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Mechanistic insights to sorptive removal of four sulfonamide antibiotics from water using magnetite-functionalized biochar

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Biochar 2023年第1期5卷 1377-1388页

作者： Shanshan Bai Yaolu Zhou Mingrong Qian Jun Xia Zhiqiang Sun Yujiao Wang Xiaochen Huang Shishu Zhu Key Laboratory of Pollution Exposure and Health Intervention of Zhejiang Province Interdisciplinary Research AcademyZhejiang Shuren UniversityHangzhou 310015People’s Republic of China State Key Laboratory of Urban Water Resource and Environment School of EnvironmentHarbin Institute of TechnologyHarbin 150090People’s Republic of China State Key Lab of Biocontrol Guangdong Provincial Key Laboratory of Plant ResourcesSchool of AgricultureShenzhen Campus of Sun Yat-Sen UniversityShenzhen 518107People’s Republic of China The Key Lab of Pollution Control and Ecosystem Restoration in Industry Clusters Ministry of EducationSchool of Environment and EnergySouth China University of TechnologyGuangzhou 510006People’s Republic of China

Magnetite-functionalized biochar(MBC)is a promising engineered material for remediation of antibiotic-contaminated ***,sorption mechanisms of ionizable organic compounds such as sulfonamide antibiotics(SAs)on MBC are still *** study employed four representative SAs including sulfamethazine(SMT),sulfamerazine(SMR),sulfadiazine(SDZ),and sulfamethoxazole(SMX),to compare the difference in sorption on *** showed that the sorption capacities and affinities of the four SAs varied with their substituents,hydrophobic properties,and dissociation constants(pKa).Synergistic effect during co-pyrolysis with Fe^(3+)enhanced the sorption performance of MBC towards SAs compared to original *** methods confirmed structural changes of MBC such as the variance in oxygen-containing groups and defective/graphitized *** of modeling pH-dependent sorption revealed that H-bonding orπ-bond assisted H-bonding determined the sorption affinities and capacities of *** particular,the SAs with lower pKa were thermodynamically favorable to form H-bonding with MBC via proton exchange with water *** calculation results quantified the contributions of H-bonding strengths and found that the energies of H-bonding were correlated with affinities of ***,contributions of oxygencontaining groups instead of minerals dominated the H-bonding *** insights from this study can be valuable in exploring engineered BC composites for practical application in field remediation.

关键词： Biochar Antibiotics Sorption capacity Synergistic effect Quantum calculation

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Boosting C_(2)H_(6)/C_(2)H_(4) separation via the precise electrostatic modulation of synthetic 1D channel at atomic level

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Nano Research 2024年第11期17卷 10083-10087页

作者： Salamanti Ainiwaner Hengcong Huang Jia-Jia Zheng Fengting Li Xue-Tong Yang Yang-Yang Guo Fangli Yuan Ming-Shui Yao Yifan Gu College of Environmental Science and Engineering State Key Laboratory of Pollution Control and Resource Reuse Tongji University Shanghai 200092 China Laboratory of Theoretical and Computational Nanoscience National Center for Nanoscience and Technology Chinese Academy of Sciences Beijing 100190 China Skate Key Laboratory of Mesoscience and Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 China Chinese Academy of Sciences University of Chinese Academy of Sciences Beijing 100049 China

The regulation of gas sorption via simple pore modification is crucial to molecular recognition and chemical ***,a rational pore surface electrostatic modulation in synthetic one dimensioned(1-D)channel is demonstrated to boost ethane/ethylene(C_(2)H_(6)/C_(2)H_(4))selectivity for one-step extraction of C_(2)H_(4) from C_(2)H_(6)/C_(2)H_(4) *** the precise modulation of the surface charge arrangement with negatively charged moieties in the 1-D channel of a metal—organic framework(MOF),enhanced C_(2)H_(6)—host framework and decreased C_(2)H_(4)—host framework electrostatic interactions were obtained,which resulted in an obvious improvement in adsorption ***,the breakthrough separation performance rendered the obtained MOF an efficient adsorbent for C_(2)H_(4) purification from C_(2)H_(6)/C_(2)H_(4) *** combined detail theoretical studies prove that the gas sorption selectivity is remarkably sensitive to framework electrostatic change even in the case of pore surface modification at the atomic *** results are of fundamental importance to the design of porous materials for challenging separation tasks.

