Dopant-tuned stabilization of intermediates promotes electrosynthesis of valuable C3 products

Tao Tao Zhuang; Dae Hyun Nam; Ziyun Wang; Hui Hui Li; Christine M. Gabardo; Yi Li; Zhi Qin Liang; Jun Li; Xiao Jing Liu; Bin Chen; Wan Ru Leow; Rui Wu; Xue Wang; Fengwang Li; Yanwei Lum; Joshua Wicks; Colin P. O’Brien; Tao Peng; Alexander H. Ip; Tsun Kong Sham; Shu Hong Yu; David Sinton; Edward H. Sargent

doi:10.1038/s41467-019-12788-0

Dopant-tuned stabilization of intermediates promotes electrosynthesis of valuable C3 products

Tao Tao Zhuang, Dae Hyun Nam, Ziyun Wang, Hui Hui Li, Christine M. Gabardo, Yi Li, Zhi Qin Liang, Jun Li, Xiao Jing Liu, Bin Chen, Wan Ru Leow, Rui Wu, Xue Wang, Fengwang Li, Yanwei Lum, Joshua Wicks, Colin P. O’Brien, Tao Peng, Alexander H. Ip, Tsun Kong ShamShu Hong Yu, David Sinton, Edward H. Sargent

Department of Energy and Science and Engineering

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

35 Scopus citations

Abstract

The upgrading of CO₂/CO feedstocks to higher-value chemicals via energy-efficient electrochemical processes enables carbon utilization and renewable energy storage. Substantial progress has been made to improve performance at the cathodic side; whereas less progress has been made on improving anodic electro-oxidation reactions to generate value. Here we report the efficient electroproduction of value-added multi-carbon dimethyl carbonate (DMC) from CO and methanol via oxidative carbonylation. We find that, compared to pure palladium controls, boron-doped palladium (Pd-B) tunes the binding strength of intermediates along this reaction pathway and favors DMC formation. We implement this doping strategy and report the selective electrosynthesis of DMC experimentally. We achieve a DMC Faradaic efficiency of 83 ± 5%, fully a 3x increase in performance compared to the corresponding pure Pd electrocatalyst.

Original language	English
Article number	4807
Journal	Nature Communications
Volume	10
Issue number	1
DOIs	https://doi.org/10.1038/s41467-019-12788-0
State	Published - 1 Dec 2019

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Publisher Copyright:
© 2019, The Author(s).

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Zhuang, T. T., Nam, D. H., Wang, Z., Li, H. H., Gabardo, C. M., Li, Y., Liang, Z. Q., Li, J., Liu, X. J., Chen, B., Leow, W. R., Wu, R., Wang, X., Li, F., Lum, Y., Wicks, J., O’Brien, C. P., Peng, T., Ip, A. H., ... Sargent, E. H. (2019). Dopant-tuned stabilization of intermediates promotes electrosynthesis of valuable C3 products. Nature Communications, 10(1), Article 4807. https://doi.org/10.1038/s41467-019-12788-0

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title = "Dopant-tuned stabilization of intermediates promotes electrosynthesis of valuable C3 products",

abstract = "The upgrading of CO2/CO feedstocks to higher-value chemicals via energy-efficient electrochemical processes enables carbon utilization and renewable energy storage. Substantial progress has been made to improve performance at the cathodic side; whereas less progress has been made on improving anodic electro-oxidation reactions to generate value. Here we report the efficient electroproduction of value-added multi-carbon dimethyl carbonate (DMC) from CO and methanol via oxidative carbonylation. We find that, compared to pure palladium controls, boron-doped palladium (Pd-B) tunes the binding strength of intermediates along this reaction pathway and favors DMC formation. We implement this doping strategy and report the selective electrosynthesis of DMC experimentally. We achieve a DMC Faradaic efficiency of 83 ± 5%, fully a 3x increase in performance compared to the corresponding pure Pd electrocatalyst.",

author = "Zhuang, {Tao Tao} and Nam, {Dae Hyun} and Ziyun Wang and Li, {Hui Hui} and Gabardo, {Christine M.} and Yi Li and Liang, {Zhi Qin} and Jun Li and Liu, {Xiao Jing} and Bin Chen and Leow, {Wan Ru} and Rui Wu and Xue Wang and Fengwang Li and Yanwei Lum and Joshua Wicks and O{\textquoteright}Brien, {Colin P.} and Tao Peng and Ip, {Alexander H.} and Sham, {Tsun Kong} and Yu, {Shu Hong} and David Sinton and Sargent, {Edward H.}",

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Zhuang, TT, Nam, DH, Wang, Z, Li, HH, Gabardo, CM, Li, Y, Liang, ZQ, Li, J, Liu, XJ, Chen, B, Leow, WR, Wu, R, Wang, X, Li, F, Lum, Y, Wicks, J, O’Brien, CP, Peng, T, Ip, AH, Sham, TK, Yu, SH, Sinton, D & Sargent, EH 2019, 'Dopant-tuned stabilization of intermediates promotes electrosynthesis of valuable C3 products', Nature Communications, vol. 10, no. 1, 4807. https://doi.org/10.1038/s41467-019-12788-0

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AU - Zhuang, Tao Tao

AU - Nam, Dae Hyun

AU - Wang, Ziyun

AU - Li, Hui Hui

AU - Gabardo, Christine M.

AU - Li, Yi

AU - Liang, Zhi Qin

AU - Li, Jun

AU - Liu, Xiao Jing

AU - Chen, Bin

AU - Leow, Wan Ru

AU - Wu, Rui

AU - Wang, Xue

AU - Li, Fengwang

AU - Lum, Yanwei

AU - Wicks, Joshua

AU - O’Brien, Colin P.

AU - Peng, Tao

AU - Ip, Alexander H.

AU - Sham, Tsun Kong

AU - Yu, Shu Hong

AU - Sinton, David

AU - Sargent, Edward H.

PY - 2019/12/1

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AB - The upgrading of CO2/CO feedstocks to higher-value chemicals via energy-efficient electrochemical processes enables carbon utilization and renewable energy storage. Substantial progress has been made to improve performance at the cathodic side; whereas less progress has been made on improving anodic electro-oxidation reactions to generate value. Here we report the efficient electroproduction of value-added multi-carbon dimethyl carbonate (DMC) from CO and methanol via oxidative carbonylation. We find that, compared to pure palladium controls, boron-doped palladium (Pd-B) tunes the binding strength of intermediates along this reaction pathway and favors DMC formation. We implement this doping strategy and report the selective electrosynthesis of DMC experimentally. We achieve a DMC Faradaic efficiency of 83 ± 5%, fully a 3x increase in performance compared to the corresponding pure Pd electrocatalyst.

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Dopant-tuned stabilization of intermediates promotes electrosynthesis of valuable C3 products

Abstract

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