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Metal-organic framework hybrid materials of ZIF-8/RGO for immobilization of D-amino acid dehydrogenase

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Nano Research 2024年第1期17卷 290-296页

作者： Hangbin Lei Qian Zhang Xiaoyan Xiang Liang Jiang Shiyan Wang Lingxuan Duan Shizhen Wang department of chemical and biochemical engineering College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Xiamen Key Laboratory of Synthetic Biotechnology Xiamen UniversityXiamen 361005China

Immobilization of D-amino acid dehydrogenase(DAADH)by the assembly of peptide linker was studied for the biosynthesis of Dphenylalanine.Hybrid material of zeolitic imidazolate framework-8(ZIF-8)combined with reduced graphene oxide(RGO)was applied for the immobilization of DAADH from Ureibacillus thermosphaericus.The recovery rate of DAADH/ZIF-8/RGO was 165.6%.DAADH/ZIF-8/RGO remained 53.4%of its initial activity at 50°C for 10 h while the free enzyme was inactivated.DAADH/ZIF-8/RGO maintained 70.5%activity in hyperalkaline solution with pH 12.Kinetic parameters indicated that DAADH/ZIF-8/RGO had greater affinity of phenylpyruvate as V_(max)/K_(m)of DAADH/ZIF-8/RGO was 1.27-fold than free enzyme.After seven recycles,the activity of DAADH/ZIF-8/RGO remained 64.3%.Furthermore,one-step separation and in situ immobilization of DAADH by ZIF-8/RGO/Ni was carried out with 1.5-fold activity enhancement.Combining peptide linker and metal-organic framework(MOF)immobilization,thermostability and activity of the immobilized DAADH were significantly improved.

关键词： D-Amino acid dehydrogenase immobilization metal-organic frameworks zeolitic imidazolate framework-8(ZIF-8) reduced graphene oxide

Rational surface charge engineering of haloalkane dehalogenase for boosting the enzymatic performance in organic solvent solutions

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Chinese Journal of chemical engineering 2024年第1期65卷 276-285页

作者： Yin Wu Yan Sun department of biochemical engineering School of Chemical Engineering and Technology and Key Laboratory of Systems Bioengineering and Frontiers Science Center for Synthetic Biology(Ministry of Education)Tianjin UniversityTianjin 300350China

Biocatalysis in organic solvents(OSs)has numerous important applications,but native enzymes in OSs often exhibit limited catalytic performance.Herein,we proposed a computation-aided surface charge engineering strategy to improve the catalytic performance of haloalkane dehalogenase DhaA in OSs based on the energetic analysis of substrate binding to the DhaA surface.Several variants with enhanced OS resistance were obtained by replacing negative charged residues on the surface with positive charged residue(Arg).Particularly,a four-substitution variant E16R/E93R/E121R/E257R exhibited the best catalytic performance(five-fold improvement in OS resistance and seven-fold half-life increase in 40%(vol)dimethylsulfoxide).As a result,the overall catalytic performance of the variant could be at least 26 times higher than the wild-type DhaA.Fluorescence spectroscopy and molecular dynamics simulation studies revealed that the residue substitution mainly enhanced OS resistance from four aspects:(a)improved the overall structural stability,(b)increased the hydrophobicity of the local microenvironment around the catalytic triad,(c)enriched the hydrophobic substrate around the enzyme molecule,and(d)lowered the contact frequency between OS molecules and the catalytic triad.Our findings validate that computationaided surface charge engineering is an effective and ingenious rational strategy for tailoring enzyme performance in OSs.

关键词： Surface charge engineering Organic solvent resistance Molecular dynamics simulation Haloalkane dehalogenase

Enhanced direct gaseous CO_(2) fixation into higher bio-succinic acid production and selectivity

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Journal of Environmental Sciences 2024年第9期143卷 164-175页

作者： Ziyi Yang Wanling Wu Qing Zhao Irini Angelidaki Samuel Gyebi Arhin Dongliang Hua Yuxiao Zhao Hangyu Sun Guangqing Liu Wen Wang Biomass Energy and Environmental engineering Research Center Beijing University of Chemical TechnologyBeijing 100029China College of chemical engineering Beijing University of Chemical TechnologyBeijing 100029China department of chemical and biochemical Environmental engineering Technical University of DenmarkDK-2800Kgs LyngbyDenmark Energy Research Institute Qilu University of Technology(Shandong Academy of Sciences)Shandong Provincial Key Laboratory of Biomass Gasification TechnologyJinan 250014China

