DataVXACS Applied Materials & InterfacesPaper
journal article·2021-04-14

Structural Evolution and Underlying Mechanism of Single-Atom Centers on Mo2C(100) Support during Oxygen Reduction Reaction

Xiang Huang, Jiong Wang, Jiajian Gao, Zhe Zhang, Li-Yong Gan, Hu Xu

ACS Applied Materials & Interfaces· Volume 13· Issue 14
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Source abstract

Abstract

The single-metal atoms coordinating with the surface atoms of the support constitute the active centers of as-prepared single-atom catalysts (SACs). However, under hash electrochemical conditions, (1) supports’ surfaces may experience structural change, which turn to be distinct from those at ambient conditions; (2) during catalysis, the dynamic responses of a single atom to the attack of reaction intermediates likely change the coordination environment of a single atom. These factors could alter the performance of SACs. Herein, we investigate these issues using Mo2C(100)-supported single transition-metal (TM) atoms as model SACs toward catalyzing the oxygen reduction reaction (ORR). It is found that the Mo2C(100) surface is oxidized under ORR turnover conditions, resulting in significantly weakened bonding between single TM atoms and the Mo2C(100) surface (TM@Mo2C(100)_O* term for SAC). While the intermediate in 2 e– ORR does not change the local structures of the active centers in these SACs, the O* intermediate emerging in 4 e– ORR can damage Rh@ and Cu@Mo2C(100)_O*. Furthermore, on the basis of these findings, we propose Pt@Mo2C(100)_O* as a qualified ORR catalyst, which exhibits extraordinary 4 e– ORR activity with an overpotential of only 0.33 V, surpassing the state-of-the-art Pt(111), and thus being identified as a promising alternative to the commercial Pt/C catalyst.
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Research context

Catalysis & surfaces

OpenAlex topics: Electrocatalysts for Energy Conversion · Catalytic Processes in Materials Science · Fuel Cells and Related Materials

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

Affiliations

Department of Physics, Southern University of Science and Technology, Shenzhen 518055, China

Institute of Advanced Synthesis (IAS), School of Chemistry and Chemical Engineering, Northwestern Polytechnical University (NPU), Xi’an 710072, China

Yangtze River Delta Research Institute of NPU, Taicang Jiangsu, 215400, China

School of Chemical and Biomedical Engineering, Nanyang Technological University, 62 Nanyang Drive, Singapore 637459, Singapore

Institute for Structure and Function and Department of Physics, Chongqing University, Chongqing 400030, China

Guangdong Provincial Key Laboratory of Computational Science and Material Design, Southern University of Science and Technology, Shenzhen 518055, China

Guangdong-Hong Kong-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices, Southern University of Science and Technology, Shenzhen 518055, China

Funding

National Natural Science Foundation of China · Guangdong-Hong Kong-Macao Joint Laboratory · Guangdong Natural Science Funds for Distinguished Young Scholars · Guangdong Provincial Key Laboratory of Computational Science and Material Design · National Natural Science Foundation of Jiangsu, China

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