Directed Structural Evolution of Nickel Nanoparticles into Atomically Dispersed Sites for Efficient CO2 Electroreduction.

文献类型： 外文期刊

第一作者： Li, Xiao

作者： Li, Xiao;Gao, Xinhua;Li, Bing;Peng, Juan;Ji, Yang;Zhang, Junjun;Zhang, Pengfei;Qiu, Yajun;Gan, Tao;Chen, Shenghua;Zhang, Jian;Das, Pradip Kumar;Peramaiah, Karthik;Ramalingam, Vinoth;Zhang, Maolin;Zhang, Pengfei

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关键词： activation; CO2 electroreduction; improved active sites density; Ni single-atom; structural evolution

期刊名称：SMALL （ 影响因子：12.1； 五年影响因子：12.5 ）

ISSN： 1613-6810

年卷期： 2025 年

页码：

收录情况： SCI

摘要： Electrochemical CO2 reduction (CO2RR) to carbon monoxide (CO) offers a sustainable pathway for carbon utilization, yet challenges remain in terms of improving selectivity and activity. Herein, we report a Ni/NC catalyst synthesized via a milling - pyrolysis method, in which Ni particles anchored on nitrogen-doped carbon (NC) are electrochemically activated under an Ar atmosphere, leading to their structural evolution into single-atom Ni sites. After activation in Ar atmosphere, the current density nearly doubles (from approximate to 30 to approximate to 60 mA cm-2), and concurrently, the Faradaic efficiency of CO stays at similar to 90% with the potential set to -0.8 V vs. RHE. Comprehensive characterizations, including X-ray photoelectron spectroscopy (XPS), aberration - corrected scanning transmission electron microscopy (AC - STEM), along with extended X - ray absorption fine structure (EXAFS), confirm the change of Ni particles into atomically dispersed Ni-Nx moieties during activation. Notably, in situ Raman spectroscopy identifies *COOH as the key intermediate, while electrochemical analyses reveal accelerated charge transfer and favorable kinetics for Ar-Ni/NC. Additionally, the catalyst shows great selectivity and stability over 24 hours of non - stop operation. This study emphasizes the dynamic change of Ni active sites under working conditions, offering useful ideas for designing transition metal catalysts for large - scale CO2 to CO conversion.

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