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一种PS给体模型化合物的合成和性能
引用本文:施锋,李宏洋,彭孝军,陈小强,张蓉,王东平,樊江莉,孙立成. 一种PS给体模型化合物的合成和性能[J]. 高等学校化学学报, 2004, 25(9): 1666-1672
作者姓名:施锋  李宏洋  彭孝军  陈小强  张蓉  王东平  樊江莉  孙立成
作者单位:大连理工大学精细化工国家重点实验室,大连,116012
基金项目:国家自然科学基金(批准号:20376010,20128005)和国家重点基础研究专项基金资助.
摘    要:
为了模拟植物光系统的给体部分,设计、合成了配合物2.在该模型化合物中,配体的邻位被2个{[2-羟基-3-(吗啉基-4-甲基)-5-叔丁基-苄基](吡啶-2-甲基)胺基-甲基}取代的苯酚通过酰胺键与光敏体[Ru(bpy)3]2+共价相连.利用ESI-MS和1D,2DNMR(gCOSY,HSQC和HMBC)对化合物结构进行了鉴定,并通过UV-Vis、荧光发射光谱、闪光光解及电化学对其光化学性能和氧化还原特性进行了研究.结果表明,化合物的吸收波长发生红移;激发态寿命长;可螯合双核高价Mn()原子;且Ru3+/Ru2+的氧化电位比Phenol+/Phenol和Mn(,)/Mn()的高,满足自然界PS电子转移的基本要求,可用于PS给体部分的初步研究.

关 键 词:配体设计  含酚配体  双核配合物  水氧化  光系统  人工光合作用
文章编号:0251-0790(2004)09-1666-07
收稿时间:2003-07-07

Synthesis and Properties of a New Donor Model Compound for PS Ⅱ
SHI Feng,LI Hong-Yang,PENG Xiao-Jun,CHEN Xiao-Qiang,ZHANG Rong,WANG Dong-Ping,FAN Jiang-Li,SUN Li-Cheng. Synthesis and Properties of a New Donor Model Compound for PS Ⅱ[J]. Chemical Research In Chinese Universities, 2004, 25(9): 1666-1672
Authors:SHI Feng  LI Hong-Yang  PENG Xiao-Jun  CHEN Xiao-Qiang  ZHANG Rong  WANG Dong-Ping  FAN Jiang-Li  SUN Li-Cheng
Affiliation:State Key Laboratory of Fine Chemicals, Dalian University of Technology, Dalian 116012, China
Abstract:
As a model compound for redox components on the donor side of photosystem Ⅱ(PSⅡ) in green plants, a supramolecular complex 2 was synthesized and characterized. In this complex, two {[(2-hydroxy-3-(morpholin-4-ylmethyl)-5-tert-butyl-benzyl)(pyridyl-2-methyl)amino]methyl} arms are linked to the ortho-positions of a phenol which is expected covalently to be linked to Ru(Ⅱ) tris-bipyridine through an amide bond. The arms on the substituted-phenol can coordinate two Mn(Ⅲ) ions. The structure of complex 2 was confirmed by electrospray ionization mass spectrometry(ESI-MS) and 2D-NMR(gCOSY, HSQC and HMBC). Its photochemical and electrochemical properties were studied. The results showed that the MLCT band of the compound was red-shifted compared to that of [Ru(bpy)3]2+ and the luminescence quantum yield was enhanced. In addition, the oxidation potential of ruthenium was higher than the phenol+/phenol and Mn(Ⅲ, Ⅳ)/Mn(Ⅲ), which was consisted with the electron transfer sequence of the donor side of PSⅡ in nature. All these showed that this compound was a good model to mimic the donor side of PSⅡ.
Keywords:Ligand design  Phenolate ligand  Dinuclear complex  Water oxidation  Photosystem Ⅱ  Artificial photosynthesis
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