科研成果 by Year: 2024

2024
Qiao, R. ; Chen, W. ; Shi, Y. ; Chai, Q. ; Fan, Y. ; Hua, Q. ; Li, A. ; Li, H. ; Li, J. ; Meng, X. ; et al. A Comparative Analysis on Indoor and Outdoor Pm2.5 and Their Hourly Associations with Acute Respiratory Inflammation Among College Students in Lhasa. Environmental Science & Technology 2024, 58, 22668–22677. 访问链接
Deng, H. ; Qiu, J. ; Zhang, R. ; Xu, J. ; Qu, Y. ; Wang, J. ; Liu, Y. J. ; Gligorovski, S. Ozone Chemistry on Greasy Glass Surfaces Affects the Levels of Volatile Organic Compounds in Indoor Environments. Environmental Science & Technology 2024, 58, 8393–8403. 访问链接Abstract
The chemistry of ozone (O3) on indoor surfaces leads to secondary pollution, aggravating the air quality in indoor environments. Here, we assess the heterogeneous chemistry of gaseous O3 with glass plates after being 1 month in two different kitchens where Chinese and Western styles of cooking were applied, respectively. The uptake coefficients of O3 on the authentic glass plates were measured in the dark and under UV light irradiation typical for indoor environments (320 nm < $łambda$ < 400 nm) at different relative humidities. The gas-phase product compounds formed upon reactions of O3 with the glass plates were evaluated in real time by a proton-transfer-reaction quadrupole-interface time-of-flight mass spectrometer. We observed typical aldehydes formed by the O3 reactions with the unsaturated fatty acid constituents of cooking oils. The formation of decanal, 6-methyl-5-hepten-2-one (6-MHO), and 4-oxopentanal (4-OPA) was also observed. The employed dynamic mass balance model shows that the estimated mixing ratios of hexanal, octanal, nonanal, decanal, undecanal, 6-MHO, and 4-OPA due to O3 chemistry with authentic grime-coated kitchen glass surfaces are higher in the kitchen where Chinese food was cooked compared to that where Western food was cooked. These results show that O3 chemistry on greasy glass surfaces leads to enhanced VOC levels in indoor environments.
Liu, W. ; He, L. ; Liu, Y. J. ; Liao, K. ; Chen, Q. ; Kuwata, M. Suppressed Atmospheric Chemical Aging of Cooking Organic Aerosol Particles in Wintertime Conditions. Atmospheric Chemistry and Physics 2024, 24, 5625–5636. 访问链接
Zhou, Y. ; He, L. ; Tan, J. ; Zhou, J. ; Liu, Y. Rapid Quantitative Analysis of Semi-Volatile Organic Compounds in Indoor Surface Film Using Direct Analysis in Real Time Mass Spectrometry: A Case Study on Phthalates. Atmospheric Measurement Techniques 2024, 17, 6415–6423. 访问链接
He, S. ; Liu, Y. ; Song, M. ; Li, X. ; Lou, S. ; Ye, C. ; Liu, Y. J. ; Liu, Y. ; Ye, J. ; Lu, S. ; et al. Empirical Approach to Quantifying Sensitivity in Different Chemical Ionization Techniques for Organonitrates and Nitroaromatics Constrained by Ion–Molecule Reaction and Transmission Efficiency. Analytical Chemistry 2024, 96, 16882–16890. 访问链接Abstract
Accurate identification and quantification of nitro-containing species are of great significance to understanding their chemical behaviors in the atmosphere. By optimizing the operational conditions of the H3O+ and NO+ ionization modes in a proton-transfer-reaction time-of-flight mass spectrometer (PTR-TOF-MS) and evaluating the performance of an iodide chemical ionization mass spectrometer (I– CIMS), this study leveraged the individual advantages of each ionization mode to effectively detect a diverse array of nitroaromatics and organonitrates (ONs). The H3O+ ionization mode largely fulfilled the criteria for real-time monitoring of gas-phase alkyl-, aryl-, and hydroxy-nitrates, and nitrophenols, albeit its reduced sensitivity toward ONs due to extensive fragmentation. In contrast, the NO+ mode demonstrated enhanced sensitivity for ONs with less fragmentation than the H3O+ mode. The I– CIMS featured distinguished sensitivity toward oxidized compounds containing polar functional groups, particularly increasing with the incorporation of hydroxyl, carboxyl, or nitrate groups. Further, we developed a calibration-based semiquantitative framework to enhance the accuracy of sensitivity estimation, constrained by ion–molecule reaction, transmission efficiency, along with possible decomposition of ion-clusters, with uncertainties ranging from 21% to 41% for H3O+ and 21–43% for NO+. Given considerable discrepancies (up to 1 order of magnitude) between measured and predicted sensitivity in I– CIMS using previously reported log–linear fitting, a declustering voltage (dV50)-based categorization approach was introduced, leading to a 5-fold improvement in measurement accuracy and an overall uncertainty of I– CIMS in quantifying nitro-containing species varying from 27% to 60%.
