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Decipher Factors controlling Sulfonamides Adsorption Onto Mesoporous Carbon

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SSRN 2022年

作者： Zhao, Hongjun Lyu, Yitao Hu, Jingrun Li, Min Sun, Weiling College of Environmental Science and Engineering Beijing Forestry University Beijing100083 China Key Lab for Source Control Technology of Water Pollution Beijing Forestry University Beijing100083 China College of Environmental Sciences and Engineering Peking University Beijing100871 China The Key Laboratory of Water and Sediment Sciences Ministry of Education Beijing100871 China State Environmental Protection Key Laboratory of All Material Fluxes in River Ecosystems Beijing100871 China International Joint Laboratory for Regional Pollution Control Ministry of Education Beijing100871 China

Mesoporous carbons (MCs) exhibit excellent removal efficiencies to various organic chemicals. However, how and what extent the properties of chemicals influence their adsorption onto MCs are poorly understood. Here, we investigated the adsorption of 22 sulfonamides (SAs) onto four MCs, and further uncovered the adsorption mechanisms and major factors determining the adsorption of SAs by density functional theory calculation and partial least-squares path model (PLS-PM). The results showed that the adsorption constants of linear and Freundlich isotherms (log K D and log K F ) displayed positive relationships with excess molar refraction (E) and McGowan’s molar volume (V), while the Freundlich nonlinearity coefficient (n) presented a negative correlation with E and V. The PLS-PM model further revealed that the binding energies of π-π interactions (BE(π-π)) and hydrogen bond (BE(H)) and the hydrophobicity (log K ow ) of SAs were the direct factors influencing the adsorption. Among them, BE(π-π) displayed the largest impacts (λ = -0.731, p 0.05) on log K D . Five molecular descriptors, E, V, energy of the highest occupied molecular orbital (E HOMO ), hardness (H), and most positive net charge on carbon atom (Q c + ), were selected as the indirect factors affecting log K D . The adsorption amounts of most SAs decreased with increasing pH, due to the increased electrostatic repulsion, reduced log K ow of SAs, and declined BE(π-π) and (BE(H) at higher pH. This study is the first attempt to decipher quantitatively the direct and indirect factors determing the adsorption of SAs onto MCs. © 2022, The Authors. All rights reserved.

关键词： Least squares approximations

Unit-Based Emissions and environmental Impacts of Industrial Condensable Particulate Matter in China in 2020

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SSRN 2022年

作者： Wang, Kun Gao, Jiajia Liu, Kaiyun Tong, Yali Dan, Mo Zhang, Xiaoxi Liu, Chunlei Department of Air Pollution Control Institute of urban safety and environmental science Beijing academy of science and technology Beijing100054 China Key Laboratory of Marine Environmental Science and Ecology Ministry of Education Ocean University of China Qingdao266100 China State Key Joint Laboratory of Environment Simulation and Pollution Control School of Environment Tsinghua University Beijing100084 China Shanghai Minhang District Qingyue Environmental Protection IT Service Center Shanghai201199 China

The emission of condensable particulate matter (CPM) and its environmental impacts are arousing concern in China with the effective control of filter particulate matter (FPM). This study established an up-to-date and unit-based CPM emission inventory for industrial sectors and systematically evaluated the effects of CPM on primary and secondary PM2.5 in China. In 2020, the national CPM emissions total for industrial sectors was estimated to be 0.98 Tg with uncertainty from −49% to 66%, including 0.62 Tg of organic CPM (CPMorg) and 0.36 Tg of inorganic CPM (CPMin). Totals of 62%, 23% and 8% CPM were emitted from coal-fired power plants, coal-fired industrial boilers and sinter plants, respectively. By filling CPM emissions in PM2.5 simulation, the normalized mean bias (NMB) of model to observation was improved from −27% to −14% in East, North and Central China. The 4 μg/m3 PM2.5 concentration was attributed to CPM emissions in this region, accounting for 10% of observations. On "polluted" days (PM2.5 >75 μg/m3), industrial CPM emissions can contribute 7 μg/m3 PM2.5 in North China, wherein more than 75% of the secondary PM2.5 can be caused by CPMorg emissions. Therefore, China should focus on controlling CPM from coal combustion to ensure continuous air quality improvement. © 2022, The Authors. All rights reserved.

