Song Qiao, Cheng Zihe, Perrier Sébastien
Department of Chemistry, University of Warwick Coventry CV4 7AL UK
Shenzhen Grubbs Institute, Southern University of Science and Technology Shenzhen 518055 China.
Polym Chem. 2023 Sep 14;14(41):4712-4718. doi: 10.1039/d3py00993a. eCollection 2023 Oct 24.
Peptide-based artificial enzymes are attracting significant interest because of their remarkable resemblance in both composition and structure to native enzymes. Herein, we report the construction of histidine-containing cyclic peptide-based supramolecular polymeric nanotubes to function as artificial enzymes for ester hydrolysis. The optimized catalyst shows a . 70-fold increase in reaction rate compared to the un-catalysed reaction when using 4-nitrophenyl acetate as a model substrate. Furthermore, the amphiphilic nature of the supramolecular catalysts enables an enhanced catalytic activity towards hydrophobic substrates. By incorporating an internal hydrophobic region within the self-assembled polymeric nanotube, we achieve a 55.4-fold acceleration in hydrolysis rate towards a more hydrophobic substrate, 4-nitrophenyl butyrate. This study introduces supramolecular peptide nanotubes as an innovative class of supramolecular scaffolds for fabricating artificial enzymes with better structural and chemical stability, catalysing not only ester hydrolysis, but also a broader spectrum of catalytic reactions.
基于肽的人工酶因其在组成和结构上与天然酶显著相似而备受关注。在此,我们报道了含组氨酸的环状肽基超分子聚合物纳米管的构建,其可作为酯水解的人工酶。当使用乙酸对硝基苯酯作为模型底物时,优化后的催化剂与未催化反应相比,反应速率提高了70倍。此外,超分子催化剂的两亲性使其对疏水底物具有更高的催化活性。通过在自组装聚合物纳米管内引入内部疏水区域,我们实现了对更疏水底物丁酸对硝基苯酯水解速率55.4倍的加速。本研究引入了超分子肽纳米管作为一类创新的超分子支架,用于制造具有更好结构和化学稳定性的人工酶,不仅能催化酯水解,还能催化更广泛的催化反应。