Atomic Bridging Structure of Nickel–Nitrogen–Carbon for Highly Efficient Electrocatalytic Reduction of CO2. Issue 6 (27th December 2021)

• Record Type: Journal Article
• Authors: Cao, Xueying; Zhao, Lanling; Wulan, Bari; Tan, Dongxing; Chen, Qianwu; Ma, Jizhen; Zhang, Jintao
• Is Part Of: Angewandte Chemie international edition. Volume 61:Issue 6(2022)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2021-12-27
• Subjects: Atomic Bridging Structure -- Electrocatalytic CO2 Reduction -- Nickel–Nitrogen–Carbon -- Zn−CO2 Electrochemical Cell; Chemistry -- Periodicals; 540
• DOI: 10.1002/anie.202113918
• Languages: English
• ISSNs: 1433-7851

Abstract

Abstract: To meet strategic applications, electrochemical reduction of CO2 into value‐added chemical molecules would be improved by the rational design of advanced electrocatalysts with atomically dispersed active sites. Herein an electrospun‐pyrolysis cooperative strategy is presented to not only modulate the porous structure of the carbon support for favorable charge and mass transfer, but also adjust the bridging structure of atomically dispersed metal species. Typically, the experimental results and theoretical calculations revealed that the unique chemical structure of binuclear nickel bridging with nitrogen and carbon atoms (namely Ni2 −N4 −C2 ) tunes the electronic nature of the d‐states for the optimal adsorption of carbon dioxide and intermediates, thus inducing the substantial enhancement of CO2 reduction via the thermodynamically more favorable pathway. The identification of such a structure demonstrates the large space to modulate the atomic bridging status for optimizing electrocatalysis. Abstract : The atomic bridging structure of nickel–nitrogen–carbon active sites confined in channel‐rich porous carbon fibers enables the highly efficient electrocatalytic reduction of CO2 .