一个"Dangling" Co (II) 离子与一个Oxo Cubane相结合的影响
Andy I Nguyen1, Lucy E Darago1, David Balcells2
1Department of Chemistry , University of California at Berkeley , Berkeley , California 94720-1460 , United States.
Journal of the American Chemical Society
|July 14, 2018
概括
合成了一种新型的 - 复合物与 (II) "". 这种五金属复合体表现出反铁磁合和增强的氧化还原活性,为光系统II模型提供了洞察力.
科学领域:
- 无机化学
- 生物有机化学
- 材料科学
背景情况:
- -氧化核心与光系统II的氧化中心相关.
- 过渡金属"危险物"复合物很少见,并提供独特的结构和电子特性.
- 对于催化剂设计来说,了解外围配体对古巴核特性的影响至关重要.
研究的目的:
- 合成和表征一种新的五金属-复合物,使用 (II) .
- 调查新复合体的结构性,磁性和电化学特性.
- 为了比较子复合体与其母体古巴体的特性,
主要方法:
- 合成五金属复合物 MnIVCoIII3CoIIO4(OAc) 6(NO3) ((py) 3 (2) 从一个-氧化前体.
- 超导量子干扰装置 (SQUID) 磁度测量以确定磁性.
- 密度函数理论 (DFT) 计算以阐明电子结构和磁合.
- 循环电压测量以调查电化学行为.
主要成果:
- 这种合成产生了五金属悬浮复合体2,其结构类似于光系统II的氧化中心.
- SQUID磁力测量和DFT计算显示,由于CoII和MnIV离子之间的反铁磁合,S=0的基本状态.
- 复合体2在低温下呈现S=0的基本状态,在高温下转变为脱状态.
- 电压测量显示了复合体2的四个电化学事件,比原始基团1多了两次,表明氧化还原状态增加.
结论:
- 添加 (II) 悬挂剂显著影响-芯的磁性和电化学性质.
- 描述的复合体是研究古巴核与外围金属离子相互作用的罕见模型.
- 这些发现有助于更深入地了解人工光合作用相关的多核金属复合体中的电子转移和磁相互作用.
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