Field of Environment and Energy, School of Materials Science, Japan Advanced Institute of Science and Technology, 1-1 Asahidai, Nomi, 923-1292, Japan.
School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, 200240, P. R. China.
Adv Mater. 2018 Apr;30(15):e1706330. doi: 10.1002/adma.201706330. Epub 2018 Mar 5.
Progress over the past decades in porous materials has exerted great effect on the design of metal-free carbon electrochemical catalysts in fuel cells. The carbon material must combine three functions, i.e., electrical conductivity for electron transport, optimal pores for ion motion, and abundant heteroatom sites for catalysis. Here, an ideal carbon catalyst is achieved by combining two strategies-the use of a 2D covalent organic framework (COF) and the development of a suitable template to guide the pyrolysis. The COF produces nanosized carbon sheets that combine high conductivity, hierarchical porosity, and abundant heteroatom catalytic edges. The catalysts achieve superior performance to authentic Pt/C with exceptional onset potential (0 V vs -0.03 V), half-wave potentials (-0.11 V vs -0.16 V), high limit current density (7.2 mA cm vs 6.0 mA cm ), low Tafel slope (110 mV decade vs 121 mV decade ), long-time stability, and methanol tolerance. These results reveal a novel material platform based on 2D COFs for designing novel 2D carbon materials.
过去几十年在多孔材料方面的进展对燃料电池中无金属碳电化学催化剂的设计产生了巨大的影响。碳材料必须结合三种功能,即电子传输的导电性、离子运动的最佳孔和丰富的杂原子催化位。在这里,通过结合两种策略——使用二维共价有机骨架(COF)和开发合适的模板来指导热解,实现了理想的碳催化剂。COF 生成了纳米级的碳片,具有高导电性、分级多孔性和丰富的杂原子催化边缘。与真实的 Pt/C 相比,催化剂具有优异的起始电位(0 V 对-0.03 V)、半波电位(-0.11 V 对-0.16 V)、高极限电流密度(7.2 mA cm 对 6.0 mA cm )、低塔菲尔斜率(110 mV 对 121 mV)、长时间稳定性和甲醇耐受性。这些结果揭示了一种基于二维 COF 的新型材料平台,用于设计新型二维碳材料。