关键词： metal—organic framework ethane/ethylene separation ethane—selective MOF adsorption electrostatic modulation

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Efficient reduction and adsorption of Cr(Ⅵ)using FeCl_(3)-modified biochar:Synergistic roles of persistent free radicals and Fe(Ⅱ)

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Journal of environmental Sciences 2024年第3期137卷 626-638页

作者： Shujie Hu Chengshuai Liu Hongling Bu Manjia Chen Ying-heng Fei National-Regional Joint Engineering Research Center for Soil Pollution Control and Remediation in South China Guangdong Key Laboratory of Integrated Agro-environmental Pollution Control and ManagementInstitute of Eco-environmental and Soil SciencesGuangdong Academy of SciencesGuangzhou 510650China State Key Laboratory of Environmental Geochemistry Institute of GeochemistryChinese Academy of ScienceGuiyang 550081China School of Environment Science and Engineering Guangzhou UniversityGuangzhou 510006China College of Resources and Environment Chongqing SchoolUniversity of Chinese Academy of SciencesChongqing 400714China School of Environmental Science and Engineering Guangdong University of TechnologyGuangzhou 510006China

Transition metal iron and persistent free radicals(PFRs)both affect the redox properties of biochar,but the electron transfer relationship between them and the coupling reduction mechanism of Cr(Ⅵ)requires further *** untangle the interplay between iron and PFRs in biochar and the infuences on redox properties,FeCl_(3)-modified rice husk biochar(FBCs)was prepared and its reduction mechanism for Cr(Ⅵ)without light was *** FBCs had higher surface positive charges,oxygen-containing functional groups,and PFRs compared with pristine rice husk biochar(BC).Phenoxyl PFRs with high electrondonating capability formed in *** pronounced electron paramagnetic resonance signals showed that the PFRs preferred to form at lower Fe(Ⅲ)*** a high concentration of Fe(Ⅲ)would be reduced to Fe(Ⅱ)and consumed the formed *** kinetics and X-ray photoelectron spectroscopy analysis indicated that the FBCs effectively enhanced the Cr(Ⅵ)removal efficiency by 1.54-8.20 fold and the Cr(Ⅵ)reduction efficiency by 1.88-9.29 fold compared to those of *** quenching and competitive reductant addition experiments revealed that the higher Cr(Ⅵ)reduction performance of FBCs was mainly attributed to the formed PFRs,which could contribute to~74.0%of Cr(Ⅵ)reduction by direct or indirect electron *** PFRs on FBCs surfaces could promote the Fe(Ⅲ)/Fe(Ⅱ)cycle through single electron transfer and synergistically accelerate~52.3%of Cr(Ⅵ)*** study provides an improved understanding of the reduction mechanism of iron-modified biochar PFRs on Cr(Ⅵ)in environments.

关键词： Biochar Iron-modification Cr(Ⅵ) Electron transfer Reduction mechanism

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Quantitative structure-activity relationship in the photodegradation of azo dyes

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Journal of environmental Sciences 2020年第4期32卷 41-50页

作者： Guoyang Zhang Shujuan Zhang State Key Laboratory of Pollution Control and Resource Reuse School of the EnvironmentNanjing UniversityNanjing 210023China

The photolysis characteristics of azo dyes are critically important in environmental pollution control,dye-sensitized solar cells,and dyeing-related ***,there is still lack of quantitative relationship between the structures of azo dyes and their photolysis *** address this issue,the photolysis of 22 azo dyes were conducted side by side at three pH(4.0,6.0,9.0).The obtained pseudo-first order photodegradation rate constants(k1)were processed with ***,the hydrazone tautomer had a smaller excitation energy and was easier to undergo photolysis than the azo *** ortho-substituted sulfonate groups had an obvious protective effect on the photo stability of azo *** softness(s),the most positive and negative partial charge on a carbon atom(qC+,qC-)were found to be crucial descriptors in the establishment of QSAR models for the photo stability of azo *** QSAR model at pH 9.0 was robust for predicting the photo stability of azo dyes under UV irradiation.N2-purging experiments and quantum chemical computation verified that the cleavage of azo bond was not a result of direct photolysis but was caused by the attack of photoinduced reactive oxygen *** results here are helpful for the design of more stable azo dyes or the selection of suitable approaches for the treatment of dyecontaminated water bodies.

