CO2 electroreduction to multicarbon products in strongly acidic electrolyte via synergistically modulating the local microenvironment

Electrochemical CO 2 reduction to multicarbon products faces challenges of unsatisfactory selectivity, productivity, and long-term stability. Herein, we demonstrate CO 2 electroreduction in strongly acidic electrolyte (pH ≤ 1) on electrochemically reduced porous Cu nanosheets by combining the confin...

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Published in	Nature communications Vol. 13; no. 1; pp. 7596 - 11
Main Authors	Ma, Zesong, Yang, Zhilong, Lai, Wenchuan, Wang, Qiyou, Qiao, Yan, Tao, Haolan, Lian, Cheng, Liu, Min, Ma, Chao, Pan, Anlian, Huang, Hongwen
Format	Journal Article
Language	English
Published	London Nature Publishing Group UK 09.12.2022 Nature Publishing Group Nature Portfolio
Subjects	119/118 140/131 140/133 147/143 639/301/299/886 639/638/161/886 639/638/675 Aqueous electrolytes Carbon dioxide Catalysts Cations Confinement Electrochemistry Electrolysis Electrolytes Electrowinning Humanities and Social Sciences Hydrogen evolution Microenvironments multidisciplinary pH effects Potassium chloride Science Science (multidisciplinary) Selectivity Sulfuric acid
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Abstract	Electrochemical CO 2 reduction to multicarbon products faces challenges of unsatisfactory selectivity, productivity, and long-term stability. Herein, we demonstrate CO 2 electroreduction in strongly acidic electrolyte (pH ≤ 1) on electrochemically reduced porous Cu nanosheets by combining the confinement effect and cation effect to synergistically modulate the local microenvironment. A Faradaic efficiency of 83.7 ± 1.4% and partial current density of 0.56 ± 0.02 A cm −2 , single-pass carbon efficiency of 54.4%, and stable electrolysis of 30 h in a flow cell are demonstrated for multicarbon products in a strongly acidic aqueous electrolyte consisting of sulfuric acid and KCl with pH ≤ 1. Mechanistically, the accumulated species (e.g., K + and OH − ) on the Helmholtz plane account for the selectivity and activity toward multicarbon products by kinetically reducing the proton coverage and thermodynamically favoring the CO 2 conversion. We find that the K + cations facilitate C-C coupling through local interaction between K + and the key intermediate *OCCO. Attaining high selectivity for CO 2 electroreduction in acid is usually difficult due to competing hydrogen evolution. Here, the authors demonstrate efficient CO 2 reduction to multicarbon products in strongly acidic medium (pH ≤ 1) on a porous Cu catalyst by combining confinement and cation effects.
AbstractList	Electrochemical CO 2 reduction to multicarbon products faces challenges of unsatisfactory selectivity, productivity, and long-term stability. Herein, we demonstrate CO 2 electroreduction in strongly acidic electrolyte (pH ≤ 1) on electrochemically reduced porous Cu nanosheets by combining the confinement effect and cation effect to synergistically modulate the local microenvironment. A Faradaic efficiency of 83.7 ± 1.4% and partial current density of 0.56 ± 0.02 A cm −2 , single-pass carbon efficiency of 54.4%, and stable electrolysis of 30 h in a flow cell are demonstrated for multicarbon products in a strongly acidic aqueous electrolyte consisting of sulfuric acid and KCl with pH ≤ 1. Mechanistically, the accumulated species (e.g., K + and OH − ) on the Helmholtz plane account for the selectivity and activity toward multicarbon products by kinetically reducing the proton coverage and thermodynamically favoring the CO 2 conversion. We find that the K + cations facilitate C-C coupling through local interaction between K + and the key intermediate OCCO. Electrochemical CO2 reduction to multicarbon products faces challenges of unsatisfactory selectivity, productivity, and long-term stability. Herein, we demonstrate CO2 electroreduction in strongly acidic electrolyte (pH ≤ 1) on electrochemically reduced porous Cu nanosheets by combining the confinement effect and cation effect to synergistically modulate the local microenvironment. A Faradaic efficiency of 83.7 ± 1.4% and partial current density of 0.56 ± 0.02 A cm-2, single-pass carbon efficiency of 54.4%, and stable electrolysis of 30 h in a flow cell are demonstrated for multicarbon products in a strongly acidic aqueous electrolyte consisting of sulfuric acid and KCl with pH ≤ 1. Mechanistically, the accumulated species (e.g., K+ and OH-) on the Helmholtz plane account for the selectivity and activity toward multicarbon products by kinetically reducing the proton coverage and thermodynamically favoring the CO2 conversion. We find that the K+ cations facilitate C-C coupling through local interaction between K+ and the key intermediate OCCO.Electrochemical CO2 reduction to multicarbon products faces challenges of unsatisfactory selectivity, productivity, and long-term stability. Herein, we demonstrate CO2 electroreduction in strongly acidic electrolyte (pH ≤ 1) on electrochemically reduced porous Cu nanosheets by combining the confinement effect and cation effect