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This investigation employs first‐principles calculations to explore the interaction between imidazolium ionic liquids (ILs) and fluoride additives on lithium metal surface. Our focus lies in the comprehensive analysis of three distinct categories of fluorinated additives, each differing in their degree of fluorination. The computations reveal that fluorination plays a significant role in determining both the ionic conductivity and the formation of the solid–electrolyte interphase (SEI) film. Specifically, heightened fluorination enhances the oxidative stability of the system but diminishes the strength of solvent binding, resulting in the formation of larger salt/anion clusters and a decrease in ionic conductivity. Conversely, increased fluorination facilitates the interaction between fluorinated additives and the lithium metal surface, thereby aiding in the formation of a stable SEI film characterized by an abundance of inorganic LiF components. This is important as it serves to suppress dendrite growth and mitigate interface side reactions. Considering the combined influences of ionic conductivity and film formation, 1FP is suggested as the optimal candidate for pyridine‐based additive systems, with FEC preferred for cyclic ester‐based additive systems and BC for chain ester‐based additive systems. This study provides theoretical references for the design of ionic liquid‐fluorinated additive electrolyte systems that can protect the lithium metal anode. [ABSTRACT FROM AUTHOR]

Ionogels are emerging as high‐potential pseudosolid electrolytes for lithium‐metal batteries (LMBs), leveraging their intrinsic high ionic conductivity from entrapped ionic liquid (IL) electrolytes. However, their practical application is hindered by poor mechanical strength stemming from the confinement of ILs within a polymer matrix. To address this challenge, the formation of conformal polyion coatings with functional groups is reported to be relevant to LMBs’ application on ionogels, utilizing a layer‐by‐layer (LbL) assembly strategy. This approach significantly enhances the mechanical strength (Young's modulus and tensile strength) and electrochemical performance of ionogels, owing to the tailored interface modifications introduced by functional groups’ specific conformal polyion coatings. The core of this methodology leverages the inherent ionic structure of ionogels to enable facile interface modification through Coulombic interactions between polyanions and polycations. These conformally coated interface functionalized membranes show improved electrochemical performance when integrated with cathode materials such as LiFePO4 (LFP) and LiNi0.8Mn0.1Co0.1O2 (NMC811) in an LMB configuration, underscoring their potential for robust, high‐conductivity, pseudosolid membranes for LMB applications. These innovative pseudosolid membranes offer improved mechanical and electrochemical properties, leading to higher battery efficiency and safety, making them promising candidates for next‐generation LMB technology. [ABSTRACT FROM AUTHOR]

To explore the influence of reaction medium on the copolymerization behavior of acrylamide‐based copolymers, three types of copolymers (P(AM‐St)(ILs), P(AM‐MMA)(ILs), and P(AM‐AMPS)(ILs)) were synthesized by combining insoluble, slightly soluble, and easily soluble monomers with acrylamide in the 1‐butyl‐3‐methylimidazolium tetrafluoroborate ([BMIM]BF4) reaction medium. The reactivity ratio, Fourier transform infrared spectroscopy, 1H NMR spectroscopy, elemental analysis, and scanning electron microscopy were employed to characterize the copolymers' properties. The results indicated that in [BMIM]BF4 copolymerization, the reactivity ratio of AM and St in P(AM‐St)(ILs) decreased, the reactivity ratio of AM in P(AM‐MMA)(ILs) will increase. While the reactivity ratio of MMA will decrease. The reactivity ratio of AM in P(AM‐AMPS)(ILs) will increase and the reactivity ratio of AMPS will decrease. The distribution of AM and St segments in P(AM‐St)(ILs) molecular chains is more uniform and compact. When AM polymerizes with hydrophobic monomers (St) in [BMIM]BF4, its copolymer solution exhibits lower viscosity loss rates in temperature, shear, and salt resistance tests. Therefore, ionic liquids are more suitable as reaction media for the synthesis of hydrophobic‐modified polyacrylamides, which facilitate a more uniform distribution of hydrophobic monomers within the copolymer chains and exhibit enhanced resistance to temperature, salt, and shear stresses. [ABSTRACT FROM AUTHOR]

The energy storage capability of supercapacitors (SCs) strongly depend on the operating cell voltage of the electrolytes of choice. In this regard, the inherent distinct electrochemical stability of cations and anions is a factor of relevance for the operating cell voltage. The use of double salts sharing one ion has been described as an approach to circumvent this problem, but whether modifying the solvation structure of cations and anions with different solvent molecules (coordinating and/or non‐coordinating) could help balance their electrochemical stability in SCs has not yet been fully addressed. In this work, electrolytes are prepared by combining solvent mixtures and double salts, specifically 1‐ethyl‐3‐methylimidazolium bis(trifluoromethylsulfonyl)imide (EMIMTFSI) and 1‐ethyl‐3‐methylimidazolium tetrafluoroborate (EMIMBF4) in mixtures of water (H2O) and dimethysulfoxide (DMSO) as coordinating co‐solvents and acetonitrile (CH3CN) as a weakly coordinating one. It is found that the presence of this latter one helped to enhanced the cation solvation structure (above 9). This increase of the entropic features allows operating at cell voltages of up to 2.2 V and the subsequent enhancement of the energy storage capabilities and capacitance retentions (up to 15 Wh kg−1 and ≈87% after 10 000 cycles, respectively). [ABSTRACT FROM AUTHOR]

A facile and highly efficient protocol has been developed for the synthesis of extensively functionalized, fully substituted N‐methyl‐1,4‐dihydropyridines. This approach is a one‐pot pseudo‐three‐constituent cyclo‐condensation of aromatic aldehydes with (E)‐N‐methyl‐1‐(methylthio)‐2‐nitroethenamine (NMSM). This reaction presumably entails the Knoevenagel reaction followed by Michael addition and regioselective N‐cyclization with removing methanethiol and producing two C─C bonds and one C─N bond. The key advantages of this strategy include an optimized reaction time, achieving moderate to excellent yields, a straightforward experimental procedure, and the use of the ionic liquid 1‐ethyl‐3‐methylimidazolium acetate [(EMIM)Ac] as the catalyst. The resulting derivatives were well characterized by IR, 1H NMR, 13C NMR, and HRMS. [ABSTRACT FROM AUTHOR]

Diverse libraries of biaryls/heterobiaryls were synthesized by aryl/hetero‐aryl tosylates as coupling partners in the ligand‐free, Ni‐catalyzed Suzuki coupling reaction, and Pd‐catalyzed Hiyama cross‐coupling reaction in ionic liquids (ILs) as green solvent. In this method easily available and economically viable tosylates were coupled with readily available boronic acids and phenyltriethoxysilanes in Suzuki and Hiyama cross‐coupling respectively to yield the corresponding biaryls/heterobiaryls. Mild reaction condition(s), easy workup, moderate to excellent yield of the isolated pure products, wide substrate scope, and recycling/reuse of the ILs are the advantages of this method over the other reported methods. [ABSTRACT FROM AUTHOR]

