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Interaction between marine and terrestrial biogenic volatile organic compounds: Non-linear effect on secondary organic aerosol formation 海洋和陆地生物挥发性有机化合物之间的相互作用:对二次有机气溶胶形成的非线性影响
IF 4.2 2区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2024-10-11 DOI: 10.1016/j.atmosenv.2024.120868
Xiaowen Chen, Lin Du, Zhaomin Yang, Shan Zhang, Narcisse Tsona Tchinda, Jianlong Li, Kun Li
Biogenic volatile organic compounds (BVOCs) are the largest source of secondary organic aerosols (SOA) globally. However, the complex interactions between marine and terrestrial BVOCs remain unclear, inhibiting our in-depth understanding of the SOA formation in the coastal areas and its environmental impacts. Here, we performed smog chamber experiments with mixed α-pinene (a typical monoterpene) and dimethyl sulfide (DMS, a typical marine emission BVOC) to investigate their possible interactions and subsequent SOA formation. It is found that DMS has a non-linear effect on SOA generation: The mass concentration and yield of SOA show increasing and then decreasing trends with the increase of the initial concentration of DMS. The increasing trend can be attributed to OH regeneration from isomerization of the CH3SCH2OO radical together with acid-catalyzed heterogeneous reactions by the oxidation of DMS, while the decreasing trend is explained by the less contribution of isomerization reaction and the high OH reactivity that inhibits the formation of low volatility products. The results from infrared spectra and mass spectra together reveal the contribution of sulfur-containing molecules in the mixed system. Moreover, the mass spectra results indicate that acidic products generated by DMS photooxidation enhance the O:C ratio, while organosulfates are produced to contribute to the formation of mixed SOA. In addition, the trends in relative abundance of highly oxygenated organic molecules (HOMs) with C8 - C10 multiple functional groups in different mixed systems agree well with the turning point of the SOA yield. The findings of this study have significant implications for understanding binary or more complex systems in the atmosphere in the coastal areas.
生物挥发性有机化合物(BVOCs)是全球二次有机气溶胶(SOA)的最大来源。然而,海洋和陆地 BVOCs 之间复杂的相互作用仍不清楚,妨碍了我们深入了解沿海地区 SOA 的形成及其对环境的影响。在这里,我们用混合α-蒎烯(一种典型的单萜)和二甲基硫醚(DMS,一种典型的海洋排放 BVOC)进行了烟雾室实验,研究它们之间可能的相互作用以及随后 SOA 的形成。研究发现,DMS 对 SOA 的生成有非线性影响:随着 DMS 初始浓度的增加,SOA 的质量浓度和产量呈现先增加后减少的趋势。上升趋势可归因于 CH3SCH2OO 自由基的异构化以及 DMS 氧化作用下的酸催化异构反应产生的羟基再生,而下降趋势则可解释为异构化反应的贡献较小以及高羟基反应性抑制了低挥发性产物的形成。红外光谱和质谱结果共同揭示了混合体系中含硫分子的贡献。此外,质谱结果表明,二甲基亚砜光氧化反应产生的酸性产物提高了 O:C 比率,而有机硫酸盐的产生则促进了混合 SOA 的形成。此外,不同混合体系中具有 C8 - C10 多种官能团的高含氧有机分子(HOMs)的相对丰度趋势与 SOA 产量的转折点非常吻合。这项研究的结果对了解沿海地区大气中的二元或更复杂的系统具有重要意义。
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引用次数: 0
Analytical optical methods for measuring organic peroxides and hydroperoxides: An evaluation 测量有机过氧化物和氢过氧化物的分析光学方法:评估
IF 4.2 2区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2024-10-11 DOI: 10.1016/j.atmosenv.2024.120858
D. Alba-Elena , M.T. Baeza-Romero , X. Wang , J. Abbatt , Carolina Hernandez , Edelmira Valero
Hydrogen peroxide, organic peroxides and hydroperoxides exhibit high reactivity and play a pivotal role in atmospheric chemistry. These compounds are formed during the oxidation of volatile organic compounds in both gaseous and aqueous phases, particularly under low NOx conditions. Their significant contribution to the mass of secondary organic aerosols (SOA) is well-documented, and they are believed to have significant health implications. Several spectrophotometric methods have been employed to measure SOA-bound peroxides in laboratory samples, but systematic comparisons are lacking. In this study, we have assessed the advantages and limitations of these methods, including the traditional and microwave-assisted iodometric methods, the 4-nitrophenyl boronic acid assay (NPBA), and the Fenton reaction-assisted ferrous-xylenol (FOX2) assay. Besides, a comprehensive evaluation of these methodologies was conducted for the first time across a substantial cohort of commercial peroxides and hydroperoxides, employing diverse solvents (namely, water, 1-propanol, acetonitrile, methanol and chloroform) to provide broader insights compared to previous work. Ultimately, the four methods were applied and compared for peroxide determination in laboratory-generated SOA resulting from gas-phase ozonolysis of α-pinene. This study opens new opportunities for future mechanistic investigation into SOA formation and reactivity.
