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Ceria-salt composites represent one type of promising electrolyte candidates for low temperature solid oxide fuel cells (LT-SOFCs), in which ceria-carbonate attracts particular attention because of its impressive ionic conductivity and unique hybrid ionic conduction behavior compared with the commonly used single-phase electrolyte materials. It has been demonstrated that the introduction of carbonate in these new ceria-based composite materials initiates multi new functionalities over single-phase oxide, which therefore needs a comprehensive understanding and review focus. In this review, the roles of carbonate in the ceria-carbonate composites and composite electrolyte-based LT-SOFCs are analyzed from the aspects of sintering aid, electrolyte densification reagent, electrolyte/electrode interfacial 'glue' and sources of super oxygen ionic and proton conduction, as well as the oxygen reduction reaction promoter for the first time. This summary remarks the significance of carbonate in the ceria-carbonate composites for low temperature, 300-600 °C, SOFCs and related highly efficient energy conversion applications. Copyright © 2016 John Wiley & Sons, Ltd. [ABSTRACT FROM AUTHOR]

This study presents the synthesis and characterization of a novel glucose electrochemical biosensor based on gold nanoparticles/bovine serum albumin/Fe 3 O 4 (AuNPs/BSA/Fe 3 O 4 ) composite nanoparticles. The prepared magnetic composite nanoparticles consist of a BSA protein shell, providing biocompatible environment for enzyme immobilization. Furthermore, in situ immobilization of gold nanoparticles greatly enhances the performance of electron transfer. Using these composite nanoparticles, the model enzyme, glucose oxidase (GOx) was readily adsorbed to surface so as the GOx/AuNPs/BSA/Fe 3 O 4 electrochemical biosensor was developed. The electrochemical performance of the biosensor was characterized by cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS), and chronoamperometry. Under the optimal preparation conditions, the resultant biosensor has a short response time of 0.8 s, an excellent sensitivity of 115.3 μA mM −1 cm −2 , and a linear dynamic range from 0.25 to 7.0 mM with a low detection limit of 3.54 μM (S/N = 3). The high sensitivity, good reproducibility and stability of the biosensor presented in this study show that the as-prepared AuNPs/BSA/Fe 3 O 4 composite nanoparticles are a promising material for the development and construction of biosensors. [ABSTRACT FROM AUTHOR]

Abstract: A novel amperometric glucose sensor was constructed by immobilizing glucose oxidase (GOx) on poly(methyl methacrylate)–bovine serum albumin (PMMA–BSA) core–shell nanoparticles. The large surface area of these nanoparticles resulted in a high enzyme loading. The BSA protein shell provided biocompatible microenvironment to retain the native structure and bioactivity of the immobilized enzymes. Such biosensors were characterized by both cyclic voltammetry and chronoamperometry. The effects of the working potential, the amount of the immobilized enzymes and the operating pH on the response of the glucose sensor were investigated. Under an optimal preparation condition, the resultant biosensor had a short response time of less than 8s, a sensitivity of 44.1μAmM−1 cm−2, and a wide linear range from 0.2 to 9.1mM with a correlation coefficient of 0.997. More important, such biosensors were thermally stable at room temperature (∼25°C); which means there was nearly no change in their performance even after they were operated in pH 7.4 phosphate buffer solution for 23 days. The biosensor can be used directly to determine glucose in serum sample. The results show that PMMA–BSA nanoparticles provide a promising material for fabricating enzyme based amperometric biosensors. [Copyright &y& Elsevier]

Here, lithium ions inserted crystalline carbon nitrides (LCCN) with different defect concentrations are prepared by elaborately regulating the mass transfer process in thermal polymerization. It is revealed that there is no conventional exciton–polarons‐induced exciton dissociation mechanism in LCCN due to the weak coupling between excitons and phonons. On the contrary, excitons continue to trap/detrap through defect‐induced traps, which weakens the Coulomb force between electron–hole pairs, thereby accelerating exciton dissociation. It is worth emphasizing that this is the first systematic research on the exciton dissociation characteristics and photocatalytic activity of LCCN of poly(heptazine imide) structure. A strategy of assisting exciton dissociation through defect‐induced traps to address the inherently high exciton binding energy and low exciton dissociation efficiency issues in polymer photocatalysts is proposed. [ABSTRACT FROM AUTHOR]

Aqueous zinc‐ion batteries (AZIBs) suffer from rampant Zn dendrites growth, corrosion and sluggish transport kinetics, all of which have a serious impact on their performance and practical applications. Therefore, porous carbon nanofibers (BTO@PCNFs) loaded with BaTiO3 nanoparticles (BTO NPs) are constructed as a multifunctional interlayer for stabilizing the Zn anodes. Owing to the synergistic effect of BTO NPs and 3D porous carbon framework, this interlayer can achieve uniform electric field distribution, accelerate Zn2+ migration, and promote ion flux homogenization, thus leading to uniform Zn deposition. Meanwhile, the BTO@PCNFs interlayer demonstrates excellent anti‐corrosion effect, which can effectively prevent the side reactions. Benefiting from the synergistic effect of interlayers, the BTO@PCNFs multifunctional interlayers achieve a comprehensive optimization of the Zn anodes. The BTO@PCNFs‐Zn electrode exhibits lower nucleation overpotential (33.5 mV) at 0.5 mA cm−2. The Zn//Zn symmetrical cell with BTO@PCNFs interlayer exhibits ultra‐low overpotential (14 mV) and ultra‐long cycle life (5250 h at 0.5 mA cm−2). Even at high current density (30 mA cm−2), the BTO@PCNFs‐Zn electrode can be stably cycled for more than 830 h, achieving an ultra‐high cumulative capacity of 12 450 mAh cm−2. The multifunctional interlayers can provide a reference for the design of high‐performance Zn anodes. [ABSTRACT FROM AUTHOR]

Low‐cost, high‐voltage‐platform, and high‐capacity MnO2 is the most promising cathode candidate for developing high‐energy‐density aqueous zinc‐ion batteries. However, the Buckets effect of runaway phase transition and irreversible dissolution restricts the electrochemical performance of MnO2. To address this issue, this report presents a bottom‐up targeted assembly concept driven by Gibbs free energy for the design of a robust Ni‐MnO2‐xFx host via Ni2+ pre‐intercalation coupled with fluorine doping. The Gibbs free energy of the host is regulated by the coordination of interlayer reinforcement and interfacial defect repair, which prevents the “layer‐to‐spinel” transition and inhibits dissolution during long‐term cycling. As expected, this cathode provides superior H+/Zn2+ storage performance across a wide temperature range. A capacity of 180.4 mAh g−1 is retained after 1000 cycles at 2 A g−1, a high specific capacity of 293.9 mAh g−1 is retained after 250 cycles at 50 °C and 2 A g−1, and a capacity of 144.5 mAh g−1 is retained after 3000 cycles at 0 °C and 0.5 A g−1. This work provides new insights into the design of stable aqueous battery‐compatible hosts for aqueous zinc‐ion batteries as well as other battery chemistries. [ABSTRACT FROM AUTHOR]

