Electrochemical reduction of carbon dioxide with nearly 100% carbon monoxide faradaic efficiency from vacancy-stabilized single-atom active sites

Chenbao Lu, Kaiyue Jiang, Diana Tranca, Ning Wang, Hui Zhu, Fermin Rodriguez-Hernandez, Zhenying Chen, Chongqing Yang, Fan Zhang, Yuezeng Su, Changchun Ke, Jichao Zhang, Yu Han, Xiaodong Zhuang

Research output: Contribution to journalArticlepeer-review

31 Scopus citations

Abstract

Single-atom catalysts (SACs) have been rapidly rising as emerging materials in the field of energy conversion, especially for CO2 reduction reaction. However, the selectivity and running current are still beyond practical applications. Herein, we report new unsaturated SACs with CO2 to CO selectivity of nearly 100% at 51 mA cm−2, and 91% at 100 mA cm−2. Such unsaturated SACs (M-Nx, M = Ni, Fe and Co, x < 4) are rationally prepared through a novel CO2-to-carbon process in large quantity and confirmed by X-ray absorption spectroscopy. As electrocatalysts for CO2 reduction, unsaturated Ni–N2 centered SACs exhibit outstanding activity for CO2 reduction, outperforming state-of-the-art unsaturated SACs. Operando X-ray absorption spectroscopy and theoretical calculation reveal that such unsaturated Ni sites with rich vacancies are favorable for production of more unpaired 3d electrons, and consequently reduce the free energy for COOH* formation, therefore boosting CO2 reduction performance. Not only does this work provide a new method towards unsaturated SACs in large quantity, but also contributes fundamental understanding of the unsaturated single-atom sites in electrochemical catalysis.
Original languageEnglish (US)
JournalJOURNAL OF MATERIALS CHEMISTRY A
DOIs
StatePublished - 2021

Bibliographical note

KAUST Repository Item: Exported on 2021-11-15
Acknowledgements: This work was financially supported by NSFC (51973114, 21720102002, 51811530013), National Key Research and Development Program of China (2017YFE9134000), and Science and Technology Commission of Shanghai Municipality (19JC412600). J. Zhang is grateful for the financial support from NSFC (11705270, 11975100). C. Ke is grateful for the financial support from NSFC (21406220) and the Key Science and Technology Project in Henan Province (Innovation Leading Project: 191110210200). The authors are grateful for the support from
Instrumental Analysis Center, Center for High Performance Computing at Shanghai Jiao Tong University, and the beamline BL14W1 and BL15U1 of the Shanghai Synchrotron Radiation Facility (SSRF, China) for providing beam time.

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