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Towards rational design of Cu-SSZ-13 catalysts with less N2O formation in NH3-SCR reaction: The effect of Brønsted acid sites

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Journal of environmental Sciences (China) 2025年 157卷 546-557页

作者： Liu, Jianqi Du, Jinpeng Wang, Jingyi Han, Shichao Shan, Yulong Zhang, Yan Wu, Xuanhao Gao, Shan Yu, Yunbo Wu, Zhongbiao Shan, Wenpo He, Hong Fujian Key Laboratory of Atmospheric Ozone Pollution Prevention Institute of Urban Environment Chinese Academy of Sciences Xiamen361021 China University of Chinese Academy of Sciences Beijing100049 China State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental Sciences Chinese Academy of Sciences Beijing100085 China Zhejiang Key Laboratory of Urban Environmental Processes and Pollution Control Ningbo Urban Environment Observation and Research Station Institute of Urban Environment Chinese Academy of Sciences Ningbo315800 China Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai201210 China Department of Environmental Engineering Zhejiang University Hangzhou310058 China Zhejiang Tianlan Environmental Protection Technology Co. Ltd. Hangzhou311202 China

Ammonia Selective Catalytic Reduction (NHs-SCR) technology has been employed to eliminate NOx from diesel engine exhaust, with Cu-SSZ-13 serving as the commercial catalyst. The greenhouse gas N2O is produced as a byproduct when using Cu-SSZ-13 as the NH3-SCR catalyst. To achieve synergistic control of pollutants and greenhouse gases in diesel engine exhaust, rational design of Cu-SSZ-13 catalysts is required. In this study, the effect of Brønsted acid sites in Cu-SSZ-13 catalysts on the formation of N2O was investigated. Mild thermal treatment was innovatively employed to prepare Cu-SSZ-13 catalysts with different amounts of Brønsted acid sites. EPR, H2-TPR, NH3-TPD, NMR were utilized to determine that the Brønsted acid sites were modified while the Cu species remained unchanged. Thereby an accurate assessment of the influence of Brønsted acid sites on N2O formation could be achieved. Our results showed that Cu-SSZ-13 with more Brønsted acid sites produced less N2O during the NH3-SCR reaction. In the low-temperature region, the presence of framework acid sites facilitates the decomposition of the NH4NO3 assisted by NO to form N2 and H2O, reducing the formation of N2O. In the high-temperature region, the Brønsted acid sites promote the decomposition of NH2NO into N2 and H2O. Meanwhile, the N2O-SCR reaction can also be promoted by Brønsted acid sites, thereby decreasing N2O emissions. This study suggests that in the future design and synthesis of Cu-SSZ-13 zeolites, attention should be paid to creating more Brønsted acid sites in Cu-SSZ-13 to reduce N2O emissions. © 2024

关键词： Emission control

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Organosulfur Compounds in Ambient Fine Particulate Matter in an Urban Region: Findings of a Nontargeted Approach

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SSRN 2023年

作者： Li, Ailin Shi, Xiaodi Qiu, Xinghua Wei, Gaoyuan Zheng, Yan Chen, Qi Chen, Shiyi Hu, Min Zhu, Tong State Key Joint Laboratory for Environmental Simulation and Pollution Control College of Environmental Sciences and Engineering Center for Environment and Health Peking University Beijing100871 China

