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Insight into the mechanisms of trichloronitromethane formation by vacuum ultraviolet: QSAR model and FTICR-MS analysis

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Journal of environmental Sciences 2023年第3期125卷 215-222页

作者： Xiaojun Chen Yangtao Wu Weiqiu Zhang Lingjun Bu Shumin Zhu Da Sheng Shiqing Zhou John C.Crittenden Key Laboratory of Building Safety and Energy Efficiency Ministry of EducationDepartment of Water Engineering and ScienceCollege of Civil EngineeringHunan UniversityChangsha 410082China school of civil and environmental engineering and the brook byers institute for sustainable systems Georgia Institute of TechnologyGeorgia 30332USA

Vacuum ultraviolet(VUV) photolysis is recognized as an environmental-friendly treatment process. Nitrate(NO-3) and natural organic matter(NOM) are widely present in water source.We investigated trichloronitromethane(TCNM) formation during chlorination after VUV photolysis, because TCNM is an unregulated highly toxic disinfection byproduct. In this study:(1) we found reactive nitrogen species that is generated under VUV photolysis of NO-3react with organic matter to form nitrogen-containing compounds and subsequently form TCNM during chlorination;(2) we found the mere presence of 0.1 mmol/L NO-3can result in the formation of up to 63.96 μg/L TCNM;(3) we found the changes in pH(6.0-8.0), chloride(1-4 mmol/L), and bicarbonate(1-4 mmol/L) cannot effectively diminish TCNM formation;and,(4) we established the quantitative structure-activity relationship(QSAR) model,which indicated a linear relationship between TCNM formation and the Hammett constant(σ) of model compounds;and,(5) we characterized TCNM precursors in water matrix after VUV photolysis and found 1161 much more nitrogen-containing compounds with higher aromaticity were generated. Overall, this study indicates more attention should be paid to reducing the formation risk of TCNM when applying VUV photolysis process at scale.

关键词： Vacuum ultraviolet Natural organic matter Hammett constant FTICR-MS Trichloronitromethane

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Influence of MnO_(x)deposition on TiO_(2)nanotube arrays for electrooxidation

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Green Energy & Environment 2023年第2期8卷 612-618页

作者： Kaihang Zhang Yuanzheng Zhang Su Liu Xin Tong Junfeng Niu Dong Wang Junchen Yan Zhaoyang Xiong John Crittenden brook byers institute of sustainable systems and school of civil and environmental engineering Georgia Institute of TechnologyAtlantaGA 30332USA College of environmental Science and engineering North China Electric Power UniversityBeijing102206China

TiO_(2)has demonstrated outstanding performance in electrochemical advanced oxidation processes(EAOPs)due to its structural stability and high oxygen overpotential.However,there is still much room for improving its electrochemical activity.Herein,narrow bandgap manganese oxide(MnO_(x))was composited with TiO_(2)nanotube arrays(TiO_(2)NTAs)that in-situ oxidized on porous Ti sponge,forming the MnO_(x)-TiO_(2)NTAs anode.XANES and XPS analysis further proved that the composition of MnO_(x)is Mn2O3.Electrochemical characterizations revealed that increasing the composited concentration of MnO_(x)can improve the conductivity and reduce oxygen evolution potential so as to improve the electrochemical activity of the composited MnO_(x)-TiO_(2)NTAs anode.Meanwhile,the optimal degradation rate of benzoic acid(BA)was achieved using MnO_(x)-TiO_(2)NTAs with a MnO_(x)concentration of 0.1 mmol L^(-1),and the role of MnO_(x)was proposed based on DFT calculation.Additionally,the required electrical energy(EE/O)to destroy BA was optimized by varying the composited concentration of MnO_(x)and the degradation voltage.These quantitative results are of great significance for the design and application of high-performance materials for EAOPs.

