生物模拟双协调球基共价有机框架可实现高效和选择性氧化
Jiamin Zhan1, Xiaoling Wu2, Xueqing Qiu3
1School of Chemistry and Chemical Engineering, Guangdong Provincial Engineering Research Center for Green Fine Chemicals, South China University of Technology, Guangzhou 510641, China.
ACS applied materials & interfaces
|August 28, 2025
概括
研究人员开发了一种以金属酶为灵感的仿生催化剂 (Fe-TAPP-TT). 这种高效的催化剂模仿自然酶进行可持续的化学转化,在furfural氧化中表现出高活性.
科学领域:
- 材料科学
- 催化剂
- 生物模拟化学
背景情况:
- 自然的金属酶具有对催化效率至关重要的层次结构.
- 开发模仿这些结构的人造催化剂是可持续化学的关键.
- 共价有机框架 (COF) 为设计先进的催化材料提供了多功能平台.
研究的目的:
- 在COF中设计具有第一和第二协调球体的仿生催化剂.
- 创建一个有效的催化剂选择性氧化生物质衍生平台化学物质.
- 研究工程协调球体在催化活动中的机械作用.
主要方法:
- 通过溶热凝结和铁金属化合成Fe-TAPP-TT催化剂.
- 催化剂的结构和协调环境的描述.
- 对过氧化酶类活性和催化效率的评估 (Kcat/KM).
- 在furfural选择性氧化到5-hydroxy-2(5H) -furanone (HFO) 的应用.
- 使用电子磁共振 (EPR) 和密度函数理论 (DFT) 计算的机制研究.
主要成果:
- Fe-TAPP-TT催化剂表现出高的过氧化酶类活性 (19. 3M-1s-1),与细胞染色体c相当.
- 在温和条件下达到99.1%的furfural转化和53.4%的HFO产量.
- 机械研究显示了催化口袋的协同H2O2激活和中间稳定.
结论:
- 在COF内设计的双协调球提高了催化性能.
- Fe-TAPP-TT 作为一种有效的酶模仿剂,用于可持续的化学转化.
- 这种策略使得能够合理设计以自然为灵感的先进催化剂.
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