关键词： Coal

Multi-scale analysis of the chemical and physical pollution evolution process from pre-co-pollution day to PM2.5 and O3 co-pollution day

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Science of the Total Environment 2024年 945卷 173729页

作者： Wang, Feng Zhang, Chun Ge, Yi Zhang, Zhang Shi, Guoliang Feng, Yinchang School of Environmental Science and Safety Engineering Tianjin University of Technology Tianjin300384 China Shaanxi Province Environmental Monitoring Center Xi'an710054 China State Environmental Protection Key Laboratory of Urban Ambient Air Particulate Matter Pollution Prevention and Control Tianjin Key Laboratory of Urban Transport Emission Research College of Environmental Science and Engineering Nankai University Tianjin300350 China Cooperative Laboratory for Atmospheric Environment-Health Research College of Environmental Science and Engineering Nankai University Tianjin300350 China

PM2.5 and O3 are two of the main air pollutants that have adverse impacts on climate and human health. The evolution process of PM2.5 and O3 co-pollution are of concern because of the increased frequency of PM2.5 and O3 co-pollution days. Here, we examined the chemical coupling and revealed the driving factors of the PM2.5 and O3 co-pollution evolution process from cleaning day, PM2.5 pollution day, or O3 pollution day, applied by theoretical analysis and model calculation methods. The results demonstrate that PM2.5 and O3 co-pollution day frequently occurred with high concentrations of gaseous precursors and higher sulfur oxidation ratio (SOR) and nitrogen oxidation ratio (NOR), which we attribute to the enhancement of atmospheric oxidation capacity (AOC). The AOC is positively correlated with O3 and weakly correlated with PM2.5. In addition, we found that the correlation coefficients of PM2.5-NO2 (0.62) were higher than that of PM2.5-SO2 (0.32), highlighting the priority of NOx controlling to mitigate PM2.5 pollution. Overall, our discovery can provide scientific evidence to design feasible solutions for the controlling PM2.5 and O3 co-pollution process. © 2024

关键词： Oxidation

Hydrogeochemical Analysis and Paleo-Hydrogeological Modeling of Shallow Groundwater Salinization Processes in North China Plain

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SSRN 2024年

作者： Huang, Yihong Yang, Jie Yu, Xuan Wang, Shijie Xie, Xianjun Li, Junxia Wang, Yanxin MOE Key Laboratory of Groundwater Quality and Health China University of Geosciences Wuhan430078 China State Environmental Protection Key Laboratory of Source Apportionment and Control of Aquatic Pollution School of Environmental Studies China University of Geosciences Wuhan430078 China Key Laboratory of Resources and Eco-environmental Geology Geological Experimental Testing Center of Hubei Province Wuhan430034 China State Key Laboratory of Soil and Sustainable Agriculture Institute of Soil Science Chinese Academy of Sciences Nanjing210008 China

Coastal groundwater salinization induced by marine transgression, sea level rising, and/or seawater intrusion due to anthropogenic activities has been a grand challenge for water security worldwide. Protecting the invaluable fresh groundwater resources from salinization necessitates the understanding of the spatial distribution of saline water and its sources. In this study, the process of groundwater salinization in two shallow aquifers of the North China Plain near Bohai Sea was characterized using hydrogeochemical analysis and paleo-hydrogeological modeling. The spatial variation in groundwater chemistry and isotopic composition in the two aquifers reflected the evident influence of paleo-transgression/regression events, while paleo-hydrogeological modeling further confirmed the primary role of several events of marine transgressions in groundwater salinization. Moreover, the fingering process of vertical saline water infiltration by free convection was identified from the results of the modeling, which was constrained by preferential flow paths and low permeability barriers of aquitards. The modeling results show that seawater infiltration was rapid, reaching a depth of 120 m B.S.L. in a short time at an average rate of 23 mm/yr. The trend of downward permeation of shallow saline water may threaten the groundwater quality of deep confined aquifers that sever as the main sources of water supply in coastal area of the North China Plain. © 2024, The Authors. All rights reserved.

关键词： Groundwater resources

Characteristics of Typical Intermediate and Semi Volatile Organic Compounds in Shanghai During China International Import Expo Episode

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SSRN 2023年

作者： An, Taikui Li, Yingjie Wang, Rui Jing, Sheng'ao Gao, Yaqin Liu, Shuyu Dai, Haixia Huang, Cheng Huang, Dandan Lu, Jun College of Chemistry and Chemical Engineering Shanghai University of Engineering Science Shanghai201620 China State Environmental Protection Key Laboratory of Formation and Prevention of Urban Air Pollution Complex Shanghai Academy of Environmental Sciences Shanghai200233 China Guangzhou Institute of Geochemistry Chinese Academy of Sciences Guangzhou510640 China