Mixed matrix membranes (MMMs) with enhanced selectivity and permeability are investigated by incorporating deep eutectic solvents (DES) functionalized CeO2 as fillers. DES is well known owing to the intrinsic benefits of low cost, environmentally friendly, biodegradable, and CO2 philic nature. Characterization confirms the collaboration of polymer and functional CeO2 fillers. Experiments of gas separation show that the introduction of DES‐modified CeO2 fillers (2%–15%) significantly improves CO2 penetrability from 27 to 48 Barrer. The ideal separation factor of CO2/CH4 and CO2/N2 also increases from 46 to 62 and 60 to 86, respectively, with increasing filler percentage. MMMs correspond to the superior gas separation performance compared with DES liquid membranes. The collaboration between DES‐treated CeO2 and CO2 contributes to the improved results. The fabricated MMM films are tested under operating parameters, confirming the potential of ceria modified fillers for CO2 capture applications. This research reveals the advancements achieved by incorporating DES‐functionalized CeO2 fillers in MMMs, enhancing selectivity and permeability for CO2 capture. These findings correspond to the development of effective and viable membrane technologies for various industrial applications. [ABSTRACT FROM AUTHOR]

With the ever‐growing global demand for sustainable energy solutions, hydrogen has garnered significant attention as a clean, efficient, and renewable energy source. In the field of hydrogen production, catalyst research stands out as one of the foremost areas of focus. In recent years, the preparation of electrocatalysts using ionic liquids (ILs) and deep eutectic solvents (DESs) has attracted widespread attention. ILs and DESs possess unique physicochemical properties and are recognized as green media as well as functional materials. Cobalt‐based catalysts have proven to be efficient electrocatalysts for water splitting. Incorporating ILs or DESs into the preparation of cobalt‐based catalysts offers a remarkable advantage by allowing precise control over their structural design and composition. This control directly influences the adsorption properties of the catalyst's surface and the stability of reaction intermediates, thereby enabling enhanced control over reaction pathways and product selectivity. Consequently, the catalytic activity and stability of cobalt‐based catalysts can be effectively improved. In the process of preparing cobalt‐based catalysts, ILs and DESs can serve as solvents and templates. Owing to the good solubility of ILs and DESs, they can efficiently dissolve raw materials and provide a special nucleation and growth environment, obtaining catalysts with novel‐structures. The main focus of this review is to provide a detailed introduction to metal cobalt and its oxide/hydroxide derivatives in the field of water splitting, with a particular emphasis on the research progress achieved through the utilization of IL and DES. The aim is to assist readers in designing and synthesizing novel and high‐performance electrochemical catalysts. [ABSTRACT FROM AUTHOR]

To solve the downhole problems correlated with clay hydration swelling and dispersion under high‐temperature conditions, a 1‐aminoethyl‐3‐vinylimidazolium bromide ([NVim]Br) and a [NVim]Br/acrylamide copolymer (poly([NVim]Br‐co‐AM)) are synthesized and used as inhibitors. The molecular structures of [NVim]Br and poly([NVim]Br‐co‐AM) are characterized by FT‐IR and 1H‐NMR. The inhibition properties of [NVim]Br and poly([NVim]Br‐co‐AM) are evaluated by free swelling and dispersion tests, linear swelling, hot roll recovery experiments and thermogravimetric analyses.The inhibition mechanisms were revealed by X‐ray diffraction, zeta potential, wettability analysis and ESEM observation. The results showed that both [NVim]Br and poly([NVim]Br‐co‐AM) has significantly superior inhibition performance compared with the common inhibitors KCl, polyether amine D230 and polyquaternium‐7. Both [NVim]Br and poly([NVim]Br‐co‐AM) can resist 250 °C. [NVim]Br performed excellently in inihibiting both crystalline and osmotic swelling, which depended on the strong electrostatic adsorption and hydrogen bonds of imidazole cations and primary amine in [NVim]+. Poly([NVim]Br‐co‐AM) exerted excellent inhibition by minimizing osmotic swelling, reducing hydrophilicity and increasing clay bonding. The results are important for understanding the rational design of novel efficient inhibitors for drilling high‐temperature shale formation. [ABSTRACT FROM AUTHOR]

The ILs ([Li (synthetic esters)] NTF2) were prepared by the in situ synthesis method. The tribological behaviour of the ILs to friction pairs of Ti‐6Al‐4V titanium alloy against silicon nitride was studied by SRV‐V under different concentrations and friction frequencies; the wear scar was studied by SEM, XPS and TOF‐SIMS. The results showed that the friction coefficient and wear loss decreased gradually with the increase of the LiNTF2 content; when the LiNTF2 content reached a certain value (10%), the friction coefficient and wear loss did not change much. Tribofilm composed of titanium oxide, Al2O3, TiFO2, AlOF2, Ti2O4F and Al2O3F plays a major role in lubrication and anti‐friction effect. [ABSTRACT FROM AUTHOR]

Ionic liquids (ILs) are incorporated into traditional porous materials to create ILs‐functionalized porous materials, which exhibit excellent absorption capacity and good catalytic activity for CO2. As a result, they are extensively utilized in the chemical conversion of CO2. This paper specifically focuses on the utilization of ILs‐functionalized organic porous materials, ILs‐functionalized inorganic porous materials, and ILs‐functionalized organic‐inorganic hybrid porous materials in the conversion of CO2. The synergistic effects of combining ILs with porous materials in CO2 conversion are thoroughly discussed. Furthermore, an in‐depth analysis is provided regarding the potential prospects and future applications of utilizing ILs‐functionalized porous materials within the broader realm of catalytic CO2 conversion technologies. [ABSTRACT FROM AUTHOR]

Ionogels (IGs) consisting of ionic liquids (ILs) confined in carbon and organic polymer matrices have recently emerged as promising materials for electrochemical systems. This perspective article explores how the structural, dynamic, and thermodynamic properties of ILs are modified by their confinement. It emphasizes the importance of combining various ILs and matrices to enhance IG properties through IL‐matrix interactions. Specifically, it highlights the significant downshift of IL melting point observed in certain porous carbons, as well as the enhanced ionic conductivity at sub‐ambient temperature in polymer networks. Accordingly, the suitability of these IGs for use in electrochemical systems operating at low temperature is discussed. Although significant progress has been made in the development and applications of carbon and polymer IGs, it is necessary to further explore the texture/structure of real host matrices, which may differ from model ones. Investigating the low‐temperature mobility of ions in IG‐based electrodes with micro/mesoporous carbons is an example of unexplored research area that may open new opportunities for increasing the energy and power density in energy storage applications. The suggested directions should facilitate innovative solutions to current and future challenges for electrochemical systems across a wide temperature range from −40 to 200 °C. [ABSTRACT FROM AUTHOR]

