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Reticular Synthesis of Highly Crystalline Three-Dimensional Mesoporous Covalent–Organic Frameworks for Lipase Inclusion
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-10-16 , DOI: 10.1021/jacs.3c07904 Haoyu Liu 1 , Yi Zhou 2 , Jinbiao Guo 3 , Rui Feng 1, 4 , Gaoli Hu 5 , Jiandong Pang 1 , Yao Chen 3 , Osamu Terasaki 2 , Xian-He Bu 1, 4
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-10-16 , DOI: 10.1021/jacs.3c07904 Haoyu Liu 1 , Yi Zhou 2 , Jinbiao Guo 3 , Rui Feng 1, 4 , Gaoli Hu 5 , Jiandong Pang 1 , Yao Chen 3 , Osamu Terasaki 2 , Xian-He Bu 1, 4
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The synthesis and application of three-dimensional (3D) mesoporous covalent–organic frameworks (COFs) are still to be developed. Herein, two mesoporous 3D COFs with an stp topology were synthesized in a highly crystalline form with aniline as the modulator. The chemical composition of these COFs was confirmed by Fourier transform infrared (FT-IR) and 13C cross-polarization magic angle spinning nuclear magnetic resonance (NMR) spectroscopies. These 3D mesoporous COFs were highly crystalline and exhibited permanent porosity and good chemical stability in both aqueous and organic media. The space group and unit cell parameters of COF HFPTP-TAE were verified by powder X-ray diffraction (PXRD), small-angle X-ray scattering, and three-dimensional electron diffraction (3D ED). The appropriate pore size of the COF HFPTP-TAE facilitated the inclusion of enzyme lipase PS with a loading amount of 0.28 g g–1. The lipase⊂HFPTP-TAE (⊂ refers to “include in”) composite exhibited high catalytic activity, good thermal stability, and a wide range of solvent tolerance. Specifically, it could catalyze the alcoholysis of aspirin methyl ester (AME) with high catalytic efficiency. Oriented one-dimensional (1D) channel mesopores in HFPTP-TAE accommodated lipase, meanwhile preventing them from aggregation, while windows on the wall of the 1D channel favored molecular diffusion; thus, this COF-enzyme design outperformed its amorphous isomer, two-dimensional (2D) mesoporous COF, 3D mesoporous COF with limited crystallinity, and mesoporous silica as an enzyme host.
中文翻译：
用于脂肪酶包合的高结晶度三维介孔共价有机框架的网状合成
三维（3D）介孔共价有机框架（COF）的合成和应用仍有待开发。在此，以苯胺作为调节剂，以高度结晶形式合成了两种具有stp拓扑的介孔3D COF。这些 COF 的化学成分通过傅里叶变换红外 (FT-IR) 和13 C 交叉偏振魔角旋转核磁共振 (NMR) 光谱得到证实。这些3D介孔COF具有高度结晶性，在水性和有机介质中均表现出永久的孔隙率和良好的化学稳定性。通过粉末X射线衍射（PXRD）、小角X射线散射和三维电子衍射（3D ED）验证了COF HFPTP-TAE的空间群和晶胞参数。COF HFPTP-TAE 适当的孔径有利于脂肪酶 PS 的包含，负载量为 0.28 gg –1。脂肪酶⊂HFTPP-TAE（⊂指“包含在”）复合材料表现出高催化活性、良好的热稳定性和广泛的溶剂耐受性。具体来说，它可以高催化效率催化阿司匹林甲酯（AME）的醇解。HFPTP-TAE 中的定向一维 (1D) 通道介孔可容纳脂肪酶，同时防止它们聚集，而 1D 通道壁上的窗口有利于分子扩散；因此，这种COF酶设计优于其无定形异构体、二维（2D）介孔COF、结晶度有限的3D介孔COF以及作为酶宿主的介孔二氧化硅。
更新日期：2023-10-16
中文翻译：
用于脂肪酶包合的高结晶度三维介孔共价有机框架的网状合成
三维（3D）介孔共价有机框架（COF）的合成和应用仍有待开发。在此，以苯胺作为调节剂，以高度结晶形式合成了两种具有stp拓扑的介孔3D COF。这些 COF 的化学成分通过傅里叶变换红外 (FT-IR) 和13 C 交叉偏振魔角旋转核磁共振 (NMR) 光谱得到证实。这些3D介孔COF具有高度结晶性，在水性和有机介质中均表现出永久的孔隙率和良好的化学稳定性。通过粉末X射线衍射（PXRD）、小角X射线散射和三维电子衍射（3D ED）验证了COF HFPTP-TAE的空间群和晶胞参数。COF HFPTP-TAE 适当的孔径有利于脂肪酶 PS 的包含，负载量为 0.28 gg –1。脂肪酶⊂HFTPP-TAE（⊂指“包含在”）复合材料表现出高催化活性、良好的热稳定性和广泛的溶剂耐受性。具体来说，它可以高催化效率催化阿司匹林甲酯（AME）的醇解。HFPTP-TAE 中的定向一维 (1D) 通道介孔可容纳脂肪酶，同时防止它们聚集，而 1D 通道壁上的窗口有利于分子扩散；因此，这种COF酶设计优于其无定形异构体、二维（2D）介孔COF、结晶度有限的3D介孔COF以及作为酶宿主的介孔二氧化硅。
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