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Interplay between structural parameters and reactivity of Zr6-based MOFs as artificial proteases
Chemical Science ( IF 8.4 ) Pub Date : 2020-05-22 , DOI: 10.1039/d0sc02136a
Alexandra Loosen 1, 2, 3, 4 , Francisco de Azambuja 1, 2, 3, 4 , Simon Smolders 2, 3, 4, 5 , Jens Moons 1, 2, 3, 4 , Charlotte Simms 1, 2, 3, 4 , Dirk De Vos 2, 3, 4, 5 , Tatjana N. Parac-Vogt 1, 2, 3, 4
Affiliation  

Structural parameters influencing the reactivity of metal–organic frameworks (MOF) are challenging to establish. However, understanding their effect is crucial to further develop their catalytic potential. Here, we uncovered a correlation between reaction kinetics and the morphological structure of MOF-nanozymes using the hydrolysis of a dipeptide under physiological pH as model reaction. Comparison of the activation parameters in the presence of NU-1000 with those observed with MOF-808 revealed the reaction outcome is largely governed by the Zr6 cluster. Additionally, its structural environment completely changes the energy profile of the hydrolysis step, resulting in a higher energy barrier ΔG for NU-1000 due to a much larger ΔS term. The reactivity of NU-1000 towards a hen egg white lysozyme protein under physiological pH was also evaluated, and the results pointed to a selective cleavage at only 3 peptide bonds. This showcases the potential of Zr-MOFs to be developed into heterogeneous catalysts for non-enzymatic but selective transformation of biomolecules, which are crucial for many modern applications in biotechnology and proteomics.

中文翻译:

基于Zr6的MOF作为人工蛋白酶的结构参数与反应性之间的相互作用

影响金属-有机骨架(MOF)反应性的结构参数很难确定。但是,了解它们的作用对于进一步开发其催化潜力至关重要。在这里,我们发现了在生理pH下用二肽水解作为模型反应,反应动力学与MOF纳米酶的形态结构之间的相关性。在NU-1000存在下的活化参数与MOF-808所观察到的活化参数的比较表明,反应结果在很大程度上受Zr 6团簇支配。此外,它的结构环境完全改变了水解步骤的能量分布,由于更大的ΔS ,导致NU-1000的能垒更高ΔG 术语。还评估了NU-1000在生理pH下对鸡蛋清溶菌酶蛋白的反应性,结果表明只有3个肽键选择性裂解。这展示了Zr-MOF可能被开发成非均相催化剂用于生物分子的非酶促选择性转化,这对于生物技术和蛋白质组学中的许多现代应用至关重要。
更新日期:2020-07-08
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