Organosulfur compounds (OSCs) are important components of fine particulate matter (PM2.5);however, little information is available on OSCs in urban regions due to their chemical complexity. In this study, we developed a nontargeted approach based on gas chromatography and high-resolution mass spectrometry (GC-HRMS) to screen OSCs in PM2.5 of urban Beijing. Seventy-six OSCs were found through mass difference of sulfur isotopes and characteristic sulfur-containing fragments. Six species were confirmed as aromatic sulfonates by authentic standards. Most OSCs showed higher levels in the heating season, presumably because of the intensive emission especially from coal combustion. While certain species, with 2-sulfobenzoic acid as the representative, were more abundant in the non-heating season. Such species were significantly correlated with ozone and aerosol liquid water content, implying an oxidation-involved aqueous-phase formation in the atmosphere. The predominance of the 2-substitution product over its isomer of 3- or 4-sulfobenzoic acid suggests a more plausible mechanism of ring-opening of naphthalene followed by sulfonation, with atmospheric reactivity indicated by ozone and temperature as the determining factor. This study provided not only a nontargeted approach for OSCs in ambient PM2.5, but also field evidence on their secondary formation proposed in previous simulation studies. © 2023, The Authors. All rights reserved.

关键词： Naphthalene

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Fine particulate matter(PM_(2.5)/PM_(1.0)) in Beijing,China: Variations and chemical compositions as well as sources

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Journal of environmental Sciences 2022年第11期34卷 187-198页

作者： Lining Luo Xiaoxuan Bai Shuhan Liu Bobo Wu Wei Liu Yunqian Lv Zhihui Guo Shumin Lin Shuang Zhao Yan Hao Jiming Hao Kai Zhang Aihua Zheng Hezhong Tian State Key Laboratory of Environmental Simulation and Pollution Control School of EnvironmentBeijing Normal UniversityBeijing 100875China Center for Atmospheric Environmental Studies Beijing Normal UniversityBeijing 100875China School of Environment Tsinghua UniversityBeijing 100084China Department of Environmental Health Sciences School of Public Health University at Albany State University of New York One University Place RensselaerNY 12144USA Analysis and Testing Center Beijing Normal UniversityBeijing 100875China

Particulate matter(i.e.,PM_(1.0) and PM_(2.5)),considered as the key atmospheric pollutants,exerts negative effects on visibility,global climate,and human health by associated chemical ***,our understanding of PM and its chemical compositions in Beijing under the current atmospheric environment is still not complete after witnessing marked alleviation during 2013–*** measurements can be crucial for further air quality improvement by better characterizing PM pollution and chemical compositions in ***,we conducted simultaneous measurements on PM in Beijing during 2018–*** indicate that annualmean PM_(1.0) and PM_(2.5) concentrations were 35.49±18.61μg/m^(3) and 66.58±60.17μg/m^(3),showing a positive response to emission *** contribution of sulfate,nitrate,and ammonium(SNA)played an enhanced role with elevated PM loading and acted as the main contributors to pollution *** observed among chemical species between PM_(1.0) and PM_(2.5) in spring suggest that sand particles trend to accumulate in the range of 1–2.5μ*** episodes occurred accompanied with southerly clusters and high formation of SNA by heterogeneous reactions in summer and winter,*** from positive matrix factorization(PMF)combined with potential source contribution function(PSCF)models showed that potential areas were seasonal dependent,secondary and vehicular sources became much more important compared with previous studies in *** study presented a continuous investigation on PM and sources origins in Beijing,which provides a better understanding for further emission control as well as a reference for other cities in developing countries.

关键词： Fine particles Haze Chemical species Seasonal variation Source apportionment

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Analysis of the Drivers of Premature Death and Life Expectancy Reduction Associated with Global Pm2.5 pollution

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SSRN 2023年

作者： Wu, Dongdong State Key Joint Laboratory of Environmental Simulation and Pollution Control School of Environment Beijing Normal University Xinjiekouwai Street No. 19 Beijing100875 China

Quantitative assessment of the health risks due to PM2.5 is a global concern. This study systematically assessed the impact of PM2.5 on global and regional premature death and per capita life expectancy reduction (LER) from 1995-2019. The number of premature death due to PM2.5 increased from 3.25 million to 4.56 million during the study period;while the per capita life expectancy reduction increased from 0.91 to 1.03 years before decreasing to 0.95 years. The number of deaths and LER were declining in Europe and North America, while the opposite was observed in Asian and African countries. Population and age structure were pulling factors for premature death, with population contributing more to African countries (90%), while other countries were more susceptible to age structure;PM2.5 concentration was a puller and then a suppressor for both premature death and LER, and the medical level was always a suppressor. All countries should take action and cooperate to reduce the harmful effects of PM2.5 pollution on humans. © 2023, The Authors. All rights reserved.

