材料科学
密度泛函理论
二氧化碳电化学还原
再分配(选举)
化学工程
掺杂剂
催化作用
拓扑(电路)
热处理
化学物理
碳纤维
法拉第效率
纳米技术
电化学
多孔性
计算化学
物理化学
兴奋剂
电极
有机化学
光电子学
一氧化碳
复合材料
化学
工程类
组合数学
复合数
政治
数学
政治学
法学
作者
Dong Yan,Qiuju Zhang,Ziqi Tian,Boran Li,Wensheng Yan,Shuo Wang,Kaiyu Jiang,Jianwei Su,Colin Oloman,Előd Gyenge,Ruixiang Ge,Zhiyi Lu,Xiulei Ji,Liang Chen
标识
DOI:10.1002/adma.202001300
摘要
Topological defects, with an asymmetric local electronic redistribution, are expected to locally tune the intrinsic catalytic activity of carbon materials. However, it is still challenging to deliberately create high-density homogeneous topological defects in carbon networks due to the high formation energy. Toward this end, an efficient NH3 thermal-treatment strategy is presented for thoroughly removing pyrrolic-N and pyridinic-N dopants from N-enriched porous carbon particles, to create high-density topological defects. The resultant topological defects are systematically investigated by near-edge X-ray absorption fine structure measurements and local density of states analysis, and the defect formation mechanism is revealed by reactive molecular dynamics simulations. Notably, the as-prepared porous carbon materials possess an enhanced electrocatalytic CO2 reduction performance, yielding a current density of 2.84 mA cm-2 with Faradaic efficiency of 95.2% for CO generation. Such a result is among the best performances reported for metal-free CO2 reduction electrocatalysts. Density functional theory calculations suggest that the edge pentagonal sites are the dominating active centers with the lowest free energy (ΔG) for CO2 reduction. This work not only presents deep insights for the defect engineering of carbon-based materials but also improves the understanding of electrocatalytic CO2 reduction on carbon defects.
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