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一个CuICoII加密用于可见光驱动的CO2减少
Julia Jökel1, Esma Birsen Boydas2, Joël Wellauer3
1Fraunhofer UMSICHT Osterfelder Str. 3 46047 Oberhausen Germany ulf-peter.apfel@umsicht.fraunhofer.de ulf.apfel@rub.de.
Chemical science
|November 29, 2023
概括
这项研究突出了铜-双金属复合物 ({N^S N^N}_m) 作为有效的光催化剂,用于将二氧化碳 (CO2) 转化为一氧化碳 (CO). 该综合体表现出高选择性和营业额,由协同金属催化驱动.
科学领域:
- 协调化学 协调化学
- 光催化作用的光催化
- 减少二氧化碳 减少二氧化碳
背景情况:
- 双金属复合物,特别是含有 CoII CoII 和 ZnII CoII 的六胺加密物,是已知的减少 CO2 的光催化剂.
- 不对称的密码体{N^S N^N}_m具有明显的富含硫和的结合点,模仿自然的减少二氧化碳的酶.
- 之前的工作报告了CuIMII (MII = CoII,NiII,CuII) 复合体与这个密码.
研究的目的:
- 为了研究CuICoII复合体的{N^S N^N}_m作为可见光驱动的二氧化碳减少的光催化剂.
- 了解金属氧化状态和硫合并对光催化活性的影响.
- 阐明铜和之间的协同催化机制.
主要方法:
- 对CuICoII-{N^S N^N}_m复合物的合成和表征.
- 使用450纳米的LED辐射在乙和水混合物中进行24小时的光触媒CO2减排实验.
- 用单核复合体进行比较研究和计算分析.
主要成果:
- 该CuICoII-{N^S N^N}_m复合物实现了高效的CO2-CO转换 (9.22μmol),具有高的周转率 (2305) 和选择性 (98%).
- 确定Cu和Co之间的协同催化是高光催化活性的主要驱动因素.
- 相关复合体中金属距离的增加导致了协同效应的丧失,有利于单位 Co 催化.
结论:
- CuICoII-{N^S N^N}_m复合体是一种高效和选择性的二氧化碳减排光催化剂.
- 铜和中心之间的协同效应对于最佳的催化性能至关重要.
- 金属离子的空间布局显著影响了催化机制和效率.
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