Designing effective electrocatalysts tailored for targeted reactions requires fundamental insights into the structure dependence of the reaction microenvironment. Herein, inspired by finite element simulations, N,O co‐doped carbon nanosheets featuring a hierarchical micro/mesoporous structure to form an oxygen‐rich and local alkaline‐like microenvironment for the two‐electron oxygen reduction reaction (2e− ORR) in a neutral medium are designed. The in situ and ex situ test results confirmed that the micro/mesoporous carbon architecture can elevate the local pH and accelerate the generation of intermediates (*O2, *OOH), leading to high‐efficiency H2O2 production. Utilizing this favorable microenvironment, N,O‐CNS0.5 demonstrated exceptional H2O2 electrosynthesis performance in neutral media, achieving a superior H2O2 yield rate (6705 mmol gcatalyst−1 h−1 in a flow cell). Additionally, comparative experiments and density‐functional theory calculations provided confirmation of the bi‐doping of N and O as the active origin responsible for the electrochemical 2e− ORR. This study synergistically manipulates the reaction microenvironment and active sites, providing an opportunity for efficient H2O2 electro‐production in a neutral medium. [ABSTRACT FROM AUTHOR]

Understanding the dynamics changes of the water network at the electrode–solution interface during the hydrogen evolution reaction (HER) process, including how it is doubly regulated by the electrode material and electrolyte pH, and its subsequent effects on the reaction intermediates (H* and OH*), is crucial in electrochemistry. However, relevant studies are limited due to water's its dual role as both a reactant and a solvent. Thus, it is essential to construct an ideal model capable of decoupling the effects of interfacial water action from the surface catalytic HER process. In this study, M‐O atom pairs doped MoSe2 model catalyst is developed to achieve this goal and tailor the water network structure in a double‐layer microenvironment. Combined with molecular dynamics simulations and in situ spectroscopic characterization, correlations between water configuration, the water network, and water dissociation with HER activity are successfully established. This findings reveal that the pH‐dependent hydrogen‐bonding environment, modulated by oxophilic species, exerts a greater influence on acidic HER compared to alkaline media. The optimized Rh,O‐MoSe2‐x catalyst demonstrates exceptional performance in both acid and alkaline electrolytes and shows no activity decay during a PEMWE test at 1.5 A cm−2, making it promising for scalable water electrolyzers. [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]

Recently, vigorous progress is made in the selective and high‐current reduction of carbon dioxide (CO2) to ethylene (C2H4) by using a flow cell. In most cases, however, the reduction is only achieved in strong alkaline electrolytes, which results in substantial deactivation of electrocatalysts due to the accumulation of precipitates. Here, porous Cu nanowires (NWs) is prepared with abundant atomic defects, which create a synergy with the pore‐induced electric field to comprehensively tune the local microenvironment of the electrode surface, thus enabling efficient and stable C2H4 production from the CO2 reduction reaction (CO2RR) in neutral media. In particular, the enhanced electric field effect increases the local K+ concentration for the generation of *CO intermediates; while the atomic defects stabilize OH− and *CO, leading to high local pH and *CO coverage. Such synergy can provide a favorable local environment and high *CO coverage for significantly decreasing the energy barrier of the C─C coupling step. Consequently, a large partial C2H4 current density of 222.3 mA cm−2 with excellent stability is achieved in a neutral electrolyte. Altogether, this work paves new pathways to promote C2H4 production in the neutral CO2RR through multiple tuning of the local environment. [ABSTRACT FROM AUTHOR]

Photocatalytic and electrocatalytic N2 reduction reactions (N2RR) for NH3 synthesis from abundant N2, H2O, solar energy, and renewable electricity is very attractive. 2D catalysts, including photocatalysts (TiO2, Bismuth‐based materials, layered double hydroxides (LDHs), carbon nitride, Fe@Graphene, MoS2 et al.) and electrocatalysts (metal, graphene, carbon, boron nitride (BN), boron carbide (B4C), black phosphorus (BP), boron, transition‐metal oxide/sulfide/nitride/phosphide), have emerged as promising candidates for N2RR due to their unique physical, chemical and electronic properties. Compared with their bulk counterparts, 2D catalysts usually possess the shortened carrier diffusion pathways, higher specific surface areas and conductivity, more vacancy‐type defects as well as exposed edge sites, which is beneficial to the separation of photogenerated carriers, and the adsorption and activation of N2 molecules. This review highlights the recent progress and developments in 2D catalysts for photocatalytic and electrocatalytic N2RR for the first time. First, the prospects for photocatalytic and electrocatalytic N2RR for NH3 synthesis, and the advantages of 2D catalysts are briefly introduced. Second, the application of 2D catalysts for N2 photoreduction and electroreduction is systematically summarized. Finally, the major challenges and future outlook of this burgeoning area are provided. [ABSTRACT FROM AUTHOR]

Many cases of light absorption modification exceeding 700 nm or near‐infrared (NIR) light are reported for capturing more than half of the solar energy, however, very few modifications can produce NIR photoactivity due to the inevitably introduced defects‐induced non‐radiative recombination. Here, taking four kinds of C/O co‐doped red polymeric carbon nitride as examples, defect‐repairing is carried out using alkali metal molten‐salts (LiCl/NaCl and LiCl/KCl) or solid‐salt (KCl) to activate their NIR photoactivity. The defect repair results from the passivation of alkali metal valence electron pairing and the formation of crystalline polyheptazine imide structure with more complete polymerization. More importantly, it sharply eliminates bulk defects (such as carbon vacancy and nitrogen vacancy) introduced by C/O co‐doping. Since structural defects are inevitably introduced in most photocatalysts during expanding light absorption, this proposed strategy is bound to be universal in suppressing defects‐induced non‐radiative recombination to activate NIR photoactivity. [ABSTRACT FROM AUTHOR]

KAP1 with porous surface structure and reasonable hydrogen bonding are used as fillers in PEO-based CPEs that could solve the compatibility of fillers in polymer-based electrolytes and provide a valuable reference for the design of high-performance ASSLMBs. [Display omitted] Achieving practical applications of PEO-based composite solid electrolyte (CPE) batteries requires the precise design of filler structures at the molecular level to form stable composite interfacial phases, which in turn improve the conductivity of Li+ and inhibit the nucleation growth of lithium dendrites. Some functional fillers suffer from severe agglomeration due to poor compatibility with the polymer base or grain boundary migration, resulting in limited improvement in cell performance. In this paper, ILs@KAP1 is reported as a filler to enhance the performance of PEO-based batteries. Thereinto, the hypercrosslinked phosphorus ligand polymer-containing KAP1, designed at the molecular level, has an abundant porous structure, hydrogen bonding network, and a rigid skeleton structure of benzene rings. These can be used both to improve the flammability with PEO-based and to reduce the crystallinity of the polymer electrolyte. Ionic liquids (ILs) are encapsulated in the nanochannels of KAP1, and thus a 3D Li+ conducting framework could be formed. In this case, it could not only facilitate the wettability of the contact interface with the electrode, significantly promoting its compatibility and providing a fast Li+ transport path, but also facilitate the formation of LiF, Li 3 N and Li 2 O rich SEI components, further fostering the uniform deposition/exfoliation of lithium. The LFP||CPE||Li battery assembled with ILs@KAP1-PEO-CPE has a high initial discharge specific capacity about 156 mAh/g at 1C and a remaining capacity about 121.8 mAh/g after 300 cycles (capacity retention of 78.07%). [ABSTRACT FROM AUTHOR]

