ACS Sustainable Chemistry & Engineering
·
2026
·
IF 7.6
Zhou Deng,Zicheng Wu,Yaxin Chen,Yanhong Zhou,Manqi Cheng,Xiang Li,Yu Feng,Shiyu Lu,Zhiwei Yi,Guangya Zhang
Efficient deployment of carbonic anhydrase (CA) in direct air capture (DAC) is constrained by the lack of enzyme durability under alkaline, chemically complex, and long-term operating conditions. A carrier-free self-immobilization strategy based on encapsulin-mediated intracellular assembly was proposed to address these challenges. The fusion of Sulphurihydrogenibium azorense carbonic anhydrase (SazCA) with the encapsulin EncMh from Mycolicibacterium hassiacum enables spontaneous self-assembly into supramolecular particles during expression in host cells, allowing high-yield production and low-energy recovery by simple centrifugation. The resulting SazCA-EncMh assemblies exhibit high thermal stability and broad tolerance toward alkaline and ion-rich environments. Notably, their supramolecular state can be reversibly switched between nano- and microscale assemblies by pH modulation without loss of catalytic activity over multiple cycles. Under DAC, free SazCA-EncMh significantly enhances long-term Chlorella cultivation over 21 days, indicating sustained extracellular catalytic function and improved inorganic carbon availability. In addition, SazCA-EncMh exbibits improved stability relative to ferritin-based assemblies in representative DAC absorbents, including amino acid salts and tertiary amines. Overall, encapsulin-enabled self-immobilization offers a practical and scalable strategy for stabilizing CA under DAC-relevant conditions, supporting its integration into biological and hybrid carbon capture systems.
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ACS Applied Bio Materials
·
2026
·
IF 5.6
Jiatao Chen,Fuyun Xia,Xinxin Zhao,Buyi Wang,Meilin Shi,Dongdong Zhang
Real-time and in situ monitoring of dynamic changes in brain neurotransmitters is of significant importance for understanding their pathophysiological regulatory mechanisms. This study employed an in situ hydrogel covalent immobilization strategy mediated by oxidized poly-tannic acid (pTAox) to modify the carbon fiber electrode (CFE), in which the click chemical reaction between pTAox and five thiol molecules of varying chain lengths enables the oriented fixation of a seeding layer, followed by the construction of an in situ hydrogel coating via hydrogen bonding interactions with negatively charged tannic acid. It was found that the long-chain SH-PEG44-OH exhibited outstanding anti-fouling stability and interference resistance while maintaining high sensitivity, and the short-chain β-mercaptoethylamine (MEA), which displayed superior selectivity for positively charged dopamine (DA), was selected as the sealing agent. The TmPEG44-pTA/CFE microelectrode constructed based on an optimal combination exhibited outstanding selectivity, sensitivity, anti-fouling stability, and biocompatibility, as well as excellent linearity across DA concentrations ranging from 0.02 to 0.5 μM and 0.5 to 20 μM, with a detection limit of 18.9 nM (S/N = 3). Furthermore, TmPEG44-pTA/CFE facilitated real-time dynamic monitoring of DA release in the striatum of a living mouse. The present study proposes a systematic screening paradigm for the rational design of functionalized electrode interfaces, thus extending the application of the oriented covalent immobilization in situ hydrogel coating strategy to in vivo neurochemical analysis.
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高影响因子
AICHE JOURNAL
·
2026
·
IF 4.4
Yuan Li,Zhiwei Zhao,Feifei Zhang,Yating Wang,Yanjie Wang,Xiaoqing Wang,Jinping Li,Jiangfeng Yang
The production of high-purity CH 4 (>99.99%) is critical for energy and advanced industrial applications, but the simultaneous removal of N 2 and O 2 remains a significant challenge. Herein, we report a Cu(I) coordination-engineered metal–organic framework (Cu-CFA-1) based on theoretical design and experimental validation, which demonstrates remarkably selective adsorption of N 2 and O 2 over CH 4 , reversing the CH 4 selectivity of the parent material. In situ infrared spectroscopy and computational modeling studies revealed that the threefold coordination of Cu(I) by nitrogen ligands (Cu(I)-3N) significantly enhances its electron-donating capability, enabling targeted adsorption of π-acidic gases (N 2 /O 2 ) through charge-transfer effects. Breakthrough experiments demonstrated that Cu-CFA-1 can provide high-purity CH 4 in a single adsorption–desorption cycle from ternary (N 2 /O 2 /CH 4 ) and even six-component (N 2 /O 2 /CH 4 /CO 2 /C 2 H 6 /C 3 H 8 ) gas mixtures. This work provides an energy-efficient solution for CH 4 purification from multicomponent systems, and establishes a theoretical and practical foundation for the mechanism of π-acidic gas adsorption.