过氧化氢、有机过氧化物和氢过氧化物具有很高的反应活性,在大气化学中起着举足轻重的作用。这些化合物是在气相和水相挥发性有机化合物氧化过程中形成的,尤其是在低氮氧化物条件下。它们对二次有机气溶胶(SOA)质量的重大影响已得到充分证实,而且人们认为它们对健康有重大影响。已有多种分光光度法用于测量实验室样本中与 SOA 结合的过氧化物,但缺乏系统的比较。在本研究中,我们评估了这些方法的优点和局限性,包括传统碘量法和微波辅助碘量法、4-硝基苯硼酸测定法(NPBA)和芬顿反应辅助亚铁-二甲酚(FOX2)测定法。此外,还首次在大量商用过氧化物和氢过氧化物中对这些方法进行了全面评估,并采用了不同的溶剂(即水、1-丙醇、乙腈、甲醇和氯仿),以提供比以往工作更广泛的见解。最终,这四种方法被用于测定实验室产生的 SOA 中的α-蒎烯气相臭氧分解产生的过氧化物,并进行了比较。这项研究为今后从机理角度研究 SOA 的形成和反应性提供了新的机会。
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引用次数: 0
Impact of urbanized atmosphere-land processing to the near-ground distribution of air pollution over Central Liaoning Urban Agglomeration 城市化大气-土地处理对辽宁中部城市群大气污染近地面分布的影响
IF 4.2 2区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2024-10-10 DOI: 10.1016/j.atmosenv.2024.120866
Wenxi Zhang , Zhenxin Liu , Xiaolan Li , Yuhao Mao , Yanjun Ma , Hong Liao
Urban heat island effect and local atmospheric boundary layer circulation caused by urbanization are important factors affecting the transport and spatial and temporal distribution of atmospheric particulate matter in cities and surrounding areas. To analyze the local atmospheric circulation and its influence on the temporal and spatial characteristics of PM2.5 concentration over the Central Liaoning Urban Agglomeration, a heavy haze process was selected. The atmospheric chemistry model WRF-Chem was applied for numerical simulations with sensitivity experiments of urban canopy physical processes. The experiment case (EXP) was set up by coupling an improved urban canopy model with WRF-Chem, in which more details of inhomogeneous wind and diffusion in the complexed street canyon were fully and reasonably considered. Compared with the control case (CTR) by the original WRF-Chem, the deviation of the simulated and observed near-surface temperature and atmospheric boundary layer height was significantly improved in EXP: the error during the daytime was reduced from −1.30% and −48.39% in CTR to −0.78% and −33.68% in EXP, respectively, while during the nighttime it was reduced from −1.15% and −48.98% to 0.05% and −24.42%. The simulation accuracy of the near-surface PM2.5 concentration in EXP was also significantly higher: the deviation during the daytime was 18.24% in CTR and 3.28% in EXP, while it was reduced from 40.69% in CTR to 28.88% in EXP during the nighttime. Thus, the EXP improved significantly in meteorological simulation during the nighttime, and then particulate matter concentrations in EXP during the nighttime were obviously improved. This study shows that improving the wind profiles and diffusion mechanism in urban canopy schemes in the air quality model can effectively improve the simulation ability of the model on the transport and diffusion processes of atmospheric pollutants in cities and surrounding areas, thus improving the simulation ability of urban near-surface air pollution concentration.
