ACS Central SciencePub Date : 2024-10-23DOI: 10.1021/acs.est.4c0681810.1021/acs.est.4c06818
Fabio E. Furcas, Shishir Mundra, Barbara Lothenbach and Ueli M. Angst*,
{"title":"Speciation Controls the Kinetics of Iron Hydroxide Precipitation and Transformation at Alkaline pH","authors":"Fabio E. Furcas, Shishir Mundra, Barbara Lothenbach and Ueli M. Angst*, ","doi":"10.1021/acs.est.4c0681810.1021/acs.est.4c06818","DOIUrl":"https://doi.org/10.1021/acs.est.4c06818https://doi.org/10.1021/acs.est.4c06818","url":null,"abstract":"<p >The formation of energetically favorable and metastable mineral phases within the Fe–H<sub>2</sub>O system controls the long-term mobility of iron complexes in natural aquifers and other environmentally and industrially relevant systems. The fundamental mechanism controlling the formation of these phases has remained enigmatic. We develop a general partial equilibrium model, leveraging recent synchrotron-based data on the time evolution of solid Fe(III) hydroxides along with aqueous complexes. We combine thermodynamic considerations and particle-morphology-dependent kinetic rate equations under full consideration of the aqueous phase in disequilibrium with one or more of the forming minerals. The new model predicts the rate of amorphous 2-line ferrihydrite precipitation, dissolution, and overall transformation to crystalline goethite. It is found that the precipitation of goethite (i) occurs from solution and (ii) is limited by the comparatively slow dissolution of the first forming amorphous phase 2-line ferrihydrite. A generalized transformation mechanism further illustrates that differences in the kinetics of Fe(III) precipitation are controlled by the coordination environment of the predominant Fe(III) hydrolysis product. The framework allows modeling of other iron(bearing) phases across a broad range of aqueous phase compositions.</p><p >The transformation of 2-line ferrihydrite is rate-limited by its dissolution as aqueous Fe(III) across a broad range of natural and industrially relevant aqueous systems.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 44","pages":"19851–19860 19851–19860"},"PeriodicalIF":10.8,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.est.4c06818","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142577679","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Central SciencePub Date : 2024-10-23DOI: 10.1021/acs.est.4c0431210.1021/acs.est.4c04312
Paul R. Tumminello, Renee Niles, Vanessa Valdez, Chamika K. Madawala, Dilini K. Gamage, Ke’La A. Kimble, Raymond J. Leibensperger III, Chunxu Huang, Chathuri Kaluarachchi, Julie Dinasquet, Francesca Malfatti, Christopher Lee, Grant B. Deane, M. Dale Stokes, Elizabeth Stone, Alexei Tivanski, Kimberly A. Prather, Brandon E. Boor and Jonathan H. Slade*,
{"title":"Size-Dependent Nascent Sea Spray Aerosol Bounce Fractions and Estimated Viscosity: The Role of Divalent Cation Enrichment, Surface Tension, and the Kelvin Effect","authors":"Paul R. Tumminello, Renee Niles, Vanessa Valdez, Chamika K. Madawala, Dilini K. Gamage, Ke’La A. Kimble, Raymond J. Leibensperger III, Chunxu Huang, Chathuri Kaluarachchi, Julie Dinasquet, Francesca Malfatti, Christopher Lee, Grant B. Deane, M. Dale Stokes, Elizabeth Stone, Alexei Tivanski, Kimberly A. Prather, Brandon E. Boor and Jonathan H. Slade*, ","doi":"10.1021/acs.est.4c0431210.1021/acs.est.4c04312","DOIUrl":"https://doi.org/10.1021/acs.est.4c04312https://doi.org/10.1021/acs.est.4c04312","url":null,"abstract":"<p >Viscosity, or the “thickness,” of aerosols plays a key role in atmospheric processes like ice formation, water absorption, and heterogeneous kinetics. However, the viscosity of sea spray aerosols (SSA) has not been widely studied. This research explored the relationship between particle size and viscosity of authentic SSA particles through particle bounce, atomic force microscopy analysis, and predictive viscosity modeling from molecular composition. The study found that 40 nm SSA particles had estimated viscosities around 10<sup>4</sup> Pa·s and bounce fractions three times higher than 100 and 200 nm particles with less than 10<sup>2</sup> Pa·s at a relative humidity (RH) of 60%. Additional studies revealed the Kelvin effect and particle density, influenced by particle size, have a greater impact on size-dependent bounce fractions than changes in RH across impactor stages. While changes in the level of surfactants can impact particle bounce, the increased viscosity in smaller SSA is attributed to the formation of gel-like phase states caused by cation–organic cross-links between divalent calcium ions and organic anions enriched in the smaller particles. This work shows the smallest gel-like SSA particles observed in the field are highly viscous, which has implications for cloud formation, secondary aerosol growth, and pollutant transport in coastal environments.