Silica-copper catalyst interfaces enable carbon-carbon coupling towards ethylene electrosynthesis

Jun Li; Adnan Ozden; Mingyu Wan; Yongfeng Hu; Fengwang Li; Yuhang Wang; Reza R. Zamani; Dan Ren; Ziyun Wang; Yi Xu; Dae-Hyun Nam; Joshua Wicks; Bin Chen; Xue Wang; Mingchuan Luo; Michael Graetzel; Fanglin Che; Edward H. Sargent; David Sinton

doi:10.1038/s41467-021-23023-0

Silica-copper catalyst interfaces enable carbon-carbon coupling towards ethylene electrosynthesis

Jun Li, Adnan Ozden, Mingyu Wan, Yongfeng Hu, Fengwang Li, Yuhang Wang, Reza R. Zamani, Dan Ren, Ziyun Wang, Yi Xu, Dae-Hyun Nam, Joshua Wicks, Bin Chen, Xue Wang, Mingchuan Luo, Michael Graetzel, Fanglin Che^*, Edward H. Sargent^*, David Sinton^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

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Abstract

Membrane electrode assembly (MEA) electrolyzers offer a means to scale up CO₂-to-ethylene electroconversion using renewable electricity and close the anthropogenic carbon cycle. To date, excessive CO₂ coverage at the catalyst surface with limited active sites in MEA systems interferes with the carbon-carbon coupling reaction, diminishing ethylene production. With the aid of density functional theory calculations and spectroscopic analysis, here we report an oxide modulation strategy in which we introduce silica on Cu to create active Cu-SiO_x interface sites, decreasing the formation energies of OCOH* and OCCOH*—key intermediates along the pathway to ethylene formation. We then synthesize the Cu-SiO_x catalysts using one-pot coprecipitation and integrate the catalyst in a MEA electrolyzer. By tuning the CO₂ concentration, the Cu-SiO_x catalyst based MEA electrolyzer shows high ethylene Faradaic efficiencies of up to 65% at high ethylene current densities of up to 215 mA cm⁻²; and features sustained operation over 50 h.

Original language	English
Article number	2808
Journal	Nature Communications
Volume	12
Online published	14 May 2021
DOIs	https://doi.org/10.1038/s41467-021-23023-0
Publication status	Published - 2021
Externally published	Yes

Funding

This work has received financial support from the Ontario Research Fund Research-Excellence Program, the Natural Sciences and Engineering Research Council (NSERC) of Canada, the CIFAR Bio-Inspired Solar Energy Program, and the University of Toronto Connaught grant. This research used synchrotron resources of the Advanced Photon Source (APS), an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science by Argonne National Laboratory, and was supported by the U.S. DOE under Contract No. DE-AC02-06CH11357, and the Canadian Light Source and its funding partners. This research also used infrastructure provided by the Canada Foundation for Innovation and the Ontario Research Fund. We thank Dr. T.P. Wu, Dr. Y.Z. Finfrock and Dr. L. Ma for technical support at 9BM beamline of APS. D.S. acknowledges the NSERC E.W.R Steacie Memorial Fellowship. J.L. acknowledges the Banting Postdoctoral Fellowships program. DFT calculations were performed on the Massachusetts Green High Performance Computing Center (MGHPCC). The authors also acknowledge the Texas Advanced Computing Center (TACC) at the University of Texas at Austin for partially providing HPC resources that have contributed to the research results reported within this paper. Our thanks also goes to institutional faculty start-up funds from University of Massachusetts Lowell.

Publisher's Copyright Statement

This full text is made available under CC-BY 4.0. https://creativecommons.org/licenses/by/4.0/

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Li, J., Ozden, A., Wan, M., Hu, Y., Li, F., Wang, Y., Zamani, R. R., Ren, D., Wang, Z., Xu, Y., Nam, D.-H., Wicks, J., Chen, B., Wang, X., Luo, M., Graetzel, M., Che, F., Sargent, E. H., & Sinton, D. (2021). Silica-copper catalyst interfaces enable carbon-carbon coupling towards ethylene electrosynthesis. Nature Communications, 12, Article 2808. https://doi.org/10.1038/s41467-021-23023-0

