期刊
CARBON
卷 194, 期 -, 页码 274-281出版社
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.carbon.2022.03.069
关键词
Graphyne; Mechanochemistry; Symmetry; Nitrogen doping; Anode material
资金
- National Natural Science Foun-dation of China [52002076]
- Natural Science Foundation of Shanghai [20ZR1403300]
- China Postdoctoral Science Foundation [2021M690644]
This study successfully synthesized graphyne material with rich pyridinic- and pyridonic-nitrogen doping via a mechanochemical route. The introduction of symmetric hexabromobenzene was found to suppress the formation of graphitic carbon impurities. By optimizing the material ratio, the obtained graphyne material exhibited higher energy storage capacity and structural stability.
Graphyne, a promising carbon candidate for energy storage and conversion, has been prepared successfully via a mechanochemical route. However, inevitable graphitic carbon species generate concomitantly. In this work, we synthesize rich pyridonic-/pyridinic-nitrogen doped graphyne (NGY) employing calcium carbide and asymmetric pentachloropyridine (PCP) as precursors and find that introducing symmetric hexabromobenzene (HBB) can suppress the formation of graphitic carbon impurities. The symmetry of organic precursors is a key to the yield of NGY during the mechanochemical process, so a competitive formation mechanism between NGY and graphitic carbon species is proposed according to experimental results and theoretical calculation. Compared with the samples obtained from single asymmetric PCP or symmetric HBB, an optimized NGY (1:1 molar ratio of PCP/HBB) increases the Listorage capacity by 11% and 52% respectively, owing to abundant Li+ adsorption and high structural stability. This work highlights organic precursor symmetry for undergoing mechanochemical crosscoupling and brings new insights to in-situ constructing heteroatom-doped alkynyl carbon frameworks. (c) 2022 Elsevier Ltd. All rights reserved.
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