The ILs ([Li (synthetic esters)] NTF2) were prepared by the in situ synthesis method. The tribological behaviour of the ILs to friction pairs of Ti‐6Al‐4V titanium alloy against silicon nitride was studied by SRV‐V under different concentrations and friction frequencies; the wear scar was studied by SEM, XPS and TOF‐SIMS. The results showed that the friction coefficient and wear loss decreased gradually with the increase of the LiNTF2 content; when the LiNTF2 content reached a certain value (10%), the friction coefficient and wear loss did not change much. Tribofilm composed of titanium oxide, Al2O3, TiFO2, AlOF2, Ti2O4F and Al2O3F plays a major role in lubrication and anti‐friction effect. [ABSTRACT FROM AUTHOR]

Shale hydration and expansion during drilling can lead to wellbore instability, sticking, and frequent leakage accidents. To prevent these issues, an ionic liquid (IL) inhibitor solution was synthesized using DL‐alanine and 98% concentrated sulphuric acid as raw materials. The optimum composition and effect of the synthesized inhibitor in oilfield water‐based drilling fluids were evaluated through anti‐expansion, linear expansion rate, water washing resistance, and clay hydration dispersion experiments. The inhibition mechanism was investigated by thermogravimetric analysis, infrared spectroscopy, zeta potential, contact angle, and X‐ray diffraction analysis. The results show that the optimum IL consists of a 1:1 molar ratio of DL‐alanine to concentrated sulphuric acid synthesized under a reaction temperature and time of 70°C and 18 h, respectively. The resulting DL‐alanine IL exhibited the best inhibitory effect on the hydration, dispersion, and expansion of clay at a concentration of 0.5% in aqueous solution, and its linear expansion rate was only 18.49%. After adding a quantitative amount of clay to different concentrations of DL‐alanine IL aqueous solution, the expansion volume of the clay decreased and the water washing resistance significantly improved. These results provide a theoretical basis for improving the safety and efficiency of shale horizontal well drilling operations. [ABSTRACT FROM AUTHOR]

Ionic liquids (ILs) are promising solvents for separating aromatics from fuel oils. However, studies for separate polycyclic aromatics with ILs are rare and insufficient, and the impact of solute structure on extraction performance still needs to be determined. In this work, we use 1‐ethyl‐3‐methylimidazolium bis([trifluoromethyl]sulfonyl)imide ([EMIM][NTF2]) as an extractant to separate 1‐methylnaphthalene, quinoline, and benzothiophene from dodecane mixtures. Liquid–liquid equilibrium experiments identified the optimal operating conditions. Nine solute molecules, including five alkanes and four aromatic hydrocarbons, were used to study the relationship between extraction performance and solute structure. Molecular dynamics simulation and quantum chemistry calculations gave a deep insight and reasonable interpretation of the structure‐performance relationship at the molecular level. An industrial‐scale extraction process was proposed. The IL can be easily regenerated using heptane as a back‐extractive solvent. A high‐purity fuel oil with aromatic content below 0.5 wt% is obtained after 8‐stage extraction. [ABSTRACT FROM AUTHOR]

Ionic liquids' (ILs) surface tension, vital in liquid interface research, faces challenges in measurement methods—time‐consuming and labor‐intensive. The Structure‐Surface Tension Relationship (SSTR) is crucial for understanding the surface tension laws of ionic liquids, helping to predict surface tension and design ionic liquids that meet target requirements. In this study, SMILES string and group contribution methods were used to generate descriptors, and the random forest and multi‐layer perceptron (MLP) models were cross combined with the two descriptor generation methods to establish the SSTR model, providing a comprehensive framework for predicting the surface tension of ionic liquids. String‐MLP excels with high accuracy (R2 = 0.995, RMSE = 0.686, AARD% = 0.71%) for diverse ILs' surface tension values. Meanwhile, the Shapley Additive exPlanning (SHAP) method was used to test the impact of different features on model prediction, increasing the transparency and interpretability of the model. [ABSTRACT FROM AUTHOR]

Owing to the adverse influences of irreversible oxidation, the development of MXene‐based materials, especially those with satisfactory performance and longevity for aqueous energy storage, continues to suffer severe challenges. Herein, the strategy of targeted passivation‐supported defect‐lock‐oxygen is conceived, whereby engineered the V2CTx material for controllable partial oxidation with enhanced regioselectivity. When the material works, inside the intrinsic defects, the outward diffusion of oxidation is confined by the Lewis bases around the defects, which allows for the controllable progress of oxidation. The defect‐locked oxygen oxidizes the exposed carbon, thus forming sufficient amorphous carbons for enhancing the capacitive‐type adsorption of K‐ions. Then the oxidized defects enabled the fast kinetics via the cross‐layer transport of K‐ions. Benefiting from the strategy, the electrode assembly V2CTx‐RTIL (V2CTx equipped with room temperature ionic liquid) exhibits high capacity, good rate capability, and ultra‐longevity compared with those of the MXene materials so far reported. This work presents the first strategy of targeted passivation‐supported defect‐lock‐oxygen for high‐rate capability and super long‐cycling aqueous K+ storage and hopefully would provide the inspiration for the future design of novel electrodes. [ABSTRACT FROM AUTHOR]

Levulinic acid is an important chemical intermediate, which has many applications in organic synthesis, industry, agriculture, and medicine. In this word, three kinds of heteropoly acid based ionic liquids ([IMPS]H2PW12O40、[PyPS] H2PW12O40 [TEAPS] H2PW12O40) were used to catalyze the one‐pot conversion of cellulose to levulinic acid. [IMPS]H2PW12O40 has the highest catalytic activity due to its strong Hammett acidity (H0). In addition, the effect of biphasic solvent systems on the conversion of cellulose to levulinic acid was also studied. The results showed that the GVL/H2O system could effectively promote the conversion of cellulose and increase the yield of levulinic acid. The yield of levulinic acid could reach 52.6% and the conversion rate of cellulose was 91.2% at 180 °C for 180 min under the GVL/H2O volume ratio of 1:1 with [IMPS]H2PW12O40 as a catalyst at 1 Mpa N2 and cellulose as raw material. And [IMPS]H2PW12O40 can be recycled up to five times without significant performance loss. This study provides a promising method for efficiently converting cellulose and other biomass resources to levulinic acid extraction. [ABSTRACT FROM AUTHOR]

