基于的共价有机框架,用于光催化固定单个原子
Ting He1, Zhanfeng Zhao2,3, Ruoyang Liu4
1School of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, Singapore 637371, Singapore.
Journal of the American Chemical Society
|March 8, 2023
概括
研究人员开发了使用单个黄金原子的新型共价有机框架 (COF),以实现高效的光催化 (N2) 固定. 这些先进材料在环境条件下显著增强了氨 (NH3) 产量.
科学领域:
- 材料科学
- 催化剂
- 纳米技术
背景情况:
- 在环境条件下,高效的 (N2) 固定光催化剂产生氨 (NH3) 是至关重要的,但具有挑战性.
- 共价有机框架 (COF) 提供可调节的结构,高孔隙性和预先设计的化学功能,使其对催化有希望.
研究的目的:
- 探索带有单个黄金 (Au) 原子的基于氨酸的COF对光催化N2固定的潜力.
- 通过调整COF的电子特性来研究结构-活性关系并优化NH3的生产率.
主要方法:
- 一系列同结构基COF (COFX-Au,X=1-5) 的合成,其中 Au单个原子被固定.
- 通过将电子提取或电子捐赠的功能组纳入氨酸单元来调整AU催化中心的电子微环境.
- 在环境条件下评估光催化NH3生产率并分析结构-活性关系.
主要成果:
- 具有强大的电子吸收组的COF1-Au显示出显著增强的NH3生产率 (333.0 ± 22.4 μmol g-1 h-1).
- 使用两种类型的强电子吸收组,COF5-Au进一步提高了NH3的演化速率,达到427.9±18.7μmolg-1h-1.
- 发现吸收电子的组可以促进光生成电子的分离和传输,从而提高催化效率.
结论:
- 用单个Au原子功能化的基于的COF是N2固定的高效光催化剂.
- COF的合理分子设计,特别是吸收电子的组合,使得光电子性质的微调成为可能,从而实现更高的NH3进化.
- 这项研究强调了定制的COF结构在高效和可持续的氨合成方面的潜力.
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