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CEMENT & CONCRETE COMPOSITES
·
2026
·
IF 14.4
Guokun Yang,Chuanlin Que,Junhui Kou,Yiye Lv,Jiuyuan Wang,Bo Qu,Rongyan Long,Guosheng Jiang,Tianle Liu
BaCO 3 -shelled phase change microcapsules improve sulfate resistance of cement paste. • The BaCO 3 shell immobilizes sulfate ions through in-situ ion exchange. • BMPCM regulates sulfate-attack products and pore-network deterioration. • Optimal BMPCM dosage reduces eroded area by 69.9% and enhances strength. Sulfate attack is one of the major degradation mechanisms responsible for expansion cracking, surface spalling, and long-term performance deterioration of cementitious materials. To improve the durability of cementitious materials in sulfate environments, a functional microcapsule (BMPCM) with a BaCO 3 shell and tetradecane core was prepared, and its effect on sulfate resistance was systematically evaluated. Cement paste specimens incorporating different BMPCM dosages were separately immersed in deionized water and MgSO 4 solution for up to 360 d. The deterioration behavior and underlying mechanisms of cement paste incorporating BMPCM were elucidated at multiple scales through macroscopic damage characterization, microstructural observation, hydration/sulfate-attack product analysis, pore connectivity assessment, and compressive strength testing. Results showed that the BaCO 3 shell reacted with invading SO 4 2− to form insoluble BaSO 4 , thereby chemically immobilizing sulfate ions. This process reduced the effective sulfate activity within the matrix, suppressed the formation of expansive products such as gypsum and ettringite, and mitigated the leaching of soluble hydration products such as Ca(OH) 2 . Compared with controls, specimens with an appropriate BMPCM dosage exhibited a 69.9% reduction in the severely deteriorated area, a 24.4% decrease in interconnected porosity, and a 44.9% increase in compressive strength after 360 d. In contrast, excessive BMPCM incorporation promoted microcapsule agglomeration and introduced initial defects, thereby weakening sulfate resistance. In addition, thermal analysis confirmed that BMPCM retained its phase-change response near the freezing point, suggesting its potential for further application in sulfate-resistant cementitious materials exposed to complex temperature-fluctuation service environments.