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abstract = "Membrane electrode assembly (MEA) electrolyzers offer a means to scale up CO2-to-ethylene electroconversion using renewable electricity and close the anthropogenic carbon cycle. To date, excessive CO2 coverage at the catalyst surface with limited active sites in MEA systems interferes with the carbon-carbon coupling reaction, diminishing ethylene production. With the aid of density functional theory calculations and spectroscopic analysis, here we report an oxide modulation strategy in which we introduce silica on Cu to create active Cu-SiOx interface sites, decreasing the formation energies of OCOH* and OCCOH*—key intermediates along the pathway to ethylene formation. We then synthesize the Cu-SiOx catalysts using one-pot coprecipitation and integrate the catalyst in a MEA electrolyzer. By tuning the CO2 concentration, the Cu-SiOx catalyst based MEA electrolyzer shows high ethylene Faradaic efficiencies of up to 65% at high ethylene current densities of up to 215 mA cm−2; and features sustained operation over 50 h.",

author = "Jun Li and Adnan Ozden and Mingyu Wan and Yongfeng Hu and Fengwang Li and Yuhang Wang and Zamani, {Reza R.} and Dan Ren and Ziyun Wang and Yi Xu and Dae-Hyun Nam and Joshua Wicks and Bin Chen and Xue Wang and Mingchuan Luo and Michael Graetzel and Fanglin Che and Sargent, {Edward H.} and David Sinton",

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AU - Ozden, Adnan

AU - Wan, Mingyu

AU - Hu, Yongfeng

AU - Li, Fengwang

AU - Wang, Yuhang

AU - Zamani, Reza R.

AU - Ren, Dan

AU - Wang, Ziyun

AU - Xu, Yi

AU - Nam, Dae-Hyun

AU - Wicks, Joshua

AU - Chen, Bin

AU - Wang, Xue

AU - Luo, Mingchuan

AU - Graetzel, Michael

AU - Che, Fanglin

AU - Sargent, Edward H.

AU - Sinton, David

PY - 2021

Y1 - 2021

N2 - Membrane electrode assembly (MEA) electrolyzers offer a means to scale up CO2-to-ethylene electroconversion using renewable electricity and close the anthropogenic carbon cycle. To date, excessive CO2 coverage at the catalyst surface with limited active sites in MEA systems interferes with the carbon-carbon coupling reaction, diminishing ethylene production. With the aid of density functional theory calculations and spectroscopic analysis, here we report an oxide modulation strategy in which we introduce silica on Cu to create active Cu-SiOx interface sites, decreasing the formation energies of OCOH* and OCCOH*—key intermediates along the pathway to ethylene formation. We then synthesize the Cu-SiOx catalysts using one-pot coprecipitation and integrate the catalyst in a MEA electrolyzer. By tuning the CO2 concentration, the Cu-SiOx catalyst based MEA electrolyzer shows high ethylene Faradaic efficiencies of up to 65% at high ethylene current densities of up to 215 mA cm−2; and features sustained operation over 50 h.

AB - Membrane electrode assembly (MEA) electrolyzers offer a means to scale up CO2-to-ethylene electroconversion using renewable electricity and close the anthropogenic carbon cycle. To date, excessive CO2 coverage at the catalyst surface with limited active sites in MEA systems interferes with the carbon-carbon coupling reaction, diminishing ethylene production. With the aid of density functional theory calculations and spectroscopic analysis, here we report an oxide modulation strategy in which we introduce silica on Cu to create active Cu-SiOx interface sites, decreasing the formation energies of OCOH* and OCCOH*—key intermediates along the pathway to ethylene formation. We then synthesize the Cu-SiOx catalysts using one-pot coprecipitation and integrate the catalyst in a MEA electrolyzer. By tuning the CO2 concentration, the Cu-SiOx catalyst based MEA electrolyzer shows high ethylene Faradaic efficiencies of up to 65% at high ethylene current densities of up to 215 mA cm−2; and features sustained operation over 50 h.

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Silica-copper catalyst interfaces enable carbon-carbon coupling towards ethylene electrosynthesis

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