[Fe4]和[Fe6]由酸盐支持的化群:合成,表征和应用在N2减少
Ryoichi Araake, Kazuki Sakadani, Mizuki Tada
1Department of Chemistry, Daido University , Takiharu-cho, Minami-ku, Nagoya 457-8530, Japan.
新的铁团催化了 (N2) 的化. 这些铁集群在温和条件下有效地将N2转化为化产品,为固定提供了潜在的途径.
科学领域:
- 无机化学
- 有机金属化学
- 催化剂
背景情况:
- 通过化物桥接的多个铁原子是 (N2) 减少的关键结构动机.
- 了解这些铁类物种的作用对于生物和工业N2固定至关重要.
研究的目的:
- 合成和描述新的化物支持的铁集群.
- 在N2化中研究这些铁的催化活性.
主要方法:
- 一个Fe (II) 胺复合物与酸在素存在/不存在的情况下的反应.
- 由此产生的[Fe4]和[Fe6]星团的晶体和光谱表征.
- 在环境条件下对合成集群进行N2化试验.
主要成果:
- 精确定义的化物支持铁集群的合成:Fe4(μ-H)4(μ3-H)2{N(SiMe3)2}2(PR3)4和Fe6(μ-H)10(μ3-H)2(P3)10.
- 这些集群的催化N2化产生了每个Fe4集群高达160±13的N3和每一个Fe6集群高达183±18的等值.
- 质谱测试和添加物形成表明,作为催化循环的一部分,连接物解离 (素和化物).
结论:
- 化物支持的铁是N2化的有效催化剂.
- 催化活性显著,并观察到高周转率.
- 联结分离在活性催化物种的产生中起作用.
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