JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Zhengqiao Yin,Yiding Zhou,Xiucai Liu,Shengmiao Zhang,Bernard P. Binks
Hypothesis Biocatalysts are key to the realization of all bioconversions in nature. However, the difficulty of combining the biocatalyst and other chemicals in one system limits their application in artificial reaction systems. Although some effort, such as Pickering interfacial catalysis and enzyme-immobilized microchannel reactors, have addressed this challenge an effective method to combine chemical substrates and biocatalysts in a highly efficient and re-usable monolith system is still to be developed. Experiments A repeated batch-type biphasic interfacial biocatalysis microreactor was developed using enzyme-loaded polymersomes in the void surface of porous monoliths. Polymersomes, loaded with Candida antarctica Lipase B (CALB), are fabricated by self-assembly of the copolymer PEO- b -P(St- co -TMI) and used to stabilize oil-in-water (o/w) Pickering emulsions as a template to prepare monoliths. By adding monomer and Tween 85 to the continuous phase, controllable open-cell monoliths are prepared to inlay CALB-loaded polymersomes in the pore walls. Findings The microreactor is proven to be highly effective and recyclable when a substrate flows through it, which offers superior benefits of absolute separation to a pure product and no enzyme loss. The relative enzyme activity is constantly maintained above 93% in 15 cycles. The enzyme is constantly present in the microenvironment of the PBS buffer ensuring its immunity to inactivation and facilitating its recycling.
研究领域:
生物技术
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化学工程
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材料科学
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生物化学
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产品关联
DOI
PubMed
高影响因子
EUROPEAN POLYMER JOURNAL
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2025
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IF 6.3
Yongbo Luo,Xiaoqin Zhang,Shuo Han,Jin Zhu,Jinggang Wang
This study focuses on the synthesis and property evaluation of a novel transparent biodegradable copolycarbonate, poly(butylene-co-1,4-cyclohexanedimethylene carbonate) (PBCC), which was synthesized via melt polycondensation. The chemical structure composition and random characteristics of PBCC were confirmed by 1 H NMR and 13 C NMR. With the increase of 1,4-cyclohexanedimethylene carbonate (CC) unit content, the thermal properties were significantly improved, T g and T d,5% increased from –22.2 °C and 307 °C for PBC 16 C to 30.4 °C and 342 °C for PBC 85 C. The maximum values of the tensile strength and tensile modulus of PBCC were achieved at a CC unit content of 85 mol%, reaching 47.33 MPa and 470.7 MPa, respectively. The barrier properties of PBCC are superior to those of commercial biodegradable poly(butylene adipate-co-terephthalate) (PBAT), with barrier capabilities being 6.2–29.9 times, 1.6–4.3 times, and 1.1–2.8 times those of PBAT for CO 2 , O 2 , and water vapor respectively. In addition, PBCCs retained the biodegradability, and their biodegradation could be accelerated by the catalytic activity of CALB enzyme. Overall, PBCC has great potential as an environmentally friendly biodegradable packaging material.
研究领域:
高分子科学
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材料工程
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环境科学
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化学合成
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生物降解
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包装技术
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产品关联
DOI
高影响因子
BIOCATALYSIS AND BIOTRANSFORMATION
·
2024
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IF 1.4
Yuyang Zhou,Rongchen Mang,Huiyi Long,Yamiao Li,Hua Zhou,Dingqiang Lu
Dioctyl sebacate is a long carbon chain dibasic acid ester with methylene as the main body. It is widely used in plasticizers because of its good cold resistance and high viscosity. And it has excellent properties of non-toxicity and easy biodegradation, so it can be used as a potential new green bio-based plasticizer. At present, most of the preparation methods of dioctyl sebacate are chemical methods, which have many by-products and cause environmental pollution. In this article, cellulose microspheres were used as a carrier to immobilize Candida antarctica lipase B (CALB) to catalyse the esterification of sebacic acid and n-octanol to prepare dioctyl sebacate. Through single factor experiments, the lipase immobilized on cellulose microspheres was optimized to determine the best process conditions: add 500 µL CALB to the erlenmeyer flask, and then add 0.02 mol/L PBS buffer (pH 8.0). After being prepared into a 5 mL system, 0.1 g of cellulose microspheres were added as a carrier and reacted for 3 h at 35 °C and 180 r/min. Added 0.5 vt% polyethylene glycol diglycidyl ether (PEGDEG) to the system for crosslinking. The final immobilization rate of lipase immobilized on cellulose microspheres was 80.06%, and the enzyme activity was 288.07 U/g. Using the cellulose-immobilized lipase as a catalyst, in the toluene system, the molar ratio of n (sebacic acid)/n (n-octanol) substrate was 1:3.5, the amount of immobilized enzyme was 0.04 g, 4 Å molecular sieve 1.5 g, 40 °C, and 150 r/min for 30 h, the conversion rate of dioctyl sebacate was 76.45%.
