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通过外层微环境调制在光触媒氧化过程中合有机框架中开启单点氧气生成

Suleman Suleman¹, Yi Zhang¹, Yunyang Qian¹

¹Hefei National Research Center for Physical Sciences at the Microscale, Department of Chemistry, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.

Angewandte Chemie (International ed. in English)

|November 28, 2023

概括

研究人员开发了基于甲的共价有机框架 (COFs),以有效地产生单片氧 (O2). 在COF上的功能组创造了一个微环境,优化了光催化氧化反应的O2生成.

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.
摄影化学的使用.

背景情况:

单片氧 (O2) 对于光催化氧化至关重要,但很难有效和选择性地生产.
共价有机框架 (COF) 为催化应用提供可调节的结构.

研究的目的:

为了合成基于甲的COF,与量身定制的孔壁功能组.
研究这些功能组对COFs单片氧生成和乙烯氧化活性的影响.

主要方法:

合成不同功能组 (,甲) 的基于甲的COF.
在O2介导的乙烯氧化中对催化活性的评估.
使用密度函数理论 (DFT) 描述电子属性和计算分析.

主要成果:

对于O2生产的COF催化活性与电子捐赠功能组增加.
甲基功能化COF在铁氧化中获得了98%的产量,比基功能化COF显著改善.
电子性质和激发性行为,受波段能量水平和轨道组成的影响,与催化活性相关.

结论:

在COF中外层微环境调制是调节活性氧物种 (ROS) 生成的有效策略.
这项研究展示了通过COF的外层微环境调制控制ROS生成的第一个实例.
这些发现为设计用于选择性光催化氧化的先进COF铺平了道路.

关键词:

协价有机框架协价有机框架能源转移能源转移外层球的微环境外层球的微环境光催化作用的光催化单片氧气单片氧气的使用

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