A metal-supported single-atom catalytic site enables carbon dioxide hydrogenation

Sung-Fu Hung, Aoni Xu, Xue Wang, Fengwang Li, Shao-Hui Hsu, Yuhang Li, Joshua Wicks, Eduardo González Cervantes, Armin Sedighian Rasouli, Yuguang C. Li, Mingchuan Luo, Dae-Hyun Nam, Ning Wang, Tao Peng, Yu Yan, Geonhui Lee and Edward H. Sargent ()
Additional contact information
Sung-Fu Hung: University of Toronto
Aoni Xu: University of Toronto
Xue Wang: University of Toronto
Fengwang Li: University of Toronto
Shao-Hui Hsu: National Applied Research Laboratories
Yuhang Li: University of Toronto
Joshua Wicks: University of Toronto
Eduardo González Cervantes: University of Toronto
Armin Sedighian Rasouli: University of Toronto
Yuguang C. Li: University of Toronto
Mingchuan Luo: University of Toronto
Dae-Hyun Nam: University of Toronto
Ning Wang: University of Toronto
Tao Peng: University of Toronto
Yu Yan: University of Toronto
Geonhui Lee: University of Toronto
Edward H. Sargent: University of Toronto

Nature Communications, 2022, vol. 13, issue 1, 1-9

Abstract: Abstract Nitrogen-doped graphene-supported single atoms convert CO2 to CO, but fail to provide further hydrogenation to methane – a finding attributable to the weak adsorption of CO intermediates. To regulate the adsorption energy, here we investigate the metal-supported single atoms to enable CO2 hydrogenation. We find a copper-supported iron-single-atom catalyst producing a high-rate methane. Density functional theory calculations and in-situ Raman spectroscopy show that the iron atoms attract surrounding intermediates and carry out hydrogenation to generate methane. The catalyst is realized by assembling iron phthalocyanine on the copper surface, followed by in-situ formation of single iron atoms during electrocatalysis, identified using operando X-ray absorption spectroscopy. The copper-supported iron-single-atom catalyst exhibits a CO2-to-methane Faradaic efficiency of 64% and a partial current density of 128 mA cm−2, while the nitrogen-doped graphene-supported one produces only CO. The activity is 32 times higher than a pristine copper under the same conditions of electrolyte and bias.

Date: 2022
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DOI: 10.1038/s41467-022-28456-9

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