Edge engineering has emerged as a powerful strategy to activate inert carbon surfaces, and thus achieve a notable enhanced electrocatalytic activity. However, the rational manipulation of carbon edges to achieve enhanced catalytic performance remains a formidable challenge, primarily hindered by immature synthesis methods and the obscured understanding of the structure‐activity relationship. Herein, an organic–inorganic hybrid co‐assembly strategy is used to fabricate a series of mesoporous carbon nanofibers (MCNFs) with controllable edge site densities and the impact of edge population on electrochemical oxygen reduction reaction (ORR) pathways is investigated. The optimized MCNFs catalyst exhibits a remarkable 2e− ORR performance, as evidenced by a high H2O2 selectivity (>90%) across a wide potential window of 0.6 V and a large cathodic current density of −3.0 mA cm−2 (at 0.2 V vs. reversible hydrogen electrode). Strikingly, the density of carbon edge sites can be changed to tune the ORR activity and selectivity. Experimental validation and density functional theory calculations confirm that the presence of edge defects can optimize the adsorption strength of *OOH intermediates and balance the selectivity and activity of the 2e− ORR process. This study provides a new path to achieve high ORR activity and 2e− selectivity in carbon‐based electrocatalysts. [ABSTRACT FROM AUTHOR]

Heteroatom doping has emerged as a highly effective strategy to enhance the activity of metal‐based electrocatalysts toward the oxygen evolution reaction (OER). It is widely accepted that the doping does not switch the OER mechanism from the adsorbate evolution mechanism (AEM) to the lattice‐oxygen‐mediated mechanism (LOM), and the enhanced activity is attributed to the optimized binding energies toward oxygen intermediates. However, this seems inconsistent with the fact that the overpotential of doped OER electrocatalysts (<300 mV) is considerably smaller than the limit of AEM (>370 mV). To determine the origin of this inconsistency, we select phosphorus (P)‐doped nickel‐iron mixed oxides as the model electrocatalysts and observe that the doping enhances the covalency of the metal‐oxygen bonds to drive the OER pathway transition from the AEM to the LOM, thereby breaking the adsorption linear relation between *OH and *OOH in the AEM. Consequently, the obtained P‐doped oxides display a small overpotential of 237 mV at 10 mA cm−2. Beyond P, the similar pathway transition is also observed on the sulfur doping. These findings offer new insights into the substantially enhanced OER activity originating from heteroatom doping. [ABSTRACT FROM AUTHOR]

Heteroatom doping has emerged as a highly effective strategy to enhance the activity of metal‐based electrocatalysts toward the oxygen evolution reaction (OER). It is widely accepted that the doping does not switch the OER mechanism from the adsorbate evolution mechanism (AEM) to the lattice‐oxygen‐mediated mechanism (LOM), and the enhanced activity is attributed to the optimized binding energies toward oxygen intermediates. However, this seems inconsistent with the fact that the overpotential of doped OER electrocatalysts (<300 mV) is considerably smaller than the limit of AEM (>370 mV). To determine the origin of this inconsistency, we select phosphorus (P)‐doped nickel‐iron mixed oxides as the model electrocatalysts and observe that the doping enhances the covalency of the metal‐oxygen bonds to drive the OER pathway transition from the AEM to the LOM, thereby breaking the adsorption linear relation between *OH and *OOH in the AEM. Consequently, the obtained P‐doped oxides display a small overpotential of 237 mV at 10 mA cm−2. Beyond P, the similar pathway transition is also observed on the sulfur doping. These findings offer new insights into the substantially enhanced OER activity originating from heteroatom doping. [ABSTRACT FROM AUTHOR]

Quick‐charge technology is of great significance for the development of aqueous zinc‐ion batteries. In this study, an unreported in situ electrochemical amorphization mechanism is highlighted to unlock the ultrafast‐kinetics electrode. Multiple characterizations, density functional theory calculation, and molecular dynamic simulation are applied to uncover the storage mechanism of electrodes, as well as the evolution of structure, and reaction kinetics after reconstruction. As revealed, the long‐range ordered ZnV2O4 crystalline can be reconstructed to a short‐range ordered Zn0.44V2O4 electrode, which exhibits significantly improved active sites, shortened diffusion path, and enhanced zinc ions capture ability. Notably, by pairing with the modified Zn anode, it can display ultrahigh rate capability (212 mAh g−1 at 50 A g−1) with a maximum power density of 23.2 kW kg−1, as well as good cycle performance (217.2 mAh g−1 after 3000 cycles at 20 A g−1). Unexpectedly, such reconstructed amorphous electrodes can also retain superior storage capability even at cryogenic conditions. A high specific capacity of 251 mAh g−1 can be delivered at −25°C and 1 A g−1, as well as an 84.3% capacity retention after 500 cycles. This brand‐new in‐situ electrochemical amorphization mechanism is expected to provide new insight into understanding the high‐performance aqueous zinc‐ion batteries. [ABSTRACT FROM AUTHOR]

Rechargeable Zn‐ion batteries (ZIBs), prospective candidates for broad‐scale energy storage, still encounter many challenges such as hydrogen evolution corrosion, Zn dendrite growth, and capacity fading. Therefore, one specific strategy for tuning the internal structure of solid polymer electrolytes (SPEs) via organic additives is proposed to address these urgent bottlenecks simultaneously. With trimethyl phosphate (TMP) addition, the coordination environment of Zn2+ in SPEs is altered and exists as Zn2+(TMP)x(OTf−)y coordinated molecules. Meanwhile, the strong interaction between TMP and Zn enables the preferential growth of Zn(002) planes during electrodeposition, which is proved based on first‐principles calculations, finite element simulations, and multiple in situ characterizations. Such excellent interfacial engineering in situ forms the solid electrolyte interface rich in Zn3(PO4)2 fast ion conductor and guarantees one ultra‐long cycle life for more than 6000 h in a Zn|Zn symmetric cell at 0.1 mA cm−2. Moreover, the universality of TMP‐modified SPEs shows 1000 times stable cycling of VO2(B)|Zn full cells at 1 A g−1 under 0 °C with 95.24% capacity retention, which satisfies potential applications of wide‐ranging energy storage based on solid‐state ZIBs. [ABSTRACT FROM AUTHOR]

Current commercially available dental composite materials have certain limitations for their use, including high monomer viscosity and high polymerization shrinkage, resulting in residual stresses and interfacial gaps. This study focused on the chemical modification of resin monomer bisphenol A-glycidyl methacrylate (bisGMA), so as to reduce the viscosity and polymerization shrinkage. In this design, the hydroxyl groups of bisGMA were transformed into ester groups with various alkyl chain length and branching. The modified monomers showed promising properties including reduced viscosity, reduced polymerization shrinkage, increased hydrophobicity, increased degree of double bond conversion, and improved mechanical properties of the resulting dental resin composites. The structure/property relationships of the new monomers were investigated, and optimal monomer structures were identified for dental composites with improved properties. [ABSTRACT FROM AUTHOR]

The undesirable side reactions and uncontrolled deposition leads to the electrochemical failure of Zn metal anodes. Herein, driven by theory calculations, a surface texture engineering and passivation layer protection dual‐interface strategy is developed. Benefiting from the complementary interface effect, such a dual‐interface can realize the integrated regulation of interfacial transport and deposition. That is, inhibiting water‐induced side reactions, accelerating the de‐solvation of hydrated zinc ions, homogenizing the ion flux, and guiding the Zn(002)‐preferred orientation deposition. As a result, such a dual‐interface modulated Zn electrode enables a significantly extended stability and a smaller nucleation barrier and polarization effect. Unexpectedly, it can steadily operate for 6600 h at 0.5 mA cm−2 and 0.5 mA h cm−2, corresponding to a lifespan >9 months. Highly reversible Zn plating and stripping can be still retained when the current density is improved up to 1, 5, 10, and even 20 mA cm−2. Beyond that, when it is applied to Zn metal batteries, enhanced rate capability, and cyclic stability can be realized in both aqueous Zn/MnO2 batteries and solid‐state Zn/VO2 batteries. This design concept of complementary interface effect is expected to provide a new insight into high reversibility Zn metal anodes. [ABSTRACT FROM AUTHOR]

