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Addressing the environmental risk of persistent organic pollutants in China

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Frontiers of Environmental Science & Engineering 2012年第1期6卷 2-16页

作者： Bin WANG Jun HUANG shubo deng Xiaoling YANG Gang YU POPs Research Center School of EnvironmentTsinghua UniversityBeijing 10084China

The Stockholm Convention on persistent organic pollutants （POPs） was adopted in 2001. This year is the 10th anniversary of the adoption of the Convention. Until now, 22 chemicals or chemical categories have been listed as POPs in the Stockholm Convention. The POPs Research Center was established in Tsinghua University in the same year when the Convention was adopted. In the last ten years, much work has been done by Chinese researchers to understand the environ- mental risk of POPs in China. This article aims to review the recent research progress of our POPs Research Center and some other Chinese researchers＇ studies in addressing the environmental risk of POPs, including the priority screening and inventory study of POPs, monitoring and modeling of POPs pollution and exposure, and environ- mental risk assessment and modeling of POPs. Although great advances in addressing the environmental risk of POPs have been made in recent years, we are still facing quite a few problems, such as data scarcity and uncertainty in environmental risk assessment of POPs. The study on the effect of POPs mixtures is in its infancy and currently POPs are usually assessed from legal perspective by risk assessment of single chemicals. These problems should be well addressed by further efforts. Further studies should also be taken in future to study environment risk of POPs by considering aspects of coupled dynamics between climate processes and POPs. Such sound scientific, riskbased information can support decision-making aiming to effectively minimize the risk level of POPs.

关键词： persistent organic pollutant (POPs) environ- mental risk assessment inventory environmental monitoring fugacity model emerging POPs

Rapid determination of pharmaceuticals from multiple therapeutic classes in wastewater by solid-phase extraction and ultra-performance liquid chromatography tandem mass spectrometry

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Chinese Science Bulletin 2009年第24期54卷 4633-4643页

作者： SUI Qian HUANG Jun deng shubo YU Gang POPs Research Centre Department of Environmental Science and Engineering Tsinghua University Beijing 100084 China

A new analytical method utilizing ultra-performance liquid chromatography (UPLC) tandem mass spectrometry (MS/MS) has been developed to determine 16 pharmaceuticals from 8 therapeutic classes in wastewater: bezafibrate, clofibric acid, carbamazepine, caffeine, chloramphenicol, diclofenac, gemfibrozil, indomethacin, ketoprofen, mefenamic acid, metoprolol, nalidixic acid, N,N-diethyl-metatoluamide, propranolol, sulpiride and trimethoprim. Key parameters of MS/MS, UPLC and solid phase extraction (SPE) were optimized. In general, recovery of target pharmaceuticals was over 70% for the wastewater effluent samples and 50% for the influent samples. The effects of matrix suppression, loss during the pretreatment as well as instrument variability were successfully corrected by two internal standards, and acceptable relative recovery was obtained. Target compounds were quantitatively analyzed using multiple reaction monitoring (MRM) mode, and the detection limits ranged from 0.3 to 20 ng/L. A detailed study, matrix effect in effluent wastewater was also present. The method was applied to detecting pharmaceuticals in the wastewater from three wastewater treatment plants (WWTPs) in Beijing, China and the results demonstrated that most target compounds were detectable in both the influent and effluent, with the mean concentrations ranging from 20.5 to 5775.6 ng/L and 4.6 to 418.6 ng/L, respectively.

关键词：高效液相色谱串联质谱法固相萃取废水药品快速测定治疗污水处理厂

Removal of clofibric acid from aqueous solution by polyethylenimine-modified chitosan beads

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Frontiers of Environmental Science & Engineering 2014年第5期8卷 675-682页

作者： Yao NIE shubo deng Bin WANG Jun HUANG Gang YU POPs Research Center School of Environment Tsinghua University Beijing 100084 China State Key Joint Laboratory of Environment Simulation and Pollution Control Tsinghua University Beijing 100084 China

