DNS/TOPO and SA/TOPO) were prepared and characterized. • The DESs were first studied by the S/L leaching to separate Yb 2 O 3 and Lu 2 O 3. • This DES S/L leaching showed better separation factor (2.11) than other methods. • The lattice energy of REEs and the dissociation energy of DESs were calculated. This research reports the first study of selective leaching of ytterbium-lutetium oxides mixture with hydrophobic deep eutectic solvents (DESs), and high-efficiency and simple-prepared were used to separate and beneficiate lutetium. With hydrophobic DESs, which were formed with hydrophobic salicylic acid (SA) or 3,5-dinitrosalicylic acid (DNS) as the hydrogen bond donor (HBD) and hydrophobic tri-n-octyl phosphine oxide (TOPO) as the hydrogen bond acceptor (HBA), powdered eutectic mixtures of ytterbium-lutetium oxides were leached. The separation factor of ytterbium-lutetium was concluded to reached 2.11 with a solid-liquid (S/L) ratio of 1/50 g/ml, a temperature of 90 °C and a 4 h leaching time, and the experimental conditions, such as the S/L ratio, temperature and reaction time, were explored. The formation of intermolecular hydrogen bonds between the HBD and HBA was revealed through multiple methods, such as IR (disappearance of OH characteristic peaks), 1H NMR (formation of sharp peaks not present for intramolecular hydrogen bonds) and 31P NMR (shift of P = O peaks to higher fields). The lattice energies of the intermolecular hydrogen bonds and the solid oxide lattice energies, which were calculated with Gaussian 16 software (0.87 eV for SA/TOPO = 1:1 and 0.94 eV for DNA/TOPO = 1:1) and the Born–Haber cycle (12957.56 kJ/Mol for Yb 2 O 3 and 12993.59 kJ/Mol for Lu 2 O 3), provided a theoretical illustration of preferential Yb/Lu dissolution leading to separation. The stripping, regeneration and recycling capabilities of the DESs were investigated with stripping and recirculation experiments. Based on these results, the new DES as the leaching agent to separation of ytterbium lutetium oxide is identified as a new efficient mothed with industrialization potential. [ABSTRACT FROM AUTHOR]

• The hydrogen bond results in opaque hydrogen-bond crosslinked hydrogel. • The transparency of the hydrogel can be tailored by pH for encryption and decryption. • Dual-encryption microdevice was fabricated by 3D printing. • The device can be reversibly decrypted and encrypted in 4 and 1 min. Hydrogel-based physical dual-encryption typically relies on the reversible shape-deformation of polymer chains for the decryption. However, the stored information is confronted by indecipherability at the microscale because the intrinsic relaxation of polymer chains would disrupt the fidelity of encoded information. Inspired by female Doryteuthis opalescens squid's camouflage strategy (i.e. , switching a stripe on its mantle from nearly transparent to opaque white), we devised a reversible transmittance-changeable hydrogel layer to fully cover the mono-encrypted information layer for dual-encryption. The micro-structured hydrogel was manufactured via 3D printing to encode the information, which can be decoded by UV-induced fluorescent emission. Then, the white camouflage hydrogel was constructed to conceal the mono-encrypted layer, which will not affect the information encoding layer during the reversible polymer chain mobility. The information can be decoded with alkaline solution and UV irradiation in a rapid speed, i.e. , in 4 min, with good reusability. Moreover, the information was accurately unveiled even at microscale resolution, holding great promise for high-level encryption at the device level. [ABSTRACT FROM AUTHOR]