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Enhanced hydrolytic removal of tylosin in wastewater using polymer-based solid acid catalysts converted from polystyrene

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Journal of Environmental Sciences 2023年第4期126卷 287-296页

作者： Shiling Li Shuhan Sun Fei Qi Xiaomin Dou Beijing Key Lab for source control Technology of water pollution College of Environmental Science and EngineeringBeijing Forestry UniversityBeijing 100083China Engineering Research Center for Water Pollution Source Control and Eco-remediation College of Environmental Science and EngineeringBeijing Forestry UniversityBeijing 100083China

Antibiotic production wastewater usually contains high concentrations of antibiotic residues,which can cause instability and deterioration of biological wastewater treatment units and also domestication and proliferation of antibiotic-resistance bacteria.An effective pretreatment on antibiotics production wastewater is expected to selectively reduce the concentration of antibiotics and decrease the toxicity,rather than mitigate organic and other contaminants before further treatments.In this work,two polymer-based solid acids,PS-S and CPS-S bearing high concentrations of-SOH_(3)groups (up to 4.57 mmol/g),were prepared and successfully used for hydrolytic mitigation of 100 mg/L tylosin within 20 min.The co-existence of high concentrations of COD and humic substances did not affect the mitigation of tylosin obviously,while more than 500 mg/L of nitrogenous compounds suppressed the hydrolytic efficiency.Recycle and reuse experiments showed that the solid acids performed well in five cycles after regeneration.Three transformation products (P1,P2 and P3)were identified using UPLC-QTOF-MS/MS.Sugar moieties including mycarse,mycaminose,and mycinose detached and released simultaneously or in order from the 16-member lactone ring through desugarization,which led to a dramatic decrease in antibacterial activity as revealed by cytotoxicity evaluations using S.aureus.ecotoxicity estimation indicated the acute toxicities of the hydrolyzed products to model species (e.g.,fish,daphnid and green algae) were classified as“not harmful”.This work suggested an effective and selective method to pretreat tylosin-contained production wastewater by using polymer-based solid acids.These results will shed light on effective elimination of antibiotics pollution from pharmaceutical industries through strengthening the pretreatments.

关键词： Polymer Sulfonation Solid acid catalysts Tylosin hydrolysis Antibiotic

Boosting oxygen vacancies by modulating the morphology of Au decorated In_(2)O_(3)with enhanced CO_(2)hydrogenation activity to CH_(3)OH

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Journal of Environmental Sciences 2024年第6期140卷 91-102页

作者： Ruxian Hou Jiewen Xiao Qian Wu Tianyu Zhang Qiang Wang Beijing Key Lab for source control Technology of water pollution College of Environmental Science and EngineeringBeijing Forestry UniversityBeijing 100083China engineering research center for water pollution source control&eco-remediation College of Environmental Science and EngineeringBeijing Forestry UniversityBeijing 100083China

CO_(2)hydrogenation to methanol has become one of the most promising ways for CO_(2)utilization,however,the CO_(2)conversion rate and methanol selectivity of this reaction still need to be improved for industrial application.Here we investigated the structure-activity relationship for CO_(2)conversion to methanol of In_(2)O_(3)-based catalysts by modulating morphology and decorating Au.Three different Au/In_(2)O_(3)catalysts were prepared,their activity follow the sequence of Au/In_(2)O_(3)-nanosphere(Au/In_(2)O_(3)-NS)>Au/In_(2)O_(3)-nanoplate(Au/In_(2)O_(3)-NP)>Au/In_(2)O_(3)-hollow microsphere(Au/In_(2)O_(3)-HM).Au/In_(2)O_(3)-NS exhibited the best performance with good CO_(2)conversion of 12.7%,high methanol selectivity of 59.8%,and large space time yield of 0.32 g CH_(3)OH/(hr·gcat)at 300℃.The high performance of Au/In_(2)O_(3)-NS was considered as the presence of Au.It contributes to the creation of more surface oxygen vacancies,which further promoted the CO_(2)adsorption and facilitated CO_(2)activation to form the formate intermediates towards methanol.This work clearly suggests that the activity of In_(2)O_(3)catalyst can be effective enhanced by structure engineering and Au decorating.