To ensure good air quality during China International Import Expo (CIIE) episode, stringent emission-reduction measures were implemented in Shanghai. To better assess the efficacy of these measures, this study explored four typical categories of intermediate/semi volatile organic compounds (I/SVOCs), including alkanes (C10–C26 n-alkanes and pristane), EPA-priority polycyclic aromatic hydrocarbons (PAHs), alkylnaphthalenes, benzothiazole (BTH) and chlorobenzenes (CBs), at an urban site of Shanghai before and during two CIIE episodes (2019 and 2020;non-CIIE versus CIIE). The average concentrations of alkanes and PAHs during both 2019 and 2020 CIIE episodes decreased by approximately 41% and 17%, respectively, compared to non-CIIE periods. However, this decline was only observed for BTH and CBs during CIIE-2019. Under atmospheric conditions, the secondary organic aerosol (SOA) production from alkanes, PAHs and BTH together was 671 ± 446 ng/m3, with considerable SOA contributions from dimethylnaphthalenes and BTH. Positive matrix factorization (PMF) source apportionment further revealed that life-related sources making a noticeable contribution (21.6%) except for the commonly concerned gasoline-vehicle sources (31.5%), diesel-related emissions (20.8%), industrial sources (18.6%) and ship emissions (7.5%). Our results provide valuable insights into the effectiveness of the implemented measures, during CIIE episodes, for the reduction of I/SVOCs emissions, and highlight more I/SVOC individual species and life-related sources should be considered for further research and policy design. © 2023, The Authors. All rights reserved.

关键词： Volatile organic compounds

The research on CO oxidation over Ce–Mn oxides: The preparation method effects and oxidation mechanism

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Chemosphere 2023年第1期336卷 139130页

作者： Ye, Zhiping Liu, Yang Nikiforov, Anton Ji, Jiayu Zhao, Bo Wang, Jiade College of Environment Zhejiang University of Technology 18 Chaowang RD Hangzhou310014 China Ghent University Faculty of Engineering Department of Applied Physics Research Unit Plasma Technology Sint-Pietersnieuwstraat 41 Ghent9000 Belgium Zhejiang Tuna Environmental Science & Technology Co. Ltd Shaoxing312071 China State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex Beijing100084 China

A series of CeO2-MnOx for highly efficient catalytical oxidation of carbon monoxide were prepared by citrate sol-gel (C), hydrothermal (H) and hydrothermal-citrate complexation (CH) methods. The outcome indicates that the catalyst generated using the CH technique (CH-1:8) demonstrated the greatest catalytic performance for CO oxidation with a T50 of 98 °C, and also good stability in 1400 min. Compared to the catalysts prepared by C and H method, CH-1:8 has the highest specific surface of 156.1 m2 g−1, and the better reducibility of CH-1:8 was also observed in CO-TPR. It is also observed the high ratio of adsorbed oxygen/lattice oxygen (1.5) in the XPS result. Moreover, characterizations by the TOF-SIMS method indicated that obtained catalyst CH–Ce/Mn = 1:8 had stronger interactions between Ce and Mn oxides, and the redox cycle of Mn3++Ce4+ ↔ Mn4++Ce3+ was a key process for CO adsorption and oxidation process. According to in-situ FTIR, the possible reaction pathway for CO was deduced in three ways. CO directly oxidize with O2 to CO2, CO adsorbed on Mn4+ and Ce3+ reacts with O to form intermediates (COO−) (T > 50 °C) and carbonates (T > 90 °C), which are further oxidized into CO2. © 2023 Elsevier Ltd

关键词： Catalysts

Synergistic Effects of Acid-Plasma Treatment on Co2 Capturetowards Carbon Materials

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SSRN 2024年

作者： Ye, Zhiping Han, Chuang Pan, Meilan Zhao, Liang Liu, Na Nikiforov, Anton Leus, Karen De Geyter, Nathalie Morent, Rino Chen, Jun Li, Junhua College of Environmental Zhejiang University of Technology 18 Chaowang RD Xiacheng District Hangzhou China Ghent University Faculty of Engineering Department of Applied Physics Research Unit Plasma Technology Sint-Pietersnieuwstraat 41 Ghent9000 Belgium Key Laboratory of Pollution Exposure and Health Intervention of Zhejiang Province Interdisciplinary Research Academy Zhejiang Shuren University Hangzhou310015 China State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex Beijing100084 China Tsinghua University China

Conventional techniques for modifying carbon materials frequently encounter challenges in controlling pore size distribution and achieving stable surface functionalization, which restrict their CO2 adsorption efficiency. This study introduces a novel two-step acid-plasma treatment that overcomes these challenges by enabling precise nitrogen incorporation, optimizing both micropore distribution and surface chemistry. Experimental results demonstrate up to 81% improvement in CO2 adsorption capacity at 298 K and 64% at 273 K compared to untreated samples. These improvements are attributed to the enhanced micropore structure and increased pyrrolic N content, both critical to boosting adsorption performance. Advanced kinetic studies, supported by density functional theory (DFT) simulations, confirmed that the adsorption mechanism is predominantly physisorptive, driven by a significant reduction in energy barriers for adsorption-desorption transitions due to strategic nitrogen doping. This work underscores the potential of nitrogen-doped activated carbon for scalable, energy-efficient CO2 capture and storage applications, offering a promising solution to the critical challenges in the field. © 2024, The Authors. All rights reserved.

