同时调整异构集金属有机框架中的水稳定性和光电活性,以实现高效的光催化生产
Yu-Jia Cheng1,2, Jian-Qiang Zhao1, Xiong-Feng Ma2
1State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, 350002, China.
Advanced materials (Deerfield Beach, Fla.)
|April 3, 2025
概括
具有集成铜集群的工程金属有机框架 (MOF) 显示了可持续生产的增强稳定性和可见光活性. 替代显著提高了性能,使得没有贵金属的进化率翻了一番.
科学领域:
- 材料科学 材料科学 材料科学
- 催化剂是一种催化剂.
- 纳米技术 纳米技术
背景情况:
- 在金属有机框架 (MOF) 中实现结构稳定性和光活性对于高效的光催化 (H2) 生产至关重要.
- 当前的MOF设计面临着在不同条件下平衡稳定性的挑战,同时具有最佳的催化电子特性.
研究的目的:
- 开发具有增强结构完整性和光电化学性质的新型MOF,用于可持续的H2生成.
- 调查精确集群工程和素替代对光催化中的MOF性能的影响.
主要方法:
- 原子精确的异构群组件,以构建具有cds净的同结构3DMOF (CuSL-CuX,X = Cl,Br).
- 在MOF结构中整合了六核铜-硫 {Cu6S6} 和二核铜-素 {Cu2X2} 集群.
- 在广泛的pH范围 (1-14),可见光吸收,氧化还原潜力,电荷载体动力学和光催化H2进化速率中对MOF稳定性的表征.
主要成果:
- 两种同结构MOF,CuSL-CuCl和CuSL-CuBr,已成功合成,在pH值1到14之间表现出异常稳定性.
- 与CuSL-CuCl (26.99 mmol g-1 h-1) 相比,CuSL-CuBr表现出明显更高的H2进化率 (50.28 mmol g-1 h-1),超过了许多现有的MOF光催化剂.
- 发现替代能优化电子结构,完善轨道分布,加速电荷分离,提高光催化效率.
结论:
- 异质集群组装方法使得能够设计出具有可调节光电子性能的强大的MOF.
- 素替代,特别是,是增强MOFs用于H2生产的光催化活性的一个关键战略.
- 这项工作通过精确的集群工程为开发高性能,稳定的基于MOF的光催化剂提供了新的范式.
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