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Mass transfer characteristics of chiral pharmaceuticals on membrane used for polar organic chemical integrative sampler

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Journal of Environmental Sciences 2024年第2期136卷 670-681页

作者： Liyang Wang Ruixia Liu Youya Zhou Peng Yuan Xiaoling Liu Hongjie Gao College of Water Science Beijing Normal UniversityBeijing 100018China State key laboratory of Environmental Criteria and risk Assessment Chinese Research Academy of Environmental ScienceBeijing 100012China Technical Centre for Soil Agriculture and Rural Ecology and EnvironmentMinistry of Ecology and EnvironmentBeijing 100012China

Passive sampling technology has good application prospects for monitoring trace pollutants in aquatic environments.Further research on the sampling mechanism of this technology is essential to improve the measurement accuracy and extend the application scope of this approach.In this study,adsorption and permeation experiments were performed to investigate the sorption and mass transfer properties of five chiral pharmaceuticals at the enantiomeric level on polyethersulfone(PES)and polytetrafluoroethylene(PTFE)membranes used in a polar organic chemical integrative sampler.Batch adsorption experiments showed that the PES membrane had an adsorption phenomenon for most selected pollutants and an insignificant sorption behavior was observed for all selected pharmaceuticals on the PTFE membrane except for R(S)-fluoxetine.The diffusion coefficients of selected pharmaceuticals onto the PTFE membrane were approximately one order of magnitude higher than those onto the PES membrane.The permeation experiment indicated that under different hydraulic conditions,the change of the relative pollutant concentration through the PTFE membrane for the composite pollutant system was more obvious than that for the single pollutant system,and mass transfer hysteresis exists for both contaminant systems through PES membranes.Using the first-order equation or 3-component model to estimate the overall mass transfer coefficients,the results showed that the overall mass transfer coefficient values of pollutants in the composite pollutant system onto both membranes were higher than those in the single pollutant system.This parameter was mainly influenced by the synergistic effects of the multi-analyte interaction and diminished water boundary layers during the mass transfer process.

关键词： Sorption phenomenon Permeation behavior Mass transfer properties modeling calculation Chiral pharmaceuticals PES and PTFE membrane

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Seasonal variation of mesoscale eddy intensity in the global ocean

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Acta Oceanologica Sinica 2024年第1期43卷 48-58页

作者： Yongcan Zu Yue Fang Shuangwen Sun Libao Gao Yang Yang Guijun Guo First Institute of Oceanography/key laboratory of Marine Science and Numerical modeling Ministry of Natural ResourcesQingdao 266061China laboratory for Regional Oceanography and Numerical modeling Laoshan LaboratoryQingdao 266237China Shandong key laboratory of Marine Science and Numerical modeling Qingdao 266061China

Mesoscale eddies are a prominent oceanic phenomenon that plays an important role in oceanic mass transport and energy conversion.Characterizing by rotational speed,the eddy intensity is one of the most fundamental properties of an eddy.However,the seasonal spatiotemporal variation in eddy intensity has not been examined from a global ocean perspective.In this study,we unveil the seasonal spatiotemporal characteristics of eddy intensity in the global ocean by using the latest satellite-altimetry-derived eddy trajectory data set.The results suggest that the eddy intensity has a distinct seasonal variation,reaching a peak in spring while attaining a minimum in autumn in the Northern Hemisphere and the opposite in the Southern Hemisphere.The seasonal variation of eddy intensity is more intense in the tropical-subtropical transition zones within latitudinal bands between 15°and 30°in the western Pacific Ocean,the northwestern Atlantic Ocean,and the eastern Indian Ocean because baroclinic instability in these areas changes sharply.Further analysis found that the seasonal variation of baroclinic instability precedes the eddy intensity by a phase of 2–3 months due to the initial perturbations needing time to grow into mesoscale eddies.