Polyethylenimine （PEI）-modified chitosan was prepared and used to remove clofibric acid （CA） from aqueous solution. PEI was chemically grafted on the porous chitosan through a crosslinking reaction, and the effects of PEI concentration and reaction time in the preparation on the adsorption of clofibric acid were optimized. Scanning electron microscopy （SEM） showed that PEI macromolecules were uniformly grafted on the porous chitosan, and the analysis of pore size distribution indicated that more mesopores were formed due to the crosslinking of PEI molecules in the macropores of chitosan. The PEI-modified chitosan had fast adsorption for CA within the initial 5 h, while this adsorbent exhibited an adsorption capacity of 349 mg· g^-1 for CA at pH 5.0 according to the Langmuir fitting, higher than 213 mg· g^-1 on the porous chitosan. The CA adsorption on the PEI- modified chitosan was pH-dependent, and the maximum adsorption was achieved at pH 4.0. Based on the surface charge analysis and comparison of different pharmaceu- ticals adsorption, electrostatic interaction dominated the sorption of CA on the PEI-modified chitosan. The PEI- modified chitosan has a potential application for the removal of some anionic rnicropollutants from water or wastewater.

关键词： clofibric acid PEI-modified chitosan adsorption capacity adsorption mechanism electrostatic interaction

Selective sorption of perfluorooctane sulfonate on molecularly imprinted polymer adsorbents

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Frontiers of Environmental Science & Engineering 2009年第2期3卷 171-177页

作者： shubo deng Danmeng SHUAI Qiang YU Jun HUANG Gang YU Department of Environmental Science and Engineering POPs Research Centerand State Key Joint Laboratory of Environment Simulation and Pollution ControlTsinghua UniversityBeijing 100084China

Perfluorooctane sulfonate(PFOS),as a potential persistent organic pollutant,has been widely detected in water environments,and has become a great concern in recent *** is very stable and difficult to decompose using conventional *** may be an attractive method to remove it from *** this study,the molecularly imprinted polymer(MIP)adsorbents were prepared through the polymerization of 4-vinylpyridine under different preparation conditions in order to remove perfluorooctane sulfonate(PFOS)from *** MIP adsorbents using perfluorooctanoic acid(PFOA)as the template had good imprinting effects and could selectively remove PFOS from aqueous *** sorption behaviors including sorption kinetics,isotherms,and effect of pH,salt,and competitive anions were *** results showed that the sorption of PFOS on the MIP adsorbents was very fast,pHdependent,and highly *** achieved fast sorption equilibrium within 1 h was attributed to the surface sorption on the fine *** sorption isotherms showed that the sorption selectivity of PFOS on the MIP adsorbents decreased at high PFOS concentrations,which may be due to the double-layer sorption and the formation of PFOS micelles on the sorbent *** sorption of PFOS on the MIP adsorbents was mainly dominated by the electrostatic interaction between the protonated vinylpyridine on the adsorbent surface and the anionic *** prepared MIP adsorbents can potentially be applied in water and wastewater treatment for selective removal of PFOS.

关键词： perfluorooctane sulfonate(PFOS) molecularly imprinted polymer(MIP)adsorbents selective sorption electrostatic interaction

Fate and removal of typical pharmaceutical and personal care products in a wastewater treatment plant from Beijing： a mass balance study

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Frontiers of Environmental Science & Engineering 2016年第3期10卷 491-501页

作者： Jie GAO Jun HUANG Weiwei CHEN Bin WANG Yujue WANG shubo deng Gang YU State Key Joint Laboratory of Environment Simulation and Pollution Control (SKJLESPC) Beijing Key Laboratory of Emerging Organic Contaminants Control (BKLEOCC) School of Environment Tsinghua University Beijing 100084 China Beijing Municipal Solid Waste and Chemical Management Center Beijing 100084 China Xiamen Urban Planning and Design Institute Xiamen 361012 China

