Iridium (Ir)-based catalysts are highly efficient for the anodic oxygen evolution reaction (OER) due to high stability and anti-corrosion ability in the strong acid electrolyte. Recently, intensive attention has been directed to novel, efficient, and low-cost Ir-based catalysts to overcome the challenges of their application in the water electrolysis technique. To make a comprehensive understanding of the recently developed Ir-based catalysts and their catalytic properties, the mechanism and catalytic promotion principles of Ir-based catalysts were discussed for OER in the acid condition aimed for the proton exchange membrane water electrolyzer (PEMWE) in this review. The OER catalytic mechanisms of the adsorbate evolution mechanism and the lattice oxygen mechanism were first presented and discussed for easy understanding of the catalytic mechanism; a brief perspective analysis of promotion principles from the aspects of geometric effect, electronic effect, synergistic effect, defect engineering, support effect was concluded. Then, the latest progress and the practical application of Ir-based catalysts were introduced in detail, which was classified into the varied composition of Ir catalyst in terms of alloys, hetero-element doping, perovskite, pyrochlore, heterostructure, core–shell structure, and supported catalysts. Finally, the problems and challenges faced by the current Ir-based catalyst in the acidic electrolyte were put forward. It is concluded that highly efficient catalysts with low Ir loading should be developed in the future, and attention should be paid to probing the structural and performance correlation, and their application in real PEMWE devices.Hopefully, the current effort can be helpful in the catalysis mechanism understanding of Ir-based catalysts for OER, and instructive to the novel efficient catalysts design and fabrication. 

https://www.sciopen.com/article_pdf/1629421774399119362.pdf

Iridium-based catalysts for oxygen evolution reaction in acidic media: mechanism, catalytic promotion effects and recent progress

For the development of aqueous zinc-ion batteries, exploiting vanadium-based cathode materials with quick kinetics and acceptable cycling stability is crucial. Herein, to achieve these goals, transition metal ions (Zn2+) and organic ions (C5H14ON+ and Ch+) are introduced into layered hydrated V2O5. The intrinsic high conductivity of Ch+ and the oxygen vacancies generated through ion pre-intercalation accelerate the electrical mobility by optimizing the electronic structure. The Zn2+ stabilizes the layered structure and the expanded interlayer spacing improves the ionic diffusivity. The synergistic effect of pre-intercalated Zn2+ and Ch+ results in the (Zn0.1, Ch0.1)V2O4.92·0.56H2O cathode exhibiting a discharge capacity of 473 mAh g−1 at 0.1 A g−1 with a high energy efficiency of 88% and excellent cycling stability with 91% retention after 2000 cycles at 4 A g−1. Ex situ characterizations and density functional theory calculations reveal a reversible intercalation mechanism of Zn2+, and the improved electrochemical kinetics are attributed to the altered electronic conductivity and the reduced binding energy between Zn2+ and host O2−. 

Dual Effects of Metal and Organic Ions Co‐Intercalation Boosting the Kinetics and Stability of Hydrated Vanadate Cathodes for Aqueous Zinc‐Ion Batteries

Solid-state electrolytes (SEs) have attracted overwhelming attention as a promising alternative to traditional organic liquid electrolytes (OLEs) for high-energy-density sodium-metal batteries (SMBs), owing to their intrinsic incombustibility, wider electrochemical stability window (ESW), and better thermal stability. Among various kinds of SEs, inorganic solid-state electrolytes (ISEs) stand out because of their high ionic conductivity, excellent oxidative stability, and good mechanical strength, rendering potential utilization in safe and dendrite-free SMBs at room temperature. However, the development of Na-ion ISEs still remains challenging, that a perfect solution has yet to be achieved. Herein, we provide a comprehensive and in-depth inspection of the state-of-the-art ISEs, aiming at revealing the underlying Na+ conduction mechanisms at different length scales, and interpreting their compatibility with the Na metal anode from multiple aspects. A thorough material screening will include nearly all ISEs developed to date, i.e., oxides, chalcogenides, halides, antiperovskites, and borohydrides, followed by an overview of the modification strategies for enhancing their ionic conductivity and interfacial compatibility with Na metal, including synthesis, doping and interfacial engineering. By discussing the remaining challenges in ISE research, we propose rational and strategic perspectives that can serve as guidelines for future development of desirable ISEs and practical implementation of high-performance SMBs.

