In:
Nature Communications, Springer Science and Business Media LLC, Vol. 10, No. 1 ( 2019-07-05)
Abstract:
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.
Type of Medium:
Online Resource
ISSN:
2041-1723
DOI:
10.1038/s41467-019-10854-1
Language:
English
Publisher:
Springer Science and Business Media LLC
Publication Date:
2019
detail.hit.zdb_id:
2553671-0