Biomass-burning organic aerosols as a pool of atmospheric reactive triplets to drive multiphase sulfate formation DOI Creative Commons
Zhancong Liang, Liyuan Zhou,

Yuqing Chang

et al.

Proceedings of the National Academy of Sciences, Journal Year: 2024, Volume and Issue: 121(51)

Published: Dec. 13, 2024

Biomass-burning organic aerosol(s) (BBOA) are rich in brown carbon, which significantly absorbs solar irradiation and potentially accelerates global warming. Despite its importance, the multiphase photochemistry of BBOA after light absorption remains poorly understood due to challenges determining oxidant concentrations reaction kinetics within aerosol particles. In this study, we explored photochemical reactivity particles S(IV) oxidation sulfate. We found that sulfate formation under is predominantly driven by photosensitization involving triplet excited states ( 3 * ) instead iron, nitrate, photochemistry. Rates three orders magnitude higher than those observed bulk solution, primarily fast interfacial reactions. Our results highlight chemistry can greatly contribute sulfate, as an example secondary pollutants. Photosensitization will likely become increasingly crucial intensified wildfires.

Language: Английский

Photoactivation of Chlorine and Its Catalytic Role in the Formation of Sulfate Aerosols DOI
Yiqun Cao, Jiarong Liu, Qingxin Ma

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(2), P. 1467 - 1475

Published: Jan. 8, 2024

We present a novel mechanism for the formation of photocatalytic oxidants in deliquescent NaCl particles, which can greatly promote multiphase photo-oxidation SO2 to produce sulfate. The photoexcitation [Cl––H3O+–O2] complex leads generation Cl and OH radicals, is key reason enhancing aqueous-phase oxidation accelerating oxidation. mass normalization rate sulfate production from photoreaction on droplets could be estimated 0.80 × 10–4 μg·h–1 at 72% RH 1.33 81% RH, equivalent known O3 liquid-phase mechanism. Our findings highlight significance particles as non-negligible source coastal areas. Furthermore, this study underscores importance Cl– photochemistry atmosphere.

Language: Английский

Citations

17
Strong electric field force at the air/water interface drives fast sulfate production in the atmosphere DOI Creative Commons
Yangyang Liu,

Qiuyue Ge,

Tao Wang

et al.

Chem, Journal Year: 2023, Volume and Issue: 10(1), P. 330 - 351

Published: Oct. 26, 2023

Language: Английский

Citations

24
Significantly Accelerated Photosensitized Formation of Atmospheric Sulfate at the Air–Water Interface of Microdroplets DOI
Wei Wang, Yangyang Liu, Tao Wang

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(10), P. 6580 - 6590

Published: March 1, 2024

The multiphase oxidation of sulfur dioxide (SO2) to form sulfate is a complex and important process in the atmosphere. While conventional photosensitized reaction mainly explored bulk medium reported be one drivers trigger atmospheric production, how this scheme functionalizes at air–water interface (AWI) aerosol remains an open question. Herein, employing advanced size-controllable microdroplet-printing device, surface-enhanced Raman scattering (SERS) analysis, nanosecond transient adsorption spectrometer, molecular level theoretical calculations, we revealed previously overlooked interfacial role SO2 humic-like substance (HULIS) aerosol, where 3–4 orders magnitude increase formation rate was speculated cloud relevant-sized particles relative bulk-phase medium. rapid battery reactive oxygen species (ROS) comes from accelerated electron transfer AWI, excited triplet state HULIS (3HULIS*) incomplete solvent cage can readily capture electrons HSO3– way that more efficient than fully blocked by water molecules. This phenomenon could explained significantly reduced desolvation energy barrier required for reagents residing AWI region with shell.

Language: Английский

Citations

12
Aqueous-Phase Photoreactions of Mixed Aromatic Carbonyl Photosensitizers Yield More Oxygenated, Oxidized, and less Light-Absorbing Secondary Organic Aerosol (SOA) than Single Systems DOI Creative Commons

Brix Raphael Go,

Yongjie Li, Dan Dan Huang

et al.

Environmental Science & Technology, Journal Year: 2024, Volume and Issue: 58(18), P. 7924 - 7936

Published: April 23, 2024

Aromatic carbonyls have been mainly probed as photosensitizers for aqueous secondary organic aerosol (aqSOA) and light-absorbing (i.e., brown carbon or BrC) formation, but due to their nature, they can also undergo oxidation form aqSOA BrC. However, photochemical transformations of aromatic carbonyl photosensitizers, particularly in multicomponent systems, are understudied. This study explored formation from the irradiation mixed single systems under cloud/fog conditions. Mixed consisting phenolic only (VL + ActSyr SyrAld: vanillin [VL] acetosyringone [ActSyr] syringaldehyde [SyrAld]) another composed both nonphenolic (DMB 3,4-dimethoxybenzaldehyde [DMB], a carbonyl, SyrAld) were compared VL (VL*) DMB (DMB*), respectively. In shorter lifetimes indicate diminished capacity trigger other compounds (e.g., guaiacol [GUA], noncarbonyl phenol). contrast slow decay minimal photoenhancement DMB*, rapid photodegradation significant VL* efficient direct photosensitized self-photosensitization). Relative increased oxidant availability promoted functionalization SyrAld accelerated conversion early generation SyrAld. Moreover, oxidizable substrates countered by stronger oxidative limited contribution light absorption. suggests weaker radiative effect BrC photosensitizer than systems. Furthermore, more oxygenated oxidized was observed with increasing complexity reaction < GUA). work offers new insights into emphasizing dual role sources substrates.

