INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2018
·
IF 3.141
Junhui Rong,Juan Han,Yang Zhou,Lei Wang,Chunmei Li,Yun Wang
In enzymatic conversion of biomass, how to degrade cellulose into fermentable glucose in an economic, efficient, and clean way has become an important subject. As for the application of cellulase in cellulose degradation, the process optimization in enzyme engineering is urgently desired. The traditional multistep purification processes lead to rising production costs and reduced activity of cellulase; meanwhile, the difficulty in reusability of cellulase has also become a big baffle in the cost-effective application of cellulase in biomass degradation. In this paper, the biocatalyst Glu-linker-ELP-GB (GLEGB) containing binary tags, elastin-like polypeptide (ELP), and graphene-binding (GB), was constructed to simplify the purification and immobilization of β-glucosidase (Glu) from Coptotermes formosanus. A high recovery rate (97.2%) and purification fold (18.7) of GLEGB was obtained by only one round of inverse transition cycling (ITC) with 0.5 M (NH4)2SO4 at 25 °C in a short incubating time of 10 min. The purification performance of the one-round ITC method is superior to the commonly used Ni-NTA resin affinity method. Furthermore, the high loading amounts of GLEGB immobilized on GO (698.2 mg g–1) and C3N4 (527.3 mg g–1) were achieved by the synergistic effects of ELP and GB tags. The storage stability and thermal stability of GLEGB was significantly enhanced after immobilization. The recombinant GLEGB immobilized on GO, MGO, graphite, C3N4, C200, and C400 retained 71.4%, 69.5%, 75.1%, 61.2%, 73.5%, and 80.2% of their initial activities respectively after eight cycles. It is worth mentioning that the Km values of GLEGB immobilized on lamellar carbon materials including GO, MGO, and C3N4 are very close to free GLEGB, showing a high affinity of recombinant GLEGB to substrate. To our knowledge, this is the first report on enzyme-linker-ELP-GB system with wide application prospect in the efficient purification and immobilization of enzyme, which can achieve the goal of reducing cost and improving efficiency of biocatalyst in enzymatic conversion of biomass.
研究领域:
生物技术
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酶工程
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生物质转化
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材料科学
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DOI
高影响因子
GREEN CHEMISTRY
·
2026
·
IF 10.6
Weixi Kong,Biao Li,Qi Zhang,Xuyang Lei,Ke Zheng,Xiaoyang Yue,Yunting Liu,Yanjun Jiang
Chiral amines are key building blocks in pharmaceuticals, yet their efficient and sustainable synthesis via amine dehydrogenase (AmDH) remains challenging due to limitations in substrate loading, enzyme stability, and process scalability. Herein, we report an integrated biocatalytic platform for asymmetric reductive amination (ARA) that synergistically combines a bienzymatic system (CalAmDH for ARA and GDH for cofactor regeneration) with green solvent engineering, enzyme co-immobilization, and continuous-flow technology. A deep eutectic solvent (DES) buffer system based on betaine and acetic acid (Bet–HAc) was designed to enable high substrate concentrations, with molecular dynamics simulations revealing that the DES enhances CalAmDH activity and stability by suppressing an unfavorable helix-to-loop transition. Co-immobilization yielded a robust catalyst that, in a continuous-flow reactor, achieved high conversion, excellent enantioselectivity (>99% ee), and a space-time yield (STY) of 49.11 g·L⁻¹·h⁻¹. This represents a 185-fold enhancement over prior reports and demonstrates the power of combining DES-mediated stabilization with process intensification for the green, scalable synthesis of chiral amines.
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ANALYTICAL CHEMISTRY
·
2026
·
IF 7.3
Simin Zhang,Xiangfeng Chen,Yaping Shi,Xiangyu Zhu,Zongwei Cai
As bioactive compounds, chiral amino acids (AAs) have been demonstrated to play pivotal roles in different physiological processes, thereby influencing human health. The assessment of the relative enantiomeric ratio through analytical methods is essential for indicating the abnormal status of disease progression, which drives the development of effective methods for resolving and identifying enantiomers. This work presents a robust strategy for the ultrahigh-resolution analysis of chiral AAs using MALDI-TIMS-MS. By employing a chiral derivatization process using S-NIFE and stabilizing the soft chain of the derivatization reagent with bimetal ion addition, the separation of 19 pairs of proteinogenic AAs was successfully achieved. This method not only demonstrates outstanding separation capability but also proves its efficiency in determining enantiomeric ratios, extending its applicability to real sample analysis.
