Enhanced CO2 Electroreduction Selectivity toward Ethylene on Pyrazolate-Stabilized Asymmetric Ni-Cu Hybrid Sites

Liang Huang; Ziao Liu; Ge Gao; Cailing Chen; Yanrong Xue; Jiwu Zhao; Qiong Lei; Mengtian Jin; Chongqin Zhu; Yu Han; Joseph S. Francisco; Xu Lu

doi:10.1021/jacs.3c10600

Enhanced CO₂ Electroreduction Selectivity toward Ethylene on Pyrazolate-Stabilized Asymmetric Ni-Cu Hybrid Sites

Liang Huang, Ziao Liu, Ge Gao, Cailing Chen, Yanrong Xue, Jiwu Zhao, Qiong Lei, Mengtian Jin, Chongqin Zhu^*, Yu Han^*, Joseph S. Francisco^*, Xu Lu^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

21 Scopus citations

Abstract

Metal-organic frameworks (MOFs) possess well-defined, designable structures, holding great potential in enhancing product selectivity for electrochemical CO₂ reduction (CO₂R) through active site engineering. Here, we report a novel MOF catalyst featuring pyrazolate-stabilized asymmetric Ni/Cu sites, which not only maintains structural stability under harsh electrochemical conditions but also exhibits extraordinarily high ethylene (C₂H₄) selectivity during CO₂R. At a cathode potential of −1.3 V versus RHE, our MOF catalyst, denoted as Cu₁Ni-BDP, manifests a C₂H₄ Faradaic efficiency (FE) of 52.7% with an overall current density of 0.53 A cm^-2 in 1.0 M KOH electrolyte, surpassing that on prevailing Cu-based catalysts. More remarkably, the Cu₁Ni-BDP MOF exhibits a stable performance with only 4.5% reduction in C₂H₄ FE during 25 h of CO₂ electrolysis.

Original language	English (US)
Pages (from-to)	26444-26451
Number of pages	8
Journal	Journal of the American Chemical Society
Volume	145
Issue number	48
DOIs	https://doi.org/10.1021/jacs.3c10600
State	Published - Dec 6 2023

Bibliographical note

Publisher Copyright:
© 2023 American Chemical Society.

ASJC Scopus subject areas

Catalysis
General Chemistry
Biochemistry
Colloid and Surface Chemistry

Access to Document

10.1021/jacs.3c10600

Cite this

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title = "Enhanced CO2 Electroreduction Selectivity toward Ethylene on Pyrazolate-Stabilized Asymmetric Ni-Cu Hybrid Sites",

abstract = "Metal-organic frameworks (MOFs) possess well-defined, designable structures, holding great potential in enhancing product selectivity for electrochemical CO2 reduction (CO2R) through active site engineering. Here, we report a novel MOF catalyst featuring pyrazolate-stabilized asymmetric Ni/Cu sites, which not only maintains structural stability under harsh electrochemical conditions but also exhibits extraordinarily high ethylene (C2H4) selectivity during CO2R. At a cathode potential of −1.3 V versus RHE, our MOF catalyst, denoted as Cu1Ni-BDP, manifests a C2H4 Faradaic efficiency (FE) of 52.7% with an overall current density of 0.53 A cm-2 in 1.0 M KOH electrolyte, surpassing that on prevailing Cu-based catalysts. More remarkably, the Cu1Ni-BDP MOF exhibits a stable performance with only 4.5% reduction in C2H4 FE during 25 h of CO2 electrolysis.",

author = "Liang Huang and Ziao Liu and Ge Gao and Cailing Chen and Yanrong Xue and Jiwu Zhao and Qiong Lei and Mengtian Jin and Chongqin Zhu and Yu Han and Francisco, {Joseph S.} and Xu Lu",

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T1 - Enhanced CO2 Electroreduction Selectivity toward Ethylene on Pyrazolate-Stabilized Asymmetric Ni-Cu Hybrid Sites

AU - Huang, Liang

AU - Liu, Ziao

AU - Gao, Ge

AU - Chen, Cailing

AU - Xue, Yanrong

AU - Zhao, Jiwu

AU - Lei, Qiong

AU - Jin, Mengtian

AU - Zhu, Chongqin

AU - Han, Yu

AU - Francisco, Joseph S.

AU - Lu, Xu

PY - 2023/12/6

Y1 - 2023/12/6

N2 - Metal-organic frameworks (MOFs) possess well-defined, designable structures, holding great potential in enhancing product selectivity for electrochemical CO2 reduction (CO2R) through active site engineering. Here, we report a novel MOF catalyst featuring pyrazolate-stabilized asymmetric Ni/Cu sites, which not only maintains structural stability under harsh electrochemical conditions but also exhibits extraordinarily high ethylene (C2H4) selectivity during CO2R. At a cathode potential of −1.3 V versus RHE, our MOF catalyst, denoted as Cu1Ni-BDP, manifests a C2H4 Faradaic efficiency (FE) of 52.7% with an overall current density of 0.53 A cm-2 in 1.0 M KOH electrolyte, surpassing that on prevailing Cu-based catalysts. More remarkably, the Cu1Ni-BDP MOF exhibits a stable performance with only 4.5% reduction in C2H4 FE during 25 h of CO2 electrolysis.

AB - Metal-organic frameworks (MOFs) possess well-defined, designable structures, holding great potential in enhancing product selectivity for electrochemical CO2 reduction (CO2R) through active site engineering. Here, we report a novel MOF catalyst featuring pyrazolate-stabilized asymmetric Ni/Cu sites, which not only maintains structural stability under harsh electrochemical conditions but also exhibits extraordinarily high ethylene (C2H4) selectivity during CO2R. At a cathode potential of −1.3 V versus RHE, our MOF catalyst, denoted as Cu1Ni-BDP, manifests a C2H4 Faradaic efficiency (FE) of 52.7% with an overall current density of 0.53 A cm-2 in 1.0 M KOH electrolyte, surpassing that on prevailing Cu-based catalysts. More remarkably, the Cu1Ni-BDP MOF exhibits a stable performance with only 4.5% reduction in C2H4 FE during 25 h of CO2 electrolysis.

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