关键词： seasonal variation mesoscale eddy intensity baroclinic instability global ocean

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Colloid-facilitated release of polybrominated diphenyl ethers at an e-waste recycling site: evidence from undisturbed soil core leaching experiments

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Frontiers of Environmental Science & Engineering 2024年第2期18卷 91-101页

作者： Zebin Huo Mengjun Xi Lianrui Xu Chuanjia Jiang Wei Chen College of Environmental Science and Engineering Ministry of Education Key Laboratory of Pollution Processes and Environmental CriteriaTianjin Key Laboratory of Environmental Remediation and Pollution ControlNankai UniversityTianjin 300350China

Polybrominated diphenyl ethers (PBDEs), a class of persistent organic pollutants, have been frequently detected in soil at e-waste recycling sites. However, the key factors controlling the transport of PBDEs from surface soil to the vadose zone and groundwater are unclear. Here, colloid-enhanced leaching of PBDEs from undisturbed soil cores collected at an e-waste recycling site in Tianjin, China, is reported. Spatially heterogeneous release of colloids and PBDEs was observed in all the tested soil cores under chemical and hydrodynamic perturbations, indicating the presence of preferential flow paths. Colloid concentration in the effluent significantly increased as ionic strength decreased (from 10 to 0.01 mmol/L), probably due to the stronger electrostatic repulsion between colloidal particles and the soil matrix at lower ionic strength. In contrast, colloid mobilization was not significantly affected by the changes in pH of the influent (from 4.0 to 10.0) and flow rate (from a Darcy velocity of 1.5 to 6.0 cm/h). The concentrations of 2,2′,3,3′,4,4′,5,5′,6,6′-decabromodiphenyl ether (BDE-209), the predominant PBDE congener at the site, detected in the leachate (ranging from 1.09 to 3.43 ng/L) were much lower than previously reported results from packed column leaching tests, and were positively correlated with colloid concentrations. This indicates that remobilization of colloids at e-waste recycling sites can promote the leaching and downward migration of PBDEs from surface soil. The findings highlight the potential risk of surface soil PBDE contamination to groundwater quality and call for further understanding of colloid-facilitated transport for predicting the fate of PBDEs at e-waste recycling sites.

关键词： Polybrominated diphenyl ether Colloid-facilitated transport E-waste recycling site Undisturbed soil core Groundwater quality

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A Long-Time-Step-Permitting Tracer Transport Model on the Regular Latitude–Longitude Grid

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Advances in Atmospheric Sciences 2024年第3期41卷 493-508页

作者： Jianghao LI Li DONG key laboratory of Earth System modeling and Prediction China Meteorological AdministrationBeijing 100081China State key laboratory of Numerical modeling for Atmospheric Sciences and Geophysical Fluid Dynamics(LASG) Institute of Atmospheric Physics(IAP)Chinese Academy of SciencesBeijing 100029China State key laboratory of Severe Weather(LaSW) Chinese Academy of Meteorological SciencesChina Meteorological AdministrationBeijing 100081China College of Earth and Planetary Sciences University of Chinese Academy of SciencesBeijing 100049China

If an explicit time scheme is used in a numerical model, the size of the integration time step is typically limited by the spatial resolution. This study develops a regular latitude–longitude grid-based global three-dimensional tracer transport model that is computationally stable at large time-step sizes. The tracer model employs a finite-volume flux-form semiLagrangian transport scheme in the horizontal and an adaptively implicit algorithm in the vertical. The horizontal and vertical solvers are coupled via a straightforward operator-splitting technique. Both the finite-volume scheme's onedimensional slope-limiter and the adaptively implicit vertical solver's first-order upwind scheme enforce monotonicity. The tracer model permits a large time-step size and is inherently conservative and monotonic. Idealized advection test cases demonstrate that the three-dimensional transport model performs very well in terms of accuracy, stability, and efficiency. It is possible to use this robust transport model in a global atmospheric dynamical core.

关键词： tracer transport numerical stability latitude–longitude grid

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Evaluation of suitability,adaptability,and reserve potential of construction land on the Qinghai-Tibet Plateau

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Journal of Geographical Sciences 2024年第1期34卷 41-61页

作者： YANG Hua XU Yong ZHOU Kan WANG Lijia XU Lin key laboratory of Regional Sustainable Development modeling Institute of Geographic Sciences and Natural Resources ResearchCASBeijing 100101China University of Chinese Academy of Sciences Beijing 100049China

