期刊
JOURNAL OF MATERIALS CHEMISTRY A
卷 6, 期 44, 页码 22277-22286出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c8ta06743k
关键词
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资金
- National Natural Science Foundation of China (NSFC) [21571035]
- Award Program for Fujian Minjiang Scholar Professorship of Xiamen University (2015-18)
- open Project Foundation of Key Laboratory of Physical Chemistry of Solid Surfaces of Xiamen University (2015-18)
- open Project Foundation of Key Laboratory of Structural Chemistry of FJIRSM
- Fritz Haber Institute of Max Planck Society
- Max Planck Institute for Chemical Energy Conversion
- Max Planck Society
Heteroatom-doped two-dimensional (2D) carbon materials have been recognized as promising metal-free catalysts for the oxygen reduction reaction (ORR) due to their impressive surface activity. Such materials are often achieved by conventional chemical vapour deposition (CVD) growth followed by post-treatment of heteroatom-doping or obtained by template-guided polymerization and carbonization of organic substances. In this contribution, we report a new strategy that allows a direct conversion of threedimensional (3D) aggregates of guanine into naturally N/O-doped ultrathin few-layer carbon nanosheets without the use of any template or guiding agent. Moreover, by pre-ionizing guanine with H2SO4/H3PO4, a group of multiple heteroatom-doped (N/O/S, N/O/P, and N/O/S/P) 2D carbons can also be readily realized. Considering the low cost of precursors and the simplicity of the synthetic procedure, largescale production of such heteroatom-doped 2D carbons is potentially available. The best catalytic performance is obtained from the N/O/S/P-doped carbons which show a half-wave potential (E1/2) of 0.84 V vs. RHE and a diffusion-limited current density (j(L)) of 5.40 mA cm(-2) in 0.1 M KOH, better than those of most graphene-based catalysts and even the commercial Pt/C catalyst. Systematic studies indicate that the observed superior ORR performance arises from a combined effect of the multiple heteroatom-doping, high surface area and abundant structural defects of the electrocatalyst.
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