Synthesis and characterization of a novel high valent dinuclear MnIII,III complex of triphenolate ligand [N4O3]3- as a model for OEC in PSII

Hong Yang Li; Feng Shi; Xiao Jun Peng; Li Cheng Sun; Rong Zhang; Li Zhu Zhang; Xiao Qiang Chen

Synthesis and characterization of a novel high valent dinuclear Mn^III,III complex of triphenolate ligand [N₄O₃]^3- as a model for OEC in PSII

Hong Yang Li, Feng Shi, Xiao Jun Peng, Li Cheng Sun, Rong Zhang, Li Zhu Zhang, Xiao Qiang Chen

Dalian University of Technology

科研成果: 期刊稿件 › 文章 › 同行评审

摘要

A novel high valent [Mn₂(III/III)L (μ-OAc)₂]·PF₆ complex is prepared, where L is 2,6-bis {[(2-hydroxy-5-tert-butylbenzyl) (pyridyl-2-methylene)-amino]methylene}-4-methylphenol, which contains additional phenolate functional groups and tert-butyl groups as compared to [Mn₂(II/II)(bpmp) (μ-OAc)₂]·ClO₄. In this complex, two pseudo-octahedrally coordinated Mn ions are bridged by a phenolate group and two bidentate acetate ligands. The stronger and more coordinate bonds between anionic phenolate groups and Mn ions in higher oxidation state prevent the dissociation of central ions. The additional tert-butyl groups improve the solubility and electronic cloud density of the ligand. These improvements narrow the disparity between the new model and (Mn)₄ cluster (oxygen-evolving center in nature). IR, ESI-MS, NMR (gCOSY, gHMBC, gHSQC) and electrochemistry characterized the new ligand or complex.

源语言	英语
页（从-至）	17-21
页数	5
期刊	Dalian Ligong Daxue Xuebao/Journal of Dalian University of Technology
卷	45
期	1
出版状态	已出版 - 1月 2005
已对外发布	是

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@article{8143f4387af84079a936ecacd2bf7f9b,

title = "Synthesis and characterization of a novel high valent dinuclear MnIII,III complex of triphenolate ligand [N4O3]3- as a model for OEC in PSII",

abstract = "A novel high valent [Mn2(III/III)L (μ-OAc)2]·PF6 complex is prepared, where L is 2,6-bis {[(2-hydroxy-5-tert-butylbenzyl) (pyridyl-2-methylene)-amino]methylene}-4-methylphenol, which contains additional phenolate functional groups and tert-butyl groups as compared to [Mn2(II/II)(bpmp) (μ-OAc)2]·ClO4. In this complex, two pseudo-octahedrally coordinated Mn ions are bridged by a phenolate group and two bidentate acetate ligands. The stronger and more coordinate bonds between anionic phenolate groups and Mn ions in higher oxidation state prevent the dissociation of central ions. The additional tert-butyl groups improve the solubility and electronic cloud density of the ligand. These improvements narrow the disparity between the new model and (Mn)4 cluster (oxygen-evolving center in nature). IR, ESI-MS, NMR (gCOSY, gHMBC, gHSQC) and electrochemistry characterized the new ligand or complex.",

keywords = "Artificial photosynthesis, Dinuclear manganese complex, Ligand design, Oxygen-evolving center, Phenolate ligand",

author = "Li, {Hong Yang} and Feng Shi and Peng, {Xiao Jun} and Sun, {Li Cheng} and Rong Zhang and Zhang, {Li Zhu} and Chen, {Xiao Qiang}",

year = "2005",

month = jan,

language = "英语",

volume = "45",

pages = "17--21",

journal = "Dalian Ligong Daxue Xuebao/Journal of Dalian University of Technology",

issn = "1000-8608",

publisher = "Dalian University of Technology",

number = "1",

}

TY - JOUR

T1 - Synthesis and characterization of a novel high valent dinuclear MnIII,III complex of triphenolate ligand [N4O3]3- as a model for OEC in PSII

AU - Li, Hong Yang

AU - Shi, Feng

AU - Peng, Xiao Jun

AU - Sun, Li Cheng

AU - Zhang, Rong

AU - Zhang, Li Zhu

AU - Chen, Xiao Qiang

PY - 2005/1

Y1 - 2005/1

N2 - A novel high valent [Mn2(III/III)L (μ-OAc)2]·PF6 complex is prepared, where L is 2,6-bis {[(2-hydroxy-5-tert-butylbenzyl) (pyridyl-2-methylene)-amino]methylene}-4-methylphenol, which contains additional phenolate functional groups and tert-butyl groups as compared to [Mn2(II/II)(bpmp) (μ-OAc)2]·ClO4. In this complex, two pseudo-octahedrally coordinated Mn ions are bridged by a phenolate group and two bidentate acetate ligands. The stronger and more coordinate bonds between anionic phenolate groups and Mn ions in higher oxidation state prevent the dissociation of central ions. The additional tert-butyl groups improve the solubility and electronic cloud density of the ligand. These improvements narrow the disparity between the new model and (Mn)4 cluster (oxygen-evolving center in nature). IR, ESI-MS, NMR (gCOSY, gHMBC, gHSQC) and electrochemistry characterized the new ligand or complex.

AB - A novel high valent [Mn2(III/III)L (μ-OAc)2]·PF6 complex is prepared, where L is 2,6-bis {[(2-hydroxy-5-tert-butylbenzyl) (pyridyl-2-methylene)-amino]methylene}-4-methylphenol, which contains additional phenolate functional groups and tert-butyl groups as compared to [Mn2(II/II)(bpmp) (μ-OAc)2]·ClO4. In this complex, two pseudo-octahedrally coordinated Mn ions are bridged by a phenolate group and two bidentate acetate ligands. The stronger and more coordinate bonds between anionic phenolate groups and Mn ions in higher oxidation state prevent the dissociation of central ions. The additional tert-butyl groups improve the solubility and electronic cloud density of the ligand. These improvements narrow the disparity between the new model and (Mn)4 cluster (oxygen-evolving center in nature). IR, ESI-MS, NMR (gCOSY, gHMBC, gHSQC) and electrochemistry characterized the new ligand or complex.

KW - Artificial photosynthesis

KW - Dinuclear manganese complex

KW - Ligand design

KW - Oxygen-evolving center

KW - Phenolate ligand

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M3 - 文章

AN - SCOPUS:16844369691

SN - 1000-8608

VL - 45

SP - 17

EP - 21

JO - Dalian Ligong Daxue Xuebao/Journal of Dalian University of Technology

JF - Dalian Ligong Daxue Xuebao/Journal of Dalian University of Technology

IS - 1

ER -

Synthesis and characterization of a novel high valent dinuclear MnIII,III complex of triphenolate ligand [N4O3]3- as a model for OEC in PSII

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Synthesis and characterization of a novel high valent dinuclear Mn^III,III complex of triphenolate ligand [N₄O₃]^3- as a model for OEC in PSII