Atomically dispersed Zn-Co-N-C catalyst boosting efficient and robust oxygen reduction catalysis in acid via stabilizing Co-N bonds

Feng Ma; Xuan Liu; Xiaoming Wang; Jiashun Liang; Jianyu Huang; Cameron Priest; Jinjia Liu; Shuhong Jiao; Tanyuan Wang; Gang Wu; Yunhui Huang; Qing Li

Fundamental Research (Nov 2023)

Atomically dispersed Zn-Co-N-C catalyst boosting efficient and robust oxygen reduction catalysis in acid via stabilizing Co-N bonds

Feng Ma,
Xuan Liu,
Xiaoming Wang,
Jiashun Liang,
Jianyu Huang,
Cameron Priest,
Jinjia Liu,
Shuhong Jiao,
Tanyuan Wang,
Gang Wu,
Yunhui Huang,
Qing Li

Affiliations

Feng Ma: State Key Laboratory of Material Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, Hubei 430074, China; State Key Laboratory of Refractories and Metallurgy, Institute of Advanced Materials and Nanotechnology, Key Laboratory of Hubei Province for Coal Conversion and New Carbon Materials, School of Chemistry and Chemical Engineering, Wuhan University of Science and Technology, Wuhan 430081, China
Xuan Liu: State Key Laboratory of Material Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, Hubei 430074, China
Xiaoming Wang: Department of Chemistry and Key Laboratory for Preparation and Application of Ordered Structural Materials of Guangdong Province, Shantou University, Shantou 515063, China
Jiashun Liang: State Key Laboratory of Material Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, Hubei 430074, China
Jianyu Huang: Clean Nano Energy Center, State Key Laboratory of Metastable Materials Science and Technology, Yanshan University, Qinhuangdao 066004, China
Cameron Priest: Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, NY 14260, United States
Jinjia Liu: State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China; National Energy Center for Coal to Clean Fuels, Synfuels China Co., Ltd, Huairou District, Beijing 101400, China
Shuhong Jiao: Department of Materials Science and Engineering, Key Laboratory of Materials for Energy Conversion Chinese Academy of Science (CAS), University of Science and Technology of China, Hefei 230026, China
Tanyuan Wang: State Key Laboratory of Material Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, Hubei 430074, China
Gang Wu: Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, NY 14260, United States
Yunhui Huang: State Key Laboratory of Material Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, Hubei 430074, China
Qing Li: State Key Laboratory of Material Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, Hubei 430074, China; Corresponding author.

Journal volume & issue: Vol. 3, no. 6
pp. 909 – 917

Abstract

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Transition metal supported N-doped carbon (M-N-C) catalysts for oxygen reduction reaction (ORR) are viewed as the promising candidate to replace Pt-group metal (PGM) for proton exchange membrane fuel cells (PEMFCs). However, the stability of M-N-C is extremely challenging due to the demetalation, H2O2 attack, etc. in the strongly oxidative conditions of PEMFCs. In this study, we demonstrate the universal effect of Zn on promoting the stability of atomically dispersed M-Nx/C (M = Co, Fe, Mn) catalysts and the enhancement mechanism is unveiled for the first time. The best-performing dual-metal-site Zn-Co-N-C catalyst exhibits a high half-wave potential (E1/2) value of 0.81 V vs. reversible hydrogen electrode (RHE) in acid and outstanding durability with no activity decay after 15,000 accelerated degradation test (ADT) cycles at 60 °C, surpassing most reported Co-based PGM-free catalysts in acid media. For comparison, the Co-N-C in the absence of Zn suffers from a rapid degradation after ADT due to the demetalation and higher H2O2 yield. X-ray adsorption spectroscopy (XAS) and density functional theory (DFT) calculations suggest the more negative formation energy (by 1.2 eV) and increased charge transfer of Zn-Co dual-site structure compared to Co-N-C could strength the Co-N bonds against the demetalation and the optimized d-band center accounts for the improved ORR kinetics.

Published in Fundamental Research

ISSN: 2667-3258 (Online)
Publisher: KeAi Communications Co. Ltd.
Country of publisher: China
LCC subjects: Science: Science (General)
Website: https://www.keaipublishing.com/en/journals/fundamental-research/

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