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氮掺杂多孔石墨碳作为先进超级电容器的优秀电极材料。

Nitrogen-doped porous graphitic carbon as an excellent electrode material for advanced supercapacitors.

机构信息

Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education of the People's Republic of China, Heilongjiang University, Harbin 150080 (P. R. China), Fax: (+86) 451-8666-1259.

出版信息

Chemistry. 2014 Jan 7;20(2):564-74. doi: 10.1002/chem.201303345. Epub 2013 Dec 4.

Abstract

An advanced supercapacitor material based on nitrogen-doped porous graphitic carbon (NPGC) with high a surface area was synthesized by means of a simple coordination-pyrolysis combination process, in which tetraethyl orthosilicate (TEOS), nickel nitrate, and glucose were adopted as porogent, graphitic catalyst precursor, and carbon source, respectively. In addition, melamine was selected as a nitrogen source owing to its nitrogen-enriched structure and the strong interaction between the amine groups and the glucose unit. A low-temperature treatment resulted in the formation of a NPGC precursor by combination of the catalytic precursor, hydrolyzed TEOS, and the melamine-glucose unit. Following pyrolysis and removal of the catalyst and porogent, the NPGC material showed excellent electrical conductivity owing to its high crystallinity, a large Brunauer-Emmett-Teller surface area (SBET =1027 m(2)  g(-1) ), and a high nitrogen level (7.72 wt %). The unusual microstructure of NPGC materials could provide electrochemical energy storage. The NPGC material, without the need for any conductive additives, showed excellent capacitive behavior (293 F g(-1) at 1 A g(-1) ), long-term cycling stability, and high coulombic efficiency (>99.9 % over 5000 cycles) in KOH when used as an electrode. Notably, in a two-electrode symmetric supercapacitor, NPGC energy densities as high as 8.1 and 47.5 Wh kg(-1) , at a high power density (10.5 kW kg(-1) ), were achieved in 6 M KOH and 1 M Et4 NBF4 -PC electrolytes, respectively. Thus, the synthesized NPGC material could be a highly promising electrode material for advanced supercapacitors and other conversion devices.

摘要

一种基于具有高比表面积的氮掺杂多孔石墨碳(NPGC)的先进超级电容器材料是通过简单的配位-热解组合工艺合成的,其中正硅酸乙酯(TEOS)、硝酸镍和葡萄糖分别用作孔原剂、石墨催化剂前体和碳源。此外,由于三聚氰胺具有富氮结构和胺基与葡萄糖单元之间的强相互作用,选择三聚氰胺作为氮源。低温处理导致催化前体、水解的 TEOS 和三聚氰胺-葡萄糖单元结合形成 NPGC 前体。经过热解和催化剂及孔原剂的去除,NPGC 材料表现出优异的导电性,这归因于其高结晶度、大 Brunauer-Emmett-Teller 比表面积(SBET=1027 m2 g-1)和高氮水平(7.72wt%)。NPGC 材料的异常微观结构可以提供电化学储能。NPGC 材料无需任何导电添加剂,在用作电极时,在 KOH 中表现出出色的电容性能(在 1 A g-1时为 293 F g-1)、长期循环稳定性和高库仑效率(超过 5000 次循环时>99.9%)。值得注意的是,在两电极对称超级电容器中,在 6 M KOH 和 1 M Et4 NBF4-PC 电解质中,NPGC 的能量密度分别高达 8.1 和 47.5 Wh kg-1,在 10.5 kW kg-1的高功率密度下,实现了高达 8.1 和 47.5 Wh kg-1的能量密度。因此,合成的 NPGC 材料可能是先进超级电容器和其他转换设备的极具前途的电极材料。

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