基质(水族馆)
化学
代谢工程
定向进化
蛋白质工程
生物催化
组合化学
酶
催化作用
生物化学
大肠杆菌
酶催化
产量(工程)
化学合成
酶动力学
商品化学品
纳米技术
活动站点
底物特异性
基因工程
谷氨酸脱羧酶
精细化工
动力学分辨率
药物发现
工业生物技术
立体化学
化学生物学
可持续生产
合成生物学
范围(计算机科学)
作者
Yaping Mao,Jialong Li,Zhiqiang Mu,Chenkai Cao,Kechun Zhang
标识
DOI:10.1021/acssuschemeng.5c07844
摘要
In recent years, the demand for β-alanine, 3-aminopropanol (3-AP), and 1-aminopropan-2-ol (MIPA) has increased because of their applications in pharmaceuticals, food additives, and polymers. The industrial production of these high-value amines relies on polluting chemical methods. To address this, we engineered Escherichia coli glutamate decarboxylase (GadB) via directed evolution to enable one-step enzymatic synthesis of all three compounds from renewable substrates (l-aspartate, l-homoserine, and l-threonine). A growth-coupled high-throughput screening platform identified the D86E mutant, which exhibits broad substrate promiscuity and enhanced kinetics: a 46-fold and 12.3-fold increase in kcat (26.36 s–1, 121.89 s–1) for β-alanine and 3-AP synthesis versus native decarboxylases, and activity toward first-time one-step MIPA production. Molecular dynamics simulations revealed that altered hydrogen-bonding interactions between the mutation site (E86) and substrates underpin the shifted specificity. In whole-cell biocatalysis, D86E achieved near-quantitative conversion (250 mM) to β-alanine (15.99 g/L) and 3-AP (13.51 g/L) within 12 h at neutral pH, with the MIPA yield reaching 8.48 g/L, demonstrating industrial feasibility. This work advances enzyme engineering for multisubstrate catalysis and provides a sustainable route for high-value chemical production.
科研通智能强力驱动
Strongly Powered by AbleSci AI