A Polymer Encapsulation Strategy to Synthesize Porous Nitrogen-Doped Carbon-Nanosphere-Supported Metal Isolated-Single-Atomic-Site Catalysts

被引:298
作者
Han, Aijuan [1 ]
Chen, Wenxing [1 ]
Zhang, Shaolong [1 ]
Zhang, Maolin [1 ]
Han, Yunhu [1 ]
Zhang, Jian [1 ]
Ji, Shufang [1 ]
Zheng, Lirong [2 ]
Wang, Yu [3 ]
Gu, Lin [4 ]
Chen, Chen [1 ]
Peng, Qing [1 ]
Wang, Dingsheng [1 ]
Li, Yadong [1 ]
机构
[1] Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
[2] Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil, Beijing 100049, Peoples R China
[3] Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China
[4] Chinese Acad Sci, Inst Phys, Beijing 100190, Peoples R China
基金
中国国家自然科学基金;
关键词
isolated-single-atomic-site; oxygen reduction reaction; polymer; porous nitrogen-doped carbon; OXYGEN REDUCTION REACTION; FREE ELECTROCATALYSTS; COBALT; GRAPHENE; SPHERES; OXIDE; HYDROGENATION; SELECTIVITY; SURFACE;
D O I
10.1002/adma.201706508
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
A novel polymer encapsulation strategy to synthesize metal isolated-single-atomic-site (ISAS) catalysts supported by porous nitrogen-doped carbon nanospheres is reported. First, metal precursors are encapsulated in situ by polymers through polymerization; then, metal ISASs are created within the polymer-derived p-CN nanospheres by controlled pyrolysis at high temperature (200-900 degrees C). Transmission electron microscopy and N-2 sorption results reveal this material to exhibit a nanospheric morphology, a high surface area (approximate to 380 m(2) g(-1)), and a porous structure (with micropores and mesopores). Characterization by aberration-corrected high-angle annular dark-field scanning transmission electron microscopy and X-ray absorption fine structure confirms the metal to be present as metal ISASs. This methodology is applicable to both noble and nonprecious metals (M-ISAS/p-CN, M = Co, Ni, Cu, Mn, Pd, etc.). In particular, the Co-ISAS/p-CN nanospheres obtained using this method show comparable (E-1/2 = 0.838 V) electrochemical oxygen reduction activity to commercial Pt/C with 20 wt% Pt loading (E-1/2 = 0.834 V) in alkaline media, superior methanol tolerance, and outstanding stability, even after 5000 cycles.
引用
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页数:7
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