Comment on egusphere-2024-642 DOI Creative Commons
Jiewen Shen, Bin Zhao, Shuxiao Wang

et al.

Published: April 26, 2024

Abstract. Clustering of gaseous sulfuric acid (SA) enhanced by dimethylamine (DMA) is a major mechanism for new particle formation (NPF) in polluted atmospheres. However, uncertainty remains regarding the SA-DMA nucleation parameterization that reasonably represents cluster dynamics and applicable across various atmospheric conditions. This hinders accurate three-dimensional (3-D) modeling NPF subsequent assessment its environmental climatic impacts. Here we extensively compare different dynamics-based parameterizations identify most reliable one through combination box-model simulations, 3-D modeling, in-situ observations. Results show derived from Atmospheric Cluster Dynamic Code (ACDC) incorporating latest theoretical insights (DLPNO-CCSD(T)/aug-cc-pVTZ//ωB97X-D/6-311++G(3df,3pd) level theory) adequate representation dynamics, exhibits dependable performance simulation both winter summer conditions Beijing shows promise application diverse Another ACDC-derived parameterization, replacing theory with RI-CC2/aug-cc-pV(T+d)Z//M06-2X/6–311++G(3df,3pd), also performs well at relatively low temperatures around 280 K but limitations higher due to inappropriate thermodynamics. Additionally, previously reported simplifications simulating atmospheres tends overestimate rates under elevated temperature (> ~300 K) condensation sink (< ~3×10-3 s-1). Our findings highlight applicability which couples holistic modeling. The framework provides valuable reference developing other systems.

Language: Английский

Environmental effects of stratospheric ozone depletion, UV radiation, and interactions with climate change: UNEP Environmental Effects Assessment Panel, Update 2021 DOI Creative Commons
Paul W. Barnes,

T. Matthew Robson,

Patrick J. Neale

et al.

Photochemical & Photobiological Sciences, Journal Year: 2022, Volume and Issue: 21(3), P. 275 - 301

Published: Feb. 21, 2022

Abstract The Environmental Effects Assessment Panel of the Montreal Protocol under United Nations Environment Programme evaluates effects on environment and human health that arise from changes in stratospheric ozone layer concomitant variations ultraviolet (UV) radiation at Earth’s surface. current update is based scientific advances have accumulated since our last assessment (Photochem Photobiol Sci 20(1):1–67, 2021). We also discuss how climate change affects depletion radiation, change. resulting interlinking depletion, UV are assessed terms air quality, carbon sinks, ecosystems, health, natural synthetic materials. further highlight potential impacts biosphere extreme events occurring with increasing frequency as a consequence These other interactive examined respect to benefits its Amendments providing life Earth by controlling production various substances contribute both

Language: Английский

Citations

78

Changes in tropospheric air quality related to the protection of stratospheric ozone in a changing climate DOI Creative Commons
S. Madronich, Barbara Sulzberger, Janice Longstreth

et al.

Photochemical & Photobiological Sciences, Journal Year: 2023, Volume and Issue: 22(5), P. 1129 - 1176

Published: June 13, 2023

Ultraviolet (UV) radiation drives the net production of tropospheric ozone (O

Language: Английский

Citations

34

Enhancement of Atmospheric Nucleation Precursors on Iodic Acid-Induced Nucleation: Predictive Model and Mechanism DOI Creative Commons
Fangfang Ma, Hong‐Bin Xie, Rongjie Zhang

et al.

Environmental Science & Technology, Journal Year: 2023, Volume and Issue: 57(17), P. 6944 - 6954

Published: April 21, 2023

Iodic acid (IA) has recently been recognized as a key driver for new particle formation (NPF) in marine atmospheres. However, the knowledge of which atmospheric vapors can enhance IA-induced NPF remains limited. The unique halogen bond (XB)-forming capacity IA makes it difficult to evaluate enhancing potential (EP) target compounds on based widely studied sulfuric systems. Herein, we employed three-step procedure EP nucleation precursors NPF. First, evaluated 63 by simulating free energies (ΔG) IA-containing dimer clusters. Among all clusters, 44 contained XBs, demonstrating that XBs are frequently formed. Based calculated ΔG values, quantitative structure–activity relationship model was developed evaluating other precursors. Second, amines and O/S-atom-containing acids were found have high EP, with diethylamine (DEA) yielding highest combining both concentration considered Finally, studying larger (IA)1–3(DEA)1–3 IA-DEA system merely 0.1 ppt (2.5×106 cm–3) DEA yields comparable rates IA–iodous system.