An N‐heterocyclic carbene palladium (NHC‐palladium)‐catalyzed denitrogenative coupling of aryldiazonium salts with terminal alkynes in ionic liquids has been accomplished. This catalytic strategy provides an effective and green synthetic protocol for the assembly of structurally diverse internal alkynes with excellent functional group compatibility and mild conditions. In the presence of 1 mol % of IMes‐Pd‐Im‐Cl2 as the catalyst, a wide range of terminal alkynes and aryldiazonium salts could be excellently tolerated. Basic ionic liquid plays a crucial role in this catalytic system, which not only acts as the green solvent, but also provides basic environment for the carbon‐carbon bond formation process. Notably, this catalytic system could be recycled up to six times and reused without significant loss of catalytic activity. [ABSTRACT FROM AUTHOR]

ABSTRACT Ionic liquids (ILs) have been recognized for their potential as environmentally friendly solvents when compared to traditional organic solvents. Additionally, their function goes beyond that of solvents, and cocatalysts, as they frequently act as stabilizing agents and ligands for the metal‐active species and intermediates in catalytic systems. This comprehensive review primarily focuses on the application of Pd‐incorporated ILs in catalyzing cross‐coupling Suzuki reactions. The responses play a vital role in creating a wide range of structurally diverse and highly functionalized organic compounds, focusing specifically on nucleopalladation Suzuki coupling reactions. The review provides a detailed summary of the reaction conditions, stereoselectivity and regioselectivity, and the underlying mechanisms. Furthermore, it underscores crucial and characteristic illustrations, displaying the practical implementations of these coupling reactions. The aim of this review is to stimulate further research efforts, with the ultimate goal of expanding our understanding and utilization of ILs in various fields in the future. [ABSTRACT FROM AUTHOR]

Sodium‐containing ionic liquids are very promising candidates as ion‐conducting materials in alternative to electrolytes based on lithium chemistry. Here we investigate a series of seven ionic liquids with formula (EMImCl/(AlCl3)1.5)/(δ‐NaCl)x (0≤x≤0.74). The salt is comprised of a disordered form of NaCl prepared by metalorganic synthesis, which assures faster dissolution in high concentration. The vibrational investigation carried out by FT‐IR spectroscopy in the medium IR region shed light on salt‐IL interactions. The ionic conductivity was investigated by Broadband Electric Spectroscopy. The direct current conductivity (σdc) profiles versus the reciprocal temperature exhibited a Vogel‐Tamman‐Fulcher behavior indicating the assistance of micro‐Brownian motions to ionic migration. The value of σdc at 25 °C for x=0.74 was found to be 1.2×10−2 S cm−1. Reversible deposition of Na and Al‐containing species take place with high Coulombic efficiency (up to 97 %) and a high Na+ cation transport number (up to 0.95). The understanding of ionic speciation was investigated in comparison with aqueous acid‐base systems exploring the benefits and limitations of such analogy. The role of a Grotthuss‐type mechanism facilitating the exchange of chlorides between acidic catenated chloroaluminate species in anionic domains of the ILs is considered. [ABSTRACT FROM AUTHOR]

Herein we demonstrate the formation of new stimuli‐responsive aqueous biphasic systems (ABS), able to respond simultaneously to temperature and pH, or just to one stimulus, therefore allowing the design of more sustainable separation processes. This dual behavior is achieved with ABS formed by mono‐ or dicationic protic ionic liquids as phase‐forming components, being defined by the ionic liquid cation chemical structure or its basicity. While ABS comprising monocationic ionic liquids only respond to the effect of temperature, systems comprising dicationic ionic liquids are simultaneously affected by both temperature and pH variations. Dicationic ionic liquids are here identified as the key to unlock a double response to stimuli, which is due to the presence of two pKa values afforded by the cation. The reported findings contribute to increase the customizability of double stimuli‐responsive ABS based on ionic liquids, whose development was up to date limited to ionic liquids bearing pH‐responsive anions, opening the door towards the development of more sustainable separation processes. [ABSTRACT FROM AUTHOR]

A catalytic system comprising a gold(I) complex with an N‐heterocyclic carbene (NHC) ligand in an ionic liquid as solvent exhibits higher catalytic efficiency compared to state of the art systems in the title reaction, which enables using down to 0.01 mol % gold. A commercial gold(I) catalyst such as IPrAuNTf2 can be employed for this purpose. In the case of less reactive substrates bearing electron‐withdrawing substituents at the phenol moiety, a tailor made NHC‐gold(I) precatalyst exhibits improved reactivity and can be advantageously employed compared to the commercial one. [ABSTRACT FROM AUTHOR]

The H2O2 generation via the green electrochemical process is of high interest. For the H2O2 electrochemical generation, the oxygen reduction reaction (ORR) is important. Unfortunately, the ORR is kinetically sluggish and catalysts are needed. However, noble metal ORR catalysts are pricy and scarcely applicable in applications. Therefore, non‐precious metal catalysts are desired. Heteroatom‐doped carbons show promise as metal‐free ORR catalysts. The ORR catalytic activity will be enhanced by the carbon's sp2 and/or sp3 engineering. For N, S co‐Cdoped and sp2/sp3 modulated carbon, a polymerizable ionic liquid of hydrolyzed vinyl imidazolium was studied. The carbon is studied as a metal‐free catalyst for the ORR via the 2e− process. It is possible to get an onset potential of 0.88 V vs. RHE with approximately 50 % selectivity for the H2O2. The current study offers a simple technique for synthesizing heteroatom‐doped sp2/sp3 designed carbon as catalysts for the electroreduction of O2 to produce H2O2, and a new way of tunning the sp3/sp2 carbon catalytic activity by modulating the ionic liquid. [ABSTRACT FROM AUTHOR]

The adsorption properties of ionic liquids containing pyrrolidinium cations and various inorganic anions as electrolytes on a platinum surface were analyzed using first principle density functional theory. Three different orientations of the alkyl cation chain were observed during the adsorption process. The strength and structural stability varied between non‐fluorinated and fluorinated anions upon adsorption, with oxygen atoms influencing the mechanism of adsorption and driving the structural stability of the anion, while fluorine atoms played a role in determining the orientation of the cation during adsorption. Net atomic charges analysis, electron density difference methods, and electron density accumulation for this complex system were utilized to further investigate these phenomena. The results of this study provide valuable insights into the role of anions in the adsorption behavior of pyrrolidinium‐based ionic liquids on platinum surfaces, shedding light on the factors that influence their adsorption properties and structural stability on a molecular level. The findings of this study contribute to a better understanding of the interplay between anions and platinum surfaces in the adsorption of pyrrolidinium based ionic liquids, which can have implications for various applications such as electrochemistry, catalysis, and energy storage. [ABSTRACT FROM AUTHOR]