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BIORESOURCE TECHNOLOGY
·
2026
·
IF 8.2
Zihan Zhang,Yu Zhang,Qingqing Liu,Wanqing Song,Yi Hu,Binbin Nian
A novel triple evolution strategy overcame the lipase activity-stability trade-off. • CM5 showed 2.3-fold higher activity and 4.8-fold solvent tolerance than WT. • MD simulations link CM5 stability to rigidity and stable hydration shell. • The VES synthesis strategy achieved the highest yield and reusability to date. • A complete chain from computational design to practical production was validated. Biocatalysts exhibit broad application prospects in industrial production. However, the inherent instability of natural enzymes in non-aqueous media severely limits their practical utilization. Using Candida rugosa lipase as a model, a synergistic evolution strategy integrating ancestral sequence reconstruction, free energy optimization and surface hydration shell modulation was developed in this study. The optimal mutant CM5 exhibited simultaneously enhanced stability and activity, showing a 4.78-fold increase in tolerance to 65% (v/v) dimethyl sulfoxide, a 1.67-fold extension in half-life at 50 ℃ and a 2.30-fold increase in activity compared to the wild type. Molecular dynamics simulations indicated that the enhanced stability of CM5 originates from improved structural rigidity and the stabilized hydration shell. Meanwhile, its increased activity is attributed to a reduced energy barrier for the lid conformational transition and an optimal enzyme substrate affinity that significantly boosts substrate turnover efficiency. Moreover, a volumetric activity of 142.71 U/mL in a 5 L bioreactor was obtained via optimization of the chassis cells, and the resulting culture was then used for the immobilization. The lipase CM5 immobilized on amino octadecyl bifunctional macroporous resin (CM5@AOMR) achieved a vitamin E succinate yield of > 99.9% and maintained an outstanding yield of 98.2% even after ten consecutive batch reactions. Overall, this study developed a comprehensive workflow from computational design and efficient fermentation to immobilization and practical applications of lipase, providing a promising new approach for developing next generation biocatalysts suited for extreme industrial environments. Download: Download high-res image (234KB) Download: Download full-size image
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高影响因子
Advanced Science
·
2025
·
IF 14.1
Jie Zhao,Xinyi Liu,Dan Li,Xuefei Jing,Weijie Wu,Liangrui He,Yizhang Tang,Zhen Liu,Yulin Zeng,Haitian Sha,Huibin Qiu,Xujiang Yu,Wanwan Li
Constructing colloidal particles into designated hierarchies with integrated functionalities offers insights into bottom-up material fabrication. However, the arbitrary and controllable assembly of individual nanoscale and microscale particles remains highly challenging due to their diverse structural properties. Here, a general paradigm for the robust co-assembly of plasmonic noble metal nanoparticles and multifunctional polymer microspheres through thermodynamically driven heterocoagulation and coordination interactions is developed. Monodisperse poly(styrene-co-maleic anhydride) microspheres (PSMA MSs) are facilely synthesized using a one-step emulsification method with optional simultaneous encapsulation of magnetic and fluorescent nanoparticles. Upon surfactant removal, the purified PSMA MSs become metastable and trigger ultrafast co-assembly of silver nanocubes (AgNCs) onto MSs within 5 min with the maximum coverage rate reaching nearly 50%. The densely immobilized AgNCs outside magnetic MSs exhibit excellent catalytic efficiency (>89% conversion across 15 cycles) and enable enzyme integration for cascade reactions. Moreover, the largest reported plasmonic-fluorescent encoded array (124 codes) is realized, achieving a significantly improved detection limit of 10 copies/reaction for respiratory viruses. This work addresses the long-standing challenge of achieving uniform distribution and dense immobilization of plasmonic noble metal nanoparticles and offers a general approach to fabricating designated hierarchies based on noble metal nanoparticles, with integrated functionalities for high-performance practical applications.
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高影响因子
Catalysts
·
2022
·Vol. 12
·期 2
·242
·
IF 4.501
Youdan Duan,Ting Zou,Sijin Wu,Haiming Cheng