关键词： CO_(2)hydrogenation Methanol Au/In_(2)O_(3) Morphology Oxygen vacancies

Surface modification of Cu_(2)O with stabilized Cu^(+) for highly efficient and stable CO_(2) electroreduction to C_(2+) chemicals

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Journal of Energy Chemistry 2023年第9期84卷 277-285页

作者： Ziyu Zhou Shuyu Liang Jiewen Xiao Tianyu Zhang Min Li Wenfu Xie Qiang Wang Beijing Key Lab for source control Technology of water pollution College of Environmental Science and EngineeringBeijing Forestry UniversityBeijing 100083China engineering research center for water pollution source control&eco-remediation College of Environmental Science and EngineeringBeijing Forestry UniversityBeijing 100083China

Copper(Cu)-based materials are known as the most attractive catalysts for electrochemical carbon dioxide reduction reaction(CO_(2)RR),especially the Cu^(+) species(e.g.,Cu_(2)O),which show excellent capability for catalyzing CO_(2) to C_(2+) chemicals because of their unique electronic structure.However,the active Cu^(+) species are prone to be reduced to metallic Cu under an electroreduction environment,thus resulting in fast deactivation and poor selectivity.Here,we developed an advanced surface modification strategy to maintain the active Cu^(+) species via assembling a protective layer of metal-organic framework(copper benzenetricarboxylate,CuBTC) on the surface of Cu_(2)O octahedron(Cu_(2)O@CuBTC).It's encouraging to see that the Cu_(2)O@CuBTC heterostructure outperforms the bare Cu_(2)O octahedron in catalyzing CO_(2) to C_(2+) chemicals and dramatically enhances the ratio of C_(2)H_(4)/CH_(4) products.A systematic study reveals that the introduced CuBTC shell plays a critical role in maintaining the active Cu^(+) species in Cu_(2)O@CuBTC heterostructure under reductive conditions.This work offers a practical strategy for improving the catalytic performance of CO_(2)RR over copper oxides and also establishes a route to maintain the state of valence-sensitive catalysts.

关键词： CO_(2)RR Copper Oxide Metal-organic Framework Core-shell Structure C_(2+)Chemicals

Characteristics of typical dissolved black carbons and their influence on the formation of disinfection by-products in chlor(am)ination

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Frontiers of Environmental Science & engineering 2022年第12期16卷 1-14页

作者： Jinhui Liang Peng Gao Benhang Li Longfei Kang Li Feng Qi Han Yongze Liu Liqiu Zhang Beijing Key Laboratory for source control Technology of water pollution Engineering Research Center for Water Pollution Source Control and Eco-remediationBeijing Forestry UniversityBeijing100083China

Dissolved black carbon(DBC)released from biochar can be one of the potential disinfection by-products(DBPs)precursors in the dissolved organic matter pool.However,the physiochemical and structural properties of DBC and the effects on the development of DBPs and DBP formation potential(DBPFP)during the disinfection process remain unclear.In this study,the characteristics of two kinds of DBC,namely,animal-derived DBC(poultry litter DBC,PL-DBC)and plant-derived DBC(wheat straw DBC,WS-DBC),were investigated.The effects of different kinds of DBC on the evolution of DBPs and DBPFP in chlorine and chloramine disinfection processes were compared with natural organic matter(NOM).The results showed that the total DBPs concentrations derived from PL-DBC,WS-DBC and NOM were similar during chlorination(i.e.,61.23µg/L,64.59µg/L and 64.66µg/L,respectively)and chloramination(i.e.,44.63µg/L,44.42µg/L and 45.58µg/L,respectively).The lower total DBPs and DBPFP concentrations in chloramination could be attributed to the fact that the introduction of ammonia in chloramine inhibited the breaking of the bond between the disinfectant and the active group of the precursor.Additionally,DBC presented much lower total DBPFP concentrations than NOM in both chlorination and chloramination.However,both kinds of DBC tended to form more monochloroacetic acids and haloacetamides than NOM,which could result from the higher organic strength,higher protein matter,and nitrogen-rich soluble microbial products of DBC.

关键词： Dissolved black carbon(DBC) Chlorine Chloramine Disinfection by-products(DBPs) Disinfection by-products formation potential(DBPFP)

Removal efficiencies of natural and synthetic progesterones in hospital wastewater treated by different disinfection processes

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Frontiers of Environmental Science & engineering 2022年第10期16卷 11-22页

作者： Jinhui Liang Yuchen Luo Benhang Li Shiqi Liu Liansheng Yang Peng Gao Li Feng Yongze Liu Ziwen Du Liqiu Zhang Beijing Key Laboratory for source control Technology of water pollution Engineering Research Center for Water Pollution Source Control and Eco-remediationBeijing Forestry UniversityBeijing 100083China