关键词： Plasma applications

Emission Characteristics of Lead and Particulate Matter from Lead and Zinc Smelters in China

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SSRN 2024年

作者： Zhang, Jiawei Sun, Xiaohui Wu, Qingru Deng, Jianguo Li, Zhijian Wen, Minneng Xu, Liwen Gu, Yongzheng Han, Tao Feng, Lei Duan, Lei State Key Joint Laboratory of Environmental Simulation and Pollution Control School of the Environment Tsinghua University Beijing100084 China Department of Aeronautics Imperial College London South Kensington Campus LondonSW7 2AZ United Kingdom State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex Beijing100084 China Guodian Power Development Co. Ltd. Beijing100101 China CHN ENERGY New Energy Technology Research Institute Co. Ltd. Beijing102209 China

Understanding the emission characteristics of particulate matter and associated heavy metals is essential for assessing their environmental and health impacts post-emission, as well as for identifying potential control technologies for the sources. Here, a field test was conducted at two advanced smelting plants equipped with comprehensive air pollution control devices. The particles emitted from different stages of lead and zinc smelting exhibited bi-modal size distributions, with peaks observed in PM0.1-1.0 and PM2.5-10, respectively. Particulate-bound Pb was identified as the predominant Pb species in the flue gas, primarily originating from ore crushing. Consequently, over 80% of Pb was emitted in the form of coarse particles, a marked contrast to coal-fired power plants where Pb concentrated on fine particles. High efficiencies in Pb removal were achieved by dust collectors, flue gas purification systems, and acid plants with desulfurization systems, resulting in overall Pb emission factors in lead and zinc smelting were only 89.3 and 2.60 g t-1 (of metal production), respectively. Importantly, the contribution of gas-phase Pb, which accounts for approximately 16.6% of total emissions, must not be neglected in future emission monitoring and control efforts. © 2024, The Authors. All rights reserved.

关键词： Fossil fuel power plants

An Increase in Primary Formaldehyde Emissions Induced by the Coal-to-Gas Policy in Beijing

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SSRN 2023年

作者： Tang, Guiqian Kang, Yanyu Liu, Baoxian Yao, Dan Wang, Yiming Wang, Yinghong Wang, Yuesi Anhui University of Science and Technology China State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry Institute of Atmospheric Physics Chinese Academy of Sciences Beijing100029 China State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex Beijing100084 China Beijing Key Laboratory of Airborne Particulate Matter Monitoring Technology Beijing Municipal Environmental Monitoring Center Beijing100048 China School of Environment Key Laboratory for Yellow River and Huai River Water Environment and Pollution Control Ministry of Education Henan Normal University Xinxiang453007 China Beijing100081 China University of Chinese Academy of Sciences Beijing100049 China

In recent years, China has implemented the "coal-to-gas" strategy. The source composition spectra of pollutants emitted from coal and natural gas combustion are substantially different. Therefore, changes in the energy structure may lead to a significant impact on the atmospheric formaldehyde (HCHO) concentration and sources. To investigate the changes in HCHO sources, this study used proton transfer reaction-time-of-flight/mass spectrometry to observe and analyze HCHO in Beijing in May (spring), August (summer), and October (autumn) of 2019 and January (winter) of 2020. The average concentrations during the observation period were 5.1 ± 2.5 ppb (spring), 7.2 ± 1.9 ppb (summer), 3.6 ± 1.9 ppb (autumn), and 1.8 ± 0.5 ppb (winter), showing a characteristic of a single peak (midday) variation. Using nonmethane hydrocarbons as tracers, the source contributions of HCHO were quantified by the positive matrix factorization method. The results showed that the average contribution of secondary + biogenic was 2.2 ppb throughout the year, while the average contribution of anthropogenic primary was 1.5 ppb, accounting for 60.0% and 40.0% of the total concentration, respectively. Importantly, compared with 2011, the contribution of anthropogenic primary increased considerably, by 18.2% in winter, which has a significant relationship with "coal-to-gas". This study emphasizes the importance of primary HCHO emissions from natural gas. With the deep promotion of "coal-to-gas", it is necessary to strengthen the control of pollutants directly emitted from natural gas combustion in the future. © 2023, The Authors. All rights reserved.

关键词： Coal