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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)

Design of a Novel Electrochemical Aptasensor Based on Molybdenum Disulfide Nanosheets for Lysozyme Detection

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Journal of Analysis and Testing 2024年第1期8卷 16-27页

作者： Tavoos Beiki Ghasem Najafpour-Darzi Maedeh Mohammadi Mohsen Shakeri biotechnology Research Laboratory Department of Chemical EngineeringBabol Noshirvani University of TechnologyBabol 47148-71167Iran department of Mechanical engineering Babol Noshirvani University of TechnologyBabol 47148-71167Iran

The precise detection of lysozyme plays a crucial role in early diagnosis of kidney failure in leukemia patients.Herein,we designed an electrochemical aptasensor to detect lysozyme using a glassy carbon electrode(GCE)modified with molybdenum disulfide(MoS_(2))nanosheets decorated with chitosan(Ch)and gold nanoparticles(Au).In the next steps of aptasensor preparation,aptamer(Apt)strands were immobilized on MoS_(2)-Au-Ch/GCE surface via electrostatic interactions,and bovine serum albumin(BSA)solution was applied to cover unbonded areas on Apt/MoS_(2)-Au-Ch/GCE.The MoS_(2)-Au-Ch nanocomposite can warrant enhanced immobilization of aptamers and strong signals because of wrinkle-like structure and base planes in MoS nanosheets,presence of abundant amino and carboxyl functional groups in chitosan and Au nanoparticles.Differential pulse voltammetry(DPV)was used to evaluate the electrochemical behavior of the aptasensor at each preparation step and its detection performance.The developed electrochemical aptasensor based on MoS nanosheets showed remarkable performance for lysozyme detection in the range from 1 pmol/L to 10 nmol/L with a limit of detection of 2.2 fmol/L.The proposed aptasensor provided excellent selectivity against BSA,uric acid,cytochrome C,lysozyme and their mixture.In addition,it displayed great stability of about 99.58%of the initial signal upon 21-day storage.Tests on human serum and urine samples yielded promising recoveries ranging from 98 to 105%.Hence,MoS_(2)-Au-Ch nanocomposite-based aptasensor could be an outstanding candidate for medical device applications and protein quantification.

关键词： Electrochemical aptasensor Lysozyme MoS_(2)nanosheets Apt/MoS_(2)-Au-Ch/GCE

Recent Advances in Catalytic Carbonylation Reactions in Alternative Reaction Media

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Chinese Journal of Chemistry 2024年第4期42卷 406-429页

作者： Csaba Árvai László T.Mika department of chemical and Environmental Process engineering Faculty of Chemical Technology and BiotechnologyBudapest University of Technology and EconomicsMűegyetem rkp.3H-1111 BudapestHungary

Since the discovery of the hydroformylation(oxo-synthesis or Roelen reaction)and the Reppe-reaction,the transition metal-catalyzed carbonylation reactions,providing versatile,facile,and even atom-economic methods for the selective incorporation of C=O functionality to various skeletons,have gained tremendous importance in synthetic organic chemistry from laboratories to industrial applications.The carbonylation of carbon-carbon multiple bonds,aromatic halides,triflates,etc.,in the presence of various nucleophiles has led the way to produce aldehydes,carboxylic acids,esters,amides,etc.,in the fine chemical industry.However,these protocols usually proceed in conventional,fossil-based,and usually toxic reaction environments.Thus,several attempts have been directed to developing efficient carbonylation methods in alternative,less harmful,non-fossil-based and even in renewable reaction media.In this review,we overview the recent applications of alternative solvents such as water,biomass-based alcohols,γ-valerolactone(GVL),2-methyltetrahydrofuran(2-MeTHF),ionic liquids(ILs),deep eutectic solvents(DES),alkyl levulinates,limonene,α-pinene,and dimethyl carbonate as well as fluorous media to improve efficiency,safety and environmentally benign nature of carbonylation protocols.

关键词： Carbonylation Catalysis Solvents Green chemistry Carbon monoxide Transition metals Homogeneous catalysis Palladium

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

Microfluidic-oriented synthesis of enriched iridium nanodots/carbon architecture for robust electrocatalytic nitrogen fixation

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Green Energy & Environment 2024年第3期9卷 544-555页

作者： Hengyuan Liu Xingjiang Wu Yuhao Geng Xin Li Jianhong Xu The State Key Laboratory of chemical engineering Department of Chemical EngineeringTsinghua UniversityBeijing100084China

