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Characterization and prediction of tailpipe ammonia emissions from in-use China 5/6 light-duty gasoline vehicles

Frontiers of environmental Science & Engineering 2024年第1期18卷 71-81页

作者： Lewei Zeng Fengbin Wang Shupei Xiao Xuan Zheng Xintong Li Qiyuan Xie Xiaoyang Yu Cheng Huang Qingyao Hu Yan You Ye Wu College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518060China State Key Laboratory of Engines Tianjin UniversityTianjin 300072China China Automotive Technology and Research Center Co.Ltd. Tianjin 300300China CATARC Automotive Test Center(Guangzhou)Co.Ltd. Guangzhou 511300China State Environmental Protection Key Laboratory of Cause and Prevention of Urban Air Pollution Complex Shanghai Academy of Environmental SciencesShanghai 200233China National Observation and Research Station of Coastal Ecological Environments in Macao Macao Environmental Research InstituteMacao University of Science and TechnologyMacao SAR 999078China School of Environment State Key Joint Laboratory of Environment Simulation and Pollution ControlTsinghua UniversityBeijing 100084China

On-road tailpipe ammonia (NH3) emissions contribute to urban secondary organic aerosol formation and have direct or indirect adverse impacts on the environment and human health. To understand the tailpipe NH3 emission characteristics, we performed comprehensive chassis dynamometer measurements of NH3 emission from two China 5 and two China 6 light-duty gasoline vehicles (LDGVs) equipped with three-way catalytic converters (TWCs). The results showed that the distance-based emission factors (EFs) were 12.72 ± 2.68 and 3.18 ± 1.37 mg/km for China 5 and China 6 LDGVs, respectively. Upgrades in emission standards were associated with a reduction in tailpipe NH3 emission. In addition, high NH3 EFs were observed during the engine warm-up period in cold-start cases owing to the intensive emissions of incomplete combustion products and suitable catalytic temperature in the TWCs. Notably, based on the instantaneous NH3 emission rate, distinct NH3–emitting events were detected under high/extra high velocity or rapid acceleration. Furthermore, NH3 emission rates correlated well with engine speed, vehicle specific power, and modified combustion efficiency, which were more easily accessible. These strong correlations were applied to reproduce NH3 emissions from China 5/6 LDGVs. The predicted NH3 EFs under different dynamometer and real-world cycles agreed well with existing measurement and prediction results, revealing that the NH3 EFs of LDGVs in urban routes were within 8.55–11.62 mg/km. The results presented here substantially contribute to improving the NH3 emission inventory for LDGVs and predicting on-road NH3 emissions in China.

关键词： NH3 instantaneous emissions Catalytic temperature Vehicle specific power Combustion efficiency Emission prediction

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Effects of Br−on NDMA Formation During Chloramination:a Review of Influencing Factors,Mechanisms,and control

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Chemical Research in Chinese Universities 2023年第3期39卷 370-377页

作者： XIA Ruanjunjie LIAO Xiaobin LIU Tianze GAO Menglan CHEN Chao Institute of Municipal and Environmental Engineering College of Civil EngineeringHuaqiao UniversityXiamen361021P.R.China State Key Joint Laboratory of Environment Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing100084P.R.China

For the invasion of seawater and the stress of human activities,bromide ion(Br−)exists widely in drinking water sources,and it was found to influence the formation of non-brominated but carcinogenic nitrogen-containing disinfection by-product nitroso-dimethylamine(NDMA)during chloramination(NH2Cl).The presence of Br−leads to the formation of bromine-active species,such as bromamines(NH2Br),bromochloramine(NHClBr),as well as hypobromous acid(HOBr),which are more reactive with NDMA precursors than chlorine-active species,so might promote NDMA *** review mainly focuses on the influencing laws,as well as the factors(disinfection conditions and characteristics of water matrixes)that affected NMDA formation during chloramination with Br−.In addition,the possible influencing pathways are ***,based on the above summary,measures pertaining to reduce the impact of Br−on NDMA production are *** review would provide a theoretical reference for drinking water treatment plants to deal with bromine-containing water during chloramination.