Progesterones are ubiquitous in hospital wastewater(HWW)with concentrations much higher than those of estrogens and androgens.To ensure that these water systems are safe to use,disinfection is crucial during HWW treatment by providing"front line"defense against biological contaminations.Here,five disinfection processes,namely,chlorine(Cl_(2)),chlorine dioxide(ClO_(2)),ozone(O_(3)),ultraviolet(UV)),and UV/chlorine(UV/Cl_(2)),were selected to investigate their removal efficiencies for progesterones in primary filtration and secondary biological treatment effluents.There were 61 natural and synthetic progesterones detected in HWW,with the natural progesterones being the main components with a concentration of 845.51 ng/L and contributing to 75.08%of the total proge-sterones.The primary filtration treatment presented insignificant removal effects on the progesterones,while the secondary biological treatment significantly reduced the progesterone content by biode-gradation.The order of removal efficiencies of total progesterones by different disinfection processes was UV/Cl_(2)>Cl_(2)>O_(3)>ClO_(2)>UV.UV/Cl_(2)showed the highest removal efficiency against progesterones mainly due to the activation of Cl_(2)by ultraviolet(UV)photolysis,which helps open the heterocyclic,aromatic,and phenolic rings,thus accelerating progesterone degradation.In addition,the removal efficiencies of natural progesterones in the five disinfection processes were higher than those of synthetic progesterones(progesterone derivatives,19-nortestosterone derivatives,and 17α-hydroxyprogesterone derivatives).

关键词： Progesterones Hospital wastewater Primary filtration treatment effluent Secondary biological treatment effluent Disinfection process

Occurrence and migration of microplastics and plasticizers in different wastewater and sludge treatment units in municipal wastewater treatment plant

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Frontiers of Environmental Science & engineering 2022年第11期16卷 203-212页

作者： Sen Dong Peng Gao Benhang Li Li Feng Yongze Liu Ziwen Du Liqiu Zhang Beijing Key Laboratory for source control Technology of water pollution Engineering Research Center for Water Pollution Source Control and Eco-remediationBeijing Forestry UniversityBeijing 100083China

Microplastics(MPs)and plasticizers,such as phthalate esters(PAEs),were frequently detected in municipal wastewater treatment plants(MWTP).Previous research mainly studied the removal of MPs and PAEs in wastewater.However,the occurrence of MPs and PAEs in the sludge was generally ignored.To comprehensively investigate the occurrence and the migration behaviors of MPs and PAEs in MWTP,a series of representative parameters including the number,size,color,shape of MPs,and the concentrations of PAEs in wastewater and sludge were systematically investigated.In this study,the concentrations of MPs in the influent and effluent were 15.46±0.37 and 0.30±0.14 particles/L.The MP removal efficiency of 98.1%was achieved and about 73.8%of MPs were accumulated in the sludge in the MWTP.The numbers of MPs in the sludge before and after digestion were 4.40±0.14 and 0.31±0.01 particles/g(dry sludge),respectively.Fourier Transform Infrared Spectroscopy(ATR FT-IR)analysis showed that the main types of MPs were polyethylene terephthalate(PET),polypropylene(PP),polyethylene(PE),and polystyrene(PS).Six PAEs,including phthalate(DMP),diethyl phthalate(DEP),diisobutyl phthalate(DIBP),ortho dibutyl phthalate(DBP),butyl benzyl phthalate(BBP),and bis(2-ethyl)hexyl phthalate(DEHP),were detected in the MWTP.The concentrations of total PAEs(ΣPAEs)in the influent and effluent were 76.66 and 6.28μg/L,respectively.The concentrations ofΣPAEs in the sludge before and after digestion were 152.64 and 31.70μg/g,respectively.In the process of thermal hydrolysis,the number and size of MPs decreased accompanied by the increase of the plasticizer concentration.

关键词： Microplastics Municipal wastewater treatment plant Phthalate esters Thermal hydrolysis

controllable synthesis of MnO_(2)/iron mesh monolithic catalyst and its significant enhancement for toluene oxidation

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Chinese Chemical Letters 2023年第2期34卷 338-341页

作者： Meijuan Qi Zhe Li Zhang Zhang Yanshan Gao Qiang Wang Beijing Key Lab for source control Technology of water pollution College of Environmental Science and EngineeringBeijing Forestry UniversityBeijing 100083China engineering research center for water pollution source control&eco-remediation College of Environmental Science and EngineeringBeijing Forestry UniversityBeijing 100083China Beijing Municipal ecological and Environmental Monitoring center Beijing 100048China

A series of monolithic MnO_(2)/iron mesh (IM) catalysts for oxidation of toluene were successfully prepared by using in situ hydrothermal growth.MnO_(2)can grow firmly on the IM substrates surface with a shedding rate of only 0.14%.Due to the highest O_(ads) and high-valent Mn^(4+) and Fe^(3+) elements,the temperature at 50% and 90% toluene conversion (T_(50%) and T_(90%)) was 252 and 265℃,respectively for the best performance catalyst (hydrothermal temperature of 80℃,hydrothermal time of 12 h,and precursor manganese ion concentration of 0.03 mol/L).The catalysts also presented good water resistance and cycle performance.In-situ DRIFTS results suggesting that toluene was first rapid transformed into the reaction intermediate species (benzoate species) and then converted to CO_(2)and H_(2)O.Therefore,this work provides a new direction for the research and application of IM-based monolithic catalysts.

