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Constructing Co and Zn Atomic Pairs in Core-Shell Co3S4/Nc@Zns/Nc Derived from Mof-on-Mof Nanostructures for Enhanced Photocatalytic Co2 Reduction to C2h4

SSRN

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SSRN 2024年

作者： Huang, Lili Mo, Shengpeng Zhao, Xin Zhou, Jiangjing Zhou, Xiaobin Zhang, Yanan Fan, Yinming Xie, Qinglin Li, Bing Li, Junhua College of Environment Science and Engineering Guilin University of Technology Guilin541004 China State Key Joint Laboratory of Environment Simulation and Pollution Control School of Environment Tsinghua University Beijing100084 China Jiangsu Zhongchuang Qingyuan Technology Co. Ltd Yancheng224001 China

Herein, a core-shell structured Co3S4/NC@ZnS/NC heterojunction has been constructed via elaborately synthesizing metal-organic framework (MOF)-on-MOF precursors (ZIF-67@ZIF-8) and following controlled carbonization-sulfidation processes. The developed Co3S4/NC@ZnS/NC achieves higher performances for CO2 photoreduction with water vapor towards CO (28.44 μmol g−1 h−1), CH4 (1.93 μmol g−1 h−1) and C2H4 (12.33 μmol g−1 h−1) in a continuous-flow condition under visible-light irradiation. 13CO2 isotope tracer analysis verifies that CO, CH4 and C2H4 originate from the carbon source of CO2. Experiment and DFT calculations confirm that constructing an electron transport layer (ZnS/NC) in Co3S4/NC@ZnS/NC can contribute to a feasible channel for the enhanced separation and transfer of charge carriers. In heterojunction, non-bonding Co and Zn atomic pairs as adsorption sites synergistically participate in the CO2 activation through the unique electron transport channel and acquire the lower energy barriers of COOH* formation. Moreover, in situ DRIFTS reveals the key intermediates and possible conversion pathways. © 2024, The Authors. All rights reserved.

关键词： Zinc sulfide

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Peroxidase-like activity of widely-used commercial inorganic pigments induces oxidative stress and antibiotic degradation: Implications for health risks

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Science of the Total environment 2025年 958卷 177979页

作者： He, Kexin Sun, Chenxi Yang, Shuxue Liu, Huiting Fu, Heyun Qu, Xiaolei State Key Laboratory of Pollution Control and Resource Reuse School of the Environment Nanjing University Jiangsu 210023 China School of Environmental and Chemical Engineering Shenyang Ligong University Liaoning 110159 China

Inorganic pigments, which often contain significant amounts of nanoparticles, are crucial chemicals for human life. They are produced in massive quantities and widely used in consumer products, food, and pharmaceuticals. Herein, we reported that a variety of commonly used commercial inorganic pigments possess peroxidase-like activity, catalyzing hydrogen peroxide (H2O2) decomposition into reactive oxygen species, primarily hydroxyl radical ([rad]OH) and superoxide radical anion (O2[rad]−). The catalytic activity of inorganic pigments exhibits saturation kinetics as described by the Michaelis-Menten model, with optimal pH and temperature conditions that can be found in the human body. The enzyme-mimicking activity is strongly correlated with the formation of [rad]OH (R2 = 0.98), indicating the radical-mediated reaction pathway. The peroxidase-like activity of inorganic pigments can induce significant oxidative stress at health-relevant H2O2 concentrations (3–30 μM), as demonstrated by the ascorbic acid assay. Additionally, the peroxidase-like activity of inorganic pigments is able to mediate the oxidation of tetracycline, with oxidation rate constants positively correlated with the pigments' peroxidase-like activity. The discovery of peroxidase-like activity of commercial inorganic pigments sheds light on the reported oxidative stress exerted by these pigments and has important implications for the health risk assessment of inorganic food and pharmaceutical colorants, as well as colored consumer products. © 2024 Elsevier B.V.

