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Recent advance of chemoenzymatic catalysis for the synthesis of chemicals: Scope and challenge

Chinese Journal of Chemical Engineering 2021年第2期34卷 146-167页

作者： Mengjiao Xu Zhuotao Tan Chenjie Zhu Wei Zhuang Hanjie Ying Pingkai Ouyang College of Biotechnology and Pharmaceutical Engineering Nanjing Tech UniversityNanjing 211816China

Chemoenzymatic catalysis can give full play to the advantages of versatile reactivity of chemocatalysis and excellent chemo-,regio-,and stereoselectivities of *** chemoenzymatic methods can not only save resource,cost,and operating time but also reduce the number of reaction steps,and avoid separating unstable intermediates,leading to the generation of more products under greener circumstances and thereby playing an indispensable role in the fields of medicine,materials and fine *** incompatible challenges between chemocatalyst and biocatalyst remain,strategies such as biphasic system,artificial metalloenzymes,immobilization or supramolecular host,and protein engineering have been designed to overcome these *** this review,chemoenzymatic catalysis according to different chemocatalysis types was classifiably described,and in particular,the classic dynamic kinetic resolutions(DKR)and cofactor regeneration were ***,the bottlenecks and development of chemoenzymatic catalysis were summarized,and future development was prospected.

关键词： Chemoenzymatic Dynamic kinetic resolution cofactor regeneration Biocatalysis Chemocatalysis

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Electrocatalytic NAD(P)H regeneration for biosynthesis

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Green Chemical Engineering 2024年第1期5卷 1-15页

作者： Yaoxuan Li Guanhua Liu Weixi Kong Suoqing Zhang Yuemei Bao Hao Zhao Lihui Wang Liya Zhou Yanjun Jiang National-Local Joint Engineering Laboratory for Energy Conservation in Chemical Process Integration and Resources Utilization School of Chemical Engineering and TechnologyHebei University of TechnologyTianjin300401China North China Pharmaceutical Group Corp Shijiazhuang050015China Tianjin Food Research Institute Tianjin301609China

The highly efficient chemoselectivity,stereoselectivity,and regioselectivity render enzyme catalysis an ideal pathway for the synthesis of various chemicals in broad *** the cofactor of an enzyme is necessary but expensive,the conversed state of the cofactor is not beneficial for the positive direction of the *** regeneration using electrochemical methods has the advantages of simple operation,low cost,easy process monitoring,and easy product separation,and the electrical energy is green and ***,bioelectrocatalysis has great potential in synthesis by combining electrochemical cofactor regeneration with enzymatic *** this review,we detail the mechanism of cofactor regeneration and categorize the common electron mediators and enzymes used in cofactor *** reaction type and the recent progress are summarized in electrochemically coupled enzymatic *** main challenges of such electroenzymatic catalysis are pointed out and future developments in this field are foreseen.

关键词： Biosynthesis cofactor regeneration Bioelectrocatalysis NAD(P)H Electron mediator

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Iron-doping Accelerating NADH Oxidation over Carbon Nitride

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Chemical Research in Chinese Universities 2020年第6期36卷 1076-1082页

作者： ZHANG Yuanyuan HUANG Xiaohua LI Jiashu LIN Gang LIU Wengang CHEN Zupeng LIU Jian College of Materials Science and Engineering Qingdao University of Science and TechnologyQingdao 266042P.R.China College of Chemical Engineering Nanjing Forestry UniversityNanjing 210037P.R.China

As a state-of-the-art conjugated polymer photocatalyst,graphitic carbon nitride(abbreviated as g-C3Na)has shown sreat potential in photocatalvtic cofactor(reduced form of nicotinamide adenine ***)***,Fe-doped g-CaNa was engineered for photocatalvtic NADH *** n-r interaction between the NADH molecule and the conjugated heptazine buildine block facilitates the adsorption of NADH onto the framework as revealed by density functional theory(DFT)calculations,Furthermore,iron doping promoted the oxidation kinetics of NADH under blue LED *** conversion ratio of NADH to its oxidized form could be up to 85.7%in 20 min,comparing with 59.4%for metal-free *** assay employing formate dehydrogenase(FDH)further verified the selectivity of the products,with 67.5%+2.6%of enzymatically active 1,4-NADH being regenerated following the oxidation *** experiments suggest the dominant role of photo-induced electrons in theoxidation of *** work could shed light on developing a novel cofactor regeneration route through the syner-gistic effect between the metal doping and noncovalent interaction based on the coniugated polymer.

