在金属有机框架中的氧化物二次建筑单元在可见光下催化演变
Yang Song1, Zhe Li1,2, Yuanyuan Zhu1
1Department of Chemistry , The University of Chicago , 929 E 57th Street , Chicago , Illinois 60637 , United States.
Journal of the American Chemical Society
|July 25, 2019
概括
我们开发了新的金属有机框架 (MOF), 这些MOF在可见光下表现出高性能,展示了它们在可再生能源应用中的潜力.
科学领域:
- 材料科学
- 光催化
- 可再生能源
背景情况:
- 金属有机框架 (MOF) 为催化应用提供可调节的结构.
- 有效的光催化演化 (HER) 对可持续的能源生产至关重要.
- 基于的MOF是光催化剂的有希望的候选物.
研究的目的:
- 设计和合成用和复合物的新型MOF.
- 在可见光下研究这些新型MOF的光催化演化活性.
- 阐明光催化演变的机制和影响催化效率的因素.
主要方法:
- 通过将光敏化对象入Ti3-BPDC框架来合成Ti3-BPDC-Ir和Ti3-BPDC-Ru MOF.
- 在可见光照射下进行光催化进化实验.
- 光物理和电化学表征 (例如,UV-Vis,光,循环电压测量).
- 密度函数理论 (DFT) 计算以了解反应机制.
主要成果:
- 成功合成了Ti3-BPDC-Ir和Ti3-BPDC-Ru的MOF.
- 在光催化演化过程中,Ti3-BPDC-Ir达到6632个,Ti3-BPDC-Ru达到786个.
- 光物理和电化学研究揭示了一种涉及降解火和电子转移到Ti3 (OH) 2SBU的机制.
- DFT计算确定了关键的中间体和反应途径,包括Ti (III) -OH的质子化和质子合电子转移.
结论:
- 设计的MOF对进化具有出色的光催化活性.
- 和光敏剂的注显著提高了HER的性能.
- 这项研究为光催化过程提供了机理性见解,指导了未来的能源应用MOF设计.
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