Construction land is the leading carrier of human activities such as production and living.Evaluating the construction land suitability(CLS)on the Qinghai-Tibet Plateau(QTP)holds significant implications for harmonizing the relationship between ecological protection and human activity and promoting population and industry layout optimization.However,no relevant studies provide a complete CLS assessment of the QTP.In this study,we developed a model-based CLS evaluation framework coupling of pattern and process to calculate the global CLS on the QTP based on a previously developed CLS evaluation model.Then,using the land-use data of 1990,2000,2010,and 2020,we examined the adaptability of existing construction land(ECL)to the CLS assessment result through the adaptability index and vertical gradient index and further analyzed the limitations of maladaptive construction land.Finally,we calculated the potential area of reserve suitable construction land.This article includes four conclusions:(1)The highly suitable,suitable,moderately suitable,marginally suitable,and unsuitable CLS classes cover areas of 0.33×10^(4)km^(2),10.42×10^(4)km^(2),18.06×10^(4)km^(2),24.12×10^(4)km^(2),and 205.29×10^(4)km^(2),respectively.Only approximately 11%of the study area on the QTP is suitable for large-scale permanent construction land,and approximately 79.50%of the area is unsuitable under current economic and technological conditions.(2)The ECL adaptability index is 85.16%,85.93%,85.18%,and 78.01%during 1990–2020,respectively,with an average adaptability index exceeding 80%on the QTP.The ECL distribution generally conforms to construction land suitable space characteristics but with a significant spatial difference.(3)From 1990 to 2020,the maladaptive ECL was dominated by rural settlement land,transport land,and special land,with a rapidly increasing proportion of urban and other construction land.The maladaptive ECL is constrained by both elevation and slope in the southern Qinghai Plateau,the Hengduan Mountains,and the Qilian Mount

关键词： land resource construction land suitability existing construction land adaptability human activity Qinghai-Tibet Plateau

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Tailoring the surface and interface structures of photocatalysts to enhance hydrogen production

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Science China Chemistry 2024年第4期67卷 1161-1174页

作者： Tao Zhang Pengfei Wang Shuai Yue Fei Li Zhiyong Zhao Sihui Zhan MOE key laboratory of Pollution Processes and Environmental Criteria/Tianjin key laboratory of Environmental remediation and Pollution Control College of Environmental Science and EngineeringNankai UniversityTianjin 300350China

Photocatalytic water splitting using semiconductor photocatalysts is a promising approach for the production of carbon-neutral,sustainable and clean hydrogen fuel.However,the separation and transport of photoinduced carriers are generally considered to be rate-limiting steps,and their low efficiency remains a major challenge.Therefore,much effort has been devoted to developing new strategies in surface/interface engineering of photocatalysts to improve the dynamics of charge separation/transport.This feature article briefly summarizes recent advances in photocatalyst surface/interface engineering by our research group,which have been achieved through the design of various novel photocatalysts,including interfacial modulation,heterostructure construction,heteroatom doping,single atom and diatom sites.The article is divided into three parts:first,we briefly introduce the three key processes involved in solar water splitting and reveal relationships between the properties of nanostructural photocatalysts and the fundamentals of water splitting;second,we detail methods and strategies for surface and interfacial structures to improve the efficiency of the fundamental processes,especially charge separation;finally,we explore prospects for photocatalytic water splitting applications.This article provides a valuable resource and strategies for researchers currently working in the field of photocatalytic water splitting.

关键词： photocatalytic water splitting surface/interface structures dual-functional photocatalysis

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A Neural-network-based Alternative Scheme to Include Nonhydrostatic Processes in an Atmospheric Dynamical Core

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Advances in Atmospheric Sciences 2024年第6期41卷 1083-1099,I0002,I0003页

作者： Yang XIA Bin WANG Lijuan LI Li LIU Jianghao LI Li DONG Shiming XU Yiyuan LI Wenwen XIA Wenyu HUANG Juanjuan LIU Yong WANG Hongbo LIU Ye PU Yujun HE Kun XIA Ministry of Education key laboratory for Earth System modeling and Department of Earth System ScienceTsinghua UniversityBeijing 100084China State key laboratory of Numerical modeling for Atmospheric Sciences and Geophysical Fluid Dynamics Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China Innovation Group 311020008 Southern Marine Science and Engineering Guangdong LaboratoryZhuhai 519000China Shanghai Ecological Forecasting and Remote Sensing Center Shanghai 200030China key laboratory of Earth System modeling and Prediction China Meteorological AdministrationBeijing 100081China College of Ocean Sciences University of Chinese Academy of SciencesBeijing 100049China

