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

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

Nature communications (2019-07-07)
Bingxing Zhang, Jianling Zhang, Jinbiao Shi, Dongxing Tan, Lifei Liu, Fanyu Zhang, Cheng Lu, Zhuizhui Su, Xiuniang Tan, Xiuyan Cheng, Buxing Han, Lirong Zheng, Jing Zhang
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.