MACROMOLECULAR BIOSCIENCE
·
2026
·Vol. 26
·期 8
·e70238
·
IF 4.2
Meng Wang,Hongzhen Jia,Chengfu Zhang,Ningli Wang,Puzhao Liu,Dong Pei,Qingli Qu
Enzyme immobilization is an effective strategy to improve catalyst recovery and operational stability, but conventional approaches are often limited by diffusion resistance, steric hindrance, and insufficient control over the enzyme microenvironment. Hydrogel-based materials are attractive supports because their hydrated, tunable, and porous networks help preserve enzyme conformation while improving substrate diffusion and mass transfer. Here, a gas-shearing microfluidic strategy was developed to fabricate alginate/chitosan hydrogel microreactors for dual-mode lipase immobilization through entrapment and genipin-mediated covalent binding. By tuning gas-liquid shear, microspheres with controllable and narrow size distribution were generated without surfactants or UV-initiated polymerization. Importantly, genipin was introduced as a mild and biocompatible cross-linker to reinforce the alginate/chitosan network and create a stable interfacial microenvironment for enzyme immobilization. Compared with conventional cross-linkers, the milder and more controllable reactivity of genipin is advantageous in preserving enzyme conformation and catalytic performance. The resulting microreactors exhibited enhanced catalytic activity, improved storage stability, and good reusability. After five consecutive cycles, the entrapped and covalently immobilized systems retained 70% and 81% of their initial activity, respectively. These results demonstrate that gas-shearing microfluidics combined with genipin-mediated network reinforcement provides a robust and biocompatible platform for constructing hydrogel-based enzymatic microreactors with improved catalytic performance and operational durability.
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CLAYS AND CLAY MINERALS
·
2026
·
IF 2.8
Yuqi Yao,Shiyong Sun,Xingyun Yang,Pan Zhou,Haoming Tang,Shanshan Pu
Halloysite nanotubes (HNTs), naturally abundant clay minerals with unique tubular
structures and biocompatibility, offer significant potential as an enzyme immobilization
matrix. Conventional functionalization methods often involve energy-intensive
processes or compromise enzyme activity, however. The study offers an approach to
functionalizing HNTs via alkali activation and polydopamine (PDA) coating for
efficient immobilization of β-glucosidase (BG). Alkali treatment enhanced surface
hydroxyl density and defect sites, while PDA deposition through mild oxidative
polymerization provided a reactive interface for covalent enzyme conjugation mediated
by N-(3-Dimethylaminopropyl)-N’-ethylcarbodiimide hydrochloride (EDC)
crosslinking. Structural characterization (XRD, FTIR, SEM-EDS) confirmed
successful PDA coating and enzyme binding while preserving the crystalline integrity
of HNTs. At an optimal loading of 167mg·g
–1
support, the immobilization efficiency was
83% with retained activity. The immobilized BG not only exhibited optimal catalytic
performance at pH 6.0 and 60°C but also enhanced stability against pH/temperature
fluctuations through immobilization. Kinetic analysis revealed a 39% increase in Vmax
(4.73 vs. 3.40 mM·L
–1
·min–1
) and sustained substrate affinity (Km=10.4 mM·L
–1
). The
biocatalyst retained ≧84% activity after 30 days of storage at 4℃ and 53% activity
over six reuse cycles, attributed to the rigid enzyme conformation stabilized by covalent
PDA coupling and HNTs confinement. The research results presented are expected to
broaden the application scope of halloysite in the field of enzyme catalysis and provide
a feasible solution for improving the catalytic stability of β-glucosidase.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Huijun Li,Wenjie Liu,Zhouqing Xu,Junjun Sun,Jianliang Cao,Yan Wang
A facile sequential crystallization strategy is developed to fabricate isostructural HOF-on-HOF architectures with periodic interfacial lattice contrast. • Spatially stepwise immobilization of hemin across core and shell regions extends visible-light harvesting and provides reversible Fe(III)/Fe(II) redox sites. • The optimized LPFC-1@hemin@NPFC-1@hemin catalyst achieves a hydrogen evolution rate of 2345.1 μmol·g −1 ·h −1 under visible light (λ ≥ 420 nm), 1.84-fold higher than pristine LPFC-1. • The synergistic effect of interfacial charge regulation and hemin sensitization opens a new avenue for high-performance HOF-based photocatalyst design. Hydrogen-bonded organic frameworks (HOFs) have emerged as promising photocatalysts for sustainable hydrogen production, yet their performance suffers from intrinsically poor visible-light absorption and sluggish photogenerated carrier transfer kinetics. To address these issues, we herein report a facile sequential crystallization strategy to construct isostructural HOF-on-HOF materials, wherein a periodic interfacial lattice contrast spontaneously forms at the core-shell boundary. Moreover, this kind of structure further enables stepwise immobilization of hemin molecules in both