关键词： Azo Hydrazone Photolysis QSAR Softness

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Mxene-Supported Mil-88a(Fe) as Persulfate Activator for Removal of Tetracycline

SSRN

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SSRN 2023年

作者： Chen, Junxia Li, Weigang Yang, Zhenzhen Yang, Yuying Zhou, Qing State Key Laboratory of Pollution Control and Resource Reuse School of Environment Nanjing University Nanjing210023 China

The poor conductivity，poor stability and agglomeration in water of MIL-88A(Fe) limit its application as persulfate (PS) activator in water purification. Herein, MXene-supported MIL-88A(Fe) composites(M88A/KMX) were synthe-sized to enhance its adsorption and catalytic capability for tetracycline (TC) removal. M88A/KMX-0.2 composites exhibits optimal degradation efficiency，reaching 98% under conditions of 0.2 g/L M88A/KMX-0.2, 1.0 mM PS, 20 ppm TC, and pH 5. The degradation rate constants of M88A/KMX-0.2 was 0.03217 min-1, which was much higher than that of MIL-88A (0.00159 min-1) and MXene (0.00626 min-1). The removal effects of reaction parameters, such as dosage of M88A/KMX-0.2 and PS, initial solution pH and the presence of the common co-existing constituents (humic acid and the inorganic anions) were investi-gated in detail. Additionally, the reuse of M88A/KMX-0.2 showed that the com-posites had good cycling stability. The results of electron paramagnetic reso-nance (EPR) and quenching experiments indicated that ·OH , ·SO4- and·O2- were involved in the M88A/KMX-0.2/PS system. This study offered a new avenue for sulfate-based degradation of Fe-based metal organic frame-work. © 2023, The Authors. All rights reserved.

关键词： Degradation

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Catalytic urea hydrolysis by composite metal oxide catalyst towards efficient urea-based SCR process:performance evaluation and mechanism investigation

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Frontiers of environmental Science & Engineering 2023年第5期17卷 67-80页

作者： Yuchen Li Zhen Chen Xiangyu Zhang Kun Yang Lidong Wang Junhua Li MOE Key Laboratory of Resources and Environmental Systems Optimization Department of Environmental Science and EngineeringNorth China Electric Power UniversityBeijing 102206China State Key Joint Laboratory of Environment Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China Xi’an Thermal Power Research Institute Co. Xi’an 710032China

As a promising option to provide gaseous NH_(3) for SCR system,catalytic urea hydrolysis has aroused great attention,and improving surface area and activity of catalysis are the crucial issues to be solved for efficient urea ***,a composite metal oxide(TiO_(2)@Al_(2)O_(3))catalyst was prepared by a simple hydrothermal method,with mesoporous alumina(γ-Al_(2)O_(3))as *** results verify the mesoporous structure and submicron cluster of TiO_(2)@Al_(2)O_(3),with exposed crystal faces of(101)and(400)for TiO_(2)andγ-Al_(2)O_(3),*** electronegativity difference of Ti4+and Al3+changes the charge distribution scheme around the interface,which provides abundant acid/base sites to boost the urea ***,for an optimal proportioning with nano TiO_(2)content at 10 wt.%,the hydrolysis efficiency can reach up to 35.2%at 100℃ in 2 h,increasing by~7.1%than that of the blank experiment.^(13)C NMR spectrum measurements provide the impossible intermediate species during urea *** calculations are performed to clarify the efficient H_(2)O decomposition at the interface of TiO_(2)@Al_(2)O_(3).The result offers a favorable technology for energy-efficiency urea hydrolysis.

