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Selective hydrodeoxygenation of polyethylene terephthalate plastic wastes into 1;4-dimethylcyclohexane by Ir-ReO_(x)/SiO_(2)+HZSM-5 catalytic system

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Science China Chemistry 2025年第4期68卷 1563-1575页

作者： Nan Wang Jieyi Liu Junde Wei Sibao Liu Guozhu Liu Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and Technology Tianjin 300072China Engineering Research Center of Polymer Green Recycling of Ministry of Education Fujian Key Laboratory of Pollution Control&Resource ReuseCollege of Environmental and ResourcesFujian Normal UniversityFuzhou 350007China Haihe Lab of Sustainable Chemical Transformations Tianjin 300192China

In order to mitigate the environmental impact of polyethylene terephthalate(PET)plastic pollution and enhance waste resource utilization;we developed a novel Ir-ReO_(x)/SiO_(2)+HZSM-5 catalytic system for the hydrodeoxygenation(HDO)of PET plastic wastes into cycloalkanes;particularly 1;4-dimethylcyclohexane(DMCH).Under mild conditions(190℃;3 MPa H_(2))with a certain amount of water in cyclopentane solvent;the highest yield of DMCH reached 95.8%;contributing to an overall yield of cycloalkanes at 98.4%within a reaction time of 4 h from HDO of virgin *** HDO of PET into DMCH involved initial hydrogenation of PET aromatic ring;then depolymerized by direct hydrogenolysis of acyl C-O bond in the ester group and subsequent cascade HDO of alcoholic C-O bond to saturated ester and alcohol intermediates;and further HDO of these oxygenates converting into desired DMCH *** Ir-ReO_(x)/SiO_(2) catalyst exhibits fully reduced metallic Ir nanoparticles along with partially reduced ReO_(x) species that are highly dispersed on both SiO_(2) surface and Ir nanoparticle *** oxophilic nature of ReO_(x) species facilitates the activation of C-O bonds;the acidic HZSM-5 zeolite for the promotion of dehydration reaction;and the protic property of H_(2)O for the enhancement of hydrogenation PET contributed to highly HDO activity of this ***;the catalytic system is applicable for the HDO of diverse real-world PET plastic wastes including Coca-ColaTM bottles;green Sprite bottles and white and red discarded fiber cloths;generating DMCH with a yield of up to 95.9%and cycloalkanes with a yield of up to 99.5%.This innovative process presents a new avenue for efficient hydrodeoxygenation conversion of PET into easily separable DMCH which serves as a crucial building block for the production of terephthalic acid to realize the chemical recycling of PET plastic wastes towards a green circular economy.

关键词： plastic wastes PET hydrodeoxygenation cycloalkane Ir-ReO_(x)/SiO_(2)

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Getting insights into gas-phase sulfation effect on catalytic performance of praseodymium oxides in NH_(3)-SCR of NO

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Journal of Rare Earths 2023年第6期41卷 952-958,I0005页

作者： Yandi Cai Peng Yang Qinglong Liu Kaili Ma Wenxin Ma Wang Song Qiuhui Qian Fei Gao Wei Tan Lin Dong State Key Laboratory of Pollution Control and Resource Reuse School of EnvironmentJiangsu Key Laboratory of Vehicle Emissions ControlCenter of Modern AnalysisKey Laboratory of Mesoscopic Chemistry of MOESchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China Analysis and Testing Center Southeast UniversityNanjing 211189China National and Local Joint Engineering Laboratory of Municipal Sewage Resource Utilization Technology School of Environmental Science and EngineeringSuzhou University of Science and TechnologySuzhou 215009China

Sulfation treatment has been widely used to promote the catalytic performance of ceria(CeO_(2))based catalysts for the selective catalytic reduction of NO by NH_(3)(NH_(3)-SCR of NO).Praseodymium oxide(PrO_(x)),another commonly used rare earth material with similar structural properties as CeO_(2),also shows satistactory redox properties due to the facile redox cycle of Pr^(3+)■Pr^(4+).In this work,gas phase sulfation treatment with varied duration was performed on PrO_(x) at 200℃,and the NH_(3)-SCR activity of sulfated PrO_(x) was *** on the results of systematic characterizations(e.g.,N_(2)-physisorption,NH_(3) oxidation,NO oxidation,in situ diffuse Fourier transform infrared spectroscopy),it is revealed that the catalytic performance of sulfated PrO_(x)is highly dependent on the sulfation time(or the amount of sulfate species deposited on PrO_(x)),which has a significant impact on the competitive reaction between NH_(3) oxidation and NH_(3)-SCR of NO,thus determining the NH_(3)-SCR activity of PrO_(x).This work provides new insight into tuning the interaction between PrO_(x) surface and reactants(NO,NH_(3))via sulfation treatment,which cam guide the design and application of PrO_(x)based catalysts for NH_(3)-SCR of NO in the future.