城市化引起的城市热岛效应和局地大气边界层环流是影响城市及周边地区大气颗粒物传输和时空分布的重要因素。为分析辽宁中部城市群上空局地大气环流及其对 PM2.5 浓度时空特征的影响,选取了一次重度雾霾过程。应用大气化学模式 WRF-Chem 对城市冠层物理过程进行数值模拟和敏感性试验。通过将改进的城市冠层模型与 WRF-Chem 模型耦合,建立了实验案例(EXP),其中充分合理地考虑了复杂街道峡谷中不均匀风和扩散的更多细节。与原 WRF-Chem 的对照案例(CTR)相比,EXP 中模拟的近地面温度和大气边界层高度与观测值的偏差有了显著改善:白天的误差分别从 CTR 的-1.30%和-48.39%减小到 EXP 的-0.78%和-33.68%,夜间的误差从-1.15%和-48.98%减小到 0.05%和-24.42%。EXP 对近地表 PM2.5 浓度的模拟精度也显著提高:白天的偏差在 CTR 中为 18.24%,在 EXP 中为 3.28%,而夜间则从 CTR 中的 40.69%降至 EXP 中的 28.88%。因此,在夜间气象模拟中,EXP 得到了明显改善,从而使夜间 EXP 中的颗粒物浓度得到明显改善。本研究表明,改进空气质量模型中城市冠层方案的风廓线和扩散机理,可有效提高模型对城市及周边地区大气污染物传输和扩散过程的模拟能力,从而提高城市近地面大气污染浓度的模拟能力。
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引用次数: 0
Impact of biomass burning on air quality: A case study of the agricultural region in South Korea 生物质燃烧对空气质量的影响:韩国农业地区案例研究
IF 4.2 2区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2024-10-09 DOI: 10.1016/j.atmosenv.2024.120864
Jihee Ban , Taehyun Park , Seokwon Kang , Siyoung Choi , Gracie Wong , Jinsoo Choi , Beom-Keun Seo , Saewung Kim , Joonyoung Ahn , Yongjae Lim , Minyoung Sung , Soyoung Jung , Jiyun Jung , Hyunjae Kim , Seung-Myung Park , Jaeyun Lee , Jongho Kim , Jeongho Kim , Soo Bog Park , Jinsoo Park , Taehyoung Lee
Various combustion processes occur concurrently during biomass burning events, emitting a complex mixture of particulate and gaseous pollutants into the atmosphere. These emissions undergo chemical transformations facilitated by factors such as solar radiation and cloud formation, thereby altering the composition of aerosols. Additionally, these pollutants can affect the region of origin and neighboring countries, presenting regional and global environmental challenges. Therefore, precise evaluation of the particulate and gaseous pollutants emitted during biomass burning is essential to formulate effective management strategies. This study aimed to assess the concentration and chemical characteristics of particulate matter emitted during biomass burning in South Korea. On June 7, 2021, a research flight was conducted utilizing a High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and a Single Particle Soot Photometer (SP2) for airborne measurements over South Korea inland areas. For data analysis based on administrative regions, the flight path was divided into four major areas (Areas A, B, C, and D). During the research flight, evidence of biomass burning events was observed primarily in Area C. A positive matrix factorization (PMF) analysis categorized the organic aerosols (OA) into five factors: biomass burning OA (BBOA), hydrocarbon-like OA (HOA1, HOA2), low-oxidized oxygenated OA (LO-OOA), and more-oxidized OOA (MO-OOA). Across all areas, MO-OOA accounted for the highest proportion of aerosols, whereas BBOA dominated in Area C at 23.8%, indicating the significant influence of biomass burning in this region. Instead of running a PMF analysis with all measurement data, a BBOA formula was derived from the previous study and this one. This allows us to estimate BBOA concentration without running PMF.
