Upgrading of abundant cellulosic biomass to isosorbide can reduce the dependence on limited fossil resources and provide a sustainable way to produce isosorbide,utilized for polymers,medicine and health care product s...Upgrading of abundant cellulosic biomass to isosorbide can reduce the dependence on limited fossil resources and provide a sustainable way to produce isosorbide,utilized for polymers,medicine and health care product synth-esis.This review comprehensively examines the key steps and catalytic systems involved in the conversion of cel-lulose to isosorbide.Initially,the reaction pathway from cellulose to isosorbide is elucidated,emphasizing three critical steps:cellulose hydrolysis,glucose hydrogenation,and the two-step dehydration of sorbitol to produce isosorbide.Additionally,the activation energy and acidic sites during cellulose hydrolysis,the impact of metal particle size and catalyst support on hydrogenation,and the effects of catalyst acidity,pore structure,and reaction conditions on sorbitol dehydration have been thoroughly examined.Finally,the progress made in cellulose con-version to isosorbide is summarized,current challenges are highlighted,and future development trends are pro-jected in this review.展开更多
Image description task is the intersection of computer vision and natural language processing,and it has important prospects,including helping computers understand images and obtaining information for the visually imp...Image description task is the intersection of computer vision and natural language processing,and it has important prospects,including helping computers understand images and obtaining information for the visually impaired.This study presents an innovative approach employing deep reinforcement learning to enhance the accuracy of natural language descriptions of images.Our method focuses on refining the reward function in deep reinforcement learning,facilitating the generation of precise descriptions by aligning visual and textual features more closely.Our approach comprises three key architectures.Firstly,it utilizes Residual Network 101(ResNet-101)and Faster Region-based Convolutional Neural Network(Faster R-CNN)to extract average and local image features,respectively,followed by the implementation of a dual attention mechanism for intricate feature fusion.Secondly,the Transformer model is engaged to derive contextual semantic features from textual data.Finally,the generation of descriptive text is executed through a two-layer long short-term memory network(LSTM),directed by the value and reward functions.Compared with the image description method that relies on deep learning,the score of Bilingual Evaluation Understudy(BLEU-1)is 0.762,which is 1.6%higher,and the score of BLEU-4 is 0.299.Consensus-based Image Description Evaluation(CIDEr)scored 0.998,Recall-Oriented Understudy for Gisting Evaluation(ROUGE)scored 0.552,the latter improved by 0.36%.These results not only attest to the viability of our approach but also highlight its superiority in the realm of image description.Future research can explore the integration of our method with other artificial intelligence(AI)domains,such as emotional AI,to create more nuanced and context-aware systems.展开更多
Intensive measurements were conducted in Xi’an,China before and during a COVID-19 lockdown period to investigate how changes in anthropogenic emissions affected the optical properties and radiative effects of brown c...Intensive measurements were conducted in Xi’an,China before and during a COVID-19 lockdown period to investigate how changes in anthropogenic emissions affected the optical properties and radiative effects of brown carbon(BrC)aerosol.The contribution of BrC to total aerosol light absorption during the lockdown(13%-49%)was higher compared with the normal period(4%-29%).Mass absorption cross-sections(MACs)of specific organic aerosol(OA)factors were calculated from a ridge regression model.Of the primary OA(POA),coal combustion OA(CCOA)had the largest MACs at all tested wave-lengths during both periods due to high molecular-weight BrC chromophores;that was followed by biomass burning OA(BBOA)and hydrocarbon-like OA(HOA).For secondary OA(SOA),the MACs of the lessoxidized oxygenated OA(OOA)species(LO-OOA)atλ=370-590 nm were higher than those of more-oxidized OOA(MO-OOA)during both periods,presumably due to chromophore bleaching.The largest contributor to BrC absorption at the short wavelengths was CCOA during both periods,but BrC absorption by LO-OOA and MO-OOA became dominant at longer wavelengths during the lockdown.The estimated radiation forcing efficiency of BrC over 370-600 nm increased from 37.5 W·gduring the normal period to 50.2 W·gduring the lockdown,and that enhancement was mainly caused by higher MACs for both LO-OOA and MO-OOA.This study provides insights into the optical properties and radiative effects of source-specific BrC aerosol when pollution emissions are reduced.展开更多
