The commercialization of Zn batteries is confronted with urgent challenges in the metal anode, such as dendrite formation, capacity loss, and cracking or dissolution. Here, surface interfacial engineering of the Zn anode is introduced for achieving safety and dendritic-free cycling for high-performance aqueous Zn batteries through a simple but highly effective chemical etching-substitution method. The chemical modification induces a rough peak-valley surface with a thin fluorine-rich interfacial layer on the Zn anode surface, which regulates the growth orientation via guiding uniform Zn plating/stripping, significantly enhances accessibility to aqueous electrolytes and improves wettability by reducing surface energy. As a result, such a synergetic surface effect enables uniform Zn plating/stripping with low polarization of 29 mV at a current density of 0.5 mA cm^-2 with stable cyclic performance up to 1000 h. Further, a full cell composed of a fluorine-substituted Zn anode coupled with a β-MnO₂ or Ba-V₆O₁₃ cathode demonstrates improved capacity retention to 1000 cycles compared to the pristine-Zn cells. The proposed valley deposition model provides the practical direction of surface-modified interfacial chemistries for improving the electrochemical properties of multivalent metal anodes via surface tuning.

Interfacial imperfections between the perovskite layer and the electron transport layer (ETL) in perovskite solar cells (PSCs) can lead to performance loss and negatively influence long-term operational stability. Here, we introduce an interface engineering method to modify the interface between perovskite and ETL by using multifunctional carbon dots (CDs). C = O in the CDs can chelate with the uncoordinated Pb²⁺ in the perovskite material, inhibit interfacial recombination, and enhance the performance and stability of device. In addition, -OH in CDs forms hydrogen bonds with I^- and organic cation in perovskite, inhibiting light-induced I₂ release and organic cation volatilization, causing irreversible degradation of perovskite films, thereby enhancing the long-term operational stability of PSCs. Consequently, we achieve the champion inverted device with an efficiency of 24.02%. The CDs-treated PSCs exhibit high operational stability, and the maximum power point tracking only attenuates by 12.5% after 1000 h. Interfacial modification engineering supported by multifunctional quantum dots can accelerate the road to stable PSCs.

Colloidal synthesis of metal nanoclusters will inevitably lead to the blockage of catalytically active sites by organic ligands. Here, taking [Au₂₅(PET)₁₈]^- (PET = 2-phenylethanethiol) nanocluster as a model catalyst, this work reports a feasible procedure to achieve the controllably partial removal of thiolate ligands from unsupported [Au₂₅(PET)₁₈]^- nanoclusters with the preservation of the core structure. This procedure shortens the processing duration by rapid heating and cooling on the basis of traditional annealing treatment, avoiding the reconfiguration or agglomeration of Au₂₅ nanoclusters, where the degree of dethiolation can be regulated by the control of duration. This work finds that a moderate degree of dethiolation can expose the Au active sites while maintaining the suppression of the competing hydrogen evolution reaction. Consequently, the activity and selectivity towards CO formation in electrochemical CO₂ reduction reaction of Au₂₅ nanoclusters can be promoted. This work provides a new approach for the removal of thiolate ligands from atomically precise gold nanoclusters.

Since low overpotential for the anodic ethanol oxidation reaction (EOR) can favor the higher output voltage and power of direct ethanol fuel cells (DEFCs), it is critical to design new EOR catalysts with efficient ethanol-to-CO₂ activity at low applied potentials. Thereby, carbon-supported Ir-Bi₂O₃ (Ir-Bi₂O₃/C) catalysts with highly dispersive bismuth oxide on the iridium surface are designed and prepared, which can merit splitting the ethanol C-C bond and promoting the oxidation of C1 intermediates at the bifunctional interfaces. The as-obtained Ir-Bi₂O₃/C catalysts show superior EOR mass activity of up to ca. 2250 mA mg^-1_Ir. Moreover, they exhibit the record lowest onset oxidation potentials (0.17-0.22 V vs. RHE) and the peak potential (ca. 0.58 V vs. RHE), being 130-300 mV lower than the previous landmark noble metallic catalysts. Furthermore, an apparent C1 pathway faraday efficiency (FE_C1) of 28% ± 5.9% at 0.5 V vs. RHE can be obtained at Ir-Bi₂O₃/C. This work might provide new insights into the new anodic EOR catalysts for increasing the power of DEFCs.

Macro- and micro-interface instability of SiO_x anode caused by its dramatic volume variation during cycling will result in low Coulombic efficiency and rapid capacity degradation. In this work, an organic-inorganic composite interfacial layer rich in benzene ring groups, polyisocyanates, and LiF was obtained on SiO_x anode by the introduction of 4-fluorophenyl isocyanate (FPI) and fluoroethylene carbonate (FEC) co-additives in electrolyte. The SiO_x anode material shows a capacity retention of 69.2% after 100 cycles at a current density of 1 A g^-1 and rate capacity of 523 mA h g^-1 at the current density of 3 A g^-1, while the SiO_x anode cycling in reference electrolyte has almost no capacity.

The bifunctional oxygen catalyst is essential for zinc-air batteries (ZABs). Here, an efficient bifunctional oxygen catalyst, PPcFeCo/3D-G, is obtained through π-π interaction between the conjugated polymerized iron-cobalt phthalocyanine (PPcFeCo) with excellent thermal stability and three-dimensional graphene (3D-G). The bimetallic synergistic effect of PPcFeCo, verified by DFT (Density functional theory) calculation, and π-π interactions enhances the catalytic activity and durability of the PPcFeCo/3D-G. Regarding electrochemical performance, the PPcFeCo/3D-G with a high electron transfer number (3.98, @0.768 V vs. RHE) has excellent half-wave potential (E_1/2=0.890 V vs. RHE) and exhibits outstanding reversibility (ΔE=0.700 V, ΔE=E_j=10-E_1/2). The liquid ZAB (LZAB) employed PPcFeCo/3D-G displays a high power density (222 mW cm^-2), a specific capacity (792 mA h g^-1), and excellent durability (120 h). This work has guiding significance for the preparation of high-efficiency bifunctional catalysts.

Under the new energy resource structure, electrocatalysts are key materials for the development of proton membrane fuel cells, electrolysis of aquatic hydrogen devices, and carbon dioxide reduction equipment, to address energy shortages and even environmental pollution issues. Although controlling the morphology or doping with heteroatoms for catalyst active centers have accelerated the reaction rate, it is difficult to solve the problems of multiple by-products, and poor stability of catalytic sites. From this, it will be seen that single regulation of metal active centers is difficult to comprehensively solve application problems. Orderly assembly and coordination of catalyst multi-hierarchy structures at the mesoscale above the nanometer level probably be more reasonable strategies, and numerous studies in thermal catalysis have supported this viewpoint. This article reviews the multi-hierarchy design of electrocatalyst active centers, high-energy supports, and peripheral structures in recent years, providing unconventional inspiration about electrocatalyst creation, which perhaps serves as a simple tutorial of electrocatalysis exploration for abecedarian.

Ammonia plays an essential role in human production and life as a raw material for chemical fertilizers. The nitrate electroreduction to ammonia reaction (NO₃RR) has garnered attention due to its advantages over the Haber-Bosch process and electrochemical nitrogen reduction reaction. Therefore, it represents a promising approach to safeguard the ecological environment by enabling the cycling of nitrogen species. This review begins by discussing the theoretical insights of the NO₃RR. It then summarizes recent advances in catalyst design and construction strategies, including alloying, structure engineering, surface engineering, and heterostructure engineering. Finally, the challenges and prospects in this field are presented. This review aims to guide for enhancing the efficiency of electrocatalysts in the NO₃RR, and offers insights for converting NO₃^- to NH₃.

