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, Edward H. Sargent*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

5 Scopus citations

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.

Original languageEnglish
Article number819
JournalNature Communications
Volume13
Issue number1
DOIs
StatePublished - Dec 2022

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