the core and shell domains via hydrogen bonding and π···π stacking interactions. Benefiting from the synergistic effects between periodic interfacial lattice contrast and hemin immobilization, the optimal LPFC-1@hemin@NPFC-1@hemin (large-sized pyrene-based hydrogen-bonded organic frameworks, denoted as LPFC-1, nano-sized pyrene-based hydrogen-bonded organic frameworks, denoted as NPFC-1) catalyst exhibits an exceptional photocatalytic hydrogen evolution rate of 2345.1 μmol·g −1 ·h −1 under visible light irradiation (≥ 420 nm), which is 1.84 times higher than that of pristine LPFC-1. This work not only establishes a robust strategy to construct continuous HOF crystalline layers on preformed HOF crystals, but also presents an efficient route for stepwise hemin immobilization toward boosted photocatalytic hydrogen evolution. A stepwise layered growth strategy constructs well-defined HOF-on-HOF materials and achieves spatial immobilization of hemin for superior photocatalytic hydrogen generation. Download: Download high-res image (255KB) Download: Download full-size image
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INORGANIC CHEMISTRY COMMUNICATIONS
·
2026
·
IF 5.9
Xinyu Zhao,Zhenzhong Liu,Chunguang Li,Zhongran Dai
Optimized SRB-ethanol synergy removes 91.8% U(VI) and 86.3% sulfate. • Sequential mineralization ensures long-term U stability via reduction and encapsulation. • SRB dominance and sulfur respiration upregulation drive alkalinity, low Eh, and multi-metal co-precipitation. • δ 34 S used as a potential tracer for evaluating the restoration of underground mining environments. The efficacy of sulfate-reducing bacteria (SRB) in remediating uranium-contaminated groundwater hinges on the coupling mechanism between sulfate reduction and U(VI) immobilization, which remains poorly understood. Herein, we confirmed that under optimal conditions (pH 6.0, 0.4% ethanol, 10% inoculation rate), the combined treatment of an acid-tolerant sulfate-reducing bacterial consortium (previously isolated from the uranium mining area and laboratory-enriched) with ethanol achieved 91.8% removal of dissolved U and 86.3% reduction of sulfate, along with significant co-precipitation of dissolved Fe and Al. Mineralogical characterization reveals a sequentially linked mineralization network of UO 2 , FeS, CaCO 3 , and Al(OH) 3 , sustained by the SRB-mediated alkaline effect and the continuous decline in redox potential (Eh). High-throughput sequencing revealed enrichment of taxa affiliated with known sulfate-reducing lineages and upregulation of sulfur metabolism pathways, suggesting enhanced sulfate-reducing potential within the microbial community. Notably, sulfur isotope analysis (δ 34 S) revealed distinctly different apparent fractionation factors (ε) between low and high sulfate removal conditions (ε ≈ 2.15‰ vs. 0.22‰). This contrast tentatively suggests a potential shift in the rate-limiting step of sulfate reduction, although further time-series isotope measurements are required to rigorously validate this hypothesis. This work demonstrates the feasibility of SRB-enhanced remediation for uranium-contaminated groundwater and establishes δ 34 S as a potential geochemical tracer for assessing the effectiveness and long-term stability of remediation measures in underground mining environments. Download: Download high-res image (187KB) Download: Download full-size image
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Food and Bioprocess Technology
·
2026
·Vol. 19
·期 10
·495
·
IF 5.6
Deng Yaoyao,Lian Kang,Feng Wenjia,Zhang Haiyang,Gao Kunpeng,Jiang Hong,Sun Jian’an,Hu Yang
Docosahexaenoic acid (DHA) glycerides are regarded as ideal functional lipids due to their high bioavailability and safety, although their efficient enzymatic synthesis faces major challenges. Herein, crescent-shaped amphiphilic semi-Janus-poly(acrylic acid)/poly(styrene) particles (JPP) and semi-Janus-poly(vinylidene imine)/octadecane particles (JPO) were prepared and used as carriers for Candida antarctica lipase B (CALB) to improve its performance in the synthesis of DHA glycerides. The surface properties of the enzyme carrier could significantly affect enzymatic performance. Immobilization of CALB on the hydrophilic side of JPO (CALB@JPO(W)) significantly enhanced its activity and stability. Compared with free enzyme, CALB@JPO(W) exhibited a 2.19-fold enhancement in catalytic efficiency, increased optimal reaction temperature from 70 to 80 °C, and substantially improved thermal stability (retaining 70% of its initial activity after 1 h of incubation at 80 °C). JPO was simultaneously employed as a solid stabilizer and a carrier to enrich the biocatalyst at the interface, forming a Pickering emulsion interfacial catalysis system for the production of DHA glycerides. The yield of DHA glycerides catalyzed by CALB@JPO(W) reached 21.35%, representing a 72.66% improvement over free CALB. These results demonstrate that the reported Pickering emulsion interfacial catalysis system provides a potential strategy for the efficient production of functional lipids.
