Size dependence of photocatalytic hydrogen generation for CdTe quantum dots

doi:10.1063/1.5125000

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	Size dependence of photocatalytic hydrogen generation for CdTe quantum dots
	Yin, Jiajia 3; Cogan, Nicole M. B.1; Burke, Rebeckah 1; Hou, Zhentao 1; Sowers, Kelly L.1; Krauss, Todd D.1,2
刊名	Journal of Chemical Physics
	2019-11-07
卷号	151 期号:17
ISSN号	0021-9606
DOI	10.1063/1.5125000
文献子类	期刊论文
英文摘要	CdTe quantum dots (QDs) are attractive photosensitizers for photocatalytic proton reduction due to their broad absorbance profile that can extend from the ultraviolet to near-infrared regions, providing access to a larger portion of the solar spectrum than possible with analogous CdSe and CdS QD photosensitizers. Here, the photocatalytic hydrogen (H2) generation from various sizes of dihydrolipoic acid (DHLA)-capped CdTe QDs, ranging from 2.5 to 7.5 nm in diameter, and a molecular Ni-DHLA catalyst in aqueous solutions was evaluated, and an unusual size-dependent photocatalytic activity with CdTe QDs was observed. Under optimized conditions, using 3.4 nm CdTe-DHLA and a 1:20 ratio of QD/Ni-DHLA catalyst, as many as 38 000 turnover numbers (mol H2 per mol QD) were achieved. However, below this critical size, the H2 production efficiency decreased; this behavior is attributed to the rapid oxidation of the QD surface, resulting in detrimental surface trap states. These results are consistent with ultrafast transient absorption spectroscopic measurements, which suggest the presence of extremely fast charge-trapping processes in the oxidized CdTe-DHLA QDs. While fast electron transfer from CdTe-DHLA QDs is observed in the presence of the Ni-DHLA catalyst, the charge trapping processes occur on a competitive time scale, thus lowering the efficiency of the CdTe/Ni-DHLA H2 production system. Understanding rapid charge trapping in CdTe QDs may help suggest potential improvements for the overall CdTe photocatalytic system. © 2019 Author(s).
WOS关键词	CHARGE-TRANSFER DYNAMICS ; ELECTRON-TRANSFER ; SEMICONDUCTOR NANOCRYSTALS ; TRANSIENT ABSORPTION ; LUMINESCENT PROBES ; CARRIER DYNAMICS ; LIGAND-EXCHANGE ; IN-SITU ; CDSE ; EFFICIENT
WOS研究方向	Chemistry, Physical ; Physics, Atomic, Molecular & Chemical
语种	英语
出版者	American Institute of Physics Inc.
WOS记录号	WOS:000496485600022
内容类型	期刊论文
源URL	[http://ir.ioe.ac.cn/handle/181551/9725]
专题	薄膜光学相机总体室
作者单位	1.Department of Chemistry, University of Rochester, Rochester; NY; 14627, United States; 2.Institute of Optics, University of Rochester, Rochester; NY; 14627, United States 3.Institute of Optics and Electronics Chinese Academy Science, Chengdu, Sichuan; 610209, China;
推荐引用方式 GB/T 7714	Yin, Jiajia,Cogan, Nicole M. B.,Burke, Rebeckah,et al. Size dependence of photocatalytic hydrogen generation for CdTe quantum dots[J]. Journal of Chemical Physics,2019,151(17).
APA	Yin, Jiajia,Cogan, Nicole M. B.,Burke, Rebeckah,Hou, Zhentao,Sowers, Kelly L.,&Krauss, Todd D..(2019).Size dependence of photocatalytic hydrogen generation for CdTe quantum dots.Journal of Chemical Physics,151(17).
MLA	Yin, Jiajia,et al."Size dependence of photocatalytic hydrogen generation for CdTe quantum dots".Journal of Chemical Physics 151.17(2019).