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DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.7
Geling Kuang,Jinchao Hou,Zichen Wang,Lixue Zhao,Yuxiao Feng,Hongwu Wang,Jiandong Cui
Developing chemo-enzymatic cascade catalysis in catalytic asymmetric synthesis is of utmost significance, but such processes often suffer from low reaction efficiency because of incompatible reaction environments and suppressed intermediate transportation. Herein, a novel compartmentalised metal–enzyme microcapsule nanohybrid, Candida antarctica lipase B@Pd(II)-loaded hydrophobic mesoporous silica nanoparticles (CALB@Pd(II)/HB-MSNs), was fabricated by spatially localizing Pd(II) active sites and CALB at the outer and inner interfacial layers of Pickering emulsion droplets, respectively. Benefiting from the localization of two catalysts in their preferred reaction microenvironments, nanoscale proximity of each other, and interfacial activation of lipase, the CALB@Pd(II)/HB-MSNs exhibited 60-fold higher activity than traditional random co-immobilized metal-enzyme catalysts (Pd(II)/HB-MSNs/CALB). Furthermore, the conversion of rac-1-phenylethanol catalyzed by CALB@Pd(II)/HB-MSNs reached 47.92 %, compared to only 4 % for the randomly co-immobilized catalyst Pd(II)/HB-MSNs/CALB, with a product enantiomeric excess of≥99 % in the cascade reaction of 4-pentynoic acid cycloisomerisation and racemic 1-phenylethanol chiral resolution. Our study offers a platform for the design of efficient chemoenzymatic catalytic cascades for the synthesis of fine chemicals.
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ACS Nano
·
2022
·
IF 18.027
Youyu Jia,Feng Shi,Hongying Li,Zhikun Yan,Jiwei Xu,Jiale Gao,Xiaoli Wu,Yifan Li,Jingtao Wang,Bing Zhang
Two-dimensional (2D) lamellar membranes, with highly ordered nanochannels between the adjacent layers, have revealed potential application prospects in various fields. To separate gases with similar kinetic diameters, intercalation of a functional liquid, especially an ionic liquid (IL), into 2D lamellar membranes is proved to be an efficient method due to the capacity of imparting solubility-based separation and sealing undesired defects. Stable immobilization of a high content of liquid is challenging but extremely required to achieve and maintain high separation performance. Herein, we describe the intercalation of a typical IL, 1-butyl-3-methylimidazolium tetrafluoroborate ([BMIM][BF4]), into the ionized nanochannels of sulfonated MXene lamellar membranes, where the sulfonate groups are anchored onto MXene nanosheets through a facile method based on metal-catechol chelating chemistry. Thanks to the intrinsic benefits of MXene as building blocks and the decorated sulfonate groups, the optimal membrane possesses adequate interlayer spacing (∼1.8 nm) and high IL uptake (∼47 wt %) and therefore presents a CO2 permeance of 519 GPU and a CO2/N2 selectivity of 210, outperforming the previously reported liquid-immobilized lamellar membranes. Moreover, the IL loss rate of the membrane within 7 days at elevated pressure (5 bar) is measured to be significantly decreased (from 43.2 to 9.0 wt %) after growing sulfonate groups on the nanochannel walls, demonstrating the excellent IL storage stability.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Caicai Fu,Tianying Lu,Xiao Dai,Ping Ding,Yonghua Xiong,Jun Ge,Xiaoyang Li
Mycotoxin is an important contaminant in food and the environment. The conventional methods for detoxification of mycotoxins are plagued by high chemical consumption, secondary pollution, and specific equipment required. In this study, we propose a chemoenzymatic cascade reaction for mycotoxin removal in an effective and green manner using an enzyme-metal hybrid catalyst synthesized by compartmental co-immobilized glucose oxidase (GOx) and Fe3O4 nanoparticles (NPs) on a flower-shaped covalent organic framework (COF). The GOx-Fe3O4@COF hybrid catalyst exhibits excellent activity in mycotoxin removal due to the enrichment of mycotoxins in COF and the cooperative catalysis between GOx and Fe3O4 NPs. The degradation efficiency of aflatoxin B1 (AFB1) in the chemoenzymatic cascade reaction catalyzed by GOx-Fe3O4@COF is 3.5 times higher than that in the Fenton reaction catalyzed by Fe3O4@COF. The GOx-Fe3O4@COF hybrid catalyst is highly active in a wide pH range of 3.0–7.0, overcoming the limitation of the Fenton reaction that can only perform below pH 3.0. This study provides a powerful tool for the efficient removal of mycotoxins.