Electrocatalytic nitrogen reduction reaction(NRR)is considered as a promising candidate to achieve ammonia synthesis because of clean electric energy,moderate reaction condition,safe operating process and harmless by-products.However,the chemical inertness of nitrogen and poor activated capacity on catalyst surface usually produce low ammonia yield and faradic efficiency.Herein,the microfluidic technology is proposed to efficiently fabricate enriched iridium nanodots/carbon architecture.Owing to in-situ co-precipitation reaction and microfluidic manipulation,the iridium nanodots/carbon nanomaterials possess small average size,uniform dispersion,high conductivity and abundant active sites,producing good proton activation and rapid electrons transmission and moderate adsorption/desorption capacity.As a result,the as-prepared iridium nanodots/carbon nanomaterials realize large ammonia yield of 28.73 μg h^(-1) cm^(-2) and faradic efficiency of 9.14%in KOH solution.Moreover,the high ammonia yield of 11.21 μg h^(-1) cm^(-2) and faradic efficiency of 24.30%are also achieved in H_(2)SO_(4) solution.The microfluidic method provides a reference for large-scale fabrication of nano-sized catalyst materials,which may accelerate the progress of electrocatalytic NRR in industrialization field.

关键词： Iridium nanodots Carbon Microfluidic technology Efficient synthesis Electrocatalytic nitrogen fixation

An efficient approach for the treatment of radioactive waste perfluoropolyether lubricants via a synergistic effect of thermal catalysis and immobilization

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Journal of Environmental Sciences 2024年第2期136卷 512-522页

作者： Xinhang Du Wenhua Tong Xinyu Zhou Jia Luo Yuqiu Liu Yabo Wang Panyu Li Yongkui Zhang department of Pharmaceutical&Biological engineering School of Chemical EngineeringSichuan UniversityChengdu 610065China

Perfluoropolyether(PFPE)lubricants are a kind of high-molecular polymer with many excellent properties.However,the use of PFPEs in the nuclear industry can lead to partial decomposition and carrying radionuclides,resulting in a large amount of radioactive waste PFPE lubricants annually.Moreover,radioactive waste PFPE lubricants are difficult to be effectively treated due to their high stability,the risk of possible leakage of radionuclides,and hypertoxic fluorine-containing by-products.In this study,without any precedent,a strategy of Mn O_(2)-catalyzed decomposition and Na_(2)CO_(3)-immobilized conversion was proposed for PFPE lubricant decomposition and fluorine immobilization simultaneously based on the Lewis acid-base and oxygen vacancies concept.A high fluorine conversion efficiency of 95.4%was achieved.Meanwhile,the mechanism of decomposition suggested that Mn O_(2)mainly provided Lewis acid sites and attacked the(basic)fluorine or oxygen atoms in PFPE molecules.The decomposition of PFPE chains was proceed down and volatile fluorine-containing gas was released by partial electron transfer,intramolecular disproportionation reaction,and unzipping fashion.Subsequently,gas by-products could be further oxidized and then immobilized into fluoride salts by carbonate solid absorbents.Overall,this study provides a simple,safe,and potentially practical strategy for the harmless conversion of refractory fluorinated organic wastes,especially perfluoropolymers.

关键词： Perfluoropolyether lubricants Catalyzed decomposition Fluorine-containing gas Immobilized conversion Fluoride

Investigating the impact of dynamic structural changes of Au/rutile catalysts on the catalytic activity of CO oxidation

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Carbon Energy 2024年第4期6卷 222-232页

作者： Xiaochun Hu Qianwenhao Fan Mingwu Tan Yuqing Luo Xianyue Wu Manoel Y.Manuputty Jie Ding Tej SChoksi Markus Kraft Rong Xu Zhiqiang Sun Wen Liu School of Energy Science and engineering Central South UniversityChangshaChina School of Chemistry Chemical Engineering and BiotechnologyNanyang Technological UniversitySingaporeSingapore Cambridge Centre for Advanced Research and Education SingaporeSingapore Institute of Sustainability for chemicals Energy and EnvironmentJurong IslandSingapore College of Chemistry and chemical engineering Central South UniversityChangshaChina department of chemical engineering and biotechnology University of CambridgeCambridgeUK

The surface properties of oxidic supports and their interaction with the supported metals play critical roles in governing the catalytic activities of oxide‐supported metal catalysts.When metals are supported on reducible oxides,dynamic surface reconstruction phenomena,including strong metal–support interaction(SMSI)and oxygen vacancy formation,complicate the determination of the structural–functional relationship at the active sites.Here,we performed a systematic investigation of the dynamic behavior of Au nanocatalysts supported on flame‐synthesized TiO_(2),which takes predominantly a rutile phase,using CO oxidation above room temperature as a probe reaction.Our analysis conclusively elucidated a negative correlation between the catalytic activity of Au/TiO_(2) and the oxygen vacancy at the Au/TiO_(2) interface.Although the reversible formation and retracting of SMSI overlayers have been ubiquitously observed on Au/TiO_(2) samples,the catalytic consequence of SMSI remains inconclusive.Density functional theory suggests that the electron transfer from TiO_(2) to Au is correlated to the presence of the interfacial oxygen vacancies,retarding the catalytic activation of CO oxidation.