关键词： NH_(3)-SCR Praseodymium oxides Sulfation treatment Surface acidity NH_(3)oxidation Rare earths

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Experimental and theoretical investigation on degradation of dimethyl trisulfide by ultraviolet/peroxymonosulfate: Reaction mechanism and influencing factors

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Journal of Environmental Sciences 2023年第5期127卷 824-832页

作者： Jianing Sun Xiaodong Xin Shaohua Sun Zhenqi Du Zhenxing Yao Mingquan Wang Ruibao Jia Shandong Province Water Supply and Drainage Monitoring Center Jinan 250101China School of Water Conservancy and Environment University of JinanJinan 250022China State Key Laboratory of Pollution Control and Resource Reuse College of Environmental Science and EngineeringTongji UniversityShanghai 200092China

With a large amount of domestic sewage and industrial wastewater discharged into the water bodies,sulfur-containing organicmatter inwastewater produced volatile organic sulfide,such as dimethyl trisulfide(DMTS)throughmicroorganisms,caused the potential danger of drinking water safety and human *** present,there is still a lack of technology on the removal of *** this study,the ultraviolet/peroxymonosulfate(UV/PMS)advanced oxidation processes was used to explore the degradation of *** than 90%of DMTS(30μg/L)was removed under the conditions of the concentration ratio of DMTS to PMS was 3:40,the temperature(T)was 25±2℃,and 10 min of irradiation by a 200 W mercury lamp(365 nm).The kinetics rate constant k of DMTS reacting with hydroxyl radical(HO·)was determined to be 0.2477 min^(−1).Mn^(2+),Cu^(2+)and NO_(3)^(-)promoted the degradation of DMTS,whereas humic acid and Cl-in high concentrations inhibited the degradation *** chromatography-mass spectrometry was used to analyze the degradation products and the degradation intermediates were dimethyl disulfide and *** functional theory was used to predict the possible degradation mechanism according to the frontier orbital theory and the bond breaking mechanism of organic *** results showed that the S–S,C–S and C–H bonds in DMTS molecular structure were prone to fracture in the presence of free radicals,resulting in the formation of alkyl radicals and sulfur-containing radicals,which randomly combined to generate a variety of degradation products.

关键词： Ultraviolet/peroxymonosulfate Dimethyl trisulfide Products Density functional theory Degradation mechanism

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MSWNet:A visual deep machine learning method adopting transfer learning based upon ResNet 50 for municipal solid waste sorting

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Frontiers of Environmental Science & Engineering 2023年第6期17卷 165-176页

作者： Kunsen Lin Youcai Zhao Lina Wang Wenjie Shi Feifei Cui Tao Zhou The State Key Laboratory of Pollution Control and Resource Reuse College of Environmental Science and EngineeringTongji UniversityShanghai 200092China Shanghai Institute of Pollution Control and Ecological Security Shanghai 200092China Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention(LAP3) Department of Environmental Science and EngineeringFudan UniversityShanghai 200433China Institute of Eco-Chongming(IEC) Shanghai 202150China Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 610054China

An intelligent and efficient methodology is needed owning to the continuous increase of global municipal solid waste(MSW).This is because the common methods of manual and semi-mechanical screenings not only consume large amount of manpower and material resources but also accelerate virus community *** the categories of MSW are diverse considering their compositions,chemical reactions,and processing procedures,etc.,resulting in low efficiencies in MSW sorting using the traditional *** machine learning can help MSW sorting becoming into a smarter and more efficient *** study for the first time applied MSWNet in MSW sorting,a ResNet-50 with transfer *** method of cyclical learning rate was taken to avoid blind finding,and tests were repeated until accidentally encountering a good *** of visualization were also considered to make the MSWNet model more transparent and *** showed transfer learning enhanced the efficiency of training time(from 741 s to 598.5 s),and improved the accuracy of recognition performance(from 88.50%to 93.50%);MSWNet showed a better performance in MSW classsification in terms of sensitivity(93.50%),precision(93.40%),F1-score(93.40%),accuracy(93.50%)and AUC(92.00%).The findings of this study can be taken as a reference for building the model MSW classification by deep learning,quantifying a suitable learning rate,and changing the data from high dimensions to two dimensions.