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FOOD RESEARCH INTERNATIONAL
·
2026
·
IF 8.8
Yuhan Li,Lingmei Dai,Dehua Liu,Wei Du
Metal-organic frameworks (MOFs) with tunable porosity are promising carriers for enzyme immobilization, but their practical application is limited by structural instability and difficult recovery. We previously developed an oxidation-reduction (O-R) pyrolysis strategy for mesoporous MIL-88 A, yielding a magnetic carrier (O-R-Meso) with excellent lipase immobilization and recyclable catalysis. Herein, we verify the applicability of this O-R pathway for Fe-based MIL-88 A with tailored pore structures (micro-, meso-, macroporous) by extending it to microporous C-MIL-88 A and macroporous SOM-MIL-88 A. The O-R derivatives (O-R C, O-R-Meso and O-R-SOM) retained the original morphology and pore channel integrity, with improved specific surface area and sufficient magnetization (13–23 emu/g) for magnetic separation. Notably, after O-R pyrolysis, MIL-88 A with various pore sizes essentially maintained or even enhanced the specific activity of immobilized lipase ( Candida antarctica lipase B, CalB), successfully deriving into magnetic carriers with enhanced catalytic efficiency and recyclability. This superiority originates from the preserved pore structure and biocompatible γ-Fe 2 O 3 surface of the O-R derivatives, which effectively retain the native conformation of CalB. Besides, this work systematically compares the secondary structure of free and immobilized CalB on MOF-derived carriers with distinct pore architectures, providing direct structural evidence for the superior enzyme-carrier compatibility of mesoporous materials. In the transesterification synthesis of phosphatidyl EPA/DHA, CalB@O-R-Meso showed the highest EPA/DHA total incorporation, prominent sn -1 positional selectivity, and optimal reusability, outperforming CalB@O-R-C and CalB@O-R-SOM. Furthermore, kinetic studies on the CalB@O-R-Meso-catalyzed system confirmed a Ping-Pong Bi Bi mechanism and revealed competitive product inhibition by phosphatidyl EPA/DHA ( K i = 29.8 mM) with negligible internal mass transfer resistance (η ≈ 1). This work establishes a O-R pyrolysis strategy for tunable porosity Fe-MOFs, clarifies pore size-dependent enzyme -carrier compatibility, and provides a fundamental kinetic basis for phosphatidyl EPA/DHA synthesis.
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BIOTECHNOLOGY LETTERS
·
2026
·Vol. 48
·期 2
·44
·
IF 2.5
Ma Li,Wang Yuyu,Liu Ruiqi,Hu Jingjia,Zheng Xiaobing,Yue Xiaoyang,Liu Guanhua,He Ying,Zhou Liya
Developing stable and easy-to-operate biocatalysts is crucial for their use as industrial catalysts. Here immobilized whole-cell catalysts were used for β-alanine production by immobilizing recombinant Escherichia coli cells (containing hydroaminase) with diatomite. E. coli BL21 (DE3)/pET-30a ( +)-HAMase was genetically engineered for the efficient synthesis of β-alanine from acrylic acid and aqueous ammonia. Using glutaraldehyde as a cross-linking agent, polyethyleneimine (PEI) as a flocculant, and diatomite as the immobilization carrier, optimal immobilization was achieved with 8% (w/v) PEI solution, 5% (w/v) glutaraldehyde, and 100 mg wet cell/mL cell suspension, along with a PEI flocculation time of 2.5 h and glutaraldehyde cross-linking time of 1.5 h. The enzyme activity recovery rate reached 70.72%. Remarkably, the immobilized whole-cell catalysts exhibited excellent stability, retaining over 90% of initial enzyme activity after 12 h incubation at 45 °C and maintaining over 72% enzyme activity after storage for 60 days at 4 °C. Additionally, the immobilized cells demonstrated enhanced reusability, maintaining consistent β-alanine yield even after ten consecutive reaction batches with an average yield of approximately 80%.
