High-efficiency oxygen reduction to hydrogen peroxide catalysed by oxidized carbon materials

Lu, Zhiyi; Chen, Guangxu; Siahrostami, Samira; Chen, Zhihua; Liu, Kai; Xie, Jin; Liao, Lei; Wu, Tong; Lin, Dingchang; Liu, Yayuan; Jaramillo, Thomas F.; Norskov, Jens K.; Cui, Yi

doi:10.1038/s41929-017-0017-x

Title: High-efficiency oxygen reduction to hydrogen peroxide catalysed by oxidized carbon materials

Journal Article · Mon Jan 15 00:00:00 EST 2018 · Nature Catalysis

DOI:https://doi.org/10.1038/s41929-017-0017-x· OSTI ID:1458611

^[1]; Chen, Guangxu ^[1]; Siahrostami, Samira ^[1]; Chen, Zhihua ^[1]; Liu, Kai ^[1]; Xie, Jin ^[1]; Liao, Lei ^[1]; Wu, Tong ^[1]; Lin, Dingchang ^[1];

^[1]; Jaramillo, Thomas F. ^[1]; Norskov, Jens K. ^[2]; Cui, Yi ^[2]

Stanford Univ., Stanford, CA (United States)
Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)

Hydrogen peroxide (H₂O₂) is a valuable chemical with a wide range of applications, but the current industrial synthesis of H₂O₂ involves an energy-intensive anthraquinone process. The electrochemical synthesis of H₂O₂ from oxygen reduction offers an alternative route for on-site applications; the efficiency of this process depends greatly on identifying cost-effective catalysts with high activity and selectivity. Here, we demonstrate a facile and general approach to catalyst development via the surface oxidation of abundant carbon materials to significantly enhance both the activity and selectivity (~90%) for H₂O₂ production by electrochemical oxygen reduction. We find that both the activity and selectivity are positively correlated with the oxygen content of the catalysts. In conclusion, the density functional theory calculations demonstrate that the carbon atoms adjacent to several oxygen functional groups (–COOH and C–O–C) are the active sites for oxygen reduction reaction via the two-electron pathway, which are further supported by a series of control experiments.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1458611

Journal Information:: Nature Catalysis, Vol. 1, Issue 2; ISSN 2520-1158

Publisher:: Springer NatureCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 789 works

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Synergistic effects of carbon-encapsulated cobalt/tricobalt tetroxide nanocapsules on hydrogenation of 4-nitrophenol Yang, Xi; Chen, Yan; Xu, Xinchao Functional Materials Letters, Vol. 12, Issue 04 https://doi.org/10.1142/s1793604719500590	journal	August 2019
Recent Advances in the Direct Synthesis of Hydrogen Peroxide Using Chemical Catalysis—A Review Ranganathan, Sumanth; Sieber, Volker Catalysts, Vol. 8, Issue 9 https://doi.org/10.3390/catal8090379	journal	September 2018
Activated Carbon as a Cathode for Water Disinfection through the Electro-Fenton Process Chen, Long; Pinto, Ameet; Alshawabkeh, Akram N. Catalysts, Vol. 9, Issue 7 https://doi.org/10.3390/catal9070601	journal	July 2019
Enhanced Electrocatalytic Behaviour of Poy(aniline-co-2-hydroxyaniline) Coated Electrodes for Hydrogen Peroxide Electrooxidation Shah, Anwar ul Haq Ali; Inayat, Ayesha; Bilal, Salma Catalysts, Vol. 9, Issue 8 https://doi.org/10.3390/catal9080631	journal	July 2019
Hydrogen peroxide synthesis on porous graphitic carbon nitride using water as a hydrogen source Cao, Yongyong; Zhou, Guobing; Chen, Xianlang Journal of Materials Chemistry A, Vol. 8, Issue 1 https://doi.org/10.1039/c9ta08103h	journal	January 2020
Designing Aqueous Organic Electrolytes for Zinc–Air Batteries: Method, Simulation, and Validation Clark, Simon; Mainar, Aroa Ramos; Iruin, Elena Karlsruhe https://doi.org/10.5445/ir/1000105839	text	January 2020
Electrosynthesis of Hydrogen Peroxide Synergistically Catalyzed by Atomic Co–N _x –C Sites and Oxygen Functional Groups in Noble‐Metal‐Free Electrocatalysts Li, Bo‐Quan; Zhao, Chang‐Xin; Liu, Jia‐Ning Advanced Materials, Vol. 31, Issue 35 https://doi.org/10.1002/adma.201904044	journal	July 2019
Designing Aqueous Organic Electrolytes for Zinc-Air Batteries: Method, Simulation, and Validation Clark, Simon; Mainar, Aroa R.; Iruin, Elena arXiv https://doi.org/10.48550/arxiv.1909.11461	text	January 2019
Electrochemically derived functionalized graphene for bulk production of hydrogen peroxide Yeddala, Munaiah; Thakur, Pallavi; A., Anugraha Beilstein Journal of Nanotechnology, Vol. 11 https://doi.org/10.3762/bjnano.11.34	journal	March 2020

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY