Tuning OH binding energy enables selective electrochemical oxidation of ethylene to ethylene glycol

Yanwei Lum; Jianan Erick Huang; Ziyun Wang; Mingchuan Luo; Dae Hyun Nam; Wan Ru Leow; Bin Chen; Joshua Wicks; Yuguang C. Li; Yuhang Wang; Cao Thang Dinh; Jun Li; Tao Tao Zhuang; Fengwang Li; Tsun Kong Sham; David Sinton; Edward H. Sargent

doi:10.1038/s41929-019-0386-4

Tuning OH binding energy enables selective electrochemical oxidation of ethylene to ethylene glycol

Yanwei Lum, Jianan Erick Huang, Ziyun Wang, Mingchuan Luo, Dae Hyun Nam, Wan Ru Leow, Bin Chen, Joshua Wicks, Yuguang C. Li, Yuhang Wang, Cao Thang Dinh, Jun Li, Tao Tao Zhuang, Fengwang Li, Tsun Kong Sham, David Sinton, Edward H. Sargent^*

^*Corresponding author for this work

Chemistry

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

162 Scopus citations

Abstract

There is significant interest in developing efficient electrochemical processes for commodity chemical manufacturing, all directly powered by renewable electricity. A vital chemical is ethylene glycol, with an annual consumption of around 20 million tonnes due to its use as antifreeze and as a polymer precursor. Here we report a one-step electrochemical route at ambient temperature and pressure in aqueous media to the selective partial oxidation of ethylene to ethylene glycol. Tuning of the catalyst OH binding energy was hypothesized to be crucial for facilitating the transfer of OH to *C₂H₄OH to form ethylene glycol. Computational studies suggested that a gold-doped palladium catalyst could perform this step efficiently, and experimentally we found it to exhibit an approximate 80% Faradaic efficiency to ethylene glycol, retaining its performance for 100 hours of continuous operation. These findings represent a significant advance in the development of selective anodic partial oxidation reactions in aqueous media under mild conditions.

Original language	English (US)
Pages (from-to)	14-22
Number of pages	9
Journal	Nature Catalysis
Volume	3
Issue number	1
DOIs	https://doi.org/10.1038/s41929-019-0386-4
State	Published - Jan 1 2020

Funding

This material is based upon work supported by the Ontario Research Fund Research Excellence Program, the Natural Sciences and Engineering Research Council (NSERC) of Canada and the CIFAR Bio-Inspired Solar Energy program. The authors thank Z. Finfrock and D. M. Meira for technical support at the 20BM beamline of the Advanced Photon Source (Lemont, IL). This research used resources of the Advanced Photon Source, an Office of Science User Facility operated for the US Department of Energy (DOE) Office of Science by Argonne National Laboratory and was supported by the US DOE under Contract No. DE-AC02-06CH11357 and the Canadian Light Source and its funding partners. We acknowledge S. Fakra and the use of Beamline 10.3.2 at the Advanced Light Source for the collection of XAS data. The authors thank C. Andrei of the Canadian Centre for Electron Microscopy (CCEM) for TEM analysis. D.S. acknowledges the NSERC for an E. W. R. Steacie Memorial Fellowship. J.L. acknowledges the Banting Postdoctoral Fellowships program. All DFT computations were performed on the IBM BlueGene/Q supercomputer with support from the Southern Ontario Smart Computing Innovation Platform (SOSCIP) and Niagara supercomputer at the SciNet HPC Consortium. SOSCIP is funded by the Federal Economic Development Agency of Southern Ontario, the Province of Ontario, IBM Canada Ltd, Ontario Centres of Excellence, Mitacs and 15 Ontario academic member institutions. SciNet is funded by: the Canada Foundation for Innovation, the Government of Ontario, Ontario Research Fund—Research Excellence and the University of Toronto. We acknowledge the Ontario Centre for the Characterization of Advanced Materials (OCCAM) for characterization facilities.