Photocatalysis is critically important for environmental remediation and renewable energy technologies. The ability to objectively characterize photocatalyst properties and photocatalysis processes is paramount for meaningful performance evaluation and fundamental studies to guide the design and development of high-performance photocatalysts and photocatalysis systems. Photocatalysis is essentially an electron transfer process, and photoelectrocatalysis (PEC) principles can be used to directly quantify transferred electrons to determine the intrinsic properties of photocatalysts and photocatalysis processes in isolation, without interference from counter reactions due to physically separated oxidation and reduction half-reactions. In this review, we discuss emphatically the PEC-based principles for characterizing intrinsic properties of photocatalysts and important processes of photocatalysis, with a particular focus on their environmental applications in the degradation of pollutants, disinfection, and detection of chemical oxygen demand (COD). An outlook towards the potential applications of PEC technique is given.

Lithium-sulfur (Li-S) batteries have attracted wide attention for their high theoretical energy density, low cost, and environmental friendliness. However, the shuttle effect of polysulfides and the insulation of active materials severely restrict the development of Li-S batteries. Constructing conductive sulfur scaffolds with catalytic conversion capability for cathodes is an efficient approach to solving above issues. Vanadium-based compounds and their heterostructures have recently emerged as functional sulfur catalysts supported on conductive scaffolds. These compounds interact with polysulfides via different mechanisms to alleviate the shuttle effect and accelerate the redox kinetics, leading to higher Coulombic efficiency and enhanced sulfur utilization. Reports on vanadium-based nanomaterials in Li-S batteries have been steadily increasing over the past several years. In this review, first, we provide an overview of the synthesis of vanadium-based compounds and heterostructures. Then, we discuss the interactions and constitutive relationships between vanadium-based catalysts and polysulfides formed at sulfur cathodes. We summarize the mechanisms that contribute to the enhancement of electrochemical performance for various types of vanadium-based catalysts, thus providing insights for the rational design of sulfur catalysts. Finally, we offer a perspective on the future directions for the research and development of vanadium-based sulfur catalysts.

Although lithium-sulfur batteries (LiSBs) are regarded as one of the most promising candidates for the next-generation energy storage system, the actual industrial application is hindered by the sluggish solid-liquid phase conversion kinetics, severe shuttle effect, and low sulfur loadings. Herein, a zeolitic imidazolate framework (ZIF) derived heterogeneous ZnSe-CoSe nanoparticles encapsulated in hollow N-doped carbon nanocage (ZnSe-CoSe-HNC) was designed by etching with tannic acid as a multifunctional electrocatalyst to boost the polysulfide conversion kinetics in LiSBs. The hollow structure in ZIF ensures large inner voids for sulfur and buffering volume expansions. Abundant exposed ZnSe-CoSe heterogeneous interfaces serve as bifunctional adsorption-catalytic centers to accelerate the conversion kinetics and alleviate the shuttle effect. Together with the highly conductive framework, the ZnSe-CoSe-HNC/S cathode exhibits a high initial reversible capacity of 1305.3 mA h g^-1 at 0.2 C, high-rate capability, and reliable cycling stability under high sulfur loading and lean electrolyte (maintaining at 745 mA h g^-1 after 200 cycles with a high sulfur loading of 6.4 mg cm^-2 and a low electrolyte/sulfur ratio of 6 μL mg^-1). Theoretical calculations have demonstrated the heterostructures of ZnSe-CoSe offer higher binding energy to lithium polysulfides than that of ZnSe or CoSe, facilitating the electron transfer to lithium polysulfides. This work provides a novel heterostructure with superior catalytic ability and hollow conductive architecture, paving the way for the practical application of functional sulfur electrodes.

To promote the development of global carbon neutrality, perovskite solar cells (PSCs) have become a research hotspot in related fields. How to obtain PSCs with expected performance and explore the potential factors affecting device performance are the research priorities in related fields. Although some classical computational methods can facilitate material development, they typically require complex mathematical approximations and manual feature screening processes, which have certain subjectivity and one-sidedness, limiting the performance of the model. In order to alleviate the above challenges, this paper proposes a machine learning (ML) model based on neural networks. The model can assist both PSCs design and analysis of their potential mechanism, demonstrating enhanced and comprehensive auxiliary capabilities. To make the model have higher feasibility and fit the real experimental process more closely, this paper collects the corresponding real experimental data from numerous research papers to develop the model. Compared with other classical ML methods, the proposed model achieved better overall performance. Regarding analysis of underlying mechanism, the relevant laws explored by the model are consistent with the actual experiment results of existing articles. The model exhibits great potential to discover complex laws that are difficult for humans to discover directly. In addition, we also fabricated PSCs to verify the guidance ability of the model in this paper for real experiments. Eventually, the model achieved acceptable results. This work provides new insights into integrating ML methods and PSC design techniques, as well as bridging photovoltaic power generation technology and other fields.

Enhancing the stability of Pt-based electrocatalysts for the sluggish cathodic oxygen reduction reaction (ORR) is critical for proton exchange membrane fuel cells (PEMFCs). Herein, high-entropy intermetallic (HEI) L1₂-Pt(FeCoNiCuZn)₃ is designed for durable ORR catalysis. Benefiting from the unique HEI structure and the enhanced intermetallic phase stability, Pt(FeCoNiCuZn)₃/C nanoparticles demonstrate significantly improved stability over Pt/C and PtCu₃/C catalysts. The Pt(FeCoNiCuZn)₃/C exhibits a negligible decay of the half-wave potential during 30,000 potential cycles from 0.6 to 1.0 V, whereas Pt/C and PtCu₃/C are negatively shifted by 46 and 36 mV, respectively. Even after 10,000 cycles at potential up to 1.5 V, the mass activity of Pt(FeCoNiCuZn)₃/C still shows ∼70% retention. As evidenced by the structural characterizations, the HEI structure of Pt(FeCoNiCuZn)₃/C is well maintained, while PtCu₃/C nanoparticles undergo severe Cu leaching and particle growth. In addition, when assembled Pt(FeCoNiCuZn)₃/C as the cathode in high-temperature PEMFC of 160 °C, the H₂-O₂ fuel cell delivers almost no degradation even after operating for 150 h, demonstrating the potential for fuel cell applications. This work provides a facile design strategy for the development of high-performance ultrastable electrocatalysts.

Scaled-up industrial water electrolysis equipment that can be used with abundant seawater is key for affordable hydrogen production. The search for highly stable, dynamic, and economical electrocatalysts could have a significant impact on hydrogen commercialization. Herein, we prepared energy-efficient, scalable, and engineering electronic structure modulated Mn-Ni bimetal oxides (Mn_0.25Ni_0.75O) through simple hydrothermal followed by calcination method. As-optimized Mn_0.25Ni_0.75O displayed enhanced oxygen and hydrogen evolution reaction (OER and HER) performance with overpotentials of 266 and 115 mV at current densities of 10 mA cm^-2 in alkaline KOH added seawater electrolyte solution. Additionally, Mn-Ni oxide catalytic benefits were attributed to the calculated electronic configurations and Gibbs free energy for OER, and HER values were estimated using first principles calculations. In real-time practical application, we mimicked industrial operating conditions with modified seawater electrolysis using Mn_0.25Ni_0.75O∥Mn_0.25Ni_0.75O under various temperature conditions, which performs superior to the commercial IrO₂∥Pt-C couple. These findings demonstrate an inexpensive and facile technique for feasible large-scale hydrogen production.

Plasma-based CO₂ conversion is promising for carbon capture and utilization. However, inconsistent reporting of the performance metrics makes it difficult to compare plasma processes systematically, complicates elucidating the underlying mechanisms and compromises further development of this technology. Therefore, this critical review summarizes the correct definitions for gas conversion in plasma reactors and highlights common errors and inconsistencies observed throughout literature. This is done for pure CO₂ splitting, dry reforming of methane and CO₂ hydrogenation. We demonstrate that the change in volumetric flow rate is a critical aspect, inherent to these reactions, that is often not correctly taken into account. For dry reforming of methane and CO₂ hydrogenation, we also demonstrate inconsistent reporting of energy efficiency, and through numerical examples, we show the significance of these deviations. Furthermore, we discuss how to measure changes in volumetric flow rate, supported by data from two experimental examples, showing that the sensitivity inherent to a standard component and a flow meter is essential to consider when deriving the performance metrics. Finally, some general recommendations and good practices are provided. This paper aims to be a comprehensive guideline for authors, to encourage more consistent calculations and stimulate the further development of this technology.