</p><p >This study shows that smaller sea spray aerosols are more viscous and denser than larger ones. This has important implications for cloud formation and air pollution.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 44","pages":"19666–19678 19666–19678"},"PeriodicalIF":10.8,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.est.4c04312","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142577469","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Central SciencePub Date : 2024-10-23DOI: 10.1021/acs.est.4c0667610.1021/acs.est.4c06676
Shurun Yang, Si Sun, Zhihui Xie, Yudan Dong, Peng Zhou, Jing Zhang, Zhaokun Xiong, Chuan-Shu He*, Yang Mu and Bo Lai*,
{"title":"Comprehensive Insight into the Common Organic Radicals in Advanced Oxidation Processes for Water Decontamination","authors":"Shurun Yang, Si Sun, Zhihui Xie, Yudan Dong, Peng Zhou, Jing Zhang, Zhaokun Xiong, Chuan-Shu He*, Yang Mu and Bo Lai*, ","doi":"10.1021/acs.est.4c0667610.1021/acs.est.4c06676","DOIUrl":"https://doi.org/10.1021/acs.est.4c06676https://doi.org/10.1021/acs.est.4c06676","url":null,"abstract":"<p >Radical-based advanced oxidation processes (AOPs) are among the most effective technologies employed to destroy organic pollutants. Compared to common inorganic radicals, such as <sup>•</sup>OH, O<sub>2</sub><sup>•–</sup>, and SO<sub>4</sub><sup>•–</sup>, organic radicals are widespread, and more selective, but are easily overlooked. Furthermore, a systematic understanding of the generation and contributions of organic radicals remains lacking. In this review, we systematically summarize the properties, possible generation pathways, detection methods, and contributions of organic radicals in AOPs. Notably, exploring organic radicals in AOPs is challenging due to (1) limited detection methods for generated organic radicals; (2) controversial organic radical-mediated reaction mechanisms; and (3) rapid transformation of organic radicals as reaction intermediates. In addition to their characteristics and reactivity, we examine potential scenarios of organic radical generation in AOPs, including during the peroxide activation process, in water matrices or with coexisting organic pollutants, and due to the addition of quenching agents. Subsequently, we summarize various methods for organic radical detection as reported previously, such as electron paramagnetic resonance spectroscopy (EPR), <sup>31</sup>P nuclear magnetic resonance spectroscopy (<sup>31</sup>P NMR), liquid/gas chromatography–mass spectroscopy (GC/LC–MS), and fluorescence probes. Finally, we review the contributions of organic radicals to decontamination processes and provide recommendations for future research.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 44","pages":"19571–19583 19571–19583"},"PeriodicalIF":10.8,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142577770","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Central SciencePub Date : 2024-10-23DOI: 10.1021/acs.est.4c0566310.1021/acs.est.4c05663
Mingjiao Tian, Han Xu, Yaruo Zhao, Zeyu Jiang, Jialei Wan, Yanfei Jian, Shouning Chai, Lu Li, Mudi Ma, Yukun Sun, Shan Ren, Xinzhe Li, Chunli Zheng, Reem Albilali and Chi He*,
{"title":"Boosted 1,2-Dichloroethane Deep Destruction over CoRu/Al2O3 Bifunctional Catalysts via Surface Oxygen and Water Molecule Synergistic Activation","authors":"Mingjiao Tian, Han Xu, Yaruo Zhao, Zeyu Jiang, Jialei Wan, Yanfei Jian, Shouning Chai, Lu Li, Mudi Ma, Yukun Sun, Shan Ren, Xinzhe Li, Chunli Zheng, Reem Albilali and Chi He*, ","doi":"10.1021/acs.est.4c0566310.1021/acs.est.4c05663","DOIUrl":"https://doi.org/10.1021/acs.est.4c05663https://doi.org/10.1021/acs.est.4c05663","url":null,"abstract":"<p >Developing efficacious catalysts with superior Cl resistance and polychlorinated byproduct inhibition capability is crucial for realizing the environmentally friendly purification of chlorinated volatile organic compounds (CVOCs). Activating CVOC molecules and desorbing Cl species by modulating the metal–oxygen property is a promising strategy to fulfill these. Herein, a bifunctional CoRu/Al<sub>2</sub>O<sub>3</sub> catalyst