Utilizing CO_(2)for bio-succinic acid production is an attractive approach to achieve carbon capture and recycling(CCR)with simultaneous production of a useful platform chemical.Actinobacillus succinogenes and Basfia succiniciproducens were selected and investigated as microbial catalysts.Firstly,the type and concentration of inorganic carbon concentration and glucose concentration were evaluated.6 g C/L MgCO_(3)and 24 g C/L glucose were found to be the optimal basic operational conditions,with succinic acid production and carbon yield of over 30 g/L and over 40%,respectively.Then,for maximum gaseous CO_(2)fixation,carbonate was replaced with CO_(2)at different ratios.The“less carbonate more CO_(2)”condition of the inorganic carbon source was set as carbonate:CO_(2)=1:9(based on the mass of carbon).This condition presented the highest availability of CO_(2)by well-balanced chemical reaction equilibrium and phase equilibrium,showing the best performance with regarding CO_(2)fixation(about 15 mg C/(L·hr)),with suppressed lactic acid accumulation.According to key enzymes analysis,the ratio of phosphoenolpyruvate carboxykinase to lactic dehydrogenase was enhanced at high ratios of gaseous CO_(2),which could promote glucose conversion through the succinic acid path.To further increase gaseous CO_(2)fixation and succinic acid production and selectivity,stepwise CO_(2)addition was evaluated.50%-65%increase in inorganic carbon utilization was obtained coupled with 20%-30%increase in succinic acid selectivity.This was due to the promotion of the succinic acid branch of the glucose metabolism,while suppressing the pyruvate branch,along with the inhibition on the conversion from glucose to lactic acid.

关键词： Succinic acid CO_(2) fixation Actinobacillus succinogenes Basfia succiniciproducens Lactic acid

Durable poly(binaphthyl-co-p-terphenyl piperidinium)-based anion exchange membranes with dual side chains

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Journal of Energy Chemistry 2024年第2期89卷 324-335,I0008页

作者： Weiting Gao Xuelang Gao Qiugen Zhang Aimei Zhu Qinglin Liu department of chemical&biochemical engineering Fujian Provincial Key Laboratory of Theoretical and Computational ChemistryThe College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005FujianChina department of Chemistry Pohang University of Science and Technology(POSTECH)Pohang 790-784South Korea

Building well-developed ion-conductive highways is highly desirable for anion exchange membranes(AEMs).Grafting side chain is a highly effective approach for constructing a well-defined phaseseparated morphological structure and forming unblocked ion pathways in AEMs for fast ion transport.Fluorination of side chains can further enhance phase separation due to the superhydrophobic nature of fluorine groups.However,their electronic effect on the alkaline stability of side chains and membranes is rarely reported.Here,fluorine-containing and fluorine-free side chains are introduced into the polyaromatic backbone in proper configuration to investigate the impact of the fluorine terminal group on the stability of the side chains and membrane properties.The poly(binaphthyl-co-p-terphenyl piperidinium)AEM(QBNp TP)has the highest molecular weight and most dimensional stability due to its favorable backbone arrangement among ortho-and meta-terphenyl based AEMs.Importantly,by introducing both a fluorinated piperidinium side chain and a hexane chain into the p-terphenyl-based backbone,the prepared AEM(QBNp TP-QFC)presents an enhanced conductivity(150.6 m S cm^(-1))and a constrained swelling at 80℃.The electronic effect of fluorinated side chains is contemplated by experiments and simulations.The results demonstrate that the presence of strong electro-withdrawing fluorine groups weakens the electronic cloud of adjacent C atoms,increasing OH^(-)attack on the C atom and improving the stability of piperidinium cations.Hence QBNp TP-QFC possesses a robust alkaline stability at 80℃(95.3%conductivity retention after testing in 2 M Na OH for 2160 h).An excellent peak power density of 1.44 W cm^(-2)and a remarkable durability at 80℃(4.5%voltage loss after 100 h)can be observed.

