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Promoting CO 2 methanation via ligand-stabilized metal oxide clusters as hydrogen-donating motifs.

Research paper by Yuhang Y Li, Aoni A Xu, Yanwei Y Lum, Xue X Wang, Sung-Fu SF Hung, Bin B Chen, Ziyun Z Wang, Yi Y Xu, Fengwang F Li, Jehad J Abed, Jianan Erick JE Huang, Armin Sedighian AS Rasouli, Joshua J Wicks, Laxmi Kishore LK Sagar, Tao T Peng, et al.

Indexed on: 05 Dec '20Published on: 05 Dec '20Published in: Nature communications



Abstract

Electroreduction uses renewable energy to upgrade carbon dioxide to value-added chemicals and fuels. Renewable methane synthesized using such a route stands to be readily deployed using existing infrastructure for the distribution and utilization of natural gas. Here we design a suite of ligand-stabilized metal oxide clusters and find that these modulate carbon dioxide reduction pathways on a copper catalyst, enabling thereby a record activity for methane electroproduction. Density functional theory calculations show adsorbed hydrogen donation from clusters to copper active sites for the *CO hydrogenation pathway towards *CHO. We promote this effect via control over cluster size and composition and demonstrate the effect on metal oxides including cobalt(II), molybdenum(VI), tungsten(VI), nickel(II) and palladium(II) oxides. We report a carbon dioxide-to-methane faradaic efficiency of 60% at a partial current density to methane of 135 milliampere per square centimetre. We showcase operation over 18 h that retains a faradaic efficiency exceeding 55%.