Ammonia Thermal Treatment toward Topological Defects in Porous Carbon for Enhanced Carbon Dioxide Electroreduction
文献类型:期刊论文
作者 | Dong, Yan; Zhang, Qiuju; Tian, Ziqi; Li, Boran; Yan, Wensheng; Wang, Shuo; Jiang, Kemin; Su, Jianwei; Oloman, Colin W.; Gyenge, Elod L. |
刊名 | ADVANCED MATERIALS |
出版日期 | 2020 |
卷号 | 32期号:28 |
关键词 | ELECTROCHEMICAL REDUCTION NANOPOROUS CARBON CO2 REDUCTION OXYGEN REDUCTION NITROGEN METAL EFFICIENT GRAPHENE CATALYSTS COPPER |
DOI | 10.1002/adma.202001300 |
英文摘要 | 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 (Delta G) 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. |
学科主题 | Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics |
源URL | [http://ir.nimte.ac.cn/handle/174433/20751] |
专题 | 2020专题 2020专题_期刊论文 |
作者单位 | 1.Su, JW 2.Chen, L (corresponding author), Chinese Acad Sci, Ningbo Inst Mat Technol & Engn, Ningbo 315201, Peoples R China. 3.Chen, L (corresponding author), Univ Chinese Acad Sci, Beijing 100049, Peoples R China. |
推荐引用方式 GB/T 7714 | Dong, Yan,Zhang, Qiuju,Tian, Ziqi,et al. Ammonia Thermal Treatment toward Topological Defects in Porous Carbon for Enhanced Carbon Dioxide Electroreduction[J]. ADVANCED MATERIALS,2020,32(28). |
APA | Dong, Yan.,Zhang, Qiuju.,Tian, Ziqi.,Li, Boran.,Yan, Wensheng.,...&Chen, Liang.(2020).Ammonia Thermal Treatment toward Topological Defects in Porous Carbon for Enhanced Carbon Dioxide Electroreduction.ADVANCED MATERIALS,32(28). |
MLA | Dong, Yan,et al."Ammonia Thermal Treatment toward Topological Defects in Porous Carbon for Enhanced Carbon Dioxide Electroreduction".ADVANCED MATERIALS 32.28(2020). |
入库方式: OAI收割
来源:宁波材料技术与工程研究所
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