Enantioselective catalysts based on metal-organic framework-supported nucleotides

被引:0
作者
Wang, Danyu [1 ,2 ]
Li, Zhe [1 ]
Luo, Tian-Yi [1 ]
Schmithorst, Michael B. [3 ]
Park, Sunghwan [1 ,4 ]
Xu, Wenqian [5 ]
Miao, Yurun [1 ]
Gawande, Kaivalya [6 ]
Tang, Chaoyun [6 ]
Bukowski, Brandon C. [2 ]
Chmelka, Bradley F. [3 ]
Fairbrother, Howard [7 ]
Kokkoli, Efrosini [1 ,2 ]
Tsapatsis, Michael [1 ,2 ,8 ]
机构
[1] Johns Hopkins Univ, Inst NanoBioTechnol, 3400 N Charles St, Baltimore, MD 21218 USA
[2] Johns Hopkins Univ, Dept Chem & Biomol Engn, 3400 N Charles St, Baltimore, MD 21218 USA
[3] Univ Calif Santa Barbara, Dept Chem Engn, Santa Barbara, CA 93106 USA
[4] Kyungpook Natl Univ, Sch Energy Mat & Chem Engn, 2559 Gyeongsang Daero, Sangju Si 37224, Gyeongsangbug D, South Korea
[5] Argonne Natl Lab, X Ray Sci Div, Adv Photon Source, Lemont, IL 60439 USA
[6] Univ Massachusetts Amherst, Dept Chem Engn, Amherst, MA 01003 USA
[7] Johns Hopkins Univ, Dept Chem, 3400 N Charles St, Baltimore, MD 21218 USA
[8] Johns Hopkins Univ, Appl Phys Lab, 11100 Johns Hopkins Rd, Laurel, MD 20723 USA
关键词
Metal-organic framework; Artificial metalloenzyme; Asymmetric catalysis; Heterogenous catalysis; DIELS-ALDER REACTION; AUXILIARY BASIS-SETS; ARTIFICIAL METALLOENZYMES; HYBRID CATALYSTS; DNA; WATER; SEPARATION; DESIGN; SITES;
D O I
10.1016/j.micromeso.2023.112703
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Adenosine triphosphate (ATP) and other nucleotides can be irreversibly bound to the metal-organic framework (MOF) MIL-101(Cr). Analysis of X-ray diffraction data suggests that the location of the adsorbed ATP molecule is in proximity of the Cr3 clusters. Solid-state NMR and DFT calculations indicate that ATP is bound to MIL-101(Cr) through linkages of the terminal phosphate group with Cr(III) of the framework. In the presence of Cu(II) ions, the MOF-supported nucleotides can function as stable and reusable enantioselective heterogeneous catalysts for reactions like Diels-Alder and Michael addition. Compared to the corresponding homogeneous nucleotide-based artificial metalloenzymes (ArMs), the MOF-supported nucleotide-based ArMs exhibit significantly enhanced activity and selectivity in certain cases, demonstrating their potential as a new class of enantioselective heterogeneous catalysts.
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页数:12
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