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Physical and chemical processes of wintertime secondary nitrate aerosol formation

Qi YING

《环境科学与工程前沿（英文）》 2011年 第5卷 第3期   页码 348-361 doi: 10.1007/s11783-011-0343-1

摘要： The UCD/CIT model was modified to include a process analysis (PA) scheme for gas and particulate matter (PM) to study the formation of secondary nitrate aerosol during a stagnant wintertime air pollution episode during the California Regional PM /PM Air Quality Study (CRPAQS) where detailed measurements of PM components are available at a few sites. Secondary nitrate is formed in the urban areas from near the ground to a few hundred meters above the surface during the day with a maximum modeled net increase rate of 4 μg·m ·d during the study episode. The secondary nitrate formation rate in rural areas is lower due to lower NO . In the afternoon hours, near-surface temperature can be high enough to evaporate the particulate nitrate. In the nighttime hours, both the gas phase N O reactions with water vapor and the N O heterogeneous reactions with particle-bound water are important for secondary nitrate formation. The N O reactions are most import near the surface to a few hundred meters above surface with a maximum modeled net secondary nitrate increase rate of 1 μg·m ·d and are more significant in the rural areas where the O concentrations are high at night. In general, vertical transport during the day moves the nitrate formed near the surface to higher elevations. During the stagnant days, process analysis indicates that the nitrate concentration in the upper air builds up and leads to a net downward flux of nitrate through vertical diffusion and a rapid increase of surface nitrate concentration.

关键词： secondary nitrate aerosol     N2O5 heterogeneous reaction     process analysis    

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Formation of secondary inorganic aerosol in a frigid urban atmosphere

《环境科学与工程前沿（英文）》 2022年 第16卷 第2期 doi: 10.1007/s11783-021-1452-0

摘要：

•Harbin showed relatively high threshold RH (80%) for apparent increase of SOR.

关键词： Haze     Sulfate     Nitrate     Heterogeneous chemistry     Biomass burning     Northeast China    

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Effects of two transition metal sulfate salts on secondary organic aerosol formation in toluene/NO

Biwu CHU, Jiming HAO, Junhua LI, Hideto TAKEKAWA, Kun WANG, Jingkun JIANG

《环境科学与工程前沿（英文）》 2013年 第7卷 第1期   页码 1-9 doi: 10.1007/s11783-012-0476-x

摘要： Aerosol phase reactions play a very important role on secondary organic aerosol (SOA) formation, and metal-containing aerosols are important components in the atmosphere. In this study, we tested the effects of two transition metal sulfate salts, manganese sulfate (MnSO ) and zinc sulfate (ZnSO ), on the photochemical reactions of a toluene/NO photooxidation system in a 2 m smog chamber. By comparing photochemical reaction products of experiments with and without transition metal sulfate seed aerosols, we evaluated the effects of transition metal sulfate seed aerosols on toluene consumption, NO conversion and the formation of ozone and SOA. MnSO and ZnSO seed aerosols were found to have similar effects on photochemical reactions, both enhance the SOA production, while showing negligible effects on the gas phase compounds. These observations are consistent when varying metal sulfate aerosol concentrations. This is attributed to the catalytic effects of MnSO and ZnSO seed aerosols which may enhance the formation of condensable semivolatile compounds. Their subsequent partitioning into the aerosol phase leads to the observed SOA formation enhancement.

关键词： manganese sulfate     zinc sulfate     seed aerosols     toluene photooxidation     secondary organic aerosol    

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New insights into the formation of ammonium nitrate from a physical and chemical level perspective

《环境科学与工程前沿（英文）》 2023年 第17卷 第11期 doi: 10.1007/s11783-023-1737-6

摘要：

● Factor analysis of ammonium nitrate formation based on thermodynamic theory.

