Cell Discovery
·
2021
·Vol. 7
·期 1
·1-12
·
IF 10.849
Meng Wensi,Zhang Lijie,Cao Menghao,Zhang Yongjia,Zhang Yipeng,Li Ping,Kang Zhaoqi,Guo Shiting,Xu Ping,Ma Cuiqing,Gao Chao
Overflow metabolism-caused acetate accumulation is a major problem that restricts industrial applications of various bacteria. 2,3-Butanediol (2,3-BD) synthesis in microorganisms is an ancient metabolic process with unidentified functions. We demonstrate here that acetate increases and then decreases during the growth of a bacterium Enterobacter cloacae subsp. dissolvens SDM. Both bifunctional acetaldehyde/ethanol dehydrogenase AdhE-catalyzed ethanol production and acetate-induced 2,3-BD biosynthesis are indispensable for the elimination of acetate generated during overflow metabolism. 2,3-BD biosynthesis from glucose supplies NADH required for acetate elimination via AdhE-catalyzed ethanol production. The coupling strategy involving 2,3-BD biosynthesis and ethanol production is widely distributed in bacteria and is important for toxic acetate elimination. Finally, we realized the co-production of ethanol and acetoin from chitin, the second most abundant natural biopolymer whose catabolism involves inevitable acetate production through the coupling acetate elimination strategy. The synthesis of a non-toxic chemical such as 2,3-BD may be viewed as a unique overflow metabolism with desirable metabolic functions.
研究领域:
微生物学
·
代谢工程
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产品关联
DOI
PubMed
高影响因子
POLYMER DEGRADATION AND STABILITY
·
2023
·
IF 5.9
Jiaxin Yu,Xiaojie Zhao,Yuhan Liu,Mingxiao Deng,Bao Zhang,Hongwei Pan,Huiliang Zhang,Baijun Liu,Yongfeng Men,Zhaoyan Sun,Wei Hu
Biodegradable plastic can decompose in the natural environment and thus effectively reduce the environmental pollution. Poly(butylene adipate-co-terephthalate) (PBAT) is a kind of polyester with good mechanical performance, degradability, and biocompatibility. In this study, a novel kind of poly(1,3-butylene adipate-co-1,4-butylene terephthalate) (PB′ABT) was synthesized with 1,3-butanediol, adipic acid, 1,4-butanediol and terephthalic acid as monomers through direct esterification and melt polycondensation to develop a kind of biodegradable polyester with more practical application value. A molecular weight of more than 50000 and intrinsic viscosity of 0.91-1.01 dL/g was achieved. The molecular structure of the polyester can be effectively adjusted with the monomer ratio, thereby affecting the properties, considering the thermal behavior, crystallinity, and mechanical performance increased with the 1,4-butadiene terephthalate (BT) unit content. Glass transition temperature (T g ), crystallization temperature (T c ), melting temperature (T m ) and crystallinity increased from -24.5 °C to 0 °C, 66.2 °C to 149.2 °C, 112.8 °C to 179.4 °C, and 20% to 33%, respectively. The highest tensile strength and elongation at break were 45 MPa and 1458%, respectively. PB′ABT-55 (molar ratio of BT: 55%) had higher thermal stability as compared with the biodegradable PBAT, and also superior tensile properties than the commercial PBAT. The results illustrated that the prepared PB′ABT is promising for wide application with good thermal stability, excellent tensile properties and biodegradability.
研究领域:
材料科学
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环境科学
·
化学工程
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产品关联
DOI
高影响因子
PROCESS BIOCHEMISTRY
·
2024
·
IF 3.7
Yanting Xu,Jing Zhuang,Shuo Wang,Jianying Dai,Zhi-Long Xiu
The aim of this work was to develop an integrated process of 2,3-butanediol production and extraction of active components from Chinese herbs via fermentation, and evaluate their potential as cosmetic ingredients in vitro. A GRAS strain DL2–2 of Bacillus licheniformis was isolated and the fermentation medium was optimized using the ingredients that could be used in cosmetics. Four types of Chinese herbs were added solely or in combination into the fermentation medium to perform 2,3-butanediol production and active components extraction simultaneously. The release of polysaccharides and flavonoids was promoted, and the antioxidant, whitening and antibacterial abilities were improved. The highest antioxidant and antibacterial activity was obtained from the ferment filtrate of Dendrobium devonianum and Gastrodia elata f. glauca , resulting from the highest contents of flavonoids (0.44 g/L) and polyphenols (0.31 g/L), and 42.2 g/L 2,3-butanediol was also produced. The highest polysaccharide concentration was obtained from the ferment filtrate containing Polygonatum kingianum , which exhibited the highest inhibitory effect on tyrosinase (65 %), similar to that of 1 g/L arbutin. Therefore, the filtrate of 2,3-butanediol-Chinese herbal fermentation broth is promising as an ingredient in the production of natural high-value cosmetics.