关键词： Health risks

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New WHO global air quality guidelines help prevent premature deaths in China

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National Science Review 2022年第4期9卷 10-12页

作者： Tao Xue Guannan Geng Xia Meng Qingyang Xiao Yixuan Zheng Jicheng Gong Jun Liu Wei Wan Qiang Zhang Haidong Kan Shiqiu Zhang Tong Zhu Institute of Reproductive and Child Health/National Health Commission Key Laboratory of Reproductive Health and Department of Epidemiology and Biostatistics School of Public HealthPeking University State Key Joint Laboratory of Environmental Simulation and Pollution Control School of EnvironmentTsinghua University School of Public Health Key Laboratory of Public Health Safety of the Ministry of Educationand Key Laboratory of Health Technology Assessment of the Ministry of HealthFudan University Center of Air Quality Simulation and System Analysis Chinese Academy of Environmental Planning College of Environmental Sciences and Engineering Peking University School of Energy and Environmental Engineering University of Science and Technology Beijing Clean Air Asia Ministry of Education Key Laboratory for Earth System Modeling Department of Earth System ScienceTsinghua University

The air quality guidelines （AQGs） issued by the World Health Organization （WHO） in 2005 are key references for the National Ambient Air Quality Standards （NAAQSs） in *** 22September 2021,the WHO issued new AQGs （NAQGs）[1],which propose more stringent targets to control exposure to multiple air pollutants,including fine particulate matter (PM2.5) and ozone （O3）,to which,in 2019,451 million premature deaths,globally,were attributable [2].

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Application of Data Quality Optimization and Machine Learning Techniques to Predict the Dissolved Oxygen Concentration in the Tide-Sensitive Tanjiang River

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SSRN 2023年

作者： Liu, Wei Lin, Shu Li, Xiaobao Li, Wenjing Fang, Huaiyang Li, Weijie Deng, Hong School of Environment and Energy Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Resource Recycling South China University of Technology Guangzhou510006 China The Key Laboratory of Water and Air Pollution Control of Guangdong Province State Environmental Protection Key Laboratory of Water Environmental Simulation and Pollution Control South China Institute of Environmental Sciences Ministry of Ecology and Environment of the People's Republic of China Guangzhou510535 China

The dissolved oxygen (DO) concentration is an important index for evaluating the quality of the water environment. Here, we constructed three models (SVR, MIC-SVR, and WT-MIC-SVR) based on data quality optimization techniques (the maximum information coefficient (MIC), wavelet transform (WT) data noise reduction) and machine learning techniques (support vector regression (SVR)) to predict the DO concentration in the Tanjiang River (a typical tide-sensitive river in southern China) and establish the optimal model. Specifically, the MIC was used to screen the main environmental factors affecting DO changes, the wavelet transform technique was used for data noise reduction, and a hybrid model was constructed to predict DO concentrations with SVR. The MIC technique can effectively screen the main environmental factors affecting the DO concentration, and the application of the WT technique did not improve the predictive performance of the model. The best performance was achieved by the MIC-SVR model;the RMSE was 4.46% lower and the R2 and NSE were 23.26% and 45.85% higher, respectively, for the MIC-SVR model compared with the SVR model. In addition, study of kernel function selection revealed that considering as many kernel functions as possible is necessary for improving the performance of the SVR model. The main factors affecting the DO changes in different regions (basins) were basically the same as those observed in previous studies;however, the secondary factors differed. Screening of these secondary factors as a supplement to the model input variables can improve the predictive performance of the model to a certain extent. Overall, the proposed MIC-SVR model can be used to analyze the relationship between DO and environmental factors in order to find the main causes of low DO, and accurately predict the DO concentration in the Tanjiang River (especially in its tidally sensitive reaches), thus providing assistance in water environment protection and water resource m

