TY - JOUR
T1 - Understanding the Roles of Hydroxide in CO2Electroreduction on a Cu Electrode for Achieving Variable Selectivity
AU - Sun, Mingxu
AU - Staykov, Aleksandar
AU - Yamauchi, Miho
N1 - Funding Information:
The authors acknowledge funding from JST (JPMJFS2132), JSPS KAKENHI (JP18H05517 “Hydrogenomics” and 22K19088), and the Moonshot Research and Development Program (JPNP18016)
Publisher Copyright:
© 2022 American Chemical Society.
PY - 2022
Y1 - 2022
N2 - Hydroxide-derived copper (OH/Cu) electrodes exhibit excellent performance for the electrocatalytic CO2 reduction reaction (CO2RR). However, the role of hydroxide (OH) in CO2RR remains controversial; therefore, the origin of the selectivity enhancement emerging on OH/Cu has not been fully understood. In the present work, we quantitatively evaluated surface OH by electroadsorption and established a direct correlation between the OH amount and selectivity for the production of CH4 and C2+ on OH/Cu with the help of computational investigations concerning work functions of the surface. Based on these findings, we demonstrated variable selectivity using OH/Cu electrodes having a controlled OH amount; three OH/Cu electrodes realized their distinct selectivity such as Faradic efficiency (FE) for the production of CH4 (CH4 FE) of 78%, C2+ FE of 71%, and the ratio of C2+-to-CH4 >355. The proposed simple strategy for selectivity control would contribute to further quantity synthesis of value-added chemicals using CO2RR.
AB - Hydroxide-derived copper (OH/Cu) electrodes exhibit excellent performance for the electrocatalytic CO2 reduction reaction (CO2RR). However, the role of hydroxide (OH) in CO2RR remains controversial; therefore, the origin of the selectivity enhancement emerging on OH/Cu has not been fully understood. In the present work, we quantitatively evaluated surface OH by electroadsorption and established a direct correlation between the OH amount and selectivity for the production of CH4 and C2+ on OH/Cu with the help of computational investigations concerning work functions of the surface. Based on these findings, we demonstrated variable selectivity using OH/Cu electrodes having a controlled OH amount; three OH/Cu electrodes realized their distinct selectivity such as Faradic efficiency (FE) for the production of CH4 (CH4 FE) of 78%, C2+ FE of 71%, and the ratio of C2+-to-CH4 >355. The proposed simple strategy for selectivity control would contribute to further quantity synthesis of value-added chemicals using CO2RR.
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U2 - 10.1021/acscatal.2c03650
DO - 10.1021/acscatal.2c03650
M3 - Article
AN - SCOPUS:85142623371
SP - 14856
EP - 14863
JO - ACS Catalysis
JF - ACS Catalysis
SN - 2155-5435
ER -