关键词： TiO_(2)nanotube arrays Oxidation mechanism Energy efficiency assessment MnO_(x)band structure Electrochemical advanced oxidation processes

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Screening ionic liquids for efficiently extracting perfluoroalkyl chemicals (PFACs) from wastewater

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Journal of environmental Sciences 2023年第5期127卷 866-874页

作者： Kaihang Zhang David Kujawski Chris Spurrell Bing Wang John CCrittenden brook byers institute of sustainable systems and school of civil and environmental engineering Georgia Institute of TechnologyAtlantaGA 30332USA Refinery Water engineering and Associates Hydrocarbon Processing Water and Waste TechnologyInc.HoustonTX 77042USA Chevron USA VancouverWA 98664USA school of Municipal and environmental engineering Shenyang Jianzhu UniversityShenyang 110000China

Liquid-liquid extraction(LLE)using ionic liquids(ILs)-based methods to remove perfluoroalkyl chemicals(PFACs),such as perfluorooctanoic acid(PFOA)and perfluorooctane sulfonic acid(PFOS),from wastewater,is an important strategy.However,the lack of physicochemical and LLE data limits the selection of the most suitable ILs for the extraction of PFACs.In this work,1763 ILs for PFACs extraction from water were systematically screened using COSMOtherm to estimate the infinite dilution activity coefficient(lnγ^(∞))of PFOA and PFOS in water and ILs.To evaluate the accuracy of COSMOtherm,8 ILs with various lnγ^(∞)values were selected,and their extraction efficiency(E)and distribution coefficient(D_(exp))were measured experimentally.The results showed that the predicted lnγ^(∞)decreased as the increase of experimental extraction efficiency of PFOA or PFOS,while the tendency of predicted distribution coefficient(D_(pre))was consistent with the experimental(D_(exp))results.This work provides an efficient basis for selecting ILs for the extraction of PFACs from wastewater.

关键词： Conductor-like screening model for real solvents(COSMO-RS) Ionic liquids Perfluorooctanoic acid(PFOA) Perfluorooctane sulfonic acid(PFOS) Liquid-liquid extraction

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Ultrafast battery heat dissipation enabled by highly ordered and interconnected hexagonal boron nitride thermal conductive composites

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Green Energy & Environment 2022年第6期7卷 1401-1410页

作者： Zhuoya Wang Kaihang Zhang Bing Zhang Zheming Tong Shulan Mao Hao Bai Yingying Lu State Key Laboratory of Chemical engineering Institute of Pharmaceutical EngineeringCollege of Chemical and Biological EngineeringZhejiang UniversityHangzhou310027China brook byers institute of sustainable systems and school of civil and environmental engineering Georgia Institute of TechnologyAtlantaGA30332USA ZJU-Hangzhou Global Scientific and Technological Innovation Center Zhejiang UniversityHangzhou311200China State Key Laboratory of Fluid Power and Mechatronic systems College of Mechanical EngineeringZhejiang UniversityHangzhou310027China

Heat dissipation involved safety issues are crucial for industrial applications of the high-energy density battery and fast charging technology.While traditional air or liquid cooling methods suffering from space limitation and possible leakage of electricity during charge process,emerging phase change materials as solid cooling media are of growing interest.Among them,paraffin wax(PW)with large latent heat capacity and low cost is desirable for heat dissipation and thermal management which mainly hindered by their relatively low thermal conductivity and susceptibility to leakage.Here,highly ordered and interconnected hexagonal boron nitride(h-BN)networks were established via ice template method and introduced into PW to enhance the thermal conductivity.The composite with 20 wt%loading amount of h-BN can guarantee a highly ordered network and exhibited high thermal conductivity(1.86 W m^(-1) K^(-1))which was 4 times larger compared with that of random dispersed h-BN involved PW and nearly 8 times larger compared with that of bare PW.The optimal thermal conductive composites demonstrated ultrafast heat dissipation as well as leakage resistance for lithium-ion batteries(LIBs),heat generated by LIBs can be effectively transferred under the working state and the surface temperature kept 6.9℃ lower at most under 2–5℃ continuous charge-discharge process compared with that of bare one which illustrated great potential for industrial thermal management.