关键词： SCR Urea hydrolysis Catalytic Water dissociation Electronegativity

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Comparison of the Arsenic Protective Effects of Four Nanomaterials on Pakchoi in an Alkaline Soil

SSRN

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SSRN 2023年

作者： Wang, Yaoyao Chen, Wanli Gu, Xueyuan Zhou, Dongmei State Key Laboratory of Pollution Control and Resource Reuse School of Environment Nanjing University Nanjing210023 China

Accurately applying engineering nanoparticles (NPs) in farmland stress management is important for sustainable agriculture and food safety. The protective effects of four engineered NPs (SiO2, CeO2, ZnO, and S) on pakchoi under arsenic (As) stress were investigated using pot experiments. The results showed that CeO2, SiO2, and S NPs resulted in biomass reduction, while ZnO NPs (100 and 500 mg kg-1) significantly increased shoot height. Although 500 mg kg-1 S NPs rapidly dissolved to release SO42-, reducing soil pH and pore water As content and further reducing shoot As content by 21.6%, the growth phenotype was inferior to that obtained with 100 mg kg-1 ZnO NPs, probably due to acid damage. The addition of 100 mg kg-1 ZnO NPs not only significantly reduced the total As content in pakchoi by 23.9% compared to the As-alone treatment but also enhanced plant antioxidative activity by increasing superoxide dismutase and peroxidase activities and decreasing malondialdehyde content. ZnO NPs in soil might inhibit As uptake by roots by increasing the dissolved organic carbon (DOC) in pore water. According to the DLVO theory, ZnO NPs were the most effective in preventing As in pore water from entering plant roots due to their smaller hydrated particle size. Redundancy analysis further confirmed that DOC and SO42- were the primary factors controlling plant As uptake under the ZnO NP and S NP treatments, respectively. Our findings provide fundamental information for the safe and sustainable application of NP-conjugated agrochemicals. © 2023, The Authors. All rights reserved.

关键词： Soils

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A passive sampler for synchronously measuring inorganic and organic pollutants in sediment porewater:Configuration and field application

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Journal of environmental Sciences 2024年第2期136卷 201-212页

作者： Pei Lei Mingying Chen Nan Rong Wenzhong Tang Hong Zhang School of Environment Nanjing Normal UniversityNanjing 210023China State Key Laboratory of Environmental Aquatic Chemistry Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China South China Institute of Environmental Sciences Ministry of Ecology and EnvironmentGuangzhou 510530China State Environmental Protection Key Laboratory of Water Environmental Simulation and Pollution Control Guangzhou 510530China University of Chinese Academy of Sciences Beijing 100049China

In situ measurement of multiple pollutants coexisting in sediment porewater is an essential step in comprehensively assessing the bioavailability and risk of pollutants,but to date,this needs to be better *** this study,a passive sampler,consisting of an“I-shaped”supporting frame and inorganic/organic sampling units,incorporating equilibrium dialysis theory and kinetic/equilibrium sorption principle,was developed for the synchronous measurement of inorganic(e.g.,phosphorus and metal(loid)s)and organic pollutants(e.g.,parent and substituted PAHs).The equilibrium time and sampling rates were explored in laboratory tests to support in situ *** of pollutants in porewater within a vertical resolution of centimeters,i.e.,1 cm and 2 cm for inorganic and organic pollutants,respectively,were obtained by field deployment of the sampler for further estimation of diffusive fluxes across the sediment-water *** results suggested that the role of sediments for a specific pollutant may change(e.g.,from“sink”to“source”)during the sampling *** study demonstrated the feasibility of synchronous measurement of inorganic and organic pollutants in sediment porewater by the passive *** addition,it provided new insight for further investigation into the combined pollution effects of various pollutants in sediments.

关键词： Passive sampling Bioavailability Polycyclic aromatic hydrocarbons Combined pollution Diffusive flux

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Understanding Surface Water-Groundwater Conversion Relationship and Associated Hydrogeochemistry Evolution in the Upper Reaches of Luan River Basin, North China

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Journal of Earth Science 2024年第3期35卷 1010-1023页

作者： Le Zhao Chunli Su Wenbo Liu Xianjun Xie School of Environmental Studies China University of GeosciencesWuhan 430078China State Environmental Protection Key Laboratory of Source Apportionment and Control of Aquatic Pollution Ministry of Ecology and EnvironmentWuhan 430078China China Geological Environmental Monitoring Institute Beijing 100081China

