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选择性甲氧化ZIF-8中的生物启发Cu (II) 缺陷点

Ying Yang¹, Siriluk Kanchanakungwankul², Suman Bhaumik²

¹Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States.

Journal of the American Chemical Society

|October 2, 2023

概括

这项研究开发了一种合铜的金属有机框架催化剂,可选择性地将甲氧化为甲醇和甲. 催化剂在多个循环中表现出高稳定性和提高的选择性,避免了二氧化碳的产生.

科学领域:

催化剂
材料科学
绿色化学

背景情况:

在化学中,直接激活和功能化C-H键是一个重大挑战.
在没有过度氧化到二氧化碳的情况下将甲氧化成有价值的产品,

研究的目的:

为选择性甲氧化合成和激活合铜的ZIF-8金属有机框架 (MOF).
研究化ZIF-8的催化活性,稳定性和转化甲的机制.

主要方法:

合成具有特定Cu/Zn比率的Cu-doped ZIF-8 MOF.
用氧气,甲和蒸汽进行催化激活和反应.
使用PXRD,DRUV-vis,SEM和XAS (XANES,EXAFS) 进行表征.
密度函数理论 (DFT) 计算以阐明反应机制.

主要成果:

添加ZIF-8MOF有效催化甲氧化成甲醇和甲.
催化剂保持至少五个循环,在第三个循环后选择性得到改善以消除二氧化碳检测.
DFT计算显示了一种催化循环,涉及氧激活的Cu (I) 物种和原子转移.

结论:

化ZIF-8MOF为选择性甲氧化提供了一个有前途的平台.
催化机制涉及特定的铜活性位点,并有利于单片反应途径.
这种方法为从甲中可持续生产甲醇提供了潜在的途径.

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