Lai Qingxue, Zheng Jing, Tang Zeming, Bi Da, Zhao Jingxiang, Liang Yanyu
Jiangsu key Laboratory of Electrochemical Energy Storage, Technologies, College of Material Science and Technology, Nanjing University of Aeronautics and Astronautics, Nanjing, 210016, P. R. China.
Department of Chemistry and Materials Science, College of Science, Nanjing Forestry University, Nanjing, 210037, P. R. China.
Angew Chem Int Ed Engl. 2020 Jul 13;59(29):11999-12006. doi: 10.1002/anie.202000936. Epub 2020 May 12.
The charge redistribution strategy driven by heteroatom doping or defect engineering has been developed as an efficient method to endow inert carbon with significant oxygen reduction reaction (ORR) activity. The synergetic effect between the two approaches is thus expected to be more effective for manipulating the charge distribution of carbon materials for exceptional ORR performance. Herein we report a novel molecular design strategy to achieve a 2D porous turbostratic carbon nanomesh with abundant N-doped carbon defects (NDC). The molecular level integration of aromatic rings as the carbon source and urea units as the N source and sacrificial template into the novel precursor of polyurea (PU) promises the formation of abundant carbon edge defects and N doping sites. A special active site-a carbon edge defect doped with a graphitic valley N atom-was revealed to be responsible for the exceptional ORR performance of NDC material.
由杂原子掺杂或缺陷工程驱动的电荷重新分布策略已被开发为一种有效的方法，使惰性碳具有显著的氧还原反应（ORR）活性。因此，预计这两种方法之间的协同效应对于操纵碳材料的电荷分布以实现卓越的ORR性能将更为有效。在此，我们报告了一种新颖的分子设计策略，以实现具有大量氮掺杂碳缺陷（NDC）的二维多孔乱层碳纳米网。将作为碳源的芳环和作为氮源及牺牲模板的尿素单元在分子水平上整合到新型聚脲（PU）前体中，有望形成大量的碳边缘缺陷和氮掺杂位点。一种特殊的活性位点——掺杂有石墨化谷氮原子的碳边缘缺陷——被揭示是NDC材料卓越ORR性能的原因。