The effects of aerosol-radiation interactions(ARI)are not only important for regional and global climate,but they can also drive particulate matter(PM)pollution.In this study,the ARI contribution to the near-surface f...The effects of aerosol-radiation interactions(ARI)are not only important for regional and global climate,but they can also drive particulate matter(PM)pollution.In this study,the ARI contribution to the near-surface fine PM(PM_(2.5))concentrations in the Guanzhong Basin(GZB)is evaluated under four unfavorable synoptic patterns,including“northlow”,“transition”,“southeast-trough”,and“inland-high”,based on WRF-Chem model simulations of a persistent heavy PM pollution episode in January 2019.Simulations show that ARI consistently decreases both solar radiation reaching down to the surface(SWDOWN)and surface temperature(TSFC),which then reduces wind speed,induces sinking motion,and influences cloud formation in the GZB.However,large differences under the four synoptic patterns still exist.The average reductions of SWDOWN and daytime TSFC in the GZB range from 15.2%and 1.04°C in the case of the“transition”pattern to 26.7%and 1.69°C in the case of the“north-low”pattern,respectively.Furthermore,ARI suppresses the development of the planetary boundary layer(PBL),with the decrease of PBL height(PBLH)varying from 18.7%in the case of the“transition”pattern to 32.0%in the case of the“north-low”pattern.The increase of daytime near-surface PM_(2.5)in the GZB due to ARI is 12.0%,8.1%,9.5%,and 9.7%under the four synoptic patterns,respectively.Ensemble analyses also reveal that when near-surface PM_(2.5)concentrations are low,ARI tends to lower PM_(2.5)concentrations with decreased PBLH,which is caused by enhanced divergence or a transition from divergence to convergence in an area.ARI contributes 15%-25%toward the near-surface PM_(2.5)concentrations during the severe PM pollution period under the four synoptic patterns.展开更多
In this study,online water-soluble inorganic ions were detected to deduce the formation mechanism of secondary inorganic aerosol in Xianyang,China during wintertime.The dominant inorganic ions of sulfate(SO_(4)^(2-)),...In this study,online water-soluble inorganic ions were detected to deduce the formation mechanism of secondary inorganic aerosol in Xianyang,China during wintertime.The dominant inorganic ions of sulfate(SO_(4)^(2-)),nitrate(NO_(3)^(-)),and ammonium(NH_(4)^(+))(the sum of those is abbreviated as SNA)accounted for 17%,21%,and 12% of PM_(2.5)mass,respectively.While the air quality deteriorated from excellent to poor grades,the precursor gas sulfur dioxide(SO_(2))of SO_(4)^(2-)increased and then decreased with a fluctuation,while nitrogen dioxide(NO_(2))and ammonia(NH_(3)),precursors of NO_(3)^(-)and NH_(4)^(+),and SNA show increasing trends.Meteorological factors including boundary layer height(BLH),temperature,and wind speed also show decline trends,except relative humidity(RH).Meanwhile,the secondary conversion ratio shows a remarkable increasing trend,indicating that there was a strong secondary transformation.From the perspective of chemical mechanisms,RH is positively correlated with sulfur oxidation ratios(SOR),nitrogen oxidation ratios(NOR),and ammonia conversion ratios,representing that the increase of humidity could promote the generation of SNA.Notably,SOR and NOR were also positively related to the ammonia.On the one hand,the low wind speed and BLH led to the accumulation of pollutants.On the other hand,the increases of RH and ammonia promoted more formations of SNA and PM_(2.5).The results advance our identification of the contributors to the haze episodes and assist to establish more efficient emission controls in Xianyang,in addition to other cities with similar emission and geographical characteristics.展开更多
Water-soluble inorganic ions(WSIIs)play a pivotal role in atmospheric chemical reactions,particularly influencing the formation of secondary particulate matter.A comprehensive grasp of the vertical distribution of atm...Water-soluble inorganic ions(WSIIs)play a pivotal role in atmospheric chemical reactions,particularly influencing the formation of secondary particulate matter.A comprehensive grasp of the vertical distribution of atmospheric pollutants holds immense significance in understanding the diffusion and transportation of these pollutants.This study investigates the WSIIs of PM_(2.5)and size-segregated particles at the top(~2060 m a.s.l.)and foot of Mt.Hua during the winter of 2020.All the measured ions present significant higher concentrations(1.9~6.9 times)at the foot than the top.Cl^(-)and K^(+)at the foot are more than 4 times of those at the top,whereas Ca^(2+)and Mg^(2+)are only 1.3-1.9 times higher.The particle size distribution of NO_(3)^(-),SO_(4)^(2-),K^(+)and Cl^(-)demonstrate a single peak distribution(0.7-1.1μm)at the foot,but with a bimodal distribution(0.7-1.1μm and 4.7-5.8μm)at the top.These differences suggest that the aerosol at the alpine region is mainly transported via long-distance from Northwest/North China,but limited influenced by vertical transport through valley breeze.The changes of concentration and size distribution of WSIIs in dust event and non-dust period indicate that the effects of dust event on aerosols at ground surface were weaker than that of the free troposphere of Guanzhong Plain.Notably,our study underscores the dominant influence of NO_(3)^(-)in shaping the gas-particle distribution of ammonia within the winter free troposphere.Our results highlight the significant role of long-range transport on aerosols in the free troposphere in Guanzhong Plain,Northwest China.展开更多
