期刊
JOURNAL OF COLLOID AND INTERFACE SCIENCE
卷 606, 期 -, 页码 177-191出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcis.2021.08.010
关键词
Imidazolium ionic liquids; Pt nanocrystals; Oxygen reduction reaction; N-doped hollow carbon spheres; Density functional theory
资金
- National Natural Science Foundation of China [52001173]
- General Project of Natural Science Research in Jiangsu Colleges and Universities [20KJB430046]
- Research Fund of Nantong University [03083030]
- Large Instruments Open Foundation of Nantong University [KFJN2128]
The Pt-NHCS catalysts with Pt nanocrystals anchored on carbon shells show excellent stability and long-term durability in both alkaline and acid electrolytes, with a high efficiency and sustainable performance for oxygen reduction reactions.
Here, N-doped hollow carbon sphere (NHCS)-supported (111)-plane-engineered sub-5-nm Pt (Pt-NHCS) catalysts regulated precisely by imidazolium ionic liquids were synthesized successfully and used to catalyze oxygen reduction. The (1 1 1)-plane engineered Pt nanocrystals with a diameter of 4.5 +/- 0.5 nm were homogeneously deposited on the 3-dimensional spherical nanoshells. The resulting Pt nanocrystals anchored on the carbon skeleton exhibit a stable configuration in both alkaline and acid electrolytes with the help of imidazolium cations and pyrolysis. Among all as-prepared catalysts, the optimized Pt-NHCS shows remarkable long-term durability. Specifically, Pt-NHCS maintains 95.3% of the original current density after 10,000 potential cycles, while Pt/C benchmarks exhibit a retention of 78.5%. Accelerated durability test results indicate that Pt-NHCS exhibits a high efficiency of 96 % in comparison with initial current density, while a value of 86% for Pt/C. Density functional theory calculations demonstrate that reactive Pt(1 1 1) planes with well-defined Schottky defects and vacancies adsorb and activate oxygen molecule rapidly while desorbing the reaction intermediates. (c) 2021 Elsevier Inc. All rights reserved.
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