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敏化TiO和ZrO上[Ru(bpy)]薄膜的激发态动力学

Excited-State Dynamics of [Ru(bpy) ] Thin Films on Sensitized TiO and ZrO.

作者信息

Leandri Valentina, Liu Peng, Sadollahkhani Azar, Safdari Majid, Kloo Lars, Gardner James M

机构信息

Department: Department of Chemistry Division of Applied Physical Chemistry, KTH Royal Institute of Technology, Teknikringen 30, SE-10044, Stockholm, Sweden.

出版信息

Chemphyschem. 2019 Feb 18;20(4):618-626. doi: 10.1002/cphc.201801010. Epub 2019 Feb 7.

DOI:10.1002/cphc.201801010
PMID:30623544
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC6593980/
Abstract

The excited state dynamics of Tris(2,2'-bipyridine)ruthenium(II) hexafluorophosphate, [Ru(bpy) (PF ) ], was investigated on the surface of bare and sensitized TiO and ZrO films. The organic dyes LEG4 and MKA253 were selected as sensitizers. A Stern-Volmer plot of LEG4-sensitized TiO substrates with a spin-coated [Ru(bpy) (PF ) ] layer on top shows considerable quenching of the emission of the latter. Interestingly, time-resolved emission spectroscopy reveals the presence of a fast-decay time component (25±5 ns), which is absent when the anatase TiO semiconductor is replaced by ZrO . It should be specified that the positive redox potential of the ruthenium complex prevents electron transfer from the [Ru(bpy) (PF ) ] ground state into the oxidized sensitizer. Therefore, we speculate that the fast-decay time component observed stems from excited-state electron transfer from [Ru(bpy) (PF ) ] to the oxidized sensitizer. Solid-state dye sensitized solar cells (ssDSSCs) employing MKA253 and LEG4 dyes, with [Ru(bpy) (PF ) ] as a hole-transporting material (HTM), exhibit 1.2 % and 1.1 % power conversion efficiency, respectively. This result illustrates the possibility of the hypothesized excited-state electron transfer.

摘要

研究了六氟磷酸三（2,2'-联吡啶）钌（II）（[Ru(bpy)₃(PF₆)₂]）在裸露的和敏化的TiO₂及ZrO₂薄膜表面的激发态动力学。选择有机染料LEG4和MKA253作为敏化剂。在顶部旋涂有[Ru(bpy)₃(PF₆)₂]层的LEG4敏化TiO₂衬底的Stern-Volmer图显示，后者的发射有相当程度的猝灭。有趣的是，时间分辨发射光谱揭示存在一个快速衰减时间成分（25±5 ns），当锐钛矿TiO₂半导体被ZrO₂取代时该成分不存在。应当指出的是，钌配合物的正氧化还原电位阻止电子从[Ru(bpy)₃(PF₆)₂]基态转移到氧化态敏化剂中。因此，我们推测观察到的快速衰减时间成分源于从[Ru(bpy)₃(PF₆)₂]到氧化态敏化剂的激发态电子转移。采用MKA253和LEG4染料、以[Ru(bpy)₃(PF₆)₂]作为空穴传输材料（HTM）的固态染料敏化太阳能电池（ssDSSCs），功率转换效率分别为1.2%和1.1%。这一结果说明了假设的激发态电子转移的可能性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8cfa/6593980/e8e6ec511265/CPHC-20-618-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8cfa/6593980/7106bf6a0258/CPHC-20-618-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8cfa/6593980/42f8a1ed17ca/CPHC-20-618-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8cfa/6593980/1cdf8533b369/CPHC-20-618-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8cfa/6593980/5436e2f38b4a/CPHC-20-618-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8cfa/6593980/21c881f42bd4/CPHC-20-618-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8cfa/6593980/2504eee4c1f5/CPHC-20-618-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8cfa/6593980/e8e6ec511265/CPHC-20-618-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8cfa/6593980/7106bf6a0258/CPHC-20-618-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8cfa/6593980/42f8a1ed17ca/CPHC-20-618-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8cfa/6593980/1cdf8533b369/CPHC-20-618-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8cfa/6593980/5436e2f38b4a/CPHC-20-618-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8cfa/6593980/21c881f42bd4/CPHC-20-618-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8cfa/6593980/2504eee4c1f5/CPHC-20-618-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8cfa/6593980/e8e6ec511265/CPHC-20-618-g007.jpg

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