关键词： Hexagonal boron nitride Paraffin wax Lithium-ion batteries Thermal conductive network Battery heat dissipation

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Precise regulation of acid pretreatment for red mud SCR catalyst:Targeting on optimizing the acidity and reducibility

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Frontiers of environmental Science & engineering 2022年第7期16卷 61-71页

作者： Xiang Zhang Yue Xuan Bin Wang Chuan Gao Shengli Niu Gaiju Zhao Dong Wang Junhua Li Chunmei Lu John C.Crittenden National engineering Laboratory for Coal-Burning Pollutants Emission Reduction School of Energy and Power EngineeringShandong UniversityJinan250061China school of civil and environmental engineering and the brook byers institute for sustainable systems Georgia Institute of TechnologyAtlantaGA30332USA State Key Joint Laboratory of Environment Simulation and Pollution Control National Engineering Laboratory for Multi Flue Gas Pollution Control Technology and EquipmentSchool of EnvironmentTsinghua UniversityBeijing100084China Energy institute Qilu University of Technology(Shandong Academy of Sciences)Jinan250013China

Red mud(RM),as an alkaline waste,was recently proved to be a promising substitute for the SCR catalyst.Dealkalization could improve the acidity and reducibility of red mud,which were critical for SCR reaction.However,the dealkalization effect depended on the reaction between acid solution and red mud.In this study,we realized the directional control of the chemical state of active sites through tuning the acid pretreatment(dealkalization)process.The pretreatment endpoint was controlled at pH values of 3–5 with diluted nitric acid.When the pH values of red mud were 3 and 5(CRM-3 and CRM-5),activated catalysts showed NOx conversion above 90%at 275℃–475℃.The high initial reaction rate,Ce^(3+)/(Ce^(3+)+Ce^(4+))ratio,and surface acidity accounted for the excellent SCR performance of CRM-5 catalyst.Meanwhile,more Fe^(3+) on the CRM-3 surface improved the NH_(3) adsorption.There was a strong interaction between Al and Fe in both CRM-5 and CRM-3 catalysts.DFT results showed that the adsorption capacity of the Al-O_(3)-Fe for NH_(3) and NO is stronger than that of Fe-O_(3)-Fe,which enhanced the NOx conversion of the catalyst.However,the almandine was formed in CRM-4,consumed part of Fe^(3+) and Al^(3+),and the interaction between Al and Fe was weakened.Also,deposited almandine on the catalyst surface covered the active sites,thus leading to lower NH_(3)-SCR activity.

关键词： Air pollution control Nitrogen oxides Selective catalytic reduction Red mud Solid waste utilization

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Ultrastable MOF-based foams for versatile applications

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Nano Research 2022年第4期15卷 2961-2970页

作者： Qian Hu Licong Xu Kaixing Fu Feichao Zhu Taoyu Yang Tao Yang Jinming Luo Minghua Wu Deyou Yu engineering Research Center for Eco-Dyeing and Finishing of Textiles Ministry of EducationZhejiang Sci-Tech UniversityHangzhou 310018China brook byers institute for sustainable systems School of Civil and Environmental EngineeringGeorgia Institute of TechnologyAtlanta 30332USA school of environmental Science and engineering Shanghai Jiao Tong UniversityShanghai 200240China State Key Laboratory of Chemo/Biosensing and Chemometrics Hunan UniversityChangsha 410082China institute for Nanomaterials Advanced Technologies and InnovationTechnical University of LiberecLiberec 46117Czech Republic Zheijiang Sci-Tech University Tongxiang Research institute Tongxiang 345000China

Metal-organic frameworks(MOFs)are attractive for promising applications but plagued by difficult recovery and deployment due to their intrinsic nano/micro powder nature.Although significant efforts have been made to develop separable solid matrixes for MOF supporting,the poor loading stability and durability of MOFs still challenge their engineering applications.Here,we present a facile and effective approach to fabricate MOF-based melamine foams(MFs)(denoted as MOFiths)with ultrahigh loading stability and operation stability,easy separation,and high-efficient performance for versatile robust applications.By adopting our approach,numbers of typical fragile MOFs characterized with wide ranges of particle size(from~nm to~μm)can be precisely incorporated into MFs with controllable loading ratios(up to~1,600%).Particularly,the produced MOFiths show excellent capacities for the highly effective and durable water purifications and acetalization reactions.100%of organic pollutants can be rapidly destructed within 10 min by MOFiths initiated Fenton or catalytic ozonation processes under five successive cycles while the maximum adsorption capacity of MOFiths toward Pb(II),Cd(II),and Cu(II)reaches to 422,222,and 105 mg·g^(-1),respectively.This study provides a critical solution to substantially facilitate the engineering applications of MOFs for long-term use in practice.