关键词： Aspartame

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The “neighbor avoidance effect” of microplastics on bacterial and fungal diversity and communities in different soil horizons

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environmental Science and Ecotechnology 2021年第4期8卷 13-21页

作者： Hong Yu Ying Zhang Wenbing Tan State Key Laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental SciencesBeijing100012China State Environmental Protection Key Laboratory of Simulation and Control of Groundwater Pollution Chinese Research Academy of Environmental SciencesBeijing100012China

Microplastics are a new type of environmental pollutant,and pose a serious threat to soil *** is important to study microplastics effects on soil microorganisms to better understand their effects on terrestrial ***,we collected soil and microplastic samples from corn,pepper,peanut and cucumber fields in Shunyi District,Beijing,China,and used Illumina MiSeq high-throughput sequencing technology to analyze bacterial and fungal community composition and *** focused on microplastic surface and its surrounding“rhizosphere-like”soil in the 0e10 cm(humus)and 10e20 cm(eluvial)deep *** richness and diversity on microplastic surface were significantly lower than those in surrounding“rhizosphere-like”soil,and microbial richness and diversity were reduced to a greater extent in the humus horizon than in the eluvial *** likely enriched the microbes involved in their *** relative abundance levels of Cyanobacteria and Basidiomycota on microplastic surfaces were significantly higher than those in surrounding“rhizosphere-like”soil,while the relative abundance levels of Acidobacteria,Chloreflexi,and Mortierellomycota were higher in“rhizosphere-like”***,the relative abundance levels of pathways related to human diseases,animal pathogen,and fungal parasites were significantly higher on microplastic surfaces than in“rhizosphere-like”*** results show that the microbial diversity,richness,community structure and function between microplastic surfaces and surrounding“rhizosphere-like”soil are significantly different,leading to a“rhizosphere-like neighbor avoidance effect”between microplastic surfaces and the surrounding soil.

关键词： Microplastics Microbial diversity Community structure Rhizosphere Metabolic function

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Determination of 27 pharmaceuticals and personal care products(PPCPs)in water:The benefit of isotope dilution

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Frontiers of environmental Science & Engineering 2020年第1期14卷 127-136页

作者： Xueqi Fan Jie Gao Wenchao Li Jun Huang Gang Yu State Key Joint Laboratory of Environment Simulation and Pollution Control(SKJLESPC) Beijing Key Laboratory for Emerging Organic Contaminants Control(BKLEOC)School of EnvironmentTsinghua UniversityBeijing 100084China CSD IDEA(Beijing)Environment Test&Analysis Co. Ltd.Beijing 100192China

Pharmaceuticals and personal care products(PPCPs)are a unique group of emerging and nonpersistent *** this study,27 PPCPs in various water samples were extracted by solid phase extraction(SPE),and determined by isotope dilution method using liquid chromatography coupled to tandem triple quadruple mass spectrometer(LC-MS/MS).A total of 27 isotopically labeled standards(ILSs)were applied to correct the concentration of PPCPs in spiked ultrapure water,drinking water,river,effluent and influent *** corrected recoveries were 73%-122%with the relative standard deviation(RSD)<16%,except for *** matrix effect for all kinds of water samples was<22%and the method quantitation limits(MQLs)were 0.45-8.6 ng/*** developed method was successfully applied on environmental water *** SPE extracts of spiked ultrapure water,drinking water,river and wastewater effluent were stored for 70 days,and the ILSscorrected recoveries of 27 PPCPs were obtained to evaluate the correction ability of ILSs in the presence of variety *** recoveries of 27 PPCPs over 70 days were within the scope of 72%-140%with the recovery variation<37%in all *** isotope dilution method seems to be of benefit when the extract has to be stored for long time before the instrument analysis.

关键词： Pharmaceuticals and personal care products(PPCPs) Isotopically labeled standard(ILSs) Water Solid-phase extraction(SPE) LC-MS/MS

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Electrolyte dependence for the electrochemical decarboxylation of medium-chain fatty acids (n-octanoic acid) into fuel on Pt electrode

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Materials Reports(Energy) 2024年第2期4卷 64-70页

作者： Zhenmin Zhang Dezhang Ren Dian Zhang Tiantian Hu Congyuan Zeng Nengneng Xu Zhibao Huo Jinli Qiao College of Marine Ecology and Environment Shanghai Ocean UniversityShanghai201306PR China Department of Mechanical Engineering Southern University and A&M CollegeBaton RougeLA70807USA State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Environmental Science and EngineeringDonghua UniversityShanghai201620PR China Shanghai Institute of Pollution Control and Ecological Security Shanghai200092PR China

