Theory-guided Sn/Cu alloying for efficient CO2 electroreduction at low overpotentials

Zheng, Xueli; Ji, Yongfei; Tang, Jing; Wang, Jiangyan; Liu, Bofei; Steinrück, Hans-Georg; Lim, Kipil; Li, Yuzhang; Toney, Michael F.; Chan, Karen; Cui, Yi

doi:10.1038/s41929-018-0200-8

Title: Theory-guided Sn/Cu alloying for efficient CO₂ electroreduction at low overpotentials

Journal Article · 16 December 2018 · Nature Catalysis

DOI: https://doi.org/10.1038/s41929-018-0200-8 · OSTI ID:1493352

^[1]; Ji, Yongfei ^[2]; Tang, Jing ^[1]; Wang, Jiangyan ^[1]; Liu, Bofei ^[1]; Steinrück, Hans-Georg ^[3]; Lim, Kipil ^[2]; Li, Yuzhang ^[1]; Toney, Michael F. ^[3];

^[3]; Cui, Yi ^[2]

Stanford Univ., Stanford, CA (United States)
Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States)

Here, electrochemical CO₂ reduction to formate provides an avenue to reduce globally accelerating CO₂ emissions and produce value-added products. Unfortunately, high selectivity in formate electrosynthesis has thus far only been achieved at highly cathodic potentials. Here we use density functional theory to investigate the effect of alloying Cu and Sn on the activity and selectivity towards formate. A theoretical thermodynamic analysis of the reaction energetics suggests that the incorporation of copper into tin could suppress hydrogen evolution and CO production, thus favouring formate generation. Consistent with theoretical trends, the designed CuSn₃ catalysts by co-electrodeposition exhibit a Faradaic efficiency of 95% towards formate generation at –0.5 V versus RHE. Furthermore, the catalysts show no degradation over 50 h of operation. In situ Sn L₃-edge and Cu K-edge X-ray absorption spectroscopy indicate electron donation from Sn to Cu, which indicates positive oxidation states of Sn in CuSn₃ under operating conditions.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1493352

Alternate ID(s):: OSTI ID: 1603144

Journal Information:: Nature Catalysis, Journal Name: Nature Catalysis Journal Issue: 1 Vol. 2; ISSN 2520-1158

Publisher:: Springer NatureCopyright Statement

Country of Publication:: United States

Language:: English

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