With the strengthened controls on SO2 emissions and extensive increases in motor vehicles'exhaust,aerosol pollution shifts from sulfate-rich to nitrate-rich in recent years in Xi'an,China.To further gain insig...With the strengthened controls on SO2 emissions and extensive increases in motor vehicles'exhaust,aerosol pollution shifts from sulfate-rich to nitrate-rich in recent years in Xi'an,China.To further gain insights into the factors on nitrate formation and efficiently mitigate air pollution,highly time-resolved observations of water-soluble inorganic ions(WSIIs)in PM_(2.5) were measured in a suburban area of Xi'an,China during wintertime.Hourly concentration of total WSIIs is 39.8μg m-3 on average,accounting for 50.3%of PM_(2.5) mass.In contrast to a slight decrease in the mass fraction of SO_(4)^(2-),NO_(3)-shows a sig-nificant increase of the PM_(2.5) contribution with the aggravation of aerosol pollution.This suggests the importance of NO_(3)-formation to haze evolution.Furthermore,homogeneous reactions govern the formation of NO_(3)-,while alkali metals such as calcium and sodium play an additional role in retaining NO_(3)-in PM_(2.5) during clean periods.However,the heterogeneous hydrolysis reaction contributed more to NO_(3)-formation during the pollution periods under high relative humidity.Our investigation reveals that temperature,relative humidity,oxidant,and ammonia emissions facilitate rapid NO_(3)-formation.Using the random forest(RF)model,NO_(3)-concentrations were successfully simulated with measured variables for the training and testing datasets(R2>0.95).Among these variables,CO,NH_(3),and NO_(2) were found to be the main factors affecting the NO_(3)-concentrations.Compared with the period without vehicle re-striction,the contributions of NO_(3)-and NH4+to PM_(2.5) mass decreased by 5.3%and 3.4%in traffic re-striction periods,respectively.The vehicle restriction leads to the decreases of precursor gases of NO_(2),SO_(2),and NH_(3) by 12.8%,5.9%,and 27.6%,respectively.The results demonstrate collaborative emission reduction of NO_(x) and NH_(3) by vehicle restrictions,and using new energy vehicles(or electric vehicles)can effectively alleviate particulate matter pollution in northwest China.展开更多
Ambient PM2.5 samples were collected at four sites in Xiamen, including Gulangyu (GLY). Hongwen (HW), Huli (HL) and Jimei (JM) during January, April, July and October 2013. Local source samples were obtained f...Ambient PM2.5 samples were collected at four sites in Xiamen, including Gulangyu (GLY). Hongwen (HW), Huli (HL) and Jimei (JM) during January, April, July and October 2013. Local source samples were obtained from coal burning power plants, industries, motor vehicles, biomass burning, fugitive dust, and sea salt for the source apportionment studies. The highest value of PM2.5 mass concentration and species related to human activities (SO42- , NO3 , Pb, Ni, V, Cu, Cd, organic carbon (OC) andelemental carbon (EC)) were found in the ambient-samples from HL, and t-he highest and lowest loadings of PM2.5 and its components occurred in winter and summer, respectively. The reconstructed mass balance indicated that ambient PM2.5 consisted of 24% OM (organic matter), 23% sulfate, 14% nitrate, 9% ammonium, 9% geological material, 6% sea salt, 5% EC and 10% others. For the source profiles, the dominant components were OC for coal burning, motor vehicle, biomass burning and sea salt; SO42 for industry; and crustal elements for fugitive dust. Source contributions were calculatedusing a chemical mass'balance (CMB) model basedon ambient PM2.5 concentrations and the source profiles. GLY was characterized by high contributions from secondary sulfate and cooking, while HL and JM were most strongly affected by motor vehicle emissions, and biomass burning and fugitivedust, respectively. The CMB results-indicated that PM2.5 from Xiamen is composed of 27.4% secondary inorganic components, 20.8% motor vehicle emissions, 11.7% fugitive dust, 9.9% sea salt, 9.3% coal burning, 5.0% biomass burning, 3.1% industry and 6.8% others.展开更多
Air pollution is serious during autumn in the Beijing-Tianjin-Hebei(BTH)region,but there are few studies that have utilized real-time observations and source apportionment of the autumn submicron aerosols in this regi...Air pollution is serious during autumn in the Beijing-Tianjin-Hebei(BTH)region,but there are few studies that have utilized real-time observations and source apportionment of the autumn submicron aerosols in this region.In this study,a quadrupole aerosol chemical speciation monitor(Q-ACSM)was deployed for the real-time measurement of the non-refractory compositions of submicron aerosols(NR-PM1)at a regional site(Xianghe)from October 3 to November 14,2017.The results showed that nitrate was the largest inorganic aerosol,and the oxygenated organic aerosol(OOA)was the largest organic aerosol in Xianghe.Hydrocarbon-like OA(HOA)was the largest organic aerosol When the NR-PM1 mass concentrations increased from the lowest to the highest bins,nitrate and biomass burning OA(BBOA)showed increasing trends in the suburban area.Enhanced nitrate formation during the pollution epi-sodes resulted from both photochemical and aqueous processing.To reduce the particulate matter(PM2.5)concentrations and eliminate heavy pollution episodes,control measures should focus on reducing NO_(x),NH_(3),and volatile organic compound(VOCs)emissions.展开更多
