Superposed Redox Chemistry of Fused Carbon Rings in Cyclooctatetraene-Based Organic Molecules for High-Voltage and High-Capacity Cathodes

doi:10.1021/acsami.7b15495

	Superposed Redox Chemistry of Fused Carbon Rings in Cyclooctatetraene-Based Organic Molecules for High-Voltage and High-Capacity Cathodes
	Zhao, Xiaolin 1; Qiu, Wujie 1; Ma, Chao 2; Zhao, Yingqin 1; Wang, Kaixue 2; Zhang, Wenqing 1; Kang, Litao ; Liu, Jianjun 1
刊名	ACS APPLIED MATERIALS & INTERFACES
	2018
卷号	10 期号:3 页码:2496
关键词	DFT COT-based molecules high-voltage aromatization double bond reformation Na+-ion battery
ISSN号	1944-8244
DOI	10.1021/acsami.7b15495
英文摘要	Even though many organic cathodes have been developed and have made a significant improvement in energy density and reversibility, some organic materials always generate relatively low voltage and limited discharge capacity because their energy storage mechanism is solely based on redox reactions of limited functional groups [N-O, C-X (X = O, N, S)] linking to aromatic rings. Here, a series of cyclooctatetraene-based (C8H8) organic molecules were demonstrated to have electrochemical activity of high-capacity and high-voltage from carbon rings by means of first-principles calculations and electronic structure analysis. Fused molecules of C-8-C-4-C-8 (C16H12) and C-8-C-4-C-8-C-4-C-8 (C24H16) contain, respectively, four and eight electron-deficient carbons, generating high-capacity by their multiple redox reactions. Our sodiation calculations predict that C16H12 and C24H16 exhibit discharge capacities of 525.3 and 357.2 mA h g(-1) at the voltage change from 3.5 to 1.0 V and 3.7 to 1.3 V versus Na+/Na, respectively. Electronic structure analysis reveals that the high voltages are attributed to superposed electron stabilization mechanisms, including double-bond reformation and aromatization from carbon rings. High thermodynamic stability of these C24H16-based systems strongly suggests feasibility of experimental realization. The present work provides evidence that cyclooctatetraene-based organic molecules fused with the C-4 ring are promising in designing high-capacity and high-voltage organic rechargeable cathodes.
学科主题	Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000423496500037
资助机构	This work is financially supported by the National Natural Science Foundation of Chinese, NSFC (51432010, 21573272, 51502194), and the research grant (no. 16DZ2260600) from Science and Technology Commission of Shanghai Municipality. L.K. also thanks the Opening Project of State Key Laboratory of High Performance Ceramics and Superfine Microstructure (SKL201511SIC), and the Opening Project of Jiangsu Provincial Engineering Laboratory for Advanced Materials of Salt Chemical Industry (SF201605) for financial support. ; This work is financially supported by the National Natural Science Foundation of Chinese, NSFC (51432010, 21573272, 51502194), and the research grant (no. 16DZ2260600) from Science and Technology Commission of Shanghai Municipality. L.K. also thanks the Opening Project of State Key Laboratory of High Performance Ceramics and Superfine Microstructure (SKL201511SIC), and the Opening Project of Jiangsu Provincial Engineering Laboratory for Advanced Materials of Salt Chemical Industry (SF201605) for financial support.
内容类型	期刊论文
源URL	[http://ir.sic.ac.cn/handle/331005/24541]
专题	中国科学院上海硅酸盐研究所
作者单位	1.Taiyuan Univ Technol, Dept Mat Sci & Engn, 79 West Yingze Rd, Taiyuan 030024, Shanxi, Peoples R China 2.Chinese Acad Sci, Shanghai Inst Ceram, State Key Lab High Performance Ceram & Superfine, 1295 Dingxi Rd, Shanghai 200050, Peoples R China 3.Shanghai Jiao Tong Univ, Sch Chem & Chem Engn, Shanghai Electrochem Energy Devices Res Ctr, Shanghai 200240, Peoples R China
推荐引用方式 GB/T 7714	Zhao, Xiaolin,Qiu, Wujie,Ma, Chao,et al. Superposed Redox Chemistry of Fused Carbon Rings in Cyclooctatetraene-Based Organic Molecules for High-Voltage and High-Capacity Cathodes[J]. ACS APPLIED MATERIALS & INTERFACES,2018,10(3):2496, 2503.
APA	Zhao, Xiaolin.,Qiu, Wujie.,Ma, Chao.,Zhao, Yingqin.,Wang, Kaixue.,...&Liu, Jianjun.(2018).Superposed Redox Chemistry of Fused Carbon Rings in Cyclooctatetraene-Based Organic Molecules for High-Voltage and High-Capacity Cathodes.ACS APPLIED MATERIALS & INTERFACES,10(3),2496.
MLA	Zhao, Xiaolin,et al."Superposed Redox Chemistry of Fused Carbon Rings in Cyclooctatetraene-Based Organic Molecules for High-Voltage and High-Capacity Cathodes".ACS APPLIED MATERIALS & INTERFACES 10.3(2018):2496.