Voltage-Gated Electrocatalysis of Efficient and Selective Methane Oxidation by Tricopper Clusters under Ambient Conditions

Yi-Fang Tsai; Thiyagarajan Natarajan; Zhi-Han Lin; I-Kuen Tsai; Damodar Janmanchi; Sunney I. Chan; Steve S.-F. Yu

doi:10.1021/jacs.2c01169

Voltage-Gated Electrocatalysis of Efficient and Selective Methane Oxidation by Tricopper Clusters under Ambient Conditions

Yi-Fang Tsai, Thiyagarajan Natarajan, Zhi-Han Lin, I-Kuen Tsai, Damodar Janmanchi, Sunney I. Chan, Steve S.-F. Yu

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

7 Scopus citations

Abstract

Selective methane oxidation is difficult chemistry. Here we describe a strategy for the electrocatalysis of selective methane oxidation by immobilizing tricopper catalysts on the cathodic surface. In the presence of dioxygen and methane, the activation of these catalysts above a threshold cathodic potential can initiate the dioxygen chemistry for O atom transfer to methane. The catalytic turnover is completed by facile electron injections into the tricopper catalysts from the electrode. This technology leads to dramatic enhancements in performance of the catalysts toward methane oxidation. Unprecedented turnover frequencies (>40 min–1) and high product throughputs (turnover numbers >30 000 in 12 h) are achieved for this challenging chemical transformation in water under ambient conditions. The technology is green and suitable for on-site direct conversion of methane into methanol.

Original language	English (US)
Journal	Journal of the American Chemical Society
DOIs	https://doi.org/10.1021/jacs.2c01169
State	Published - May 27 2022
Externally published	Yes

Bibliographical note

KAUST Repository Item: Exported on 2022-06-01
Acknowledgements: S.I.C. and S.S.S.F. acknowledge helpful discussions with Dr. David Wu, Institute of Chemistry, Academia Sinica, Taiwan and Dr. Cafer T. Yavuz, Chemical Science, Physical Science and Engineering Division, King Abdullah University of Science and Technology, Saudia Arabia.
This publication acknowledges KAUST support, but has no KAUST affiliated authors.

ASJC Scopus subject areas

Biochemistry
Colloid and Surface Chemistry
General Chemistry
Catalysis

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10.1021/jacs.2c01169

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title = "Voltage-Gated Electrocatalysis of Efficient and Selective Methane Oxidation by Tricopper Clusters under Ambient Conditions",

abstract = "Selective methane oxidation is difficult chemistry. Here we describe a strategy for the electrocatalysis of selective methane oxidation by immobilizing tricopper catalysts on the cathodic surface. In the presence of dioxygen and methane, the activation of these catalysts above a threshold cathodic potential can initiate the dioxygen chemistry for O atom transfer to methane. The catalytic turnover is completed by facile electron injections into the tricopper catalysts from the electrode. This technology leads to dramatic enhancements in performance of the catalysts toward methane oxidation. Unprecedented turnover frequencies (>40 min–1) and high product throughputs (turnover numbers >30 000 in 12 h) are achieved for this challenging chemical transformation in water under ambient conditions. The technology is green and suitable for on-site direct conversion of methane into methanol.",

author = "Yi-Fang Tsai and Thiyagarajan Natarajan and Zhi-Han Lin and I-Kuen Tsai and Damodar Janmanchi and Chan, {Sunney I.} and Yu, {Steve S.-F.}",

note = "KAUST Repository Item: Exported on 2022-06-01 Acknowledgements: S.I.C. and S.S.S.F. acknowledge helpful discussions with Dr. David Wu, Institute of Chemistry, Academia Sinica, Taiwan and Dr. Cafer T. Yavuz, Chemical Science, Physical Science and Engineering Division, King Abdullah University of Science and Technology, Saudia Arabia. This publication acknowledges KAUST support, but has no KAUST affiliated authors.",

year = "2022",

month = may,

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doi = "10.1021/jacs.2c01169",

language = "English (US)",

journal = "Journal of the American Chemical Society",

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T1 - Voltage-Gated Electrocatalysis of Efficient and Selective Methane Oxidation by Tricopper Clusters under Ambient Conditions

AU - Tsai, Yi-Fang

AU - Natarajan, Thiyagarajan

AU - Lin, Zhi-Han

AU - Tsai, I-Kuen

AU - Janmanchi, Damodar

AU - Chan, Sunney I.

AU - Yu, Steve S.-F.

N1 - KAUST Repository Item: Exported on 2022-06-01 Acknowledgements: S.I.C. and S.S.S.F. acknowledge helpful discussions with Dr. David Wu, Institute of Chemistry, Academia Sinica, Taiwan and Dr. Cafer T. Yavuz, Chemical Science, Physical Science and Engineering Division, King Abdullah University of Science and Technology, Saudia Arabia. This publication acknowledges KAUST support, but has no KAUST affiliated authors.

PY - 2022/5/27

Y1 - 2022/5/27

N2 - Selective methane oxidation is difficult chemistry. Here we describe a strategy for the electrocatalysis of selective methane oxidation by immobilizing tricopper catalysts on the cathodic surface. In the presence of dioxygen and methane, the activation of these catalysts above a threshold cathodic potential can initiate the dioxygen chemistry for O atom transfer to methane. The catalytic turnover is completed by facile electron injections into the tricopper catalysts from the electrode. This technology leads to dramatic enhancements in performance of the catalysts toward methane oxidation. Unprecedented turnover frequencies (>40 min–1) and high product throughputs (turnover numbers >30 000 in 12 h) are achieved for this challenging chemical transformation in water under ambient conditions. The technology is green and suitable for on-site direct conversion of methane into methanol.

AB - Selective methane oxidation is difficult chemistry. Here we describe a strategy for the electrocatalysis of selective methane oxidation by immobilizing tricopper catalysts on the cathodic surface. In the presence of dioxygen and methane, the activation of these catalysts above a threshold cathodic potential can initiate the dioxygen chemistry for O atom transfer to methane. The catalytic turnover is completed by facile electron injections into the tricopper catalysts from the electrode. This technology leads to dramatic enhancements in performance of the catalysts toward methane oxidation. Unprecedented turnover frequencies (>40 min–1) and high product throughputs (turnover numbers >30 000 in 12 h) are achieved for this challenging chemical transformation in water under ambient conditions. The technology is green and suitable for on-site direct conversion of methane into methanol.

UR - http://hdl.handle.net/10754/678350

UR - https://pubs.acs.org/doi/10.1021/jacs.2c01169

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DO - 10.1021/jacs.2c01169

M3 - Article

C2 - 35622083

SN - 0002-7863

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

ER -

Voltage-Gated Electrocatalysis of Efficient and Selective Methane Oxidation by Tricopper Clusters under Ambient Conditions

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Bibliographical note

ASJC Scopus subject areas

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