Daily fine particulate (PM2.5) samples were collected in Chengdu from April 2009 to February 2010 to investigate their chemical profiles during dust storms (DSs) and several types of pollution events, including ha...Daily fine particulate (PM2.5) samples were collected in Chengdu from April 2009 to February 2010 to investigate their chemical profiles during dust storms (DSs) and several types of pollution events, including haze (HDs), biomass burning (BBs), and fireworks displays (FDs). The highest PM2.5 mass concentrations were found during DSs (283.3 μg/m^3), followed by FDs (212.7 μg/m^3), HDs (187.3 μg/m^3 ), and BBs (130.1 μ g/m^3). The concentrations of most elements were elevated during DSs and pollution events, except for BBs. Secondary inorganic ions (NO3^- , SO4^2-, and NH4^+) were enriched during HDs, while PM2.5 from BBs showed high K^+ but low SO4^2- , FDs caused increases in K^+ and enrichment in SO4^2-. Ca^2+. was abundant in DS samples, Ion-balance calculations indicated that PM2.5 from HDs and FDs was more acidic than on normal days, but DS and BB particles were alkaline. The highest organic carbon (OC) concentration was 26.1 μg/m^3 during FDs, followed by BBs (23.6 μg/m^3 ), HDs (19.6 μg/m^3 ), and DSs (18.8 μg/m^3 ). In contrast, elemental carbon (EC) concentration was more abundant during HDs (10.6μg/m^3) and FDs (9.5 μg/m^3) than during BBs (6.2μg/m^3) and DSs (6.0 μg/m^3). The highest OC/EC ratios were obtained during BBs, with the lowest during HDs. SO4^2+ /K^+ and TCA/SO4^2- ratios proved to be effective indicators for differentiating pollution events. Mass balance showed that organic matter, SO4^2-, and NO3^- were the dominant chemical components during pollution events, while soil dust was dominant during DSs.展开更多
Mineral dust is an important type of ice nucleating particles in the troposphere;however,the effects of heterogeneous reactions on ice nucleation(IN)activities of mineral dust remain to be elucidated.A droplet-freezin...Mineral dust is an important type of ice nucleating particles in the troposphere;however,the effects of heterogeneous reactions on ice nucleation(IN)activities of mineral dust remain to be elucidated.A droplet-freezing apparatus(Guangzhou Institute of Geochemistry Ice Nucleation Apparatus,GIGINA)was developed in thiswork to measure IN activities of atmospheric particles in the immersion freezingmode,and its performancewas validated by a series of experimental characterizations.This apparatus was then employed to measure IN activities of feldspar and Arizona Test Dust(ATD)particles before and after heterogeneous reaction with NO_(2)(10±0.5 ppmv)at 40%relative humidity.The surface coverage of nitrate,θ(NO_(3)^(−)),increased to 3.1±0.2 for feldspar after reaction with NO_(2) for 6 hr,and meanwhile the active site density per unit surface area(ns)at-20℃ was reduced from 92±5 to<1.0 cm^(−2) by about two orders of magnitude;however,no changes in nitrate content or IN activities were observed for further increase in reaction time(up to 24 hr).Both nitrate content and IN activities changed continuously with reaction time(up to 24 hr)for ATD particles;after reaction with NO_(2) for 24 hr,θ(NO_(3)^(−))increased to 1.4±0.1 and ns at-20℃ was reduced from 20±4 to 9.7±1.9 cm^(−2) by a factor of∼2.Our work suggests that heterogeneous reaction with NO_(2),an abundant reactive nitrogen species in the troposphere,may significantly reduce IN activities of mineral dust in the immersion freezing mode.展开更多
The Northeast Plain in China ranks among the top five regions that have been significantly impacted by haze pollution.To effectively control pollution,it is crucial to accurately assess the effects of emission reducti...The Northeast Plain in China ranks among the top five regions that have been significantly impacted by haze pollution.To effectively control pollution,it is crucial to accurately assess the effects of emission reduction measures.In this study,we analyzed surveillance data and found substantial decreases(ranging from 19.0%to 50.1%)in average annual mass concentrations of key pollutants(such as CO,SO_(2),NO_(2),and PM_(2.5))in the Northeast Plain from 2016 to 2020.To precisely determine the contributions of meteorological conditions and emission reductions to the improvement of air quality in the Northeast Plain,we conducted three scenario simulations.By comparing source emissions in December 2016 and 2020 using the WRF-Chem model(except for SO_(2)),we observed significant reductions of 21.3%,8.8%,and 9.8%in mass concentrations of PM_(2.5),NO_(2),and CO,respectively,from 2016 to 2020.This highlights the essential role that meteorological conditions play in determining air quality in the Northeast Plain.Moreover,further reducing source emissions by 30%in December 2016 resulted in subsequent reductions of 25.3%,29.0%,4.5%,and 30.3%in mass concentrations of PM_(2.5),SO_(2),NO_(2),and CO,respectively,under the same meteorological conditions.Notably,source emission reduction was effective for PM_(2.5),SO_(2),and CO,but not for NO_(2).The improvement in air quality in the Northeast Plain from 2016 to 2020 can be attributed to the combined effects of improved meteorological conditions and reduced pollution sources.展开更多
文摘Upgrading of abundant cellulosic biomass to isosorbide can reduce the dependence on limited fossil resources and provide a sustainable way to produce isosorbide,utilized for polymers,medicine and health care product synth-esis.This review comprehensively examines the key steps and catalytic systems involved in the conversion of cel-lulose to isosorbide.Initially,the reaction pathway from cellulose to isosorbide is elucidated,emphasizing three critical steps:cellulose hydrolysis,glucose hydrogenation,and the two-step dehydration of sorbitol to produce isosorbide.Additionally,the activation energy and acidic sites during cellulose hydrolysis,the impact of metal particle size and catalyst support on hydrogenation,and the effects of catalyst acidity,pore structure,and reaction conditions on sorbitol dehydration have been thoroughly examined.Finally,the progress made in cellulose con-version to isosorbide is summarized,current challenges are highlighted,and future development trends are pro-jected in this review.