with synergistic Co and Ru interactions (Ru–O–Co species) was rationally fabricated, which possesses abundant surface Co<sup>2+</sup> and Ru<sup>δ+</sup> sites and collaboratively facilitates the activation of lattice oxygen (O<sup>2–</sup>) and molecular oxygen (O<sub>2</sub> → O<sup>2–</sup> → O<sup>–</sup>), accelerating 1,2-dichloroethane (1,2-DCE) decomposition <i>via</i> the reaction route of enolic species → aldehydes → carboxylate/carbonate. Furthermore, CoRu/Al<sub>2</sub>O<sub>3</sub> stimulates 1,2-DCE oxidation under humid conditions as H<sub>2</sub>O molecules can be easily activated to active *OH (potential oxidizing agent) over Ru species, accelerating C–Cl dissociation and Cl desorption and promoting the transformation of catecholate-type (C═O) species to easily oxidizable carboxylic acid (COOH) species, remarkably suppressing the formation of hazardous CCl<sub>4</sub> and CHCl<sub>2</sub>CH<sub>2</sub>Cl. This study provides critical insights into the development of bifunctional catalysts to synergistically activate surface oxygen species and H<sub>2</sub>O molecules for industrial CVOC stable and efficient elimination.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 44","pages":"19872–19882 19872–19882"},"PeriodicalIF":10.8,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142577468","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Central SciencePub Date : 2024-10-23DOI: 10.1021/acs.est.4c0973710.1021/acs.est.4c09737
Yongping Shan, and , Wentao Jiao*,
{"title":"Rebuttal to Correspondence on “Effects of Temperature and DC Electric Fields on Perfluorooctanoic Acid Sorption Kinetics to Activated Carbon”","authors":"Yongping Shan, and , Wentao Jiao*, ","doi":"10.1021/acs.est.4c0973710.1021/acs.est.4c09737","DOIUrl":"https://doi.org/10.1021/acs.est.4c09737https://doi.org/10.1021/acs.est.4c09737","url":null,"abstract":"","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 44","pages":"19904–19905 19904–19905"},"PeriodicalIF":10.8,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142577470","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Central SciencePub Date : 2024-10-23DOI: 10.1021/acs.est.4c0561610.1021/acs.est.4c05616
Bumjun Park*, Hyunseung Kang and Christopher Zahasky,
{"title":"Statistical Mapping of PFOA and PFOS in Groundwater throughout the Contiguous United States","authors":"Bumjun Park*, Hyunseung Kang and Christopher Zahasky, ","doi":"10.1021/acs.est.4c0561610.1021/acs.est.4c05616","DOIUrl":"https://doi.org/10.1021/acs.est.4c05616https://doi.org/10.1021/acs.est.4c05616","url":null,"abstract":"<p >Per-and polyfluoroalkyl substances (PFAS) are synthetic chemicals that are increasingly being detected in groundwater. The negative health consequences associated with human exposure to PFAS make it essential to quantify the distribution of PFAS in groundwater systems. Mapping PFAS distributions is particularly challenging because a national patchwork of testing and reporting requirements has resulted in sparse and spatially biased data. In this analysis, an inhomogeneous Poisson process (IPP) modeling approach is adopted from ecological statistics to continuously map PFAS distributions in groundwater across the contiguous United States. The model is trained on a unique data set of 8910 PFAS groundwater measurements, using combined concentrations of two PFAS analytes. The IPP model predictions are compared with results from random forest models to highlight the robustness of this statistical modeling approach on sparse data sets. This analysis provides a new approach to not only map PFAS contamination in groundwater but also prioritize future sampling efforts.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 44","pages":"19843–19850 19843–19850"},"PeriodicalIF":10.8,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142577768","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Central SciencePub Date : 2024-10-22DOI: 10.1021/acs.est.4c0826010.1021/acs.est.4c08260
Qihui Kan, Pengfei Hou, Chunxiao Wang, Kun Lu, Shipeng Dong, Hang Zeng, Mian Li, Xing Meng*, Qing Huang and Liang Mao*,