Synergy engineering is an important way to enhance the kinetic activity of oxygen‐evolution‐reaction (OER) electrocatalysts. Here, we fabricated NiFe amorphous nanoreactor (NiFe‐ANR) oxide as OER electrocatalysts via a mild self‐catalytic reaction. Firstly, the amorphousness helps transform NiFe‐ANR into highly active hydroxyhydroxides, and its many fine‐grain boundaries increase active sites. More importantly, as proved by experiments and finite element analysis, the nanoreactor structure alters the spatial curvature and the mass transfer over the catalyst, thereby enriching OH− in the catalyst surface and inner part. Thus, the catalyst with the structure of amorphous nanoreactors gained excellent activity, far superior to the NiFe catalyst with the structure of crystalline nanoreactor or amorphous non‐nanoreactor. This work provides new insights into the applications and mechanisms of amorphousness and nanoreactors, embodying the "1+1>2" synergy of crystalline state and morphology. [ABSTRACT FROM AUTHOR]

Synergy engineering is an important way to enhance the kinetic activity of oxygen‐evolution‐reaction (OER) electrocatalysts. Here, we fabricated NiFe amorphous nanoreactor (NiFe‐ANR) oxide as OER electrocatalysts via a mild self‐catalytic reaction. Firstly, the amorphousness helps transform NiFe‐ANR into highly active hydroxyhydroxides, and its many fine‐grain boundaries increase active sites. More importantly, as proved by experiments and finite element analysis, the nanoreactor structure alters the spatial curvature and the mass transfer over the catalyst, thereby enriching OH− in the catalyst surface and inner part. Thus, the catalyst with the structure of amorphous nanoreactors gained excellent activity, far superior to the NiFe catalyst with the structure of crystalline nanoreactor or amorphous non‐nanoreactor. This work provides new insights into the applications and mechanisms of amorphousness and nanoreactors, embodying the "1+1>2" synergy of crystalline state and morphology. [ABSTRACT FROM AUTHOR]

Total internal reflection microscopy (TIRM) measures the interactions between a colloidal particle and a flat surface in aqueous solution. Recently, TIRM has further integrated with video microscopy (VM) and enabled the simultaneous measurements of multi-particle colloid-surface interactions in the same ensemble. However, there still remain challenges about accurate image acquisition due to blooming. Blooming means the number of photons reaching the detector exceeds its maximum capacity, and the excess photons will either spill to adjacent pixels or not be counted, leading to an obstacle from precise determination of intensity. Our result shows that blooming gives rise to a deviation of the measured potential energy from the classical theory of Derjaguin, Landau, Verway, and Overbeek (DLVO). Therefore, a correction method was developed in this work to deduce the real intensity from the experimental measurement. The relationship between scattered light intensity and exposure time deviates from linearity when blooming occurs. A correction equation was developed to recover the real intensity, which was then confirmed by the accordance between the corresponding potential energy profiles and the DLVO theory. This correction method is suitable for VM systems of colloidal probes illuminated by scattered light, broadening the application of VM imaging to investigate colloidal interactions. [ABSTRACT FROM AUTHOR]

Highlights: The introduction of PEG 400 additive in the aqueous electrolyte enables regulating the Zn2+ solvation structure and inhibiting the ionization of free water molecules. Such anti-proton electrolyte can not only reduce the lattice expansion of cathode hosts and inhibit the associated by-products, but also guide the uniform Zn deposition and inhibit the hydrogen evolution reaction. A high-rate Zn-V2O3/C battery with 18,000-cycle shelf-life can be demonstrated via the integrated synergetic modification mechanism.Large volumetric expansion of cathode hosts and sluggish transport kinetics in the cathode–electrolyte interface, as well as dendrite growth and hydrogen evolution at Zn anode side are considered as the system problems that cause the electrochemical failure of aqueous Zn-vanadium oxide battery. In this work, a multifunctional anti-proton electrolyte was proposed to synchronously solve all those issues. Theoretical and experimental studies confirm that PEG 400 additive can regulate the Zn2+ solvation structure and inhibit the ionization of free water molecules of the electrolyte. Then, smaller lattice expansion of vanadium oxide hosts and less associated by-product formation can be realized by using such electrolyte. Besides, such electrolyte is also beneficial to guide the uniform Zn deposition and suppress the side reaction of hydrogen evolution. Owing to the integrated synergetic modification, a high-rate and ultrastable aqueous Zn-V2O3/C battery can be constructed, which can remain a specific capacity of 222.8 mAh g−1 after 6000 cycles at 5 A g−1, and 121.8 mAh g−1 even after 18,000 cycles at 20 A g−1, respectively. Such “all-in-one” solution based on the electrolyte design provides a new strategy for developing high-performance aqueous Zn-ion battery. [ABSTRACT FROM AUTHOR]

Sodium (Na) metal has been considered as the most promising anode for achieving next‐generation battery system with high energy density and low cost. Nevertheless, the uncontrolled dendrites growth, infinite volume expansion and unstable solid/electrolyte interphase severely hinder the practical application of Na metal anode. Herein, a functional composite Na anode (Na2Se/Cu@Na) is achieved via infusing molten Na into the porous copper framework modified by cuprous selenide nanosheets. Combining experimental studies and theoretical calculations, the 3D framework and derivatives of Na2Se/Cu can synergistically buffer the volume expansion, redistribute Na+ flux, promote ions migration, and induce uniform Na+ deposition. Benefiting from these merits, the symmetrical cell of Na2Se/Cu@Na demonstrates a stable cycle lifespan over 500 h at 1 mA cm−2 in carbonate electrolyte. And the full battery paired with Na3V2(PO4)3 cathode delivers a stable capacity of 97 mAh g−1 after 800 cycles at 10 C. Furthermore, this structured framework can also be employed to construct composite potassium (K) anode and an outstanding cycle performance is achieved in the symmetrical cell (operating for 1000 h at 0.5 mA cm−2). This study paves a significant way of designing structured Na (K) metal anodes for synergistically improving the electrode stability. [ABSTRACT FROM AUTHOR]

The rational design and development of highly efficient oxygen evolution reaction (OER) electrocatalysts is vital for the application of renewable energy devices. Recently, the strategy of defect engineering draws much attention due to its positive effect on regulating the electronic structure, and thus, promoting the electrocatalytic performance of various materials. In this review, the main focus is on the cation vacancy defects of transition metal‐based electrocatalysts; the latest progress in cation vacancy defect engineering for the electrocatalytic OER is summarized. The different effects of cation vacancy defects on OER are well discussed together with the reaction mechanism, mainly including improving the conductivity, optimizing the adsorption of key intermediates, guiding the surface reconstruction to form active species, and enhancing the long‐term stability. Then, methods to construct cation vacancy defects on different electrocatalysts and the characterization of cation vacancies are systematically introduced. Finally, the remaining challenges and future prospects of cation vacancy defect engineering for promoting OER performance are further proposed. [ABSTRACT FROM AUTHOR]

The electrochemical nitrate reduction reaction (NO3−RR) provides a promising route to produce ammonia (NH3) while addressing environmental issues of NO3−. Although great success has been achieved on the development of efficient NO3−RR electrocatalysts, few has concerned about how to capture NH3 from the electrolyte, despite that the production and capture of NH3 are equally important to the practical application of NO3−RR. Here, inspired by the fact that nearly all in situ generated NH3 is gaseous at the electrode surface during the small‐current NO3−RR, a "two‐in‐one" flow cell electrolyzer is smartly designed that integrates the chambers of NO3−RR electrolysis and NH3 capture through a commercial gas diffusion electrode, aiming at achieving the synchronization of NH3 production and capture. Remarkably, this electrolyzer also enables rapid transport of NH3 products away from the three‐phase reaction interfaces, thereby significantly promoting the conversion of NO3− to NH3. By using robust electrocatalysts with the function like nanoreactors, the electrolyzer delivers a maximum ammonia Faradaic efficiency of 90.2%, along with a large current density (−528.0 mA cm−2) and NH3 capture rate of 90.4%. Clearly, this work provides opportunities to concurrently produce and capture NH3 and thus help the realization of nitrogen cycle. [ABSTRACT FROM AUTHOR]