The deoxygenation of organic acids, important biomass feedstocks and derivatives, to synthesize hydrocarbon products under mild electrochemical conditions, holds significant importance for the production of carbon-neutral biofuels. There is still limited research on the influential factors of the electrochemical decarboxylation reaction of medium-chain fatty acids. In this study, n-octanoic acid (OA) was chosen as the research subject to investigate the electrochemical decarboxylation behavior of OA on a platinum electrode, focusing on the influence of different alkali metal cations (Li^(+), Na^(+), K^(+)), common anions (SO^(4)^(2−), Cl^(−)), and electrolyte pH. It was found that KOH as an electrolyte exhibited the best performance for OA. Possibly, the larger size of K^(+) increased the alkalinity of the electrode surface, facilitating OA deprotonation. LiOH electrolyte reduced the solubility of OA, thereby inhibiting the decarboxylation reaction. SO^(4)^(2−) exhibited a weak promoting effect on the decarboxylation reaction of OA, while Cl^(−) showed no adverse effect although Cl^(−) may adsorb on the electrode surface. Furthermore, unlike short-chain fatty acids, medium-chain OA can only achieve efficient decarboxylation under alkaline conditions due to its solubility properties. This study provides references and foundations for future efforts to enhance the efficiency of electrochemical decarboxylation synthesis of hydrocarbon biofuels from medium-chain fatty acids.

关键词： Fatty acids Kolbe reaction Decarboxylation Hydrocarbon Electrolyte

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Anaerobic stabilization and landscape utilization of rural sewage sludge from the enhanced membrane coagulation process

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Science of the Total environment 2025年 958卷 177902页

作者： Xu, Heng Wei, Shanghui Chen, Song Wang, Kaijun Holmes, Dawn E. Yuan, Quan Beijing100083 China School of Ecology and Environment Beijing Technology and Business University Beijing100048 China State Key Joint Laboratory of Environment Simulation and Pollution Control School of Environment Tsinghua University Beijing100084 China Department of Physical and Biological Sciences Western New England University 1215 Wilbraham Road SpringfieldMA01119 United States

In this study, enhanced membrane coagulation (EMC) sludge was subjected to various alkaline (pH 7.2, 10, and 11), temperature (35 °C and 55 °C), and duration (0.5 h and 1 day) pretreatment conditions before being inoculated into biogas reactors operated for 176 days. Optimal pretreatment (pH 11, 55 °C, and 1 day) effectively hydrolyzed particulate COD to SCOD (8435 ± 121 mg/L). Higher pH levels also facilitated the dissolution of amphoteric aluminum-phosphorus (Al-P) compounds, enhancing phosphorus release (91.8 mg/L) from the sludge. This alkaline pretreatment, especially under optimal conditions, significantly increased biogas production and methane concentrations in long-term semi-continuous anaerobic digesters, with methane yields of 188.4 mL/gVS. The microbial community structure in all three reactors exhibited similar shifts, with saccharolytic and proteolytic fermentative bacteria dominating early stages and Thermovirga and an uncultured bacterium (Run-SP154) prevalent in later stages. Methanothrix, an acetotrophic methanogen, dominated the archaeal community in the inoculum (>91 %) and remained prominent (>40 %) throughout the experiment, while hydrogenotrophic methanogens from the genus Methanolinea increased over time, accounting for >24 % of the sequences in the final stages. Additionally, the feasibility of using EMC digestate as fertilizer for mulberry plants was tested, showing that digestate from optimally pretreated sludge promoted better growth than conventional chemical fertilizers. This suggests that this approach is a promising method for decentralized sewage treatment systems. © 2024

关键词： Anaerobic digestion

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Kinetic Modeling of Secondary Organic Aerosol in a Weather-Chemistry Model: Parameterizations, Processes, and Predictions for GOAmazon

ACS ES&T Air

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ACS ES&T Air 2025年第2期2卷 249-263页