在生物质燃烧过程中,各种燃烧过程同时进行,向大气中排放颗粒和气体污染物的复杂混合物。这些排放物会在太阳辐射和云层形成等因素的作用下发生化学变化,从而改变气溶胶的成分。此外,这些污染物还会影响来源地区和周边国家,给地区和全球环境带来挑战。因此,精确评估生物质燃烧过程中排放的颗粒和气体污染物对于制定有效的管理策略至关重要。本研究旨在评估韩国生物质燃烧过程中排放的颗粒物的浓度和化学特征。2021 年 6 月 7 日,利用高分辨率飞行时间气溶胶质谱仪(HR-ToF-AMS)和单颗粒烟尘光度计(SP2)对韩国内陆地区进行了空中测量。为了根据行政区域进行数据分析,飞行路径被划分为四个主要区域(A、B、C 和 D 区)。研究飞行期间,主要在 C 区观测到生物质燃烧事件的证据。正矩阵因式分解(PMF)分析将有机气溶胶(OA)分为五个因子:生物质燃烧 OA(BBOA)、类碳氢化合物 OA(HOA1、HOA2)、低氧含氧 OA(LO-OOA)和高氧 OOA(MO-OOA)。在所有区域中,MO-OOA 占气溶胶的比例最高,而 BBOA 在 C 区域占 23.8%,表明生物质燃烧对该区域的影响很大。我们没有使用所有测量数据进行 PMF 分析,而是根据之前的研究和本次研究得出了一个 BBOA 公式。这样,我们就可以在不运行 PMF 的情况下估算出 BBOA 的浓度。
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引用次数: 0
Gas-liquid interfacial reaction mechanisms of typical small α-dicarbonyls in the neutral and acidic droplets: Implications for secondary organic aerosol formation 中性和酸性液滴中典型小 α-二羰基的气液界面反应机制:对二次有机气溶胶形成的影响
IF 4.2 2区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2024-10-09 DOI: 10.1016/j.atmosenv.2024.120859
Qiuju Shi , Ruize Ma , Yongpeng Ji , Weina Zhang , Yuemeng Ji , Taicheng An
Small α-dicarbonyls (SαDs) are well-known as the important precursors of secondary organic aerosol (SOA). Hence, it is imperative to understand the atmospheric chemistry of SαDs to contribute to SOA formation. In this work, we investigated the interfacial chemistry of typical SαDs, including methylglyoxal (MG) and biacetyl (BA) in the neutral and acidic droplets by combined molecular dynamics and quantum chemical calculations. The trans configurations of MG and BA are found to be the favorable configurations at the interfaces and are prone to stay at the gas-liquid interface of the acidic droplet. The C=O group exhibits a preferential uptake orientation towards the interface because the carbonyl-O atom has a strong interaction with interfacial H2O. The uptakes and accumulations of MG and BA at the interfaces are promoted by the acidic condition. Subsequent interfacial hydrations of MG and BA in the acidic droplet are beneficial to yield diols, which can engage in oligomerization in the droplet interior to contribute SOA formation. Our results provide the theoretical insight into the interfacial chemistry of SαDs and their role in SOA formation.
众所周知,小的α-二羰基(SαDs)是二次有机气溶胶(SOA)的重要前体。因此,了解 SαDs 在大气中的化学性质对 SOA 的形成有重要意义。在这项研究中,我们结合分子动力学和量子化学计算,研究了典型 SαDs 的界面化学性质,包括中性和酸性液滴中的甲基乙二醛(MG)和生物乙酰(BA)。研究发现,MG 和 BA 的反式构型是界面上的有利构型,容易停留在酸性液滴的气液界面上。由于羰基-O 原子与界面上的 H2O 有很强的相互作用,因此 C=O 基团表现出倾向于向界面吸收的取向。酸性条件促进了 MG 和 BA 在界面上的吸收和积累。随后,MG 和 BA 在酸性液滴中的界面水合作用有利于生成二元醇,二元醇可在液滴内部发生低聚作用,促进 SOA 的形成。我们的研究结果为 SαDs 的界面化学及其在 SOA 形成过程中的作用提供了理论依据。
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引用次数: 0
Enhanced mass scattering efficiencies of background dust aerosols over East Asia following the passage of dust plumes 尘羽通过后东亚上空背景尘埃气溶胶的质量散射效率增强
IF 4.2 2区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2024-10-09 DOI: 10.1016/j.atmosenv.2024.120862
Chenguang Tang , Yingjing Lin , Pengfei Tian , Jinsen Shi , Tao Deng , Xuejiao Deng , Yu Zou , Lei Zhang
The transported dust particles significantly impact global weather and climate. Previous studies focused primarily on the physical and chemical properties of dust plumes, but the interaction mechanism between these dust plumes and background dust aerosols remains unclear. We explored this issue using in-situ observation data of the East Asia dust from the Semi-Arid Climate and Environment Observatory of Lanzhou University (SACOL) during January 2013. We identified a dust plume originating from the Gurbantunggut Desert, which triggered a four-day dust event with an average dust concentration of 67.2 μg m−3. Notably, this dust event led to a significant increase in mass scattering efficiencies of dust, shifting from an inverted U-shape to a continuously increasing pattern with wavelength. The enhanced dust mass scattering efficiency inhibited the development of the planetary boundary layer. These changes persisted for at least two weeks after the event, primarily due to the resuspension of deposited dust particles altering the size of background dust particle. Our findings highlight the ability of dust plumes to enhance the scattering efficiency of background dust aerosols and providing new insights into the complex interactions between dust and the atmosphere.
