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通过取向引导与原位活化方法相结合制备的氮掺杂多孔碳具有优异的电容存储性能。

Excellent capacitive storage performance of N-doped porous carbon derived from the orientation-guidance coupled with in-situ activation methodology.

作者信息

Yang Yin, Du Haisheng, Wang Aocheng, Lu Changbo, Sun Dong, Lu Chun, Wang Xilong, Xiao Zhihua, Ma Xinlong

机构信息

State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Beijing 102249, China.

State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Beijing 102249, China.

出版信息

J Colloid Interface Sci. 2024 Nov;673:657-668. doi: 10.1016/j.jcis.2024.05.237. Epub 2024 Jun 5.

DOI:10.1016/j.jcis.2024.05.237
PMID:38901356
Abstract

The orientation-guidance coupled with in-situ activation methodology is developed to synthesize the N-doped porous carbon (NPC) with well-developed porosity and high specific surface area, using coal pitch as a carbon precursor. The orientation-guidance and activation are dedicated to generating microporous and mesoporous channels, respectively. The in-situ N incorporation into the carbon skeleton is realized along with the formation of porous carbon (PC), ensuring the uniformity of N doping. As an electrode material of supercapacitor, benefiting from the robust hexagon-like building block decorated with micro-mesoporous channels and N doping, NPC electrode affords a significant improvement in capacitive energy-storage performance, achieving a specific capacitance of up to 333F g at 1 A/g, which far exceeds those of PC and activated carbon. Notably, even under high mass loading of 10 mg cm, the NPC maintains a satisfactory capacitance of 258F g at 1 A/g. When employed as the anode in Li-ion capacitor (LIC), apart from exhibiting enhanced anode behavior compared to graphite anode, NPC also delivers exceptional cyclability. Furthermore, density functional theory calculations have validated the enhanced electrical conductivity and Li storage ability contributed by N doping, providing a theoretical foundation for the observed improvements in electrochemical performance. A full LIC configured with NPC anode delivers extraordinary Ragone performance and outstanding cyclability. This work also proposes a feasible way to realize the oriented conversion of coal pitch into high-performance electrode materials for electrochemical energy-storage devices.

摘要

本文开发了一种取向引导与原位活化相结合的方法,以煤沥青为碳前驱体,合成具有发达孔隙率和高比表面积的氮掺杂多孔碳(NPC)。取向引导和活化分别致力于生成微孔和介孔通道。氮原位掺入碳骨架的过程与多孔碳(PC)的形成同步实现,确保了氮掺杂的均匀性。作为超级电容器的电极材料,得益于由微介孔通道修饰的坚固六边形结构单元以及氮掺杂,NPC电极在电容储能性能方面有显著提升,在1 A/g电流密度下比电容高达333 F/g,远远超过PC和活性炭。值得注意的是,即使在10 mg/cm²的高质量负载下,NPC在1 A/g电流密度下仍保持258 F/g的令人满意的电容。当用作锂离子电容器(LIC)的阳极时,NPC除了表现出比石墨阳极更强的阳极性能外,还具有出色的循环稳定性。此外,密度泛函理论计算验证了氮掺杂对电导率和锂存储能力的增强作用,为观察到的电化学性能改善提供了理论基础。配置NPC阳极的全LIC展现出卓越的Ragone性能和出色的循环稳定性。这项工作还提出了一种将煤沥青定向转化为用于电化学储能装置的高性能电极材料的可行方法。

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