to synergistically modulate the local microenvironment. A Faradaic efficiency of 83.7 ± 1.4% and partial current density of 0.56 ± 0.02 A cm-2, single-pass carbon efficiency of 54.4%, and stable electrolysis of 30 h in a flow cell are demonstrated for multicarbon products in a strongly acidic aqueous electrolyte consisting of sulfuric acid and KCl with pH ≤ 1. Mechanistically, the accumulated species (e.g., K+ and OH-) on the Helmholtz plane account for the selectivity and activity toward multicarbon products by kinetically reducing the proton coverage and thermodynamically favoring the CO2 conversion. We find that the K+ cations facilitate C-C coupling through local interaction between K+ and the key intermediate OCCO. Electrochemical CO 2 reduction to multicarbon products faces challenges of unsatisfactory selectivity, productivity, and long-term stability. Herein, we demonstrate CO 2 electroreduction in strongly acidic electrolyte (pH ≤ 1) on electrochemically reduced porous Cu nanosheets by combining the confinement effect and cation effect to synergistically modulate the local microenvironment. A Faradaic efficiency of 83.7 ± 1.4% and partial current density of 0.56 ± 0.02 A cm −2 , single-pass carbon efficiency of 54.4%, and stable electrolysis of 30 h in a flow cell are demonstrated for multicarbon products in a strongly acidic aqueous electrolyte consisting of sulfuric acid and KCl with pH ≤ 1. Mechanistically, the accumulated species (e.g., K + and OH − ) on the Helmholtz plane account for the selectivity and activity toward multicarbon products by kinetically reducing the proton coverage and thermodynamically favoring the CO 2 conversion. We find that the K + cations facilitate C-C coupling through local interaction between K + and the key intermediate OCCO. Attaining high selectivity for CO 2 electroreduction in acid is usually difficult due to competing hydrogen evolution. Here, the authors demonstrate efficient CO 2 reduction to multicarbon products in strongly acidic medium (pH ≤ 1) on a porous Cu catalyst by combining confinement and cation effects. Electrochemical CO2 reduction to multicarbon products faces challenges of unsatisfactory selectivity, productivity, and long-term stability. Herein, we demonstrate CO2 electroreduction in strongly acidic electrolyte (pH ≤ 1) on electrochemically reduced porous Cu nanosheets by combining the confinement effect and cation effect to synergistically modulate the local microenvironment. A Faradaic efficiency of 83.7 ± 1.4% and partial current density of 0.56 ± 0.02 A cm−2, single-pass carbon efficiency of 54.4%, and stable electrolysis of 30 h in a flow cell are demonstrated for multicarbon products in a strongly acidic aqueous electrolyte consisting of sulfuric acid and KCl with pH ≤ 1. Mechanistically, the accumulated species (e.g., K+ and OH−) on the Helmholtz plane account for the selectivity and activity toward multicarbon products by kinetically reducing the proton coverage and thermodynamically favoring the CO2 conversion. We find that the K+ cations facilitate C-C coupling through local interaction between K+ and the key intermediate *OCCO.Attaining high selectivity for CO2 electroreduction in acid is usually difficult due to competing hydrogen evolution. Here, the authors demonstrate efficient CO2 reduction to multicarbon products in strongly acidic medium (pH ≤ 1) on a porous Cu catalyst by combining confinement and cation effects. Attaining high selectivity for CO2 electroreduction in acid is usually difficult due to competing hydrogen evolution. Here, the authors demonstrate efficient CO2 reduction to multicarbon products in strongly acidic medium (pH ≤ 1) on a porous Cu catalyst by combining confinement and cation effects.
ArticleNumber	7596
Author	Lai, Wenchuan Ma, Zesong Wang, Qiyou Pan, Anlian Tao, Haolan Ma, Chao Yang, Zhilong Qiao, Yan Lian, Cheng Huang, Hongwen Liu, Min
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Snippet	Electrochemical CO 2 reduction to multicarbon products faces challenges of unsatisfactory selectivity, productivity, and long-term stability. Herein, we... Electrochemical CO2 reduction to multicarbon products faces challenges of unsatisfactory selectivity, productivity, and long-term stability. Herein, we... Attaining high selectivity for CO2 electroreduction in acid is usually difficult due to competing hydrogen evolution. Here, the authors demonstrate efficient...
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SubjectTerms	119/118 140/131 140/133 147/143 639/301/299/886 639/638/161/886 639/638/675 Aqueous electrolytes Carbon dioxide Catalysts Cations Confinement Electrochemistry Electrolysis Electrolytes Electrowinning Humanities and Social Sciences Hydrogen evolution Microenvironments multidisciplinary pH effects Potassium chloride Science Science (multidisciplinary) Selectivity Sulfuric acid
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Title	CO2 electroreduction to multicarbon products in strongly acidic electrolyte via synergistically modulating the local microenvironment
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