关键词： Bromide ion Disinfection by-product Nitrosodimethylamine(NDMA) Chloramination

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Comprehensive evaluation of an ionic liquid based deep purification process for NH_(3)-containing industrial gas

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Journal of environmental Sciences 2024年第2期136卷 698-708页

作者： Guoxiong Zhan Fei Cao Jianjun Chen Zhen Chen Yuanmeng Duan Fei Chang Shaojuan Zeng Yinge Bai Zengxi Li Xiangping Zhang Junhua Li State Key Joint Laboratory of Environment Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China Sino-Danish College University of Chinese Academy of SciencesBeijing 100049China Institute of Process Engineering Chinese Academy of SciencesBeijing 100190China College of Chemical and Engineering University of Chinese Academy of SciencesBeijing 100049China

Ammonia(NH_(3))emission has caused serious environment issues and aroused worldwide *** emerging ionic liquid(IL)provides a greener way to efficiently capture NH_(3).This paper provides rigorous process simulation,optimization and assessment for a novel NH_(3)deep purification process using *** process was designed and investigated by simulation and optimization using ionic liquid[C_(4)im][NTF_(2)]as *** objective functions,total purification cost(TPC),total process CO_(2)emission(TPCOE)and thermal efficiency(ηeff)were employed to optimize the absorption *** simulation and optimization results indicate that at same purification standard and recovery rate,the novel process can achieve lower cost and CO_(2)emission compared to benchmark *** process optimization,the optimal functions can achieve 0.02726$/Nm~3(TPC),311.27 kg CO_(2)/hr(TP-COE),and 52.21%(ηeff)for enhanced ***,compared with conventional process,novel process could decrease over$3 million of purification cost and 10000 tons of CO_(2)emission during the life *** results provide a novel strategy and guidance for deep purification of NH_(3)capture.

关键词： NH_(3) Capture Process Ionic Liquid Process simulation Process Optimization Deep purification

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Efficient Pt/KFI zeolite catalysts for the selective catalytic reduction of NOxby hydrogen

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Journal of environmental Sciences 2024年第4期138卷 102-111页

作者： Ligang Zhang Yulong Shan Zidi Yan Zhongqi Liu Yunbo Yu Hong He School of Rare Earths University of Science and Technology of ChinaHefei 230026China Ganjiang Innovation Academy Chinese Academy of SciencesGanzhou 341119China State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China

Aiming at purification of NO_(x)from hydrogen internal combustion engines(HICEs),the hydrogen selective catalytic reduction(H_(2)-SCR)reaction was investigated over a series of Pt/KFI zeolite catalysts.H_(2)can readily reduce NO_(x)to N_(2)and N_(2)O while O_(2)inhibited the deNO_(x)efficiency by consuming the reductant H_(2).The Pt/KFI zeolite catalysts with Pt loading below 0.1wt.% are optimized H_(2)-SCR catalysts due to its suitable operation temperature window since high Pt loading favors the H_(2)-O_(2)reaction which lead to the insufficient of *** to metal Pt^(0)species,Pt^(δ+)species showed lower activation energy of H_(2)-SCR reaction and thought to be as reasonable active ***,Eley-Rideal(E-R)reaction mechanism was proposed as evidenced by the reaction orders in kinetic ***,the optimized reactor was designed with hybrid Pt/KFI catalysts with various Pt loading which achieve a high NO_(x)conversion in a wide temperature range.

关键词： Pt/KFI zeolite Pt loading H_(2)-SCR Reaction conditions Kinetics studies

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Design of Ca-type todorokite catalysts with highly active for the selective reduction of NO_(x) by NH_(3) at low temperatures

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Journal of environmental Sciences 2024年第4期138卷 697-708页

作者： Chuang Chang Zidi Yan Chunlei Zhang Yanshuang Zhang Miao Jiang Luna Ruan Min Xiao Yunbo Yu Hong He School of Rare Earths University of Science and Technology of ChinaHefei 230026China Ganjiang Innovation Academy Chinese Academy of SciencesGanzhou 341000China State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China