研究领域:
生物技术
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化妆品科学
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微生物学
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产品关联
DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2024
·
IF 3.7
Lifang Ge,Meizhen Gao,Xiaosheng Zhang,Jiang Wang,Qi Shi,Jinxiang Dong
The adsorption and separation of diols from dilute aqueous solution using hydrophobic materials is very challenging due to the strong diol–water hydrogen-bonding interactions. Herein, we screened hydrophobic zeolitic imidazolate frameworks (ZIFs) with chabazite (CHA) topology for separation of 2,3-butanediol (2,3-BDO) and 1,3-propanediol (1,3-PDO), which had junctional and hydrophobic traps matching the two end methyl groups of the 2,3-BDO molecule. Based on CHA-ZIFs with the same small-sized ligand 2-methylimidazole (mIm) and different large-sized ligand benzimidazole derivatives (RbIm), CHA-ZIFs with larger surface areas were obtained by the addition of excess small-sized ligand mIm in the synthesis process. We showed that all of the hydrophobic CHA-ZIFs preferentially adsorbed 2,3-BDO over 1,3-PDO by static batch adsorption and dynamic column adsorption experiments. But ZIF-301 and ZIF-300 with halogen groups exhibited better adsorptive separation performance for 2,3-BDO/1,3-PDO than ZIF-302 with methyl groups. For a typical ZIF-301, its adsorption capacity for 2,3-BDO was 116.4 mg·g –1 and selectivity for 2,3-BDO/1,3-PDO was 3.8 in dynamic column adsorption of the binary-component system (2,3-BDO/1,3-PDO: 50/50 g·L –1 ). Computational simulations revealed that 2,3-BDO preferentially adsorbed in a trap at the junction between the cha and d6r cages of CHA-ZIFs, meaning the strong host–guest interactions. Therefore, the hydrophobic CHA-ZIFs with a junctional trap were promising candidate materials for adsorbing 2,3-BDO, which also provided a new perspective for separating diols in dilute aqueous solutions.
研究领域:
材料科学
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化学工程
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产品关联
DOI
高影响因子
MOLECULES
·
2024
·
IF 4.2
Jiming Zhang,Hui Lin,Chaosong Zheng,Bin Yang,Miao Liang,Yi Lin,Liaoyuan Zhang
2,3-butanediol (2,3-BD) is a versatile bio-based platform chemical. An artificial four-enzyme synthetic biosystem composed of ethanol dehydrogenase, NADH oxidase, formolase and 2,3-butanediol dehydrogenase was designed for upgrading ethanol to 2,3-BD in our previous study. However, a key challenge in developing in vitro enzymatic systems for 2,3-BD synthesis is the relatively sluggish catalytic efficiency of formolase, which catalyzes the rate-limiting step in such systems. Herein, this study reports how engineering the tunnel and substrate binding pocket of FLS improved its catalytic performance. A series of single-point and combinatorial variants were successfully obtained which displayed both higher catalytic efficiency and better substrate tolerance than wild-type FLS. Subsequently, a cell-free biosystem based on the FLS:I28V/L482E enzyme was implemented for upgrading ethanol to 2,3-BD. Ultimately, this system achieved efficient production of 2,3-BD from ethanol by the fed-batch method, reaching a concentration of 1.39 M (124.83 g/L) of the product and providing both excellent productivity and yield values of 5.94 g/L/h and 92.7%, respectively. Taken together, this modified enzymatic catalysis system provides a highly promising alternative approach for sustainable and cost-competitive production of 2,3-BD.
研究领域:
生物化学
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合成生物学
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酶学
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产品关联
DOI
PubMed
高影响因子
MOLECULAR BIOTECHNOLOGY
·
2021
·Vol. 63
·期 6
·491-501
·
IF 2.695
Tang Wanggang,Lian Chaoqun,Si Yu,Chang Jianrong
2,3-Butanediol dehydrogenase (BDH), also known as acetoin/diacetyl reductase, is a pivotal enzyme for the formation of 2,3-butanediol (2,3-BD), a chiral compound with potential roles in the virulence of certain pathogens. Here, a NAD(H)-dependent (2 R ,3 R )-BDH from Neisseria gonorrhoeae FA1090 (NgBDH), the causative agent of gonorrhoea, was functionally characterized. Sequence analysis indicated that it belongs to zinc-containing medium-chain dehydrogenase/reductase family. The recombinant NgBDH migrated as a single band with a size of around 45 kDa on SDS-PAGE and could be confirmed by Western blotting and mass spectrometry. For the oxidation of either (2 R ,3 R )-2,3-BD or meso -2,3-BD, the enzyme exhibited a broad pH optimum between pH 9.5 to 11.5. For the reduction of (3 R /3 S )-acetoin, the pH optimum was around 6.5. The enzyme could catalyze the stereospecific oxidation of (2 R ,3 R )-2,3-BD ( K m = 0.16 mM, k cat / K m = 673 s −1 · mM −1 ) and meso -BD ( K m = 0.72 mM, k cat / K m = 165 s −1 · mM −1 ). Moreover, it could also reduce (3 R /3 S )-acetoin with a K m of 0.14 mM and a k cat / K m of 885 s −1 · mM −1 . The results presented here contribute to understand the 2,3-BD metabolism in N. gonorrhoeae and pave the way for studying the influence of 2,3-BD metabolism on the virulence of this pathogen in the future.
