Electrochemical CO₂ reduction reaction (CO₂RR), powered by renewable electricity, has attracted great attention for producing high value-added fuels and chemicals, as well as feasibly mitigating CO₂ emission problem. Here, this work reports a facile hard template strategy to prepare the Ni@N-C catalyst with core–shell structure, where nickel nanoparticles (Ni NPs) are encapsulated by thin nitrogen-doped carbon shells (N-C shells). The Ni@N-C catalyst has demonstrated a promising industrial current density of 236.7 mA cm⁻² with the superb FE_CO of 97% at −1.1 V versus RHE. Moreover, Ni@N-C can drive the reversible Zn-CO₂ battery with the largest power density of 1.64 mW cm⁻², and endure a tough cycling durability. These excellent performances are ascribed to the synergistic effect of Ni@N-C that Ni NPs can regulate the electronic microenvironment of N-doped carbon shells, which favor to enhance the CO₂ adsorption capacity and the electron transfer capacity. Density functional theory calculations prove that the binding configuration of N-C located on the top of Ni slabs (Top-Ni@N-C) is the most thermodynamically stable and possess a lowest thermodynamic barrier for the formation of COOH^* and the desorption of CO. This work may pioneer a new method on seeking high-efficiency and worthwhile electrocatalysts for CO₂RR and Zn-CO₂ battery.

中文翻译：

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用于高效电化学 CO2 还原和水性 Zn-CO2 电池的超薄氮掺杂碳封装 Ni 纳米颗粒

以可再生电力为动力的电化学CO ₂还原反应(CO ₂ RR)因其生产高附加值燃料和化学品以及切实缓解CO ₂排放问题而受到广泛关注。在这里，这项工作报告了一种简便的硬模板策略来制备具有核壳结构的Ni@NC催化剂，其中镍纳米粒子（Ni NPs）被薄的氮掺杂碳壳（NC壳）封装。Ni@NC 催化剂表现出 236.7 mA cm ^-2的工业电流密度，在 -1.1 V（相对于 RHE）下具有 97% 的优异 FE _CO。此外，Ni@NC可以驱动可逆Zn-CO ₂电池，最大功率密度为1.64 mW cm^-2，并具有坚韧的循环耐久性。这些优异的性能归因于Ni@NC的协同效应，即Ni NPs可以调节N掺杂碳壳的电子微环境，有利于增强CO 2_吸附能力和电子传递能力。密度泛函理论计算证明，位于Ni板顶部的NC的结合构型（Top-Ni@NC）是热力学最稳定的，并且对于COOH * 的形成和CO的解吸具有最低的热力学势^垒。可能会开创一种寻找高效且有价值的CO ₂ RR和Zn-CO ₂电池电催化剂的新方法。