基金This research was funded by the Natural Science Foundation of Gansu Province with Approval Numbers 20JR10RA334 and 21JR7RA570Funding is provided for the 2021 Longyuan Youth Innovation and Entrepreneurship Talent Project with Approval Number 2021LQGR20+1 种基金the University Level Innovation Project with Approval NumbersGZF2020XZD18jbzxyb2018-01 of Gansu University of Political Science and Law.
文摘Image description task is the intersection of computer vision and natural language processing,and it has important prospects,including helping computers understand images and obtaining information for the visually impaired.This study presents an innovative approach employing deep reinforcement learning to enhance the accuracy of natural language descriptions of images.Our method focuses on refining the reward function in deep reinforcement learning,facilitating the generation of precise descriptions by aligning visual and textual features more closely.Our approach comprises three key architectures.Firstly,it utilizes Residual Network 101(ResNet-101)and Faster Region-based Convolutional Neural Network(Faster R-CNN)to extract average and local image features,respectively,followed by the implementation of a dual attention mechanism for intricate feature fusion.Secondly,the Transformer model is engaged to derive contextual semantic features from textual data.Finally,the generation of descriptive text is executed through a two-layer long short-term memory network(LSTM),directed by the value and reward functions.Compared with the image description method that relies on deep learning,the score of Bilingual Evaluation Understudy(BLEU-1)is 0.762,which is 1.6%higher,and the score of BLEU-4 is 0.299.Consensus-based Image Description Evaluation(CIDEr)scored 0.998,Recall-Oriented Understudy for Gisting Evaluation(ROUGE)scored 0.552,the latter improved by 0.36%.These results not only attest to the viability of our approach but also highlight its superiority in the realm of image description.Future research can explore the integration of our method with other artificial intelligence(AI)domains,such as emotional AI,to create more nuanced and context-aware systems.
基金financially supported by the Key Research and Development Program of Shaanxi Province(2018-ZDXM3-01)the Strategic Priority Research Program of Chinese Academy of Sciences(XDB40000000)+3 种基金the Sino-Swiss Cooperation on Air Pollution for Better Air(7F-09802.01.02)the Youth Innovation Promotion Association of the Chinese Academy of Sciences(2019402)the Sino-Swiss Science and Technology Cooperation(SSSTC)project HAZECHINA(IZLCZ2_169986)the SDC Clean-Air-China Program(7F-09802.01.03)。
文摘Intensive measurements were conducted in Xi’an,China before and during a COVID-19 lockdown period to investigate how changes in anthropogenic emissions affected the optical properties and radiative effects of brown carbon(BrC)aerosol.The contribution of BrC to total aerosol light absorption during the lockdown(13%-49%)was higher compared with the normal period(4%-29%).Mass absorption cross-sections(MACs)of specific organic aerosol(OA)factors were calculated from a ridge regression model.Of the primary OA(POA),coal combustion OA(CCOA)had the largest MACs at all tested wave-lengths during both periods due to high molecular-weight BrC chromophores;that was followed by biomass burning OA(BBOA)and hydrocarbon-like OA(HOA).For secondary OA(SOA),the MACs of the lessoxidized oxygenated OA(OOA)species(LO-OOA)atλ=370-590 nm were higher than those of more-oxidized OOA(MO-OOA)during both periods,presumably due to chromophore bleaching.The largest contributor to BrC absorption at the short wavelengths was CCOA during both periods,but BrC absorption by LO-OOA and MO-OOA became dominant at longer wavelengths during the lockdown.The estimated radiation forcing efficiency of BrC over 370-600 nm increased from 37.5 W·gduring the normal period to 50.2 W·gduring the lockdown,and that enhancement was mainly caused by higher MACs for both LO-OOA and MO-OOA.This study provides insights into the optical properties and radiative effects of source-specific BrC aerosol when pollution emissions are reduced.
基金This work is financially supported by the National Key R&D Plan(Grant No.2017YFC0210000)the Strategic Priority Research Program of Chinese Academy of Sciences(Grant No.XDB40030200)+1 种基金the National Natural Science Foundation of China(Grant No.41975175)the Fundamental Research Funds for the Central Universities of China。
文摘The effects of aerosol-radiation interactions(ARI)are not only important for regional and global climate,but they can also drive particulate matter(PM)pollution.In this study,the ARI contribution to the near-surface fine PM(PM_(2.5))concentrations in the Guanzhong Basin(GZB)is evaluated under four unfavorable synoptic patterns,including“northlow”,“transition”,“southeast-trough”,and“inland-high”,based on WRF-Chem model simulations of a persistent heavy PM pollution episode in January 2019.Simulations show that ARI consistently decreases both solar radiation reaching down to the surface(SWDOWN)and surface temperature(TSFC),which then reduces wind speed,induces sinking motion,and influences cloud formation in the GZB.However,large differences under the four synoptic patterns still exist.The average reductions of SWDOWN and daytime TSFC in the GZB range from 15.2%and 1.04°C in the case of the“transition”pattern to 26.7%and 1.69°C in the case of the“north-low”pattern,respectively.Furthermore,ARI suppresses the development of the planetary boundary layer(PBL),with the decrease of PBL height(PBLH)varying from 18.7%in the case of the“transition”pattern to 32.0%in the case of the“north-low”pattern.The increase of daytime near-surface PM_(2.5)in the GZB due to ARI is 12.0%,8.1%,9.5%,and 9.7%under the four synoptic patterns,respectively.Ensemble analyses also reveal that when near-surface PM_(2.5)concentrations are low,ARI tends to lower PM_(2.5)concentrations with decreased PBLH,which is caused by enhanced divergence or a transition from divergence to convergence in an area.ARI contributes 15%-25%toward the near-surface PM_(2.5)concentrations during the severe PM pollution period under the four synoptic patterns.