The hydrophobicity of a support plays a critical role in the catalytic efficiency of immobilized lipases. 3-aminopropyltriethoxysilane (APTES)-modified silica clay (A-SC) was coupled with silane coupling agents of different alkyl chains (methyl triethoxysilane, vinyl triethoxysilane, octyl triethoxysilane, and dodecyl triethoxysilane) to prepare a series of hydrophobic support for lipase immobilization. The lipases were immobilized onto the support by conducting glutaraldehyde cross-linking processes. The results showed that the activity of the immobilized biocatalyst increased with hydrophobicity. The hydrolytic activity of Lip-Glu-C12-SC (contact angle 119.8°) can reach 5900 U/g, which was about three times that of Lip-Glu-A-SC (contact angle 46.5°). The immobilized lipase was applied as a biocatalyst for biodiesel production. The results showed that the catalytic yield of biodiesel with highly hydrophobic Lip-Glu-C12-SC could be as high as 96%, which is about 30% higher than that of Lip-Glu-A-SC. After being recycled five times, the immobilized lipase still maintained good catalytic activity and stability. This study provides a good strategy to improve the efficiency of immobilized lipases, showing great potential for future industrial application on biodiesel production.Keywords:lipase;silica;biodiesel;immobilization;hydrophobic modification
研究领域:
生物化学
·
可再生能源
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高影响因子
TALANTA
·
2016
·
IF 4.035
Yun Guan,Lanjunzi Liu,Chao Chen,Xiuzhi Kang,Qingji Xie
The facile preparation of poly( l -DOPA)-tyrosinase (PD M -Tyr) composite and its application both in substrate (phenol) and inhibitor (atrazine) sensing is reported here for the first time. Effective immobilization of enzyme is realized via in-situ entrapping Tyr in poly( l -DOPA) (PD M ), which is formed by Tyr catalytic polymerization of l -DOPA. The Tyr modified electrode is simply prepared by dipping the PD M -Tyr composite on an Au electrode and then covered by Nafion. The thus-prepared Tyr-immobilized electrode exhibits excellent performance superior to most Tyr-based electrochemical biosensors, the sensitivity to phenol is as high as 5122 μA mM −1 in the linear range of 10 nM~1.25 μM, the apparent Michaelis-Menten constant ( K M app ) determined as low as 3.13 μM indicates strong substrate binding and high catalytic activity of the immobilized Tyr. The biosensor also works well in atrazine biosensing, with a linear detection range of 50 ppb~30 ppm and a low detection limit of 10 ppb obtained. In addition, the biosensor shows excellent stability, precision, high sensitivity and fabrication simplicity.
研究领域:
生物化学
·
环境科学
·
分析化学
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2020
·
IF 9.038
Shuyao Yu,Bing Du,Amanjiao Baheiduola,Chao Geng,Jianguo Liu
Municipal solid waste incineration fly ash (MSWI-FA) has been strictly controlled as hazardous waste globally because it contains various heavy metals and dioxins. This study prepared a nanometallic Al/CaO (n-Al/CaO) dispersion mixture via ball-milling as a reductive stabilization reagent for the simultaneous immobilization of heavy metals and detoxification of POPs like substance in MSWI-FA. Under optimal conditions, Cu, Zn, Cd, Cr, Ni, and Pb had been significantly immobilized (over 99.9 %) and the leaching concentration of Zn, Cd, Cr, Ni, and Pb were below the detectable limit. Simultaneously, 82.43 % of HCB can be destructed into alkanes and amorphous carbon. The porous structure of the fly ash and alkaline surface of n-Al/CaO promoted the adsorption and cracking of HCB. The highly active n-Al/CaO interacted with water as the hydrogen donor to promote the reductive dechlorination process. Hydrocalumite was a new mineral formed from the adsorption and complexation of heavy metal. Therefore, n-Al/CaO can strengthen the control of heavy metals in the S/S treatment of MSWI-FA, effectively detoxify chlorinated organics, and reduce environmental health risks.
研究领域:
环境科学
·
化学工程
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2020
·
IF 9.038
Xiang Qiu,Shushu Wang,Shanshan Miao,Hongbo Suo,Huajin Xu,Yi Hu
This work aims to achieve the co-immobilization of laccase and 2,2-binamine-di-3-ethylbenzothiazolin-6-sulfonic acid (ABTS) to improve removal capability of the biocatalyst for pollutants while avoiding potential pollution caused by ABTS. The laccase was immobilized on magnetic chitosan nanoparticles modified with amino-functionalized ionic liquid containing ABTS (MACS-NIL) based on Cu ion chelation (MACS-NIL-Cu-lac). The carrier was characterized by Fourier transform infrared spectroscopy, thermogravimetric analysis, x-ray diffraction and etc., and electron paramagnetic resonance confirmed the mediator molecule ABTS on the carrier could also play the role of electron transmission. MACS-NIL-Cu-lac presented relatively high immobilization capacity, enhanced activity (1.7-fold that of free laccase), improved pH and temperature adaptability, and increased thermal and storage stability. The removal performance assay found that MACS-NIL-Cu-lac had a good removal efficiency with 100.0 % for 2,4-dichlorophenol in water at 25 °C, even when the concentration reached 50 mg/L. Reusability study showed that after six catalytic runs, the removal efficiency of 2,4-dichlorophenol by MACS-NIL-Cu-lac could still reach 93.2 %. Additionally, MACS-NIL-Cu-lac exhibited higher catalytic efficiencies with 100.0 %, 70.5 % and 93.3 % for bisphenol A, indole, and anthracene, respectively. The high catalytic performance in pure water system obtained by the novel biocatalyst co-immobilizing laccase and electron mediator ABTS showed greater practical application value.