作者： Yicong He Kelsey R. Bilsback Manish Shrivastava Rahul A. Zaveri John E. Shilling John H. Seinfeld Bin Zhao Shuxiao Wang Christopher D. Cappa Jeffrey R. Pierce Shantanu H. Jathar Department of Mechanical Engineering Colorado State University Fort Collins Colorado 80523 United States；State Key Joint Laboratory of Environmental Simulation and Pollution Control School of Environment Tsinghua University Beijing 100084 China；State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex Beijing 100084 China Department of Mechanical Engineering Colorado State University Fort Collins Colorado 80523 United States；PSE Healthy Energy Oakland California 94612 United States Pacific Northwest National Laboratory Richland Washington 99354 United States Divison of Chemistry and Chemical Engineering California Institute of Technology Pasadena California 91125 United States State Key Joint Laboratory of Environmental Simulation and Pollution Control School of Environment Tsinghua University Beijing 100084 China；State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex Beijing 100084 China Department of Atmospheric Science Colorado State University Fort Collins Colorado 80521 United States Department of Civil and Environmental Engineering University of California Davis Davis California 95616 United States Department of Mechanical Engineering Colorado State University Fort Collins Colorado 80523 United States

Secondary organic aerosol (SOA) forms and evolves in the atmosphere through many pathways and processes, over diverse spatial and time scales. Hence, there is a need to represent these widely varying kinetic processes in large-scale atmospheric models to allow for accurate predictions of the abundance, properties, and impacts of SOA. In this work, we integrated a kinetic, process-level model (simpleSOM-MOSAIC) into a weather-chemistry model (WRF-Chem) to simulate the oxidation chemistry and microphysics of atmospheric SOA. simpleSOM-MOSAIC simulates multigenerational gas-phase chemistry, autoxidation reactions, aqueous chemistry, heterogeneous oxidation, oligomerization, and phase-state-influenced gas/particle partitioning of SOA. As a case study, the integrated WRF-Chem-simpleSOM-MOSAIC (WC-SSM) model was used to simulate the photochemical evolution downwind of a large city (Manaus, Brazil) in the Amazon and, in turn, study the anthropogenic and biogenic interactions in an otherwise pristine environment. Consistent with previous work, we found that OA was enhanced by up to a factor of 4 in the urban plume due to elevated hydroxyl radical (OH) concentrations, relative to the background, and that this OA was dominated by SOA from biogenic precursors (80%). In addition to accurately simulating the OA enhancement in the urban plume, the model reproduced the magnitude of the OA oxygen-to-carbon (O:C) ratio and broadly tracked the evolution of the aerosol number size distribution. Our work highlights the importance of including an integrated, kinetic representation of SOA processes in an atmospheric model.

关键词：

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Impacts of strong El Ninon summertime near-surface ozone over China

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Atmospheric and Oceanic Science Letters 2022年第4期15卷 13-18页

作者： Mengyun Li Yang Yang Pinya Wang Dongsheng Ji Hong Liao Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control Jiangsu Collaborative Innovation Center of Atmospheric Environment and Equipment TechnologySchool of Environmental Science and EngineeringNanjing University of Information Science and TechnologyNanjingChina State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry Institute of Atmospheric PhysicsChinese Academy of SciencesBeijingChina

The influences of strong El Nino events(1997/98 and 2015/16)on summertime near-surface ozone(O_(3))concentrations over China are investigated using the GEOS-Chem *** results show that near-surface O_(3) concentrations increased by a maximum of 6 ppb(parts per billion)during the summer of the developing phase of the 1997/98 El Nino in northeastern China,mainly due to the increased chemical production related to the hot and dry ***,the O_(3) concentration increased by 3 ppb during the developing summer of both the 1997/98 and 2015/16 El Nino in southern *** was linked to the weakened prevailing monsoon winds,which led to the accumulation of O_(3) in southern *** contrast,in the summer of the decaying phase of the two El Nino events,O_(3) concentrations decreased over many regions of China when the El Nino reversed to the cooling *** highlights that El Nino plays an important role in modulating near-surface O_(3) concentrations over China.

