Robust Nitro-Functionalized {Zn<sub>3</sub>}-Organic Framework for Excellent Catalytic Performance on Cycloaddition Reaction of CO<sub>2</sub> with Epoxides and Knoevenagel Condensation
作者:Meiyu Ren、Chong Li、Tuoping Hu、Liming Fan、Xiutang Zhang
DOI:10.1021/acs.cgd.4c00209
日期:2024.4.17
Adjusting the Lewis acid–base sites in MOF-based catalysts to meet the demand for catalytic CO2 chemical fixation is a huge challenge. Herein, a highly robust rectilinear Zn3}-based metal–organic framework of [Zn3(TNTNB)2(4,4′-bip)(H2O)2]·5DMF·9H2O}n (NUC-80) was generalized from the solvothermal condition (H3TNTNB = 1,3,5-tri(3-nitro-4-carboxyphenyl)-2,4,6-trinitrobenzene, 4,4′-bip = 4,4′-bipyridine)
调整MOF基催化剂中的路易斯酸碱位以满足催化CO 2化学固定的需求是一个巨大的挑战。本文中,一种高度鲁棒的直线Zn 3 }基金属有机骨架[Zn 3 (TNNTB) 2 (4,4'-bip)(H 2 O) 2 ]·5DMF·9H 2 O} n ( NUC -80 ) 由溶剂热条件推广 (H 3 TNTNB = 1,3,5-三(3-硝基-4-羧基苯基)-2,4,6-三硝基苯, 4,4'-bip = 4,4' -联吡啶)。活化的NUC-80a不仅拥有大的空隙体积(58%)和两种溶剂可进入的通道:沿轴的菱形(约14.24 × 14.57 Å)和矩形(约11.72 × 14.48 Å)沿b轴,但也通过其内表面上丰富的金属位点和大量硝基进行功能化。催化实验证实NUC-80a可以在温和条件下以高周转频率(TOF)有效催化CO 2与环氧化物的环加成反应以及醛和丙二腈的Knoevenagel缩合反应。因