Band-to-Band Visible-Light Photon Excitation and Photoactivity Induced by Homogeneous Nitrogen Doping in Layered Titanates

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	Band-to-Band Visible-Light Photon Excitation and Photoactivity Induced by Homogeneous Nitrogen Doping in Layered Titanates
	G. Liu; L. Z. Wang; C. H. Sun; X. X. Yan; X. W. Wang; Z. G. Chen; S. C. Smith; H. M. Cheng; G. Q. Lu
	2009
发表期刊	Chemistry of Materials
ISSN	0897-4756
卷号	21 期号:7 页码:1266-1274
摘要	The distribution of dopants in semiconductors can intrinsically determine the electronic structure and consequently the absorbance, redox potential, and charge-carrier mobility of the semiconductor photocatalysts. In contrast to most reported nitrogen-doped titania photocatalysts with some localized states in the intrinsic band gap and small visible light absorption shoulders induced by inhomogeneous nitrogen doping near the particle surface, we report here the homogeneous substitution of O by N in the whole particles of layered titanates. The resultant materials Cs(0.68)Ti(1.83)O(4-x)N(x) exhibited extraordinary band-to-band excitation in the visible-light ranging up to blue light. From photoelectron spectroscopy and first-principles calculations, the upward shift of valence band maximum by N 2p states is concluded as the cause of the band-to-band visible light excitation. The holes generated upon visible light excitation in the newly formed valence bands Of Cs(0.68)Ti(1.83)O(4-x)N(x) and H(0.68)Ti(1.83)O(4-x)N(x) had strong oxidation ability in oxidizing OH(-) into active center dot OH radicals in photocatalysis. These findings are the clear evidence for the substantial role of homogeneous nitrogen doping in obtaining band-to-band visible-light photon excitation in layered titanates. The new physical insights into the electronic structure of homogeneous substitutional N in layered titanates gained here may have important implications for developing other efficient visible light photocatalysts by nonmetal doping.
部门归属	[liu, gang; wang, xuewen; chen, zhigang; cheng, hui-ming] chinese acad sci, inst met res, shenyang natl lab mat sci, shenyang 110016, peoples r china. [liu, gang; wang, lianzhou; sun, chenghua; yan, xiaoxia; lu, gao qing] univ queensland, sch engn, arc ctr excellence funct nanomat, brisbane, qld 4072, australia. [sun, chenghua; smith, sean c.] univ queensland, australian 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 maxlu@uq.edu.au
关键词	Doped Titanium-dioxide Sensitized Solar-cells Photocatalytic H-2 Evolution Tio2 Photocatalysts Photoelectrochemical Properties Mechanochemical Reaction Driven Photocatalysts Electronic-structure Water Oxidation Tungsten-oxide
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WOS记录号	WOS:000265029100017
引用统计	被引频次：281[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/321006/32082
专题	中国科学院金属研究所
推荐引用方式 GB/T 7714	G. Liu,L. Z. Wang,C. H. Sun,et al. Band-to-Band Visible-Light Photon Excitation and Photoactivity Induced by Homogeneous Nitrogen Doping in Layered Titanates[J]. Chemistry of Materials,2009,21(7):1266-1274.
APA	G. Liu.,L. Z. Wang.,C. H. Sun.,X. X. Yan.,X. W. Wang.,...&G. Q. Lu.(2009).Band-to-Band Visible-Light Photon Excitation and Photoactivity Induced by Homogeneous Nitrogen Doping in Layered Titanates.Chemistry of Materials,21(7),1266-1274.
MLA	G. Liu,et al."Band-to-Band Visible-Light Photon Excitation and Photoactivity Induced by Homogeneous Nitrogen Doping in Layered Titanates".Chemistry of Materials 21.7(2009):1266-1274.