关键词： Forecasting

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Phthalate levels in Chinese residences:Seasonal and regional variations and the implication on human exposure

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National Science Open 2023年第6期2卷 65-79页

作者： Yatai Li Jing Hou Zukun Wang Xilei Dai Yuexia Sun Junjie Liu Yingjun Liu Key Joint Laboratory of Environmental Simulation and Pollution Control College of Environmental Sciences and EngineeringPeking UniversityBeijing 100871China College of Public Health Zhengzhou UniversityZhengzhou 450001China Tianjin Key Lab of Indoor Air Environmental Quality Control School of Environmental Science and EngineeringTianjin UniversityTianjin 300072China College of Design and Engineering National University of SingaporeSingapore 117566Singapore Center for Environment and Health Peking UniversityBeijing 100871China

Indoor pollution of manmade semivolatile organic compounds(SVOCs)such as phthalates are a growing threat to human *** we summarize the dust-phase phthalate concentrations in Chinese residences reported from 2011 to 2021and simulate corresponding airborne concentrations based on equilibrium *** simulation considers seasonal and regional variations in indoor temperature and PM_(2.5)concentration,in contrast to the common practice of using constant *** show that variations in these two environmental factors lead to up to ten-and six-fold variations in the monthly median gas-and particle-phase concentrations of phthalates,respectively,in residences in individual climate *** higher-vaporpressure species di-n-butyl phthalate and di-isobutyl phthalate,the resultant seasonal and regional variations in aggregate nondiet intake can reach six-and three-fold,*** results have important implications on exposure assessment of SVOCs and epidemiological evaluation of their health effects.

关键词： SVOCs indoor air temperature dust

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Exploring the biosynthetic possibilities of hydroxylated polybrominated diphenyl ethers from bromophenols in Prorocentrum donghaiense: Implications for bioremediation

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Chemosphere 2024年 362卷 142611页

作者： Li, Bin Shi, Jianghong Xiang, Xueling Zhang, Mengtao Ge, Hui Sun, Shuhan School of Environment Harbin Institute of Technology Harbin150090 China Guangdong Provincial Key Laboratory of Soil and Groundwater Pollution Control School of Environmental Science and Engineering Southern University of Science and Technology Shenzhen518055 China

Bromophenols has been proven to synthesize hydroxylated polybrominated diphenyl ethers (OH-PBDEs), which may pose additional environmental and health risks in the process of bioremediation. In this study, the removal of 2,4-dibromophenol (2,4-DBP) and 2,4,6-tribromophenol (2,4,6-TBP) and the biosynthetic of OH-PBDEs by Prorocentrum donghaiense were explored. The removal efficiencies of 2,4-DBP and 2,4,6-TBP ranged from 32.71% to 76.89% and 31.15%–78.12%, respectively. Low concentrations of 2,4-DBP stimulated algal growth, while high concentrations were inhibitory. Furthermore, exposure to 10.00 mg L−1 2,4-DBP resulted in the detection of 2′-hydroxy-2,3′,4,5′-tetrabromodiphenyl ether (2′–OH–BDE-68) within P. donghaiense. In contrast, increasing concentrations of 2,4,6-TBP considerably inhibited P. donghaiense growth, with 4′-hydroxy-2,3′,4,5′,6-pentabromodiphenyl ether (4′–OH–BDE-121) detected within P. donghaiense under 5.00 mg L−1 2,4,6-TBP. Metabolomic analysis further revealed that the synthesized OH-PBDEs exhibited higher toxicity than their precursors and identified the oxidative coupling as a key biosynthetic mechanism. These findings confirm the capacity of P. donghaiense to remove bromophenols and biosynthesize OH-PBDEs from bromophenols, offering valuable insights into formulating algal bioremediation to mitigate bromophenol contamination. © 2024 Elsevier Ltd