B-containing electrolyte additives are widely used to enhance the cycle performance at low temperature and the rate capability of lithium-ion batteries by constructing an efficient cathode electrolyte interphase (CEI) to facilitate the rapid Li⁺ migration. Nevertheless, its wide-temperature application has been limited by the instability of B-derived CEI layer at high temperature. Herein, dual electrolyte additives, consisting of lithium tetraborate (Li₂TB) and 2, 4-difluorobiphenyl (FBP), are proposed to boost the wide-temperature performances of LiNi_0.6Co_0.2Mn_0.2O₂ (NCM) cathode. Theoretical calculation and electrochemical performances analyses indicate that Li₂TB and FBP undergo successive decomposition to form a unique dual-layer CEI. FBP acts as a synergistic filming additive to Li₂TB, enhancing the high-temperature performance of NCM cathode while preserving the excellent low-temperature cycle stability and the superior rate capability conferred by Li₂TB additive. Therefore, the capacity retention of NCM||Li cells using optimal FBP-Li₂TB dual electrolyte additives increases to 100% after 200 cycles at -10 °C, 99% after 200 cycles at 25 °C, and 83% after 100 cycles at 55 °C, respectively, much superior to that of base electrolyte (63%/69%/45%). More surprisingly, galvanostatic charge/discharge experiments at different temperatures reveal that NCM||Li cells using FBP-Li₂TB additives can operate at temperatures ranging from -40 °C to 60 °C. This synergistic interphase modification utilizing dual electrolyte additives to construct a unique dual-layer CEI adaptive to a wide temperature range, provides valuable insights to the practical applications of NCM cathodes for all-climate batteries.

Cu-Li battery with Cu metal cathode and Li metal anode is a candidate for next-generation energy storage system. While self-discharge of the battery can be suppressed with an anion exchange membrane, the voltage polarization depends strongly on the electrolyte. Specifically, when an electrolyte with 3 M LiTFSI (lithium bis(trifluoromethanesulfonyl)imide) in dimethyl carbonate (DMC) is used, overpotential increases with cycling. In this work, we reveal why the voltage polarization changes, and reduce and stabilize it by replacing DMC solvent with a mixed solvent composed of dimethoxyethane (DME) and propylene carbonate (PC). The new electrolyte has higher ionic conductivity and stable solvation structure with more free TFSI^- anions upon cycling, which also facilitates uniform plating of metal ions on the metal electrodes. These characteristics enable a stable Cu-Li battery with minimal change in overpotential for more than 1500 cycles at a current density of 2 mA cm^-2.

Efficient, stable and economical catalysts play a crucial role in enhancing the kinetics of slow oxygen reduction reactions (ORR) in Aluminum-air batteries. Among the potential next-generation candidates, Ag catalysts are promising due to their high activity and low cost, but weaker oxygen adsorption has hindered industrialization. To address this bottleneck, Ag-alloying has emerged as a principal strategy. In this work, we successfully prepared Ag-Cu nanoparticles (NPs) with a rich eutectic phase and uniform dispersion structure using plasma evaporation. The increased solid solution of Ag and Cu led to changes in the electronic structure, resulting in an upward shift of the d-band center, which significantly improved oxygen adsorption. The combination of Ag and Cu in the NPs synergistically enhanced the adsorption of Ag and the desorption of Cu. Density functional theory (DFT) calculations revealed that Ag-Cu25 NPs exhibited the smallest limiting reaction barrier, leading to increased ORR activity. To further optimize the catalyst's performance, we utilized N-doped porous nanocarbon (N-PC) with high electrical conductivity and abundant mesoporous channels as the support for the Ag-Cu NPs. The N-PC support provided optimal mass transfer carriers for the highly active Ag-Cu25 NPs. As a result, the Ag-Cu25/NPC catalyst displayed excellent ORR activity in alkaline media, with a half-wave potential (E_1/2) of 0.82 V. Furthermore, the Al-air battery incorporating the Ag-Cu25/NPC catalyst exhibited outstanding electrochemical performance. It demonstrated high open-circuit voltages of 1.89 V and remarkable power densities of 193 mW cm^-2. The battery also sustained a high current output and maintained a stable high voltage for 120 hours under mechanical charging, showcasing its significant potential for practical applications.

Hard carbon (HC) is considered a promising anode material for sodium-ion batteries due to its relatively low price and high specific capacity. However, HC still suffers from unclear reaction mechanisms and unsatisfactory cycling stability. The study of mechano-electrochemical coupling behavior by in-situ measurement techniques is expected to understand the sodium storage and degradation mechanisms. In this paper, the strain and stress evolution of HC anodes at different sodiation/desodiation depths and cycles are investigated by combining electrochemical methods, digital image correlation, and theoretical equations. The observation by monitoring the in-situ strain evolution during the redox process supports the “adsorption-intercalation/filling” mechanism in reduction and the “de-filling/de-intercalation-desorption” mechanism in oxidation. Further studies have demonstrated that the strain and stress of the electrode show periodic changes accompanied by a continuous accumulation of residual stress during cycles, explaining the capacity degradation mechanism of HC from a mechanical perspective. In addition, when the higher current density is applied, the electrodes experience greater strain and stress associated with the Na⁺ insertion rate. This work clarifies the Na-storage mechanism and the mechano-electrochemical coupling mechanism of HC anodes by in-situ strain measurement, which helps optimize and design the anode materials of sodium-ion batteries from the perspective of interface microstructure and multi-field coupling, such as in situ integrated interface structure design.

Aluminum-selenium (Al-Se) batteries, which possess a high theoretical specific capacity of 1357 mA h g^-1, represent a promising energy storage technology. However, they suffer from significant attenuation of capacity and low cycle life due to the shuttle effect. To mitigate the shuttle effect induced by soluble selenium chloroaluminate compound that tends to migrate towards the negative electrode, a quasi-solid-state Al-Se battery was fabricated through the synthesis of a multi-aperture structure quasi-solid-state electrolyte (MOF@GPE) based on metal-organic framework (MOF) material and gel-polymer electrolyte (GPE). The high ionic conductivity (1.13 × 10^-3 S cm^-1) of MOF@GPE at room temperature, coupled with its wide electrochemical stability window (2.45 V), can facilitate ion transport kinetics and enhance the electrochemical performance of Al-Se batteries. The MOF@GPE-based quasi-solid-state Al-Se batteries exhibit outstanding long-life cycling stability, delivering a high specific discharge capacity of 548 mA h g^-1 with a maintained discharge specific capacity of 345 mA h g^-1 after 500 cycles at a current density of 200 mA g^-1. The stable ion transmission and high ion transport kinetics in MOF@GPE can be attributed to the stable structure and permeable channel of MOF, which effectively captures the soluble selenium chloroaluminate compound and further restrains the shuttle effect, resulting in improved cycling performance.

