文献类型： 外文期刊

作者： Li, Xiao ¹ ; Gan, Tao ² ; Gao, Xinhua ¹ ; Li, Bing ¹ ; Peng, Juan ¹ ; Ji, Yang ¹ ; Chen, Shenghua ³ ; Zhang, Jian ⁴ ; Zhang, Junjun ¹ ; Das, Pradip Kumar ⁵ ; Ramalingam, Vinoth ⁶ ; Zhang, Maolin ⁷ ; Zhang, Pengfei ¹ ; Peramaiah, Karthik ⁵ ; Qiu, Yajun ¹ ;

作者机构： 1.Ningxia Univ, Coll Chem & Chem Engn, State Key Lab High efficiency Utilizat Coal & Gree, Yinchuan 750021, Ningxia, Peoples R China

2.Chinese Acad Sci, Shanghai Adv Res Inst, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China

3.Xi An Jiao Tong Univ, Natl Innovat Platform Ctr Ind Educ Integrat Energy, Sch Chem, Xian 710049, Peoples R China

4.Wenzhou Univ, Coll Chem & Mat Engn, Key Lab Carbon Mat Zhejiang Prov, Key Lab Biohlth Mat & Chem Wenzhou, Wenzhou 325035, Zhejiang, Peoples R China

5.ASTAR, Inst Inst Sustainabil Chem Energy & Environm ISCE2, 1 Pesek Rd, Singapore 627833, Singapore

6.Robert Gordon Univ, Sch Comp Engn & Technol, Garthdee Rd, Aberdeen AB10 7GJ, Scotland

7.Chinese Acad Agr Sci, Inst Environm & Sustainable Dev Agr, Beijing 100081, Peoples R China

8.Shanghai Jiao Tong Univ, Sch Chem & Chem Engn, Shanghai 200240, Peoples R China

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.