飘移的尘埃粒子对全球天气和气候有重大影响。以往的研究主要关注沙尘卷的物理和化学性质,但这些沙尘卷与背景尘埃气溶胶之间的相互作用机制仍不清楚。我们利用兰州大学半干旱气候与环境观测站(SACOL)2013年1月对东亚沙尘的原位观测数据探讨了这一问题。我们确定了一股源自古尔班通古特沙漠的沙尘羽流,它引发了为期四天的沙尘事件,平均沙尘浓度为 67.2 μg m-3。值得注意的是,这次沙尘事件导致沙尘的质量散射效率显著增加,从倒 U 型转变为随波长持续增加的模式。尘埃质量散射效率的提高抑制了行星边界层的发展。这些变化在事件发生后至少持续了两周,主要是由于沉积尘粒的再悬浮改变了背景尘粒的大小。我们的研究结果凸显了尘羽提高背景尘埃气溶胶散射效率的能力,并为了解尘埃与大气之间复杂的相互作用提供了新的视角。
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引用次数: 0
Estimation of nighttime PM2.5 concentrations over Seoul using Suomi NPP/VIIRS Day/Night Band 利用 Suomi NPP/VIIRS 日/夜波段估算首尔上空的夜间 PM2.5 浓度
IF 4.2 2区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2024-10-09 DOI: 10.1016/j.atmosenv.2024.120861
Gyo-Hwang Choo, Kyunghwa Lee, Goo Kim
With rapid economic development and urban growth, Seoul experiences severe air pollution due to fine particulate matter with an aerodynamic diameter of ≤2.5 μm (PM2.5), which is detrimental to human health. Although recent studies have extensively focused on estimating daytime PM2.5 concentrations using various types of satellite data, there remains a significant lack of research on nighttime PM2.5 estimations. This study estimated nighttime PM2.5 in Seoul from December 2018 to November 2019 using multiple linear regression (MLR) and random forest (RF) models. These models, which incorporated data on radiance, moon illumination fraction, and terrain height from the Visible Infrared Imaging Radiometer Suite (VIIRS) Day/Night Band (DNB) on board the Suomi National Polar-orbiting Partnership satellite covering all moon phases, also utilized meteorological data from the ERA5 reanalysis by the European Centre for Medium-Range Weather Forecasts (ECMWF). To address multicollinearity, seasonal models were developed using forward stepwise regression and variance inflation factor analysis. DNB radiance analysis indicates that the high intensity of artificial light sources in Seoul significantly reduces the impact of moonlight, leading to notable changes in the DNB radiation associated with PM2.5 concentrations. Consequently, this study estimated nighttime PM2.5 over Seoul across all moon phases. These estimates were then validated through 10-fold cross-validation. The RF model exhibited superior accuracy, with a coefficient of determination (R2) of 0.65–0.90, compared to MLR, with R2 of 0.15–0.50, reflecting seasonal fluctuations in the model performance. The developed models can be applied to estimate reliable nighttime PM2.5 concentrations in megacities with strong artificial light sources, utilizing a comprehensive dataset from satellite observations for all moon phases. Additionally, our findings can serve as scientific data for establishing environmental policies by providing valuable insights into understanding air pollution primarily caused by PM2.5.