Polyethylene oxide (PEO)/lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) is among the most promising candidates for developing solid polymer electrolytes (SPEs) for all‐solid‐state lithium‐metal batteries (ASSLMBs). However, practical applications of the PEO/LiTFSI system face challenges due to its relatively low ionic conductivity and low Li+ transference number. To address these issues, a method is proposed that incorporates multiple components, including zeolitic imidazolate frameworks (ZIF‐67) as fillers and ionic liquid electrolytes (ILEs) as plasticizers, into a PEO/LiTFSI matrix. By optimizing the fabrication process, ultra‐thin membranes of the integrated electrolyte PEO/LiTFSI‐ILE‐ZIF‐67 (PLiZ) with a thickness of 32 µm are developed, achieving high ionic conductivity (1.19 × 10−4 S cm−1 at 25 °C), broad electrochemical stability (5.66 V), and high lithium‐ion mobility (0.8). As a result, the fabricated ASSLMBs exhibited excellent cycle stability at both room temperature and 60 °C, delivering an initial specific discharge capacity of 166.4 mAh g−1 and an impressive capacity retention of 83.7% after 1000 cycles at 3C under 60 °C, corresponding to a low fading rate of 0.0163% per cycle. Additionally, the designed SPEs demonstrated high safety properties, as shown by the successful cutting and folding of a working LiFePO4/PLiZ/Li pouch cell. Therefore, this study presents a comprehensively improved method for developing high‐performance ASSLMBs. [ABSTRACT FROM AUTHOR]

Selective CO2 photoreduction to value‐added multi‐carbon (C2+) feedstocks, such as C2H4, holds great promise in direct solar‐to‐chemical conversion for a carbon‐neutral future. Nevertheless, the performance is largely inhibited by the high energy barrier of C−C coupling process, thereby leading to C2+ products with low selectivity. Here we report that through facile surface immobilization of a 1‐ethyl‐3‐methylimidazolium tetrafluoroborate (EMIM‐BF4) ionic liquid, plasmonic Cu nanowires could enable highly selective CO2 photoreduction to C2H4 product. At an optimal condition, the resultant plasmonic photocatalyst exhibits C2H4 production with selectivity up to 96.7 % under 450 nm monochromatic light irradiation, greatly surpassing its pristine Cu counterpart. Combined in situ spectroscopies and computational calculations unravel that the addition of EMIM‐BF4 ionic liquid modulates the local electronic structure of Cu, resulting in its enhanced adsorption strength of *CO intermediate and significantly reduced energy barrier of C−C coupling process. This work paves new path for Cu surface plasmons in selective artificial photosynthesis to targeted products. [ABSTRACT FROM AUTHOR]

Herein, we present a density functional theory with dispersion correction (DFT‐D) calculations that focus on the intercalation of ionic liquids (ILs) electrolytes into the two‐dimensional (2D) Ti3C2Tx MXenes. These ILs include the cation 1‐ethyl‐3‐methylimidazolium (Emim+), accompanied by three distinct anions: bis(trifluoromethylsulfonyl)imide (TFSA−), (fluorosulfonyl)imide (FSA−) and fluorosulfonyl(trifluoromethanesulfonyl)imide (FTFSA−). By altering the surface termination elements, we explore the intricate geometries of IL intercalation in neutral, negative, and positive pore systems. Accurate estimation of charge transfer is achieved through five population analysis models, such as Hirshfeld, Hirshfeld‐I, DDEC6 (density derived electrostatic and chemical), Bader, and VDD (voronoi deformation density) charges. In this work, we recommend the DDEC6 and Hirshfeld‐I charge models, as they offer moderate values and exhibit reasonable trends. The investigation, aimed at visualizing non‐covalent interactions, elucidates the role of cation‐MXene and anion‐MXene interactions in governing the intercalation phenomenon of ionic liquids within MXenes. The magnitude of this role depends on two factors: the specific arrangement of the cation, and the nature of the anionic species involved in the process. [ABSTRACT FROM AUTHOR]

Recent developments in molecular mechanics modelling of metal catalyst surfaces with interfaces to complex ad‐layers or bulk liquids enable the study of 10 nm scale systems by molecular dynamics simulations of up to microseconds. Therein, electronic polarization as otherwise benchmarked by quantum calculations is mimicked via atom‐centered partial charges that are adjusted dynamically to account for changes in local environment. Apart from thermal fluctuations, this encompasses molecule association and dissociation processes as well as externally applied voltage. Here, we elaborate the concept of employing the charge equilibration method to the molecular dynamics simulation of solid catalysts, namely metal surfaces and substrate‐supported metal nanoparticles. This showcases the association of reactants and their interplay with local charge polarization upon co‐adsorption of ionic liquids or application of external voltage – thus paving the way to understanding complex interfaces in (electro−)catalysis from molecular dynamics simulation. [ABSTRACT FROM AUTHOR]

Significant attention has been devoted to using biomass as a renewable resource to address the energy crisis and mitigate environmental pollution. Biomass, a potential substitute for fossil fuels, contains a substantial amount of lignin, ranging from 10 % to 25 %. Hence, it is crucial to research lignin depolymerization. In this study, the use of electrochemically catalyzed ionic liquids enabled the cracking of lignin at low temperatures. Specifically, by applying a low voltage at 230 °C, the controlled generation of vanillin and guaiacol was achieved. The concentration of vanillin in the depolymerized lignin reached 88.54 % under 3 V conditions. Similarly, it is presumed that the yield of guaiacol at 4 V is 48.24 %. These findings have significant implications for the targeted management of lignin depolymerization byproducts. Ultimately, this project establishes a framework for the high‐value utilization of biomass and provides new perspectives on addressing the energy problem and environmental degradation. [ABSTRACT FROM AUTHOR]

Real‐time monitoring of carbon dioxide (CO2) is imperative for medical diagnosis and effective environmental preservation. Despite the formidable challenge posed by the inherent chemical inertness of CO₂ molecules, a pioneering CO2 sensor based on MOF‐804 cofunctionalized with ionic liquid (IL) and m‐cresol purple (mCP) is successfully developed. By ingeniously integrating hydrogen bonding, electrostatic interactions, and hydrophobic properties within the sensitive layer, the sensor achieves a state‐of‐the‐art sensitivity (Δf = 384 Hz), an exceptionally vast detection range spanning 400–80 000 ppm, and remarkable stability with minimal sensitivity drift even at relative humidity (RH) levels exceeding 80%. Furthermore, the inherent gasochromic property, stemming from the zwitterionic mechanism, paves the way for innovative self‐sustaining CO2 test strips and groundbreaking applications, including CO2 tracking and CO2‐encrypted security labeling technology. Collectively, the realization of this ultra‐sensitive and robust CO2 monitoring approach, coupled with its CO2‐triggered visual and multifunctional capabilities, opens up novel avenues for dynamic CO2 detection, advanced military encryption strategies, and enhanced health management systems. [ABSTRACT FROM AUTHOR]