Sluggish transport kinetics and unstable electrode–electrolyte interface are the main obstacles that greatly impair the electrochemical performance of solid‐state Zn metal batteries. Herein, the concept of multifunctional MXene bonded transport network‐embedded poly(vinylidene fluoride co‐hexafluoropropylene)/Zn(OTf)2 solid polymer electrolyte (PH/MXene SPE) is proposed as "all‐in‐one" strategy for designing robust SPE. In order to uncover the mechanism of such rational designed SPE on regulating the ion transport, as well as the interphase chemistry and Zn deposition, comprehensive research including density functional theory calculation, simulation, and multiple characterization techniques are carried out. As the results indicate, the formation of hydrogen bond network between the MXene nanofiller and PH polymer benefits fast and homogeneous ion transport. Then, the in situ formation of stable organic/inorganic hybrid interphase is capable to ensure the efficient interfacial transport kinetics and uniform Zn deposition. When such PH/MXene SPE is applied, ultrastable Zn plating/stripping behavior with small polarization voltage can be realized. In addi, solid‐state Zn/VO2 batteries with significantly improved rate performance and cyclic stability also can be demonstrated. The unique strategy proposed in this study offer a new insight into SPE design and the development of high‐performance solid‐state Zn metal batteries. [ABSTRACT FROM AUTHOR]

Most near‐infrared (NIR) light‐responsive photocatalysts inevitably suffer from low charge separation due to the elevated Coulomb interaction between electrons and holes. Here, an n‐type doping strategy of alkaline earth metal ions is proposed in crystalline K+ implanted polymeric carbon nitride (KCN) for visible and NIR photoactivity. The n‐type doping significantly increases the electron densities and activates the n→π* electron transitions, producing NIR light absorption. In addition, the more localized valence band (VB) and the regulation of carrier effective mass and band decomposed charge density, as well as the improved conductivity by 1–2 orders of magnitude facilitate the charge transfer and separation. The proposed n‐type doping strategy improves the carrier mobility and conductivity, activates the n→π* electron transitions for NIR light absorption, and breaks the limitation of poor charge separation caused by the elevated Coulomb interaction. [ABSTRACT FROM AUTHOR]

Exploring advanced technologies to efficiently produce green hydrogen energy is imperative to alleviate the energy crisis and environmental pollution. Conventional overall water electrolysis (OWE) has been regarded as a promising approach for effective H2 production, however, it is largely restricted by the sluggish kinetics of the anodic oxygen evolution reaction (OER). Coupling kinetically favorable anodic reactions, such as biomass‐derived compound oxidation and pollutant degradation, with the hydrogen evolution reaction (HER) in hybrid water electrolysis (HWE), can not only solve the biomass recycling and pollutant emission problems but also save the energy cost for clean H2 generation. Hence, various advanced earth‐abundant electrocatalysts have been developed to catalyze those promising anodic reactions, yet some problems such as tedious preparation and unsatisfactory performance still exist. Given the gap between research and practical applications, this review summarizes the recent progress in electrocatalysts for diverse alternative anodic oxidation reactions over the last five years together with their application in HWE systems. An in‐depth understanding of different reaction mechanisms and assessments toward electrocatalysts is discussed to further enhance anodic efficiency. The advantages, differences, and critical issues of different HWE systems are thoroughly discussed as well, providing a new avenue for low‐voltage H2 production from renewable resources and waste products. [ABSTRACT FROM AUTHOR]

Abstracts Silicon (Si) is regarded as one of the most promising anode materials for Li-ion batteries due to its high theoretical specific capacity (4200 mAh g −1 ). To overcome the poor cycling stability issue associated with its low conductivity and large volume changes (∼300%) during charge/discharge processes, a novel approach to fabricate three-dimensional (3D) network structure of silicon-graphene-polyaniline (Si-G-PANI) has been developed. During this synthetic, the graphene sheet was first coated on the surface of Si from a pyrolysis reaction of the liquid-polyacrylonitrile (LPAN), which not only improves conductivity but also constrains the serious mechanical stress caused by the volume expansion of Si. Subsequently, Si-G-PANI composite was obtained through an in-situ polymerization, the PANI layer is tightly bounded to graphene owing to an enhancement of π conjugation between the PANI and graphene-grafted Si nanoparticles. Herein, PANI layer offers a 3D conductive and protective network to allow the volume variation of Si during cycling, as well as facilitate the electron and lithium ion transfer processes. With the dual protection of graphene and PANI, the Si-G-PANI electrode can deliver a reversible specific capacity of 1001.8 mAh·g −1 at a current density of 1.5 A g −1 after 50 cycles. [ABSTRACT FROM AUTHOR]

Sluggish transport kinetics and rapid dendrite growth are considered the main obstacles that impair the performance of Zn metal batteries. This work has developed a unique strategy of dual‐interface engineering (DIE) to design the separator as efficient ions transport modulator. The dual function of spontaneous polarization effect and high zincophilicity of BaTiO3 (BTO) is revealed by combining the theoretical and experimental studies. Benefiting from the decoration of BTO on glass fiber and well filling of the surface interspace, the DIE‐modified separator can not only effectively capture and accelerate Zn2+ transport between the fiber–electrolyte interface, but also redistribute the ions transport into homogenization in the separator–anode interface. Therefore, the modified Zn anodes perform highly reversible Zn plating/stripping with ultrahigh cumulative capacity even up to 9500 mAh cm−2 at the high current density of 10 mA cm−2. Meanwhile, the modified Zn‐MnO2 battery can retain a specific capacity of 108 mAh g−1 after 1800 cycles at 1 A g−1. Furthermore, the capacity retention of the battery also can be improved from 37.5% up to 115% at 0.2 A g−1 after 100 cycles. Such a novel concept for separator engineering provides a new perspective to enable ultra‐stable Zn metal anodes and high‐performance Zn metal batteries. [ABSTRACT FROM AUTHOR]

[Display omitted] Magnesium rechargeable batteries are promising candidates for large-scale energy storage due to their -high safety, low material cost, and earthabundant materials. Many redox-active polymers have recently been reported to show excellent cycling stability with decent Mg-storage performance. However, compared to their Li counterparts, these polymers exhibit lower Mg-storage capacity, resulting in a low ratio of materials utilization (η Mg/ η Li) for the same polymer in two electrolyte systems (i.e., Mg vs. Li electrolytes). Herein, we present a sulfur-linked porous polymer, poly(hexaazatrinaphthalene sulfide) (PSHATN), which sets a record for material utilization of 98% among all polymer electrodes and delivers a reversible capacity of 196 mAh g−1 in Mg electrolytes. Based on electrochemical impedance spectroscopy and operando optical microscopy, we discover a strong correlation between specific capacity and degree of electrochemical swelling of polymers in both electrolytes. Importantly, the high ratio (η Mg/ η Li) of PSHATN is ascribed to sufficient electrochemical swelling due to its large pore volume and flexible polymer nature, in contrast to linear polymers and rigid covalent organic frameworks that swell less effectively. This work highlights the critical need for polymer swelling in promoting ion transport in redox polymers for high material utilization and offers important polymer structural design insights for multivalent ion-based energy storage. [ABSTRACT FROM AUTHOR]