关键词： Toluene oxidation Iron mesh monoliths catalysts MnO_(2) Resistance properties Reaction mechanism

Effect of allelochemicals sustained-release microspheres on the ingestion, incorporation, and digestion abilities of Daphnia magna Straus

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Journal of Environmental Sciences 2023年第2期124卷 205-214页

作者： Benhang Li Yijun Yin Xiaohong Zhou Li Feng Yongze Liu Ziwen Du Yajun Tian Liqiu Zhang Beijing Key Laboratory for source control Technology of water pollution Engineering Research Center for Water Pollution Source Control and EcoremediationBeijing Forestry UniversityBeijing 100083China College of Environment Zhejiang University of TechnologyHangzhou 310014China

Allelochemicals sustained-release microspheres(ACs-SMs)exhibited great inhibition effect on algae,however,few studies have focused on ACs-SMs toxicity on invertebrate.In this study,the effects of single high-concentration ACs(15 mg/L,SH-ACs),repeated lowconcentration ACs(3×5 mg/L,RL-ACs)and ACs-SMs containing 15 mg/L ACs exposure on the ingestion,incorporation,and digestion of Daphniamagna Straus(DS)were investigated by stable isotope 15N labeling method.Meanwhile,the diversity and abundance of microflora in DS guts were determined by 16S rRNA genes and cloning methods.The results showed that SH-ACs exposure caused 50%and 33.3%death rates for newborn and adult DS,while RL-ACs exposure caused 10%death rate for newborn DS and no obvious effect on the activity of adult DS.And ACs-SMs exposure did not diminish the motility of both newborn and adult DS,indicating the lower acute toxicity of ACs-SMs.Furthermore,SH-ACs inhibited the ingestion(-6.45%),incorporation(-47.1%)and digestion(-53.8%)abilities of DS and reduced the microbial abundance(-27.7%)in DS guts.Compared with SH-ACs,RL-ACs showed relatively low impact on the ingestion(-3.23%),incorporation(-5.89%)and digestion(-23.9%)abilities of DS.Interestingly,ACs-SMs enhanced the ingestion(+9.68%),incorporation(+52.9%)and digestion(+51.3%)abilities of DS and increased the microbial abundance(+10.7%)in DS guts.Overall ACs and ACs-SMs reduced the diversity of microflora in DS guts.In conclusion,ACs-SMs can release ACs sustainably and prolong the sustained release time,which not only effectively reduce the toxicity of ACs,but also had positive effects on DS.

关键词： Allelochemicals(ACs) Sustained-release microspheres (SMs) Daphnia magna Straus(DS)

Pre-combustion mercury removal with co-production of hydrogen via coal electrolysis

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Journal of Environmental Sciences 2024年第2期136卷 382-389页

作者： Xiang Lyu Runming Tao Tianyu Zhang Chemical and Biomolecular engineering Department Ohio University165 Stocker CenterAthensOH45701USA Electrification and Energy Infrastructures Division Oak Ridge National LaboratoryOak RidgeTN37831USA Beijing Key Lab for source control Technology of water pollution College of Environmental Science and EngineeringBeijing Forestry UniversityBeijing 100083China engineering research center for water pollution source control&eco-remediation College of Environmental Science and EngineeringBeijing Forestry UniversityBeijing 100083China

Pre-combustion mercury removal via coal electrolysis was performed and investigated on a bench-scale coal electrolytic cell(CEC)systemically,and factorial design was used to determine the effect of different operating conditions(coal particle size,operating temperature,operating cell voltage,and flow rate of slurry)on the percentage of mercury removal,percentage of ash removal,and dry heating value change.The results showed that the operating cell voltage,as well as the interaction between operating cell voltage and coal particle size,are significant factors in the percentage of mercury removal.There is no significant factor in the percentage of ash removal and the dry heating value change,but the coal could be purified while keeping the dry heating value almost constant after electrolysis.A co-product of hydrogen could be produced during coal electrolysis with 50%lower energy consumption compared with water electrolysis.Meanwhile,a mechanism for mercury removal in coal was proposed.The facts indicate that coal electrolysis is a promising method for precombustion mercury removal.

关键词： Pre-combustion mercury removal Coal electrolysis Ash removal Dry heating value Hydrogen production