Haibin Wang , Yuanyuan Cong , Yi Wang , Chunlei Li , Mengling Liu , Qiuping Zhao , Xueliang Wang , Junying Tian
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引用次数: 0
Abstract
Platinum (Pt)-based single atoms and alloys represent reasonable structures to reduce the cost of electrocatalysts for the oxygen reduction reaction (ORR). However, the poor oxygen adsorption of single Pt atoms and the unfavorable surface microenvironment of alloy electrodes limit their practical applications. To address these issues, we have engineered a synergistic hybrid structure by anchoring PtNi alloys onto defective carbon (DC) modified with Pt and Ni single atoms, followed by surface modification with 2,6-diacetylpyridine (DAP) molecules. The mass activity (MA) of the optimized DAP-PtNi/Pt&Ni-SAC electrocatalyst reaches 1678.9 mA mgPt−1, which is 10.21 times that of commercial JM Pt/C (164.5 mA mgPt−1). Moreover, after 20,000 accelerated durability tests (ADTs), DAP-PtNi/Pt&Ni-SAC shows only a 7.9% loss in MA, demonstrating its outstanding stability. Structural characterization and theoretical calculations reveal that the interaction of Ni single atoms and PtNi alloys enhances the adsorption stability of O2 molecules at Pt single atoms, facilitating a 4-electron ORR pathway. Meanwhile, DAP molecules adsorbed on Pt alloy sites associate with various oxygen-containing intermediates and protons through electrostatic interactions, promoting their combination. This synergistic effect between the intrinsic structure and the electrochemical microenvironment optimizes the ORR pathway in an overall manner, thus improving the kinetics of ORR.
期刊介绍:
The Journal of Energy Chemistry, the official publication of Science Press and the Dalian Institute of Chemical Physics, Chinese Academy of Sciences, serves as a platform for reporting creative research and innovative applications in energy chemistry. It mainly reports on creative researches and innovative applications of chemical conversions of fossil energy, carbon dioxide, electrochemical energy and hydrogen energy, as well as the conversions of biomass and solar energy related with chemical issues to promote academic exchanges in the field of energy chemistry and to accelerate the exploration, research and development of energy science and technologies.
This journal focuses on original research papers covering various topics within energy chemistry worldwide, including:
Optimized utilization of fossil energy
Hydrogen energy
Conversion and storage of electrochemical energy
Capture, storage, and chemical conversion of carbon dioxide
Materials and nanotechnologies for energy conversion and storage
Chemistry in biomass conversion
Chemistry in the utilization of solar energy