State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai, 200050, P. R. China.
State Key Laboratory of Silicon Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, P. R. China.
Adv Mater. 2017 Aug;29(31). doi: 10.1002/adma.201701674. Epub 2017 Jun 19.
Conductive carbon nitride, as a hypothetical carbon material demonstrating high nitrogen doping, high electrical conductivity, and high surface area, has not been fabricated. A major challenge towards its fabrication is that high conductivity requires high temperature synthesis, but the high temperature eliminates nitrogen from carbon. Different from conventional methods, a facile preparation of conductive carbon nitride from novel thermal decomposition of nickel hydrogencyanamide in a confined space is reported. New developed nickel hydrogencyanamide is a unique precursor which provides self-grown fragments of ⋅NCN⋅ or NCCN and conductive carbon (C-sp ) catalyst of Ni metal during the decomposition. The final product is a tubular structure of rich mesoporous and microporous few-layer carbon with extraordinarily high N doping level (≈15 at%) and high extent of sp carbon (≈65%) favoring a high conductivity (>2 S cm ); the ultrahigh contents of nongraphitic nitrogen, redox active pyridinic N (9 at%), and pyrrolic N (5 at%), are stabilized by forming NiN bonds. The conductive carbon nitride harvests a large capacitance of 372 F g with >90% initial capacitance after 10 000 cycles as a supercapacitor electrode, far exceeding the activated carbon electrodes that have <250 F g .
导电氮化碳,作为一种理论上具有高氮掺杂、高导电性和高比表面积的碳材料,尚未被制备出来。其制备的一个主要挑战是,高导电性需要高温合成,但高温会将氮从碳中去除。与传统方法不同,本文报道了一种通过新颖的镍氢氰酸盐在受限空间内热分解来制备导电氮化碳的简便方法。新开发的镍氢氰酸盐是一种独特的前体,它在分解过程中提供了自生长的 ⋅NCN⋅ 或 NCCN 片段和镍金属的导电碳 (C-sp ) 催化剂。最终产物是一种具有丰富介孔和微孔的少层富碳的管状结构,具有极高的 N 掺杂水平(≈15 at%)和高比例的 sp 碳(≈65%),有利于高导电性(>2 S cm );非石墨氮、氧化还原活性的吡啶 N(9 at%)和吡咯 N(5 at%)的超高含量通过形成 NiN 键得以稳定。作为超级电容器电极,导电氮化碳具有 372 F g 的大电容,经过 10000 次循环后,初始电容保持率>90%,远超过具有<250 F g 的活性炭电极。