Confined local oxygen gas promotes electrochemical water oxidation to hydrogen peroxide

Chuan Xia, Seoin Back, Stefan Ringe, Fanhong Chen, Xiaoming Sun, Samira Siahrostami, Karen Chan*, Haotian Wang

*Corresponding author for this work

Research output: Contribution to journalJournal articleResearchpeer-review

Abstract

Electrochemical two-electron water oxidation is a promising route for renewable and on-site H2O2 generation as an alternative to the anthraquinone process. However, it is currently restricted by low selectivity due to strong competition from the traditional four-electron oxygen evolution reaction, as well as large overpotential and low production rates. Here we report an interfacial engineering approach, where by coating the catalyst with hydrophobic polymers we confine in-situ produced O2 gas to tune the water oxidation reaction pathway. Using carbon catalysts as a model system, we show a significant increase of the intrinsic H2O-to-H2O2 selectivity and activity compared to that of the pristine catalyst. The maximal H2O2 Faradaic efficiency was enhanced by 6-fold to 66% with an overpotential of 640 mV, under which H2O2 production rate of 23.4 µmol min-1 cm-2 (75.2 mA cm-2 partial current) was achieved. This approach was successfully extended to nickel metal, demonstrating the wide applicability of our local gas confinement concept.
Original languageEnglish
JournalNature Catalysis
DOIs
Publication statusAccepted/In press - 2020

Cite this

Xia, C., Back, S., Ringe, S., Chen, F., Sun, X., Siahrostami, S., ... Wang, H. (Accepted/In press). Confined local oxygen gas promotes electrochemical water oxidation to hydrogen peroxide. Nature Catalysis. https://doi.org/10.1038/s41929-019-0402-8
Xia, Chuan ; Back, Seoin ; Ringe, Stefan ; Chen, Fanhong ; Sun, Xiaoming ; Siahrostami, Samira ; Chan, Karen ; Wang, Haotian. / Confined local oxygen gas promotes electrochemical water oxidation to hydrogen peroxide. In: Nature Catalysis. 2020.
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title = "Confined local oxygen gas promotes electrochemical water oxidation to hydrogen peroxide",
abstract = "Electrochemical two-electron water oxidation is a promising route for renewable and on-site H2O2 generation as an alternative to the anthraquinone process. However, it is currently restricted by low selectivity due to strong competition from the traditional four-electron oxygen evolution reaction, as well as large overpotential and low production rates. Here we report an interfacial engineering approach, where by coating the catalyst with hydrophobic polymers we confine in-situ produced O2 gas to tune the water oxidation reaction pathway. Using carbon catalysts as a model system, we show a significant increase of the intrinsic H2O-to-H2O2 selectivity and activity compared to that of the pristine catalyst. The maximal H2O2 Faradaic efficiency was enhanced by 6-fold to 66{\%} with an overpotential of 640 mV, under which H2O2 production rate of 23.4 µmol min-1 cm-2 (75.2 mA cm-2 partial current) was achieved. This approach was successfully extended to nickel metal, demonstrating the wide applicability of our local gas confinement concept.",
author = "Chuan Xia and Seoin Back and Stefan Ringe and Fanhong Chen and Xiaoming Sun and Samira Siahrostami and Karen Chan and Haotian Wang",
year = "2020",
doi = "10.1038/s41929-019-0402-8",
language = "English",
journal = "Nature Catalysis",
issn = "2520-1158",
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Confined local oxygen gas promotes electrochemical water oxidation to hydrogen peroxide. / Xia, Chuan; Back, Seoin; Ringe, Stefan; Chen, Fanhong; Sun, Xiaoming; Siahrostami, Samira; Chan, Karen; Wang, Haotian.

In: Nature Catalysis, 2020.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - Confined local oxygen gas promotes electrochemical water oxidation to hydrogen peroxide

AU - Xia, Chuan

AU - Back, Seoin

AU - Ringe, Stefan

AU - Chen, Fanhong

AU - Sun, Xiaoming

AU - Siahrostami, Samira

AU - Chan, Karen

AU - Wang, Haotian

PY - 2020

Y1 - 2020

N2 - Electrochemical two-electron water oxidation is a promising route for renewable and on-site H2O2 generation as an alternative to the anthraquinone process. However, it is currently restricted by low selectivity due to strong competition from the traditional four-electron oxygen evolution reaction, as well as large overpotential and low production rates. Here we report an interfacial engineering approach, where by coating the catalyst with hydrophobic polymers we confine in-situ produced O2 gas to tune the water oxidation reaction pathway. Using carbon catalysts as a model system, we show a significant increase of the intrinsic H2O-to-H2O2 selectivity and activity compared to that of the pristine catalyst. The maximal H2O2 Faradaic efficiency was enhanced by 6-fold to 66% with an overpotential of 640 mV, under which H2O2 production rate of 23.4 µmol min-1 cm-2 (75.2 mA cm-2 partial current) was achieved. This approach was successfully extended to nickel metal, demonstrating the wide applicability of our local gas confinement concept.

AB - Electrochemical two-electron water oxidation is a promising route for renewable and on-site H2O2 generation as an alternative to the anthraquinone process. However, it is currently restricted by low selectivity due to strong competition from the traditional four-electron oxygen evolution reaction, as well as large overpotential and low production rates. Here we report an interfacial engineering approach, where by coating the catalyst with hydrophobic polymers we confine in-situ produced O2 gas to tune the water oxidation reaction pathway. Using carbon catalysts as a model system, we show a significant increase of the intrinsic H2O-to-H2O2 selectivity and activity compared to that of the pristine catalyst. The maximal H2O2 Faradaic efficiency was enhanced by 6-fold to 66% with an overpotential of 640 mV, under which H2O2 production rate of 23.4 µmol min-1 cm-2 (75.2 mA cm-2 partial current) was achieved. This approach was successfully extended to nickel metal, demonstrating the wide applicability of our local gas confinement concept.

U2 - 10.1038/s41929-019-0402-8

DO - 10.1038/s41929-019-0402-8

M3 - Journal article

JO - Nature Catalysis

JF - Nature Catalysis

SN - 2520-1158

ER -