随着经济的快速发展和城市的不断扩大,空气动力学直径≤2.5 μm 的细颗粒物(PM2.5)造成首尔空气污染严重,对人体健康造成危害。尽管最近的研究广泛关注利用各种类型的卫星数据估算白天的 PM2.5 浓度,但仍然严重缺乏对夜间 PM2.5 估算的研究。本研究使用多元线性回归(MLR)和随机森林(RF)模型估算了首尔 2018 年 12 月至 2019 年 11 月的夜间 PM2.5。这些模型纳入了来自Suomi国家极轨伙伴关系卫星上覆盖所有月相的可见红外成像辐射计套件(VIIRS)日/夜波段(DNB)的辐照度、月球照度分数和地形高度数据,还利用了来自欧洲中期天气预报中心(ECMWF)ERA5再分析的气象数据。为解决多重共线性问题,使用前向逐步回归和方差膨胀因子分析建立了季节模型。DNB 辐射分析表明,首尔高强度的人工光源大大降低了月光的影响,导致与 PM2.5 浓度相关的 DNB 辐射发生显著变化。因此,本研究估算了首尔所有月相的夜间 PM2.5。然后通过 10 倍交叉验证对这些估计值进行了验证。与 R2 为 0.15-0.50 的 MLR 相比,RF 模型表现出更高的准确性,其判定系数 (R2) 为 0.65-0.90,反映了模型性能的季节性波动。所开发的模型可用于估算人工光源较强的特大城市的可靠夜间 PM2.5 浓度,利用的是卫星观测到的所有月相的综合数据集。此外,我们的研究结果可作为制定环境政策的科学数据,为了解主要由 PM2.5 造成的空气污染提供宝贵的见解。
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引用次数: 0
Two different approaches for source apportionment of ambient black carbon in highly polluted environments 高污染环境中环境黑碳来源分配的两种不同方法
IF 4.2 2区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2024-10-09 DOI: 10.1016/j.atmosenv.2024.120863
Ajit Kumar , Vikas Goel , Mohd Faisal , Umer Ali , Rakesh Maity , Dilip Ganguly , Vikram Singh , Mayank Kumar
The aethalometer model (AM) is widely used for source apportionment (SA) of black carbon (BC) in regions with mixed BC sources despite being initially developed for a relatively simplistic and low-pollution environments. The present study interrogates the applicability of AM in highly polluted metropolitan environments by comparing its results with the more nuanced Positive Matrix Factorization (PMF) model. The measurements were conducted in Delhi during the winter and summer season. PMF apportions the BC into diverse sources by taking help from complementary trace elemental measurements, thereby acknowledging the complex pollution landscape of the Delhi region. The AM estimates BCbb (BC from biomass burning) and BCff (BC from fossil fuel combustion) contributions as 48.3% and 51.7% during the winter and 16.6% and 83.4% during the summer, respectively.
In contrast, the PMF model-derived biomass burning factor is the dominant source of BC during both winter and summer seasons, contributing 53.9% and 44% of the total BC, respectively. The decrease in light absorption at UV wavelengths of biomass-burning aerosols owing to escalated ambient aging is posited to be the reason for BCbb underprediction by the AM model during summers. Furthermore, while the AM model identifies fossil fuel combustion as the only other BC source apart from biomass burning, the PMF model apportions BC to five additional sources during winter, including vehicle emissions (22.9%), Pb-rich factor (10%), power plant (5.7%), waste incineration (4%) and industrial emission (3.6%). The contribution of these BC sources during summer is vehicular emission (16.5%), power plant (14.5%), waste incineration (11.5%), Pb-rich factor (9.5%), and industrial emission (4%). Additionally, the spectral variation of the light absorption properties of black carbon (bBCabs) and brown carbon (bBrCabs), delta-C effect, and sensitivity of the AM are reported for the study period. The present study cautions that BC source apportionment can be complex in highly polluted metropolitan environments, and complementary tracer measurements are recommended for reliable results.
