Department of Chemical Sciences and Centre for Advanced Functional Materials, Indian Institute of Science Education and Research (IISER) Kolkata, Mohanpur, 741246, India.
Nat Commun. 2024 May 28;15(1):4515. doi: 10.1038/s41467-024-48930-w.
In extant biology, large and complex enzymes employ low molecular weight cofactors such as dihydronicotinamides as efficient hydride transfer agents and electron carriers for the regulation of critical metabolic processes. In absence of complex contemporary enzymes, these molecular cofactors are generally inefficient to facilitate any reactions on their own. Herein, we report short peptide-based amyloid nanotubes featuring exposed arrays of cationic and hydrophobic residues that can bind small molecular weak hydride transfer agents (NaBH) to facilitate efficient reduction of ester substrates in water. In addition, the paracrystalline amyloid phases loaded with borohydrides demonstrate recyclability, substrate selectivity and controlled reduction and surpass the capabilities of standard reducing agent such as LiAlH. The amyloid microphases and their collaboration with small molecular cofactors foreshadow the important roles that short peptide-based assemblies might have played in the emergence of protometabolism and biopolymer evolution in prebiotic earth.
在现存的生物学中，大型复杂的酶利用低分子量的辅酶，如二氢烟酰胺，作为有效的氢化物转移剂和电子载体，以调节关键的代谢过程。在没有复杂的当代酶的情况下，这些分子辅酶本身通常效率不高，无法促进任何反应。在此，我们报告了基于短肽的淀粉样纳米管，其特征是暴露的阳离子和疏水性残基阵列，可以结合小分子弱氢化物转移剂（NaBH），以促进酯底物在水中的有效还原。此外，负载硼氢化物的准晶淀粉样相具有可回收性、底物选择性和可控还原能力，超过了标准还原剂如 LiAlH 的能力。淀粉样微相及其与小分子辅酶的协同作用预示着基于短肽的组装可能在原始地球中前代谢和生物聚合物进化的出现中发挥了重要作用。