Here,a nonhydrostatic alternative scheme(NAS)is proposed for the grey zone where the nonhydrostatic impact on the atmosphere is evident but not large enough to justify the necessity to include an implicit nonhydrostatic solver in an atmospheric dynamical core.The NAS is designed to replace this solver,which can be incorporated into any hydrostatic models so that existing well-developed hydrostatic models can effectively serve for a longer time.Recent advances in machine learning(ML)provide a potential tool for capturing the main complicated nonlinear-nonhydrostatic relationship.In this study,an ML approach called a neural network(NN)was adopted to select leading input features and develop the NAS.The NNs were trained and evaluated with 12-day simulation results of dry baroclinic-wave tests by the Weather Research and Forecasting(WRF)model.The forward time difference of the nonhydrostatic tendency was used as the target variable,and the five selected features were the nonhydrostatic tendency at the last time step,and four hydrostatic variables at the current step including geopotential height,pressure in two different forms,and potential temperature,respectively.Finally,a practical NAS was developed with these features and trained layer by layer at a 20-km horizontal resolution,which can accurately reproduce the temporal variation and vertical distribution of the nonhydrostatic tendency.Corrected by the NN-based NAS,the improved hydrostatic solver at different horizontal resolutions can run stably for at least one month and effectively reduce most of the nonhydrostatic errors in terms of system bias,anomaly root-mean-square error,and the error of the wave spatial pattern,which proves the feasibility and superiority of this scheme.

关键词： neural network nonhydrostatic alternative scheme atmospheric model dynamical core

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Pd Pt VO_(x)/CeO_(2)-ZrO_(2):Highly efficient catalysts with good sulfur dioxide-poisoning reversibility for the oxidative removal of ethylbenzene

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Journal of Environmental Sciences 2024年第4期138卷 153-166页

作者： Jia Wang Yuxi Liu Jiguang Deng Lin Jing Xiuqing Hao Xing Zhang Xiaohui Yu Hongxing Dai beijing key laboratory for Green Catalysis and Separation Key Laboratory of Beijing on Regional Air Pollution ControlKey Laboratory of Advanced Functional MaterialsEducation Ministry of ChinaLaboratory of Catalysis Chemistry and NanoscienceDepartment of Chemical EngineeringFaculty of Environment and LifeBeijing University of TechnologyBeijing 100124China

The PdPtVO_(x)/CeO_(2)-ZrO_(2)(PdPtVO_(x)/CZO)catalysts were obtained by using different approaches,and their physical and chemical properties were determined by various techniques.Catalytic activities of these materials in the presence of H_(2)O or SO_(2)were evaluated for the oxidation of ethylbenzene(EB).The PdPtVO_(x)/CZO sample exhibited high catalytic activity,good hydrothermal stability,and reversible sulfur dioxide-poisoning performance,over which the specific reaction rate at 160℃,turnover frequency at 160℃(TOF_(Pd or Pt)),and apparent activation energy were 72.6 mmol/(g_(Pt)·sec)or 124.2 mmol/(g_(Pd)·sec),14.2 sec^(-1)(TOF_(Pt))or 13.1 sec^(-1)(TOF_(Pd)),and 58 k J/mol,respectively.The large EB adsorption capacity,good reducibility,and strong acidity contributed to the good catalytic performance of PdPtVO_(x)/CZO.Catalytic activity of PdPtVO_(x)/CZO decreased when 50 ppm SO_(2)or(1.0 vol.%H_(2)O+50 ppm SO_(2))was added to the feedstock,but was gradually restored to its initial level after the SO_(2)was cut off.The good reversible sulfur dioxide-resistant performance of PdPtVO_(x)/CZO was associated with the facts:(i)the introduction of SO_(2)leads to an increase in surface acidity;(ii)V can adsorb and activate SO_(2),thus accelerating formation of the SO_(x)^(2-)(x=3 or 4)species at the V and CZO sites,weakening the adsorption of sulfur species at the PdPt active sites,and hence protecting the PdPt active sites to be not poisoned by SO_(2).EB oxidation over PdPtVO_(x)/CZO might take place via the route of EB→styrene→phenyl methyl ketone→benzaldehyde→benzoic acid→maleic anhydride→CO_(2)and H_(2)O.