Zhu, T. ; Liu, Y. J. ; Xu, S. ; Dong, G. ; Huang, C. ; Sang, N. ; Zhang, Y. ; Su, G. ; Chen, J. ; Gong, J. ; et al. Advances and Perspectives in Environmental Health Research in China. Front. Environ. Sci. Eng. 2024, 18, 76.
Li, Y. ; Zhang, S. ; Guo, Z. ; Wang, L. ; Qiao, L. ; Chen, Y. ; Fan, G. ; Sun, C. ; Sun, Y. ; Liu, Y. J. ; et al. An In-Situ Versatile Screening Method for Identifying Svoc Sources in Indoor Environments. Environment International 2024, 189, 108794. 访问链接Abstract
Indoor semivolatile organic compounds (SVOCs) pose a substantial threat to human health. However, identifying the sources of these emissions has been challenging owing to the scarcity of convenient and practical on-site methodologies. Herein, a novel method for source screening was proposed using aluminum silicate sampling strips to adsorb SVOCs from the surface air of indoor materials. The adsorbed SVOC levels indicate the emission intensity of these materials into indoor environments. Additionally, compact sampling strips can be readily fixed to any vertical surface using a static sticker, facilitating the characterization of various materials in practical settings. Laboratory-simulated experiments demonstrated the capability of the proposed method to differentiate between source and non-source materials within a 10-cm distance in the same space. In practical scenarios, the primary emission sources identified via this method exhibited a consistent correlation with the contents of the corresponding materials obtained from the traditional solvent-extraction method. As the adsorbed SVOCs were directly transferred to a GC–MS through thermal desorption instead of the solvent-extraction procedure, the proposed method demonstrated several-fold improvements in analytical sensitivity and efficiency. Using this versatile screening technique, some emerging and important SVOC species were identified within specific indoor materials. Eliminating these sources has been demonstrated as an effective approach to mitigate SVOC pollution. Overall, the proposed method offers a powerful tool for managing indoor pollutants and safeguarding human health.
Meng, X. ; Hua, Q. ; Xu, R. ; Shi, Y. ; Zhang, Y. ; Yan, M. ; Chen, W. ; Xu, Y. ; Fan, Y. ; Yao, Y. ; et al. A Prospective Study on the Cardiorespiratory Effects of Air Pollution Among Residents of the Tibetan Plateau. Hygiene and Environmental Health Advances 2024, 12, 100115. 访问链接Abstract
The Tibetan Plateau is characterized by high ozone concentration which poses a significant public health concern. However, the causal evidence linking ozone pollution to adverse cardiopulmonary health impacts, as well as the understanding of its underlying biological mechanisms, remains limited. Additionally, exposure levels to particulate and other gaseous air pollutants along with their associated health effects in this region are largely unknown. To address these gaps, we conducted a prospective follow-up study in Tibet from May 2021 to November 2021. In consideration of the potential synergistic effects of chronic hypobaric hypoxia, two Tibetan cities with different altitudes, Lhasa (3650 m) and Nyingchi (3000 m), were chosen to implement atmospheric monitoring and health measurement. We employed cutting-edge, high-precision instruments at stationary monitoring sites to measure ambient air pollution and collected particle samples. Portable devices were used to monitor personal exposure levels of ozone and black carbon. A total of 212 healthy Tibetan college students participated in up to four clinical visits, yielding 774 visits in total, during which functional endpoints were measured and biological samples were collected. The primary aim of this study is to evaluate the cardiorespiratory effects of ambient ozone under hypoxic conditions, where its impact may be amplified due to the region's unique environmental characteristics. The secondary aim is to provide a comprehensive assessment of other air pollutants, including their exposure levels, sources, and health effects. By addressing these aims, the study offers valuable insights into air quality and its health implications in this unique high-altitude setting. This paper outlines the research motivation, measurement framework, and preliminary findings.