Luan River is the main water source in Beijing-Tianjin-Hebei region,northern China,where the groundwater system is vulnerable and pollution issue is *** is significant for regional groundwater resources protection to identify the hydrogeochemistry evolution and affecting factors along flow direction occurred in the upper reaches,especially the surface water-groundwater(SWGW)conversion *** this study,recharge,conversion and geochemistry evolution of SW and GW were elucidated based on physical-hydrochemical indicators and stable isotopes in 36 GW samples and 20 SW samples,which were collected in July 2019 and July *** factor analysis was further utilized to determine the main factors responsible for regional hydrogeochemical *** indicate that GW recharged SW in plateau area,and SW and GW recharged each other in typical Alpine valley *** hydrochemical types are HCO3-Ca·Mg and HCO3-Ca,and the hydrochemical evolution is dominated by weathering of silicate and carbonate *** cation exchange adsorption has minor impact on groundwater *** rise of SO42-and NO3-contents in groundwater is related to industrial and agricultural *** main controlling factors of SW hydrochemical components included recharge from groundwater,industrial and mining activities,explaining 90.04%of data ***,water-rock interaction,agricultural and domestic sewage are responsible for GW quality,accounting for 83.38%.

关键词： groundwater water sources conversion relationship hydrogeochemical characteristics evolutional processes water-rock interaction factor analysis Luan River Basin.

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Revealing the intrinsic mechanisms for accelerating nitrogen removal efficiency in the Anammox reactor by adding Fe(Ⅱ)at low temperature

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Chinese Chemical Letters 2024年第8期35卷 341-348页

作者： Linjing Li Wenlai Xu Jianyong Ning Yaping Zhong Chuyue Zhang Jiane Zuo Zhicheng Pan State Key Laboratory of Geohazard Prevention and Geoenvironment Protection Chengdu University of TechnologyChengdu 610059China State Key Joint Laboratory of Environment Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China National Postdoctoral Research Station Haitian Water GroupChengdu 610213China National Enterprise Technology Center Haitian Water GroupChengdu 610213China Water Safety and Water Pollution Control Engineering Technology Research Center in Sichuan Province Chengdu 610213China Laboratory of Municipal Wastewater Treatment Technology in Sichuan Province Chengdu 610213China Institute of Environment and Ecology Tsinghua Shenzhen International Graduate SchoolShenzhen 518055China

Fe(Ⅱ)is an essential trace element for anaerobic ammonium oxidation bacteria(AAOB)metabolism,and can improve the nitrogen removal efficiency of anaerobic ammonia oxidation(Anammox).Here we oper-ated two identical expanded granular sludge bed(EGSB)reactors at low temperature(15±3℃)for 154 *** 1(R_(1))received additional Fe(Ⅱ)(0.12 mmol/L)during the late startup phase,while reactor 0(R_(0))served as the control and did not receive extra Fe(Ⅱ).Nitrogen removal in R_(1)became stable at 55 d of operation,ten days earlier than R_(0).The nitrogen removal rate(NRR)of R_(1) was 1.64 kg N m^(−3)d^(−1)and its TN removal rate was as high as 89%,while R_(0)only reached 75%.The addition of Fe(Ⅱ)was fur-ther beneficial to aggregation and stability of the granular sludge,and the used sludge of both reactors showed enrichment for AAOB populations compared to the inoculum,for instance,increased abundance of Candidatus-Kuenenia and in particular of Candidatus-Brocadia(from 0.17%to 10.10%in R_(0)and 7.79%in R_(1)).Diverse microbial species and complex microbial network structure in R_(1)compared to R_(0)promoted the coupled denitrogenation by Anammox,dissimilatory nitrate reduction to ammonium(DNRA),nitrate-dependent Fe oxidation(NDFO),and ferric ammonium oxidation(Feammox).In addition,the microbial community in R_(1)was more resistant to short-term low temperature(2-7℃)starvation,illustrating a further positive effect of adding Fe(Ⅱ)during the startup phase of an Anammox reactor.

关键词： Ambient low temperature Anammox Fe(Ⅱ) Extracellular polymeric substances Microbial community Microbial network analysis

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