Chemoenzymatic two-step synthesis of tartaric acid employing glucose oxidase in combination with bimetallic AuPt/TiO2 catalyst

Tartaric acid (TA) is a crucial hydroxy-carboxylic acid chelating agent extensively employed in the pharmaceutical, food, dye, and energy industries. The utilization of glucose oxidation for TA synthesis represents an appealing yet challenging, environmentally-friendly approach. In this study, we developed a two-step chemoenzymatic strategy involving the efficient generation of gluconic acid (GA) through glucose oxidase (Gox) catalysis, followed by chemical decarboxylation to synthesize TA from GA. To optimize the production efficiency of GA and eliminate substrate inhibition in chemocatalysis, we successfully engineered a quadruple variant GoxM10 by implementing rigidifying structure strategies and refining the pH curve. This resulted in a substantial increase in the conversion rate of GA from 45% to 100%, along with improved thermo- and pH stability, as well as enhanced catalytic efficiency. Subsequently, durable bimetallic catalysts were designed for the conversion of Gox-bioconverted GA (bio-GA) to TA. Given the presence of impurities such as acetic acid and sodium acetate in bio-GA, which impacted the selectivity of TA, our focus was on investigating the influence of impurities in bio-GA on the performance of a bimetallic AuPt/TiO 2 catalyst and elucidating an inhibition mechanism that reveals a strong interaction between acetate and Au site, resulting in the formation of a complex compound while promoting uncontrollable C-C cleavage reactions. Through employing a chemoenzymatic two-step strategy, we successfully achieved an environmentally friendly and sustainable route from glucose to TA. This study provides valuable insights into catalyst design and optimization of reaction routes for renewable carboxylic acids and their derivatives synthesized through chemoenzymatic methods. This study utilizes glucose as a substrate and combines durable glucose oxidase with bimetallic catalysts to construct a chemoenzymatic cascade reaction for the green synthesis of tartaric acid.

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Journal
Green Synthesis and Catalysis
Published
2025-03-01
DOI
https://doi.org/10.1016/j.gresc.2025.03.005
Primary Topic
Enzyme-mediated dye degradation
Type
article
Field-Weighted Citation Impact
0.00

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article

Chemoenzymatic two-step synthesis of tartaric acid employing glucose oxidase in combination with bimetallic AuPt/TiO2 catalyst

Ruyue Dong, Bin Yao, Yiwen Shen, Huiying Luo et al.
Green Synthesis and Catalysis
Enzyme-mediated dye degradation
article

Chemoenzymatic two-step synthesis of tartaric acid employing glucose oxidase in combination with bimetallic AuPt/TiO2 catalyst

Ruyue Dong, Bin Yao, Yiwen Shen, Huiying Luo, Xing Qin, Tao Tu, Xin Jin, Lanxue Li, Yingguo Bai, Xiaoqing Liu, Xiaolu Wang, Mengyuan Liu, Yaru Yan
article en

Abstract

Tartaric acid (TA) is a crucial hydroxy-carboxylic acid chelating agent extensively employed in the pharmaceutical, food, dye, and energy industries. The utilization of glucose oxidation for TA synthesis represents an appealing yet challenging, environmentally-friendly approach. In this study, we developed a two-step chemoenzymatic strategy involving the efficient generation of gluconic acid (GA) through glucose oxidase (Gox) catalysis, followed by chemical decarboxylation to synthesize TA from GA. To optimize the production efficiency of GA and eliminate substrate inhibition in chemocatalysis, we successfully engineered a quadruple variant GoxM10 by implementing rigidifying structure strategies and refining the pH curve. This resulted in a substantial increase in the conversion rate of GA from 45% to 100%, along with improved thermo- and pH stability, as well as enhanced catalytic efficiency. Subsequently, durable bimetallic catalysts were designed for the conversion of Gox-bioconverted GA (bio-GA) to TA. Given the presence of impurities such as acetic acid and sodium acetate in bio-GA, which impacted the selectivity of TA, our focus was on investigating the influence of impurities in bio-GA on the performance of a bimetallic AuPt/TiO 2 catalyst and elucidating an inhibition mechanism that reveals a strong interaction between acetate and Au site, resulting in the formation of a complex compound while promoting uncontrollable C-C cleavage reactions. Through employing a chemoenzymatic two-step strategy, we successfully achieved an environmentally friendly and sustainable route from glucose to TA. This study provides valuable insights into catalyst design and optimization of reaction routes for renewable carboxylic acids and their derivatives synthesized through chemoenzymatic methods. This study utilizes glucose as a substrate and combines durable glucose oxidase with bimetallic catalysts to construct a chemoenzymatic cascade reaction for the green synthesis of tartaric acid.

Green Synthesis and Catalysis
Chinese Academy of Agricultural Sciences (CN), Institute of Animal Sciences (CN), China University of Petroleum, East China (CN), State Key Laboratory of Heavy Oil (CN)
National Natural Science Foundation of China, Agriculture Research System of China, Ministry of Agriculture and Rural Affairs of the People's Republic of China, National Key Research and Development Program of China
Openalex Percentile: Top 97%
Enzyme-mediated dye degradation
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