Proton Capture Strategy for Enhancing Electrochemical CO2 Reduction on Atomically Dispersed Metal-Nitrogen Active Sites*

Xinyue Wang; Xiahan Sang; Chung-Li Dong; Siyu Yao; Ling Shuai; Jianguo Lu; Bin Yang; Zhongjian Li; Lecheng Lei; Ming Qiu; Liming Dai; Yang Hou

doi:10.1002/anie.202100011

Proton Capture Strategy for Enhancing Electrochemical CO₂ Reduction on Atomically Dispersed Metal-Nitrogen Active Sites*

Angew Chem Int Ed Engl. 2021 May 17;60(21):11959-11965. doi: 10.1002/anie.202100011. Epub 2021 Apr 12.

Authors

Xinyue Wang¹, Xiahan Sang², Chung-Li Dong³, Siyu Yao¹, Ling Shuai⁴, Jianguo Lu⁵, Bin Yang^{1

6}, Zhongjian Li^{1

6}, Lecheng Lei^{1

6}, Ming Qiu⁴, Liming Dai⁷, Yang Hou^{1

6}

Affiliations

¹ Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027, China.
² Nanostructure Research Center, Wuhan University of Technology, Wuhan, 430070, China.
³ Department of Physics, Tamkang University, New Taipei, 25137, Taiwan.
⁴ Institute of Nanoscience and Nanotechnology, College of Physical Science and Technology, Central China Normal University, Wuhan, 430079, China.
⁵ Department of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, China.
⁶ Institute of Zhejiang University-Quzhou, Quzhou, 324002, China.
⁷ Australian Carbon Materials Center (A-CMC), School of Chemical Engineering, University of New South Wales, Sydney, NSW, 2051, Australia.

PMID: 33599063
DOI: 10.1002/anie.202100011

Abstract

Electrocatalysts play a key role in accelerating the sluggish electrochemical CO₂ reduction (ECR) involving multi-electron and proton transfer. We now develop a proton capture strategy by accelerating the water dissociation reaction catalyzed by transition-metal nanoparticles (NPs) adjacent to atomically dispersed and nitrogen-coordinated single nickel (Ni-N_x ) active sites to accelerate proton transfer to the latter for boosting the intermediate protonation step, and thus the whole ECR process. Aberration-corrected scanning transmission electron microscopy, X-ray absorption spectroscopy, and calculations reveal that the Ni NPs accelerate the adsorbed H (H_ad ) generation and transfer to the adjacent Ni-N_x sites for boosting the intermediate protonation and the overall ECR processes. This proton capture strategy is universal to design and prepare for various high-performance catalysts for diverse electrochemical reactions even beyond ECR.

Keywords: dynamic understanding; electrochemical CO2 reduction; proton capture; single-atom catalysts.

Abstract

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