关键词： metal-organic framework melamine foam ultrastability versatile applications long-term use

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Cerium-tungsten oxides supported on activated red mud for the selective catalytic reduction of NO_(x)

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Green Energy & Environment 2023年第1期8卷 173-182页

作者： Qiuzhun Chen Dong Wang Chuan Gao Bin Wang Shengli Niu Gaiju Zhao Yue Peng Junhua Li Chunmei Lu John Crittenden National engineering Laboratory for Coal-Burning Pollutants Emission Reduction School of Energy and Power EngineeringShandong UniversityJinan250061China State Key Joint Laboratory of Environment Simulation and Pollution Control National Engineering Laboratory for Multi Flue Gas Pollution Control Technology and EquipmentSchool of EnvironmentTsinghua UniversityBeijing100084China brook byers institute for sustainable systems and school of civil and environmental engineering Georgia Institute of Technology828 West Peachtree StreetAtlantaGA30332United States Energy institute Qilu University of Technology(Shandong Academy of Sciences)Jinan250013ShandongChina

Activated red mud(RM)has been proved to be a promising base material for the selective catalysis reduction(SCR)of NOx.The inherent low reducibility and acidity limited its low-temperature activity.In this work,molybdenum oxide,tungsten oxide,and cerium oxide were used to reconfigure the redox sites and acid sites of red mud based catalyst.When activated red mud was reconfigured by cerium-tungsten oxide(Ce-W@RM),the NOx conversion kept above 90%at 219-480℃.The existence of Ce^(3+)/Ce^(4+) redox electron pairs provided more surface adsorbed oxygen(O_(α)) and served as a redox cycle.Positive interactions between Ce,W species and Fe oxide in red mud occurred,which led to the formation of unsaturated chemical bond and promoted the activation of adsorbed NH_(3) species.WO_(3) and Ce_(2)(WO_(4))_(3)(formed by solid-state reaction between Ce and W species)could provide more Brønsted acid sites(W-O modes of WO_(3),W=O or W-O-W modes of Ce_(2)(WO_(4))_(3)).CeO_(2) species could provide more Lewis acid sites.The Langmuir-Hinshelwood(L-H)routes and Eley-Rideal(E-R)routes occurred in the low-temperature SCR reaction on the Ce-W@RM surface.NH_(4)^(+) species on Brønsted acid sites,NH_(3) species on Lewis acid sites,bidentate nitrate and bridging nitrate species were key active intermediates species.

关键词： Air pollution control NOx Selective catalytic reduction Cerium Tungsten

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Key findings of the 2016 symposium on the frontiers of chemical science and engineering： Environment and sustainable development

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Frontiers of Chemical Science and engineering 2017年第3期11卷 305-307页

作者： Zhongming Lu Duo Li John C. Crittenden school of Environment Beijing Normal University Beijing 100875 China Crittenden and Associates Beijing 100102 China brook byers institute for sustainable systems School of Civil and Environmental Engineering Georgia Institute of Technology Atlanta GA 30332-0355 USA

There were 30 speakers and the proceedings contained 28 abstracts that discussed the start-of-the art applications of sustainable chemical engineering [1]. We summarized topics that were discussed in the 28 abstracts using the non-negative matrix factorization （NMF） algorithm. The ＂topics＂ were synthesized without reading the abstracts. Here we will not discuss the algorithm of NMF in detail because of the space limitation and please refer to references for the description of NMF [2,3]. Topic modeling will be more valuable as the number of the abstracts increases.

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Activated carbon enhanced ozonation of oxalate attributed to HO·oxidation in bulk solution and surface oxidation: Effect of activated carbon dosage and pH

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Journal of environmental Sciences 2014年第10期26卷 2095-2105页

作者： Linlin Xing Yongbing Xie Daisuke Minakata Hongbin Cao Jiadong Xiao Yi Zhang John C. Crittenden National engineering Laboratory for Hydrometallurgical Cleaner Production Technology Key Laboratory of Green Process and engineering Institute of Process Engineering Chinese Academy of Sciences Beijing engineering Research Center of Process Pollution Control University of Chinese Academy of Sciences Department of civil and environmental engineering Michigan Technological UniversityHoughton MI 49931 United States school of civil and environmental engineering Brook Byers Institute for Sustainable Systems Georgia Institute of TechnologyAtlantaGA 30332 United States