研究领域:
生物催化
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化学工程
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绿色化学
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材料科学
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产品关联
DOI
高影响因子
Engineering
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2022
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IF 12.834
Xue Cai,Jiang-Wei Shen,Yu Qiang,Jing Hua,Zhang-Qi Ma,Zhi-Qiang Liu,Yu-Guo Zheng
Lipase-catalyzed stereoselective resolution of cis -(±)-dimethyl 1-acetylpiperidine-2,3-dicarboxylate ( cis -(±)-1) is an attractive route for the synthesis of ( S,S )-2,8-diazobicyclo[4.3.0]nonane, an important chiral intermediate of the fluoroquinolone antibiotic, moxifloxacin. In our previous study, a lipase from Sporisorium reilianum (SRL) was identified to possess excellent thermostability and pH stability. However, the low enzymatic activity of the SRL is a challenge that must be addressed. A rational design was initially employed for SRL tailoring according to the engineered Candida antarctica lipase B (CALB), resulting in a beneficial variant called SRL-I194N/V195L. Subsequently, two key amino acid residues in loop 6, L145 and L154, which might modulate the lid conformation between open and closed, were identified. A tetra-site variant, SRL-I194N/V195L/L145V/L154G (V13), with a significantly enhanced activity of 87.8 U∙mg −1 was obtained; this value was 2195-fold higher than that of wild-type SRL. Variant V13 was used to prepare optically pure (2 S ,3 R )-dimethyl 1-acetylpiperidine-2,3-dicarboxylate ((2 S ,3 R )-1), resolving 1 mol∙L −1 cis -(±)-1 with a conversion of 49.9% in 2 h and absolute stereoselectivity ( E > 200). Excellent stability with a half-life of 92.5 h was also observed at 50 °C. Overall, the study findings reveal a lipase with high activity toward cis -(±)-1 at an industrial level and may offer a general strategy for enhancing the enzyme activity of other lipases and other classes of enzymes with a lid moiety.
研究领域:
生物化学
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生物技术
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酶学
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药物化学
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有机化学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
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2021
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IF 5.706
Qian Wang,Meiling Ge,Xuan Guo,Zhijun Li,Agen Huang,Fu Yang,Rong Guo
The mesoporous supports of alkylated poly(ionic liquid)s (PILs) are got through free radical copolymerization . With an immobilization yield of 99% for Candida antarctica lipase B (CalB), the biocatalyst showed high advantage for biodiesel production under mild conditions. Typical catalyst CalB 0.2 @PIL-C8 was capable of effectively converting soybean oil into biodiesel with a yield of 68.2%, which is higher than Novozym 435 for 57.5%. The biodiesel yield was almost 1.5 folds compared to that of free CalB under the same conditions. And the catalyst remained about 80% activity in a seven-run recovery test with no CalB leaching in the whole process. The hydrophobic PILs not only provide a suitable reaction micro-environment but also can help CalB keep an open conformation in immobilizing with its flexible hydrophobic alkyl chains. This research offered a green and effective strategy for regulating the hydrophobicity and surface potential of support to enhance the performance of immobilized lipase.
研究领域:
化学工程
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生物技术
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材料科学
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环境科学
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产品关联
DOI
高影响因子
PROCESS BIOCHEMISTRY
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2024
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IF 3.7
Shihao Liang,Wei Zhuang,Zhenfu Wang
In this work, isocyanate-based strategy was developed for efficient immobilization of Candida antarctica lipase B (CALB). Of 41 commercial resins, EP109 was chosen and hydrophobized with hydroxyl-terminated polydimethylsiloxane (HTPDMS) for tert-butyl isocyanate (tBIC)-based CALB immobilization due to high loading amount and specific activity. The tBIC-based strategy exhibited shorter immobilization time, higher loading and activity than adsorption strategy by hydrophobic interaction. When compared with free CALB, EP109-HTPDMS-tBIC@CALB owned improved stability (against acid, alkali, and heat) and storability. Subsequently, EP109-HTPDMS-tBIC@CALB was employed in the bio-synthesis of 1,3-diacylglycerol in a solvent-free system with a yield of 76.31%, which was higher than commercial Novozym 435 (53.93%). EP109-HTPDMS-tBIC@CALB exhibited 76.34% of residual activity after 20 repeat uses.
研究领域:
生物技术
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酶工程
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化学工程
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生物化学
✓ 已验证
产品关联
DOI
高影响因子
Synthetic and Systems Biotechnology
·
2020
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IF 0
Shiyi Che,Jie Wang,Xiaoyuan Ji,Zhiguo Su,Shaomin Wang,Songping Zhang
Polyelectrolyte-doped microcapsules (PDM) was fabricated by coaxial electrospray of a mixture of glycerol and water containing 10 mg/mL cationic polyelectrolyte poly(allylamine hydrochloride) (PAH) fed as the core phase solution, and a N,N-dimethylacetylamide solution of 10 wt% polyurethane fed as the shell phase solution. Multi-enzyme system involving Candida Antarctica lipase B (CALB), glucose oxidase (GOD), and horseradish peroxidase (HRP) for cascade reaction was assembled in the PDM at three different places, namely, surface, shell, and lumen. Placing of enzyme inside aqueous lumen of the PDM was realized by in situ encapsulation through adding the enzyme in the core-phase solution for coaxial electrospray. By ion-pairing of enzyme with cationic surfactant CTAB, an organic soluble enzyme-CTAB complex was prepared, so that in situ embedding of enzyme in the shell of the PDM was realized by adding it into the shell phase solution. Surface attachment of enzymes was achieved by layer-by-layer (LbL) technology, which is based on the ion-exchange interactions between oppositely charged enzymes and PAH that was doped in PDM. The enzyme-decorated microcapsule was then studied as a micro-bioreactor, in which 1-Oxododecyla-α-glucopyranoside was converted by CALB to glucose, which was oxidised by GOD to gluconolactone in a second step. The hydrogen peroxide produced was then used by HRP to oxidize ABTS to form coloured radical cation ABTS • + for activity analysis. The successful fabrication of the PDM and precise localization of enzymes in the PDM by different strategies were fully characterized. By varying the immobilization strategy, totally six PDM bioreactors with three enzymes precisely positional assembled in different strategies were constructed and their activities for the cascade reaction were investigated and compared. The PDM micro-bioreactor prepared by novel electrospray technologies provide a smart platform for positional assembly of multi-enzyme cascade reaction in a precise and well-controlled manner.
研究领域:
材料科学
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生物技术
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化学工程
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生物化学
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产品关联
DOI
PubMed
Catalysis Science & Technology
·
2018
·Vol. 8
·期 18
·4718-4725
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IF 5.365
Jiang-Wei Shen,Jia-Mei Qi,Xiao-Jian Zhang,Zhi-Qiang Liu,Yu-Guo Zheng
Candida antarctica lipase B (CALB) is a versatile and robust lipase with high activity and enantioselectivity in the resolution of alcohols and amines. Poor specific activity toward carboxylic esters that are branched or substituted in close proximity to the carboxyl group limits the application of CALB. In this study, a semi-rational engineering approach was successfully applied to tailor CALB for efficient synthesis of the moxifloxacin chiral intermediate through enzymatic resolution of cis-(±)-dimethyl 1-acetylpiperidine-2,3-dicarboxylate. The combinatorial active-site saturation test was performed on CALB and two key residue sites, 189 and 190, were identified in the determination of hydrolytic activity. The specific activity and catalytic efficiency (kcat/Km) of the best variant mut-I189K were increased by 286- and 193-fold, respectively, without impacting its enantioselectivity. With 0.1 g L−1 of purified mut-I189K loading, 1 M substrate was asymmetrically hydrolyzed with 49.9% conversion within 5 h, resulting in a space–time yield of 583.8 g L−1 d−1. These results demonstrated that mut-I189K is a competitive biocatalyst for large-scale preparation of the moxifloxacin chiral intermediate.
研究领域:
生物催化
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酶工程
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药物化学
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有机合成
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）