Manganese acting as a high-performance heterogeneous electrocatalyst in carbon dioxide reduction

Bingxing Zhang, Jianling Zhang (), Jinbiao Shi, Dongxing Tan, Lifei Liu, Fanyu Zhang, Cheng Lu, Zhuizhui Su, Xiuniang Tan, Xiuyan Cheng, Buxing Han, Lirong Zheng and Jing Zhang
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Bingxing Zhang: Chinese Academy of Sciences
Jianling Zhang: Chinese Academy of Sciences
Jinbiao Shi: Chinese Academy of Sciences
Dongxing Tan: Chinese Academy of Sciences
Lifei Liu: Chinese Academy of Sciences
Fanyu Zhang: Chinese Academy of Sciences
Cheng Lu: Chinese Academy of Sciences
Zhuizhui Su: Chinese Academy of Sciences
Xiuniang Tan: Chinese Academy of Sciences
Xiuyan Cheng: Chinese Academy of Sciences
Buxing Han: Chinese Academy of Sciences
Lirong Zheng: Chinese Academy of Sciences
Jing Zhang: Chinese Academy of Sciences

Nature Communications, 2019, vol. 10, issue 1, 1-8

Abstract: Abstract Developing highly efficient electrocatalysts based on cheap and earth-abundant metals for CO2 reduction is of great importance. Here we demonstrate that the electrocatalytic activity of manganese-based heterogeneous catalyst can be significantly improved through halogen and nitrogen dual-coordination to modulate the electronic structure of manganese atom. Such an electrocatalyst for CO2 reduction exhibits a maximum CO faradaic efficiency of 97% and high current density of ~10 mA cm−2 at a low overpotential of 0.49 V. Moreover, the turnover frequency can reach 38347 h−1 at overpotential of 0.49 V, which is the highest among the reported heterogeneous electrocatalysts for CO2 reduction. In situ X-ray absorption experiment and density-functional theory calculation reveal the modified electronic structure of the active manganese site, on which the free energy barrier for intermediate formation is greatly reduced, thus resulting in a great improvement of CO2 reduction performance.

Date: 2019
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DOI: 10.1038/s41467-019-10854-1

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