The identification of optimal active boron sites for N-2 reduction
作者:Yin, H (Yin, Hui)[ 1 ] ; Gan, LY (Gan, Li-Yong)[ 1,2,3 ] ; Wang, P (Wang, Ping)[ 1 ]
JOURNAL OF MATERIALS CHEMISTRY A
卷: 8 期: 7 页: 3910-3917
DOI: 10.1039/c9ta13700a
出版年: FEB 21 2020
文献类型:Article
查看期刊影响力
摘要
Identifying the nature of active centers and structure-performance correlations is of fundamental importance for the successful design of more energy-efficient and/or selective catalysts. Recently, the studies of metal-free catalysts containing sp(2)- or sp(3)-hybridized B sites have displayed an attractive prospect for N-2 reduction but have obscured the nature of the optimal active B species. Herein, with the aid of first-principles calculations, we explicitly disclose that sp(2)-hybridized B is the optimal species for providing high activity for N-2 reduction and particularly outstanding capability to suppress the competing hydrogen evolution reaction. Specifically, the system with B substituting an edge N atom in the cavity of C2N is proposed to be highly promising for N-2 reduction under mild conditions. The developed comprehensive insight is of clear significance for the rational design of advanced catalysts for NH3 synthesis under mild conditions.
关键词
KeyWords Plus:ELECTROCHEMICAL REDUCTION; AMMONIA-SYNTHESIS; NITROGEN-FIXATION; OXYGEN REDUCTION; ELECTRONIC-STRUCTURE; CATALYTIC-REDUCTION; ENERGY CALCULATIONS; ATOM CATALYSTS; TRANSITION; SURFACE
作者信息
通讯作者地址: Gan, LY; Wang, P (通讯作者)
显示更多South China Univ Technol, Sch Mat Sci & Engn, Key Lab Adv Energy Storage Mat Guangdong Prov, Guangzhou 510641, Peoples R China.
通讯作者地址: Gan, LY (通讯作者)
显示更多Chongqing Univ, Inst Struct & Funct, Chongqing 400030, Peoples R China.
通讯作者地址: Gan, LY (通讯作者)
显示更多Chongqing Univ, Dept Phys, Chongqing 400030, Peoples R China.
地址:
显示更多[ 1 ] South China Univ Technol, Sch Mat Sci & Engn, Key Lab Adv Energy Storage Mat Guangdong Prov, Guangzhou 510641, Peoples R China
显示更多[ 2 ] Chongqing Univ, Inst Struct & Funct, Chongqing 400030, Peoples R China
显示更多[ 3 ] Chongqing Univ, Dept Phys, Chongqing 400030, Peoples R China
电子邮件地址:ganly@cqu.edu.cn; mspwang@scut.edu.cn
基金资助致谢
基金资助机构显示详情授权号
National Natural Science Foundation of China
51621001
National Key R&D Program of China
2018YFB1502104
Foundation for Research Groups of the Natural Science Foundation of Guangdong Province
2016A030312011
National Natural Science Foundation of China
51671087
11504303
Special Support Plan for National 10000-talents Program
查看基金资助信息
出版商
ROYAL SOC CHEMISTRY, THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND
期刊信息
Impact Factor (影响因子): Journal Citation Reports
类别 / 分类
研究方向:Chemistry; Energy & Fuels; Materials Science
Web of Science 类别:Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary