Journal of Oleo Science
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2020
·
IF 1.304
Maomao Kou,Siting Feng,Nanjing Zhong
In this study, Lecitase® Ultra (LU) was immobilized onto the parent and the amino-functionalized SBA-15. The immobilization conditions were studied and the activity of the parent SBA-15 supported LU (SBA-15-LU) was found to be at 2177.78 ± 101.84 U/g. After 3-aminopropyl and n-(2-aminoethyl)-3-aminopropyl groups functionalization, enzymatic activity was increased to 3555.56 ± 200.21 and 3444.44 ± 346.41 U/g respectively. The immobilized LU samples were then used to catalyze glycerolysis. The possibility for diacylglycerols (DAG) and monoacylglycerols (MAG) production was evaluated and it was found only suitable for DAG production. In addition, the glycerolysis activity of the immobilized LU was impaired by the tert-pentanol and solvent-free was found suitable. Similar DAG content over 50 wt% could be obtained from glycerolysis by the three immobilized LU samples. The reusability in glycerolysis was evaluated, and 9.79 % of the initial glycerolysis activity was remained from the SBA-15-LU after 5 cycles of reuse. Encouragingly, after 3-aminopropyl and n-(2-aminoethyl)-3-aminopropyl groups functionalization, 62.93 and 83.91% of their initial activity was respectively remained after 5 cycles of reuse.
研究领域:
生物化学
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酶工程
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食品科学
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DOI
PubMed
高影响因子
JOURNAL OF MATERIALS CHEMISTRY
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2012
·Vol. 22
·期 15
·7456-7460
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IF 5.968
Chengfei Yuan,Wufeng Chen,Lifeng Yan
Metal-free catalysts are essential for various chemical reactions in industrial chemistry. Amino-functionalized carbon is a cheap and environmentally friendly solid basic catalyst. Here, NEt3-graphene solid basic catalyst has been synthesized through a consecutive deprotonation/carbometalation and electrophilic substituent. Transmission electron microscopy (TEM), scanning electron microscopy (SEM), elemental analyses, thermal analyses, Raman spectroscopy, and X-ray photoelectron spectroscopy (XPS) studies confirmed the formation of the target structure. Catalytic hydrolysis of ethyl acetate reveals that the amino-grafted graphene has a high catalytic activity.
研究领域:
材料科学
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催化化学
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2017
·
IF 2.843
Xiaoda Wang,Hongxing Wang,Jinyi Chen,Weiyue Zheng,Ting Qiu
We show the superiority of reactive dividing wall column (RDWC) to the single reactive distillation (RD) column in improving the conversion of reactant, taking the hydrolysis of methyl acetate (MA) as example. It is difficult to achieve above 99% conversion for MA in a traditional reactive distillation column (TRDC) due to the existence of self-catalyzed methanol (MeOH)-acetic acid (HAc) esterification reaction in the column bottom. In this work, more than 99% conversion of MA hydrolysis was realized experimentally in an RDWC by separating MeOH from the hydrolysis mixture. The effects of several operation parameters on hydrolysis conversion were systematically investigated, including feedwater–MA mole ratio, heat duty, mole flow rate of feed MA, and vapor distribution. The simulation results by Aspen Plus showed that RDWC has several improvements in MA hydrolysis over TRDC, including lower energy consumption, lower water–MA mole ratio, and larger production capacity. With the increase in MA conversion, the superiorities became more obvious and contribute to the weaker self-catalyzed MeOH–HAc esterification reaction in the RDWC.
研究领域:
化学工程
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工业化学
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DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
·
IF 5.2
Jinxiang Yang,Zihao Wang,Wei Xiao,Yan Peng,Meishuang Qiu,Xiaorong Xiong,Yizhuo Lu,Tianyou Chen,Zushun Xu
Zn(II)-complex-based nanozymes have been extensively used for the cleavage of carboxylic esters and phosphate esters. Cooperativity between neighboring Zn(II) complexes is of paramount importance for the development of Zn(II)-complex-based nanozymes with excellent efficiency. Here, we have developed a controllable synthetic strategy for the construction of Zn(II)-complex-based nanozymes by using the nanoprecipitation technique, which could bring Zn(II) complexes in close proximity and regulate their microenvironments. Linear copolymers containing di(2-picolyl)amine moieties were used for the preparation of Zn(II)-complex-based nanozymes by the coordination between di(2-picolyl)amine and Zn(II) ion. These Zn(II)-complex-based nanozymes displayed excellent catalytic performance in the hydrolysis of carboxylic esters. Moreover, hydrophobic Fe 3 O 4 nanoparticles could be incorporated into Zn(II)-complex-based nanozymes via the one-step nanoprecipitation approach, enabling the recovery of nanozymes by using a permanent magnet. Such nanozymes effectively catalyzed the hydrolysis of methyl parathion , which is highly resistant to spontaneous hydrolysis and is extremely hazardous. These nanozymes may find application in the hydrolysis of hazardous carboxylic esters and phosphate esters.
研究领域:
生物化学
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环境科学
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材料科学
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DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2024
·
IF 4.8
Zhi-Xing Han,Wei-Jie Cai,Fang-Ru Lin,Kai-Xin Zhao,Hong-Bin Luo,Zhi-Yuan Liu,Yangyang Liu,Jian-Lan Liu,Xiao-Ming Ren
Zirconium-based metal-organic frameworks (Zr-MOFs) with periodic Lewis acidic nodes have demonstrated impressive catalytic activity in the hydrolysis of organophosphorus nerve agents. Nevertheless, the powdered form of Zr-MOFs and the necessity of a base-buffered aqueous solution during the catalytic reaction pose significant challenges to their practical utilization. In this study, we demonstrate the efficient hydrolysis of an organophosphorus nerve agent simulant, dimethyl-4-nitrophenyl phosphate (DMNP), in both pure water and the solid phase under high humidity conditions, catalyzed by a membrane material. This material, denoted as Im@MOF-808/PVDF, was synthesized through the integration of MOF-808 particles onto PVDF membrane fibers, with imidazole (Im) molecular bases incorporated into the pores of MOF-808. Our findings emphasize the excellent flexibility and processability inherent in Im@MOF-808/PVDF. More notably, it exhibits exceptional catalytic performance in the hydrolysis of DMNP in pure water. Additionally, it demonstrates fair catalytic activity for solid-phase DMNP hydrolysis under high humidity conditions. These features position Im@MOF-808/PVDF as one of the most promising protective materials, showcasing substantial practical applicability.
研究领域:
化学工程
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材料科学
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环境科学
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DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2022
·
IF 5.518
Zihao Wang,Jinxiang Yang,Wei Xiao,Tianyou Chen,Changfeng Yi,Zushun Xu
To develop simple catalytic systems without well-defined tertiary structures is of paramount importance to perform bio-inspired chemistry but remains challenge. Here, we have developed a simple one-step strategy for preparing polystyrene-supported artificial catalytic triad (ACT) systems. Polymers containing ACTs and a polymer containing urea groups were designed and synthesized for the preparation of catalysts via nanoprecipitation. The coil-globule collapse of polystyrene chains created hydrophobic microenvironments. The catalytic performance could be regulated by altering polymer compositions . The hydrophobic microenvironments played important roles in the efficiency of polystyrene-supported artificial catalytic triads, arising from varied affinity for the hydrophobic substrates and/or regulating the local pK a of artificial catalytic triads. A postulated mechanism for ester hydrolysis over polystyrene-supported catalysts was presented. This strategy has potential applications for engineering other multifunctional, enzyme-inspired catalysts.
研究领域:
生物化学
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材料科学
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酶工程
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DOI
高影响因子
ACS Applied Nano Materials
·
2023
·
IF 5.9
Jiawei Lu,Ying-Nan Li,Youran Li,Huilin Zhu,Guiyang Shi
The reusability of immobilized lipases, including their hydrolysis activity, is greatly affected by lipase leakage, mass transfer channel blockage, and compound deposition on the outside surface. In this study, Candida antarctica lipase B (CALB) was immobilized on Fe3O4 nanoparticle-polyacrylonitrile (PAN) composite magnetic beads through phase inversion (L/FP). The hydrolysis activity of lipase was investigated using p-nitrophenyl palmitate (p-npp) as a model ester. To overcome the limitations of immobilized lipase in ester hydrolysis, three modification strategies were employed. First, lipase was covalently immobilized on Fe3O4 nanoparticles modified with methallyl (M9) and chloro (M13) silane modifiers, which exhibited faster immobilization with reduced lipase leaching and higher activity expression and stability. Second, poly(ethylene glycol) (PEG6000) and polylactic acid (PLA) were added to the precursors to physically modify the composite structures of L/FP, resulting in modified beads with larger specific surface area (15.26 m2·g–1) and smaller average pore size (19 nm). The modified beads, L/FP-9-M and L/FP-13-M, demonstrated superior reusability in long-term hydrolysis activity over 250 cycles. L/FP-9-M retained 63 and 34% of the initial activity at the 100th cycle and the 250th cycle, respectively. L/FP-13-M retained 55 and 36% of the initial activity at the 100th cycle and the 250th cycle, respectively. Furthermore, even after 250 repeated uses, the unit activities (U·gsupport–1) of both L/FP-9-M and L/FP-13-M remained higher than the initial activity of Novo 435.
研究领域:
生物化学
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材料科学
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酶工程
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DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-14
·
IF 15.7
Jia Donglin,Li Jiaxin,Zhu Kefan,Qiu Hengwei,Li Liang,Zhao Xing,Lan Zhineng,Yan Huilin,Yang Fu,Cui Peng,Sun Xin,Li Haifang,Zhu Pengkun,Liu Shaofeng,Li Meicheng
Perovskite quantum dots (PQD) hold great promise for next-generation photovoltaics. However, neat ester antisolvents hydrolyze inefficiently into target ligands under ambient conditions, compromising the formation of integral conductive capping on PQD surfaces. Herein, we construct alkaline environments, which facilitate the rapid substitution of pristine insulating oleate ligands with up to twice the conventional amount of hydrolyzed conductive counterparts. Theoretical calculations reveal that this environment renders ester hydrolysis thermodynamically spontaneous and lowers reaction activation energy by approximately 9-fold. Through tailoring potassium hydroxide coupled with methyl benzoate antisolvent for interlayer rinsing of PQD solids, the assembled light-absorbing layers exhibit fewer trap-states, homogeneous orientations, and minimal particle agglomerations. Consequently, the fabricated solar cells (0.036 cm 2 ) achieve a certified efficiency of 18.3%, the highest value among published PQD solar cell reports, alongside a steady-state efficiency of 17.85% and an average efficiency of 17.68% over 20 devices. Moreover, the alkaline treatment is broadly compatible with diverse solid-state treatments and PQD compositions, demonstrating universality in modulating PQD surface chemistry.
研究领域:
材料科学
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纳米科技
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光伏技术
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表面化学
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能源材料
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产品关联
DOI
PubMed
高影响因子
Catalysts
·
2017
·Vol. 7
·期 2
·49
·
IF 3.082
Chenhui Wang,Haobo Han,Wei Jiang,Xiaobo Ding,Quanshun Li,Yanbo Wang
Here, core-shell structured polydopamine-coated Fe3O4nanoparticles were constructed to immobilize thermostable lipase QLM fromAlcaligenessp. Systematical characterization indicated that lipase QLM was successfully immobilized on the surface of nanoparticles with an enzyme loading of 21.4 ± 1.47 mg/g immobilized enzyme. Then, the immobilized enzyme was demonstrated to possess favorable catalytic activity and stability in the ester hydrolysis, usingp-nitrophenyl caprylate as the substrate. Further, it was successfully employed in the kinetic resolution of (R,S)-2-octanol, and satisfactory enantioselectivity and recyclability could be obtained with an enantiomeric ratio (E) of 8–15 over 10 cycle reactions. Thus, core-shell structured polydopamine-coated Fe3O4nanoparticles can be potentially used as a carrier for enzyme immobilization to improve their activity, stability, and reusability, which is beneficial for constructing efficient catalysts for industrial biocatalysis.Keywords:lipase;immobilization;polydopamine;Fe3O4nanoparticle;core-shell structure;ester hydrolysis;kinetic resolution
研究领域:
生物化学
·
生物催化
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材料科学
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DOI
高影响因子
Molecular Catalysis
·
2025
·
IF 4.9
Hui Xia,Yameng Zhou,Yuanyuan Zheng,Qing Xu,Feng Xue
There is increasing interest in the protein engineering of β-glucosidases for improving transformation of glycosides. In this study, a novel steric hindrance scanning strategy is applied to β-glucosidase BgMd, resulting in six single-point mutants with significantly increased activity. Further iteration results in the optimized mutant E329K/R72N/A94H/T135H showed a remarkable 26.1-fold improvement in activity over the wild type. The time needed for the hydrolysis of 20 g/L polydatin is cut in half, and the conversion rate is increased to 95.93 %. Mutant A94T/V336T hydrolyzes 2 g/L of ginsenoside Rba1 in 48 h to generate CK with a yield increase from 26.94 to 76.38 %. The mutant E329N hydrolyses 2 g/L of astragaloside in 48 h with a yield increase from 30.19 to 96.23 %. BgMd and mutants exhibit optimal activity at 50–60 °C and pH 7.0, with enhanced stability and improved tolerance in select mutants. Molecular docking and molecular dynamics showed that the substrate pocket is split in two, and the catalytic effect of the mutants is largely explained. Molecular dynamics simulations provided evidence of structural changes and reduced interaction energies in the mutants. These results validate the steric hindrance strategy as an effective method to apply β-glucosidase in the biotransformation of glycosides.
研究领域:
生物化学
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蛋白质工程
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分子生物学
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DOI
高影响因子
RSC Advances
·
2020
·Vol. 10
·期 68
·41551-41559
·
IF 3.119
Jinyan Du,Shuangqing Qi,Juan Chen,Ying Yang,Tingting Fan,Ping Zhang,Shujuan Zhuo,Changqing Zhu
Ce-Doped carbon dots (CeCDs) were fabricated via a one-step hydrothermal carbonization using Ce(NO3)3·6H2O and EDTA·2H2O as precursors, and various experimental techniques were employed to characterize the morphology, structure and composition of the as-obtained CeCDs. Using the disodium salt of bis(4-nitrophenyl)phosphate (BNPP) as a DNA model substrate, mimetic phosphatase activity toward phosphate ester hydrolysis cleavage was investigated. It was found that similar to the catalytic character of the natural enzyme, CeCDs as a hydrolase mimic can exhibit a good catalytic activity for promoting BNPP hydrolysis, in which metal Ce(III) acts as a center for binding and activation of the metal-bound hydroxide complex as well as a source of nucleophilic metal hydroxides. Additionally, based on the Inner Filter Effect (IFE), fluorescence spectra can be used to monitor the hydrolysis of BNPP using CeCDs, which mimic phosphatase. Thus, the unique properties of the CeCD mimetic phosphatases as well as the IFE sensing strategy would provide an ideal platform to monitor the catalytic phosphate ester hydrolysis processes. Finally, to validate the availability of the established catalytic systems, the CeCDs were further applied for degradation of organophosphorus pesticide chlorpyrifos. The degradation efficiency was estimated to be a satisfactory value of 74.50%, exhibiting a potential application prospect for treatment of the pollutants in the soil and water.
研究领域:
材料科学
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生物化学
·
环境科学
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DOI
高影响因子
Molecular Catalysis
·
2020
·
IF 3.687
Qianqian Zhang,Xianbao Cui,Tianyang Feng,Ying Zhang,Xuemei Zhang,Jie He,Jixiao Wang
Acidic ionic liquids were employed to catalyze the hydrolysis of methyl acetate . The optimal ionic liquid catalyst 1-butylsulfonic-3-methylimidazolium trifluoromethanesulfonate ([BSO 3 HMIm][OTf]) was selected from four Brönsted acidic ionic liquids. The reaction kinetics and chemical equilibrium of hydrolysis reaction catalyzed by [BSO 3 HMIm][OTf] were investigated. The hydrolysis mechanism catalyzed by [BSO 3 HMIm][OTf] was proposed, and non-ideal pseudo-homogeneous (NIPH) model was derived based on the hydrolysis mechanism. The hydrolysis reaction with mixed ionic liquids as catalyst and solvent was also conducted. The influence of solvent 1-octyl-2,3-dimethylimidazolium bis((trifluoromethyl)sulfonyl)imide ([OMMIm][Tf 2 N]) on the reaction rate was investigated. The chemical-phase equilibrium (CPE) was measured to investigate the effects of [BSO 3 HMIm][OTf] and [OMMIm][Tf 2 N] on chemical equilibrium and vapor-liquid equilibrium of the reaction mixture. The results show that chemical equilibrium constant is not affected by IL catalyst and solvent, but the vapor-liquid equilibrium is significantly influenced by IL solvent.
研究领域:
化学工程
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催化科学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）