Flores J Gabriel, Sánchez-González Elí, Gutiérrez-Alejandre Aída, Aguilar-Pliego Julia, Martínez Ana, Jurado-Vázquez Tamara, Lima Enrique, González-Zamora Eduardo, Díaz-García Manuel, Sánchez-Sánchez Manuel, Ibarra Ilich A
UAM-Azcapotzalco, San Pablo 180, Col. Reynosa-Tamaulipas, Azcapotzalco, C.P. 02200, Ciudad de México, Mexico.
Dalton Trans. 2018 Mar 26;47(13):4639-4645. doi: 10.1039/c7dt04701k.
A greener synthesis of Cu-MOF-74 was obtained, for the first time, in methanol as the unique solvent and at room temperature. Full characterisation of the MOF material showed its purity and also its nanocrystalline nature. Complete activation (150 °C for 1 h and 10-3 bar) of Cu-MOF-74 afforded unsaturated Cu metal sites and this was corroborated by in situ DRIFT spectroscopy. The access to these Cu open metal sites was tested for the catalytic transformation of trans-ferulic acid to vanillin (yield of 71% and 97% selectivity) and a plausible catalytic reaction mechanism was postulated based on quantum chemical calculations.
首次在甲醇作为唯一溶剂且室温条件下实现了Cu-MOF-74的绿色合成。对该金属有机框架材料的全面表征显示了其纯度及其纳米晶体性质。对Cu-MOF-74进行完全活化(150℃下1小时,压力为10⁻³ 巴)可得到不饱和铜金属位点,原位漫反射红外傅里叶变换光谱证实了这一点。测试了利用这些铜开放金属位点将反式阿魏酸催化转化为香草醛(产率为71%,选择性为97%),并基于量子化学计算推测了一个合理的催化反应机理。