关键词： El Nino Ozone GEOS-Chem

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Simulating Micropollutant Abatement During Cobalt Mediated Peroxymonosulfate Process by Probe-Based Kinetic Models

SSRN

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SSRN 2022年

作者： Gao, Lingwei Guo, Yang Huang, Jun Wang, Bin Deng, Shubo Yu, Gang Wang, Yujue School of Environment Beijing Key Laboratory for Emerging Organic Contaminants Control State Key Joint Laboratory of Environmental Simulation and Pollution Control Tsinghua University Beijing100084 China

Prediction of micropollutant abatement during advanced oxidation processes by modelling can provide valuable information to optimize the process for efficient water treatment. In this study, a probe-based kinetic model was developed to simulate micropollutant abatement during water treatment by a cobalt-mediated peroxymonosulfate (Co/PMS) process. Eight micropollutants (atrazine, primidone, sulfisoxazole, sulfamethoxypyridazine, gemfibrozil, chloramphenicol, p -chlorobenzoic acid, and perfluorooctanoic acid) were spiked in various water matrices (synthetic water and real surface water), which were then treated by the Co/PMS process. By following the decay of PMS, atrazine, and primidone (as sulfate and hydroxyl radical ( [[EQUATION]] and • OH) probes) [[EQUATION]] during the process, the exposures of PMS, [[EQUATION]] and • OH were calculated using the model. Then, based on the determined exposures, the abatement efficiencies of the other micropollutants could be reasonably predicted with the model. The results indicate that by using a couple of probes to measure the [[EQUATION]] and • OH exposures, the model can be used for the generalized prediction of the abatement of various micropollutants during water treatment by the Co/PMS process. In addition, modelling results show that for a given water matrix, the ratios of [[EQUATION]] and • OH concentrations to PMS concentrations (R SP and R HP ) are almost constant during the Co/PMS process. This finding allows the transient concentrations of [[EQUATION]] and • OH to be quantified based on the constant R SP and R HP ratios and the PMS concentrations observed during the process. The results of this study suggest that the probe-based kinetic models can provide a useful tool to characterize the persulfate-based process and to predict the abatement efficiencies of various micropollutants during water treatment. © 2022, The Authors. All rights reserved.

关键词： Kinetic parameters

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Releases of Microplastics and Chemicals from Nonwoven Polyester Fabric-Based Polyurethane Synthetic Leather by Photoaging

SSRN

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SSRN 2023年

作者： Shi, Yanqi Huang, Hexinyue Zheng, Lezhou Tian, Yechao Gong, Zhimin Wang, Jiahao Li, Wentao Gao, Shixiang State Key Laboratory of Pollution Control and Resource Reuse School of the Environment Nanjing University Jiangsu Nanjing210093 China

The nonwoven PET fabrics are chemically, mechanically and thermally treated fiber aggregate without weaving, knitting or braiding, which could be used as a base to make polyurethane (PU) synthetic leather through a series of processing. Our research systematically compared the photoaging behaviors of pure non-woven PET base fabric (NPET-P) and PU synthetic leather (nonwoven PET-base fabrics with PU coating, NPET-U), and their possibilities for microplastic fibers (MPFs) generation and chemical transformation in water. NPET-U was found at a higher oxidation degree with higher O/C ratios and more distinct changes in chemical structures but a slower degradation speed with postponed MPFs release than NPET-P. Different spinning ways of fabrics partly affected the resistance of MPFs release, but the difference between nonwoven and interlocked fabrics was within an order of magnitude. And sunlight aging of fabrics for 365 days approximately equaled 91.9-100.6 hours in the laboratory, which indicated the lab accelerated experiments to simulate natural sunlight aging was extraordinarily intense. Furthermore, elemental concentrations in original fabrics and the leachate of 360 h light aged fabrics were characterized using the inductively coupled plasma optical emission spectrometer (ICP-OES) and analyzed by principal component analysis (PCA). The organic components of the leachate were separated according to their molecular weight with the changes of dissolved organic carbon (DOC), dissolved organic nitrogen (DON), and the UV response over aging time. UV stimulation aggravated the role of plastic polymers as disinfection by-product (DBP) precursors. Nevertheless, NPET-U had similar formation potentials of nitrogen-containing DBPs with NPET-P, even though it could produce more nitrogen-contained chemicals. The discussion lucubrated the potential risks of the production of MPFs and chemical release in the leachate with regard to combined plastic pollution. © 2023, The Authors.

关键词： Weaving

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