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APPLIED CLAY SCIENCE
·
2026
·
IF 5.2
Shuli Wang,Fang Guo,Shufeng Chen,Siyuan Wang,Zhuoying Shan,Hang Lu,Wenbo Wang
Phosphorus pollution and the growing scarcity of phosphorus resources necessitate advanced materials capable of both efficient phosphorus removal and subsequent recovery. In this study, natural mineral intergrowths of mixed-phase palygorskite clay, in which carbonates are intergrown with clay minerals, were engineered to develop a high-performance adsorbent (WPAC700) via one-step thermal activation. This activation strategy generates in-situ multi-metallic sites by converting native carbonates and inert mineral surfaces into highly dispersed active metal centers comprising Ca, Mg, Al, and Fe. The clay matrix imposed a confinement effect that inhibits particle coalescence, thereby yielding a high density of accessible multi-metal sites. WPAC700 demonstrated exceptional phosphorus uptake kinetics, with a rate of 6.372 mg·g −1 ·min −1 at an initial phosphate concentration ≤ 10 mg·L −1 , achieving over 99.9% removal within 10 min and an adsorption capacity of 61.4 mg·g −1 . In real water matrices, including Yellow River water and seawater, residual phosphorus concentrations were consistently reduced to below 0.2 mg·L −1 , substantially outperforming commercial activated carbons. Site energy distribution analysis quantified the dominance of high-energy binding sites responsible for rapid sequestration. Mechanistic investigations revealed a synergistic interplay among Ca-dominated precipitation, Al/Fe-mediated ligand exchange, and pore filling. Notably, the phosphorus-laden material can be directly repurposed as a slow-release fertilizer, which promoted plant growth without phytotoxicity and reduced phosphorus leaching from soil. This work establishes a closed-loop paradigm that integrates deep water purification with phosphorus recovery, offering a transformative strategy for converting natural mineral architectures into advanced environmental materials.
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PROCESS BIOCHEMISTRY
·
2026
·
IF 4.4
Wenbin Jin,Gulina Bektursun,Xinyue Lin,Zuomo Ding,Xiaohong Yu
Efficient recovery and reuse of lipase remain major challenges in lipid biocatalysis. In this study, aldehyde-functionalized gum arabic-modified magnetic chitosan nanoparticles (GA-CHO/MCNPs) were developed as a biopolymer-based magnetic carrier for lipase immobilization. The carrier was prepared by in situ coprecipitation followed by surface modification with periodate-oxidized gum arabic. Under optimized conditions, the protein loading and protein-based immobilization yield reached 112.5 ± 4.8 mg g −1 and 84.6 ± 2.9%, respectively, while the recovered activity was 62.7 ± 3.1%. Compared with free lipase, Lipase@GA-CHO/MCNPs showed a higher optimum temperature (45 versus 35 °C), improved tolerance to pH and thermal treatment, and convenient magnetic recovery. Immobilization increased the apparent K m from 2.12 to 3.85 mM and decreased V max and k cat , indicating diffusional and steric limitations associated with the carrier. Nevertheless, the immobilized lipase achieved a soybean oil hydrolysis yield of 91.2%, retained 82.3% of its initial activity after 10 reuse cycles, and retained 84.8% activity after 30 d of storage at 4 °C. The results support successful lipase immobilization through an aldehyde-amine-mediated coupling strategy and demonstrate the potential of GA-CHO/MCNPs as a recoverable biopolymer-based carrier for soybean oil hydrolysis.