{"title":"The Impact of Metal Ions on MXene Membranes: Critical Role of Titanium Vacancies","authors":"Qihui Kan, Pengfei Hou, Chunxiao Wang, Kun Lu, Shipeng Dong, Hang Zeng, Mian Li, Xing Meng*, Qing Huang and Liang Mao*, ","doi":"10.1021/acs.est.4c0826010.1021/acs.est.4c08260","DOIUrl":"https://doi.org/10.1021/acs.est.4c08260https://doi.org/10.1021/acs.est.4c08260","url":null,"abstract":"<p >Two-dimensional transition metal carbides and nitrides (MXenes) and MXene-based membranes hold promise for applications including water purification and seawater desalination; however, their environmental behavior and fate in these matrices remain unknown. In this study, we systematically assessed the reaction efficiencies of Ti<sub>3</sub>C<sub>2</sub>T<i><sub>x</sub></i> at varying important environmental conditions. Our experiments revealed that copper and iron ions accelerated the oxidation rate of Ti<sub>3</sub>C<sub>2</sub>T<i><sub>x</sub></i> 55.4 and 33.4 times, respectively. TiO<sub>2</sub> and amorphous carbon were identified as the primary solid products. Based on <i>in situ</i> water-phase atomic force microscopy, atomic high-angle annular dark-field scanning transmission electron microscopy, and theoretical results, we postulate that metal ions enhance Ti<sub>3</sub>C<sub>2</sub>T<i><sub>x</sub></i> oxidation by spontaneously migrating and anchoring at Ti vacancies, which then become active sites for this reaction. This process increases the adsorption of H<sub>2</sub>O and oxygen, making the Ti vacancy-rich surface convex area the most vulnerable site to attack. The findings in this study provide useful information for a comprehensive understanding of the interaction between MXene structural defects and metal ions as well as for the design and modification of MXene membranes resistant to metal ion impact.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 44","pages":"19861–19871 19861–19871"},"PeriodicalIF":10.8,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142577597","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Central SciencePub Date : 2024-10-22DOI: 10.1021/acs.est.4c0701010.1021/acs.est.4c07010
Ziyu Wang, Jiangyan Chen, Jianyu Song, Zixuan Pan, Yanqing Cong, Chunhui Du, Qiangbiao Li and Xuchun Li*,
{"title":"Insight into the Efficient Selective Reduction of Cr(VI) in Sulfite/UV Process under Near-Neutral Conditions: The Critical Role of In Situ-Generated Sulfite Radical","authors":"Ziyu Wang, Jiangyan Chen, Jianyu Song, Zixuan Pan, Yanqing Cong, Chunhui Du, Qiangbiao Li and Xuchun Li*, ","doi":"10.1021/acs.est.4c0701010.1021/acs.est.4c07010","DOIUrl":"https://doi.org/10.1021/acs.est.4c07010https://doi.org/10.1021/acs.est.4c07010","url":null,"abstract":"<p >Efficient removal of contaminants in complex water matrices under mild conditions is highly desirable but still challenging. In this study, we unraveled the overlooked but crucial role of sulfite radical (SO<sub>3</sub><sup>·–</sup>) in the efficient selective reduction of toxic Cr(VI) under near-neutral conditions. Fast removal of Cr(VI) at around pH 7 in sulfite/UV was found to be attributable to high reactivity of SO<sub>3</sub><sup>·–</sup> toward HCrO<sub>4</sub><sup>–</sup> (∼5.3 × 10<sup>6</sup> M<sup>–1</sup> s<sup>–1</sup>). Furthermore, SO<sub>3</sub><sup>·–</sup> was fast generated in situ via one-electron oxidation of S(IV) by transient reactive protonated Cr(V) and Cr(IV) intermediates. Therefore, the specific reactivity of SO<sub>3</sub><sup>·–</sup> and its in situ generation together resulted in the surprisingly positive effect of nitrate and the efficient reduction of Cr(VI) in authentic surface water and industrial wastewater. A mathematical model was developed to simulate Cr(VI) removal in the process, and thus quantitatively demonstrated the roles of reactive species, i.e., SO<sub>3</sub><sup>·–</sup> contributed to ∼93% of Cr(VI) reduction in surface water. Overall, this study provides an insight into the pivotal role of SO<sub>3</sub><sup>·–</sup> in Cr(VI) reduction, and underscores its significance in selective reduction and detoxification of contaminants.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 44","pages":"19893–19901 19893–19901"},"PeriodicalIF":10.8,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142577481","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Investigation of the Mechanism of Oxidative Potential Increase in Atmospheric Particulate Matter during Photoaging: Important Role of Aromatic Nitrogenous Compounds","authors":"Qingwen Wang, Qingcai Chen*, Hao Lin, Jiale Ding, Tong Sha and Yuemei Han, ","doi":"10.1021/acs.est.4c0319910.1021/acs.est.4c03199","DOIUrl":"https://doi.org/10.1021/acs.est.4c03199https://doi.org/10.1021/acs.est.4c03199","url":null,"abstract":"<p >Particulate matter (PM) undergoing various aging processes in the atmosphere changes its toxicity. However, the mechanism of toxicity evolution is