Control of evolution of porous copper-based metal-organic materials for electroreduction of CO2 to multi-carbon products

Lili Li; Lutong Shan; Meng He; Yujie Ma; Yiqi Zhou; Marek Nikiel; Laura Lopez Odriozola; Louise Natrajan; Eric J. L. Mcinnes; Martin Schroder; Sihai Yang; Floriana Tuna

Control of evolution of porous copper-based metal-organic materials for electroreduction of CO2 to multi-carbon products

Lili Li, Lutong Shan, Meng He, Yujie Ma, Yiqi Zhou, Marek Nikiel, Laura Lopez Odriozola, Louise Natrajan, Eric J. L. Mcinnes, Martin Schroder, Sihai Yang, Floriana Tuna

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

Abstract

Electrochemcial reduction of CO2 to multi-carbon (C2+) products is an important but challenging task.
Here, we report the control of structural evolution of two porous Cu(II)-based materials (HKUST-1 and CuMOP, MOP = metal-organic polyhedra) under electrochemical conditions by adsorption of 7,7,8,8-tetracyanoquinodimethane (TNCQ) as an additional electron acceptor. The formation of Cu(I) and Cu(0) species during the structural evolution has been confirmed and analysed by powder X-ray diffraction, and by EPR, Raman, XPS, IR and UV-vis spectroscopies. An electrode decorated with evolved TCNQ@CuMOP shows a selectivity of 68% for C2+ products with a total current density of 268 mA/cm2 and Faradaic efficiency of 37% for electrochemcial reduction of CO2 in 1 M aqueous KOH electrolyte at −2.27 V vs RHE (reversible hydrogen electrode). In situ electron paramagnetic resonance spectroscopy reveals the presence of carbon-centred radicals as key reaction intermediates. This study demonstrates the positive impact of additional electron acceptors on the structural evolution of Cu(II)-based porous materials to promote the electroreduction of CO2 to C2+ products.

Original language	English
Journal	Materials Advances
Publication status	Accepted/In press - 12 Mar 2023

Cite this

@article{d795882701ed47d7851be4b91323d67d,

title = "Control of evolution of porous copper-based metal-organic materials for electroreduction of CO2 to multi-carbon products",

abstract = "Electrochemcial reduction of CO2 to multi-carbon (C2+) products is an important but challenging task. Here, we report the control of structural evolution of two porous Cu(II)-based materials (HKUST-1 and CuMOP, MOP = metal-organic polyhedra) under electrochemical conditions by adsorption of 7,7,8,8-tetracyanoquinodimethane (TNCQ) as an additional electron acceptor. The formation of Cu(I) and Cu(0) species during the structural evolution has been confirmed and analysed by powder X-ray diffraction, and by EPR, Raman, XPS, IR and UV-vis spectroscopies. An electrode decorated with evolved TCNQ@CuMOP shows a selectivity of 68% for C2+ products with a total current density of 268 mA/cm2 and Faradaic efficiency of 37% for electrochemcial reduction of CO2 in 1 M aqueous KOH electrolyte at −2.27 V vs RHE (reversible hydrogen electrode). In situ electron paramagnetic resonance spectroscopy reveals the presence of carbon-centred radicals as key reaction intermediates. This study demonstrates the positive impact of additional electron acceptors on the structural evolution of Cu(II)-based porous materials to promote the electroreduction of CO2 to C2+ products.",

author = "Lili Li and Lutong Shan and Meng He and Yujie Ma and Yiqi Zhou and Marek Nikiel and {Lopez Odriozola}, Laura and Louise Natrajan and Mcinnes, {Eric J. L.} and Martin Schroder and Sihai Yang and Floriana Tuna",

year = "2023",

month = mar,

day = "12",

language = "English",

journal = "Materials Advances",

issn = "2633-5409",

publisher = "Royal Society of Chemistry",

}

TY - JOUR

T1 - Control of evolution of porous copper-based metal-organic materials for electroreduction of CO2 to multi-carbon products

AU - Li, Lili

AU - Shan, Lutong

AU - He, Meng

AU - Ma, Yujie

AU - Zhou, Yiqi

AU - Nikiel, Marek

AU - Lopez Odriozola, Laura

AU - Natrajan, Louise

AU - Mcinnes, Eric J. L.

AU - Schroder, Martin

AU - Yang, Sihai

AU - Tuna, Floriana

PY - 2023/3/12

Y1 - 2023/3/12

N2 - Electrochemcial reduction of CO2 to multi-carbon (C2+) products is an important but challenging task. Here, we report the control of structural evolution of two porous Cu(II)-based materials (HKUST-1 and CuMOP, MOP = metal-organic polyhedra) under electrochemical conditions by adsorption of 7,7,8,8-tetracyanoquinodimethane (TNCQ) as an additional electron acceptor. The formation of Cu(I) and Cu(0) species during the structural evolution has been confirmed and analysed by powder X-ray diffraction, and by EPR, Raman, XPS, IR and UV-vis spectroscopies. An electrode decorated with evolved TCNQ@CuMOP shows a selectivity of 68% for C2+ products with a total current density of 268 mA/cm2 and Faradaic efficiency of 37% for electrochemcial reduction of CO2 in 1 M aqueous KOH electrolyte at −2.27 V vs RHE (reversible hydrogen electrode). In situ electron paramagnetic resonance spectroscopy reveals the presence of carbon-centred radicals as key reaction intermediates. This study demonstrates the positive impact of additional electron acceptors on the structural evolution of Cu(II)-based porous materials to promote the electroreduction of CO2 to C2+ products.

AB - Electrochemcial reduction of CO2 to multi-carbon (C2+) products is an important but challenging task. Here, we report the control of structural evolution of two porous Cu(II)-based materials (HKUST-1 and CuMOP, MOP = metal-organic polyhedra) under electrochemical conditions by adsorption of 7,7,8,8-tetracyanoquinodimethane (TNCQ) as an additional electron acceptor. The formation of Cu(I) and Cu(0) species during the structural evolution has been confirmed and analysed by powder X-ray diffraction, and by EPR, Raman, XPS, IR and UV-vis spectroscopies. An electrode decorated with evolved TCNQ@CuMOP shows a selectivity of 68% for C2+ products with a total current density of 268 mA/cm2 and Faradaic efficiency of 37% for electrochemcial reduction of CO2 in 1 M aqueous KOH electrolyte at −2.27 V vs RHE (reversible hydrogen electrode). In situ electron paramagnetic resonance spectroscopy reveals the presence of carbon-centred radicals as key reaction intermediates. This study demonstrates the positive impact of additional electron acceptors on the structural evolution of Cu(II)-based porous materials to promote the electroreduction of CO2 to C2+ products.

M3 - Article

JO - Materials Advances

JF - Materials Advances

SN - 2633-5409

ER -

Control of evolution of porous copper-based metal-organic materials for electroreduction of CO2 to multi-carbon products

Abstract

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