Article, 2024

Effect of Deep Eutectic Mixtures in Hydroxylation of Fatty Acids: A Correlation between Water Activity and Thermostability of FA-HY1

ACS Sustainable Chemistry & Engineering, ISSN 2168-0485, Volume 12, 5, Pages 1918-1929, 10.1021/acssuschemeng.3c05867

Contributors

Zhou, Peng-Fei 0000-0002-1846-6074 [1] [2] Zhang, Yan 0000-0002-9173-7029 [1] Liu, Weiqi [2] Jones, Nykola C 0000-0002-4081-6405 [1] Hoffmann, Søren Vrønning 0000-0002-8018-5433 [1] Eser, Bekir Engin 0000-0002-8836-1251 [1] Zhang, Mingliang [1] [3] Ouyang, Yi [1] Wang, Fang 0000-0003-0775-801X [1] [4] Deng, Yuan-Yuan [2] Zhang, Ming-Wei (Corresponding author) [2] [5] Guo, Zheng (Corresponding author) [1]

Affiliations

  1. [1] Aarhus University
    2. [NORA names: AU Aarhus University; University; Denmark; Europe, EU; Nordic; OECD];
  2. [2] Guangdong Academy of Agricultural Sciences
    3. [NORA names: China; Asia, East];
  3. [3] Fujian Normal University
    4. [NORA names: China; Asia, East];
  4. [4] Jilin University
    5. [NORA names: China; Asia, East];
  5. [5] Food Laboratory of Zhongyuan, Luohe, 462300, Henan, P. R. China
    6. [NORA names: China; Asia, East]

Abstract

To validate the performance and application of fatty acid hydratases in green and sustainable deep eutectic solvents (DESs), a robust system with the combination of fatty acid hydratase-1 (FA-HY1) from Lactobacillus acidophilus and DESs for the biocatalytic hydroxylation of fatty acids was developed. As the cosubstrate of hydroxylation reactions, water molecules have been proven to be a key factor for the thermostability of FA-HY1 in DES systems. We found that FA-HY1 displayed improved thermostability at lower water activity. In particular, the half-life time of FA-HY1 increased 6-fold in a choline chloride/sorbitol system with water activity (a w = 0.84) compared to an aqueous buffer system. Moreover, the thresholds of a w for regulating the synthesis of hydroxy fatty acids (HFAs) in FA-HY1/DES systems were determined. We further investigated the recyclability of FA-HY1 in a choline chloride/sorbitol system, where significantly, after three rounds of recycling, a high hydroxylation efficiency of 83.2% was still observed. Monitoring the secondary structure of FA-HY1 using synchrotron radiation circular dichroism analysis revealed that the DESs appear to delay the change in confirmation of FA-HY1. In addition, molecular dynamics simulations were performed in DES and aqueous systems, which revealed the mechanistic features of the thermostability of FA-HY1 in DESs.

Keywords

FA-HY1, Lactobacillus acidophilus, acid, activity, analysis, applications, aqueous buffer systems, aqueous systems, biocatalytic hydroxylation, buffer system, choline, circular dichroism analysis, combination, correlation, cosubstrate, deep eutectic mixture, deep eutectic solvent system, deep eutectic solvents, dichroism analysis, dynamics simulations, effect, efficiency, eutectic mixture, eutectic solvents, factors, fatty acid hydratases, fatty acids, features, half-life time, hydratase, hydroxy fatty acids, hydroxyl, hydroxylation efficiency, hydroxylation of fatty acids, hydroxylation reaction, low water activity, mechanistic features, mixtures, molecular dynamics simulations, molecules, performance, reaction, recycling, round, rounds of recycling, secondary structure, simulation, solvent, synchrotron, synthesis, synthesis of hydroxy fatty acids, system, thermostability, threshold, water, water activity, water molecules

Funders

  • China Scholarship Council
  • Department of Finance
  • Novo Nordisk Foundation

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