关键词： CO oxidation electronic metal-support interactions flame‐synthesis metal-support interactions oxygen vacancy strong metal-support interaction

Constructing a biofunctionalized 3D-printed gelatin/sodium alginate/chitosan tri-polymer complex scaffold with improvised biological andmechanical properties for bone-tissue engineering

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Bio-Design and Manufacturing 2024年第1期7卷 57-73页

作者： Amit Kumar Singh Krishna Pramanik Amit Biswas Centre of Excellence in Tissue engineering Department of Biotechnology and Medical EngineeringNational Institute of TechnologyRourkela 769008India

Sodium alginate(SA)/chitosan(CH)polyelectrolyte scaffold is a suitable substrate for tissue-engineering application.The present study deals with further improvement in the tensile strength and biological properties of this type of scaffold to make it a potential template for bone-tissue regeneration.We experimented with adding 0%–15%(volume fraction)gelatin(GE),a protein-based biopolymer known to promote cell adhesion,proliferation,and differentiation.The resulting tri-polymer complex was used as bioink to fabricate SA/CH/GEmatrices by three-dimensional(3D)printing.Morphological studies using scanning electron microscopy revealed the microfibrous porous architecture of all the structures,which had a pore size range of 383–419μm.X-ray diffraction and Fourier-transform infrared spectroscopy analyses revealed the amorphous nature of the scaffold and the strong electrostatic interactions among the functional groups of the polymers,thereby forming polyelectrolyte complexes which were found to improve mechanical properties and structural stability.The scaffolds exhibited a desirable degradation rate,controlled swelling,and hydrophilic characteristics which are favorable for bone-tissue engineering.The tensile strength improved from(386±15)to(693±15)kPa due to the increased stiffness of SA/CH scaffolds upon addition of gelatin.The enhanced protein adsorption and in vitro bioactivity(forming an apatite layer)confirmed the ability of the SA/CH/GE scaffold to offer higher cellular adhesion and a bone-like environment to cells during the process of tissue regeneration.In vitro biological evaluation including the MTT assay,confocal microscopy analysis,and alizarin red S assay showed a significant increase in cell attachment,cell viability,and cell proliferation,which further improved biomineralization over the scaffold surface.In addition,SA/CH containing 15%gelatin designated as SA/CH/GE15 showed superior performance to the other fabricated 3D structures,demonstrating its potential for use in bone-tissue engineering.

关键词： Scaffold Biomaterial Sodium alginate Chitosan Gelatin 3D printing Tissue engineering

Novel self-assembled porous yolk-shell NiO nanospheres with excellent electrochromic performance for smart windows

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Particuology 2024年第1期84卷 72-80页

作者： Baoshun Wang Ya Huang Siming Zhao Run Li Di Gao Hairong Jiang Rufan Zhang Beijing Key Laboratory of Green chemical Reaction engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing100084China

With the rapid development of optoelectronics,electrochromic(EC)materials(ECMs)with the advan-tages of low power consumption,easy viewing,high contrast ratio,etc have attached more and more attention from the fields of smart windows,electronic billboards,emerging wearable and portable electronics,and other next-generation displays.Nickel oxide(NiO)is a promising candidate for high-performance ECMs because of its neutral-colored states and low cost.However,NiO-based ECMs still face the problem of slow switching speed due to their low electrical conductivity and small lattice spacing.Metal-organic frameworks(MOFs)are promising candidates to fabricate hollow and porous transition metal oxides(TMOs)with high ion transport efficiency,excellent specific capacitance,and electrochemical activities.In this work,porous yolk-shell NiO nanospheres(PYS-NiO NSs)were syn-thesized via a solvothermal and subsequent calcination process of Ni-MOF,which exhibited outstanding EC performance.Because the large specific surface areas and hollow porous nanostructures were conducive to ionic transport,PYS-NiO NSs exhibited a fast coloring/bleaching speed(3.6/3.9 s per one coloring/bleaching cycle)and excellent cycling stability(82%of capacity retention after 3000 cycles).These superior EC properties indicated that the PYS-NiO NSs was a promising candidate for high-performance EC devices.This work provides a new and feasible strategy for the efficient preparation of TMOs ECMs with good EC performance,especially fast switching speed.

关键词： Electrochromic Nickel oxide Metal-organic frameworks Hollow structure Smart windows