journal article·2022-10Open access

Black Phosphorous Mediates Surface Charge Redistribution of CoSe2 for Electrochemical H2O2 Production in Acidic Electrolytes

Ya‐Rong Zheng, ShaoJin Hu, Xiao‐Long Zhang, Huanxin Ju, Zhenbin Wang, Peng‐Ju Tan, Rui Wu, Fei‐Yue Gao, Taotao Zhuang, Xiao Zheng, Junfa Zhu, Min‐Rui Gao, Shu‐Hong Yu

Advanced Materials· Volume 34· Issue 43

Abstract

Abstract Electrochemical generation of hydrogen peroxide (H2O2) by two‐electron oxygen reduction offers a green method to mitigate the current dependence on the energy‐intensive anthraquinone process, promising its on‐site applications. Unfortunately, in alkaline environments, H2O2 is not stable and undergoes rapid decomposition. Making H2O2 in acidic electrolytes can prevent its decomposition, but choices of active, stable, and selective electrocatalysts are significantly limited. Here, the selective and efficient two‐electron reduction of oxygen toward H2O2 in acid by a composite catalyst that is composed of black phosphorus (BP) nailed chemically on the metallic cobalt diselenide (CoSe2) surface is reported. It is found that this catalyst exhibits a 91% Faradic efficiency for H2O2 product at an overpotential of 300 mV. Moreover, it can mediate oxygen to H2O2 with a high production rate of ≈1530 mg L−1 h−1 cm−2 in a flow‐cell reactor. Spectroscopic and computational studies together uncover a BP‐induced surface charge redistribution in CoSe2, which leads to a favorable surface electronic structure that weakens the HOO* adsorption, thus enhancing the kinetics toward H2O2 formation.
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Research context

OpenAlex topics: Electrocatalysts for Energy Conversion · Advanced battery technologies research · Chalcogenide Semiconductor Thin Films

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Chemistry Institute of Biomimetic Materials & Chemistry Anhui Engineering Laboratory of Biomimetic Materials Division of Nanomaterials & Chemistry Hefei National Laboratory for Physical Sciences at the Microscale University of Science and Technology of China Hefei Anhui 230026 P. R. China

Anhui Province Key Laboratory of Advanced Catalytic Materials and Reaction Engineering School of Chemistry and Chemical Engineering Hefei University of Technology Hefei Anhui 230009 P. R. China

Department of Chemical Physics Division of Theoretical and Computational Sciences Hefei National Laboratory for Physical Sciences at the Microscale University of Science and Technology of China Hefei Anhui 230026 P. R. China

National Synchrotron Radiation Laboratory University of Science and Technology of China Hefei Anhui 230026 P. R. China

CatTheory Department of Physics Technical University of Denmark 2800 Kongens Lyngby Denmark

Institute of Innovative Materials Department of Materials Science and Engineering Department of Chemistry Southern University of Science and Technology Shenzhen 518055 P. R. China

Funding

National Natural Science Foundation of China · National Basic Research Program of China · China Postdoctoral Science Foundation

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