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

• Published in: Nature communications Vol. 10; no. 1; pp. 2980 - 8
• Main Authors: Zhang, Bingxing, Zhang, Jianling, Shi, Jinbiao, Tan, Dongxing, Liu, Lifei, Zhang, Fanyu, Lu, Cheng, Su, Zhuizhui, Tan, Xiuniang, Cheng, Xiuyan, Han, Buxing, Zheng, Lirong, Zhang, Jing
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 05.07.2019; Nature Publishing Group; Nature Portfolio
• Subjects: 140/131; 140/146; 140/58; 147/135; 147/137; 147/143; 147/28; 147/3; 639/301/299/886; 639/638/549/884; 639/925/357; Carbon dioxide; Density functional theory; Electrocatalysts; Electronic structure; Free energy; Heavy metals; Humanities and Social Sciences; Manganese; multidisciplinary; Reduction; Reduction (metal working); Science; Science (multidisciplinary); X ray absorption
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-019-10854-1

Developing highly efficient electrocatalysts based on cheap and earth-abundant metals for CO 2 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 CO 2 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 CO 2 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 CO 2 reduction performance. While renewable CO 2 conversion provides a means to remove and recycle waste emissions, there are few earth-abundant materials that are both efficient and active. Here, authors prepare N-doped carbon with atomic manganese as high-performance CO 2 reduction electrocatalyst.