The electronic band structure of MoS2 exerts far‐ranging effects on the applications of these materials, ranging from chemical catalysis, electronic, and magnetic behaviors. However, the underlying relationship between the electronic band structure and activity is largely unknown in heterogeneous catalysis including the hydrogen evolution reaction, partly due to the lack of a controllable methodology to achieve desirable electronic band structures in the 2H‐phase MoS2. Herein it is demonstrated that dual dopants can engineer the band structure of MoS2 by substituting into the adjacent Mo sites. Specifically, these constructed PdRe dimers bridged by sulfur (PdSRe sites) introduce conducting electronic states around the Fermi level to increase the metallic characteristics of MoS2, resulting in metallic‐like behavior, which is initially semiconducting. Furthermore, the efficacy of inducing a phase conversion from 2H to metallic 1T is higher for codoping with dual dopants as compared to that for the use of a single dopant, thereby generating more intrinsically active PdS*Mo sites to further increase active sites density. Ultimately, this leads to the MoS2 catalyst showing a low overpotential of 46 mV at a current density of 10 mA cm−2 and a high exchange current density of 1.524 mA cm−2, along with superior operating durability. [ABSTRACT FROM AUTHOR]

Deeply understanding of the chemical adsorption and polysulfide conversion reaction roles of Zinc protoporphyrin framework-embedded triple-layer nanofiber separator in Li-S batteries. [Display omitted] The practical application of Lithium-sulfur (Li-S) batteries is significantly inhibited by (i) the notable 'shuttle effect' of lithium polysulfides (LiPS), (ii) the corrosion of the lithium interface, and (iii) the sluggish redox reaction kinetics. The functional separator in the Li-S battery has the potential to provide the perfect solution to these problems. Herein a triple-layer multifunctional PVDF-based nanofiber separator, which contains GoTiN/PVDF layer on the top and bottom and ZnTPP/PVDF layer on the middle, is designed. The polarity and porous structure of this multifunctional separator can greatly improve the wettability of electrolytes and enhance the transportation of Li+. With the zinc-based porphyrin framework (ZnTPP) structure, this separator has a strong chemisorption and LiPS conversion ability, which greatly prevent the 'shuttle effect'. Consequently, the designed multilayer separator showed excellent electrochemical performance. As a result, the cell with GoTiN@ZnTPP@GoTiN nanofiber membrane displayed an initial discharge capacity of 1180 mAh/g with a benign capacity retention of 65.9% at 0.5C and high coulombic efficiency of more than 98.5% after 100 cycles. Even at 2C, it can still release a capacity of 798 mAh/g. Moreover, the remarkable capacity of 591 mAh/g could be achieved with a high sulfur load of 5.76 mg/cm2 under a current density of 0.1C. Based on these merits, this novel and scalable multifunctional separator is a promising candidate to replace the conventional PP separator for advanced Li-S batteries to deal with various challenges. [ABSTRACT FROM AUTHOR]

Dendrite growth and parasitic side reactions are thorny issues that seriously damage the anode–electrolyte interface during Zn plating/stripping process, leading to uncontrollable Zn deposition and restraining application of aqueous Zn‐ion batteries (AZIBs). Here, a unique facile strategy to in situ build indium (In) metal interphase on the Zn anode is first proposed. The combination of experimental and theoretical investigations demonstrate that such metallic interphase prevents the hydrogen evolution reaction (HER) and Zn corrosion, and guides preferential growth along the Zn(002) plane to achieve smooth Zn deposition. As a result, the modified Zn anodes achieve the ultrahigh cumulative capacities of 5600 and 5000 mAh cm−2 at the high current densities of 2 and 5 mA cm−2, respectively, demonstrating an ultrastable plating/stripping behavior. More encouragingly, the rate performance and cyclic stability of the Zn–V2O5 battery with the electrolyte additive can still deliver a specific capacity of 383.6 mAh g−1 after 5000 cycles at the high current density of 5 A g−1. The strategy presented here as well as the in‐depth understanding of modified mechanism can not only provide an effective solution to address the Zn anode concerns, but also deepen the understanding of AZIBs. [ABSTRACT FROM AUTHOR]

Abstract: In recent years, modifying cathode materials' surfaces become a popular pursuit. This paper reveals a novel spinel LiMn2O4 in situ coated with graphene-like membrane prepared using liquid-polyacrylonitrile (LPAN) as the carbon source. The structure and electrochemical performance of graphene-like membrane-coated spinel LiMn2O4 are investigated systematically. The membrane has a typical graphene-like layer carbon structure that can be applied the LiMn2O4 particles' surfaces in situ without affecting their crystal structure. Moreover, the graphene-like membrane helps to increase the particle size. The electrochemical performance reveals that coating the graphene-like membrane in situ significantly improves the discharge capacity and cycling stability of the spinel LiMn2O4. In particular, the spinel LiMn2O4 coated with a calcined 20 wt% LPAN graphene-like membrane in situ reached 131.1 mAh g−1 at room temperature, and up to 96% capacity is retained after 50 cycles at 0.1 C. The cyclic voltammetry and electrochemical impedance spectra analyses indicate that the graphene-like membrane does not influence the insertion or desertion of Li+. The improved electrochemical performance is attributed to the decreased manganese dissolution in the electrolyte and the smaller charge transfer resistance generated by the graphene-like membrane coating. [Copyright &y& Elsevier]

The preparation of Hydrogen peroxide (H 2 O 2) by electrochemical two-electron oxygen reduction reaction (2e- ORR) and water oxidation reaction (2e- WOR) is a highly desirable method that can be green, clean and safe. However, the sluggish reaction kinetics and poor 2e- ORR and WOR selectivity severely limits scale-up applications. To resolve these challenges, research on cost-effective catalysts have been intensively explored, which have made great progress. Herein, we first introduced the fundamental chemistry and catalytic mechanism of ORR and WOR, including the possible reaction pathways, the binding modes of oxygen and water on the catalytic sites, and the energy-barrier diagrams of each stage of the reaction obtained by theoretical calculations. Then, the current progress of catalyst research for electrocatalytic synthesis of H 2 O 2 is discussed. Among them, single-atom catalysts as well as molecular catalysts are the hot spots of current research. Single-atom catalysts can reduce the amount of precious or non-precious metals used, and maintain catalytic activity while reducing costs; meanwhile, molecular catalysts have the advantages of single reaction performance, high selectivity, and clear mechanism, which are easy to design and grasp. Finally, on the basis of previous studies, the remaining challenges and development prospects of the current research on electrocatalytic production of H 2 O 2 are discussed, and suggestions are provided for the development of this field in the future. [Display omitted] • The current progress of catalyst research for electrocatalytic synthesis of H 2 O 2 is discussed. • In this review, we introduced some strategies to improve the performance of H 2 O 2. • The remaining challenges and development prospects of the current research on electrocatalytic production of H 2 O 2 are discussed. [ABSTRACT FROM AUTHOR]

