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Significant interest has emerged for the application of Pd-In2O3 catalysts as high-performance catalysts for CO2 hydrogenation to CH3OH. However, precise active site control in these catalysts and understanding their reaction mechanisms remain major challenges. In this investigation, a series of Pd-InOx catalysts were synthesized, revealing three distinct types of active sites: In-O, Pd-O(H)-In, and Pd2In3. Lower Pd loadings exhibited Pd-O(H)-In sites, while higher loadings resulted in Pd2In3 intermetallic compounds. These variations impacted catalytic performance, with Pd-O(H)-In catalysts showing heightened activity at lower temperatures due to the enhanced CO2 adsorption and H2 activation, and Pd2In3 catalysts performing better at elevated temperatures due to the further enhanced H2 activation. In situ DRIFTS studies revealed an alteration in key intermediates from *HCOO over In-O bonds to *COOH over Pd-O(H)-In and Pd2In3 sites, leading to a shift in the main reaction pathway transition and product distribution. Our findings underscore the importance of active site engineering for optimizing catalytic performance and offer valuable insights for the rational design of efficient CO2 conversion catalysts. [ABSTRACT FROM AUTHOR]

High‐voltage spinel‐type structured LiNi0.5Mn1.5O4 (LNMO) shows promise as a next‐generation high‐energy‐density lithium‐ion battery cathode material, however, capacity decay on extended cycling hinders its widespread adoption, underscoring an urgent need for further development. In this work, we introduce Zn at octahedral 16c crystal sites in LNMO with Fd3‾ ${\bar{3}}$ m space group to improve rate capability and reduce the rapid capacity decay otherwise experienced during extended cycling. The current work resolves the detailed influence of isolated modification at octahedral 16c crystal sites, unveiling the mechanism for these performance improvements. We show that occupation of Zn at previously empty 16c sites prevents the migration of Ni/Mn to adjacent 16c sites, eliminating transformation to a rock‐salt type structured Ni0.25Mn0.75O2 phase above 4.8 V, preventing structure degradation and suppressing voltage polarization. This study provides insights into the fundamental structure‐function relationship of the LNMO battery cathode, pointing to pathways for the crystal structure engineering of materials with superior performance. [ABSTRACT FROM AUTHOR]

Sluggish kinetics of the CO2 reduction/evolution reactions lead to the accumulation of Li2CO3 residuals and thus possible catalyst deactivation, which hinders the long-term cycling stability of Li-CO2 batteries. Apart from catalyst design, constructing a fluorinated solid-electrolyte interphase is a conventional strategy to minimize parasitic reactions and prolong cycle life. However, the catalytic effects of solid-electrolyte interphase components have been overlooked and remain unclear. Herein, we systematically regulate the compositions of solid-electrolyte interphase via tuning electrolyte solvation structures, anion coordination, and binding free energy between Li ion and anion. The cells exhibit distinct improvement in cycling performance with increasing content of C-N species in solid-electrolyte interphase layers. The enhancement originates from a catalytic effect towards accelerating the Li2CO3 formation/decomposition kinetics. Theoretical analysis reveals that C-N species provide strong adsorption sites and promote charge transfer from interface to *CO22− during discharge, and from Li2CO3 to C-N species during charge, thereby building a bidirectional fast-reacting bridge for CO2 reduction/evolution reactions. This finding enables us to design a C-N rich solid-electrolyte interphase via dual-salt electrolytes, improving cycle life of Li-CO2 batteries to twice that using traditional electrolytes. Our work provides an insight into interfacial design by tuning of catalytic properties towards CO2 reduction/evolution reactions. Sluggish kinetics of the CO2 reactions lead to the accumulation of Li2CO3 residuals, which hinders the cycling stability of Li-CO2 batteries. Here, the authors reveal the catalytic role of in-situ formed C-N species in enhancing the reversibility of Li2CO3 and cycle life of Li-CO2 batteries. [ABSTRACT FROM AUTHOR]

Growth in intermittent renewable sources including solar and wind has sparked increasing interest in electrical energy storage. Grid‐scale energy storage integrated with renewable sources has significant advantages in energy regulation and grid security. Aqueous zinc‐ion batteries (AZIBs) have emerged as a practically attractive option for electrical storage because of environmentally benign aqueous‐based electrolytes, high theoretical capacity of Zn anode, and significant global reserves of Zn. However, application of AZIBs at the grid‐scale is restricted by drawbacks in cathode material(s). Herein, a comprehensive summary of the features and storage mechanisms of the latest cathode materials is provided. The fundamental problems and corresponding in‐depth causes for cathode materials is critically reviewed. It is also assess practical challenges, appraise their translation to commerce and industry, and systematically summarize and discuss the potential solutions reported in recent works. It is established necessary design strategies for Zn anodes and electrolytes that are matched with cathode materials for commercializing AZIBs. Finally, it is concluded with a perspective on the practical prospects for advancing the development of future AZIBs. Findings will be of interest and benefit to a range of researchers and manufacturers in the design and application of AZIBs for grid‐scale energy storage. [ABSTRACT FROM AUTHOR]