Language: Английский

Citations

30

Continuing benefits of the Montreal Protocol and protection of the stratospheric ozone layer for human health and the environment DOI Creative Commons
S. Madronich, G. Bernhard, Patrick J. Neale

et al.

Photochemical & Photobiological Sciences, Journal Year: 2024, Volume and Issue: 23(6), P. 1087 - 1115

Published: May 19, 2024

Abstract The protection of Earth’s stratospheric ozone (O 3 ) is an ongoing process under the auspices universally ratified Montreal Protocol and its Amendments adjustments. A critical part this assessment environmental issues related to changes in O . United Nations Environment Programme’s Environmental Effects Assessment Panel provides annual scientific evaluations some key arising recent collective knowledge base. This current update includes a comprehensive incidence rates skin cancer, cataract other eye diseases observed worldwide; effects UV radiation on tropospheric oxidants, air water quality; trends breakdown products fluorinated chemicals information their toxicity; technological innovations building materials for greater resistance radiation. These span wide range topics, including both harmful beneficial exposure radiation, complex interactions with climate change. While has succeeded preventing large reductions , future may occur due number natural anthropogenic factors. Thus, frequent assessments potential impacts are essential ensure that policies remain based best available knowledge. Graphical abstract

Language: Английский

Citations

8

The Global Threat from the Irreversible Accumulation of Trifluoroacetic Acid (TFA) DOI Creative Commons
Hans Peter H. Arp, Andrea Gredelj, Juliane Glüge

et al.

Environmental Science & Technology, Journal Year: 2024, Volume and Issue: 58(45), P. 19925 - 19935

Published: Oct. 30, 2024

Trifluoroacetic acid (TFA) is a persistent and mobile substance that has been increasing in concentration within diverse environmental media, including rain, soils, human serum, plants, plant-based foods, drinking water. Currently, TFA concentrations are orders of magnitude higher than those other per- polyfluoroalkyl substances (PFAS). This accumulation due to many PFAS having as transformation product, several fluorinated gases (F-gases), pesticides, pharmaceuticals, industrial chemicals, addition direct release industrially produced TFA. Due TFA's extreme persistence ongoing emissions, irreversibly. What remains less clear the thresholds where irreversible effects on local or global scales occur. There indications from mammalian toxicity studies toxic reproduction it exhibits liver toxicity. Ecotoxicity data scarce, with most being for aquatic systems; fewer available terrestrial bioaccumulates readily. Collectively, these trends imply meets criteria planetary boundary threat novel entities because planetary-scale exposure, potential disruptive impacts vital earth system processes could The rational response this instigate binding actions reduce emissions its precursors.

Language: Английский

Citations

8

Rapid sulfuric acid–dimethylamine nucleation enhanced by nitric acid in polluted regions DOI Open Access
Ling Liu, Fangqun Yu, Lin Du

et al.

Proceedings of the National Academy of Sciences, Journal Year: 2021, Volume and Issue: 118(35)

Published: Aug. 27, 2021

Recent research [Wang et al., Nature 581, 184-189 (2020)] indicates nitric acid (NA) can participate in sulfuric (SA)-ammonia (NH3) nucleation the clean and cold upper free troposphere, whereas NA exhibits no obvious effects at boundary layer with relatively high temperatures. Herein, considering that an SA-dimethylamine (DMA) mechanism was detected megacities [Yao Science 361, 278-281 (2018)], roles of SA-DMA are investigated. Different from SA-NH3 nucleation, we found enhance SA-DMA-based particle formation rates polluted atmospheric layer, such as Beijing winter, enhancement up to 80-fold. Moreover, promote number concentrations clusters (up 27-fold) contribute 76% cluster pathways 280 K. The enhancements on by critical for particulate pollution DMA concentrations.

Language: Английский

Citations

41

Measurement of atmospheric nanoparticles: Bridging the gap between gas-phase molecules and larger particles DOI Open Access
Chao Peng,

Chenjuan Deng,

Ting Lei

et al.

Journal of Environmental Sciences, Journal Year: 2022, Volume and Issue: 123, P. 183 - 202

Published: March 11, 2022

Language: Английский

Citations

17

A novel formation mechanism of sulfamic acid and its enhancing effect on methanesulfonic acid–methylamine aerosol particle formation in agriculture-developed and coastal industrial areas DOI Creative Commons
Hui Wang,

Shuqin Wei,

Jihuan Yang

et al.