关键词： Municipal solid waste sorting Deep residual network Transfer learning Cyclic learning rate Visualization

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MOF-based materials facilitate efficient anaerobic digestion of organic wastes:integrating substrate bioavailability and microbial syntrophism

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Frontiers of Environmental Science & Engineering 2024年第8期18卷 153-157页

作者： Haoyu Liu Ying Xu Xiang Chen Xiankai Wang Hang Wang Xiaohu Dai State Key Laboratory of Pollution Control and Resource Reuse School of Environmental Science and EngineeringTongji UniversityShanghai 200092China Shanghai Institute of Pollution Control and Ecological Security Shanghai 200092China YANGTZE Eco-Environment Engineering Research Center China Three Gorges CorporationWuhan 430010China National Engineering Research Center of Eco-Environment Protection for Yangtze River Economic Belt Wuhan 430010China

Anaerobic digestion(AD)of organic waste(OW)for methane production is generally *** of AD systems with traditional materials(e.g.,electroconductive materials)is a current focus of research and has been reported to assist methanogenesis by enhancing the productivity of microbial metabolism among syntrophic *** in the AD of organic wastewater,in which microbial cells come into direct contact with the dissolved substrate,in the complex multiphase AD system of OW,low substrate bioavailability is an inevitable obstacle to microbial syntrophism for ***,we propose that improving substrate bioavailability and microbial syntrophism is a powerful strategy for ensuring material-assisted efficient AD of *** on the above considerations,metal-organic frameworks(MOFs),with their exceptionally high porosity,outstanding multi-functionality,and tuneable structures,have excellent potential for application in multiphase anaerobic systems of OW to integrate substrate bioavailability and microbial syntrophism and drive efficient *** addition,MOFs with designable and tuneable natures have great potential for use in identifying suitable materials for anaerobic systems for different types of OW via machine-learning technologies,thereby effectively enhancing methanogenesis from ***,the sustainable application of MOFs in AD and the corresponding environmental risks warrant further investigation.

关键词： Anaerobic digestion Methane production Biodegradability Functional materials Metal-organic frameworks

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The simultaneous removal of methylene blue (MB) and Ca2+ by recyclable adsorbents based the scales derived from coal gasification system

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Environmental Science and pollution Research 2024年第22期31卷 32519-32537页

作者： An, Bai-Hong Xu, Da-Mao Wang, Run-Ting Wen, Ye-Xuan Geng, Rui Wu, Jia-Yun Tang, Xian-Chun Chen, Hong-Bin State Key Laboratory of Pollution Control and Resource Reuse College of Environmental Science and Engineering Tongji University Shanghai200092 China National Engineering Research Center for Urban Pollution Control Tongji University Shanghai200092 China Department of Materials Science Fudan University Shanghai200433 China Sinopec Ningbo Engineering Co. LTD Ningbo315103 China

The transformation of solid wastes from industrial production into effective adsorbents could significantly contribute to wastewater treatment. In this study, after acidizing and burning soft scale (SS) from coal gasification system, two magnetic adsorbents (mag-ASS and mag-BASS) were prepared via the combination of magnetite with ultrasonic, respectively. The treatment effects of mag-ASS and mag-BASS were then investigated for simulated wastewater containing macromolecular organic matter [i.e., methylene blue (MB)] and Ca2+. The results indicated that the pseudo second order kinetic, Elovich, Freundlich, Langmuir and Temkin model could well describe the adsorption behavior of MB and Ca2+ onto mag-ASS and mag-BASS. The maximum adsorption capacities of mag-ASS for MB and mag-BASS for Ca2+ were 600.53 mg/g and 102.54 mg/g, respectively. Surprisingly, the adsorption abilities of mag-ASS for MB and mag-BASS for Ca2+ show significantly higher than the others. The adsorption mechanisms of MB mainly included electrostatic interaction, π-π conjugate interaction and cation exchange, while those of Ca2+ were mainly electrostatic interaction and cation exchange. The diffusion of MB and Ca2+ onto the magnetic adsorbents might be controlled by the combined effects of intraparticle and liquid film diffusion. There was no significant reduction in adsorption capacity after 8 cycles of adsorption and desorption, indicating that SS-based magnetic adsorbents had good recyclability and stability. Moreover, the removal efficiency of mag-BASS for total hardness and total organic carbon in real coal gasification gray water (CGGW) was 82.60 and 64.10%, respectively. The treatment of CGGW and the resource of wastes would significantly promote the reasonable disposal of coal gasification scales. Graphical abstract: (Figure presented.) © The Author(s), under exclusive licence to Springer-Verlag GmbH Germany, part of Springer Nature 2024.