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Journal of Material Cycles and Waste Management
·
2023
·Vol. 25
·期 4
·1781-1791
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IF 3.1
Duan Yin,Zheng Lin,Zhao Yimeng,Long Ling,Liu Xiaobo,Jiang Xuguang
MgO-based cementitious material (MCM) is a potential green substitute for solidifying municipal solid waste incineration fly ash (MSWI FA). Sodium hexametaphosphate (SHMP), a commonly used dispersant, has a great influence on the hydration process of MCM-MSWI FA blends. In this study, the effect of different SHMP additions on the performance of the MCM-MSWI FA (3:7 in mass ratio) blends was investigated. The compressive strength and leaching toxicity of the blends were measured, and the structural evolution was analyzed by XRD, FTIR, TG/DTG, and SEM. These tests revealed that the addition of SHMP could significantly optimize the effect of MCM solidifying MSWI FA since SHMP could promote the dispersion of hydration products in the blends. The blends containing more than 1% SHMP exhibited immobilization efficiencies higher than 97.5% for heavy metals (Cd, Pb, and Zn) after curing for 28 days. Collectively, this work demonstrates the indispensable role of SHMP in the application of MCM solidifying MSWI FA, providing theoretical support for practical engineering.
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Materials Today Chemistry
·
2022
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IF 7.613
Yipin Zhang,Chenyang Qi,Jing Tu
The poor stability and low reusability of enzymes have always been the hindrances to their large-scale applications. Herein, hollow mesoporous silica (HMS) nanoparticles have been constructed as nanoreactors for in situ enzyme immobilization, hemoglobin (Hb) was selected as a model enzyme. By utilizing zeolitic imidazolate framework-8 (ZIF-8) as the sacrificial template, the synthesis mechanism of Hb@ZIF-8 has been explored by adjusting the molar ratios of Zn 2+ and 2-methylimidazole. When the amount of Hb was constant, the shape of Hb@ZIF-8 gradually changed from flake to granular (from 50:200 mM to 50:800 mM). Furthermore, when the molar ratio of Zn 2+ and 2-methylimidazole was fixed, with the amount of Hb increasing, the size of Hb@ZIF-8 decreased gradually, with maximum loading capacity of 460 μg/mg. Subsequently, Hb@ZIF-8 was coated with silica shells and followed by the removal of ZIF-8 in phosphate-buffered saline (pH 5), resulting in Hb@HMS. Compared to free Hb, Hb in HMS nanoreactors maintained over 74% of original catalytic activity under extreme conditions, showing significant improvements on the stability. Further, Hb@HMS still retains 80% of enzymatic activity after 5 cycles, exhibiting its excellent reusability. This work provides an efficient strategy for enzyme immobilization, giving new horizons for biosensing, biocatalysis and biomedicine.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Peide An,Defeng Hu,Yide Han,Hao Meng,Xia Zhang
On accounting of the structure advantages of MOFs in the enzyme mimics and enzyme immobilization, in this work, the Hemin@PCN-222 (Mn) is constructed through an in-situ hydrothermal route by covalently bonded the –COOH of Hemin with the Zr(IV) of PCN-222 (Mn). With the help of the synergistic effects, the resulting Hemin@PCN-222 (Mn) represents excellent peroxidase-like activities in comparison with the single Hemin and PCN-222 (Mn) with a special enzyme activity of 6.71 U mg −1 . The Hemin@PCN-222 (Mn) was then employed as a carrier to immobilize the glucose oxidase (GOx), the immobilization conditions were optimized. Based on that, the optimized GOx@hemin@PCN-222 (Mn) was applied in the following cascade reaction: the glucose oxidation in the presence of oxygen catalyzed by the immobilized GOx firstly, and then the produced H 2 O 2 worked as an oxidant to oxidize ABTS. The quantity of produced ABTS + was monitored to assess the catalytic efficiency, and the contrast experiments were conducted over the mixture of the natural GOx and HRP. The above cascade process could also be used to detect the glucose, and the detection limit is determined. The high efficiency and the stability of the resulting GOx@hemin@PCN-222 (Mn) highlights the prospect applications of the MOFs-based enzyme mimics in the bio-catalysis and biosensing.