关键词： Ammonium nitrate formation     Thermodynamic theory     Aerosol liquid water content     Source apportionment    

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Secondary aerosol formation in winter haze over the Beijing-Tianjin-Hebei Region, China

Dongjie Shang, Jianfei Peng, Song Guo, Zhijun Wu, Min Hu

《环境科学与工程前沿（英文）》 2021年 第15卷 第2期 doi: 10.1007/s11783-020-1326-x

摘要： Abstract • Characteristics and interannual variation of aerosol pollution are illustrated. • Mechanisms of secondary aerosol formation in winter haze of North China are reviewed. • Directions in future studies of secondary aerosol formation are provided. Severe haze pollution occurs frequently in the winter over the Beijing-Tianjin-Hebei (BTH) region (China), exerting profound impacts on air quality, visibility, and human health. The Chinese Government has taken strict mitigation actions since 2013 and has achieved a significant reduction in the annual mean PM2.5 concentration over this region. However, the level of secondary aerosols during heavy haze episodes showed little decrease during this period. During heavy haze episodes, the concentrations of secondary aerosol components, including sulfate, nitrate and secondary organics, in aerosol particles increase sharply, acting as the main contributors to aerosol pollution. To achieve effective control of particle pollution in the BTH region, the precise and complete secondary aerosol formation mechanisms have been investigated, and advances have been made about the mechanisms of gas phase reaction, nucleation and heterogeneous reactions in forming secondary aerosols. This paper reviews the research progress in aerosol chemistry during haze pollution episodes in the BTH region, lays out the challenges in haze formation studies, and provides implications and directions for future research.

关键词： Secondary aerosol formation     Regional haze     Photochemical reaction     Aqueous reaction     Chemical mechanism    

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Homogeneous and heterogeneous photolysis of nitrate in the atmosphere: state of the science, current

《环境科学与工程前沿（英文）》 2023年 第17卷 第4期 doi: 10.1007/s11783-023-1648-6

摘要：

● Recent advances in the photolysis of nitrate/HNO3 are reviewed.

关键词： Nitrate     Photolysis     Renoxification     Aerosol    

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Size-resolved aerosol ionic composition and secondary formation at Mount Heng in South Central China

Xinfeng WANG, Wenxing WANG, Likun XUE, Xiaomei GAO, Wei NIE, Yangchun YU, Yang ZHOU, Lingxiao YANG, Qingzhu ZHANG, Tao WANG

《环境科学与工程前沿（英文）》 2013年 第7卷 第6期   页码 815-826 doi: 10.1007/s11783-013-0503-6

摘要： To understand the size-resolved aerosol ionic composition and the factors influencing secondary aerosol formation in the upper boundary layer in South Central China, size-segregated aerosol samples were collected using a micro-orifice uniform deposit impactor (MOUDI) in spring 2009 at the summit of Mount Heng (1269 m asl), followed by subsequent laboratory analyses of 13 inorganic and organic water-soluble ions. During non-dust-storm periods, the average PM concentration was 41.8 μg·m , contributing to 55% of the PM . Sulfates, nitrates, and ammonium, the dominant ions in the fine particles, amounted to 46.8% of the PM . Compared with Mount Tai in the North China Plain, the concentrations of both fine and coarse particles and the ions contained therein were substantially lower. When the air masses from Southeast Asia prevailed, intensive biomass burning there led to elevated concentrations of sulfates, nitrates, ammonium, potassium, and chloride in the fine particles at Mount Heng. The air masses originating from the north Gobi brought heavy dust storms that resulted in the remarkable production of sulfates, ammonium, methane sulfonic acid, and oxalates in the coarse particles. Generally, the sulfates were primarily produced in the form of (NH ) SO in the droplet mode via heterogeneous aqueous reactions. Only approximately one-third of the nitrates were distributed in the fine mode, and high humidity facilitated the secondary formation of fine nitrates. The heterogeneous formation of coarse nitrates and ammonium on dry alkaline dust surfaces was found to be less efficient than that on the coarse particles during non-dust-storm periods.

