Highly Dispersed NiO Clusters Induced Electron Delocalization of NiNC Catalysts for Enhanced CO2 Electroreduction. (26th October 2022)

• Record Type: Journal Article
• Authors: Li, Hongqiang; Gan, Kaining; Li, Ran; Huang, Huawei; Niu, Jiabao; Chen, Zhipeng; Zhou, Jian; Yu, Yan; Qiu, Jieshan; He, Xiaojun
• Is Part Of: Advanced functional materials. Volume 33:Number 1(2023)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2022-10-26
• Subjects: CO 2 electroreductions -- Ni single‐atom catalysts -- NiO clusters -- electron delocalizations -- coal tar pitch; Materials -- Periodicals; Chemical vapor deposition -- Periodicals; 620.11
• DOI: 10.1002/adfm.202208622
• Languages: English
• ISSNs: 1616-301X

Abstract

Abstract: Oxygen‐regulated Ni‐based single‐atom catalysts (SACs) show great potential in accelerating the kinetics of electrocatalytic CO2 reduction reaction (CO2 RR). 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 CO2, 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. Abstract : NiO clusters‐decorated NiNC single‐atom catalysts show remarkable CO2 reduction reaction (CO2 RR) performance over a wide potential range. Even at a high overpotential of 1.19 V, NiO/NiNC‐800 exhibits a high CO production turnover frequency of 10120 h −1, which exceeds the value recently reported for MNC catalysts recently. The highly dispersed NiO clusters induce electron delocalization of NiNx sites and lower the reaction energy barrier for CO2 RR.