关键词： cofactor regeneration NADH oxidation Photocatalysis Carbon nitride π-πinteraction

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Synergetic engineering of Escherichia coli for efficient production of L-tyrosine

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Synthetic and Systems Biotechnology 2023年第4期8卷 724-731页

作者： Jurong Ping Lian Wang Zhijie Qin Zhemin Zhou Jingwen Zhou Engineering Research Center of Ministry of Education on Food Synthetic Biotechnology Jiangnan University1800 Lihu RoadWuxiJiangsu214122China Science Center for Future Foods Jiangnan University1800 Lihu RoadWuxiJiangsu214122China Key Laboratory of Industrial Biotechnology Ministry of Education and School of BiotechnologyJiangnan University1800 Lihu RoadWuxiJiangsu214122China Jiangsu Province Engineering Research Center of Food Synthetic Biotechnology Jiangnan UniversityWuxi214122China

L-Tyrosine,an aromatic non-essential amino acid,is the raw material for many important chemical products,including levodopa,resveratrol,and *** is widely used in the food,drug,and chemical *** are many studies on the synthesis of L-tyrosine by microorganisms,however,the low titer of L-tyrosine limited the industrial large-scale *** order to enhance L-tyrosine production in Escherichia coli,the expression of key enzymes in the shikimate pathway was up-or *** L-tyrosine transport system and the acetic acid biosynthesis pathway were modified to further enhance L-tyrosine *** addition,the phosphoketolase pathway was introduced in combination with cofactor engineering to redirect carbon flux to the shikimate ***,after adaptive laboratory evolution to low pH an optimal strain was *** strain can produce 92.5 g/L of L-tyrosine in a 5-L fermenter in 62 h,with a yield of 0.266 g/g glucose.

关键词： L-tyrosine cofactor regeneration Phosphoketolase pathway Escherichia coli

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Asymmetric reduction of conjugated C=C bonds by immobilized fusion of old yellow enzyme and glucose dehydrogenase

Green Synthesis and Catalysis

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Green Synthesis and Catalysis 2024年第2期5卷 80-87页

作者： Yongxing Li Pengqian Luan Lele Dong Jianqiao Liu Luying Jiang Jing Bai Fufeng Liu Yanjun Jiang School of Chemical Engineering and Technology Hebei University of TechnologyTianjin 300130China College of Food Science and Biology Hebei University of Science&Technology26 Yuxiang StreetYuhua DistrictShijiazhuang 050018China Key Laboratory of Industrial Fermentation Microbiology of Ministry of Education Tianjin Key Laboratory of Industrial MicrobiologyCollege of BiotechnologyTianjin University of Science&TechnologyTianjin 300457China

Asymmetric reduction of the conjugated C=C bonds by the old yellow enzymes(OYEs)presents a promising field in the synthesis of chiral ***,few natural OYEs have been applied in large-scale applications due to the requirement of costly NADPH and low operational ***,a stable and efficient fusion of YqjM from Bacillus subtilis and glucose dehydrogenase(GDH)from Bacillus megaterium was constructed to stereoselectively reduce the conjugated C=C bonds in a self-sufficient continuous *** effects of the enzyme order and different linkers on the fusions were investigated by structural analysis and all-atom molecular dynamics *** best fusion YqjM_G_GDH gave 98% conversion of 100 mmol/L 2-methylcyclopentenone with an excellent ee value(>99%)in 3 h,while the mixture of individual enzymes only obtained 68% conversion after more than 8 *** improved substrate conversion of YqjM_G_GDH fusion was probably attributed to the increased flexibility of each fused enzyme and the shortening of the diffusion distance of NADPH regenerated.A one-pot process was designed to purify and immobilize the fusion on the Ni2t-nitrilotriacetic acid functionalized magnetic mesoporous silica *** resulting immobilized biocatalyst not only catalyzed the asymmetric reduction of various α,β-unsaturated ketones(20 mmol/L)continuously with only 50μmol/L NADPt to initiate the whole process,but also retained more than 82%of the initial activity after seven cycles,serving as a good candidate for the industrial applications.