Language: Английский

Citations

6
Enhanced Sulfate Formation through Synergistic Effects of Chlorine Chemistry and Photosensitization in Atmospheric Particles DOI
Ruifeng Zhang, Chak K. Chan

ACS ES&T Air, Journal Year: 2024, Volume and Issue: 1(2), P. 92 - 102

Published: Jan. 23, 2024

Numerous studies have demonstrated that organic photosensitizers from biomass burning can generate oxidants to effectively convert inorganic and precursors into secondary aerosols. Particulate chloride ions be internally mixed with in particles. In this study, we investigate the impact of interaction chlorine chemistry photosensitization on oxidative potential aerosols by utilizing SO2 oxidation form sulfate as an indicator. Mixed particles glyoxal its reaction products ammonia imidazole-2-carboxaldehyde (IC) were studied. Premixed NH4Cl + a 4–5 times higher formation rate than premixed NaCl glyoxal, particularly at low relative humidity, suggesting role photosensitization. Furthermore, addition IC resulted ∼73-fold increase production compared alone. No noticeable was observed presence alone, likely due high particle acidity study (i.e., pH = 2). The kinetic analysis these results yields constant triplet state IC, 3IC*, ∼3 orders magnitude previously reported values bulk solution. These findings underscore significance synergetic effect enhancing atmospheric capacity.

Language: Английский

Citations

5
Enhanced sulfate formation in mixed biomass burning and sea-salt interactions mediated by photosensitization: effects of chloride, nitrogen-containing compounds, and atmospheric aging DOI Creative Commons
Rongzhi Tang,

Jialiang Ma,

Ruifeng Zhang

et al.

Atmospheric chemistry and physics, Journal Year: 2025, Volume and Issue: 25(1), P. 425 - 439

Published: Jan. 13, 2025

Abstract. Discrepancies persist between modeled simulations and measured sulfate concentrations in the marine boundary layer, especially when air is influenced by biomass burning plumes. However, there has been a notable dearth of research conducted on interactions sea-salt aerosol plumes, impeding comprehensive understanding formation. This work studied formation mixing real (BB) extracts NaCl, mimicking internal mixtures BB particles. BB–NaCl particles had significantly higher rate than incense (IS)–NaCl For fresh particles, followed trend corn straw (CS)–NaCl > rice (RS)–NaCl wheat (WS)–NaCl IS–NaCl. The filter sample aging was achieved exposure to OH• generated from UV irradiation. After aging, RS–NaCl exhibited highest enhancement rates among all due RS NaCl. Bulk aqueous experiments spiked with NaCl using model photosensitizers (PSs) nitrogen-containing organic compounds (NOCs), pyrazine (CHN), 4-nitrocatechol (CHON) revealed positive effects chloride PS–CHON system negative PS–CHN Our suggests that reaching or near coastal areas can affect via photosensitizer-mediated reactions, potentially exacerbating pollution.

Language: Английский

Citations

0
Invited Perspective: Incense Burning and Cardiovascular Risk—A Rising Concern DOI Creative Commons
Yifei Qin,

Gaetano Santulli

Environmental Health Perspectives, Journal Year: 2025, Volume and Issue: 133(1)

Published: Jan. 1, 2025

Language: Английский

Citations

0
Light Absorption of Black and Brown Carbon in Eastern China DOI
Rongzhi Tang,

Weizhen Cui,

Xiuli Zhang

et al.

Journal of Hazardous Materials, Journal Year: 2025, Volume and Issue: 489, P. 137530 - 137530

Published: Feb. 8, 2025

Language: Английский

Citations

0
Complexities of Photosensitization in Atmospheric Particles DOI Creative Commons
Zhancong Liang, Yongjie Li,

Brix Raphael Go

et al.

ACS ES&T Air, Journal Year: 2024, Volume and Issue: 1(11), P. 1333 - 1351

Published: Oct. 10, 2024

Brown carbons (BrCs) play a pivotal role in the light absorption by aerosol particulates exerting positive radiative forcing effect that contributes to global warming. Beyond impacts on balance, some BrCs, as photosensitizers, can generate reactive triplet-state molecules toward various atmospheric upon photoexcitation. The significance of photosensitization has been increasingly recognized, particularly context escalated wildfire incidents emit substantial BrCs. We focus complex discussing current challenges, including (1) diverse reactivities photosensitizer mixture particles, (2) methodologies for investigating processes, (3) driving factors photosensitization, and (4) typical pathways mechanisms photosensitized reactions. Lastly, we advise future research refined parametrization triplet singlet oxygen concentrations, alongside their reactivities.

Language: Английский

Citations

2
Evaporation-Induced Transformations in Volatile Chemical Product-Derived Secondary Organic Aerosols: Browning Effects and Alterations in Oxidative Reactivity DOI Creative Commons
Liyuan Zhou, Zhancong Liang, Yiming Qin

et al.

Environmental Science & Technology, Journal Year: 2024, Volume and Issue: 58(25), P. 11105 - 11117

Published: June 12, 2024

Volatile chemical products (VCPs) are increasingly recognized as significant sources of volatile organic compounds (VOCs) in urban atmospheres, potentially serving key precursors for secondary aerosol (SOA) formation. This study investigates the formation and physicochemical transformations VCP-derived SOA, produced through ozonolysis VOCs evaporated from a representative room deodorant air freshener, focusing on effects evaporation its molecular composition, light absorption properties, reactive oxygen species (ROS) generation. Following evaporation, solutes become concentrated, accelerating reactions within matrix that lead to 42% reduction peroxide content noticeable browning SOA. process occurs most effectively at moderate relative humidity (∼40%), reaching maximum solute concentration before solidification. Molecular characterization reveals evaporating SOA produces highly conjugated nitrogen-containing interactions between existing or transformed carbonyl reduced nitrogen species, likely acting chromophores responsible observed brownish coloration. Additionally, reactivity was elucidated heterogeneous oxidation sulfur dioxide (SO

Language: Английский

Citations

1