关键词： Anion exchange membranes Backbone structure Fluorinated side chain Alkaline stability

Synergistic effect of adsorption and photocatalytic degradation of oilfield-produced water by electrospun photocatalytic fibers of Polystyrene/Nanorod-Graphitic carbon nitride

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Journal of Environmental Sciences 2024年第7期141卷 287-303页

作者： Parisa Azmoon Mehrdad Farhadian Alireza Pendashteh Amir H.Navarchian department of chemical engineering Faculty of EngineeringUniversity of IsfahanIsfahanIran department of chemical engineering Faculty of EngineeringUniversity of GuilanRashtIran department of Water and Environmental engineering Caspian Sea Basin Research CenterUniversity of GuilanRashtIran

Graphitic carbon nitride with nanorod structure(Nr-GCN)was synthesized using melamine as a precursor without any other reagents by hydrothermal pretreatment method.XRD,FTIR,SEM,N_(2)adsorption-desorption from BET,UV-Vis DRS spectroscopy,and photoluminescence were used to characterize the prepared samples.Also,the photoelectrochemical behavior of nanoparticles was studied by photocurrent transient response and cyclic voltammetry analysis.Polystyrene(PS)fibrous mat was fabricated by electrospinning technique and used as a support for the stabilization of the nanoparticles.The performance of the synthesized nanoparticles and photocatalytic fibers(PS/Nr-GCN)was evaluated in oilfield-produced water treatment under visible light irradiation.During this process,oil contaminants were adsorbed by hydrophobic polystyrene fibers and simultaneously degraded by Nr-GCN.The removal efficiency of chemical oxygen demand(COD)has been obtained 96.6%and 98.4%by Nr-GCN and PS/Nr-GCN,respectively,at the optimum conditions of pH4,photocatalyst dosage 0.5 g/L,COD initial concentration 550 mg/L,and illumination time 150 min.The gas chromatography-mass spectroscopy analysis results showed 99.3%removal of total petroleum hydrocarbons using photocatalytic fibers of PS/Nr-GCN.The results demonstrated that the GCN has outstanding features like controllable morphology,visible-light-driven,and showing high potential in oily wastewater remediation.Moreover,the synergistic effect of adsorption and photocatalytic degradation is an effective technique in oilfield-produced water treatment.

关键词： Graphitic carbon nitride(GCN) Nanorod structure Polystyrene fibrous mat Photocatalytic fibers Oilfield-produced water(OPW)

Neuronal conversion from glia to replenish the lost neurons

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Neural Regeneration Research 2024年第7期19卷 1446-1453页

作者： Shiyu Liang Jing Zhou Xiaolin Yu Shuai Lu Ruitian Liu National Key Laboratory of biochemical engineering Institute of Process EngineeringChinese Academy of SciencesBeijingChina School of chemical engineering University of Chinese Academy of SciencesBeijingChina department of Geriatric Rehabilitation Beijing Rehabilitation HospitalCapital Medical UniversityBeijingChina

Neuronal injury,aging,and cerebrovascular and neurodegenerative diseases such as cerebral infarction,Alzheimer’s disease,Parkinson’s disease,frontotemporal dementia,amyotrophic lateral sclerosis,and Huntington’s disease are characte rized by significant neuronal loss.Unfo rtunately,the neurons of most mammals including humans do not possess the ability to self-regenerate.Replenishment of lost neurons becomes an appealing therapeutic strategy to reve rse the disease phenotype.Transplantation of pluripotent neural stem cells can supplement the missing neurons in the brain,but it carries the risk of causing gene mutation,tumorigenesis,severe inflammation,and obstructive hydrocephalus induced by brain edema.Conversion of neural or non-neural lineage cells into functional neurons is a promising strategy for the diseases involving neuron loss,which may overcome the above-mentioned disadvantages of neural stem cell therapy.Thus far,many strategies to transfo rm astrocytes,fibroblasts,microglia,Muller glia,NG2 cells,and other glial cells to mature and functional neurons,or for the conversion between neuronal subtypes have been developed thro ugh the regulation of transcription factors,polypyrimidine tra ct binding protein 1(PTBP1),and small chemical molecules or are based on a combination of several factors and the location in the central nervous system.However,some recent papers did not obtain expected results,and discrepancies exist.Therefore,in this review,we discuss the history of neuronal transdifferentiation,summarize the strategies for neuronal replenishment and conversion from glia,especially astrocytes,and point out that biosafety,new strategies,and the accurate origin of the truly co nverted neurons in vivo should be focused upon in future studies.It also arises the attention of replenishing the lost neurons from glia by gene therapies such as up-regulation of some transc ription factors or downregulation of PTBP1 or drug interfe rence therapies.

