Unique Electronic Structure Induced High Photoreactivity of Sulfur-Doped Graphitic C(3)N(4)

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	Unique Electronic Structure Induced High Photoreactivity of Sulfur-Doped Graphitic C(3)N(4)
	G. Liu; P. Niu; C. H. Sun; S. C. Smith; Z. G. Chen; G. Q. Lu; H. M. Cheng
	2010
发表期刊	Journal of the American Chemical Society
ISSN	0002-7863
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 C(3)N(4) (C(3)N(4-x)S(x)) 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 C(3)N(4-x)S(x) shows a photoreactivity of H(2) evolution 7.2 and 8.0 times higher than C(3)N(4) under lambda > 300 and 420 nm, respectively. More strikingly, the complete oxidation process of phenol under lambda > 400 nm can occur for sulfur-doped C(3)N(4), which is impossible for C(3)N(4) 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 C(3)N(4-x)S(x). The results acquired may shed light on general doping strategies for designing potentially efficient photocatalysts.
部门归属	[liu, gang; niu, ping; cheng, hui-ming] chinese acad sci, inst met res, shenyang natl lab mat sci, shenyang 110016, peoples r china. [sun, chenghua; chen, zhigang; lu, gao qing (max)] univ queensland, arc ctr excellence funct nanomat, brisbane, qld 4072, australia. [sun, chenghua; smith, sean c.] univ queensland, australia inst bioengn & nanotechnol, ctr computat mol sci, brisbane, qld 4072, australia.;cheng, hm (reprint author), chinese acad sci, inst met res, shenyang natl lab mat sci, 72 wenhua rd, shenyang 110016, peoples r china;cheng@imr.ac.cn
关键词	Visible-light Irradiation Metal-free Catalysts Carbon Nitride Hydrogen-production Titanium-dioxide Photocatalytic Activity Water Semiconductor Tio2 Evolution
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文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/31281
专题	中国科学院金属研究所
推荐引用方式 GB/T 7714	G. Liu,P. Niu,C. H. Sun,et al. Unique Electronic Structure Induced High Photoreactivity of Sulfur-Doped Graphitic C(3)N(4)[J]. Journal of the American Chemical Society,2010,132(33):11642-11648.
APA	G. Liu.,P. Niu.,C. H. Sun.,S. C. Smith.,Z. G. Chen.,...&H. M. Cheng.(2010).Unique Electronic Structure Induced High Photoreactivity of Sulfur-Doped Graphitic C(3)N(4).Journal of the American Chemical Society,132(33),11642-11648.
MLA	G. Liu,et al."Unique Electronic Structure Induced High Photoreactivity of Sulfur-Doped Graphitic C(3)N(4)".Journal of the American Chemical Society 132.33(2010):11642-11648.