Ca-type todorokite catalysts were designed and prepared by a simple redox method and applied to the selective reduction of NO_(x) by NH_(3)(NH_(3)-SCR)for the first *** with the Na-type manjiroite prepared by the same method,the todorokite catalysts with different Mn/Ca ratios showed greatly improved catalytic activity for NO_(x) *** them,Mn8Ca4 catalyst exhibited the best NH_(3)-SCR performance,achieving 90%NO_(x) conversion within temperature range of 70-275℃ and having a high sulphur *** to the Na-type manjiroite sample,Ca-type todorokite catalysts possessed an increased size of tunnel,resulting in a larger specific surface *** increased the amounts of Ca doping,the Na content in Ca-type todorokite catalysts significantly decreased,providing larger amounts of Bronsted acid sites for NH_(3) adsorption to produce NH_(4)^(+).The NH_(4)^(+)species were highly active for reaction with NO+O_(2),playing a determining role in NH_(3)-SCR process at low ***,larger amounts of surface adsorbed oxygen contained over the Ca-doping samples than that over Na-type manjiroite,promoting the oxidation of NO and fast SCR *** the Ca-type todorokite catalysts,furthermore,nitrates produced during the flow of NO+O_(2),were more active for reaction with NH_(3) than that over Na-type manjiroite,benefiting the occurrence of NH_(3)-SCR *** study provides novel insights into the design of NH_(3)-SCR catalysts with high performance.

关键词： NO_(x) NH_(3)-SCR Mn-based oxides Ca-type todorokite Bronsted acid sites

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Boosting the catalytic performance of Cu-SAPO-34in NO_(x) removal via hydrothermal treatment

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Journal of environmental Sciences 2024年第1期135卷 640-655页

作者： Xiaoyan Tian Huimin Wang Siyuan Xu Lianyun Gao Jinyan Cao Jianjun Chen Qiulin Zhang Ping Ning Jiming Hao Faculty of Environmental Science and Engineering Kunming University of Science and TechnologyKunming 650500China National-Regional Engineering Center for Recovery of Waste Gases from Metallurgical and Chemical Industries Kunming University of Science and TechnologyKunming 650500China School of Environment State Key Joint Laboratory of Environment Simulation and Pollution ControlTsinghua UniversityBeijing 100084China

Phosphate ions promoted Cu-SAPO-34(P-Cu-SAPO-34)were prepared using bulk CuO particles as Cu^(2+)precursor by a solid-state ion exchange technique for the selective catalytic reduction of NO_(x) with NH_3(NH_3-SCR).The effects of high temperature(H-T)hydrothermal aging on the NO_(x) removal(de-NO_(x))performance of Cu-SAPO-34 with and without phosphate ions were systematically investigated at atomic *** results displayed that both Cu-SAPO-34 and P-Cu-SAPO-34 presented relatively poor NO_(x) removal activity with a low conversion(<30%)at 250-500℃.However,after H-T hydrothermal treatment(800℃ for 10 hr at 10%H_2O),these two samples showed significantly satisfied NO_(x) elimination performance with a quite high conversion(70%-90%)at 250-500℃.Additionally,phosphate ions decoration can further enhance the catalytic performance of Cu-SAPO-34 after hydrothermal treatment(Cu-SAPO-34H).The textural properties,morphologies,structural feature,acidity,redox characteristic,and surface-active species of the fresh and hydrothermally aged samples were analyzed using various characterization *** systematical characterization results revealed that increases of 28%of the isolated Cu^(2+)active species(Cu^(2+)-2Z,Cu(OH)^(+)-Z)mainly from bulk CuO and 50%of the Bronsted acid sites,the high dispersion of isolated Cu^(2+)active component as well as the Bronsted acid sites were mainly responsible for the accepted catalytic activity of these two hydrothermally aged samples,especially for P-Cu-SAPO-34H.