关键词： astrocytes neural stem cells neurodegenerative diseases neuron polypyrimidine tract binding protein 1 repair reprogramming small molecule transcription factor transdifferentiation

Aggregation-regulated bioreduction process of graphene oxide by Shewanella bacteria

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Chinese Journal of chemical engineering 2024年第5期69卷 56-62页

作者： Kaixin Han Yibo Zeng Yinghua Lu Ping Zeng Liang Shen department of chemical and biochemical engineering College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Pen-Tung Sah Institute of Micro-Nano Science and Technology Xiamen UniversityXiamen 361005China Chinese Research Academy of Environmental Sciences Beijing 100012China

The bioreduction of graphene oxide(GO)using environmentally functional bacteria such as Shewanella represents a green approach to produce reduced graphene oxide(rGO).This process differs from the chemical reduction that involves instantaneous molecular reactions.In bioreduction,the contact of bacterial cells and GO is considered the rate-limiting step.To reveal how the bacteria-GO integration regulates rGO production,the comparative experiments of GO and three Shewanella strains were carried out.Fourier-transform infrared spectroscopy,X-ray photoelectron spectroscopy,Raman spectroscopy,and atomic force microscopy were used to characterize the reduction degree and the aggregation degree.The results showed that a spontaneous aggregation of GO and Shewanella into the condensed entity occurred within 36 h.A positive linear correlation was established,linking three indexes of the aggregation potential,the bacterial reduction ability,and the reduction degree(ID/IG)comprehensively.

关键词： Graphene oxide Reduced graphene oxide Bioreduction Aggregation Shewanella

Inhibition of Defect-Induced Ice Nucleation, Propagation, and Adhesion by Bioinspired Self-Healing Anti-Icing Coatings

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Research 2024年第1期2023卷 237-246页

作者： Shu Tian Ruiqi Li Xinmeng Liu Jiancheng Wang Junyu Yu Sijia Xu Yunqing Tian Jing Yang Lei Zhang department of biochemical engineering Frontier Science Center for Synthetic Biology and Key Laboratory of Systems Bioengineering(MOE)School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300350China Binzhou Institute of Technology Weiqiao-UCAS Science and Technology ParkBinzhou CityShandong Province 256606China

Anti-icing coatings on outdoor infrastructures inevitably suffer from mechanical injuries in numerous icing scenarios such as hailstorms,sandstorms,impacts of foreign objects,and icing–deicing cycles.Herein,the mechanisms of surface-defect-induced icing are clarified.At the defects,water molecules exhibit stronger adsorption and the heat transfer rate increases,accelerating the condensation of water vapor as well as ice nucleation and propagation.Moreover,the ice–defect interlocking structure increases the ice adhesion strength.Thus,a self-healing(at−20℃)antifreeze-protein(AFP)-inspired anti-icing coating is developed.The coating is based on a design that mimics the ice-binding and non-ice-binding sites in AFPs.It enables the coating to markedly inhibit ice nucleation(nucleation temperature<−29.4℃),prevent ice propagation(propagation rate<0.00048 cm^(2)/s),and reduce ice adhesion on the surface(adhesion strength<38.9 kPa).More importantly,the coating can also autonomously self-heal at−20℃,as a result of multiple dynamic bonds in its structure,to inhibit defect-induced icing processes.The healed coating sustains high anti-icing and deicing performance even under various extreme conditions.This work reveals the in-depth mechanism of defect-induced ice formation as well as adhesion,and proposes a self-healing anti-icing coating for outdoor infrastructures.

关键词： coating defect clarified

Recent advances in the microfluidic generation of shape-controllable hydrogel microparticles and their applications

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Green chemical engineering 2024年第1期5卷 16-30页

作者： Yingzhe Liu Zhuo Chen Jianhong Xu The State Key Lab of chemical engineering Department of Chemical EngineeringTsinghua UniversityBeijing100084China

Hydrogel microparticles,generally accepted as significant green materials,have been widely used in chemical,biological,and biomedical fields owing to their excellent biocompatibility,biodegradability,and noncytotoxicity.Among these,non-spherical hydrogel microparticles with diverse shape anisotropy have great potential in applications such as drug delivery,cellular interaction,micromotors,etc.Benefiting from their shapes,their functionalities in such fields cannot be satisfied by the typical spherical types.Recently,microfluidics with precise control and domination of fluids at microflow sizes has emerged as a powerful method for synthesizing shape-controllable hydrogel microparticles with good monodispersity and unique morphology.In this review,we tried to provide an overview of the production of non-spherical microparticles composed of green hydrogel materials,emphasizing the microfluidic approaches.Furthermore,a brief introduction to their current applications is also presented.

关键词： Microfluidics Hydrogel Microparticles Non-spherical Anisotropic Green materials