Zheng, M. ; Zhang, T. ; Xiang, Y. ; Tang, X. ; Wang, Y. ; Geng, G. ; Wang, Y. ; Liu, Y. J. ; Ye, C. ; Yan, C. ; et al. A Newly Established Air Pollution Data Center in China. Advances in Atmospheric Sciences 2024. 访问链接Abstract
Air pollution in China covers a large area with complex sources and formation mechanisms, making it a unique place to conduct air pollution and atmospheric chemistry research. The National Natural Science Foundation of China's Major Research Plan entitled “Fundamental Researches on the Formation and Response Mechanism of the Air Pollution Complex in China” (or the Plan) has funded 76 research projects to explore the causes of air pollution in China, and the key processes of air pollution in atmospheric physics and atmospheric chemistry. In order to summarize the abundant data from the Plan and exhibit the long-term impacts domestically and internationally, an integration project is responsible for collecting the various types of data generated by the 76 projects of the Plan. This project has classified and integrated these data, forming eight categories containing 258 datasets and 15 technical reports in total. The integration project has led to the successful establishment of the China Air Pollution Data Center (CAPDC) platform, providing storage, retrieval, and download services for the eight categories. This platform has distinct features including data visualization, related project information querying, and bilingual services in both English and Chinese, which allows for rapid searching and downloading of data and provides a solid foundation of data and support for future related research. Air pollution control in China, especially in the past decade, is undeniably a global exemplar, and this data center is the first in China to focus on research into the country's air pollution complex.
He, L. ; Liu, W. ; Li, Y. ; Wang, J. ; Kuwata, M. ; Liu, Y. J. Wall Loss of Semi-Volatile Organic Compounds in a Teflon Bag Chamber for the Temperature Range of 262–298 k: Mechanistic Insight on Temperature Dependence. Atmospheric Measurement Techniques 2024, 17, 755–764. 访问链接Abstract
Teflon bag chambers have long been used for investigating atmospheric chemical processes, including secondary organic aerosol formation. The wall-loss process of gas-phase species in Teflon bag chambers has typically been investigated at around room temperature. Recent laboratory studies started employing Teflon bag chambers at sub-273 K conditions for simulating wintertime and upper-tropospheric environments. However, temperature dependence in vapor-wall-loss processes of semi-volatile organic compounds (SVOCs) in a Teflon bag chamber has not been well investigated. In this study, we experimentally investigated wall-loss processes of C14–C19 n-alkanes in a 1 m3 Teflon bag for the temperature range of 262 to 298 K. Enhanced wall losses of the tested n-alkanes were observed following the decrease in temperature. For instance, 65 %​​​​​​​ of C14 n-alkane was lost to the wall 15 h after injection at room temperature, while the corresponding value was 95 % at 262 K. The experimental data were analyzed using a two-layer kinetic model, which considers both absorption of gas-phase species to the surface layer of the Teflon wall and diffusion to the inner layer. The experimental data demonstrated that absorption of gas-phase species by the surface layer was enhanced at lower temperatures. The temperature dependence in absorption was well accounted for using the equilibrium-dissolution model of organic compounds to the Teflon surface by considering reduced saturation vapor pressure at lower temperatures. On the contrary, diffusion of n-alkanes from the surface to the inner layer slowed down at reduced temperatures. Mechanistic studies on these processes will need to be conducted in the future to quantitatively predict the influence of temperature-dependent wall-loss processes of SVOCs on laboratory experimental results.
Qu, Y. ; D., X. ; Liu, Y. Emissions of Volatile Organic Compounds from Human Occupants in a Student Office: Dependence on Ozone Concentration. ACS Environmental Au 2024, 4, 3-11. 访问链接Abstract
Human occupants themselves constitute an important source of volatile organic compounds (VOCs) in indoor environments through breath and dermal emissions. In order to quantify VOC emissions from occupants under real-world settings, previous indoor observational studies often determined emission factors (i.e., average emission rates per person). However, the values obtained across these studies exhibited large variability, and the causes of this variability still need to be understood. Herein we report 10-day real-time VOC measurements in a university student office, using a proton transfer reaction-quadrupole interface-time-of-flight mass spectrometer. A method was developed to identify VOCs of primary human origin and to quantify the corresponding emission factors, accounting for the dynamically changing occupancy level and ventilation rate in the assessed office. We found that the emission factors of many dermally emitted VOCs strongly increased as the ozone concentration increased from <3 to 10–15 ppb. These VOCs include geranyl acetone, 6-methyl-5-hepten-2-one (6-MHO), and C10-C12 saturated aldehydes, which align with characteristic first-generation ozonolysis products of skin oil. The strongest increase occurred for 6-MHO, from 113 to 337 μg/h/p. In comparison, acetone and isoprene, which are primarily emitted from human breath, varied little with the ozone level. In light of this finding, we conducted an integrated analysis of emission factors reported in the literature for two frequently reported species, namely, 6-MHO and decanal. Ozone concentration alone can explain 94–97% of the variation in their emission factors across previous studies, and the best-estimated ozone dependence obtained using the literature data is consistent with those obtained in the current study. These results suggest that the ozone concentration is a key factor regulating emission factors of many dermally emitted VOCs in real indoor environments, which has to be considered when reporting or using the emission factors.