期刊
JOURNAL OF COLLOID AND INTERFACE SCIENCE
卷 606, 期 -, 页码 1833-1841出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcis.2021.08.180
关键词
Metal-organic framework; Porous carbon; Carbon nanotube; Oxygen reduction reaction; Zn-air battery
资金
- State Key Laboratory of Structural Chemistry, Chinese Academy of Sciences [20190008]
- Basic Science and Technology Research Project of Wenzhou, Zhejiang Province [G20190007, ZG2017027]
- Graduate Scientific Research Foundation of Wenzhou University [316202002038]
The rational design and preparation of hierarchically porous N-doped carbon nanotubes grafted onto zinc-based coordination polymer derived carbon nanomaterials for efficient oxygen reduction reaction (ORR) catalysis is proposed in this study. The Fe-NCNT catalyst exhibits optimal ORR activity with high onset potential, half-wave potential, and diffusion-limited current density, showcasing potential for high-performance Zn-air batteries. This method demonstrates a new route for the facile construction of efficient nanocatalysts for advanced energy applications.
The rational design and preparation of nonprecious metal-based oxygen reduction reaction (ORR) catalysts to facilitate electron and mass transport are of great significance in oxygen-involved energy applications. Herein, a stepwise approach to synthesize a type of hierarchically porous N-doped carbon nanotubes (CNTs) grafted onto zinc-based coordination polymer derived carbon nanomaterials (M-NCNT, M = Fe/Co/Ni) is proposed. At first, an isostructural zinc-based metal-organic framework (MOF) to HKUST-1(Cu) (ZnHKUST-1) is solvothermally prepared, and then under pyrolysis to obtain MOF-derived porous carbon. After the secondary calcination, the in-situ formed N-doped CNTs are efficiently catalyzed by iron group metal-based nanoparticles (Fe/Co/Ni), which are thermally reduced by porous carbon together with additional urea. The synergistic effect between ultrahigh porosity, large surface area, suitable N-doping, high graphitization degree, and ultrafine metal particles prompts M-NCNT series to exhibit satisfactory electrocatalysis in oxygen reduction. Among them, Fe-NCNT owns the optimal ORR activity with high positive onset potential (0.987 V), half-wave potential (0.860 V) and large diffusion-limited current density (4.893 mA cm-2). Meanwhile, it shows a high current retention of 90.7% after the 24-hour stability, and the obtained Zn-air battery by Fe-NCNT with open-circuit voltage of 1.44 V owns moderate capacity and satisfying stability. The demonstrated method to prepare hierarchically porous N-doped carbon nanomaterials stemmed from MOF precursors unfolds a new route for the facile construction of efficient nanocatalysts for advanced energy applications. (C) 2021 Elsevier Inc. All rights reserved.
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