The electrochemical reduction of CO2 (CO2RR) mainly occurs at the three‐phase interface, and the properties of an interface can directly affect the CO2RR pathway. Cu‐based materials can produce considerable amounts of alcohols and hydrocarbons, but it is hard to precisely regulate the reaction interface and obtain specific target products. Herein, the properties of the Cu surface through a facile strategy of ionic liquid modification are successfully adjusted. According to theoretical calculations and in situ Raman and FTIR spectra characterizations, it is revealed that the introduction of ionic liquids (e.g., [Bmim][PF6]) can control the energy barriers and distribution density of key intermediates on Cu interface, thus totally change the reaction pathway of CO2 electroreduction. Consequently, the dominant products from the Cu catalyst will be dramatically switched between C2H4 with a 71.1% Faraday efficiency (FE) and CH4 with a 67.2% FE. It is rarely seen in previous reports that the CO2RR products can be fundamentally changed through simple interface modifications. This work offers a straightforward approach to tune the interfacial properties and understand the mechanisms in various electrocatalytic reactions. [ABSTRACT FROM AUTHOR]

Low ionic migration and compromised interfacial stability pose challenges for low‐temperature batteries. In this work, we discovered that even with the state‐of‐the‐art localized high‐concentration electrolytes (LHCEs), uncontrolled Na electrodeposition occurs with a huge overpotential of >1.2 V at −20 °C, leading to cell failure within tens of hours. To address this, we introduce a new electrolyte category that incorporates an ionic liquid as a key solvation species. Diverging from traditional LHCEs, the IL‐tailored LHCE facilitates an anion–solvent‐molecules exchange within the solvation sheath between Na+ and organic cations at low temperatures. This behavior reduces solvation cluster size and strengthens Na+–anion coordination, which proves instrumental in enabling fast ionic dynamics in both the bulk liquid and at the interface. Therefore, durable Na electrodeposition and shuttle‐free, 0.5 Ah sodium–sulfur pouch cells are achieved at −20 °C, for the first time, surpassing the limitations of typical LHCEs. This tailoring strategy opens a  new design direction for advanced batteries operating in fast‐charge and wide‐temperature scenarios. [ABSTRACT FROM AUTHOR]

ABSTRACT A practical and straightforward strategy for the synthesis of ferrocene appended furopyranone, furochromenone, and benzofuranone via a metal‐free annulation reaction of imidazolium ylide with enone mediated by saccharin‐based ionic liquid has been reported. The mechanistic studies show an approach through synergistic dual activation of enone and imidazolium ylide via cation and anion of ionic liquid, respectively. This operationally simple protocol offers an easy and rapid access to a library of ferrocene appended furopyranone, furochromenone, and benzofuranone in moderate to good yields through the involvement of a six‐membered transition state. [ABSTRACT FROM AUTHOR]

The increasing awareness of environmental issues and the transition to green analytical chemistry (GAC) have gained popularity among academia and industry in recent years. One of the principles of GAC is the reduction and replacement of toxic solvents with more sustainable and environmentally friendly ones. This review gives an overview of the advances in applying green solvents as an alternative to the traditional organic solvents for peptide and protein purification and analysis by liquid chromatography (LC) and capillary electrophoresis (CE) methods. The feasibility of using greener LC and CE methods is demonstrated through several application examples; however, there is still plenty of room for new developments to fully realize their potential and to address existing challenges. Thanks to the tunable properties of designer solvents, such as ionic liquids and deep eutectic solvents, and almost infinite possible mixtures of components for their production, it is possible that some new designer solvents could potentially surpass the traditional harmful solvents in the future. Therefore, future research should focus mainly on developing new solvent combinations and enhancing analytical instruments to be able to effectively work with green solvents. [ABSTRACT FROM AUTHOR]

Actuator systems are among the most noteworthy aspects of the rapidly expanding field of smart and multifunctional materials, which is having a substantial impact on a number of application areas. Ionic liquids (ILs) are a particularly relevant option for the development of hybrid materials for actuator applications, because of their simple processing and tailored response. This review work focuses on ionic liquid‐based polymer blends for soft actuator applications. The main properties of IL for these applications are highlighted and the state of the art of actuator devices is presented by the type of polymer matrix. Finally, the main conclusions and future trends are presented, in order to properly tailor the characteristics and functional response of IL‐blends for actuator applications. [ABSTRACT FROM AUTHOR]

Ionogels are promising for soft iontronics, with their network structure playing a pivotal role in determining their performance and potential applications. However, simultaneously achieving mechanical toughness, low hysteresis, self‐healing, and fluorescence using existing network structures is challenging. Drawing inspiration from jellyfish, we propose a novel hierarchical crosslinking network structure design for in situ formation of hyperbranched cluster aggregates (HCA) to fabricate polyurea ionogels to overcome these challenges. Leveraging the disparate reactivity of isocyanate groups, we induce the in situ formation of HCA through competing reactions, enhancing toughness and imparting the clustering‐triggered emission of ionogel. This synergy between supramolecular interactions in the network and plasticizing effect in ionic liquid leads to reduced hysteresis of the ionogel. Furthermore, the incorporation of NCO‐terminated prepolymer with dynamic oxime–urethane bonds (NPU) enables self‐healing and enhances stretchability. Our investigations highlight the significant influence of HCA on ionogel performance, showcasing mechanical robustness including high strength (3.5 MPa), exceptional toughness (5.5 MJ m−3), resistance to puncture, and low hysteresis, self‐healing, as well as fluorescence, surpassing conventional dynamic crosslinking approaches. This network design strategy is versatile and can meet the various demands of flexible electronics applications. [ABSTRACT FROM AUTHOR]

Viologens, with their unique redox‐active properties, have garnered increasing attention in the development of electrochromic devices. This review focuses on key strategies in molecular design, synthesis methodologies, and tailored functionalities that have propelled the field forward from 2019 to the present. The convergence of these approaches has led to the construction of viologen‐based electrochromic materials with enhanced performance, stability, and responsiveness. The review not only examines the current state of the field but also explores promising outlooks and opportunities, including tailored applications, environmental sustainability, and integration with emerging technologies. The synergy between molecular engineering and viologen‐based electrochromic materials holds significant promise, shaping the future of dynamic, responsive materials in diverse technological domains. This review serves as a valuable resource for researchers, offering insights into recent breakthroughs and inspiring further advancements in this rapidly evolving field. [ABSTRACT FROM AUTHOR]

