摘要
Bismuth-based materials are prevalent catalysts for CO_(2)electroreduction to formate,enduring high hydrogen evolution reactions and inadequate activity and stability.Herein,we reveal that in-situ electrochemical transformation of Cu_(2)BiS_(x)solid solution into Bi/Cu_(x)S_(y)heterointerfaces,which can stabilize the intermediates and achieve highly selective and consistent CO_(2)electroreduction.It shows over 85%Faraday efficiency(FE)of formate with a potential window of−0.8 to−1.2 VRHE(RHE:reversible hydrogen electrode)and a stability above 90%over 27 h in H-type cell at−0.9 VRHE.It maintains more than 85%of FEformate at the current density of−25 to−200 mA·cm^(−2),has stability of about 80%of FEformate at least 10 h at−150 mA·cm^(−2)in flow cell.In-situ Fourier transform infrared(FT-IR)spectroscopy measurement confirms that the preferred route of catalytic reaction is to generate *CO_(2)^(−) and *OCHO intermediates.The density functional theory(DFT)calculations illustrate that heterointerfaces facilitate the prior process of CO_(2)to HCOOH through *OCHO by additional Bi hybrid orbitals.This study is expected to open up a new idea for the design of CO_(2)electroreduction catalyst.
基金
the National Natural Science Foundation of China(Nos.21871005 and 22171005)
the University Synergy Innovation Program of Anhui Province(Nos.GXXT-2020-005,GXXT-2021-012,and GXXT-2021-013).
