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Revealing the Origin of Activity in Nitrogen-Doped Nanocarbons towards Electrocatalytic Reduction of Carbon Dioxide
Xu, Junyuan; Kan, Yuhe; Huang, Rui; Zhang, Bingsen; Wang, Bolun; Wu, Kuang-Hsu; Lin, Yangming; Sun, Xiaoyan; Li, Qingfeng; Centi, Gabriele; Su, Dangsheng; Su, DS (reprint author), Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, 72 Wenhua Rd, Shenyang 110016, Peoples R China.
2016-05-23
发表期刊CHEMSUSCHEM
ISSN1864-5631
卷号9期号:10页码:1085-1089
摘要Carbon nanotubes (CNTs) are functionalized with nitrogen atoms for reduction of carbon dioxide (CO2). The investigation explores the origin of the catalyst's activity and the role of nitrogen chemical states therein. The catalysts show excellent performances, with about 90% current efficiency for CO formation and stability over 60 hours. The Tafel analyses and density functional theory calculations suggest that the reduction of CO2 proceeds through an initial rate-determining transfer of one electron to CO2, which leads to the formation of carbon dioxide radical anion (CO2 center dot-). The initial reduction barrier is too high on pristine CNTs, resulting in a very high overpotentials at which the hydrogen evolution reaction dominates over CO2 reduction. The doped nitrogen atoms stabilize the radical anion, thereby lowering the initial reduction barrier and improving the intrinsic activity. The most efficient nitrogen chemical state for this reaction is quaternary nitrogen, followed by pyridinic and pyrrolic nitrogen.
部门归属[xu, junyuan ; huang, rui ; zhang, bingsen ; wang, bolun ; wu, kuang-hsu ; lin, yangming ; sun, xiaoyan ; su, dangsheng] chinese acad sci, inst met res, shenyang natl lab mat sci, 72 wenhua rd, shenyang 110016, peoples r china ; [kan, yuhe] huaiyin normal univ, sch chem & chem engn, jiangsu key lab chem low dimens mat, 111 changjiang west rd, huaian 223300, peoples r china ; [li, qingfeng] tech univ denmark, dept energy convers & storage, kemitorvet 207, dk-2800 lyngby, denmark ; [centi, gabriele] univ messina, sect ind chem, dept elect engn ind chem & engn, vle f stagno dalcontres 31, i-98166 messina, italy ; [centi, gabriele] univ messina, instm, caspe lab catalysis sustainable prod & energy, vle f stagno dalcontres 31, i-98166 messina, italy
关键词Carbon Dioxide Carbon Nanotubes Doping Electrochemistry Nitrogen
学科领域Chemistry ; Science & Technology - Other Topics
资助者National Natural Science Foundation of China [21133010, 51221264, 21261160487, 91545119]; "Strategic Priority Research Program" of the Chinese Academy of Sciences [XDA09030103]; Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences
收录类别sci
语种英语
文献类型期刊论文
条目标识符http://ir.imr.ac.cn/handle/321006/75868
专题中国科学院金属研究所
通讯作者Su, DS (reprint author), Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, 72 Wenhua Rd, Shenyang 110016, Peoples R China.
推荐引用方式
GB/T 7714
Xu, Junyuan,Kan, Yuhe,Huang, Rui,et al. Revealing the Origin of Activity in Nitrogen-Doped Nanocarbons towards Electrocatalytic Reduction of Carbon Dioxide[J]. CHEMSUSCHEM,2016,9(10):1085-1089.
APA Xu, Junyuan.,Kan, Yuhe.,Huang, Rui.,Zhang, Bingsen.,Wang, Bolun.,...&Su, DS .(2016).Revealing the Origin of Activity in Nitrogen-Doped Nanocarbons towards Electrocatalytic Reduction of Carbon Dioxide.CHEMSUSCHEM,9(10),1085-1089.
MLA Xu, Junyuan,et al."Revealing the Origin of Activity in Nitrogen-Doped Nanocarbons towards Electrocatalytic Reduction of Carbon Dioxide".CHEMSUSCHEM 9.10(2016):1085-1089.
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