ASJC Scopus subject areas

Catalysis
Bioengineering
Biochemistry
Process Chemistry and Technology

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This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1038/s41929-019-0386-4

Cite this

Lum, Y., Huang, J. E., Wang, Z., Luo, M., Nam, D. H., Leow, W. R., Chen, B., Wicks, J., Li, Y. C., Wang, Y., Dinh, C. T., Li, J., Zhuang, T. T., Li, F., Sham, T. K., Sinton, D., & Sargent, E. H. (2020). Tuning OH binding energy enables selective electrochemical oxidation of ethylene to ethylene glycol. Nature Catalysis, 3(1), 14-22. https://doi.org/10.1038/s41929-019-0386-4

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abstract = "There is significant interest in developing efficient electrochemical processes for commodity chemical manufacturing, all directly powered by renewable electricity. A vital chemical is ethylene glycol, with an annual consumption of around 20 million tonnes due to its use as antifreeze and as a polymer precursor. Here we report a one-step electrochemical route at ambient temperature and pressure in aqueous media to the selective partial oxidation of ethylene to ethylene glycol. Tuning of the catalyst OH binding energy was hypothesized to be crucial for facilitating the transfer of OH to *C2H4OH to form ethylene glycol. Computational studies suggested that a gold-doped palladium catalyst could perform this step efficiently, and experimentally we found it to exhibit an approximate 80% Faradaic efficiency to ethylene glycol, retaining its performance for 100 hours of continuous operation. These findings represent a significant advance in the development of selective anodic partial oxidation reactions in aqueous media under mild conditions.",

author = "Yanwei Lum and Huang, {Jianan Erick} and Ziyun Wang and Mingchuan Luo and Nam, {Dae Hyun} and Leow, {Wan Ru} and Bin Chen and Joshua Wicks and Li, {Yuguang C.} and Yuhang Wang and Dinh, {Cao Thang} and Jun Li and Zhuang, {Tao Tao} and Fengwang Li and Sham, {Tsun Kong} and David Sinton and Sargent, {Edward H.}",

note = "Funding Information: This material is based upon work supported by the Ontario Research Fund Research Excellence Program, the Natural Sciences and Engineering Research Council (NSERC) of Canada and the CIFAR Bio-Inspired Solar Energy program. The authors thank Z. Finfrock and D. M. Meira for technical support at the 20BM beamline of the Advanced Photon Source (Lemont, IL). This research used resources of the Advanced Photon Source, an Office of Science User Facility operated for the US Department of Energy (DOE) Office of Science by Argonne National Laboratory and was supported by the US DOE under Contract No. DE-AC02-06CH11357 and the Canadian Light Source and its funding partners. We acknowledge S. Fakra and the use of Beamline 10.3.2 at the Advanced Light Source for the collection of XAS data. The authors thank C. Andrei of the Canadian Centre for Electron Microscopy (CCEM) for TEM analysis. D.S. acknowledges the NSERC for an E. W. R. Steacie Memorial Fellowship. J.L. acknowledges the Banting Postdoctoral Fellowships program. All DFT computations were performed on the IBM BlueGene/Q supercomputer with support from the Southern Ontario Smart Computing Innovation Platform (SOSCIP) and Niagara supercomputer at the SciNet HPC Consortium. SOSCIP is funded by the Federal Economic Development Agency of Southern Ontario, the Province of Ontario, IBM Canada Ltd, Ontario Centres of Excellence, Mitacs and 15 Ontario academic member institutions. SciNet is funded by: the Canada Foundation for Innovation, the Government of Ontario, Ontario Research Fund—Research Excellence and the University of Toronto. We acknowledge the Ontario Centre for the Characterization of Advanced Materials (OCCAM) for characterization facilities. Publisher Copyright: {\textcopyright} 2020, The Author(s), under exclusive licence to Springer Nature Limited.",

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AU - Leow, Wan Ru

AU - Chen, Bin

AU - Wicks, Joshua

AU - Li, Yuguang C.

AU - Wang, Yuhang

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AU - Li, Jun

AU - Zhuang, Tao Tao

AU - Li, Fengwang

AU - Sham, Tsun Kong

AU - Sinton, David

AU - Sargent, Edward H.

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Tuning OH binding energy enables selective electrochemical oxidation of ethylene to ethylene glycol

Abstract

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