尽管乙硫计模型(AM)最初是针对相对简单和低污染的环境而开发的,但它被广泛用于混合碳源地区的黑碳(BC)源分配(SA)。本研究通过将 AM 的结果与更精细的正矩阵因式分解(PMF)模型进行比较,对 AM 在高污染大都市环境中的适用性进行了探讨。测量是在德里的冬季和夏季进行的。正矩阵因式分解模型通过补充痕量元素测量结果,将 BC 分解为不同的来源,从而反映了德里地区复杂的污染状况。根据 AM 估计,BCbb(生物质燃烧产生的 BC)和 BCff(化石燃料燃烧产生的 BC)在冬季分别占 48.3% 和 51.7%,在夏季分别占 16.6% 和 83.4%。由于环境老化加剧,生物质燃烧气溶胶对紫外线波长的光吸收减少,这被认为是夏季 AM 模式对 BCbb 预测不足的原因。此外,调幅模式认为化石燃料燃烧是除生物质燃烧之外唯一的其他 BC 来源,而 PMF 模式则将冬季的 BC 分配给另外五个来源,包括汽车尾气排放(22.9%)、富铅因子(10%)、发电厂(5.7%)、垃圾焚烧(4%)和工业排放(3.6%)。这些 BC 源在夏季的贡献是车辆排放(16.5%)、发电厂(14.5%)、垃圾焚烧(11.5%)、富铅因子(9.5%)和工业排放(4%)。此外,还报告了研究期间黑碳(bBCabs)和褐碳(bBrCabs)光吸收特性的光谱变化、delta-C 效应以及 AM 的灵敏度。本研究提醒说,在高度污染的大都市环境中,BC 源分配可能很复杂,建议进行补充示踪测量以获得可靠的结果。
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引用次数: 0
Estimation of carbon emissions in various clustered regions of China based on OCO-2 satellite XCO2 data and random forest modelling 基于 OCO-2 卫星 XCO2 数据和随机森林模型的中国各集群地区碳排放估算
IF 4.2 2区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2024-10-08 DOI: 10.1016/j.atmosenv.2024.120860
Yibing Tan , Shanshan Wang , Ruibin Xue , Sanbao Zhang , Tianyu Wang , Jiaqi Liu , Bin Zhou
Atmospheric carbon dioxide (CO2) stands as one of the most important greenhouse gasses, with steadily increasing concentrations attributable to human activities. In the pursuit of reaching peak carbon and carbon neutrality goals, it is essential to quantify carbon emissions and evaluate carbon reduction strategies. To establish a high-precision observation with full time series and spatial coverage, a spatio-temporal interpolation method was developed to obtain XCO2 data over mainland China at a resolution of 0.5° × 0.5° for the years 2015–2021. An east-west gradient, higher levels in the east and lower levels in the west, was observed, exhibiting a seasonal pattern of elevation in spring and reduction in summer. Subsequently, the research area is classified into seven clusters based on time-series XCO2 anomalies (ΔXCO2) and ODIAC (Open Source Data Inventory of Anthropogenic Carbon Dioxide) carbon emission data. This classification aims to emphasize the differentiation of spatial heterogeneity in carbon emissions and the results highlight that regions with high ΔXCO2 reflect higher carbon emission. Finally, the carbon emissions of each cluster were estimated by using a random forest model individually yielding an R2 of approximately 0.6. For assessing the variables influencing carbon emission predictions, the importance of each variable was calculated. Specifically, NightTime Lighting data (NTL), representing human production activities, emerged as a crucial variable influencing carbon emission predictions in most clusters. In comparison, Gross Primary Productivity (GPP) is considered a more critical variable in Southwest China (SWC), primarily owing to the intricate vegetation carbon sink system in this region. Temperature (T) emerges as a key variable influencing the estimation of carbon emissions in certain developed cities in Eastern China (EC), driven by the urban heat island effect which amplifies energy consumption, modifies land use, and impacts urban systems, influencing the spatial patterns of carbon emissions. Carbon emissions in different characteristic regions was quantified by establishing machine learning models with remote sensing data, which can provide new insights and support for refined carbon monitoring and management strategy.
