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It is still a challenge to develop electrocatalyst for the efficient adsorption and conversion of organic molecule in aqueous media. Herein, a hetero‐interface structure based on CuO@Ni(OH)2 is rationally designed to enhance the performance of benzyl alcohol oxidation to benzoic acid. A high Faradaic efficiency of 99% and the yield of 3.09 mmol cm−2 h−1 are achieved at 1.70 V versus reversible hydrogen electrode, outperforming the previously reported electrocatalysts. Furthermore, a membrane‐free flow electrolyzer was assembled based on CuO@Ni(OH)2 hetero‐interface, exhibiting a much high yielding of benzoic acid (6.73 mmol cm−2 h−1) and hydrogen (0.35 L cm−2 h−1) with excellent stability. Both experimental data and density functional theory calculations verify that the electron is tend to accumulate at the hetero‐interface, thus accelerating the adsorption of reactant and intermediate and reducing the energy barrier of the conversion of benzyl alcohol to benzoic acid. [ABSTRACT FROM AUTHOR]

Sustainable energy-powered carbon dioxide (CO2) electroreduction into methane (CH4) under ambient conditions holds great promise for achieving carbon neutrality and mitigating environmental pollution. Despite the significant advancements in this field, the unsatisfactory selectivity and stability remain the major obstacles to its large-scale applications. With this background, we present a comprehensive summary of recent progress and future opportunities of CO2 electroreduction into CH4. Firstly, we delve into the elucidation of the reaction mechanism involved in CO2 electroreduction into CH4. A thorough understanding of the individual steps within this process is paramount for designing electrocatalysts and improving selectivity and efficiency. In particular, the development of advanced electrocatalysts (such as copper-based materials, carbon-based materials and other materials) for CO2 electroreduction into CH4 is elaborated. Meanwhile, a special focus has been placed on the enhanced strategies, including coordination environment manipulation, element doping, surface modification, and morphology engineering, for CO2 electroreduction into CH4. Finally, the future challenges of CO2 electroreduction into CH4 are proposed. The review aims to serves as a guiding framework for systematic exploration and optimization of electrocatalysts, thus fostering the development and advancement of CO2 electroreduction into CH4. [ABSTRACT FROM AUTHOR]

Single‐atom catalysts (SACs) exhibit intriguing performance in electrocatalysis owing to their maximized atom utilizations and unique electronic structures, but effective anchoring metal atoms with defined coordination structure on hierarchical integrated electrode remain a challenge. Herein, a fast and facial flame‐assisted strategy is developed to construct oxygen‐coordinated SACs on integrated carbon nanotube (CNT) arrays with promising applications in electrocatalysis. Density functional theory calculations show that oxygen in carbon substrate imparts homogeneous sites for the efficient anchoring of metal atoms, thereby enabling SACs to disperse uniformly and firmly and thus bringing optimized activities. Moreover, the integrated CNT array with abundant oxygen‐containing groups is constructed and has been used as an efficient matrix for anchoring metal atoms (CNT‐O@M) via a flame‐assisted method. The as‐prepared CNT‐O@M (M = Co and Pt as typical examples) shows excellent activities in electrocatalytic oxygen reduction reaction and hydrogen evolution reaction with utilization of active site as high as 75.7%, which is superior to the reported SACs. Particularly, the performance of CNT‐O@M can maintain stably under various harsh conditions, showing a promising prospect in the long‐time applications. The methodology and concept proposed in this work could be extended to the synthesis of a variety of integrated SACs for efficient electrocatalysis. [ABSTRACT FROM AUTHOR]

The development of efficient electrocatalysts for the CO2 reduction reaction (CO2RR) remains a challenge. Demonstrated here is a NiSn atomic‐pair electrocatalyst (NiSn‐APC) on a hierarchical integrated electrode, which exhibits a synergistic effect in simultaneously promoting the activity and selectivity of the CO2RR to formate. The NiSn atomic pair consists of adjacent Ni and Sn, each coordinated with four nitrogen atoms (N4‐Ni‐Sn‐N4). The as‐prepared NiSn‐APC displays exceptional activity for the CO2RR to formate with a turnover frequency of 4752 h−1, a formate productivity of 36.7 mol h−1 gSn−1 and an utilization degree of active sites (57.9 %), which are superior to previously reported single‐atomic catalysts. Both experimental data and density‐functional theory calculations verify the electron redistribution of Sn imposed by adjacent Ni, which reduces the energy barrier of the *OCHO intermediate and makes this potential‐determining step thermodynamically spontaneous. This synergistic catalysis provides a successful paradigm for rational design and preparation of atomic‐pair electrocatalysts with enhanced performance. [ABSTRACT FROM AUTHOR]

Highly efficient and low‐cost electrodes have a key role in the development of advanced energy devices such as fuel cells and metal–air batteries. However, electrode performance is typically limited by low utilization of active sites, which causes a considerable drop in energy density. To overcome this issue, a single‐atom‐containing integrated electrode is developed through a confinement synthesis strategy by using organic molecule‐intercalated layered double hydroxides (LDHs) as precursors. The as‐prepared integrated electrode has a well‐defined nanosheet array structure with a homogeneous anchored single atomic Co catalyst and many exposed hierarchical pores. Moreover, the coordination environment of single atoms (CoN or CoS) is precisely controlled by regulating the type of interlayer molecules in the LDHs. Consequently, the optimized electrode exhibits high bifunctional activity toward both the oxygen reduction and oxygen evolution reactions. This electrode is directly assembled into an all‐solid‐state zinc–air battery that showed outstanding flexibility and long‐term charge/discharge stability. Because of the versatility of LDH materials, it is expected that the proposed strategy can be extended to the construction of other integrated electrodes for high‐performance energy storage and conversion devices. [ABSTRACT FROM AUTHOR]