关键词： aerosol water-soluble ions     size distributions     secondary formation     dust storm     Mount Heng    

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Response of organic aerosol characteristics to emission reduction in Yangtze River Delta region

《环境科学与工程前沿（英文）》 2023年 第17卷 第9期 doi: 10.1007/s11783-023-1714-0

摘要：

● The emission reduction causes significant change in organic aerosol composition.

关键词： Emission control     Secondary organic aerosol     Atmospheric oxidizing capacity     Holiday effects     COVID-19 lockdown    

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Effects of seed particles Al

Xiao Zhang, Biwu Chu, Junhua Li, Chaozhi Zhang

《环境科学与工程前沿（英文）》 2017年 第11卷 第4期 doi: 10.1007/s11783-017-0936-4

摘要： Seed particles Al O , Al (SO ) and H SO were selected to investigate their effects on secondary aerosol (SA) formation in toluene/NO photooxidation under sulfur dioxide (SO ) and ammonia (NH ). Effect of seed particles on SA formation was related to their acid-base properties and the presence of acid or alkaline gases. Under NH -poor condition, SA formation increased with increasing SO concentration due to the acid-catalyzing effect of the oxidation products of SO (i.e. H SO ). The enhancing effect of SO became unobvious under NH -rich condition, because NH would eliminate the acid-catalyzing effect by neutralizing the acid products. Acidic seeds H SO accelerated SA formation under either SO or NH condition. Weak acidic Al (SO ) seeds didn’t affect obviously on SA formation. The inhibiting effect of amphoteric seeds Al O on SA formation was related to the presence of SO / NH due to their acid-base property. Under NH -poor condition, the inhibiting effect of Al O on SA formation decreased with increasing concentration of SO , while under NH -rich condition, the inhibiting effect wasn’t remarkable.

关键词： Seed particle     Secondary aerosol     Sulfur dioxide     Ammonia     Acid-catalyzing effect    

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On secondary new particle formation in China

Markku Kulmala,Tuukka Petäjä,Veli-Matti Kerminen,Joni Kujansuu,Taina Ruuskanen,Aijun Ding,Wei Nie,Min Hu,Zhibin Wang,Zhijun Wu,Lin Wang,Douglas R. Worsnop

《环境科学与工程前沿（英文）》 2016年 第10卷 第5期 doi: 10.1007/s11783-016-0850-1

摘要： Formation of new atmospheric aerosol particles is a global phenomenon that has been observed to take place in even heavily-polluted environments. In China, new particle production has been observed at very high pollution levels (condensation sink about 0.1s ) in several megacities. A holistic scientific understanding on the atmospheric phenomena associated with air quality as a whole, as well as on the connection between air quality and climate, is lacking at the moment.With a network of observation stations, we will be able to understand the interactions and feedbacks associated with the urban pollution mixture, and ultimately, are ready to make targeted strategies for the pollution control. This paper summaries the recent advances in studying secondary new aerosol formation in China and shows how increased process-level understanding will help us to understand air quality-climate-weather interactions and how the feedbacks and interactions affect the air quality in highly-polluted environments such as those frequently encountered in Chinese megacities. Formation of new atmospheric aerosol particles is a global phenomenon that has been observed to take place in even heavily-polluted environments. However, in all environments there appears to be a threshold value of the condensation sink (due to pre-existing aerosol particles) after which the formation rate of 3 nm particles is no longer detected. In China, new particle production has been observed at very high pollution levels (condensation sink about 0.1 s ) in several megacities, including Beijing, Shanghai and Nanjing as well as in Pearl River Delta (PRD). Here we summarize the recent findings obtained from these studies and discuss the various implications these findings will have on future research and policy.