Supercapacitors are known for their highpower density and excellent cycling stability, but their practicality is often hindered by limited energy density and a narrow potential window. Herein, the energy density can be enhanced by modifying the electrode material and the potential window can be expanded through the use of ionic liquid (IL) electrolytes. In the present study, Co(OH)2/reduced graphene oxide (rGO) (Co‐G) nanocomposite electrodes was synthesized using a simple hydrothermal method while IL‐based electrolyte was used as an electrolyte for supercapacitor device fabrication. Morphological analysis reveals a porous honeycomb‐like nanostructure with a vertical orientation on the rGO sheet. Electrochemical analysis of the samples is conducted to assess electrode performance, with the Co‐G electrode achieving a capacitance of 2156 F g−1 at 1 A g−1. This electrode exhibits lower electrochemical resistance than pure Co(OH)2. The synthesized material's practicality evaluated in an asymmetric device Co‐G/C//AC/C using ionic gel and aqueous gel‐based electrolytes. IL‐based gel electrolyte device demonstrated superior performance, delivering an energy density of 130 Wh kg−1 and a power density of 3860 W kg−1, maintaining 91% capacitance after 5000 charge–discharge cycles, and outperforming the KOH/PVA gel‐based device, highlighting the advantages of ionic gel electrolytes. [ABSTRACT FROM AUTHOR]

Porous liquids (PLs) with unique porous frameworks and good flow properties can achieve coupling enhancement for CO2 capture and conversion. In this paper, a series of novel PLs were designed and synthesized using UiO‐66 as the framework and novel bi‐cationic ionic liquids (ILs) as an excluded solvent. The prepared PLs showed significant improvement in CO2 uptake capacity over ILs at different pressures and exhibited excellent CO2 catalytic conversion performance, exceeding the sum of the effects of ILs and UiO‐66. Especially at low pressure, the PLs still showed excellent catalytic performance, but the catalytic performance of the corresponding ILs was significantly reduced, which was due to the rapid adsorption and conversion of CO2 by the porous framework of UiO‐66 to improve the CO2 uptake and transfer efficiency within the ILs, thus achieving coupling enhancement. It can provide a new way to realize the efficient conversion of CO2 under milder conditions. [ABSTRACT FROM AUTHOR]

This work aims to synthesize novel amphiphilic ionic liquids (AILs), AH‐PM, and AD‐PM as well as apply them to chemically demulsifying crude oil emulsions. Two AILs containing different long alkyl chains were synthesized and characterized using several techniques. The surface and interfacial indicated AILs’ surface activity and ability to form micelles. For that, the demulsification efficacy (DE) of these AILs was explored using different factors affecting, e.g., AIL dose, settling time (ST), water content, and temperature. The results indicated that the AIL hydrophobicity resulting from the longer alkyl chain could improve AIL DE. Moreover, increased AIL dose, ST, water content, and temperature improved DE. [ABSTRACT FROM AUTHOR]

Choline oxidase from Alcaligenes sp. (ChOx) is used to generate hydrogen peroxide in situ from choline‐based ionic liquids (ILs) to fuel peroxidase‐mediated biocatalysis while mitigating oxidative degradation of the heme‐dependent enzymes. Horseradish peroxidase (HRP) and chloroperoxidase from Caldariomyces fumago (CPO), in combination with the ChOx, are evaluated in enzymatic cascades for the ability of the biocatalytic systems to withstand elevated concentrations of different choline additives in oxidative and halogenative enzymatic assays. The findings are applied in various synthetic scenarios to produce important oxygen‐ and nitrogen‐containing heterocycles, using choline ILs in a dual‐purpose fashion, as a substrate‐solubilizing component in the reaction medium as well as the source for hydrogen peroxide. The ChOx/HRP couple is used to induce intramolecular cyclizations of hydroxamic acids and hydroxycarbamates in a nitroso‐ene‐type pathway with choline dihydrogen phosphate as IL additive. The ChOx/CPO cascade successfully mediates brominative cyclizations of α‐allenic alcohols, while amphiphilic surfactants are employed to turn the aqueous choline propionate IL media into a colloidal suspension. ChOx/CPO partnering is also evaluated in an oxygenative rearrangement of 1‐furylethanol with choline acetate IL. The results show the wide potential of choline oxidase for hydrogen peroxide‐driven biocatalysis with both aqueous and micellar choline ionic liquid solutions. [ABSTRACT FROM AUTHOR]

The increasing need for ionic circuits has driven the demand for patterning methods with excellent wear resistance and ease of preparation. However, the traditional method of the circuits modified on the surface frequently suffers from wear and detachment during use. Herein, an interpenetrating network of poly(ionic liquid) and polyurethane is employed, creating a patternable ionic circuit that can resist the abrasion of sandpaper or taping. Hydrophobic ionic liquids are successfully polymerized inside the polyurethane to achieve a waterproof ionic circuit, simultaneously reducing the impact of environmental humidity. Additionally, this ionic circuit possesses the capability to perceive the multisignals of temperature, pressure, and pressing shapes with the assistance of artificial intelligence. The interpenetrating network provides a simple and practical solution for the fabrication of wear‐resistant and stable patterned ionic circuits. [ABSTRACT FROM AUTHOR]

Compared to aqueous ions, ionic liquids (ILs) consist entirely of cations and anions, and they function in energy conversion and storage owing to unique properties. Classical electric double layer (EDL) theory born a century ago gives essential insights into aqueous interfaces, whereas it fails in ILs due to overlooking ionic geometries and interactions, leaving a theoretical gap in describing IL interfaces. This study captures IL fingerprints by combining nuclear magnetic resonance experiments, quantum chemistry investigations, and first‐principles molecular simulations. Based on these findings, an EDL theory is proposed to reflect hierarchical aggregation structure and anisotropic dynamics for interfacial ILs. It involves four elements including ion geometries, ion–ion interactions, ion–wall interactions, and temperature and interfacial electric field effects. Specifically, polyatomic ions with nonuniform shapes are cornerstones for successive elements. Cation–anion non‐oxygen hydrogen bonds and cation–cation π+–π+ stacking generate bound clusters. Ion–wall adsorption causes hierarchical aggregation patterns, and cation–wall parallel stacking creates anisotropic dynamics at interfaces. Moreover, the thermal‐weakened ionic interactions and electric field‐enhanced interfacial electron transfer alter the aggregation states and dynamic properties of interfacial ILs. This theory is adaptable to various IL–wall combinations, advancing electrolyte design for next‐generation electrochemical energy devices. [ABSTRACT FROM AUTHOR]

