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原位热解追踪与实时相演变:从二元锌簇到超级电容多孔碳

In Situ Pyrolysis Tracking and Real-Time Phase Evolution: From a Binary Zinc Cluster to Supercapacitive Porous Carbon.

作者信息

Wang Yi-Fan, Liang Yiyu, Wu Yan-Fang, Yang Jian, Zhang Xu, Cai Dandan, Peng Xu, Kurmoo Mohamedally, Zeng Ming-Hua

机构信息

Hubei Collaborative Innovation Center for Advanced Organic Chemical Materials, Ministry-of-Education Key Laboratory for the Synthesis and Application of Organic Functional Molecules, College of Chemistry & Chemical Engineering, Hubei University, Wuhan, 430062, P. R. China.

School of Chemistry and Pharmaceutical Sciences, Guangxi Normal University, Key Laboratory for the Chemistry and Molecular Engineering of Medicinal Resources, Guilin, 541004, P. R. China.

出版信息

Angew Chem Int Ed Engl. 2020 Aug 3;59(32):13232-13237. doi: 10.1002/anie.202004072. Epub 2020 May 20.

DOI:10.1002/anie.202004072
PMID:32431056
Abstract

The in situ tracking of the pyrolysis of a binary molecular cluster [Zn (μ -CH O) (L) ][ZnLCl ] is presented with one brucite disk and two mononuclear fragments (L=mmimp: 2-methoxy-6-((methylimino)-methyl)phenolate) to porous carbon using TG-MS from 30 to 900 °C. Following up the spilled gas product during the decomposed reaction of zinc cluster along the temperature rising, and in conjunction with XRD, SEM, BET and other materials characterization, where three key steps were observed: 1) cleavage of the bulky external ligand; 2) reduction of ZnO and 3) volatilization of Zn. The real-time-dependent phase-sequential evolution of the remaining products and the processing of pore forming template transformation are proposed simultaneously. The porous carbon structure featuring a uniform nano-sized pore distribution synthesized at 900 °C with the highest surface area of 1644 m  g and pore volume of 0.926 cm  g exhibits the best known capacitance of 662 F g at 0.5 A g .

摘要

采用热重-质谱联用技术,在30至900°C范围内,展示了二元分子簇[Zn(μ-CH₂O)(L)][ZnLCl₂](其中一个水镁石盘和两个单核片段,L = mmimp:2-甲氧基-6-((甲基亚氨基)-甲基)苯酚盐)转化为多孔碳的原位热解过程。随着锌簇在升温过程中分解反应的进行,对溢出的气体产物进行跟踪,并结合XRD、SEM、BET等材料表征,观察到三个关键步骤:1)庞大外部配体的裂解;2)ZnO的还原;3)Zn的挥发。同时提出了剩余产物的实时相关相序演变以及孔形成模板转化的过程。在900°C合成的具有均匀纳米尺寸孔分布、最高表面积为1644 m² g⁻¹和孔体积为0.926 cm³ g⁻¹的多孔碳结构,在0.5 A g⁻¹时表现出662 F g⁻¹的最佳已知电容。

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