关键词： Aerosol particles     Heavily-polluted environments     Condensation sink     New particle production     Megacities    

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Screening the emission sources of volatile organic compounds (VOCs) in China by multi-effects evaluation

He NIU,Ziwei MO,Min SHAO,Sihua LU,Shaodong XIE

《环境科学与工程前沿（英文）》 2016年 第10卷 第5期 doi: 10.1007/s11783-016-0828-z

摘要： We develop a multi-effect evaluation method to assess integrated impact of VOCs. Enable policy-makers to identify important emission sources, regions, and key species. Solvent usage and industrial process are the most important anthropogenic sources. Styrene, toluene, ethylene, benzene, and m/p-xylene are key species to be cut. Volatile organic compounds (VOCs) play important roles in the atmosphere via three main pathways: photochemical ozone formation, secondary organic aerosol production, and direct toxicity to humans. Few studies have integrated these effects to prioritize control measures for VOCs sources. In this study, we developed a multi-effects evaluation methodology based on updated emission inventories and source profiles, by combining the ozone formation potential (OFP), secondary organic aerosol potential (SOAP), and VOC toxicity data. We derived species-specific emission inventories for 152 sources. The OFPs, SOAPs, and toxicity of each source were estimated, the contribution and sharing of source to each of these adverse effects were calculated. Weightings were given to the three adverse effects by expert scoring, and then the integrated effect was determined. Taking 2012 as the base year, solvent use and industrial process were found to be the most important anthropogenic sources, accounting for 24.2% and 23.1% of the integrated effect, respectively, followed by biomass burning, transportation, and fossil fuel combustion, each had a similar contribution ranging from 16.7% to 18.6%. The top five industrial sources, including plastic products, rubber products, chemical fiber products, the chemical industry, and oil refining, accounted for nearly 70.0% of industrial emissions. Beijing, Chongqing, Shanghai, Jiangsu, and Guangdong were the five provinces contributing the largest integrated effects. For the VOC species from emissions showed the largest contributions were styrene, toluene, ethylene, benzene, and m/p-xylene.

关键词： Ozone formation     Secondary organic aerosol     Multi-effects evaluation     VOC abatement strategy    

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Recent advances and challenges of nitrogen/nitrate electro catalytic reduction to ammonia synthesis

《能源前沿（英文）》 2024年 第18卷 第2期   页码 128-140 doi: 10.1007/s11708-023-0908-2

摘要： The Haber-Bosch process is the most widely used synthetic ammonia technology at present. Since its invention, it has provided an important guarantee for global food security. However, the traditional Haber-Bosch ammonia synthesis process consumes a lot of energy and causes serious environmental pollution. Under the serious pressure of energy and environment, a green, clean, and sustainable ammonia synthesis route is urgently needed. Electrochemical synthesis of ammonia is a green and mild new method for preparing ammonia, which can directly convert nitrogen or nitrate into ammonia using electricity driven by solar, wind, or water energy, without greenhouse gas and toxic gas emissions. Herein, the basic mechanism of the nitrogen reduction reaction (NRR) to ammonia and nitrate reduction reaction (NO3− RR) to ammonia were discussed. The representative approaches and major technologies, such as lithium mediated electrolysis and solid oxide electrolysis cell (SOEC) electrolysis for NRR, high activity catalyst and advanced electrochemical device fabrication for NO3 − RR and electrochemical ammonia synthesis were summarized. Based on the above discussion and analysis, the main challenges and development directions for electrochemical ammonia synthesis were further proposed.

关键词： electrochemical ammonia synthesis     nitrogen     nitrate     nitrogen reduction reaction (NRR) to ammonia     nitrate reduction reaction (NO–3 RR)    

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Computational fluid dynamics simulation of aerosol transport and deposition

Yingjie TANG, Bing GUO

《环境科学与工程前沿（英文）》 2011年 第5卷 第3期   页码 362-377 doi: 10.1007/s11783-011-0365-8

摘要： In this article computational fluid dynamics (CFD) simulation of aerosol transport and deposition, i.e. the transport and deposition of particles in an aerosol, is reviewed. The review gives a brief account of the basics of aerosol mechanics, followed by a description of the general CFD approach for flow field simulation, turbulence modeling, wall treatments and simulation of particle motion and deposition. Then examples from the literature are presented, including CFD simulation of particle deposition in human respiratory tract and particle deposition in aerosol devices. CFD simulation of particle transport and deposition may provide information that is difficult to obtain through physical experiments, and it may help reduce the number of experiments needed for device design. Due to the difficulty of describing turbulent flow and particle-eddy interaction, turbulent dispersion of particles remains one of the greatest challenges for CFD simulation. However, it is possible to take a balanced approach toward quantitative description of aerosol dispersion using CFD simulation in conjunction with empirical relations.