大气中的二氧化碳(CO2)是最重要的温室气体之一,其浓度因人类活动而稳步上升。为了实现碳峰值和碳中和目标,量化碳排放和评估碳减排战略至关重要。为了建立具有全时间序列和空间覆盖的高精度观测,我们开发了一种时空插值方法,以 0.5° × 0.5° 的分辨率获得了 2015-2021 年中国大陆的 XCO2 数据。结果表明,中国大陆的 XCO2 呈东西梯度变化,东部水平较高,西部水平较低,并呈现出春季升高、夏季降低的季节性规律。随后,根据时间序列 XCO2 异常值(ΔXCO2)和 ODIAC(人为二氧化碳开放源数据清单)碳排放数据,将研究区域划分为七个组群。这种分类旨在强调碳排放的空间异质性差异,其结果突出表明,ΔXCO2 高的地区反映了较高的碳排放量。最后,利用随机森林模型估算了每个集群的碳排放量,R2 约为 0.6。为评估影响碳排放预测的变量,计算了每个变量的重要性。具体而言,代表人类生产活动的夜间照明数据(NTL)成为影响大多数集群碳排放预测的关键变量。相比之下,初级生产力总值(GPP)在中国西南部(SWC)被认为是一个更关键的变量,这主要是由于该地区错综复杂的植被碳汇系统。温度(T)是影响华东(EC)某些发达城市碳排放量估算的关键变量,其驱动力是城市热岛效应,该效应放大了能源消耗,改变了土地利用,影响了城市系统,从而影响了碳排放的空间模式。通过利用遥感数据建立机器学习模型,对不同特征区域的碳排放量进行量化,可为精细化碳监测和管理策略提供新的见解和支持。
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引用次数: 0
Assessment of VOCs emission inventory in Seoul through spatiotemporal observations using passive and online PAMS measurements 利用被动和在线 PAMS 测量,通过时空观测评估首尔的挥发性有机化合物排放清单
IF 4.2 2区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2024-10-08 DOI: 10.1016/j.atmosenv.2024.120857
Jimin Lee , Meehye Lee , Limseok Chang , Sun-A Shin , Kwangrae Kim , Yongsuk Choi , Hakmyeong Lim , Sung-Deuk Choi , Gangwoong Lee
We have conducted a quantitative analysis of volatile organic compounds (VOCs) in Seoul from September 2022 to June 2023, employing passive air samplers (PAS) at 25 sites and continuous monitoring at five photochemical assessment monitoring stations (PAMS). Comparing VOCs concentrations and compositions from PAS and PAMS during the same time periods, we found that most VOCs showed no significant difference (p-value >0.05) between the methods, except for olefins, which were overestimated by 24 % in passive sampling, confirming PAS as an effective tool for assessing the spatial distribution of VOCs species over large areas. Throughout Seoul, median values of total volatile organic compounds (TVOCs) concentrations collected with passive samplers remained stable with a standard deviation of 1.22 ppbv, typically ranging from 11 to 13 ppbv, except for an increase during winter in the southwestern regions of the city, where intense industrial and vehicular emissions are reported in the current Clean Air Policy Support System (CAPSS) emissions inventory. Positive matrix factorization (PMF) analysis using the passive data revealed general consistency in the spatial distribution of area and road emissions when compared with CAPSS emission inventory, although localized discrepancies were observed. In quantitative assessments of TVOCs comparing PAS observations with emission-based models, modeled values were within 1.5 times the interquartile range of observed PAS concentrations over Seoul. However, the lack of detection of emission hotspots in southeastern Seoul in the PAS data, coupled with the omission of photochemical loss in our dispersion-only models, indicates that the current CAPSS emission inventory may significantly underestimate actual ambient VOCs levels, especially in summer.
从 2022 年 9 月到 2023 年 6 月,我们在 25 个地点使用被动式空气采样器(PAS),并在 5 个光化学评估监测站(PAMS)进行连续监测,对首尔的挥发性有机化合物(VOCs)进行了定量分析。通过比较被动式空气采样器和光化学评估监测站在相同时间段内的挥发性有机化合物浓度和成分,我们发现除了烯烃在被动式采样中被高估了 24% 之外,大多数挥发性有机化合物在两种方法之间没有显著差异(p 值为 0.05),这证明被动式空气采样器是评估大面积挥发性有机化合物空间分布的有效工具。在整个首尔,使用被动采样器收集的总挥发性有机化合物 (TVOC) 浓度的中值保持稳定,标准偏差为 1.22 ppbv,通常在 11 至 13 ppbv 之间,但在冬季,该市西南部地区的浓度会有所上升,因为在当前的清洁空气政策支持系统 (CAPSS) 排放清单中,该地区的工业和车辆排放十分密集。利用被动数据进行的正矩阵因式分解(PMF)分析表明,与 CAPSS 排放清单相比,区域和道路排放的空间分布基本一致,但也发现了局部差异。在对 TVOCs 进行定量评估时,将 PAS 观测数据与基于排放的模型进行比较,发现模型值是首尔地区 PAS 观测浓度四分位数中间值范围的 1.5 倍。然而,PAS 数据没有检测到首尔东南部的排放热点,加上我们的纯扩散模型忽略了光化学损失,这表明当前的 CAPSS 排放清单可能大大低估了实际的环境 VOCs 水平,尤其是在夏季。
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Atmospheric Environment
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