Zan Qijia, Long Mengfei, Zheng Nan, Zhang Zehua, Zhou Huimin, Xu Xinjie, Osire Tolbert, Xia Xiaole
Key Laboratory of Industrial Biotechnology, Ministry of Education, School of Biotechnology, Jiangnan University, Wuxi, 214122, Jiangsu, China.
Faculty of Biology, Shenzhen MSU-BIT University, Shenzhen, 518172, Guangdong, China.
AMB Express. 2023 Mar 15;13(1):32. doi: 10.1186/s13568-023-01538-7.
Ethyl carbamate (EC) is mainly found in fermented foods and fermented alcoholic beverages, which could cause carcinogenic potential to humans. Reducing EC is one of the key research priorities to address security of fermented foods. Enzymatic degradation of EC with EC hydrolase in food is the most reliable and efficient method. However, poor tolerance to ethanol severely hinders application of EC hydrolase. In this study, the mutants of EC hydrolase were screened by diphasic high pressure molecular dynamic simulations (dHP-MD). The best variant with remarkable improvement in specific activity and was H68A/K70R/S325N, whose specific activity was approximately 3.42-fold higher than WT, and relative enzyme activity under 20% (v/v) was 5.02-fold higher than WT. Moreover, the triple mutant increased its stability by acquiring more hydration shell and forming extra hydrogen bonds. Furthermore, the ability of degrading EC of the immobilized triple mutant was both detected in mock wine and under certain reaction conditions. The stability of immobilized triple mutant and WT were both improved, and immobilized triple mutant degraded nearly twice as much EC as that of immobilized WT. Overall, dHP-MD was proved to effectively improve enzyme activity and ethanol tolerance for extent application at industrial scale.
氨基甲酸乙酯(EC)主要存在于发酵食品和发酵酒精饮料中,可能对人类具有致癌潜力。降低EC含量是解决发酵食品安全问题的关键研究重点之一。利用食品中的EC水解酶对EC进行酶促降解是最可靠、最有效的方法。然而,对乙醇的耐受性较差严重阻碍了EC水解酶的应用。在本研究中,通过双相高压分子动力学模拟(dHP-MD)筛选了EC水解酶的突变体。比活性有显著提高的最佳变体是H68A/K70R/S325N,其比活性比野生型高约3.42倍,在20%(v/v)乙醇浓度下的相对酶活性比野生型高5.02倍。此外,三重突变体通过获得更多的水合壳层并形成额外的氢键提高了其稳定性。此外,在模拟葡萄酒和特定反应条件下均检测了固定化三重突变体降解EC的能力。固定化三重突变体和野生型的稳定性均得到提高,固定化三重突变体降解的EC几乎是固定化野生型的两倍。总体而言,dHP-MD被证明能有效提高酶活性和乙醇耐受性,以实现工业规模的广泛应用。