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Photocatalytic H-2 production using a hybrid assembly of an [FeFe]-hydrogenase model and CdSe quantum dot linked through a thiolato-functionalized cyclodextrin
Cheng, Minglun1; Wang, Mei1; Zhang, Shuai1; Liu, Fengyuan1; Yang, Yong1; Wan, Boshun2; Sun, Licheng1,3
刊名FARADAY DISCUSSIONS
2017-06-01
DOI10.1039/c6fd00207b
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
关键词[WOS]PHOTOCHEMICAL HYDROGEN-PRODUCTION ; METAL-ORGANIC FRAMEWORK ; MOLECULAR-SYSTEMS ; ACTIVE-SITE ; AQUEOUS-SOLUTION ; VISIBLE-LIGHT ; WATER ; CATALYST ; EFFICIENT ; PHOTOGENERATION
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.
语种英语
WOS记录号WOS:000402870300012
引用统计
文献类型期刊论文
条目标识符http://cas-ir.dicp.ac.cn/handle/321008/152231
专题中国科学院大连化学物理研究所
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
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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.
APA Cheng, Minglun.,Wang, Mei.,Zhang, Shuai.,Liu, Fengyuan.,Yang, Yong.,...&Sun, Licheng.(2017).Photocatalytic H-2 production using a hybrid assembly of an [FeFe]-hydrogenase model and CdSe quantum dot linked through a thiolato-functionalized cyclodextrin.FARADAY DISCUSSIONS,198,197-209.
MLA Cheng, Minglun,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".FARADAY DISCUSSIONS 198(2017):197-209.
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