Volume 60, Issue 52 pp. 26922-26931
Research Article

Strongly Coupled Cobalt Diselenide Monolayers for Selective Electrocatalytic Oxygen Reduction to H2O2 under Acidic Conditions

Dr. Xiao-Long Zhang

Dr. Xiao-Long Zhang

Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, 230026 China

These authors contributed equally to this work.

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Xiaozhi Su

Xiaozhi Su

Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, CAS, Shanghai, 201210 China

These authors contributed equally to this work.

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Dr. Ya-Rong Zheng

Dr. Ya-Rong Zheng

Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, 230026 China

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Dr. Shao-Jin Hu

Dr. Shao-Jin Hu

Division of Theoretical and Computational Sciences, Hefei National Laboratory for Physical Sciences at Microscale, CAS Centre for Excellence and Synergetic Innovation Centre in Quantum Information and Quantum Physics, University of Science and Technology of China, Hefei, 230026 China

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Dr. Lei Shi

Dr. Lei Shi

Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, 230026 China

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Dr. Fei-Yue Gao

Dr. Fei-Yue Gao

Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, 230026 China

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Dr. Peng-Peng Yang

Dr. Peng-Peng Yang

Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, 230026 China

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Dr. Zhuang-Zhuang Niu

Dr. Zhuang-Zhuang Niu

Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, 230026 China

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Zhi-Zheng Wu

Zhi-Zheng Wu

Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, 230026 China

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Shuai Qin

Shuai Qin

Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, 230026 China

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Dr. Rui Wu

Dr. Rui Wu

Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, 230026 China

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Dr. Yu Duan

Dr. Yu Duan

Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, 230026 China

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Dr. Chao Gu

Dr. Chao Gu

Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, 230026 China

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Dr. Xu-Sheng Zheng

Dr. Xu-Sheng Zheng

National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230026 China

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Prof. Jun-Fa Zhu

Prof. Jun-Fa Zhu

National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230026 China

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Prof. Min-Rui Gao

Corresponding Author

Prof. Min-Rui Gao

Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, 230026 China

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First published: 22 September 2021
Citations: 100

Graphical Abstract

A strategy that narrows the interlayer distance of cobalt diselenide (CoSe2) is reported, which enables strong coupling between CoSe2 monolayers. The strongly coupled CoSe2 can catalyze electrosynthesis of H2O2 in acidic media efficiently, which yields Faradaic efficiency of 96.7 %, current density of 50.04 mA cm−2, and product rate of 30.60 mg cm−2 h−1, outperforming all catalysts reported previously in acidic environments.

Abstract

Electrosynthesis of hydrogen peroxide (H2O2) in the acidic environment could largely prevent its decomposition to water, but efficient catalysts that constitute entirely earth-abundant elements are lacking. Here we report the experimental demonstration of narrowing the interlayer gap of metallic cobalt diselenide (CoSe2), which creates high-performance catalyst to selectively drive two-electron oxygen reduction toward H2O2 in an acidic electrolyte. The enhancement of the interlayer coupling between CoSe2 atomic layers offers a favorable surface electronic structure that weakens the critical *OOH adsorption, promoting the energetics for H2O2 production. Consequently, on the strongly coupled CoSe2 catalyst, we achieved Faradaic efficiency of 96.7 %, current density of 50.04 milliamperes per square centimeter, and product rate of 30.60 mg cm−2 h−1. Moreover, this catalyst shows no sign of degradation when operating at −63 milliamperes per square centimeter over 100 hours.

Conflict of interest

The authors declare no conflict of interest.

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