The continuous and excessive emission of CO₂ into the atmosphere presents a pressing challenge for global sustainable development. In response, researchers have been devoting significant efforts to develop methods for converting CO₂ into valuable chemicals and fuels. These conversions have the potential to establish a closed artificial carbon cycle and provide an alternative resource to depleting fossil fuels. Among the various conversion routes, thermochemical CO₂ reduction stands out as a promising candidate for industrialization. Within the realm of heterogeneous catalysis, single atom catalysts (SACs) have garnered significant attention. The utilization of SACs offers tremendous potential for enhancing catalytic performance. To achieve optimal activity and selectivity of SACs in CO₂ thermochemical reduction reactions, a comprehensive understanding of key factors such as single atom metal-support interactions, chemical coordination, and accessibility of active sites is crucial. Despite extensive research in this field, the atomic-scale reaction mechanisms in different chemical environments remain largely unexplored. While SACs have been found successful applications in electrochemical and photochemical CO₂ reduction reactions, their implementation in thermochemical CO₂ reduction encounters challenges due to the sintering and/or agglomeration effects that occur at elevated temperatures. In this review, we present a unique approach that combines theoretical understanding with experimental strategies to guide researchers in the design of controlled and thermally stable SACs. By elucidating the underlying principles, we aim to enable the creation of SACs that exhibit stable and efficient catalytic activity for thermochemical CO₂ reduction reactions. Subsequently, we provide a comprehensive overview of recent literature on noble metal- and transition metal-based SACs for thermochemical CO₂ reduction. The current review is focused on certain CO₂-derived products involving one step reduction only for simplicity and for better understanding the SACs enhancement mechanism. We emphasize various synthesis methods employed and highlight the catalytic activity of these SACs. Finally, we delve into the perspectives and challenges associated with SACs in the context of thermochemical CO₂ reduction reactions, providing valuable insights for future research endeavor. Through this review, we aim to contribute to the advancement of SACs in the field of thermochemical CO₂ reduction, shedding light on their potential as effective catalysts and addressing the challenges that need to be overcome for their successful implementation as paradigm shift in catalysis.

Electrochemical water splitting is a straightforward process that involves two distinct reactions: the oxygen evolution reaction (OER) which produces oxygen (O₂) and the hydrogen evolution reaction (HER) which generates hydrogen (H₂). However, in the whole process, the OER is a bottleneck as it requires more energy than a four-electron reaction involving critical raw materials (such as RuO₂ or IrO₂) as electrocatalysts. Therefore, here, we address the challenge of erratic kinetics/limited durability of OER in water electrolysis. In this paper, we demonstrate that the deposition of ultrasmall amounts of nickel(II) nitrate in zeolitic imidazolate framework-67 (ZIF-67) can be used as a general approach to enhance the electrocatalytic performance of the framework. We investigated the influence of Ni(NO₃)₂·x6H₂O loading on ZIF-67 (from 0.1 to 0.0001 M) and found that ZIF-67 enriched with only 0.001 M of Ni(NO₃)₂·x6H₂O (ZIF-67 0.001Ni) exhibited massive promotion in OER. The ZIF-67 0.001Ni showed a large specific surface area of 2577 m² g^-1, a low overpotential of 299 mV, a lower Tafel slope of 94.1 mA dec^-1, and an outstanding overpotential retention of 99.8% (at 50 mA cm^-2). By conducting electron paramagnetic resonance (EPR) measurements, we also discovered that the 0.001 M of Ni(NO₃)₂·x6H₂O loading in ZIF-67 introduces Ni²⁺ dimers, which contribute to the enhanced electroactivity of the modified ZIF-67. This phenomenon was further revealed during density-functional theory (DFT) calculations, which allowed us to identify different possible forms of Ni²⁺ dimers and modeling of active centers. Along with in situ experiments, we provide mechanistic insight into the OER mechanism under alkaline conditions and found that it follows the lattice oxygen mechanism (LOM). Our study proposes a facile and efficient room-temperature route to boost the electrochemical performance of ZIF-67 in OER. For the first time, we demonstrate that modifying ZIF-67 with an ultrasmall amount of different nickel(II) salts opens a general route to enhance its electroactivity during water-splitting reactions.

Owing to their high luminous efficiency and tunable emission in both red light and far-red light regions, Mn⁴⁺ ion-activated phosphors have appealed significant interest in photoelectric and energy conversion devices such as white light emitting diode (W-LED), plant cultivation LED, and temperature thermometer. Up to now, Mn⁴⁺ has been widely introduced into the lattices of various inorganic hosts for brightly red-emitting phosphors. However, how to correlate the structure-activity relationship between host framework, luminescence property, and photoelectric device is urgently demanded. In this review, we thoroughly summarize the recent advances of Mn⁴⁺ doped phosphors. Meanwhile, several strategies like co-doping and defect passivation for improving Mn⁴⁺ emission are also discussed. Most importantly, the relationship between the protocols for tailoring the structures of Mn⁴⁺ doped phosphors, increased luminescence performance, and the targeted devices with efficient photoelectric and energy conversion efficiency is deeply correlated. Finally, the challenges and perspectives of Mn⁴⁺ doped phosphors for practical applications are anticipated. We cordially anticipate that this review can deliver a deep comprehension of not only Mn⁴⁺ luminescence mechanism but also the crystal structure tailoring strategy of phosphors, so as to spur innovative thoughts in designing advanced phosphors and deepening the applications.

Severe mechanical fracture and unstable interphase, associated with the large volumetric expansion/contraction, significantly hinder the application of high-capacity SiO_x materials in lithium-ion batteries. Herein, we report the design and facile synthesis of a layer stacked SiO_x microparticle (LS-SiO_x) material, which presents a stacking structure of SiO_x layers with abundant disconnected interstices. This LS-SiO_x microparticle can effectively accommodate the volume expansion, while ensuring negligible particle expansion. More importantly, the interstices within SiO_x microparticle are disconnected from each other, which efficiently prevent the electrolyte from infiltration into the interior, achieving stable electrode/electrolyte interface. Accordingly, the LS-SiO_x material without any coating delivers ultrahigh average Coulombic efficiency, outstanding cycling stability, and full-cell applicability. Only 6 cycles can attain >99.92% Coulombic efficiency and the capacity retention at 0.05 A g^-1 for 100 cycles exceeds 99%. After 800 cycles at 1 A g-1, the thickness swelling of LS-SiO_x electrode is as low as 0.87%. Moreover, the full cell with pure LS-SiO_x anode exhibits capacity retention of 91.2% after 300 cycles at 0.2 C. This work provides a novel concept and effective approach to rationally design silicon-based and other electrode materials with huge volume variation for electrochemical energy storage applications.

Heat accumulation inside perovskite solar cells causes the decomposition of the perovskite layer and hole transport materials (HTMs) under working conditions, yielding a decrease in long-term stability. Here, we present a zeolite-assisted heat conduction strategy by introducing economic zeolite crystals (e.g., NaX, NaY, and ZSM-5) as a cooling filter to induce heat diffusion. The fitted thermal diffusion kinetic equation from real-time infrared thermal imaging technology reveals the zeolite skeleton assisted thermal conduction mechanism of internal lattice vibration. Additionally, the nearly twofold improved conductivity of the modified HTM film is benefited from Na⁺ hopping on the supercages of the zeolite, therefore, the best-performed device with a rapid heat diffusion and defect inhibition obtains a remarkable power conversion efficiency of 23.42%. Both of NaX modified sprio-OMeTAD and PTAA based devices exhibit excellent operational stability after heating 1000 h at 85 °C under N₂ condition. This work demonstrates the potential application of economical porous zeolite materials in improving the thermal stability of PSCs.