关键词： Metal ions

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Developing zirconium xerogel coagulants for deep removal of phosphorous

Environmental Surfaces and Interfaces

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Environmental Surfaces and Interfaces 2024年第1期2卷 66-74页

作者： Haoming Zhang Yonghai Gan Wenchang Zhang Shuangshuang Wei Shujuan Zhang State Key Laboratory of Pollution Control and Resource Reuse School of Environment Nanjing University 210023 China

Deep removal of phosphorous (P) from water is a necessary measure to solve the eutrophication problem. Coagulation is both a basic treatment method for P removal and an important pretreatment process for membrane filtration. However, few coagulants can meet the both requirements. Based on the analysis on the hydrolysis behaviors of some earth-abundant metals and the solubility products of their phosphates, a series of zirconium xerogel coagulants (ZXC) was fabricated with a novel approach (the sol-gel method) and was evaluated for the removal of both organic and inorganic P in coagulation and coagulation-ultrafiltration. In terms of P removal and anti-fouling of membrane, the resultant ZXC outperformed polyzirconium chloride (PZC), polyaluminum chloride (PAC), polyferric sulfate (PFS), as well as titanium xerogel coagulant (TXC) in a wide range of pH and dose. The rapid hydrolysis of Zr 4+ and the formation of Zr 3 (PO 4 ) 4 with a rather low solubility product are attributable to the great performance of ZXC in coagulation. This study highlights the potential of ZXC as an effective solution for enhancing the treatment of water and wastewater, particularly in achieving deep P removal and improving membrane fouling resistance, thereby contributing to more sustainable and efficient strategies for addressing eutrophication and pollutant removal.

关键词： Coagulation Phosphate Membrane fouling Turbidity Zirconium Sol-gel

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Synergistic enhancement of pollutant removal from high-salt wastewater using coagulation-flotation combined process

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Green Chemical Engineering 2025年第3期6卷 410-419页

作者： Li, Enze Dong, Jing Jia, Yongsheng Pan, Zihe Lv, Hongzhou Du, Zhiping Gao, Guandao Cheng, Fangqin Institute of Resources and Environmental Engineering State Environmental Protection Key Laboratory of Efficient Utilization Technology of Coal Waste Resources Shanxi Laboratory of Yellow River Shanxi University Taiyuan030006 China School of Environmental Science & Engineering Huazhong University of Science and Technology Wuhan430074 China State Key Laboratory of Pollution Control and Resource Reuse School of Environment Nanjing University Nanjing210023 China

Sufficient treatment of industrial organic wastewater with high salt and large amounts of suspended particulate matter remains a challenge worldwide. In this work, a novel coagulation-flotation combined process was developed to treat the suspended particles as well as significantly reduce organic pollutants content in the actual high-salt organic wastewater. Four typical inorganic and organic flocculants (poly aluminum chloride (PAC), poly ferric sulfate (PFS), polyacrylamide (PAM), and modified cationic starch (CS)) were selected for compounding to obtain an optimized flocculation system for high-salt wastewater. The results showed that the PAC-PAM with a 10:1 ratio in mass exhibited the best coagulation behaviors with the removal efficiency of turbidity and chemical oxygen demand (COD) being 95.33% and 9.21%, respectively, under the optimal operation conditions, and the sedimentation process of coagulant conformed to the quasi-second-order kinetics. The PAC-PAM flocs exhibited stronger netting, sweeping, and adsorption bridging capabilities, which were conducive to removing suspended particles. When the flotation was conducted after coagulation, the COD decreased significantly by 20.82%. In addition, this combined process could reduce the treatment time by 50% compared to the process with only coagulation treatment. During the flotation process, floc particles companies with hydrophobic polycyclic aromatic hydrocarbons could collide and adhere to microbubbles and be floated to the surface, resulting in an effective reduction of COD. This work could provide a novel strategy and step forward to design and optimize the pretreatment process engineering for organic high-salt wastewater. © 2024 Institute of Process Engineering, Chinese Academy of Sciences.