Atmospheric chemistry and physics, Journal Year: 2025, Volume and Issue: 25(5), P. 2829 - 2844

Published: March 7, 2025

Abstract. Sulfamic acid (SFA) significantly impacts atmospheric pollution and poses potential risks to human health. Although traditional sources of SFA their role in sulfuric acid–dimethylamine new particle formation (NPF) have received increasing attention, the mechanism from HNSO2 hydrolysis with methanesulfonic (MSA) its enhancing effect on MSA-methylamine (MA) NPF not been studied, which will limit understanding source loss agriculture-developed coastal industrial areas. Here, gaseous interfacial MSA was investigated using quantum chemical calculations Born–Oppenheimer molecular dynamics (BOMD) simulations. Furthermore, MSA-MA system assessed Atmospheric Cluster Dynamic Code (ACDC) kinetic model. Our simulation results indicate that can be competitive catalyzed by H2O within an altitude 5–15 km. At air–water interface, two types reactions, ion-forming proton exchange form SFA− … H3O+ ion pair, were observed timescale picoseconds. Considering overall environment emission reduction, present findings suggest may play a significant growth aerosol particles, as (i) directly participate MSA-MA-based clusters enhance rate these approximately 103 times at 278.15 K (ii) species interface attract molecules aqueous surface thus promote growth.

Language: Английский

Citations

0

Reaction of SO3 with H2SO4 and its implications for aerosol particle formation in the gas phase and at the air–water interface DOI Creative Commons
Rui Wang, Yang Cheng,

Shasha Chen

et al.

Atmospheric chemistry and physics, Journal Year: 2024, Volume and Issue: 24(7), P. 4029 - 4046

Published: April 4, 2024

Abstract. The reactions between SO3 and atmospheric acids are indispensable in improving the formation of aerosol particles. However, relative to those with organic acids, reaction inorganic has not received much attention. Here, we explore H2SO4, a typical acid, gas phase at air–water interface using quantum chemical (QC) calculations Born–Oppenheimer molecular dynamics simulations. We also report effect H2S2O7, product on new particle (NPF) various environments Atmospheric Cluster Dynamics Code (ACDC) kinetic model QC calculations. present findings show that gas-phase + H2SO4 without water molecules both low-energy-barrier processes. With involvement interfacial molecules, H2O induced S2O72-⋯H3O+ ion pair, HSO4- mediated HSO4-⋯H3O+ deprotonation H2S2O7 was observed proceeded picosecond timescale. suggest potential contribution SO3–H2SO4 NPF growth, showing (i) although is easily hydrolyzed form it can directly participate H2SO4–NH3-based cluster more obvious enhancement SA–A-based formation, (ii) formed S2O72- attract candidate species from surface and, thus, accelerate growth.

Language: Английский

Citations

3

Pyruvic acid, an efficient catalyst in SO&lt;sub&gt;3&lt;/sub&gt; hydrolysis and effective clustering agent in sulfuric-acid-based new particle formation DOI Creative Commons
Narcisse T. Tsona, Lin Du, Ling Liu

et al.

Atmospheric chemistry and physics, Journal Year: 2022, Volume and Issue: 22(3), P. 1951 - 1963

Published: Feb. 11, 2022

Abstract. The role of pyruvic acid (PA), one the most abundant α-keto carboxylic acids in atmosphere, was investigated both SO3 hydrolysis reaction to form sulfuric (SA) and SA-based aerosol particle formation using quantum chemical calculations a cluster dynamics model. We found that PA-catalyzed is thermodynamically driven transformation process, proceeding with negative Gibbs free-energy barrier, ca. −1 kcal mol−1 at 298 K, ∼ 6.50 lower than water-catalyzed hydrolysis. Results indicated can potentially compete SA production, especially dry polluted areas, where it be 2 orders magnitude more efficient reaction. Given effective stabilization product as SA⚫PA cluster, we proceeded examine PA clustering efficiency sulfuric-acid–pyruvic-acid–ammonia (SA-PA-NH3) system. Our thermodynamic data used Atmospheric Cluster Dynamics Code under relevant tropospheric temperatures concentrations (106 molec.cm-3), (1010 molec.cm-3) NH3 (1011 5 × 1011 PA-enhanced involves clusters containing molecule. Namely, these monomer 238 (SA)2⚫PA⚫(NH3)2 contribute by 100 % net flux formation. At higher (258 278 K), however, dominated pure SA-NH3 clusters, while would rather evaporate from high not enhancing effect examined evaluating ratio ternary SA-PA-NH3 rate binary rate. results show enhancement factor almost insensitive concentrations, 4.7 102 K [NH3] = 1.3 molec.cm-3. This indicates may actively participate formation, only cold regions troposphere highly NH3-polluted environments. inclusion this mechanism models reduce uncertainties prevail modeling impact on climate.

Language: Английский

Citations

12