This paper brings the comparison of performances of CO₂ conversion by plasma and plasma-assisted catalysis based on the data collected from literature in this field, organised in an open access online database. This tool is open to all users to carry out their own analyses, but also to contributors who wish to add their data to the database in order to improve the relevance of the comparisons made, and ultimately to improve the efficiency of CO₂ conversion by plasma-catalysis. The creation of this database and database user interface is motivated by the fact that plasma-catalysis is a fast-growing field for all CO₂ conversion processes, be it methanation, dry reforming of methane, methanolisation, or others. As a result of this rapid increase, there is a need for a set of standard procedures to rigorously compare performances of different systems. However, this is currently not possible because the fundamental mechanisms of plasma-catalysis are still too poorly understood to define these standard procedures. Fortunately however, the accumulated data within the CO₂ plasma-catalysis community has become large enough to warrant so-called “big data” studies more familiar in the fields of medicine and the social sciences. To enable comparisons between multiple data sets and make future research more effective, this work proposes the first database on CO₂ conversion performances by plasma-catalysis open to the whole community. This database has been initiated in the framework of a H2020 European project and is called the “PIONEER DataBase”. The database gathers a large amount of CO₂ conversion performance data such as conversion rate, energy efficiency, and selectivity for numerous plasma sources coupled with or without a catalyst. Each data set is associated with metadata describing the gas mixture, the plasma source, the nature of the catalyst, and the form of coupling with the plasma. Beyond the database itself, a data extraction tool with direct visualisation features or advanced filtering functionalities has been developed and is available online to the public. The simple and fast visualisation of the state of the art puts new results into context, identifies literal gaps in data, and consequently points towards promising research routes. More advanced data extraction illustrates the impact that the database can have in the understanding of plasma-catalyst coupling. Lessons learned from the review of a large amount of literature during the setup of the database lead to best practice advice to increase comparability between future CO₂ plasma-catalytic studies. Finally, the community is strongly encouraged to contribute to the database not only to increase the visibility of their data but also the relevance of the comparisons allowed by this tool.

Aqueous Zn-ion batteries (AZIBs) are the potential options for the next-generation energy storage scenarios due to the cost effectiveness and intrinsic safety. Nevertheless, the industrial application of AZIBs is still impeded by a series of parasitic reactions and dendrites at zinc anodes. In this study, taurine (TAU) is used in electrolyte to simultaneously optimize the coordination condition of the ZnSO₄ electrolyte and interfacial chemistry at the anode. TAU can preferentially adsorb with the zinc metal and induce an in situ stable and protective interface on the anode, which would avoid the connection between H₂O and the zinc metal and promote the even deposition of Zn²⁺. The resulting Zn//Zn batteries achieve more than 3000 hours long cyclic lifespan under 1 mA cm^-2 and an impressive cumulative capacity at 5 mA cm^-2. Moreover, Zn//Cu batteries can realize a reversible plating/stripping process over 2,400 cycles, with a desirable coulombic efficiency of 99.75% (1 mA cm^-2). Additionally, the additive endows Zn//NH₄V₄O₁₀ batteries with more stable cyclic performance and ultrafast rate capability. These capabilities can promote the industrial application of AZIBs.

Ni-based catalysts are widely investigated non-noble metal-based systems for CO₂ methanation. However, their industrial application is still limited due to lower activity at low-temperature and catalyst deactivation. Incorporating a second metal such as Ru and Fe is considered as a successful strategy to overcome these challenges through alloy formation or the synergies provided by the interplay of two adjacent metallic sites. Nonetheless, their promotional effect on the CO₂ methanation mechanism under similar conditions has not been reported yet. In this work, Fe and Ru-promoted Ni/ZrO₂ catalysts were investigated to evaluate their promotional effect on the mechanism. The Ni/Fe ratio was first optimized and a CO₂ conversion rate of 37.7 mmolCO₂/(mol_Ni+Fe s) and 96.3% CH₄ selectivity was obtained over the Ni_0.8Fe_0.2/ZrO₂ catalyst. In comparison with Ni_0.8Fe_0.2/ZrO₂, Ni_0.8Ru_0.2/ZrO₂ prepared with the same composition showed higher activity and stability in CO₂ methanation. Characterization results indicate alloys formation and H spillover for Ni_0.8Ru_0.2/ZrO₂ to be responsible for promotion. Besides, in situ DRIFTS studies evidenced the occurrence of both CO₂ dissociative and associative pathways over Ni_0.8Ru_0.2/ZrO₂ catalyst, while solely the CO₂ associative pathway occurred for Ni_0.8Fe_0.2/ZrO₂.

Maximizing the utilization of lithium-ion battery capacity is an important means to alleviate the range anxiety of electric vehicles. Battery pack inconsistency is the main limiting factor for improving battery pack capacity utilization, and poses major safety hazards to energy storage systems. To solve this problem, a maximum capacity utilization scheme based on a path planning algorithm is proposed. Specifically, the reconfigurable topology proposed is highly flexible and fault-tolerant, enabling battery pack consistency through alternating cell discharge and reducing the increased risk of short circuits due to relay error. The Dijkstra algorithm is used to find the optimal energy path, which can effectively remove faulty cells and find the current path with the best consistency of the battery pack and the lowest relay loss. Finally, the effectiveness of the scheme is verified by hardware-in-the-loop experiments, and the experimental results show that the state-of-charge SOC consistency of the battery pack at the end of discharge is increased by 34.18%, the relay energy loss is reduced by 0.16%, and the fault unit is effectively isolated.

Aqueous Zn-ion energy storage systems, which are expected to be integrated into intelligent electronics as a secure power supply, suffer poor reversibility of Zn anodes, predominantly associated with dendritic growth and side reactions. This study introduces a polyanionic strategy to address these formidable issues by developing a hydrogel electrolyte (PACXHE) with carboxyl groups. Notably, the carboxyl groups within the hydrogel structure establish favorable channels to promote the transport of Zn²⁺ ions. They also expedite the desolvation of hydrated Zn²⁺ ions, leading to enhanced deposition kinetics. Additionally, these functional groups confine interfacial planar diffusion and promote preferential deposition along the (002) plane of Zn, enabling a smooth surface texture of the Zn anode. This multifaceted regulation successfully achieves the suppression of Zn dendrites and side reactions, thereby enhancing the electrochemical reversibility and service life during plating/stripping cycles. Therefore, such an electrolyte demonstrates a high average Coulombic efficiency of 97.7% for 500 cycles in the Zn||Cu cell and exceptional cyclability with a duration of 480 h at 1 mA cm^-2/1 mA h cm^-2 in the Zn||Zn cell. Beyond that, the Zn-ion hybrid micro-capacitor employing PACXHE exhibits satisfactory cycling stability, energy density, and practicality for energy storage in flexible, intelligent electronics. The present polyanionic-based hydrogel strategy and the development of PACXHE represent significant advancements in the design of hydrogel electrolytes, paving the way for a more sustainable and efficient future in the energy storage field.

The sulfide-based solid-state electrolytes (SEs) reactivity toward moisture and Li-metal are huge barriers that impede their large-scale manufacturing and applications in all-solid-state lithium batteries (ASSLBs). Herein, we proposed an Al and O dual-doped strategy for Li₃PS₄ SE to regulate the chemical/electrochemical stability of anionic PS₄^3- tetrahedra to mitigate structural hydrolysis and parasitic reactions at the SE/Li interface. The optimized Li_3.08Al_0.04P_0.96S_3.92O_0.08 SE presents the highest σ_Li+ of 3.27 mS cm^-1, which is ∼6.8 times higher than the pristine Li₃PS₄ and excellently inhibits the structural hydrolysis for ∼25 min @25% humidity at RT. DFT calculations confirmed that the enhanced chemical stability was revealed to the intrinsically stable entities, e.g., POS₃^3- units. Moreover, Li_3.08Al_0.04P_0.96S_3.92O_0.08 SE cycled stably in Li//Li symmetric cell over 1000 h @0.1 mA cm^-2/0.1 mA h cm^-2, could be revealed to Li-Al alloy and Li₂O at SE/Li interface impeding the growth of Li-dendrites during cycling. Resultantly, LNO@LCO/Li_3.08Al_0.04P_0.96S_3.92O_0.08/Li-In cell delivered initial discharge capacities of 129.8 mA h g^-1 and 83.74% capacity retention over 300 cycles @0.2 C at RT. Moreover, the Li_3.08Al_0.04P_0.96S_3.92O_0.08 SE presented >90% capacity retention over 200 and 300 cycles when the cell was tested with LiNi_0.8Co_0.15Al_0.05O₂ (NCA) cathode material vs. 5 and 10 mg cm^-2 @RT.

