Hydrophobic Copper Interfaces Boost Electroreduction of Carbon Dioxide to Ethylene in Water

TY - JOUR

T1 - Hydrophobic Copper Interfaces Boost Electroreduction of Carbon Dioxide to Ethylene in Water

AU - Liang, Hong Qing

AU - Zhao, Siqi

AU - Hu, Xin Ming

AU - Ceccato, Marcel

AU - Skrydstrup, Troels

AU - Daasbjerg, Kim

N1 - Funding Information: We thank the Danish National Research Foundation (grant no. DNRF118) for generous financial support. X.-M.H. acknowledges the support of the “Qilu Young Scholars” program from Shandong University. We are grateful to Associate Professor Steen U. Pedersen for fruitful discussions. Publisher Copyright: © 2021 American Chemical Society. Copyright: Copyright 2021 Elsevier B.V., All rights reserved.

PY - 2021/1

Y1 - 2021/1

N2 - Cu is in the spotlight as it represents the only metal capable of catalyzing CO2 reduction to multicarbon products. However, its catalytic performance is determined collectively by a number of parameters including its composition and structure, electrolyte, and cell configuration. It remains a challenge to disentangle and understand the individual effect of these parameters. In this work, we study the effect of the electrode-electrolyte interface on CO2 reduction in water by coating CuO electrodes with polymers of varying hydrophilicities/phobicities. Hydrophilic polymers such as poly(vinyl alcohol) and poly(vinylpyrrolidone) exert negligible influence, while hydrophobic polymers such as poly(vinylidene fluoride) and polyethylene significantly enhance the activity, selectivity, and stability of CuO-derived electrodes toward C2H4 production. From ex situ characterizations, electrolysis in deuterated water, and molecular dynamics simulations, we propose that the improved catalytic performance triggered by hydrophobic polymers originates from restricted water diffusion and a higher local pH near the electrode surface. These observations shed light on interfacial manipulation for promoted CO2-to-C2H4 conversion.

AB - Cu is in the spotlight as it represents the only metal capable of catalyzing CO2 reduction to multicarbon products. However, its catalytic performance is determined collectively by a number of parameters including its composition and structure, electrolyte, and cell configuration. It remains a challenge to disentangle and understand the individual effect of these parameters. In this work, we study the effect of the electrode-electrolyte interface on CO2 reduction in water by coating CuO electrodes with polymers of varying hydrophilicities/phobicities. Hydrophilic polymers such as poly(vinyl alcohol) and poly(vinylpyrrolidone) exert negligible influence, while hydrophobic polymers such as poly(vinylidene fluoride) and polyethylene significantly enhance the activity, selectivity, and stability of CuO-derived electrodes toward C2H4 production. From ex situ characterizations, electrolysis in deuterated water, and molecular dynamics simulations, we propose that the improved catalytic performance triggered by hydrophobic polymers originates from restricted water diffusion and a higher local pH near the electrode surface. These observations shed light on interfacial manipulation for promoted CO2-to-C2H4 conversion.

KW - COreduction

KW - ethylene production

KW - interfacial hydrophobicity

KW - polymer coating

KW - water diffusion

UR - http://www.scopus.com/inward/record.url?scp=85099663704&partnerID=8YFLogxK

U2 - 10.1021/acscatal.0c03766

DO - 10.1021/acscatal.0c03766

M3 - Journal article

AN - SCOPUS:85099663704

SN - 2155-5435

VL - 11

SP - 958

EP - 966

JO - ACS Catalysis

JF - ACS Catalysis

IS - 2

ER -