关键词： computational fluid dynamics (CFD)     aerosol     transport     deposition    

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Calculation of collision frequency function for aerosol particles in free molecule regime in presence

Xiaowei LUO, Yannick BENICHOU, Suyuan YU

《能源前沿（英文）》 2013年 第7卷 第4期   页码 506-510 doi: 10.1007/s11708-013-0275-5

摘要： The collision frequency function for aerosol particles has already been calculated for the free molecule regime and for the continuum range. The present work, taking into account the influence of internal force fields such as magnetic force, electric force and molecular forces, created by particles themselves, recalculated the collision frequency in the case of particles much smaller than the mean free path of the gas (free molecule regime). Attractive forces increase naturally the collision frequency, while repulsive forces decrease it. The calculation was performed for all types of central forces deriving from a potential, including Coulomb forces and Van der Waals forces.

关键词： aerosol particles     collision frequency function     coagulation    

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Aerosol exposure assessment during reclaimed water utilization in China and risk evaluation in case of

《环境科学与工程前沿（英文）》 2022年 第16卷 第7期 doi: 10.1007/s11783-021-1516-1

摘要：

• The Chinese population exposure habits were surveyed.

关键词： Legionella     QMRA     Reclaimed water     Aerosol     Water reuse    

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标题 作者 时间 类型 操作

Physical and chemical processes of wintertime secondary nitrate aerosol formation

Qi YING

期刊论文

Formation of secondary inorganic aerosol in a frigid urban atmosphere

期刊论文

Effects of two transition metal sulfate salts on secondary organic aerosol formation in toluene/NO

Biwu CHU, Jiming HAO, Junhua LI, Hideto TAKEKAWA, Kun WANG, Jingkun JIANG

期刊论文

New insights into the formation of ammonium nitrate from a physical and chemical level perspective

期刊论文

Secondary aerosol formation in winter haze over the Beijing-Tianjin-Hebei Region, China

Dongjie Shang, Jianfei Peng, Song Guo, Zhijun Wu, Min Hu

期刊论文

Homogeneous and heterogeneous photolysis of nitrate in the atmosphere: state of the science, current

期刊论文

Size-resolved aerosol ionic composition and secondary formation at Mount Heng in South Central China

Xinfeng WANG, Wenxing WANG, Likun XUE, Xiaomei GAO, Wei NIE, Yangchun YU, Yang ZHOU, Lingxiao YANG, Qingzhu ZHANG, Tao WANG

期刊论文

Response of organic aerosol characteristics to emission reduction in Yangtze River Delta region

期刊论文

Effects of seed particles Al

Xiao Zhang, Biwu Chu, Junhua Li, Chaozhi Zhang

期刊论文

On secondary new particle formation in China

Markku Kulmala,Tuukka Petäjä,Veli-Matti Kerminen,Joni Kujansuu,Taina Ruuskanen,Aijun Ding,Wei Nie,Min Hu,Zhibin Wang,Zhijun Wu,Lin Wang,Douglas R. Worsnop

期刊论文

Screening the emission sources of volatile organic compounds (VOCs) in China by multi-effects evaluation

He NIU,Ziwei MO,Min SHAO,Sihua LU,Shaodong XIE

期刊论文

Recent advances and challenges of nitrogen/nitrate electro catalytic reduction to ammonia synthesis

期刊论文

Computational fluid dynamics simulation of aerosol transport and deposition

Yingjie TANG, Bing GUO

期刊论文

Calculation of collision frequency function for aerosol particles in free molecule regime in presence

Xiaowei LUO, Yannick BENICHOU, Suyuan YU

期刊论文

Aerosol exposure assessment during reclaimed water utilization in China and risk evaluation in case of

期刊论文