Taking copper doped ZnS (ZnS:Cu) nanocrystals as the main body of photocatalyst, the influence of different base transition metal ions (M²⁺ = Ni²⁺, Co²⁺, Fe²⁺ and Cd²⁺) on photocatalytic CO₂ reduction in inorganic reaction system is investigated. Confined single-atom Ni²⁺, Co²⁺, and Cd²⁺ sites were created via cation-exchange process and enhanced CO₂ reduction, while Fe²⁺ suppressed the photocatalytic activity for both water and CO₂ reduction. The modified ZnS:Cu photocatalysts (M/ZnS:Cu) demonstrated tunable product selectivity, with Ni²⁺ and Co²⁺ showing high selectivity for syngas production and Cd²⁺ displaying remarkable formate selectivity. DFT calculations indicated favorable H adsorption free energy on Ni²⁺ and Co²⁺ sites, promoting the hydrogen evolution reaction. The selectivity of CO₂ reduction products was found to be sensitive to the initial intermediate adsorption states. *COOH formed on Ni²⁺ and Co²⁺ while *OCHO formed on Cd²⁺, favoring the production of CO and HCOOH as the main products, respectively. This work provides valuable insights for developing efficient solar-to-fuel platforms with controlled CO₂ reduction selectivity.

Photoelectrochemical (PEC) H₂O₂ production through water oxidation reaction (WOR) is a promising strategy, however, designing highly efficient and selective photoanode materials remains challenging due to competitive reaction pathways. Here, for highly enhanced PEC H₂O₂ production, we present a conformal amorphous titanyl phosphate (a-TP) overlayer on nanoparticulate TiO₂ surfaces, achieved via lysozyme-molded in-situ surface reforming. The a-TP overlayer modulates surface adsorption energies for reaction intermediates, favoring WOR for H₂O₂ production over the competing O₂ evolution reaction. Our density functional theory calculations reveal that a-TP/TiO₂ exhibits a substantial energy uphill for the O* formation pathway, which disfavors O₂ evolution but promotes H₂O₂ production. Additionally, the a-TP overlayer strengthens the built-in electric field, resulting in favorable kinetics. Consequently, a-TP/TiO₂ exhibits 3.7-fold higher Faraday efficiency (FE) of 63% at 1.76 V vs. reversible hydrogen electrode (RHE) under 1 sun illumination, compared to bare TiO₂ (17%), representing the highest FE among TiO₂-based WOR H₂O₂ production systems. Employing the a-TP overlayer constitutes a promising strategy for controlling reaction pathways and achieving efficient solar-to-chemical energy conversion.

The development of urbanization and industrialization leads to rapid depletion of fossil fuels. Therefore, the production of fuel from renewable resources is highly desired. Electrotechnical energy conversion and storage is a benign technique with reliable output and is eco-friendly. Developing an exceptional electrochemical catalyst with tunable properties like a huge specific surface area, porous channels, and abundant active sites is critical points. Recently, Metal-organic frameworks (MOFs) and two-dimensional (2D) transition-metal carbides/nitrides (MXenes) have been extensively investigated in the field of electrochemical energy conversion and storage. However, advances in the research on MOFs are hampered by their limited structural stability and conventionally low electrical conductivity, whereas the practical electrochemical performance of MXenes is impeded by their low porosity, inadequate redox sites, and agglomeration. Consequently, researchers have been designing MOF/MXene nanoarchitectures to overcome the limitations in electrochemical energy conversion and storage. This review explores the recent advances in MOF/MXene nanoarchitectures design strategies, tailoring their properties based on the morphologies (0D, 1D, 2D, and 3D), and broadening their future opportunities in electrochemical energy storage (batteries, supercapacitors) and catalytic energy conversion (HER, OER, and ORR). The intercalation of MOF in between the MXene layers in the nanoarchitectures functions synergistically to address the issues associated with bare MXene and MOF in the electrochemical energy storage and conversion. This review gives a clear emphasis on the general aspects of MOF/MXene nanoarchitectures, and the future research perspectives, challenges of MOF/MXene design strategies and electrochemical applications are highlighted.

Proton conducting ceramic cells (PCCs) are an attractive emerging technology operating in the intermediate temperature range of 500 to 700 °C. In this work, we evaluate the production of hydrogen at intermediate temperatures by proton conducting ceramic cell electrolysis (PCCEL). We demonstrate a high-performance steam electrolysis owing to a composite positrode based on BaGd_0.8La_0.2Co₂O_6-δ (BGLC1082) and BaZr_0.5Ce_0.4Y_0.1O_3-δ (BZCY541). The high reliability of PCCEL is demonstrated for 1680 h at a current density as high as -0.8 A cm^-2 close to the thermoneutral cell voltage at 600 °C. The electrolysis cell showed a specific energy consumption ranging from 54 to 66 kW h kg^-1 that is comparable to state-of-the-art low temperature electrolysis technologies, while showing hydrogen production rates systematically higher than commercial solid oxide ceramic cells (SOCs). Compared to SOCs, the results verified the higher performances of PCCs at the relevant operating temperatures, due to the lower activation energy for proton transfer comparing with oxygen ion conduction. However, because of the p-type electronic conduction in protonic ceramics, the energy conversion rate of PCCs is relatively lower in steam electrolysis. The faradaic efficiency of the PCC in electrolysis mode can be increased at lower operating temperatures and in endothermic conditions, making PCCEL a technology of choice to valorize high temperature waste heat from industrial processes into hydrogen. To increase the faradaic efficiency by optimizing the materials, the cell design, or the operating strategy is a key challenge to address for future developments of PCCEL in order to achieve even more superior techno-economic merits.

Steam reforming (SR) of fossil methane is already a well-known, documented and established expertise in the industrial sector as it accounts for the vast majority of global hydrogen production. From a sustainable development perspective, hydrogen production by SR of biomass-derived feedstock represents a promising alternative that could help to lower the carbon footprint of the traditional process. In this regard, bio-alcohols such as methanol, ethanol or glycerol are among the attractive candidates that could serve as green hydrogen carriers as they decompose at relatively low temperatures in the presence of water compared to methane, allowing for improved H₂ yields. However, significant challenges remain regarding the activity and stability of nickel-based catalysts, which are most widely used in alcohol SR processes due to their affordability and ability to break C-C, O-H and C-H bonds, yet are prone to rapid deactivation primarily caused by coke deposition and metal particle sintering. In this state-of-the-art review, a portfolio of strategies to improve the performance of Ni-based catalysts used in alcohol SR processes is unfolded with the intent of pinpointing the critical issues in catalyst development. Close examination of the literature reveals that the efforts tackling these recurring issues can be directed at the active metal, either by tuning Ni dispersion and Ni-support interactions or by targeting synergistic effects in bimetallic systems, while others focus on the support, either by modifying acid-base character, oxygen mobility, or by embedding Ni in specific crystallographic structures. This review provides a very useful tool to orient future work in catalyst development.

5-Hydroxymethylfurfural electrooxidation reaction (HMFOR) is a promising route to produce value-added chemicals from biomass. Since it involves HMF adsorption and C-H/O-H cleavage, understanding the adsorption behavior and catalytic process of organic molecules on catalysts is important. Herein, the selective adsorption sites of NiMoO are tuned by Ni particles for HMFOR-assisted H₂ production. Experimental and theoretical calculation results indicate that the synergistic interaction between Ni and NiMoO optimizes the adsorption/desorption of HMF/intermediates/2,5-furandicarboxylic acid (FDCA) and promotes the C-H/O-H bond cleavage, thereby improving the HMFOR kinetics (k_NiMoO-Ni/k_NiMoO = 1.97) and FDCA selectivity (99.3%). When coupled as a two-electrode system, it can drive efficient HMF conversion (FDCA yield: 98.5%) and H₂ production (Faradaic efficiency: 99.1%) at 1.45 V. This work thus offers a strategy to tune the adsorption sites of catalyst for efficient HMFOR-assisted H₂ production.