Recent progress and strategic perspectives of inorganic solid electrolytes: fundamentals, modifications, and applications in sodium metal batteries.

Designing novel single-atom catalysts (SACs) supports to modulate the electronic structure is crucial to optimize the catalytic activity, but rather challenging. Herein, a general strategy is proposed to utilize the metalloid properties of supports to trap and stabilize single-atoms with low-valence states. A series of single-atoms supported on the surface of tungsten carbide (M-WCx, M=Ru, Ir, Pd) are rationally developed through a facile pyrolysis method. Benefiting from the metalloid properties of WCx, the single-atoms exhibit weak coordination with surface W and C atoms, resulting in the formation of low-valence active centers similar to metals. The unique metal-metal interaction effectively stabilizes the low-valence single atoms on the WCx surface and improves the electronic orbital energy level distribution of the active sites. As expected, the representative Ru-WCx exhibits superior mass activities of 7.84 and 62.52 A mgRu-1 for the hydrogen oxidation and evolution reactions (HOR/HER), respectively. In-depth mechanistic analysis demonstrates that an ideal dual-sites cooperative mechanism achieves a suitable adsorption balance of Had and OHad, resulting in an energetically favorable Vollmer step. This work offers new guidance for the precise construction of highly active SACs.

Stabilizing Low-Valence Single Atoms by Constructing Metalloid Tungsten Carbide Supports for Efficient Hydrogen Oxidation and Evolution.

Aqueous zinc-ion batteries have attracted extensive attention ascribing to affordability, intrinsic safety, and environmental benignity, which have revealed ideal alternative to lithium-ion batteries for large-scale energy storage systems. Nevertheless, the design of aqueous zinc-ion batteries is plagued by obstacles, such as dissolution of cathode materials, dendrites and side reactions of anode, and electrolyte consumption as compared to commercial lithium-ion batteries. In this regard, from the perspective of predominant issues encountered with aqueous zinc-ion batteries, this comprehensive review aims to systematically summarize the design principles and optimization strategies associated with the cathode, anode, electrolyte, and separator. Meanwhile, the impact of design strategies on electrochemistry, and the relationship between issues and strategies are revealed for guiding the rational design of advanced aqueous zinc-ion batteries. Eventually, a series of critical challenges, constructive solutions, and future trends toward cathode, anode, electrolyte and separator are dedicatedly proposed. We envisage that this review would endow researchers a readily accessible means to rapidly acquaint with optimization strategies and design principles for advanced aqueous zinc-ion batteries. 

Optimization Strategies Toward Advanced Aqueous Zinc-ion Batteries: From Facing Key Issues to Viable Solutions

Aqueous zinc–ion batteries (ZIBs) have been promptly developed as a competitive and promising system for future large‐scale energy storage. In recent years, vanadium (V)‐based compounds, with diversity of valences and high electrochemical‐activity, have been widely studied as cathodes for aqueous ZIBs because of their rich reserves and high theoretical capacity. However, the stubborn issues including low conductivity and sluggish kinetics, plague their smooth application in aqueous ZIBs. Among various countermeasures, defect engineering is believed as an effective method to alleviate the above limitations. This review highlights the challenges of different V‐based cathode materials (e.g., vanadium oxides and vanadates) and summarizes the advances in defect engineering strategies including types and effects of the defects, designed strategies, and characterization techniques for high‐energy ZIBs. Finally, several sound prospects in this fervent field are also rationally proposed for fundamental research and practical application.

Advances on Defect Engineering of Vanadium‐Based Compounds for High‐Energy Aqueous Zinc–Ion Batteries

