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JOURNAL ARTICLE

On the Role of Sulfur for the Selective Electrochemical Reduction of CO 2 to Formate on CuS x Catalysts

Yilin Deng, Yun Huang, Dan Ren, Albertus D Handoko, Zhi Wei Seh, Pussana Hirunsit, Boon Siang Yeo
ACS Applied Materials & Interfaces 2018 August 29, 10 (34): 28572-28581
30125083
The efficient electroreduction of CO2 has received significant attention as it is one of the crucial means to develop a closed-loop anthropogenic carbon cycle. Here, we describe the mechanistic workings of an electrochemically deposited CuS x catalyst that can reduce CO2 to formate with a Faradaic efficiency (FEHCOO - ) of 75% and geometricĀ current density ( jHCOO - ) of -9.0 mA/cm2 at -0.9 V versus the reversible hydrogen electrode. At this potential, the formation of other CO2 reduction products such as hydrocarbons and CO was notably suppressed (total FE < 4%). The formate intermediate (HCOO*) was identified by operando Raman spectroscopy with isotopic labeling. A combination of electrochemical and materials characterization techniques revealed that the high selectivity toward formate production can be attributed to the effect of S dopants on the Cu catalyst, rather than surface morphology. Density functional theory calculations showed that the presence of sulfur weakens the HCOO* and *COOH adsorption energies, such that the formation of *COOH toward CO is suppressed, while the formation of HCOO* toward formate is favored.

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