关键词： Coagulation

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Metal-free diatomaceous carbon-based catalyst for ultrafast and anti-interference Fenton-like oxidation

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Chinese Chemical Letters 2024年第12期35卷 351-355页

作者： Kexin Yin Jingren Yang Yanwei Li Qian Li Xing Xu Shandong Key Laboratory of Water Pollution Control and Resource Reuse School of Environmental Science and EngineeringShandong UniversityQingdao 266237China Environment Research Institute Shandong UniversityQingdao 266237China State Environmental Protection Key Laboratory of Environmental Health Impact Assessment of Emerging Contaminants Shanghai Academy of Environmental SciencesShanghai 200233China

Herein,a diatomite biomorphic Si-O doped carbon-based catalyst(DB-SiOC)was prepared using natura mineral diatomite as the silicon source and porous *** results showed that the metal-free DB SiOC catalyst exhibited ultrafast oxidation towards chlorophenol(CP)via peroxymonosulfate(PMS)activa tion,which was almost one order of magnitudes than most of carbon-based *** DB-SiOC/PMS system also showed the high ability to resist the interference of environmental *** radicals(^(·)OH and SO_(4)^(·–))exhibited a very small contribution to the CP oxidation while the electron transfer processe(ETP)played the major role in the DB-SiOC/PMS *** electron shuttles from the electron-donating CP molecules to the adjacent DB-SiOC/PMS^(*)could be efficiently triggered via Si-O bonds as bridges,mak ing it possible for ultrafast oxidation of *** addition,the hollow-disc shaped DB-Si OC provided the biomorphic DE structures with abundant pores for enriching the PMS and pollutants,thus further ac celerating the oxidation *** work provided a new routine for the fabrication of Si-O doped carbon-based catalysts with excellent Fenton-like catalytic activity,which would greatly promote thei application prospects in Fenton-like systems.

关键词： Peroxymonosulfate Diatomite Si-O doping Fenton-like reaction Electron transfer process(ETP)

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Material flow analysis and global warming potential assessment of an industrial insect-based bioconversion plant using housefly larvae

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Journal of Environmental Sciences 2024年第5期139卷 483-495页

作者： Tao Lu Fan Lü Nanlin Liao Honghui Chai Hua Zhang Pinjing He Institute of Waste Treatment and Reclamation Tongji UniversityShanghai 200092China State Key Laboratory of Pollution Control and Source Reuse Tongji UniversityShanghai 200092China Zhejiang Qihe Ecological Technology Co. Ltd.Hangzhou 310052China

The significant increase in the demand for biomass waste treatment after garbage classification has led to housefly larvae treatment becoming an attractive treatment *** can provide a source of protein while treating biomass waste,which means that nutrients can be returned to the natural food ***,the performance of this technology in terms of its environmental impacts is still unclear,particularly with regards to global warming potential(GWP).This study used a life cycle assessment(LCA)approach to assess a housefly larvae treatment plant with a treatment capacity of 50 tons of biomass waste per *** LCA results showed that the 95% confidence intervals for the GWP in summer and winter were determined to be 24.46-32.81 kg CO_(2) equivalent(CO_(2)-eq)/ton biomass waste and5.37-10.08 kg CO_(2)-eq/ton biomass waste,*** greater GWP value in summer is due to the longer ventilation time and higher ventilation intensity in summer,which consumes more *** main GWP contributions are from(1)electricity needs(accounting for 78.6% of emissions in summer and 70.2%in winter)and(2)product substitution by mature housefly larvae and compost(both summer and winter accounting for 96.8% of carbon reduction).

关键词： Biomass waste Musca domestica Housefly larvae Life cycle assessment Global warming potential

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