关键词： Bioremediation

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Hydroxyl,hydroperoxyl free radicals determination methods in atmosphere and troposphere

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Journal of environmental Sciences 2021年第1期33卷 324-335页

作者： Guoying Wang Yves Iradukunda Gaofeng Shi Pascaline Sanga Xiuli Niu Zhijun Wu School of Petrochemical Engineering Lanzhou University of TechnologyLanzhou 730050China Gansu Food Inspection and Research Institute Lanzhou 730050China State Key Joint Laboratory of Environment Simulation and Pollution Control(Peking University) College of Enuironmental Sciences and EngineeringPeking UniversityBeijing 100871China

The hydroxyl radical(·OH)has a crucial function in the oxidation and removal of many atmospheric compounds that are harmful to ***,high reactivity,low atmospheric abundance,determination of hydroxyl,and hydroperoxyl radical’s quantity is very *** the atmosphere and troposphere,hydroperoxyl radicals(HO_(2))are closely demanded in the chemical oxidation of the *** advances in technology have allowed researchers to improve the determination methods on the research of free radicals through some spectroscopic *** far,several methods such as laser-induced fluorescence(LIF),high-performance liquid chromatography(HPLC),and chemical ionization mass spectroscopy have been identified and mostly used in determining the quantity of hydroxyl and hydroperoxyl *** this systematic review,we have advised the use of scavenger as an advance for further researchers to circumvent some of these problems caused by free *** primary goal of this review is to deepen our understanding of the functions of the most critical free radical(·OH,HO_(2))and also understand the currently used methods to quantify them in the atmosphere and troposphere.

关键词： Atmosphere Determination method Hydroxyl radical Hydroperoxyl radical Troposphere

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Enhanced phosphate removal using zirconium hydroxide encapsulated in quaternized cellulose

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Journal of environmental Sciences 2020年第3期32卷 102-112页

作者： Shuoxun Dong Qinghua Ji Yili Wang Huijuan Liu Jiuhui Qu Center for Water and Ecology State Key Joint Laboratory of Environment Simulation and Pollution ControlSchool of EnvironmentTsinghua UniversityBeijing 100084China College of Environmental Science and Engineering Beijing Key Lab for Source Control Technology of Water PollutionBeijing Forestry UniversityBeijing 100083China

Zirconium-based materials are efficient adsorbent for aqueous phosphate ***,current zirconium-based materials still show unsatisfied performance on adsorption capacity and ***,we demonstrate a zirconium hydroxide encapsulated in quaternized cellulose(QC-Zr) for the selective phosphate *** hydroxide nanoparticles were simultaneously generated in situ with the QC framework and firmly anchored in the three-dimensional(3D) cross-linked cellulose *** maximum P adsorption capacity of QC-Zr was 83.6 mg P/***,the QC-Zr shows high P adsorption performance in a wide pH range,generally due to the electrostatic effects of quaternized *** enhanced adsorption of P was also achieved in the presence of competing anions(including Cl^-,NO3^-,SO4^2-,SO4^4-) and humic acid(HA) even at a molar ratio up to 20 *** column adsorption capacity of QC-Zr reached 4000 bed volumes(BV) at EBCT=0.5 min as the P concentration decreased from 2.5 to 0.5 mg/*** study revealed that both-N^+(CH3)3 groups and zirconium hydroxide were involved in phosphate adsorption via electrostatic interactions between -N^+(CH3)3 and phosphate,and the formation of zirconium hydrogen phosphate(Zr(HPO4)x).The 31 P nuclear magnetic resonance(NMR) study implied that P surface-precipitated and inner-sphere complexed with zirconium hydroxide at a ratio of 3:1.

关键词： Adsorption Phosphate removal Zirconium hydroxide aerogel Quaternized cellulose

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