A surge of interest has been brought to all‐solid‐state batteries (ASSBs) as they show great prospects for enabling higher energy density and improved safety compared to conventional liquid batteries. Na Super Ionic CONductors (NaSICONs) proposed by Goodenough and Hong in 1976 are the most promising materials class for Na‐based ASSBs owing to their excellent ion conductivity (>1 mS cm−1), high thermal and chemical/electrochemical stability, as well as good chemical/electrochemical compatibility with electrode materials. The major challenge facing NaSICON‐type electrolytes is the generally high interfacial resistance and thus sluggish charge transfer kinetics across the NaSICON/cathode interface. Great endeavors in the past few years have led to progress in the improvement of the ion‐conducting property, and a dramatic decrease in the NaSICON/electrode interface resistance. Excellent cycling performance and rate capability have been achieved through interface engineering. In this review article, we summarize the state‐of‐the‐art findings for various derivatives of NaSICON structured solid electrolytes, with the aim of providing a deeper understanding of the underlying mechanism for the improvement of ion conductivity, and the intrinsic reasons for the enhanced interface charge transfer kinetics. These strategies can be readily extended to other solid electrolytes. We hope this review will inspire more work on NaSICON‐type solid electrolytes and solid‐state batteries.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/idm2.12044

NaSICON: A promising solid electrolyte for solid‐state sodium batteries

Highly active and stable amorphous IrOx/CeO2 nanowires for acidic oxygen evolution

All-solid-state batteries (ASSBs) based on metallic Na have received an upsurge of interest in the past few years owing to the low cost of Na resources combined with enhanced safety compared to conventional liquid lithium-ion batteries. Solid electrolytes (SEs) serve as the central of ASSBs as they, together with the composite cathode layer, largely determine the power density, energy density, and cycling performance of ASSBs. Among the several categories of SE materials, halides are considered one of the most promising candidates due to their favorable combination of high ionic conductivity and chemical/electrochemical stability against high-voltage cathode materials. Excellent examples have been demonstrated by lithium halides, while their sodium counterparts have been less explored. Herein, we evaluate the phase stability, electrochemical stability, and conducting property of a series of Na-based bromides Na3MBr6 with the joint utilization of density functional theory calculations, the bond valence site energy (BVSE) method, and ab initio molecular dynamics (AIMD) simulations. Our computations reveal that Na3MBr6 could crystallize in three structures, trigonal P3̅1c, monoclinic P21/n, and trigonal R3̅ phases, with the structural preference highly related to the type and ionic radii of the M cations. The BVSE and AIMD suggest that the P3̅1c phase exhibits a higher conductivity and lower migration barrier than P21/n and R3̅ phases. With the introduction of Na vacancies, a significant enhancement in the conductivity was achieved, giving rise to a high extrapolated conductivity of 0.70 mS cm–1 at room temperature. In addition, the thermodynamic stability and chemical stability against cathode materials were also assessed. Our work provides insights into the fundamental understanding of sodium bromides and points to the importance of this family of materials to be used as potential candidates for SE materials in ASSBs. 

Computational Screening of Na3MBr6 Compounds as Sodium Solid Electrolytes

Conversion-type cathodes for aqueous zinc ion batteries (ZIBs) can provide flat plateau slop and stable output potential, compared to general intercalation-type cathodes. The high volumetric capacity and stable output potential of Te make it a promising cathode for ZIBs, but sluggish kinetics and large volume change hinder its further application. To address these issues, we revisit fully-zinced ZnTe and construct ZnTe/rGO composites as the new conversion-type cathode. The electrode undergoes a solid-to-solid conversion reaction and shows a stable output potential with ultra-flat discharge plateau slop of 0.09 V (Ah g-1)-1. When ZnTe is de-zinced and transformed to Te during charge process, it has a volume shrinkage which generates empty space in graphene matrix for latter volume expansion of Te. The graphene matrix also improves conductivity and reaction kinetics of the cathode. Due to the combination of pre-zincation of ZnTe, graphene matrix and the elimination of "shuttle effects" process, ZnTe/rGO electrode exhibits a high and stable capacity of 186 mAh g-1 at 500 mA g-1 after 300 cycling, with almost no decay after initial 10 cycles.

ZnTe/rGO composite as the Fully-Zinced Conversion-Type Cathodes for Aqueous Zinc Ion Batteries.

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Advances on Defect Engineering of Vanadium‐Based Compounds for High‐Energy Aqueous Zinc–Ion Batteries

NaSICON: A promising solid electrolyte for solid‐state sodium batteries

Highly active and stable amorphous IrOx/CeO2 nanowires for acidic oxygen evolution

Computational Screening of Na3MBr6 Compounds as Sodium Solid Electrolytes

ZnTe/rGO composite as the Fully-Zinced Conversion-Type Cathodes for Aqueous Zinc Ion Batteries.