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Unique Electronic Structure Induced High Photoreactivity of Sulfur-Doped Graphitic C3N4
Liu, Gang1; Niu, Ping1; Sun, Chenghua2,3; Smith, Sean C.3; Chen, Zhigang2; Lu, Gao Qing (Max)2; Cheng, Hui-Ming1
通讯作者Cheng, Hui-Ming(cheng@imr.ac.cn)
2010-08-25
发表期刊JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
ISSN0002-7863
卷号132期号:33页码:11642-11648
摘要Electronic structure intrinsically controls the light absorbance, redox potential, charge-carrier mobility, and consequently, photoreactivity of semiconductor photocatalysts. The conventional approach of modifying the electronic structure of a semiconductor photocatalyst for a wider absorption range by anion doping operates at the cost of reduced redox potentials and/or charge-carrier mobility, so that its photoreactivity is usually limited and some important reactions may not occur at all. Here, we report sulfur-doped graphitic C3N4 (C3N4-xSx) with a unique electronic structure that displays an increased valence bandwidth in combination with an elevated conduction band minimum and a slightly reduced absorbance. The C3N4-xSx shows a photoreactivity of H-2 evolution 7.2 and 8.0 times higher than C3N4 under lambda > 300 and 420 nm, respectively. More strikingly, the complete oxidation process of phenol under lambda > 400 nm can occur for sulfur-doped C3N4, which is impossible for C3N4 even under lambda > 300 nm. The homogeneous substitution of sulfur for lattice nitrogen and a concomitant quantum confinement effect are identified as the cause of this unique electronic structure and, consequently, the excellent photoreactivity of C3N4-xSx. The results acquired may shed light on general doping strategies for designing potentially efficient photocatalysts.
资助者Ministry of Science and Technology of China ; NSFC ; Solar Energy Initiative of the Chinese Academy of Sciences (CAS), CAS ; China Postdoctoral Science Foundation ; IMR SYNL
DOI10.1021/ja103798k
收录类别SCI
语种英语
资助项目Ministry of Science and Technology of China[2009CB220001] ; NSFC[50921004] ; Solar Energy Initiative of the Chinese Academy of Sciences (CAS), CAS[KJCX2-YW-H21-01] ; China Postdoctoral Science Foundation[20100471486] ; IMR SYNL
WOS研究方向Chemistry
WOS类目Chemistry, Multidisciplinary
WOS记录号WOS:000281066400051
出版者AMER CHEMICAL SOC
引用统计
被引频次:1869[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://ir.imr.ac.cn/handle/321006/99764
专题中国科学院金属研究所
通讯作者Cheng, Hui-Ming
作者单位1.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China
2.Univ Queensland, ARC Ctr Excellence Funct Nanomat, Brisbane, Qld 4072, Australia
3.Univ Queensland, Australia Inst Bioengn & Nanotechnol, Ctr Computat Mol Sci, Brisbane, Qld 4072, Australia
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GB/T 7714
Liu, Gang,Niu, Ping,Sun, Chenghua,et al. Unique Electronic Structure Induced High Photoreactivity of Sulfur-Doped Graphitic C3N4[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2010,132(33):11642-11648.
APA Liu, Gang.,Niu, Ping.,Sun, Chenghua.,Smith, Sean C..,Chen, Zhigang.,...&Cheng, Hui-Ming.(2010).Unique Electronic Structure Induced High Photoreactivity of Sulfur-Doped Graphitic C3N4.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,132(33),11642-11648.
MLA Liu, Gang,et al."Unique Electronic Structure Induced High Photoreactivity of Sulfur-Doped Graphitic C3N4".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 132.33(2010):11642-11648.
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