Novel fluorinated, pyrrolidinium‐based dicationic ionic liquids (FDILs) as high‐performance electrolytes in energy storage devices have been prepared, displaying unprecedented electrochemical stabilities (up to 7 V); thermal stability (up to 370 °C) and ion transport (up to 1.45 mS cm−1). FDILs were designed with a fluorinated ether linker and paired with TFSI/FSI counterions. To comprehensively assess the impact of the fluorinated spacer on their electrochemical, thermal, and physico‐chemical properties, a comparison with their non‐fluorinated counterparts was conducted. With a specific focus on their application as electrolytes in next‐generation high‐voltage lithium‐ion batteries, the impact of the Li‐salt on the characteristics of dicationic ILs was systematically evaluated. The incorporation of a fluorinated linker demonstrates significantly superior properties compared to their non‐fluorinated counterparts, presenting a promising alternative towards next‐generation high‐voltage energy storage systems. [ABSTRACT FROM AUTHOR]

Transitioning toward a carbon‐negative direction necessitates continued development and enhancement of existing lithium battery technologies. A key impediment for these technologies is the utilization of flammable organic solvent‐based electrolytes, which pose significant safety risks. Furthermore, the recyclability of batteries has not reached the level required for transitioning to a circular economy. Here, poly(ionic liquid)‐based dual network gel electrolytes are reported as safer and sustainable alternative materials. The materials employ both, dynamic (up to 45 mol%) and covalent crosslinking (up to 10 mol%), allowing the fabrication of mechanically stable gels with a high content (up to 65 wt%) of ionic liquid/salt both via thermal and photo polymerization. The dual nature of this network in interplay with other key components is systematically investigated. Mechanical stability (up to 0.7 MPa), combined with enhanced ionic conductivity (surpassing 10−4 S cm−1 at room temperature) is achieved via the synergetic combination of dynamic non‐covalent and covalent crosslinking, resulting in improved electrochemical (up to 5 V) and thermal stability (reaching 300 °C) by the embedded ionic liquid. Moreover the presence of the dynamic crosslinks facilitates reprocessing at 70 °C without comrpomising the electrochemical performance, thus reaching full recyclability and reusability. [ABSTRACT FROM AUTHOR]

Mutual separation of Y(III) and Sr(II) from their waste solution has been an emerging research domain due to their various industrial applications. In this investigation, we emphasize the feasibility of selective separation of Y(III) from Sr(II) present in nitric acid medium using undiluted cyphos nitrate ionic liquid (IL): trihexyl(tetradecyl)phosphonium nitrate ([P66614][NO3]) as the ligating phase. The set experimental parameters were the feed phase acidity, initial nitrate ion concentration, initial feed metal ion concentration, equilibration time and temperature to unveil the efficacy of the proposed system. Efficient extraction of Y(III) selectively in presence of Sr(II) using only a salting agent in aqueous phase without additional extractant in IL phase was highlighted. A remarkable separation factor (SF) obtained for Y(III) over Sr(II) explored the efficacy of the proposed IL system. Y(III) loading in IL phase both in unirradiated and irradiated conditions was compared to evaluate the coordination behavior of irradiated moieties. In addition, a most important advantage of the proposed system is that it employs Milli‐Q water for the back extraction (stripping) of the loaded Y(III) from IL phase and does not demand any complexing agent (water soluble). This undoubtedly corroborates the economic and environmental benefits of the proposed IL system. [ABSTRACT FROM AUTHOR]

The use of homogeneous catalysts dissolved in ionic liquids (ILs) is an established field of research. Thin IL films containing dissolved catalyst complexes can be immobilized on solid porous supports, thereby creating a heterogenized catalyst material. Aiming at the deliberate positioning of such supported ionic liquid phase (SILP) catalyst, we carried out investigations of two very similar Pt‐complexes: depending on the ligand periphery, the first one is homogeneously dissolved in the IL while the second one strongly enriches at the gas/IL interface. To study these different locations within thick IL films of approximately 1 mm thickness, we investigated the hydrogenation of ethene in a continuous pool‐reactor setup. The two complexes dissolved in the IL [C4C1Im][PF6] showed different activity which can be attributed to their different locations. At 313 K and 0.62 MPa total pressure, the surface‐enriched complex was approximately two times more active. However, under these conditions the formation of Pt particles could be observed, with the surface‐enriched complex exhibiting a stronger tendency for particle formation compared to the one homogeneously distributed in the IL, as derived from XPS and light‐scattering measurements. [ABSTRACT FROM AUTHOR]

Pure organic films consisting of polypyrrole, polyaniline and a composite of polypyrrole and polyaniline electrodeposited in the ionic liquid EMIM‐TFSI onto mesoporous carbon electrodes are tested for their hydrogen evolution reaction capabilities. The use of these intrinsically conducting polymers is seen as a way of stepping away from expensive and rare metallic catalysts. Co‐polymerisation of polypyrrole and polyaniline in a 1 : 10 ratio in EMIM‐TFSI was found to be doped with the TFSI− anion and be much more active to the hydrogen evolution reaction when compared to pure polymers. Tafel analysis of the composite gave a value of 144 mV/dec indicating that the Volmer step is the rate limiting step. However, stability tests showed an improvement in the composite's overpoential performance for the hydrogen evolution reaction. [ABSTRACT FROM AUTHOR]

Porous liquids (PLs) represent a new frontier in material design combining the merits of solid porous host and liquid phase in gas separation and catalysis. Herein, the PL construction approach is harnessed to tailor the gating effect of organic cages toward enhanced gas separation. A type‐II fluorinated PL (F‐PL) is developed via liquifying a fluorinated organic cage (F‐cage) by a fluorinated ionic liquid (F‐IL). The F‐cage is featured by a small window size (≈5.1 Å), high surface area, good stability under highly ionic conditions, and abundant fluorine moieties. The F‐IL possesses high steric hindrance (bulky cation) and structure similarity with the F‐cage (fluorinated alkyl chain in the anion). The existing status structure integrity of F‐cage in F‐IL upon F‐PL formation is illustrated via spectroscopy and X‐ray‐based techniques. The existence of rigid voids in F‐PL is illustrated by positron annihilation lifetime spectroscopy (PALS) and the improved gas uptake capacity than F‐IL via pressure‐swing CO2 uptake isotherms (0−40) bar. The comparison of the gas uptake behavior (CO2, N2, CH4, and Xe) of F‐PL and F‐cage, combining the computational simulation, highlights that the PL construction can be leveraged to tune the window size of porous scaffolds, leading to enhanced gas selectivity. [ABSTRACT FROM AUTHOR]