基于结构调节碳材料的掺氮种类和含量及其超级电容器储能应用  

Tuning Nitrogen Species and Content in Carbon Materials through Constructing Variable Structures for Supercapacitors

作　　者：孙鹏 张绍宁 毕辉[1] 董武杰 黄富强[1,3,4] SUN Peng;ZHANG Shaoning;BI Hui;DONG Wujie;HUANG Fuqiang(State Key Laboratory of High Performance Ceramics and Superfine Microstructure,Shanghai Institute of Ceramics,Chinese Academy of Sciences,Shanghai 200050,China;Center of Materials Science and Optoelectronics Engineering,University of Chinese Academy of Sciences,Beijing 100049,China;School of Physical Science and Technology,ShanghaiTech University,Shanghai 200031,China;State Key Laboratory of Rare Earth Materials Chemistry and Applications,College of Chemistry and Molecular Engineering,Peking University,Beijing 100871,China)

机构地区：[1]中国科学院上海硅酸盐研究所,高性能陶瓷和超微结构国家重点实验室,上海200050 [2]中国科学院大学材料科学与光电技术学院,北京100049 [3]上海科技大学物理科学与技术学院,上海200031 [4]北京大学化学与分子工程学院,稀土材料化学及应用国家重点实验室,北京100871

出　　处：《无机材料学报》2021年第7期766-772,I0007-I0011,共12页Journal of Inorganic Materials

基　　金：National Key Research and Development Program of China(2016YFB0901600);National Natural Science Foundation of China(51972326,51672295,21871008,51672301);Science and Technology Commission of Shanghai(18YF1427200);The Key Research Program of Chinese Academy of Sciences(QYZDJ-SSW-JSC013)。

摘　　要：碳材料是极具潜力的超级电容器电极材料,但是其容量较低。异质原子掺杂,尤其是氮掺杂,是大幅度提高碳材料电化学性能的有效方法。但是在碳材料中实现高含量的活性氮掺杂仍极具挑战。本研究通过Si–O–Si网络和氧化铝之间的相互作用成功调节碳材料的掺氮种类及其含量。除此之外,通过调节前驱体组成,碳材料的结构可以从珊瑚状转变为三维结构。在反应中,氧化物中的氧原子可以和碳材料中氮原子成键,氮原子不易逃离,从而实现高含量氮掺杂(5.29at%@1000℃)。另一方面,相互作用使碳材料孔体积增大(1.78 m^(3)·g^(-1))和孔径分布加宽(0.5~60 nm)。因此,获得的富氮掺杂碳材料具有302 F·g^(-1)@1 A·g^(-1)的高容量和177 F·g^(-1)@120 A·g^(-1)的杰出倍率性能。此独特的固氮方法是一种有潜力的制备高性能超级电容器电极材料的策略。Carbon materials are favorable for supercapacitors but suffer from insufficient capacitance.Heteroatom doping,especially nitrogen(N)doping,is an effective method to significantly improve the electrochemical performance,but it is still a big challenge to achieve high active nitrogen content in carbon materials.This work successfully tuned nitrogen species and content by interaction between Si–O–Si network and aluminum oxide.Besides,the structure of carbon materials varies from a coral-like network to three-dimensional structure by adjusting the precursor composition.Oxygen(O)in oxides bonds with N in carbon materials during the reaction,which makes it difficult to escape,achieving high nitrogen content of 5.29at%at 1000℃.On the other hand,the interaction empowers the carbon material with large pore volume of~1.78 cm^(3)·g^(-1) and broad pore size distribution of 0.5–60 nm.Thus,the N-rich carbon material harvests high capacitance of 302 F·g^(-1) at 1 A·g^(-1) and excellent rate capability of 177 F·g^(-1) at 120 A·g^(-1).This unique nitrogen fixation method is a promising strategy for preparing high performance electrode materials of supercapacitors.

关 键 词：碳材料 氮原子固定 相互作用 形貌设计 超级电容器 

分 类 号：O782[理学—晶体学]