Lithium-ion batteries (LIBs) require separators with high performance and safety to meet the increasing demands for energy storage applications. Coating electrochemically inert ceramic materials on conventional polyolefin separators can enhance stability but comes at the cost of increased weight and decreased capacity of the battery. Herein, a novel separator coated with lithium iron phosphate (LFP), an active cathode material, is developed via a simple and scalable process. The LFP-coated separator exhibits superior thermal stability, mechanical strength, electrolyte wettability, and ionic conductivity than the conventional polyethylene (PE) separator. Moreover, the LFP coating can actively participate in the electrochemical reaction during the charge-discharge process, thus enhancing the capacity of the battery. The results show that the LFP-coated separator can increase the cell capacity by 26%, and improve the rate capability by 29% at 4 C compared with the conventional PE separator. The LFP-coated separator exhibits only 1.1% thermal shrinkage at 140 °C, a temperature even above the melting point of PE. This work introduces a new strategy for designing separators with dual functions for the next-generation LIBs with improved performance and safety.

The (electro)chemical stability and Li dendrite suppression capability of sulfide solid electrolytes (SEs) need further improvement for developing all-solid-state Li batteries (ASSLBs). Here, we report advanced halogen-rich argyrodites via I and Cl co-occupation on the crystal lattice. Notably, a proper I content forms a single phase, whereas an excessive I causes precipitation of two argyrodite phases like a superlattice structure. The resultant synergistic effect of the optimized composition allows to gain high ionic conductivities at room temperature and -20 °C, and enhances the (electro)chemical stability against Li and Li dendrite suppression capability. The Li|argyrodite interface is very sensitive to the ratio of I and Cl. A LiCl- and LiI-rich double-layer interface is observed from the cell using the SE with optimized composition, whereas too high I content forms only a single interface layer with a mixture of LiI and LiCl. This double-layer interface is found to effectively mitigate the Li/SE reaction. The proper designed argyrodite enables ASSLBs to achieve good electrochemical properties at a broad temperature range regardless of the electrode materials. This co-occupation strategy provides a novel exploration for advanced halogen-rich argyrodite system.

Ru with Pt-like hydrogen bond strength, knockdown cost (∼1/3 of Pt), and eximious stability is a competitive replacement for Pt-based catalysts towards the hydrogen evolution reaction (HER) in water splitting. The design of Ru-based catalysts via interface construction, crystal phase control, and specific light element doping to realize the impressive promotion of limited activity and stability remains challenging. Herein, we report the fabrication of Pd@RuP core-shell nanorods (NRs) via an epitaxial growth method, where ultrathin RuP shells extend the face-centered cubic (fcc) crystal structure and (111) plane of the Pd NRs core. Density functional theory results confirm that the core-shell interface engineering and P doping synergistically accelerate electron transfer and moderate the d-band center to generate a suitable affinity for H*, thus optimizing HER kinetics. Compared with Pd@Ru NRs and Pt/C, the Pd@RuP NRs exhibit preferable electrocatalytic stability and superior activity with a low overpotential of 18 mV at 10 mA cm^-2 in the alkaline HER process. Furthermore, the integrated Pd@RuP//RuO₂-based electrolyzer also displays a low operation potential of 1.42 V to acquire 10 mA cm^-2, demonstrating great potential for practical water electrolysis. Our work presents an efficient avenue to design Ru-based electrocatalysts via epitaxial growth for extraordinary HER performance.

Hydrogen is a popular clean high-energy-density fuel. However, its utilization is limited by the challenges toward low-cost hydrogen production and safe hydrogen storage. Fortunately, these issues can be addressed using promising hydrogen storage materials such as B-H compounds. Hydrogen stored in B-H compounds can be released by hydrolysis at room temperature, which requires catalysts to increase the rate of the reaction. Recently, several effective approaches have been developed for hydrogen generation by catalyzing the hydrolysis of B-H compounds. This review summarizes the existing research on the use of nanoparticles loaded on hydrogels as catalysts for the hydrolysis of B-H compounds. First, the factors affecting the hydrolysis rate, such as temperature, pH, reactant concentration, and type of nano particles, were investigated. Further, the preparation methods (in situ reduction, one-pot method, template adsorption, etc.) for the hydrogel catalysts and the types of loaded catalysts were determined. Additionally, the hydrogel catalysts that can respond to magnetic fields, ultrasound fields, optical fields, and other physical fields are introduced. Finally, the issues and future developments of hydrogel-based catalysts are discussed. This review can inspire deeper investigations and provide guidance for the study of hydrogel catalysts in the field of hydrogen production via hydrolysis.

High entropy oxides (HEOs) with ideal element tunability and enticing entropy-driven stability have exhibited unprecedented application potential in electrochemical lithium storage. However, the general control of dimension and morphology remains a major challenge. Here, scalable HEO morphology modulation is implemented through a salt-assisted strategy, which is achieved by regulating the solubility of reactants and the selective adsorption of salt ions on specific crystal planes. The electrochemical properties, lithiation mechanism, and structure evolution of composition- and morphology-dependent HEO anode are examined in detail. More importantly, the potential advantages of HEOs as electrode materials are evaluated from both theoretical and experimental aspects. Benefiting from the high oxygen vacancy concentration, narrow band gap, and structure durability induced by the multi-element synergy, HEO anode delivers desirable reversible capacity and reaction kinetics. In particular, Mg is evidenced to serve as a structural sustainer that significantly inhibits the volume expansion and retains the rock salt lattice. These new perspectives are expected to open a window of opportunity to compositionally/morphologically engineer high-performance HEO electrodes.

Thermal runaway (TR) of lithium-ion (Li-ion) batteries (LIBs) involves multiple forms of hazards, such as gas venting/jetting, fire, or even explosion. Explosion, as the most extreme case, is caused by the generated flammable gases, and a deflagration to detonation transition (DDT) may occur in this process. Here, overheat-to-TR tests and the corresponding outgas-induced explosion tests were conducted on 42 Ah Li-ion cells with Li[Ni_1/3Co_1/3Mn_1/3]O₂ cathode. The sum of CO₂, H₂, C₂H₄, CO, and CH₄ accounted for more than 90% of the gases. Lower/upper explosion limits (LEL/UEL), laminar flame speed, and ideal stable detonation pressure were calculated to interpret the explosion characteristics and boundary. It turned out that shockwave was easily to be compressed and accelerated under higher state of charge (SOC) conditions. Thus, Li-ion cells explosion may evolve into unstable detonation in encapsulated battery pack and its evolution mechanism was explained, which provides a new idea for explosion-proof design of LIBs system. Additionally, a comprehensive assessment method was developed to intuitively characterize TR hazards. Severity of explosion presented an upward trend with the increase of SOC while the sensitivity was not the same. This study provides a further anatomy of TR, which is instructive to the safety of power battery systems.

Hetero-element doping is a promising strategy to improve the cycling stability of nickel-rich cobalt-free cathodes for the next-generation high energy-density Li ion batteries. To make doping effective, it is important to understand the mechanism of how the dopants regulate the electronic band, lattice parameter adjusting, or hetero-phase formation to achieve high stability. In this study, we investigate LiNi_0.9Mn_0.1O₂ cathodes doped with IVB grouping elements via multiple characterization techniques. By utilizing in situ XRD and TEM methods, we found that the stronger Ti-O bond effectively improves the cathode stability via a dual protection mechanism. Specifically, the bulk lattice of cathode is well-preserved during cycling as a result of the suppressed H2-H3 phase transition, while a in situ formed Ti-rich surface layer can prevent continuous surface degradation. As a result, the 5% Ti doped LiNi_0.9Mn_0.1O₂ cathode exhibits a high capacity retention of 96% after 100 cycles. Whereas, despite IVB group elements Zr and Hf have stronger bonding energy with oxygen, their larger ionic radii actually impede their diffusion into the cathode, thereby they can not improve the cycling stability. Our findings uncover the functional origin of doped elements with their dynamic modification on cathode structure, providing mechanistic insights into the design of nickel-rich cobalt-free cathodes.