基金supported by the National Key R&D Program of China(No.2022YFF0802501)the Key Research and Development Program of Shaanxi Province(No.2018-ZDXM3-01)the Youth Innovation Promotion Association of the Chinese Academy of Sciences(No.2019402)。
文摘In this study,online water-soluble inorganic ions were detected to deduce the formation mechanism of secondary inorganic aerosol in Xianyang,China during wintertime.The dominant inorganic ions of sulfate(SO_(4)^(2-)),nitrate(NO_(3)^(-)),and ammonium(NH_(4)^(+))(the sum of those is abbreviated as SNA)accounted for 17%,21%,and 12% of PM_(2.5)mass,respectively.While the air quality deteriorated from excellent to poor grades,the precursor gas sulfur dioxide(SO_(2))of SO_(4)^(2-)increased and then decreased with a fluctuation,while nitrogen dioxide(NO_(2))and ammonia(NH_(3)),precursors of NO_(3)^(-)and NH_(4)^(+),and SNA show increasing trends.Meteorological factors including boundary layer height(BLH),temperature,and wind speed also show decline trends,except relative humidity(RH).Meanwhile,the secondary conversion ratio shows a remarkable increasing trend,indicating that there was a strong secondary transformation.From the perspective of chemical mechanisms,RH is positively correlated with sulfur oxidation ratios(SOR),nitrogen oxidation ratios(NOR),and ammonia conversion ratios,representing that the increase of humidity could promote the generation of SNA.Notably,SOR and NOR were also positively related to the ammonia.On the one hand,the low wind speed and BLH led to the accumulation of pollutants.On the other hand,the increases of RH and ammonia promoted more formations of SNA and PM_(2.5).The results advance our identification of the contributors to the haze episodes and assist to establish more efficient emission controls in Xianyang,in addition to other cities with similar emission and geographical characteristics.
基金supported by the program from National Natural Science Foundation of China(Nos.42207555,41977332)Natural Science Basic Research Program of Shaanxi(Nos.2021JQ-971,2022JQ-242)+2 种基金Open Foundation of SKLLQG(No.SKLLQGZR2101)Strategic Priority Research Program of CAS(No.XDB40000000)the support of the Youth Innovation Promotion Association CAS(No.2020407)。
文摘Water-soluble inorganic ions(WSIIs)play a pivotal role in atmospheric chemical reactions,particularly influencing the formation of secondary particulate matter.A comprehensive grasp of the vertical distribution of atmospheric pollutants holds immense significance in understanding the diffusion and transportation of these pollutants.This study investigates the WSIIs of PM_(2.5)and size-segregated particles at the top(~2060 m a.s.l.)and foot of Mt.Hua during the winter of 2020.All the measured ions present significant higher concentrations(1.9~6.9 times)at the foot than the top.Cl^(-)and K^(+)at the foot are more than 4 times of those at the top,whereas Ca^(2+)and Mg^(2+)are only 1.3-1.9 times higher.The particle size distribution of NO_(3)^(-),SO_(4)^(2-),K^(+)and Cl^(-)demonstrate a single peak distribution(0.7-1.1μm)at the foot,but with a bimodal distribution(0.7-1.1μm and 4.7-5.8μm)at the top.These differences suggest that the aerosol at the alpine region is mainly transported via long-distance from Northwest/North China,but limited influenced by vertical transport through valley breeze.The changes of concentration and size distribution of WSIIs in dust event and non-dust period indicate that the effects of dust event on aerosols at ground surface were weaker than that of the free troposphere of Guanzhong Plain.Notably,our study underscores the dominant influence of NO_(3)^(-)in shaping the gas-particle distribution of ammonia within the winter free troposphere.Our results highlight the significant role of long-range transport on aerosols in the free troposphere in Guanzhong Plain,Northwest China.
基金supported by the West Light Foundation of the Chinese Academy of Sciences (grant No.XAB2021YN05)the National Natural Science Foundation of China (grant No.41503123)the National Atmospheric Research Program (grant No.2017YFC0212200).