研究领域:
微生物学
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生物化学
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DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Zixin Zhong,Haolan Liu,Ruru Zhou,Boyong Ye,Jie Fu,Zhaoyin Hou
3-Hydroxybutyric acid (3-HBA) is an important monomer for manufacturing biodegradable polymers such as polyhydroxyalkanoates, which are currently produced via an expensive and time-consuming microbial fermentation route. Herein, the catalytic synthesis of 3-HBA via the selective oxidation of 1,3-butanediol (1,3-BDO) in the presence of molecular oxygen is reported for the first time. It was found that the PtSb2 alloy could catalyze the selective formation of 3-HBA, and the selectivity of 3-HBA was 82.3% at a 1,3-BDO conversion level of 95.5%. The calculated turnover frequency of each surface Pt atom in the PtSb2/AC catalyst was 344.3 h–1 at 70 °C. The characterization results indicated that the prominent performance of the PtSb2 alloy over monometallic Pt nanoparticles could be because the alloy could promote the tandem oxidation of the 3-hydroxybutyraldehyde (3-HBAD) intermediate to 3-HBA and reduce the dehydration of 3-HBAD to the byproduct. At the same time, the PtSb2 alloy was also effective for the selective oxidation of several diols to hydroxyl-substituted acids.
研究领域:
化学工程
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催化科学
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材料科学
✓ 已验证
DOI
高影响因子
GREEN CHEMISTRY
·
2016
·Vol. 18
·期 22
·6029-6034
·
IF 8.506
Na Li,Wenjun Yan,Pengju Yang,Hongxia Zhang,Zhijian Wang,Jianfeng Zheng,Suping Jia,Zhenping Zhu
Theoretically, selective C–H manipulation in ethanol can result in a direct C–C coupling synthesis of 2,3-butanediol (2,3-BDO). However, this process is typically extremely difficult to achieve because of the high complexity of the involved chemical bonds. In this work, we determine that hydroxide radicals generated from the photolysis of H2O2 can selectively attack the α-hydrogen atom in ethanol aqueous solutions and crack the C–H bond to produce hydroxyethyl radicals, which subsequently undergo C–C coupling to form 2,3-BDO. This selective C–H breakage is determined by the reaction rate, which is primarily controlled by the local H2O2 concentration at a given irradiation intensity. At a moderate reaction rate of ethanol (37 mmol h−1), the 2,3-BDO selectivity reaching as high as 91% can be obtained. The introduction of a catalyst can further increase ethanol conversion and enhance the 2,3-BDO formation rate by controlling the reaction rate. This result provides an environment-friendly approach to convert bio-ethanol directly to 2,3-BDO and to manipulate a single bond selectively in complex bonding situations.
研究领域:
化学工程
·
环境科学
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产品关联
DOI
高影响因子
PROCESS BIOCHEMISTRY
·
2020
·
IF 2.952
Jian-Ying Dai,Wen-Tian Guan,Zhi-Long Xiu
Inulin could be converted to bio-based chemicals by an inulinase producer without external inulinase, and the production of 2,3-butanediol was less than 50 g/L. In this work, a novel inulinase producer of Klebsiella pneumoniae H3 was isolated, and inulinase catalytic properties as well as 2,3-butanediol fermentation were investigated. The enzyme was an intracellular inulinase with an optimal pH of 6 ∼ 7 and a temperature of 30 °C. The use of inulin by H3 was dependent on the degree of polymerization (DP), and the average DP of inulin in fermentation broth increased from 2.82 to 8.08 in 24-h culture of batch fermentation. Acidic pretreatment was developed to increase inulin utilization by adjusting medium pH to 3.0 prior to sterilization. In batch fermentation with optimized medium and fermentation conditions, the concentration of target product (2,3-butanediol and acetoin) was 80.4 g/L with a productivity of 2.23 g/(L⋅h), and a yield of 0.426 g/g inulin.