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BIORESOURCE TECHNOLOGY
·
2026
·
IF 8.2
Hangbin Lei,Xuefu Zeng,An-Ping Zeng,Shizhen Wang
Conductive DES stabilizes hydrogenase conformation via a dynamic hydrogen-bond network. • DES-modified MOF creates an anaerobic microenvironment that enhances the oxygen tolerance of the immobilized hydrogenase. • DES induces a 3D nanoflower to 2D nanosheet morphological transformation of the immobilized hydrogenase. Hydrogenases can reversibly catalyze the conversion of protons and electrons into hydrogen, which are widely applied in green biohydrogen production. However, hydrogenases face challenges of poor stability and oxygen sensitivity. In this work, conductive deep eutectic solvents (DES) modified metal–organic frameworks (MOFs) were studied as carriers for Pyrococcus furiosus [NiFe]-hydrogenase (pfSHI) immobilization to improve the stability and oxygen tolerance of the enzyme. Choline chloride-ethylene glycol (ChCl-EG) modification of MOFs stabilized the enzyme conformation. After 8 reuses, pfSHI@ChCl-EG-ZIF-67 retained 63.02 % relative activity, higher than that of pfSHI@ZIF-67 (56.18 %). This enhancement is due to ChCl-EG with dynamic hydrogen-bond network. Furthermore, ChCl-EG regulated the pore of MOFs through non-covalent host–guest interactions to create the anaerobic microenvironment, which enhances oxygen tolerance of hydrogenase. After 48 h of air exposure, pfSHI@ChCl-EG-ZIF-67 retained 45.64 % activity, representing 2.67-fold increases compared to free pfSHI. Additionally, ChCl-EG in-situ modulated the structural evolution from 3D nanoflowers (pfSHI@ZIF-67) to 2D nanosheets (pfSHI@ChCl-EG-ZIF-67) during hydrogenase immobilization. The k cat / K m of pfSHI@ChCl-EG-ZIF-67 was 851 s −1 ·mM −1 , which was 1.49-fold of that of pfSHI@ZIF-67. The immobilized hydrogenases by DES-modified MOF exhibits enhanced stability and oxygen tolerance, which is promising for applications in biohydrogen production. Download: Download high-res image (158KB) Download: Download full-size image
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JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Lei Liao,Shilong Song,Gaoling Liang,Xiaoqiang Wang,Ning Pan,Hao Lei,Yongde Zhang,Hao Zou,Jiajia Cheng,Jie Wen,Weifeng Zhang,Tingting Deng
Silver-loaded silica gel is widely used in spent fuel reprocessing plant due to its high adsorption efficiency of iodine and low influence of humidity and NO x . This study proposed a novel method for the disposal of iodine-loaded silver-silica gel. The elution of iodine using Na 2 S solution, the leaching of silver through HNO 3 solution. Subsequently, Zero-valent silver was synthesized via reduction of Ag + with NaBH 4 to recover silver. Additionally, the eluted iodide ions were transformed into iodosodalite and then combined with borosilicate glass powder for secondary immobilization. The results demonstrated that the elution efficiency of Na 2 S was 99.03%, the leaching efficiency of HNO 3 was 99.20%, and the recovery efficiency of Ag reached 86.93%. The iodine static saturated adsorption capacity of the silver-loaded silica gel prepared using recycled silver was 129.95 ± 3.46 mg/g, higher than original silver-loaded silica gel. In addition, the secondary immobilization body had a dense structure. The iodine leaching rate was 1.2×10 -4 g ⋅ m -2 ⋅ d -1 , which showed a good chemical stability. This work successfully realized the recycling of silver in iodine-containing silver-loaded silica gel and the safe disposal of iodine, which can provide new ideas for the disposal of iodine waste in spent fuel reprocessing plant.
研究领域:
核化学与化工
·
环境科学
·
材料科学
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2020
·
IF 5.162
Xin Wang,Lihong He,Jianrong Huang,Nanjing Zhong
In this study, SBA-15 was modified by halogen & haloalkanes and later used to immobilize lipases. The hydrolysis activity and the glycerolysis performance of the immobilized lipases was carefully studied. Highest activity of the immobilized Candida antarctica lipase B (CALB), Lipase from Aspergillus oryzae (AOL), Lecitase® Ultra (LU) and lipase from Rhizomucor miehei (RML) was respectively at 5577, 12000, 2822 and 11,577 U/g; in addition, the highest activity was obtained from the lowest or moderate lipase loading, at 25.73, 90.72, 89.52 and 30.56 mg/g respectively. The mechanism of lipase immobilization was studied and it was through interfacial activation. The halogen & haloalkanes modification of SBA-15 afforded considerable glycerolysis activity for diacylglycerols (DAG) preparation. CALB@SBA-15-CH 2 CH 2 (CF 2 ) 5 CF 3 and CALB@SBA-15-CH 2 CH 2 (CF 2 ) 7 CF 3 were suitable for DAG production, they both exhibited good reusability in glycerolysis reaction, with 117.36% and 93.06% of their initial glycerolysis activity retained respectively after ten cycles of reuse. The relationships between temperature with triacylglycerols (TAG) conversion were ln V 0 = 3.13–3.07/T and ln V 0 = 7.90–4.64/T respectively for CALB@SBA-15-CH 2 CH 2 (CF 2 ) 5 CF 3 and CALB@SBA-15-CH 2 CH 2 (CF 2 ) 7 CF 3 ; in addition, their activation energy ( Ea ) was respectively at 25.50 and 38.54 kJ/mol.
研究领域:
生物化学
·
酶工程
·
材料科学
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