not fully clarified currently. This study demonstrates that photoaging promotes an increase in the oxidative potential (OP) of atmospheric PM by about 30%, and the increased OP is mainly attributed to the production of secondary organic compounds, while water-soluble metal ions contribute only 11%. The OP of nonextractable matters (NEMs) of atmospheric PM was mostly increased after photoaging, followed by water-soluble matters (WSMs). NEM can produce quinone-like functional groups and secondary persistent free radicals during photoaging, which are most likely to produce reactive oxygen species (ROS). For WSM, the conversion of low-oxidation humic-like substances (HULIS) to high-oxidation HULIS is the main reason for the increase in OP. Quinones, nitrophenols, and N-containing heterocycles are the OP contributors produced during the conversion process. Among them, quinones are the main secondary oxidizing active compounds, while nitro-phenolic compounds and N-containing heterocyclic compounds may play a catalyst-like role, facilitating the production of oxidizing active compounds and ROS in the newly converted high-oxidation HULIS. This study clarifies the secondary OP generation mechanism and provides new insights into the uncertainty of PM toxicity during atmospheric aging.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 44","pages":"19818–19831 19818–19831"},"PeriodicalIF":10.8,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142577767","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Central SciencePub Date : 2024-10-22DOI: 10.1021/acs.est.4c0618710.1021/acs.est.4c06187
Havala O. T. Pye*, Lu Xu, Barron H. Henderson, Demetrios Pagonis, Pedro Campuzano-Jost, Hongyu Guo, Jose L. Jimenez, Christine Allen, T. Nash Skipper, Hannah S. Halliday, Benjamin N. Murphy, Emma L. D’Ambro, Paul O. Wennberg, Bryan K. Place, Forwood C. Wiser, V. Faye McNeill, Eric C. Apel, Donald R. Blake, Matthew M. Coggon, John D. Crounse, Jessica B. Gilman, Georgios I. Gkatzelis, Thomas F. Hanisco, L. Gregory Huey, Joseph M. Katich, Aaron Lamplugh, Jakob Lindaas, Jeff Peischl, Jason M. St Clair, Carsten Warneke, Glenn M. Wolfe and Caroline Womack,
{"title":"Evolution of Reactive Organic Compounds and Their Potential Health Risk in Wildfire Smoke","authors":"Havala O. T. Pye*, Lu Xu, Barron H. Henderson, Demetrios Pagonis, Pedro Campuzano-Jost, Hongyu Guo, Jose L. Jimenez, Christine Allen, T. Nash Skipper, Hannah S. Halliday, Benjamin N. Murphy, Emma L. D’Ambro, Paul O. Wennberg, Bryan K. Place, Forwood C. Wiser, V. Faye McNeill, Eric C. Apel, Donald R. Blake, Matthew M. Coggon, John D. Crounse, Jessica B. Gilman, Georgios I. Gkatzelis, Thomas F. Hanisco, L. Gregory Huey, Joseph M. Katich, Aaron Lamplugh, Jakob Lindaas, Jeff Peischl, Jason M. St Clair, Carsten Warneke, Glenn M. Wolfe and Caroline Womack, ","doi":"10.1021/acs.est.4c0618710.1021/acs.est.4c06187","DOIUrl":"https://doi.org/10.1021/acs.est.4c06187https://doi.org/10.1021/acs.est.4c06187","url":null,"abstract":"<p >Wildfires are an increasing source of emissions into the air, with health effects modulated by the abundance and toxicity of individual species. In this work, we estimate reactive organic compounds (ROC) in western U.S. wildland forest fire smoke using a combination of observations from the 2019 Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) field campaign and predictions from the Community Multiscale Air Quality (CMAQ) model. Standard emission inventory methods capture 40–45% of the estimated ROC mass emitted, with estimates of primary organic aerosol particularly low (5–8×). Downwind, gas-phase species abundances in molar units reflect the production of fragmentation products such as formaldehyde and methanol. Mass-based units emphasize larger compounds, which tend to be unidentified at an individual species level, are less volatile, and are typically not measured in the gas phase. Fire emissions are estimated to total 1250 ± 60 g·C of ROC per kg·C of CO, implying as much carbon is emitted as ROC as is emitted as CO. Particulate ROC has the potential to dominate the cancer and noncancer risk of long-term exposure to inhaled smoke, and better constraining these estimates will require information on the toxicity of particulate ROC from forest fires.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 44","pages":"19785–19796 19785–19796"},"PeriodicalIF":10.8,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142577572","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}