Self-Assembled Framework Enhances Electronic Communication of Ultrasmall-Sized Nanoparticles for Exceptional Solar Hydrogen Evolution
文献类型：期刊论文
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| 作者 | Li, XB ; Gao, YJ; Wang, Y; Zhan, F; Zhang, XY; Kong, QY; Zhao, NJ; Guo, Q; Wu, HL; Li, ZJ
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| 刊名 | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
 ; JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
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| 出版日期 | 2017 ; 2017 |
| 卷号 | 139期号:13页码:4789-4796 |
| ISSN号 | 0002-7863 ; 0002-7863 |
| DOI | 10.1021/jacs.6b12976 ; 10.1021/jacs.6b12976 |
| 文献子类 | Article ; Article |
| 英文摘要 | Colloidal quantum dots (QDs) have demonstrated great promise in artificial photosynthesis. However, the ultrasmall size hinders its controllable and effective interaction with cocatalysts. To improve the poor interparticle electronic communication between free QD and cocatalyst, we design here a self-assembled architecture of nanoparticles, QDs and Pt nanoparticles, simply jointed together by molecular polyacrylate to greatly enhance the rate and efficiency of interfacial electron transfer (ET). The enhanced interparticle electronic communication is confirmed by femtosecond transient absorption spectroscopy and X-ray transient absorption. Taking advantage of the enhanced interparticle ET with a time scale of similar to 65 ps, 5.0 mL of assembled CdSe/CdS QDs/cocatalysts solution produces 94 +/- 1.5 mL (4183 +/- 67 mu mol) of molecular H-2 in 8 h, giving rise to an internal quantum yield of similar to 65% in the first 30 min and a total turnover number of >1.64 x 10(7) per Pt nanoparticle. This study demonstrates that self-assembly is a promising way to improve the sluggish kinetics of the interparticle ET process, which is the key step for advanced H2 photosynthesis.; Colloidal quantum dots (QDs) have demonstrated great promise in artificial photosynthesis. However, the ultrasmall size hinders its controllable and effective interaction with cocatalysts. To improve the poor interparticle electronic communication between free QD and cocatalyst, we design here a self-assembled architecture of nanoparticles, QDs and Pt nanoparticles, simply jointed together by molecular polyacrylate to greatly enhance the rate and efficiency of interfacial electron transfer (ET). The enhanced interparticle electronic communication is confirmed by femtosecond transient absorption spectroscopy and X-ray transient absorption. Taking advantage of the enhanced interparticle ET with a time scale of similar to 65 ps, 5.0 mL of assembled CdSe/CdS QDs/cocatalysts solution produces 94 +/- 1.5 mL (4183 +/- 67 mu mol) of molecular H-2 in 8 h, giving rise to an internal quantum yield of similar to 65% in the first 30 min and a total turnover number of >1.64 x 10(7) per Pt nanoparticle. This study demonstrates that self-assembly is a promising way to improve the sluggish kinetics of the interparticle ET process, which is the key step for advanced H2 photosynthesis. |
| WOS关键词 | CDSE/CDS CORE/SHELL NANOCRYSTALS ; CDSE/CDS CORE/SHELL NANOCRYSTALS ; PHOTOCATALYTIC H-2 EVOLUTION ; METAL-ORGANIC FRAMEWORKS ; ION LAYER ADSORPTION ; QUASI-TYPE-II ; QUANTUM DOTS ; SEMICONDUCTOR NANOCRYSTALS ; AQUEOUS-SOLUTION ; CHALCOGENIDE NANOCRYSTALS ; HIGHLY LUMINESCENT ; PHOTOCATALYTIC H-2 EVOLUTION ; METAL-ORGANIC FRAMEWORKS ; ION LAYER ADSORPTION ; QUASI-TYPE-II ; QUANTUM DOTS ; SEMICONDUCTOR NANOCRYSTALS ; AQUEOUS-SOLUTION ; CHALCOGENIDE NANOCRYSTALS ; HIGHLY LUMINESCENT |
| WOS研究方向 | Chemistry ; Chemistry |
| 语种 | 英语 ; 英语 |
| WOS记录号 | WOS:000398764000031 ; WOS:000398764000031 |
| 源URL | [http://ir.ihep.ac.cn/handle/311005/285111]  |
| 专题 | 高能物理研究所_多学科研究中心 高能物理研究所_加速器中心 高能物理研究所_粒子天体物理中心 高能物理研究所_东莞分部 |
| 作者单位 | 中国科学院高能物理研究所 |
| 推荐引用方式 GB/T 7714 | Li, XB,Gao, YJ,Wang, Y,et al. Self-Assembled Framework Enhances Electronic Communication of Ultrasmall-Sized Nanoparticles for Exceptional Solar Hydrogen Evolution, Self-Assembled Framework Enhances Electronic Communication of Ultrasmall-Sized Nanoparticles for Exceptional Solar Hydrogen Evolution[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2017, 2017,139, 139(13):4789-4796, 4789-4796. |
| APA | Li, XB.,Gao, YJ.,Wang, Y.,Zhan, F.,Zhang, XY.,...&陶冶.(2017).Self-Assembled Framework Enhances Electronic Communication of Ultrasmall-Sized Nanoparticles for Exceptional Solar Hydrogen Evolution.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,139(13),4789-4796. |
| MLA | Li, XB,et al."Self-Assembled Framework Enhances Electronic Communication of Ultrasmall-Sized Nanoparticles for Exceptional Solar Hydrogen Evolution".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 139.13(2017):4789-4796. |
入库方式： OAI收割
来源：高能物理研究所
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