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高影响因子
COLLOIDS AND SURFACES B-BIOINTERFACES
·
2022
·
IF 5.999
Wenfeng Zhou,Xiaohong Zhou,Yuan Rao,Rijia Lin,Lei Ge,Pengpeng Yang,Hongman Zhang,Chenjie Zhu,Hanjie Ying,Wei Zhuang
Enzyme catalysis has clear advantages in the process of oxidizing glucose to produce gluconic acid . In the enzyme cascade, the improvement of the cascade efficiency is desired but challenging. Graphene oxide (GO) and ZIF-8 composites as enzyme support offer the promising opportunity that not only the cascade efficiency can be improved by control the distance between two enzymes, but also the stability can be improved. Here, a new strategy of GO assisted co-growth of ZIF-8 and enzyme was carried in a one-pot synthesis. Glucose oxidase&catalase immobilized in the ZIF-8/GO composites can obtain 98% residual activity after 15 days of storage with almost no enzyme shedding. The residual activity is still higher than 75% after 5 repeated uses. The presented method of controllable growth of metal organic frameworks on 2D nanosheet can also be extended for renewable energy devices, gas storage and separation of small molecules .
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高影响因子
Energies
·
2022
·Vol. 15
·期 12
·4242
·
IF 3.252
Xue-Yong Li,Jia-Ying Huang,Qiang Zhou,Yuan-Yuan Xu,Ponnandy Prabhu,Ye-Wang Zhang
Acetoin, a four-carbon hydroxyl-keto compound, is used in the food, pharmaceutical, and chemical industries. The cascade enzymatic production is considered a promising and efficient method to produce acetoin. However, the stability and compatibility of the enzymes under the same catalytic conditions are challenges that need to be resolved. In this work, alcohol dehydrogenase, acetaldehyde lyase, and NADH oxidase were selected to work at the same conditions to efficiently convert ethanol into acetoin. These three enzymes were immobilized on epoxy-modified magnetic nanomaterials to obtain highly stable biocatalysts. The stability and the immobilization conditions, including temperature, pH, enzyme–carrier ratio, and immobilization time, were optimized to obtain the immobilized enzymes with a high catalytic activity. The cascade reactions catalyzed by the immobilized enzymes yielded a high conversion of 90%, suggesting that the use of immobilized enzymes is a promising way to produce acetoin.Keywords:immobilization;NADH oxidase;acetaldehyde lyase;alcohol dehydrogenase;acetoin;cascade enzymatic reactions
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Yuliang Tu,Dongye Zhao,Yanyan Gong,Zhiliang Li,Hong Deng,Xueming Liu
Soil contamination by heavy metals and metalloids has been a major environmental challenge. While various remediation technologies have been reported, field data on the remediation effectiveness have been limited. We tested a new remediation technology for on-site immobilization of As(III) and Pb(II) in a contaminated soil at an abandoned chemical plant site. A novel ternary amending agent consisting of Fe 2 O 3 , MnO 2 , and Mg(OH) 2 (molar ratio = 1.0:5.5:5.5) was used to amend the soil on-site . Field monitoring data indicated that the amendment severed as a pH buffer and a long-term sequester for both As and Pb in the soil. At a dosage of 3 wt%, the acid-leachable As and Pb were lowered from 0.042–0.077 mg/L and 0.013–0.022 mg/L to 0.0062–0.0093 mg/L and 0.0030–0.0080 mg/L, respectively, after one day of the amendment, and to 0.0020–0.0050 mg/L and 0.0020–0.0054 mg/L after 240 days of aging. As(III) was oxidized to As(V) and subsequently immobilized via complexation and precipitation, whereas Pb(II) was sequestered via electrostatic attraction and chemical precipitation . The treatment cost was estimated at $31.5/m 3 . The results indicate that complex contaminants in soil can be effectively immobilized using combined amending agents that can interact with the target chemicals and induce synergistic immobilization reactions.
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