研究领域:
微生物学
·
生物技术
·
酶学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Wang Yue,Yang Genji,Wu Bowen,Mi Yaozu,Zhou Yang,Ma Tian,Zang Hailian,Xi Chuanwu,Cheng Yi,Li Chunyan
The simultaneous bioremediation and bioconversion of papermaking wastewater by psychrotrophic microorganisms holds great promise for developing sustainable environments and economies in cold regions. Here, the psychrotrophic bacterium Raoultella terrigena HC6 presented high endoglucanase (26.3 U/mL), xylosidase (732 U/mL), and laccase (8.07 U/mL) activities for lignocellulose deconstruction at 15 °C. mRNA monitoring and phenotypic variation analyses confirmed that cold-inducible cold shock protein A (CspA) facilitated the expression of the cel208 , xynB68 , and lac432 genes to increase the enzyme activities in strain HC6. Furthermore, the cspA gene-overexpressing mutant (strain HC6- cspA ) was deployed in actual papermaking wastewater and achieved 44.3%, 34.1%, 18.4%, 80.2% and 100% removal rates for cellulose, hemicellulose, lignin, COD, and NO 3 - -N at 15 °C. Simultaneously, 2,3-butanediol (2,3-BD) was produced from the effluent with a titer of 2.98 g/L and productivity of 0.154 g/L/h. This study reveals an association between the cold regulon and lignocellulolytic enzymes and provides a promising candidate for simultaneous papermaking wastewater treatment and 2,3-BD production.
研究领域:
环境微生物学
·
生物工程
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2017
·Vol. 92
·期 9
·2477-2487
·
IF 3.135
Niyomukiza Samuel,Teng Bao,Xian Zhang,Taowei Yang,Meijuan Xu,Xin Li,Irene Komera,Tuyishime Philibert,Zhiming Rao
BACKGROUND 2,3-Butanediol (2,3-BD) has a wide range of applications in chiral molecular synthesis, biofuel additives, and in food flavor additive manufacturing. Fermentation is a favorable method for 2,3-BD production. However, it requires much time and produces several NADH related byproducts which compete with 2,3-BD production. Bacillus subtilis has an excellent ability for 2,3-BD production by biocatalysis. However, its production is limited by low intracellular NADH and the reversible property of acetoin reductase (AR/2,3-BDH). The whole cell biocatalyst process with two different NADH regeneration systems was designed for efficient production of 2,3-BD in B. subtilis 168. RESULTS Formate dehydrogenase and glucose dehydrogenase for NADH regeneration were successfully co-expressed with acetoin reductase in B. subtilis 168. After optimization of biocatalyst bioconversion conditions, B. subtilis 168/pMA5- bdhA-Hpa II- fdh yielded 74.5 g L −1 of 2, 3-BD with 9.3 g L −1 h −1 productivity by fed batch and 115.4 g of 2,3-BD was achieved using same batch bacterium by three repeated batch bioconversions. On the other hand, 63.7 g L −1 of 2, 3-BD was produced with 7.92 g L −1 h −1 productivity by B. subtilis 168/pMA5- bdhA-Hpa II- gdh . To our knowledge, the volume productivity obtained here is the highest ever reported for biocatalysis. CONCLUSION A higher productivity of 2,3-BD from acetoin was achieved by whole cell biocatalysis with NADH regeneration systems in B. subtilis 168. This approach can be applied for NADH related bio-based chemicals production to improve titer, yield and productivity. © 2017 Society of Chemical Industry
研究领域:
生物化学
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微生物学
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代谢工程
✓ 已验证
DOI
高影响因子
ACS Catalysis
·
2016
·
IF 9.307
Zhixin Zhang,Yehong Wang,Jianmin Lu,Chaofeng Zhang,Min Wang,Mingrun Li,Xuebin Liu,Feng Wang
Conversion of low-carbon olefins to higher alcohols or olefins via the formation of C–C bonds is an increasingly important topic. We herein report an example of converting isobutene and formaldehyde (38 wt % aqueous solution) to 3-methyl-1,3-butanediol (MBD), a precursor for isoprene. The reaction occurs through a Prins condensation–hydrolysis reaction over a praseodymium (Pr)-doped CeO2 catalyst. The best MBD yield (70%) is achieved over the Pr-doped CeO2 catalyst. Catalyst characterizations with high-angle annular dark field transmission electron microscopy (HAADF-TEM), pyridine adsorption infrared (IR) and Raman spectroscopy, and density functional theory (DFT) calculations show that the doped Pr is uniformly and highly dispersed in the CeO2 crystalline phase. In addition, the Pr doping creates more oxygen vacancy sites on CeO2 and thus enhances the Lewis acidity of the catalyst, which is responsible for the catalytic performance of the Pr-CeO2 catalyst.
研究领域:
催化化学
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材料科学
·
有机合成
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）