The fate and removal of pharmaceuticals and personal care products （PPCPs） in wastewater treatment plants （WWTPs） has received great attention during the last decade. Numerous data concerning concentrations in the water phase can be found in the literature, however corresponding data from sludge as well as associated mass balance calculations are very limited. In the present study, the adsorbed and dissolved concentrations of 9 PPCPs were investigated in each unit of a WWTP in Beijing, China. Based on the calculation of mass balance, the relative mass distribution and removal efficiency of each target compound was obtained at each process. The amount of PPCPs entering into the WWTP ranged from 12 g·d^-1 to 3848 g·d^-1. Five target compounds （caffeine, chloramphenicol, bezafibrate, clofibric acid, and N,N- diethyl-meta-toluamide） were effectively removed, with rates of 57%-100%. Negative removal efficiencies were obtained for sulpiride, metoprolol, nalidixic acid, and carbamazepine, ranging from -19% to -79%. PPCPs mainly existed in dissolved form （≥92%） in both the raw influent and the final effluent. The sludge cake carried a much lower amount of PPCPs （17 g·d^-1） compared with the discharged effluent （402 g·d^-1）. In A^2/O treatment tanks, the anaerobic and anoxic tanks showed good performance for PPCPs removal, and the amount of adsorbed PPCPs was increased. The results reveal that both the dissolved and the adsorbed phases should be considered when assessing the removal capacity of each A^2/O tank.

关键词： PPCPs A^2/O mass balance removal efficiency sludge

Removal of fluoride from water using titanium-based adsorbents

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Frontiers of Environmental Science & Engineering 2010年第4期4卷 414-420页

作者： Zhijian LI shubo deng Xueying ZHANG Wei ZHOU Jun HUANG Gang YU Department of Environmental Science and Engineering POPs Research CenterTsinghua UniversityBeijing 100084China

Three adsorbents including TiO_(2),Ti-Ce,and Ti-La hybrid oxides were prepared to remove fluoride from aqueous *** Ti-Ce and Ti-La hybrid adsorbents obtained by the hydrolysis-precipitation method had much higher sorption capacity for fluoride than the TiO_(2) adsorbent prepared through *** earth(Ce and La)oxides and TiO_(2) exhibited a synergistic effect in the hybrid adsorbents for fluoride *** sorption equilibrium of fluoride on the three adsorbents was achieved within 4 h,and the pseudo-second-order model described the sorption kinetics *** sorption isotherms fitted the Langmuir model well,and the adsorption capacities of fluoride on the Ti-Ce and Ti-La adsorbents were about 9.6 and 15.1 mg·g^(-1),respectively,at the equilibrium fluoride concentration of 1.0 mg·L^(-1),much higher than the 1.7 mg·g^(-1) on the TiO_(2).The sorption capacities of fluoride on the three adsorbents decreased significantly when the solution pH increased from 3 to *** electrostatic interaction played an important role in fluoride removal by the three adsorbents,and Fourier transform infrared(FTIR)analysis indicated that the hydroxyl groups on the adsorbent surface were involved in fluoride adsorption.

关键词： fluoride adsorption titanium dioxide titanium-based adsorbent sorption mechanism

Activated carbons and amine-modified materials for carbon dioxide capture- a review

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Frontiers of Environmental Science & Engineering 2013年第3期7卷 326-340页

作者： Zhenhe CHEN shubo deng Haoran WEI Bin WANG Jun HUANG Gang YU State Key Joint Laboratory of Environment Simulation and Pollution Control School of Environment POPs Research Center Tsinghua University Beijing 100084 China Tsinghua University .- Veolia Environment Joint Research Center for Advanced Technotogy Tsinghua University Beijing 100084 China

Rapidly increasing concentration of CO2 in the atmosphere has drawn more and more attention in recent years, and adsorption has been considered as an effective technology for CO2 capture from the anthropogenic sources. In this paper, the attractive adsorbents including activated carbons and amine-modified materials were mainly reviewed and discussed with particular attention on progress in the adsorbent preparation and C02 adsorption capacity. Carbon materials can be prepared from different precursors including fossil fuels, biomass and resins using the carbonization-activation or only activation process, and activated carbons prepared by KOH activation with high CO2 adsorbed amount were reviewed in the preparation, adsorption capacity as well as the relationship between the pore characteristics and CO2 adsorption. For the amine-modified materials, the physical impregnation and chemical graft of polyethylenimine （PEI） on the different porous materials were introduced in terms of preparation method and adsorption perfor- mance as well as their advantages and disadvantages for CO2 adsorption. In the last section, the issues and prospect of solid adsorbents for CO2 adsorption were summarized, and it is expected that this review will be helpful for the fundamental studies and industrial applications of acti- vated carbons and amine-modified adsorbents for CO2 capture.