关键词： NH_(3)-SCR Cu-SAPO-34 Hydrothermal induced Phosphate ions

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Advanced modeling of the absorption enhancement of black carbon particles in chamber experiments by considering the morphology and coating thickness

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Frontiers of environmental Science & Engineering 2024年第9期18卷 129-142页

作者： Xiaodong Wei Jianlin Hu Chao Liu Xiaodong Xie Junjie Yin Song Guo Min Hu Jianfei Peng Huijun Wang Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control Collaborative Innovation Center of Atmospheric Environment and Equipment TechnologySchool of Environmental Science and EngineeringNanjing University of Information Science&TechnologyNanjing 210044China Collaborative Innovation Center on Forecast and Evaluation of Meteorological Disasters Key Laboratory of Meteorological Disaster(Ministry of Education)Nanjing University of Information Science and TechnologyNanjing 210044China Nansen−Zhu International Research Centre Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China East China Air Traffic Management Bureau CAAC Shanghai 200335China State Key Joint Laboratory of Environmental Simulation and Pollution Control International Joint Laboratory for Regional Pollution Control(IJRC)(Ministry of Education)College of Environmental Sciences and EngineeringPeking UniversityBeijing 100871China Tianjin Key Laboratory of Urban Transport Emission Research&State Environmental Protection Key Laboratory of Urban Ambient Air Particulate Matter Pollution Prevention and Control College of Environmental Science and EngineeringNankai UniversityTianjin 300071China

Measurements studies have shown that the absorption of radiation by black carbon(BC)increases as the particles ***,there are significant discrepancies between the measured and modeled absorption enhancement(E_(abs)),largely due to the simplifications used in modeling the mixing states and shape *** took advantage of chamber experiments on BC aging and developed an efficient method to resolve the particle shape based on the relationship between the coating fraction(ΔD_(ve)/D_(ve),0)and fractal dimension(D_(f)),which can also reflect the variations of D_(f)during the whole BC aging *** with externally and partly mixed states(0≤ΔD_(ve)/D_(ve),0≤0.5)can be considered to be uniformly distributed with the D_(f)values of 1.8–2.1,whereas the Df values are constrained in the range 2.2–2.8 for fully mixed states(ΔD_(ve)/D_(ve),0>0.5).The morphological parameters(i.e.,the effective density and the dynamic shape factor)were compared with the measured values to verify the simulated *** simulated mean deviations of morphological parameters were smaller than 8%for the method resolving the particle *** applying a realistic shape and refractive index,the mass absorption cross for fully mixed states can be improved by 11%compared with a simplified core–shell *** on our understanding of the influence of D_(f)andΔD_(ve)/D_(ve),0 on E_(abs),we propose a two-stage calibration equation to correct the E_(abs)values estimated by the core–shell model,which reduces the simulation error in the Mie calculation by 6%–14%.

关键词： Black carbon Mixing states Fractal dimension Dynamic shape factor Absorption enhancement

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Interface sites on vanadia-based catalysts are highly active for NO_(x) removal under realistic conditions

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Journal of environmental Sciences 2024年第2期136卷 523-536页

作者： Zhihui Lv Guangzhi He Wenshuo Zhang Jingjing Liu Zhihua Lian Yang Yang Zidi Yan Guangyan Xu Wenpo Shan Yunbo Yu Hong He State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China University of Chinese Academy of Sciences Beijing 100049China Center for Excellence in Regional Atmospheric Environment and Key Laboratory of Urban Pollutant Conversion Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China Ganjiang Innovation Academy Chinese Academy of SciencesGanzhou 341000China Ningbo Research Center for Urban Environment Chinese Academy of SciencesNingbo 315800China

TiO_(2)-supported V_(2)O_(5)catalysts are commonly used in NO_(x)reduction with ammonia due to their robust catalytic *** these catalysts,it is generally considered that the active species are mainly derived from the vanadia species rather than the intrinsic structure of V-O-Ti entities,namely the interface *** reveal the role of V-O-Ti entities in NH_(3)-SCR,herein,we prepared TiO_(2)/V_(2)O_(5)catalysts and demonstrated that V-O-Ti entities were more active for NO_(x)reduction under wet conditions than the V sites(V=O)working *** the V-O-Ti entities,kinetic measurements and first principles calculations revealed that NH_(3)activation exhibited a much lower energy barrier than that on V=O *** wet conditions,the V-O-Ti interface significantly inhibited the transformation of V=O to V-OH sites thus benefiting NH_(3)*** wet conditions,meanwhile,the migration of NH_(4)^(+)from Ti site neighboring the V-O-Ti interface to Ti site of the V-O-Ti interface was exothermic;thus,V-O-Ti entities together with neighboring Ti sites could serve as channels linking NH_(3)pool and active centers for activation of NH_(4)^(+).This finding reveals that the V-O-Ti interface sites on V-based catalysts play a crucial role in NO_(x)removal under realistic conditions,providing a new perspective on NH_(3)-SCR mechanism.

