Details

Autor(en) / Beteiligte

• 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

Titel

Elucidating the Electrocatalytic CO2 Reduction Reaction over a Model Single‐Atom Nickel Catalyst

Ist Teil von

• Angewandte Chemie (International ed.), 2020-01, Vol.59 (2), p.798-803

Auflage

International ed. in English

Ort / Verlag

Weinheim: Wiley Subscription Services, Inc

Erscheinungsjahr

2020

Link zum Volltext

Quelle

Alma/SFX Local Collection

Beschreibungen/Notizen

• Designing effective electrocatalysts for the carbon dioxide reduction reaction (CO2RR) 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 CO2RR 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 CO2RR. 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 CO2RR. Furthermore, through combination with a kinetics study, the rate‐determining step of the CO2RR was determined to be *CO2−+H+→*COOH. This study tackles the four challenges faced by the CO2RR; namely, activity, selectivity, stability, and dynamics. Ni‐che reaction: In situ reduction of nickel(II) 2,9,16,23‐tetra(amino)phthalocyanine, anchored on the surface of carbon nanotubes, yields nickel single atoms. Advanced spectroscopy of the single‐atom catalyst reveals that Ni+ is a highly active catalytic site for CO2 activation and reduction.