Ozonation of oxalate in aqueous phase was performed with a commercial activated carbon（AC）in this work. The effect of AC dosage and solution pH on the contribution of hydroxyl radicals（HOU） in bulk solution and oxidation on the AC surface to the removal of oxalate was studied. We found that the removal of oxalate was reduced by tert-butyl alcohol（tBA） with low dosages of AC,while it was hardly affected by tBA when the AC dosage was greater than 0.3 g/L. tBA also inhibited ozone decomposition when the AC dosage was no more than 0.05 g/L, but it did not work when the AC dosage was no less than 0.1 g/L. These observations indicate that HOUin bulk solution and oxidation on the AC surface both contribute to the removal of oxalate. HOU oxidation in bulk solution is significant when the dosage of AC is low, whereas surface oxidation is dominant when the dosage of AC is high. The oxalate removal decreased with increasing pH of the solution with an AC dosage of 0.5 g/L. The degradation of oxalate occurs mainly through surface oxidation in acid and neutral solution, but through HOUoxidation in basic bulk solution. A mechanism involving both HOUoxidation in bulk solution and surface oxidation was proposed for AC enhanced ozonation of oxalate.

关键词： Activated carbon Oxalate Ozonation Hydroxyl radicals Surface oxidation Catalytic ozonation

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Wastewater surveillance provides 10-days forecasting of COVID-19 hospitalizations superior to cases and test positivity:A prediction study

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Infectious Disease Modelling 2023年第4期8卷 1138-1150页

作者： Dustin T.Hill Mohammed A.Alazawi E.Joe Moran Lydia J.Bennett Ian Bradley Mary B.Collins Christopher J.Gobler Hyatt Green Tabassum Z.Insaf Brittany Kmush Dana Neigel Shailla Raymond Mian Wang Yinyin Ye David A.Larsen Department of Public Health Syracuse UniversitySyracuseNY13244USA Center for environmental Health New York State Department of HealthAlbanyNYUSA CDC Foundation AtlantaGAUSA Department of civil Structural and Environmental EngineeringUniversity at BuffaloBuffaloNYUSA school of Marine and Atmospheric Sciences Sustainability Studies DivisionStony Brook UniversityStony BrookNYUSA institute for Advanced Computational Science Stony Brook UniversityStony BrookNYUSA New York State Center for Clean Water Technology Stony Brook UniversityStony BrookNYUSA school of Marine and Atmospheric Sciences Stony Brook UniversityStony BrookNYUSA Department of environmental Biology State University of New York College of Environmental Science and ForestrySyracuseNYUSA Department of Epidemiology and Biostatistics School of Public HealthUniversity at AlbanyRensselaerNYUSA Department of civil engineering College of Engineering and Applied SciencesStony Brook UniversityStony BrookNYUSA

Background:The public health response to COVID-19 has shifted to reducing deaths and hospitalizations to prevent overwhelming health systems.The amount of SARS-CoV-2 RNA fragments in wastewater are known to correlate with clinical data including cases and hospital admissions for COVID-19.We developed and tested a predictive model for incident COVID-19 hospital admissions in New York State using wastewater data.Methods:Using county-level COVID-19 hospital admissions and wastewater surveillance covering 13.8 million people across 56 counties,we fit a generalized linear mixed model predicting new hospital admissions from wastewater concentrations of SARS-CoV-2 RNA from April 29,2020 to June 30,2022.We included covariates such as COVID-19 vaccine coverage in the county,comorbidities,demographic variables,and holiday gatherings.Findings:Wastewater concentrations of SARS-CoV-2 RNA correlated with new hospital admissions per 100,000 up to ten days prior to admission.Models that included wastewater had higher predictive power than models that included clinical cases only,increasing the accuracy of the model by 15%.Predicted hospital admissions correlated highly with observed admissions(r¼0.77)with an average difference of 0.013 hospitalizations per 100,000(95%CI¼[0.002,0.025])Interpretation:Using wastewater to predict future hospital admissions from COVID-19 is accurate and effective with superior results to using case data alone.The lead time of ten days could alert the public to take precautions and improve resource allocation for seasonal surges.

关键词： COVID-19 hospitalizations Wastewater-based epidemiology Forecasting Prediction SARS-CoV-2

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