The electrocatalytic carbon dioxide reduction reaction (eCO₂RR) into high-value-added chemicals and fuels is a promising strategy to mitigate global warming. However, it remains a significant stumbling block to the rationally tuning lattice plane of the catalyst with high activity to produce the target product in the eCO₂RR process. To attempt to solve this problem, the CuIn bimetallic alloy nanocatalyst with specifically exposed lattice planes is modulated and electrodeposited on the nitrogen-doped porous carbon cloth by a simple two-step electrodeposition method, which induces high Faraday efficiency of 80% towards HCOO^- (FE_HCOO-) with a partial current density of 13.84 mA cm^-2 at -1.05 V (vs. RHE). Systematic characterizations and theoretical modeling reveal that the specific coexposed CuIn (200) and In (101) lattice facets selectively adsorbed the key intermediate of OCHO*, reducing the overpotential of HCOOH and boosting the FE_HCOO- in a wide potential window (-0.65--1.25 V). Moreover, a homogeneous distribution of CuIn nanoparticles with an average diameter of merely ∼3.19 nm affords exposure to abundant active sites, meanwhile prohibiting detachment and agglomeration of nanoparticles during eCO₂RR for enhanced stability attributing to the self-assembly electrode strategy. This study highlights the synergistic effect between catalytic activity and facet effect, which opens a new route in surface engineering to tune their electrocatalytic performance.

Zinc-based flow batteries (ZFBs) have aroused great favor in large-scale energy storage due to the high security and low cost. However, the low areal capacity arising from the limited space for Zn plating hinders the further development. Herein, a novel carbon felt-Sn-carbon felt sandwich host (CSCH) is designed and constructed. Benefiting from the strong chemical absorption and the dehydration effect on Zn(H₂O)₆²⁺, the Sn activation layer in the CSCH demonstrates the lowest comprehensive resistance for Zn deposition. Thus, Zn is induced to nucleate preferentially on the Sn activation layer, and grows towards the membrane, regulating the spatial distribution of Zn electrochemical deposits, which remarkably improves the areal capacity and cyclic stability of Zn anode. Consequently, the zinc-bromine flow batteries equipped with CSCH electrodes can achieve the ultra-high areal capacity of 120 mA h cm^-2 at 80 mA cm^-2, and run stably for 140 h with average energy efficiency of 80.3% in the extreme condition (80 mA cm^-2, 80 mA h cm^-2). This innovative work will inspire future advanced designs for high areal capacity electrodes in ZFBs.

Although the fast development of potassium-ion hybrid capacitors (PIHC) recently, the issues such as the slow kinetics and poor durability of potassium ion hosts greatly restric their applications. Herein, a freestanding fiber (NHF fiber) with necklace-like configuration and CoPSe@N-doped carbon (CoPSe@NCNT) heterostructured units is introduced as the anode in PIHC. The highly porous network of NHF fiber facilitates the fast ion transports and promises the good high-rate property. Additionally, the nanoscle crystallites inside in-situ grown NCNT favor the high adaption to volume expansion/shrinkage and endow good structure stability during ion insertion/deinsertion. Density function theoretical (DFT) calculations disclose the CoPSe@NCNT heterostructure has improved intrinsic conductivity, fast potassium migration, and decreased energy barrier. Meanwhile, the finite element simulation analysis (FEA) reveals the decreased stress inside the NHF architecture during charge/discharge processes. Moreover, the electrochemical tests confirm the fast and durable properties of the CoPSe@NCNT NHF fibers for potassium storage. Furthermore, the PIHC full cell with the anode of CoPSe@NCNT NHF fiber is assembled, which obtains the superior energy/power densities and high capacity retention (89%) after 2000 cycles at 2 A g^-1. When the polymer electrolyte is incooperated, the flexible PIHC device achieves the good pliability and good adaptation during wide temperature changes from -20 to 25 °C. Therefore, this work introduces a novel anode for fast potassium ion storage, and opens a new approach to assemble the power sources for flexible electronics in diverse conditions.

Engineering the specific active sites of photocatalysts for simultaneously promoting CO₂ and H₂O activation is important to achieve the efficient conversion of CO₂ to hydrocarbon with H₂O as a proton source under sunlight. Herein, we delicately design the In/TiO₂-V_O photocatalyst by engineering In single atoms (SAs) and oxygen vacancies (V_Os) on porous TiO₂. The relation between structure and performance of the photocatalyst is clarified by both experimental and theoretical analyses at the atomic levels. The In/TiO₂-V_O photocatalyst furnish a high CH₄ production rate up to 35.49 μmol g^-1 h^-1 with a high selectivity of 91.3% under simulated sunlight, while only CO is sluggishly generated on TiO₂-V_O. The combination of in situ spectroscopic analyses with theoretical calculations reveal that the V_O sites accelerate H₂O dissociation and increase proton feeding for CO₂ reduction. Furthermore, the V_O regulated In-Ti dual sites enable the formation of a stable adsorption conformation of In-C-O-Ti intermediate, which is responsible for the highly selective reduction of CO₂ to CH₄. This work demonstrates a new strategy for the development of effective photocatalysts by coupling metal SA sites with the adjacent metal sites of support to synergistically enhance the activity and selectivity of CO₂ photoreduction.

Herein, Pd nanoparticles loaded Co₃O₄ catalysts (Pd@Co₃O₄) are constructed from zeolitic imidazolate framework-67 (ZIF-67) for the ethanol oxidation reaction (EOR). It is demonstrated for the first time that the electrochemical conversion of Co₃O₄ support would result in the charge distribution alignment at the Pd/Co₃O₄ interface and induce the formation of highly reactive Pd-O species (PdO*), which can further catalyze the consequent reactions of the intermediates of the ethanol oxidation. The catalyst, Pd@Co₃O₄-450, obtained under the optimized conditions exhibits excellent EOR performance with a high mass activity of 590 mA mg^-1, prominent operational stability, and extraordinary capability for the electro-oxidation of acetaldehyde intermediates. Importantly, the detailed mechanism investigation reveals that Pd@Co₃O₄-450 could be benefit to the C-C bond cleavage to promote the desirable C1 pathway for the ethanol oxidation reaction. The present strategy based on the metal-support interaction of the catalyst might provide valuable inspiration for the design of high-performing catalysts for the ethanol oxidation reaction.

Promising room-temperature sodium-sulfur (RT Na-S) battery systems rely on purposely designed high-performing and low-cost electrode materials. Nevertheless, there are the challenges of irreversible dissolution and slow redox kinetics of NaPSs in the complete discharge of sulfur capacity. Herein, engineered CoMoO₄ in reduced graphene oxide (CoMoO₄@rGO) is reported as a class of superior cathode hosts for RT Na-S batteries. The CoMoO₄@rGO matrix is designed to facilitate the reversible sodiation and desodiation of sulfur, considering the strong chemisorption between sulfur (and short-chain sodium sulfides) and CoMoO₄, which alleviates the shuttle effect of sodium sulfides and accelerates the electrochemical reaction rate at RT. The obtained S/CoMoO₄@rGO cathode with ∼52% S loading exhibits a high capacity of 520.1 mA h g^-1 after 100 cycles at 0.1 A g^-1. Moreover, an enhanced long-term performance at high current densities (212.2 mA h g^-1 at 4 A g^-1 over 1000 cycles) with high Coulombic efficiency (∼100%) is also achieved. This work demonstrates a novel multifunctional additive for RT Na-S battery cathodes, which is expected to promote the long-waited development towards practical applications of RT Na-S batteries.