Metal/metal-oxide heterointerfaces receive extensive attention in electrocatalysis on account of the strong synergy between the two components at the interface. However, the key factor governing such interfacial synergy is still unclear, making it extremely challenging to rationally design electrocatalyst with desired heterointerfaces. Here, we select metallic copper/cobalt-oxide (i.e., Cu/Co 3 O 4) heterointerfaces as model catalysts for the nitrate reduction reaction (NO 3 -RR) and tuned work function difference (ΔΦ) between Cu/Co 3 O 4 by introducing oxygen vacancies (O v) on Co 3 O 4. By combing experimental and theoretic results, we observe that the ΔΦ is a key factor that governs the interfacial synergy, which included the transfer of electrons from Cu to Co 3 O 4 and the spillover of hydrogen from Co 3 O 4 to Cu. Consequently, the Cu/Co 3 O 4 interface with an optimized ΔΦ displayed the best NO 3 −RR performance, outperforming most of other reported electrocatalysts. The above findings will create new opportunities for rationally designing heterointerfaces for efficient electrocatalysis by tuning ΔΦ. [Display omitted] • Tuning ΔΦ between Cu/CoO x by introducing different concentration of O v on CoO x. • The ΔΦ between Cu/CoO x plays a crucial role in controlling *H overflow and interfacial charge transfer. • A suitable ΔΦ between the Cu/CoO x is a key factor that improves NO 3 −RR electrocatalytic activity. • Optimized Cu/CoO x shows a maximum NH 3 FE of 95.1% along with a high current density to 400 mA cm−2. [ABSTRACT FROM AUTHOR]

Lithium metal batteries (LMBs) have attracted extensive attention for their ultrahigh energy density. However, the uncontrollable growth of Li-dendrites results in poor cyclability and potential safety risks, thus preventing their practical application. Herein, a flexible and cost-effective aqueous polyethylene oxide (PEO)-based solid-state electrolyte is prepared, which enables uniform and dendrite-free Li deposition by introducing Cs+ with an electrostatic shielding mechanism at high current densities. The self-assembly of PEO and bacterial cellulose by hydrogen bonding reduces the crystallinity of PEO and increases uniformly the distribution of lithium ions. With excellent flexibility and thermal stability, such a 3D polymer solid-state electrolyte exhibits an enhanced electrochemical stability window of 5.8 V versus Li/Li+ potential and a high ionic conductivity of 1.28 × 10−4 S cm−1 at 60 °C. The Li‖BC-PEO-Cs+‖Li symmetric cells operate stably for more than 1000 h. Furthermore, Li‖BC-PEO-Cs+‖LiFePO4 (LFP) cells show remarkable enhancement in capacity (163.4 mA h g−1 at 0.1 C), cycling stability (with a capacity retention of 96% after 500 cycles at 1 C) and high functionality and safety (withstanding folding and cutting) in practical applications. [ABSTRACT FROM AUTHOR]

Abstract: Antifouling coatings based on the cross-linked terpolymer chains made of methyl methacrylate (MMA), the hydrolyzable tributylsilyl methacrylate (TBSM) or triisopropylsilyl methacrylate (TIPSM) and acrylic acid (AA) were developed. By varying the hydrolyzable monomer content and the cross-linking degree, a set of such prepared coatings were evaluated in terms of their degradation rate, swelling degree, contact angle and antifouling properties. After immersed in seawater, such coatings quickly self-generate a thin and swollen hydrogel layer at the water-contacting surface due to the hydrolysis of the hydrolyzable groups on the surface. Further hydrolysis leads to a gradual degradation and self-peeling of this hydrogel layer. Their antifouling properties were evaluated by both the adsorption of fluorescence-labeled bovine serum albumin and the field-testing in a real marine environment. Our results reveal that it is such a layer-by-layer hydrogel formation and self-peeling process that leads to an excellent antifouling property. Therefore, it is vitally important to delicately balance the hydrogel formation and the self-peeling rate to achieve the best antifouling of such a coating by carefully choosing a proper cross-linking degree and a suitable content and type of the hydrolyzable comonomer. [Copyright &y& Elsevier]

Abstract: We prepared a coating by mixing a polyfunctional axiridine cross-linking agent and a self-polishing resin pre-synthesized via the polymerization of methyl methacrylate (MMA), acrylic acid (AA) and tributylsilyl methacrylate (TBSM). The coating can be easily applied on a surface to form a cross-linked polymer film by conventional brushing or spraying method. After immersing it into seawater, the film self-generates a thin soft and dynamic layer of hydrogel at the water-contacting surface because of the hydrolysis of TBSM. Such a hydrogel-formation process continues after gradual corrosion and detachment of each top hydrophilic layer. This hydrogel-formation and self-peeling property makes it ideal in various antifouling applications. In the current study, besides the synthesis and preparation of this novel kind of coatings, we focused on the correlation between the TBSM content and the antifouling property by using contact angle, water-absorption, and antifouling measurements. The results of immersing different coatings in shallow submergence for two months reveal that the addition of more TBSM leads to a more hydrophilic surface and a better antifouling property. [Copyright &y& Elsevier]

The microrheology of thermoresponsive poly(N -isopropylacrylamide) (PNIPAM) microgel dispersions near a substrate surface is investigated using active microrheometry by incorporation of multipole magnetic tweezers with a total internal reflection microscope (TIRM). The microrheological behaviors and structural inhomogeneity of such a soft colloidal system in a near-wall case are analyzed by scaling theories with respect to the effective volume fraction of PNIPAM microgels (ϕ eff). [Display omitted] • Near-surface microrheology of PNIPAM microgel dispersions has been revealed. • G′ and G" exhibit distinct dependences on ω , T , and ϕ eff relative to bulk. • Regimes of ϕ eff with distinct scaling laws are observed in phase transitions. • Softness fluctuation can reveal the structural heterogeneity of microgel dispersions. Relative to the bulk systems, the near-wall (<500 nm) rheological responses of soft poly(N -isopropylacrylamide) (PNIPAM) microgel dispersions may exhibit distinct dependence on the frequency (ω), temperature (T), and effective volume fraction (ϕ eff) during the volume phase transitions. The microrheological behaviors are expected to be governed by the near-wall microstructure and its spatial heterogeneity. The combination of active microrheometry (multipole magnetic tweezers) and total internal reflection microscopy (TIRM) was employed to probe the structure–rheology relationships of microgel dispersions near a substrate surface. The ω , T , and ϕ eff -dependences of the storage modulus (G′), loss modulus (G"), and softness (J) were analyzed by power-law and Arrhenius-like scaling theories. The fluctuation of J was further analyzed to give a quantitative description of the inhomogeneity in the near-wall regions. (1) Remarkable differences in the rheological behaviors between the bulk and near-wall cases are revealed, where the latter shows a segmented overlap behavior in ϕ eff ; (2) Five regimes of ϕ eff that correspond to distinct physical states of the microgel dispersions are determined; (3) The near-wall local structures exhibit more heterogeneity in the glass and colloidal gel regimes as compared to the liquid regime. [ABSTRACT FROM AUTHOR]

All‐solid‐state (ASS) lithium metal batteries (LMBs) are considered the most promising next‐generation batteries due to their superior safety and high projected energy density. To access the practically desired high energy density of ASS LMBs, an ultrathin solid‐state electrolyte (SSE) film with fast ion‐transport capability presents as an irreplaceable component to reduce the proportion of inactive materials in ASS batteries. In this contribution, an ultrathin (60 µm), flexible, and free‐standing argyrodite (Li6PS5Cl) SSE film is designed through a self‐limited strategy. A chemically compatible cellulose membrane is employed as the self‐limiting skeleton that not only defined the thinness of the sulfide SSE film but also strengthened its mechanical properties. The ionic conductivity of the SSE film reaches up to 6.3 × 10−3 S cm−1 at room temperature, enabling rapid lithium‐ion transportation. The self‐limited SSE thin films are evaluated in various ASS LMBs with different types of cathode (sulfur and lithium titanate) and anode materials (lithium and lithium‐indium alloy) at both mold‐cell and pouch‐cell levels, demonstrating a stable performance and high‐rate capability. This study provides a general strategy for the rational design of an SSE thin film towards high‐energy‐density ASS batteries. [ABSTRACT FROM AUTHOR]