关键词： Enzyme fusion Old yellowenzymes Asymmetricreduction C=C bond cofactor regeneration Immobilization

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Characterization of a flavoprotein:soluble pyridine nucleotide transhydrogenase from Salmonella typhimurium 14028

Characterization of a flavoprotein:soluble pyridine nucleoti...

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第八届全国医学生物化学与分子生物学第五届全国临床应用生物化学与分子生物学2013华东六省一市生物化学与分子生物学联合学术研讨会

作者： Zhengyu Cao Peng Wang Xiaoyu Zhao Guoping Zhu Institute of Molecular Biology and Biotechnology Anhui Normal University

Soluble pyridine nucleotide transhydrogenase(STH or UdhA) was widely utilized in the industrial application through genetic and metabolic *** the gene encoding Salmonella typhimurium 14028 STH(StSTH) was cloned and expressed in Escherichia coli Rosetta(DE3).The molecular mass of the purified StSTH enzyme was estimated to be 540 kDa by gel filtration chromatography,suggesting that the enzyme is a *** recombinant StSTH exhibited maximum activity at pH 7.2 and 32 ℃.The half-life of StSTH was 5 hours at50 ℃ and 30 min at 60 ℃.The enzyme had high storage stability and retained over 80% of its initial activity after stored for 40 days at 4 ℃.The apparent kinetic parameters,K and V for thio-NAD,were 168.9 μM and 43.0 μM·min,and K,V and K for NADPH were 69.5 μM,36.3 μM·min and 607.3 μ*** activity of StSTH was strongly inhibited by metal ions(such as K,Li,Ca,Mn,Co,Zn,Ni and Cu),and stimulated by 2 mM ATP,ADP and AMP,*** characteristics of StSTH make it an attractive alternative to many industrial applications such as cofactor regeneration.

关键词： soluble pyridine nucleotide transhydrogenase Salmonella typhimurium biochemical characterization cofactor regeneration

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Characterization of a flavoprotein:soluble pyridine nucleotide transhydrogenase from Salmonella typhimurium 14028

Characterization of a flavoprotein:soluble pyridine nucleoti...

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第四届全国微生物资源学术暨国家微生物资源平台运行服务研讨会

作者： Zhengyu Cao,Yunyun Pei,Guoping Zhu(Institute of Molecular Biology and Biotechnology,Anhui Normal University,Wuhu 241000) 安徽师范大学分子生物学及生物技术研究所

As cofactors are often much more expensive than the end products of industry,the demand of cofactor regenerating systems is increasing to lower input ***,soluble pyridine nucleotide transhydrogenase(STH or UdhA) was widely utilized in the industrial application for cofactor regeneration by regulating the intracellular redox state through metabolic ***,the biochemical information is not sufficient and limits the utilizations of STHs in cofactor regenerating *** this study,the gene encoding STH of Salmonella typhimurium 14028(StSTH) was cloned and expressed in Escherichia coli Rosetta(DE3).The molecular mass of purified StSTH enzyme was estimated to be 540 kDa by gel filtration chromatography,suggesting that the enzyme has a unique decameric structure of all known *** recombinant StSTH exhibited maximum activity at pH 7.2 and 32 °*** half-life of StSTH was about 5 hours at 50 °C and 30 min at 60 °*** enzyme had high storage stability and retained over 80% of its initial activity after stored for 40 days at 4 °*** apparent kinetic parameters,Km and Vmax for thio-NAD+,were 168.9 μM and 43.0 μM?min-1,and Km,Vmax and Ki for NADPH were 69.5 μM,36.3 μM?min-1 and 607.3 μM,*** activity of StSTH was strongly inhibited by metal ions such as K+,Li+,Ca2+,Mn2+,Co2+,Zn2+,Ni2+ and Cu2+,and stimulated by 2 mM ATP,ADP and AMP,*** together,the detailed information would be very helpful to improve the efficiency of coenzyme-regeneration,reduce the costs of coenzymes and increase the product yields by metabolic engineering or synthetic biology.

关键词： soluble pyridine nucleotide transhydrogenase Salmonella typhimurium biochemical characterization cofactor regeneration

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