关键词： adsorption capacity CO2 capture activatedcarbon amine-impregnated adsorbents

Electrochemical oxidation of 1H,1H,2H,2H-perfluorooctane sulfonic acid(6:2 FTS) on DSA electrode:Operating parameters and mechanism

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Journal of Environmental Sciences 2014年第8期26卷 1733-1739页

作者： Qiongfang Zhuo Xiang Li Feng Yan Bo Yang shubo deng Jun Huang Gang Yu POPs Research Center School of EnvironmentTsinghua University South China Institute of Environmental Sciences the Ministry of Environment Protection College of Chemistry and Chemical Engineering Shenzhen University

The 6：2 FTS was the substitute for perfluorooctane sulfonate（PFOS） in the chrome plating industry in Japan. Electrochemical oxidation of 6：2 FTS was investigated in this study. The degradabilities of PFOS and 6：2 FTS were tested on the Ti/SnO2–Sb2O5–Bi2O3anode. The effects of current density,potential,and supporting electrolyte on the degradation of 6：2 FTS were evaluated. Experimental results showed that 6：2 FTS was more easily degraded than PFOS on the Ti/SnO2–Sb2O5–Bi2O3anode. At a low current density of 1.42 mA/cm2,6：2 FTS was not degraded on Ti/SnO2–Sb2O5–Bi2O3,while the degradation ratio increased when the current density ranged from 4.25 to 6.80 mA/cm2. The degradation of 6：2 FTS at current density of 6.80 mA/cm2 followed pseudo first-order kinetics with the rate constant of 0.074 hr-1. The anodic potential played an important role in the degradation of 6：2 FTS,and the pseudo first-order rate constants increased with the potential. The surface of Ti/SnO2–Sb2O5–Bi2O3was contaminated after electrolysis at constant potential of 3 V,while the fouling phenomenon was not observed at 5 V. The fouled anode could be regenerated by incinerating at 600°C. The intermediates detected by ultra-performance liquid chromatography coupled with a triple-stage quadrupole mass spectrometer（UPLC–MS/MS） were shorter chain perfluorocarboxylic acids. The 6：2 FTS was first attacked by hydroxyl radical,and then formed perfluorinated carboxylates,which decarboxylated and removed CF2 units to yield shorter-chain perfluorocarboxylic acids.

关键词： 6:2 FTS Electrochemical oxidation Intermediates Mechanism

Rapid removal of bisphenol A on highly ordered mesoporous carbon

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Journal of Environmental Sciences 2011年第2期23卷 177-182页

作者： Qian Sui Jun Huang Yousong Liu Xiaofeng Chang Guangbin Ji shubo deng Tao Xie Gang Yu Department of Environmental Science and Engineering Tsinghua University - VEOLIA Environnement Joint Research Center for Advanced Environmental Technology Tsinghua University Beijing 100084 Nanomaterials Research Institute College of Materials Science and TechnologyNanjing University of Aeronautics and Astronautics Nanjing 210016 China

Bisphenol A （BPA） is of global concern due to its disruption of endocrine systems and ubiquity in the aquatic environment. It is important, therefore, that efforts are made to remove it from the aqueous phase. A novel adsorbent, mesoporous carbon CMK-3, prepared from hexagonal SBA- 15 mesoporous silica was studied for BPA removal from aqueous phase, and compared with conventional powdered activated carbon （PAC）. Characterization of CMK-3 by transmission electron microscopy （TEM）, X-ray diffraction, and nitrogen adsorption indicated that prepared CMK-3 had an ordered mesoporous structure with a high specific surface area of 920 m^2/g and a pore-size of about 4.9 nm. The adsorption of BPA on CMK-3 followed a pseudo second-order kinetic model. The kinetic constant was 0.00049 g/（***）, much higher than the adsorption of BPA on PAC. The adsorption isotherm fitted slightly better with the Freundlich model than the Langmuir model, and adsorption capacity decreased as temperature increased from 10 to 40℃. No significant influence of pH on adsorption was observed at pH 3 to 9; however, adsorption capacity decreased dramatically from pH 9 to 13.

关键词： mesoporous carbon CMK-3 powdered activated carbon bisphenol A endocrine disrupting chemicals