Elucidating the Electrocatalytic CO2 Reduction Reaction over a Model Single‐Atom Nickel Catalyst. (10th December 2019)

• Record Type: Journal Article
• Authors: Liu, Song; Yang, Hong Bin; Hung, Sung‐Fu; Ding, Jie; Cai, Weizheng; Liu, Linghui; Gao, Jiajian; Li, Xuning; Ren, Xinyi; Kuang, Zhichong; Huang, Yanqiang; Zhang, Tao; Liu, Bin
• Is Part Of: Angewandte Chemie. Volume 132:Number 2(2020)
• Page Start: 808
• Page End: 813
• Publication Date: 2019-12-10
• Subjects: Aktive Zentren -- Einzelatomkatalyse -- Elektrochemie -- In-situ-Reaktionen -- Reaktionsmechanismen; Chemistry -- Periodicals; 540
• DOI: 10.1002/ange.201911995
• Languages: English
• ISSNs: 0044-8249

Abstract

Abstract: Designing effective electrocatalysts for the carbon dioxide reduction reaction (CO2 RR) is an appealing approach to tackling the challenges posed by rising CO2 levels and realizing a closed carbon cycle. However, fundamental understanding of the complicated CO2 RR mechanism in CO2 electrocatalysis is still lacking because model systems are limited. We have designed a model nickel single‐atom catalyst (Ni SAC) with a uniform structure and well‐defined Ni‐N4 moiety on a conductive carbon support with which to explore the electrochemical CO2 RR. Operando X‐ray absorption near‐edge structure spectroscopy, Raman spectroscopy, and near‐ambient X‐ray photoelectron spectroscopy, revealed that Ni + in the Ni SAC was highly active for CO2 activation, and functioned as an authentic catalytically active site for the CO2 RR. Furthermore, through combination with a kinetics study, the rate‐determining step of the CO2 RR was determined to be *CO2 − +H + →*COOH. This study tackles the four challenges faced by the CO2 RR; namely, activity, selectivity, stability, and dynamics. Abstract : Erfolgreicher Einzelgänger : Die In‐situ‐Reduktion von Nickel(II)‐2, 9, 16, 23‐tetra(amino)phthalocyanin, verankert auf der Oberfläche von Kohlenstoffnanoröhren, ergibt einzelne Nickelatome. Spektroskopische Messungen dieses Einzelatomkatalysators zeigen, dass Ni + ein hoch aktives katalytisches Zentrum für die Aktivierung und Reduktion von CO2 darstellt.