Synergy effects on Sn-Cu alloy catalyst for efficient CO2 electroreduction to formate with high mass activity (original) (raw)

Abstract

To acquire the synergy effects between Sn and Cu for the jointly high Faradaic efficiency and current density, we develop a novel strategy to design the Sn-Cu alloy catalyst via a decorated co-electrodeposition method for CO 2 electroreduction to formate. The Sn-Cu alloy shows high formate Faradaic efficiency of 82.3% ± 2.1% and total C 1 products Faradaic efficiency of 90.0% ± 2.7% at À1.14 V vs. reversible hydrogen electrode (RHE). The current density and mass activity of formate reach as high as (79.0 ± 0.4) mA cm À2 and (1490.6 ± 7.5) mA mg À1 at À1.14 V vs. RHE. Theoretical calculations suggest that Sn-Cu alloy can obtain high Faradaic efficiency for CO 2 electroreduction by suppressing the competitive hydrogen evolution reaction and that the formate formation follows the path of CO 2 ? HCOO* ? HCOOH. The stepped (2 1 1) surface of Sn-Cu alloy is beneficial towards selective formate production.

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  56. Ke Ye received his B.S. and M.S. degrees from Harbin Engineering University in 2009 and Ph.D. degree in Physical Chemistry from Hokkaido University (Japan) in 2013. At present, he is a postdoctoral researcher in Prof. Xinhe Bao's Group at Dalian Institute of Chemical Phy- sics, Chinese Academy of Sciences (DICP, CAS). His research interests include highly efficient electrocat- alytic materials and processes for electrochemical energy conversion and storage.
  57. Ang Cao received her Ph.D. degree at Tianjin University in 2018 and then joined in Prof. Xiao's group. At present, she is a postdoctoral researcher at Denmark Technology University in Jens Norskov's Group. She recently focuses on the theoretical study of CO 2 hydrogenation on noble metal and clusters.
  58. Jiaqi Shao is now a M.S. candidate at Harbin Engineering University and doing his dissertation research work at DICP, CAS under the supervision of Prof. Ke Ye and Prof. Guoxiong Wang. His research is focused on electro- chemical reduction reaction of carbon dioxide with metal and metal oxides.
  59. Jianping Xiao studied his Ph.D. degree at Bremen Center for Computational Materials Science, Universität Bre- men, from 2009 to 2013. Then, he spent two years as a postdoc fellow with Prof. Xinhe Bao at DICP, CAS. At the end of 2015, he joined the group led by Prof. Jens K. Nørskov at Stanford University. Since 2019, he has been appointed as full professor and group leader of Theo- retical Catalysis at DICP, CAS. His research interests include theoretical calculations for electrocatalysis and thermocatalysis.