• Constructing a series of O-doped K+ implanted CCN with narrowed bandgap (2.71-1.62 eV) for the first time. • Adopting oxygen doping strategy to activate the n→π* transition to enhance visible light and even near-infrared light harvesting. • An approximately 45- and 10- times enhancement than pristine CN and CCN for H2 generation at λ > 500 nm. • Excellent photoactive up to 650 nm owns prominent advantages over most CCN. Crystalline carbon nitride (CCN) materials with photoresponse of more than 600 nm are rare. Here, we successfully prepared a series of oxygen doped K+ implanted CCN (KCN) with narrowed bandgap (2.71−1.62 eV) for the first time. Compared with most of the O-doped amorphous CN, the optical absorption can only reach 500 nm, and a few more than 500 nm, our oxygen doping strategy is adopted to activate more n→π* transitions to enhance visible light and even near-infrared light harvesting. This active-optimized O-doped KCN accounts for 45- and 10- times promotion than pristine CN and KCN in H 2 generation under λ > 500 nm. Most importantly, its maximum active wavelength is up to 650 nm, which has obvious advantages than most CCN-based photocatalysts in the utilization of solar energy. This excellent solar capture and H 2 production is attributed to the activated n→π* electron transition, and high crystallinity and conduction band (CB) position caused by oxygen doping. [ABSTRACT FROM AUTHOR]

Keywords: 2D catalysts; electrocatalysis; N2 reduction reaction; NH3; photocatalysis EN 2D catalysts electrocatalysis N2 reduction reaction NH3 photocatalysis 1 1 1 03/22/21 20210318 NES 210318 The Cowherd and Weaving Maid is a famous folk love story in ancient China. 2D Electrocatalysts: Recent Progress in 2D Catalysts for Photocatalytic and Electrocatalytic Artificial Nitrogen Reduction to Ammonia (Adv. 2D catalysts, electrocatalysis, N2 reduction reaction, NH3, photocatalysis. [Extracted from the article]

Electrochemical reduction reaction is an important approach to utilize CO 2 and convert it into valuable products. Exceptional reaction kinetics at a high temperature of solid oxide electrolysis cells (SOECs) attracts particular attention. In this work, we propose to investigate CO 2 -RR kinetics using a new theoretical method based on the electrical conductivity relaxation (ECR) technique on a typical mixed-conducting Sr 2 Fe 1.5 Mo 0.5 O 6-δ (SFM) electrode. Three kinetic parameters that are commonly adopted in the typical electrochemical test experiments consisting of overpotential, current density and area-specific resistance (ASR) are derived. The overpotential resulted from the difference in the oxygen partial pressure is caused by the change of CO 2 partial pressure, while current density from the surface reaction rate constant. Accordingly, area-specific resistance, as well as overpotential-current density relationship, can be derived. We believe that this work brings a new method to study the kinetic process of CO 2 electrolysis and to evaluate the electrocatalyst activity of developed new electrode materials as well as to benefit the designing of novel electrode electrocatalysts for highly efficient solid oxide electrolysis cells. • A new theoretical method of investigating CO 2 reduction kinetics is proposed. • The electrical conductivity relaxation technique is applied to CO 2 -SOEC cathode. • The formulations of η , i and ASR are derived by k chem. [ABSTRACT FROM AUTHOR]

Titanium dioxide (TiO2) is a promising anode material for sodium‐ion batteries (SIBs) due to its low cost, natural abundance, nontoxicity, and excellent electrochemical stability. Oxygen vacancies, the most common point defects in TiO2, can dramatically influence the physical and chemical properties of TiO2, including band structure, crystal structure and adsorption properties. Recent studies have demonstrated that oxygen‐deficient TiO2 can significantly enhance sodium storage performance. Considering the importance of oxygen vacancies in modifying the properties of TiO2, the structural properties, common synthesis strategies, characterization techniques, as well as the contribution of oxygen‐deficient TiO2 on initial Coulombic efficiency, cyclic stability, rate performance for sodium storage are comprehensively described in this review. Finally, some perspectives on the challenge and future opportunities for the development of oxygen‐deficient TiO2 are proposed. [ABSTRACT FROM AUTHOR]

The role of exciton dissociation in charge separation dominated by in-plane crystallinity has been rarely addressed, although it is the decisive step of polymeric carbon nitride (CN) photocatalysis. Here, taking ten kinds of crystalline carbon nitride (CCN) as examples, the relationship between exciton dissociation, carrier mobility, conductivity, charge separation and photocatalytic activity under different in-plane crystallinity has been investigated. Although the in-plane crystallinity dominates charge separation and photocatalytic activity, it does not significantly reduce excitons binding energy (EBE) or improve exciton dissociation efficiency (EDE), only decreasing by 1.5 meV and increasing by 2.3 %, respectively. It is the greatly improved carrier mobility and conductivity that are more responsible for the increased charge separation and photocatalytic activity than the slight change in EDE. To our knowledge, this is the first reported case of overall water splitting in CCN of poly(heptazine imide) structure, resulting from the optimized in-plane crystallinity. [Display omitted] • Demonstrating the role of exciton dissociation in charge separation dominated by in-plane crystallinity. • Providing modification strategies for layered photoelectric conversion materials. • The first reported case of overall water splitting in CCN of poly(heptazine imide) structure. [ABSTRACT FROM AUTHOR]

• The Fe-doped cathode exhibited superior catalytic activity for CO 2 reduction compared to pristine La 0.5 Sr 0.5 MnO 3. • The incorporation of Fe into the unit cell increased its size and facilitated the CO 2 reduction activity. • Fe substitution improves CO 2 adsorption and decreased the energy barrier of the rate-determining step. • The Fe-doped cathode resulted in an increased maximum power density in the Zn-CO 2 battery. Aqueous Zn-CO 2 batteries are a new technology for reducing carbon dioxide emissions and converting CO 2 into valuable products. The development of high-performance catalysts is crucial for improving the efficiency of the CO 2 reduction reaction(CO 2 RR) in these batteries. The technical challenges of CO 2 RR catalysts include high cost, complicated synthesis and low Faraday efficiency. In this study, we developed an efficient and cost-effective CO 2 RR perovskite catalyst, by partially substituting Fe to the B site of precious metal-free La 0.5 Sr 0.5 MnO 3 (LSM) perovskite. Comprehensive investigation into the Structure, morphology, coordination information and electrochemical performance of pristine La 0.5 Sr 0.5 MnO 3 (LSM) and substituted La 0.5 Sr 0.5 Fe 0.6 MnO 3 (LSF 0.6 M) catalysts were conducted, LSF 0.6 M catalyst shows enhanced electrochemical performance, Faraday efficiency, battery durability and battery power density than LSM. Specifically, the Fe-doped catalyst shows a significant improvement in CO 2 reduction reaction (CO 2 RR) performance, with an 80% increase in current density, an 82% Faraday efficiency, and a 50% increase in power density of Zn-CO 2 battery. Characterization experimental results and DFT calculation reveal that Fe substitution can increase the perovskite lattice size to favor CO 2 absorption and *COOH formation, thus the improved CO yields. These analyses provided insights into the underlying mechanisms of the catalyst's performance in CO 2 RR within the battery system. These results highlight LSF 0.6 M perovskite as a very promising CO 2 RR electrocatalyst for Zn-CO 2 battery. [ABSTRACT FROM AUTHOR]