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题名: Photocatalytic H-2 production using a hybrid assembly of an [FeFe]-hydrogenase model and CdSe quantum dot linked through a thiolato-functionalized cyclodextrin
作者: Cheng, Minglun1;  Wang, Mei1;  Zhang, Shuai1;  Liu, Fengyuan1;  Yang, Yong1;  Wan, Boshun2;  Sun, Licheng1, 3
刊名: FARADAY DISCUSSIONS
发表日期: 2017-06-01
DOI: 10.1039/c6fd00207b
卷: 198, 页:197-209
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Chemistry, Physical
研究领域[WOS]: Chemistry
英文摘要: It is a great challenge to develop iron-based highly-efficient and durable catalytic systems for the hydrogen evolution reaction (HER) by understanding and learning from [FeFe]-hydrogenases. Here we report photocatalytic H-2 production by a hybrid assembly of a sulfonate-functionalized [FeFe]-hydrogenase mimic (1) and CdSe quantum dot (QD), which is denoted as 1/beta-CD-6-S-CdSe (beta-CD-6-SH = 6-mercapto-beta-cyclodextrin). In this assembly, thiolato-functionalized beta-CD acts not only as a stabilizing reagent of CdSe QDs but also as a host compound for the diiron catalyst, so as to confine CdSe QDs to the space near the site of diiron catalyst. In addition, another two reference systems comprising MAA-CdSe QDs (HMAA = mercaptoacetic acid) and 1 in the presence and absence of beta-CD, denoted as 1/beta-CD/MAA-CdSe and 1/MAA-CdSe, were studied for photocatalytic H-2 evolution. The influences of beta-CD and the stabilizing reagent beta-CD-6-S- on the stability of diiron catalyst, the fluorescence lifetime of CdSe QDs, the apparent electron transfer rate, and the photocatalytic H-2-evolving efficiency were explored by comparative studies of the three hybrid systems. The 1/beta-CD-6-SCdSe system displayed a faster apparent rate for electron transfer from CdSe QDs to the diiron catalyst compared to that observed for MAA-CdSe-based systems. The total TON for visible-light driven H-2 evolution by the 1/beta-CD-6-S-CdSe QDs in water at pH 4.5 is about 2370, corresponding to a TOF of 150 h(-1) in the initial 10 h of illumination, which is 2.7- and 6.6-fold more than the amount of H-2 produced from the reference systems 1/beta-CD/MAA-CdSe and 1/MAA-CdSe. Additionally, 1/beta-CD-6-S-CdSe gave 2.4-5.1 fold enhancement in the apparent quantum yield and significantly improved the stability of the system for photocatalytic H-2 evolution.
关键词[WOS]: PHOTOCHEMICAL HYDROGEN-PRODUCTION ;  METAL-ORGANIC FRAMEWORK ;  MOLECULAR-SYSTEMS ;  ACTIVE-SITE ;  AQUEOUS-SOLUTION ;  VISIBLE-LIGHT ;  WATER ;  CATALYST ;  EFFICIENT ;  PHOTOGENERATION
语种: 英语
WOS记录号: WOS:000402870300012
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/152231
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Peoples R China
2.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian 116023, Peoples R China
3.KTH Royal Inst Technol, Dept Chem, S-10044 Stockholm, Sweden

Recommended Citation:
Cheng, Minglun,Wang, Mei,Zhang, Shuai,et al. Photocatalytic H-2 production using a hybrid assembly of an [FeFe]-hydrogenase model and CdSe quantum dot linked through a thiolato-functionalized cyclodextrin[J]. FARADAY DISCUSSIONS,2017,198:197-209.
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