文摘With the strengthened controls on SO2 emissions and extensive increases in motor vehicles'exhaust,aerosol pollution shifts from sulfate-rich to nitrate-rich in recent years in Xi'an,China.To further gain insights into the factors on nitrate formation and efficiently mitigate air pollution,highly time-resolved observations of water-soluble inorganic ions(WSIIs)in PM_(2.5) were measured in a suburban area of Xi'an,China during wintertime.Hourly concentration of total WSIIs is 39.8μg m-3 on average,accounting for 50.3%of PM_(2.5) mass.In contrast to a slight decrease in the mass fraction of SO_(4)^(2-),NO_(3)-shows a sig-nificant increase of the PM_(2.5) contribution with the aggravation of aerosol pollution.This suggests the importance of NO_(3)-formation to haze evolution.Furthermore,homogeneous reactions govern the formation of NO_(3)-,while alkali metals such as calcium and sodium play an additional role in retaining NO_(3)-in PM_(2.5) during clean periods.However,the heterogeneous hydrolysis reaction contributed more to NO_(3)-formation during the pollution periods under high relative humidity.Our investigation reveals that temperature,relative humidity,oxidant,and ammonia emissions facilitate rapid NO_(3)-formation.Using the random forest(RF)model,NO_(3)-concentrations were successfully simulated with measured variables for the training and testing datasets(R2>0.95).Among these variables,CO,NH_(3),and NO_(2) were found to be the main factors affecting the NO_(3)-concentrations.Compared with the period without vehicle re-striction,the contributions of NO_(3)-and NH4+to PM_(2.5) mass decreased by 5.3%and 3.4%in traffic re-striction periods,respectively.The vehicle restriction leads to the decreases of precursor gases of NO_(2),SO_(2),and NH_(3) by 12.8%,5.9%,and 27.6%,respectively.The results demonstrate collaborative emission reduction of NO_(x) and NH_(3) by vehicle restrictions,and using new energy vehicles(or electric vehicles)can effectively alleviate particulate matter pollution in northwest China.
基金This work was supported by the Xiamen Environ- mental Protection Special Project (No. 19 (10), 2013), Science and Technology Project of Fujian Provincial Environmental Protection Depart- ment (2014), and also supported by a project from Ministry of Science and Technology (2013FY 112700) and the Natural Science Foundation of China (Grant No. 41673125).
文摘Ambient PM2.5 samples were collected at four sites in Xiamen, including Gulangyu (GLY). Hongwen (HW), Huli (HL) and Jimei (JM) during January, April, July and October 2013. Local source samples were obtained from coal burning power plants, industries, motor vehicles, biomass burning, fugitive dust, and sea salt for the source apportionment studies. The highest value of PM2.5 mass concentration and species related to human activities (SO42- , NO3 , Pb, Ni, V, Cu, Cd, organic carbon (OC) andelemental carbon (EC)) were found in the ambient-samples from HL, and t-he highest and lowest loadings of PM2.5 and its components occurred in winter and summer, respectively. The reconstructed mass balance indicated that ambient PM2.5 consisted of 24% OM (organic matter), 23% sulfate, 14% nitrate, 9% ammonium, 9% geological material, 6% sea salt, 5% EC and 10% others. For the source profiles, the dominant components were OC for coal burning, motor vehicle, biomass burning and sea salt; SO42 for industry; and crustal elements for fugitive dust. Source contributions were calculatedusing a chemical mass'balance (CMB) model basedon ambient PM2.5 concentrations and the source profiles. GLY was characterized by high contributions from secondary sulfate and cooking, while HL and JM were most strongly affected by motor vehicle emissions, and biomass burning and fugitivedust, respectively. The CMB results-indicated that PM2.5 from Xiamen is composed of 27.4% secondary inorganic components, 20.8% motor vehicle emissions, 11.7% fugitive dust, 9.9% sea salt, 9.3% coal burning, 5.0% biomass burning, 3.1% industry and 6.8% others.
基金supported by the Strategic Priority Research Program of Chinese Academy of Sciences(grant No.XDB40000000)the National Natural Science Foundation of China(grant Nos.71804115,72102182)+1 种基金the Youth Innovation Promotion Association of the Chinese Academy of Sciences(grant No.2019402)the Soft Science Research Program of Shaanxi Province(grant No.2022KRM071).
文摘Air pollution is serious during autumn in the Beijing-Tianjin-Hebei(BTH)region,but there are few studies that have utilized real-time observations and source apportionment of the autumn submicron aerosols in this region.In this study,a quadrupole aerosol chemical speciation monitor(Q-ACSM)was deployed for the real-time measurement of the non-refractory compositions of submicron aerosols(NR-PM1)at a regional site(Xianghe)from October 3 to November 14,2017.The results showed that nitrate was the largest inorganic aerosol,and the oxygenated organic aerosol(OOA)was the largest organic aerosol in Xianghe.Hydrocarbon-like OA(HOA)was the largest organic aerosol When the NR-PM1 mass concentrations increased from the lowest to the highest bins,nitrate and biomass burning OA(BBOA)showed increasing trends in the suburban area.Enhanced nitrate formation during the pollution epi-sodes resulted from both photochemical and aqueous processing.To reduce the particulate matter(PM2.5)concentrations and eliminate heavy pollution episodes,control measures should focus on reducing NO_(x),NH_(3),and volatile organic compound(VOCs)emissions.