关键词： NO_(x)removal Vanadia-based catalysts V-O-Ti entities Interface sites Reaction mechanism

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Mechanism for the promotional formation of NH_(4)^(+) by SO_(2) on different mineral dust surfaces

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Particuology 2023年第4期75卷 109-118页

作者： Hao Li Qingxin Ma Biwu Chu Hong He State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-environmental SciencesChinese Academy of SciencesBeijing100085China Center for Excellence in Regional Atmospheric Environment Institute of Urban EnvironmentChinese Academy of SciencesXiamen361021China Institute of Atmospheric Physics Chinese Academy of SciencesBeijing100029China

Ammonium is an important atmospheric particulate component that dictates many environmental *** promotion of the heterogeneous conversion of NH_(3) to NH_(4)^(+) by SO_(2) on different mineral dust surfaces displays remarkable discrepancies,especially on MgO and α-Fe2O3 surfaces,however,the underlying mechanisms are not well ***,using periodic density functional theory(DFT)calculation and Born-Oppenheimer molecular dynamics(BOMD)simulation,we explored the hetero-geneous adsorption of NH_(3) on MgO(110)and α--Fe2O3(001)surfaces in the presence and absence of SO_(2).The results show that on MgO(110)surface,hydrogen-bonding interactions of NH_(3) on both adsorbed hydroxyl or bisulfite/bisulfate sites are observed no matter whether SO_(2) is present or ***,on theα-Fe2O3(001)surface,significant conversion of NH_(3) to NH_(4)^(+)occurs with the coexistence of SO_(2),which is due to the hydrogen transfer reaction from surface HSO4 to N in NH_(3).The fundamental reason may be that the stronger electron affinity of Fe3+than Mg2+results in adsorbed bisulfate and/or bisulfite with greater acidity on α-Fe2O3 surface than MgO *** results give a molecular-level explanation for the heterogeneous conversion of NH_(3) to NH_(4)^(+)on different mineral dust surfaces under complex air pollution *** the fact that ammonium is abundant in secondary particulates,this work would help in understanding the rapid conversion of ammonia to ammonium and in developing classification governance policies for the key precursor pollutants in China.

关键词： Mineral dust Heterogeneous reaction Theoretical calculation Ammonium SO_(2)

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Insight into the effects of C_(3)H_(6)on fresh and hydrothermally aged Cu-SSZ-39 catalysts

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Chinese Chemical Letters 2025年第3期36卷 164-169页

作者： Jinpeng Du Junlin Chen Yulong Shan Tongliang Zhang Yu Sun Zhongqi Liu Xiaoyan Shi Wenpo Shan Yunbo Yu Hong He State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China University of Chinese Academy of Sciences Beijing 100049China Ganjiang Innovation Academy Chinese Academy of SciencesGanzhou 341119China Center for Excellence in Regional Atmospheric Environment Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China

Hydrocarbons(HCs),as major poisoning substances,have a crucial influence on NH_(3)-SCR *** this work,the effects of C_(3)H_(6)on fresh and hydrothermally aged Cu-SSZ-39 catalysts with different copper contents were *** catalysts suffered a deactivation above 250℃,especially between 300-400℃,which was mainly related to the reaction between NH_(3)and C_(3)H_(6).However,the hydrothermally aged and the high-copper-loaded Cu-SSZ-39 catalysts could achieve a recovery of NH_(3)-SCR performance at high *** activity recovery was attributed to the oxidation of C_(3)H_(6)by CuxOy species,which therefore inhibited the reaction between NH_(3)and C_(3)H_(6).As a result,more NH_(3)could be available for the NH_(3)-SCR reaction and the Cu-SSZ-39 catalysts could maintain a good catalytic *** on these findings,we proposed that high loaded Cu-SSZ-39 catalysts with a little CuOx formed are preferred for application.

关键词： Diesel vehicle emission NO_(x)abatement NH3-SCR Cu-SSZ-39 zeolite C_(3)H_(6)poisoning

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