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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

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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

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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

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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

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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

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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

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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

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Enhancing Stability of Copper-Based Catalysts By Regulating of Oxygen Vacancy for Resourcing Hcl Waste Gas

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SSRN 2024年

作者： Ye, Zhiping Pan, Ruoyan Chen, Kai Ma, Yutong Nikiforov, Anton Wang, Jiade College of Environment Zhejiang University of Technology 18 Chao-wang Road Hangzhou310014 China State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex Beijing100084 China Faculty of Engineering Department of Applied Physics Research Unit Plasma Technology Ghent University Sint-Pietersnieuwstraat 41 Ghent9000 Belgium

The utilization of copper-based catalysts for the conversion of by-product hydrogen chloride (HCl) to chlorine gas (Cl2) presents an attractive approach for the efficient treatment of HCl waste gas. However, this process encounters a notable challenge associated with catalyst deactivation due to the loss of copper in the form of Cu-Cl. In this study, we synthesized a Cu2.4CeV0.5Ox catalyst, which demonstrated remarkable performance, achieving a space-time yield of 2.26 g Cl2/gcat*h and maintaining a stable conversion efficiency of approximately 83% over a period of up to 600 hours. This level of stability represents a significant advancement compared to prior findings on copper-based catalysts. It is also shown that the reduction evolution of the Cu-Cl bond has been validated by in-situ DRFITS in combination with ToF-SIMS. In addition, ab-initio calculations were used to elucidate the rate-limiting step of oxygen vacancy replenishment by O2 instead of Cl over CeO2 and CeVO4, which inhibit the formation of Cu-Cl bonds. As a result, a novel strategy for the resourceful treatment of HCl waste gas was identified, laying the groundwork for its prospective industrial application. © 2024, The Authors. All rights reserved.

关键词： Oxygen vacancies

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Opportunity and shift of nitrogen use in China

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Geography and Sustainability 2024年第1期5卷 33-40页

作者： Wangzheng Shen Jing He Sisi Li Yanhua Zhuang Hongyuan Wang Hongbin Liu Liang Zhang Andreas Kappler Hubei Provincial Engineering Research Center of Non-Point Source Pollution Control Innovation Academy for Precision Measurement Science and TechnologyChinese Academy of SciencesWuhan 430077China University of Chinese Academy of Sciences Beijing 100049China School of Environmental Studies China University of Geosciences(Wuhan)Wuhan 430078China State Environmental Protection Key Laboratory of Source Apportionment and Control of Aquatic Pollution Ministry of Ecology and Environment of the People's Republic of ChinaWuhan 430078China Hubei Key Laboratory of Yangtze River Basin Environmental Aquatic Science Wuhan 430078China Institute of Agricultural Resources and Regional Planning Chinese Academy of Agricultural SciencesBeijing 100081China Geomicrobiology Group Center for Applied Geosciences(ZAG)University of TuebingenTuebingen D-72076Germany

It is never an easy task for China to feed 1.4 billion people with only 7%of the world's arable *** nearly 30%of the world's nitrogen(N)fertilizer applied,China achieves high crop yields while facing N pollution result-ing from excessive N ***,we calculate the farmland N budget on the national and regional *** N use efficiency(NUE)in China increased by 28.0%during *** improvement is due to the reduction in fertilization and the improvement of crop *** fragmented farmland is changing to large-scale farmland with the increase in cultivated land area per rural population and the development of agricultural *** opportunity brings more possibilities for precision farmland management,thus further improving *** goal of an NUE of 0.6 may be achieved in the 2040s based on the current development *** striking N use shift in China has important implications for other developing countries.

关键词： environmental Kuznets curve Nitrogen surplus Greenhouse gas emission Climate change Non-point source pollution

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Determination of Arsenic and Antimony by Atmospheric Pressure Glow Discharge Portable Emission Spectrometer with Solid Acid Hydride Generation

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SSRN 2023年

作者： Han, Shanru Zhu, Zhenli Liu, Ying Dong, Junhang Xu, Chaoyu Liu, Xing Liu, Jinzhao Zheng, Hongtao State Key Laboratory of Biogeology and Environmental Geology School of Earth Sciences China University of Geosciences Wuhan430074 China School of Mechanical Engineering and Electronic Information China University of Geosciences Wuhan430074 China State Environmental Protection Key Laboratory of Source Appointment and Control of Aquatic Pollution Ministry of Ecology and Environment China Faculty of Material Science and Chemistry China University of Geosciences Wuhan430074 China

In this work, the use of solid acid hydride generation (HG) for the simultaneous determination of As and Sb in environmental water samples by miniaturized atmospheric pressure glow discharge plasma atomic emission spectrometer (APGD-OES) was evaluated. It was found that HG with the use of sulfamic acid tablets can achieve similar sensitivity with conventional HCl-KBH4 for As and Sb determination by APGD-OES, which avoids the safety problem caused by the use of hydrochloric acid and greatly facilitates field analysis. In addition, the whole detection procedure does not require complex pretreatment of liquid samples, thereby enabling analysis in an environmentally friendly manner. Under optimal conditions, the obtained detection limits (LODs) are as low as 1.14 μg L-1 for As and 0.62 μg L-1 for Sb, respectively. In addition, it offers good repeatability, where the relative standard deviations (RSDs) are less than 5% at 20 μg L-1. The accuracy of the proposed method was validated by the analysis of simulated natural water reference samples. Moreover, it has been successfully applied to the determination of tap water, pond water, and hot spring samples. All these results clearly demonstrate the proposed simple, cost-effective and field-deployable method provides a promising approach for the field analysis of As and Sb. © 2023, The Authors. All rights reserved.

关键词： Arsenic

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