基金supported in part by projects from the Natural Science Foundation of China(NSFC40925009,41230641)project from the "Strategic Priority Research Program" of the Chinese Academy of Sciences(Grant No.XDA05100401)the Meteorological Innovative Research Project of Baoji Meteorological Bureau (NO.T2012-01)
文摘Daily fine particulate (PM2.5) samples were collected in Chengdu from April 2009 to February 2010 to investigate their chemical profiles during dust storms (DSs) and several types of pollution events, including haze (HDs), biomass burning (BBs), and fireworks displays (FDs). The highest PM2.5 mass concentrations were found during DSs (283.3 μg/m^3), followed by FDs (212.7 μg/m^3), HDs (187.3 μg/m^3 ), and BBs (130.1 μ g/m^3). The concentrations of most elements were elevated during DSs and pollution events, except for BBs. Secondary inorganic ions (NO3^- , SO4^2-, and NH4^+) were enriched during HDs, while PM2.5 from BBs showed high K^+ but low SO4^2- , FDs caused increases in K^+ and enrichment in SO4^2-. Ca^2+. was abundant in DS samples, Ion-balance calculations indicated that PM2.5 from HDs and FDs was more acidic than on normal days, but DS and BB particles were alkaline. The highest organic carbon (OC) concentration was 26.1 μg/m^3 during FDs, followed by BBs (23.6 μg/m^3 ), HDs (19.6 μg/m^3 ), and DSs (18.8 μg/m^3 ). In contrast, elemental carbon (EC) concentration was more abundant during HDs (10.6μg/m^3) and FDs (9.5 μg/m^3) than during BBs (6.2μg/m^3) and DSs (6.0 μg/m^3). The highest OC/EC ratios were obtained during BBs, with the lowest during HDs. SO4^2+ /K^+ and TCA/SO4^2- ratios proved to be effective indicators for differentiating pollution events. Mass balance showed that organic matter, SO4^2-, and NO3^- were the dominant chemical components during pollution events, while soil dust was dominant during DSs.
基金supported by the National Natural Science Foundation of China(No.42022050)the Guangdong Basic and Applied Basic Research Fund Committee(No.2020B1515130003)+3 种基金the Guangdong Foundation for Program of Science and Technology Research(Nos.2019B121205006 and 2020B1212060053)the Guangdong Science and Technology Department(No.2017GC010501)the CAS Pioneer Hundred Talents program.We would like to thank Ryan Sullivan(Carnegie Mellon University,USA)the Nadine Borduas-Dedekind(University of British Columbia,Canada)for sharing their original data.
文摘Mineral dust is an important type of ice nucleating particles in the troposphere;however,the effects of heterogeneous reactions on ice nucleation(IN)activities of mineral dust remain to be elucidated.A droplet-freezing apparatus(Guangzhou Institute of Geochemistry Ice Nucleation Apparatus,GIGINA)was developed in thiswork to measure IN activities of atmospheric particles in the immersion freezingmode,and its performancewas validated by a series of experimental characterizations.This apparatus was then employed to measure IN activities of feldspar and Arizona Test Dust(ATD)particles before and after heterogeneous reaction with NO_(2)(10±0.5 ppmv)at 40%relative humidity.The surface coverage of nitrate,θ(NO_(3)^(−)),increased to 3.1±0.2 for feldspar after reaction with NO_(2) for 6 hr,and meanwhile the active site density per unit surface area(ns)at-20℃ was reduced from 92±5 to<1.0 cm^(−2) by about two orders of magnitude;however,no changes in nitrate content or IN activities were observed for further increase in reaction time(up to 24 hr).Both nitrate content and IN activities changed continuously with reaction time(up to 24 hr)for ATD particles;after reaction with NO_(2) for 24 hr,θ(NO_(3)^(−))increased to 1.4±0.1 and ns at-20℃ was reduced from 20±4 to 9.7±1.9 cm^(−2) by a factor of∼2.Our work suggests that heterogeneous reaction with NO_(2),an abundant reactive nitrogen species in the troposphere,may significantly reduce IN activities of mineral dust in the immersion freezing mode.
基金supported by the National Key R&D Program of China(No.2022YFF0802501)the Youth Innovation Promotion Association of the Chinese Academy of Sciences(No.2022416)+1 种基金the Natural Science Basic Research Program of Shaanxi(No.2022JQ-267)the State Key Laboratory of Loess and Quaternary Geology(No.SKLLQG2335).
文摘The Northeast Plain in China ranks among the top five regions that have been significantly impacted by haze pollution.To effectively control pollution,it is crucial to accurately assess the effects of emission reduction measures.In this study,we analyzed surveillance data and found substantial decreases(ranging from 19.0%to 50.1%)in average annual mass concentrations of key pollutants(such as CO,SO_(2),NO_(2),and PM_(2.5))in the Northeast Plain from 2016 to 2020.To precisely determine the contributions of meteorological conditions and emission reductions to the improvement of air quality in the Northeast Plain,we conducted three scenario simulations.By comparing source emissions in December 2016 and 2020 using the WRF-Chem model(except for SO_(2)),we observed significant reductions of 21.3%,8.8%,and 9.8%in mass concentrations of PM_(2.5),NO_(2),and CO,respectively,from 2016 to 2020.This highlights the essential role that meteorological conditions play in determining air quality in the Northeast Plain.Moreover,further reducing source emissions by 30%in December 2016 resulted in subsequent reductions of 25.3%,29.0%,4.5%,and 30.3%in mass concentrations of PM_(2.5),SO_(2),NO_(2),and CO,respectively,under the same meteorological conditions.Notably,source emission reduction was effective for PM_(2.5),SO_(2),and CO,but not for NO_(2).The improvement in air quality in the Northeast Plain from 2016 to 2020 can be attributed to the combined effects of improved meteorological conditions and reduced pollution sources.