关键词： Ceria-zirconia Supported palladium-platinum-vanadium catalyst Volatile organic compound Ethylbenzene oxidation Sulfur dioxide resistance

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Characteristics and triggering mechanisms of early negative Indian Ocean Dipole

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Acta Oceanologica Sinica 2024年第3期43卷 59-65页

作者： Yue Fang Shuangwen Sun Yongcan Zu Jianhu Wang Lin Feng First Institute of Oceanography and Key Laboratory of Marine Science and Numerical ModelingMinistry of Natural ResourcesQingdao 266061China laboratory for Regional Oceanography and Numerical modeling Qingdao Marine Science and Technology CenterQingdao 266237China Shandong key laboratory of Marine Science and Numerical modeling Qingdao 266061China

Negative Indian Ocean Dipole(nIOD)can exert great impacts on global climate and can also strongly influence the climate in China.Early nIOD is a major type of nIOD,which can induce more pronounced climate anomalies in summer than La Niña-related nIOD.However,the characteristics and triggering mechanisms of early nIOD are unclear.Our results based on reanalysis datasets indicate that the early nIOD and La Niña-related nIOD are the two major types of nIOD,and the former accounts for over one third of all the nIOD events in the past six decades.These two types of nIODs are similar in their intensities,but are different in their spatial patterns and seasonal cycles.The early nIOD,which develops in spring and peaks in summer,is one season earlier than the La Niña-related nIOD.The spatial pattern of the wind anomaly associated with early nIOD exhibits a winter monsoon-like pattern,with strong westerly anomalies in the equatorial Indian Ocean and eastly anomalies in the northern Indian Ocean.Opposite to the triggering mechanism of early positve IOD,the early nIOD is induced by delayed Indian summer monsoon onset.The results of this study are helpful for improving the prediction skill of IOD and its climate impacts.

关键词： Indian Ocean Dipole(IOD) triggering mechanism Indian summer monsoon seasonal cycle negative IOD

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In-situ construction of abundant active centers on hierarchically porous carbon electrode toward high-performance phosphate electrosorption: Synergistic effect of electric field and capture sites

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Green Energy & Environment 2024年第1期9卷 126-137页

作者： Peng Zhang Fukuan Li Mingming He Silu Huo Xueli Zhang Benqiang Cen Dezhi Fang Kexun Li Hao Wang College of Environmental Science and Engineering Nankai UniversityTianjin300350China MOE key laboratory of Pollution Processes and Environmental Criteria Tianjin Key Laboratory of Environmental Remediation and Pollution ControlTianjin Key Laboratory of Environmental Technology for Complex Trans-Media PollutionNankai UniversityTianjin300350China State key laboratory of Simulation and Regulation of Water Cycles in River Basins China Institute of Water Resources and Hydropower ResearchBeijing100038China

Phosphate removal is crucial for eutrophication control and water quality improvement.Electro-assisted adsorption,an eco-friendly elec-trosorption process,exhibited a promising potential for wastewater treatment.However,there are few works focused on phosphate electro-sorption,and reported electrodes cannot attach satisfactory removal capacities and rates.Herein,electro-assisted adsorption of phosphate via in-situ construction of La active centers on hierarchically porous carbon(LaPC)has been originally demonstrated.The resulted LaPC composite not only possessed a hierarchically porous structure with uniformly dispersed La active sites,but also provided good conductivity for interfacial electron transfer.The LaPC electrode achieved an ultrahigh phosphate electrosorption capability of 462.01 mg g^(-1) at 1 V,outperforming most existing electrodes.The superior phosphate removal performance originates from abundant active centers formed by the coupling of electricﬁeld and capture sites.Besides,the stability and selectivity toward phosphate capture were maintained well even under comprehensive conditions.Moreover,a series of kinetics and isotherms models were employed to validate the electrosorption process.This work demonstrates a deep understanding and promotes a new level of phosphate electrosorption.

关键词： Electro-assisted adsorption Electrosorption Phosphate removal Active centers MOF-derived carbon

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