调节坚固的金属结有机框架的微环境,以促进光催化的进化
Chong-Jiu Lu1, Wen-Jie Shi1, Yun-Nan Gong1
1Institute for New Energy Materials and Low Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin, 300384, China.
Angewandte Chemie (International ed. in English)
|July 20, 2024
概括
稳定的金属有机框架 (MOFs) 对光催化进化有希望. 新的基HOF表现出了显著的稳定性和高的H2生产率,没有贵金属,超过了Pt辅助系统.
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.
- 可再生能源可再生能源是可再生能源.
背景情况:
- 与结合的有机框架 (HOFs) 对光催化进化有希望.
- 现有的HOF往往缺乏稳定性,并且需要合金催化剂才能有效地活动.
研究的目的:
- 为光催化生产开发稳定和高度活跃的HOF.
- 研究功能组对HOF稳定性和催化性能的影响.
主要方法:
- 一系列基于二核复合物的HOF (Co2-HOF-X) 的合理构建.
- 在恶劣的酸性和基本性条件下评估HOF稳定性.
- 评估光催化H2生产速度与不同的-X功能组.
- 电子结构和反应机制的计算分析.
主要成果:
- Co2-HOF-X材料在12M HCl和5M NaOH中表现出超过10天的特殊稳定性.
- 光催化 H2 生产速率与 -X 组不同: -COOMe > -Br > -tBu > -OMe.
- 优化的CO2-HOF-COOMe在没有贵金属催化剂的情况下实现了12.8 mmol g-1 h-1的速率.
- 功能组电子提取能力调节的催化中心和质子激活屏障.
结论:
- 基于双核复合体的HOF为光催化进化提供了稳定高效的平台.
- 在HOF上调整功能组为优化催化活性提供了一种策略.
- 这些HOF为绿色生产提供了与基系统的可行替代方案.
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