研究领域:
环境科学
·
生物技术
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BIOCHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 2.892
Yinzhou Guo,Jiangtao Liu,Kehu Zhang,Honghong Zhang,Yan Li,Zhongli Lei
In this study, a novel type of stimuli-responsive support materials was synthesized successfully by atom transfer radical polymerization (ATRP) and ring opening polymerization (ROP) of N-isopropylacrylamide (NIPAAm), tert -butyl methacrylate (tBMA) and ε-caprolactone (CL). β-Cyclodextrin (β-CD) and azobenzene (Azo) were employed as the starting groups to form PCL-hv-PNIPAAm by host–guest inclusion complexation, while PCL-PMAA was converted by simple hydrolysis of PCL-PtBMA with trifluoroacetic acid. Both PCL-PMAA and PCL-hv-PNIPAAm formed the microspheres by self-assembly. Their characteristics were confirmed by NMR, TEM, GPC, DLS, etc. Then, the microspheres were used for the immobilization of pectinase by electrostatic interaction. The optimal immobilization reaction parameters were 10 U/mL for pectinase at 25 °C for 4 h at pH = 6. Compared with free pectinase, the immobilized enzymes were found to exhibit better tolerance of variations in pH and temperature, as well as improved storage stability. Furthermore, the relative activity of the immobilized pectinase was controlled at approximately 13% when the temperature was higher than the LCST of PNIPAAm. With different light irradiation, there is approximately a 15% influence on the relative activity of the immobilized pectinase. This new enzyme support material has good environmental adaptability and can make the activity of immobilized enzymes be tailored predictably and enable the enzyme to be used as a biocatalyst for various applications in the food industry.
研究领域:
生物化学
·
材料科学
·
食品科学
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高影响因子
POLYMER ENGINEERING AND SCIENCE
·
2026
·
IF 3.6
Yunfeng Zhu,Lang Feng,Jiaqi Lai,Guangyao Hu,Jingjing Yang,Juan Zhang
The versatile polyurethane (PU) has been widely used in industrial and civil products due to the diversity of structure composition and adjustable mechanical properties. However, PU is prone to aging under UV light and thermal exposure due to its molecular structure, which includes UV-sensitive carbonyl and urethane groups as well as oxygen-susceptible ether bonds. Thus, this study proposes to modify rutile titanium dioxide (TiO 2 ) nanoparticles with 2,2′-methylenebis(6-tert-butyl-4-methyl-phenol) (antioxidant 2246) by using toluene-2,4-diisocyanate (TDI) as a molecular bridge to form a nanoscaled titanium dioxide-immobilized antioxidant, M-TiO 2 composites, and then incorporate M-TiO 2 composites into PU adhesives to achieve synergistic effects in improving their photo- and thermo-oxidative aging resistance. The results indicate that the antioxidant 2246 molecules are chemically anchoring onto the surface of the TiO 2 particles and the modified TiO 2 particles show better dispersibility in PU matrix and are more efficient in improving the lap shear strength of PU adhesives than pure TiO 2 . PU adhesives containing M-TiO 2 composites exhibits superior aging resistance during the long-time accelerated photo- and thermo-oxidative aging, because of the synergistic effects of the UV-shielding properties of titanium dioxide particles and the neutralizing free radical capacity of antioxidant 2246. Highlights Antioxidant 2246 was chemically immobilized onto TiO 2 nanoparticles. TDI functioned as a molecular bridge between TiO 2 and antioxidant 2246. Surface modification improved TiO 2 dispersibility in the PU matrix. M-TiO 2 enhanced lap shear strength of PU adhesives. M-TiO 2 improved photo- and thermo-oxidative aging resistance of PU adhesives.
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危险品化学品经营许可证（带存储）