Highly Dispersed NiO Clusters Induced Electron Delocalization of Ni-N-C Catalysts for Enhanced CO_2 Electroreduction

Hongqiang Li; Kaining Gan; Ran LiHuawei HuangJiabao NiuZhipeng ChenJian ZhouYan YuJieshan QiuXiaojun He

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Highly Dispersed NiO Clusters Induced Electron Delocalization of Ni-N-C Catalysts for Enhanced CO_2 Electroreduction

机译：Highly Dispersed NiO Clusters Induced Electron Delocalization of Ni-N-C Catalysts for Enhanced CO_2 Electroreduction

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Oxygen-regulated Ni-based single-atom catalysts (SACs) show great potential in accelerating the kinetics of electrocatalytic CO_2 reduction reaction (CO_2RR). However, it remains a challenge to precisely control the coordination environment of Ni-O moieties and achieve high activity at high overpotentials. Herein, a facile carbonization coupled oxidation strategy is developed to mass produce NiO clusters-decorated Ni-N-C SACs that exhibit a high Faradaic efficiency of CO (maximum of 96.5%) over a wide potential range (?0.9 to ?1.3 V versus reversible hydrogen electrode) and a high turnover frequency for CO production of 10 120 h?1 even at the high overpotential of 1.19 V. Density functional theory calculations reveal that the highly dispersed NiO clusters induce electron delocalization of active sites and reduce the energy barriers for *COOH intermediates formation from CO_2, leading to an enhanced reaction kinetics for CO production. This study opens a new universal pathway for the construction of oxygen-regulated metal-based SACs for various catalytic applications.

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《Advanced functional materials》 |2023年第1期|2208622.1-2208622.10|共10页
作者
Hongqiang Li; Kaining Gan; Ran LiHuawei HuangJiabao NiuZhipeng ChenJian ZhouYan YuJieshan QiuXiaojun He;
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College of Chemical Engineering State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical Technology Beijing 100029, P. R. China;

School of Chemistry and Chemical Engineering Anhui Key Laboratory of Coal Clean Conversion and High Valued Utilization Key Laboratory of Metallurgical Emission Reduction & Resources Recycling Ministry of Education Anhui University of Technology Maanshan 2;

KAUST Catalysis Center (KCC) King Abdullah University of Science and Technology (KAUST) Thuwal 23955–6900, Kingdom of Saudi ArabiaHefei National Laboratory for Physical Sciences at the Microscale Department of Materials Science and Engineering, National Synchrotron Radiation Laboratory CAS Key Laboratory of Materials for Energy Conversion University of Science and Technology of Chin;

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正文语种英语
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CO_2 electroreductions; Ni single-atom catalysts; NiO clusters; electron delocalizations; coal tar pitch;

Highly Dispersed NiO Clusters Induced Electron Delocalization of Ni-N-C Catalysts for Enhanced CO_2 Electroreduction

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