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All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Ozone Gas: Scientific Justification and Practical Guidelines for Improvised Disinfection using Consumer-Grade Ozone Generators and Plastic Storage Boxes

Here, we describe direct measurements of ozone concentration achievable in small enclosed containers (plastic storage boxes) for use as improvised decontamination systems for small articles such as disposable PPE (N95 masks, nitrile gloves, etc.), clothing, mail and small packages, food, and other miscellaneous articles. The emphasis is on the reliable and sustained generation of ozone gas concentrations of sufficient concentration and duration to create an effective virucidal environment to achieve more than 95% to 99% viral inactivation, based upon the data already published in the peer-review literature on this topic. The suggestion that ozone be used to inactivate virus is certainly not a new idea. Our objective in this report is to make clear that the necessary levels of ozone can be improvised using simple, easy-to-use, inexpensive, and widely available supplies, and that there is every theoretical and experimental reason to believe that this approach is as highly effective in viral inactivation by ozone as are the far more expensive, complex, cumbersome, and less available equivalent ozone (and other) disinfectant systems that have themselves become unavailable during times of pandemic crisis. Using multiple types of readily available commercial ozone generators, concentration in the tested improvised enclosure is tracked over time to assess ozone charging and decay rates, and the ozone quenching effects of items placed in the box. Generator performance is compared against published ozone dosage values for virucidal and antimicrobial activity. Bubbler and box-fan-type ozone generators were found to be effective at achieving and maintaining target concentrations of 10ppm ozone or higher, whereas automotive cigarette lighter and universal serial bus type plug in “air freshener” ozone generators could not achieve the target concentrations in these experiments. Calculations and practical guidelines for assembly and effective use of an ozone box for improvised decontamination are offered. The majority of this report is directed toward the scientific justification and rationale for this approach. The end of the document summarizes the findings and offers simplified designs for the construction and use of ozone boxes as an improvised method of disinfection.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2023

Low ozone dry deposition rates to sea ice during the MOSAiC field campaign: Implications for the Arctic boundary layer ozone budget

Dry deposition to the surface is one of the main removal pathways of tropospheric ozone (O 3 ). We quantified for the first time the impact of O 3 deposition to the Arctic sea ice on the planetary boundary layer (PBL) O 3 concentration and budget using year-round flux and concentration observations from the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) campaign and simulations with a single-column atmospheric chemistry and meteorological model (SCM). Based on eddy-covariance O 3 surface flux observations, we find a median surface resistance on the order of 20,000 s m –1 , resulting in a dry deposition velocity of approximately 0.005 cm s –1 . This surface resistance is up to an order of magnitude larger than traditionally used values in many atmospheric chemistry and transport models. The SCM is able to accurately represent the yearly cycle, with maxima above 40 ppb in the winter and minima around 15 ppb at the end of summer. However, the observed springtime ozone depletion events are not captured by the SCM. In winter, the modelled PBL O 3 budget is governed by dry deposition at the surface mostly compensated by downward turbulent transport of O 3 towards the surface. Advection, which is accounted for implicitly by nudging to reanalysis data, poses a substantial, mostly negative, contribution to the simulated PBL O 3 budget in summer. During episodes with low wind speed (<5 m s –1 ) and shallow PBL (<50 m), the 7-day mean dry deposition removal rate can reach up to 1.0 ppb h –1 . Our study highlights the importance of an accurate description of dry deposition to Arctic sea ice in models to quantify the current and future O 3 sink in the Arctic, impacting the tropospheric O 3 budget, which has been modified in the last century largely due to anthropogenic activities.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Ozone Monitor (OZONE) Instrument Handbook

The primary measurement output from the Thermo Scientific Ozone Analyzer is the concentration of the analyte (O3) reported at 1-s resolution in units of ppbv in ambient air. Note that because of internal pneumatic switching limitations the instrument only makes an independent measurement every 4 seconds. Thus, the same concentration number is repeated roughly 4 times at the uniform, monotonic 1-s time base used in the AOS systems. Accompanying instrument outputs include sample temperatures, flows, chamber pressure, lamp intensities and a multiplicity of housekeeping information. There is also a field for operator comments made at any time while data is being collected.

47 OTHER INSTRUMENTATION↗
DOE OSTI2020

Chemical changes in thirdhand smoke associated with remediation using an ozone generator

Ozonation is a common remediation approach to eliminate odors from mold, tobacco and fire damage in buildings. Little information exists to: 1) assess its effectiveness; 2) provide guidance on operation conditions; and 3) identify potential risks associated with the presence of indoor ozone and ozonation byproducts. The goal of this study is to evaluate chemical changes in thirdhand smoke (THS) aerosols induced by high levels of ozone, in comparison with THS aerosols aged under similar conditions in the absence of ozone. Samples representing different stages of smoke aging in the absence of ozone, including freshly emitted secondhand smoke (SHS) and THS, were collected inside an 18-m 3 room-sized chamber over a period of 42 h after six cigarettes were consumed. The experiments involved collection and analysis of gas phase species including volatile organic compounds (VOCs), volatile carbonyls, semivolatile organic compounds (SVOCs), and particulate matter. VOC analysis was carried out by gas chromatography/mass spectrometry with a thermal desorption inlet (TD-GC/MS), and volatile carbonyls were analyzed by on-line derivatization with dinitrophenylhydrazine (DNPH), followed by liquid chromatography with UV/VIS detection. SVOCs were extracted from XAD-coated denuders and Teflon-coated fiberglass filters in the absence of ozone. In those extracts, tobacco-specific nitrosamines (TSNAs) and other SVOCs were analyzed by gas chromatography with positive chemical ionization-triple quadrupole mass spectrometric detection (GC/PCI-QQQ-MS), and polycyclic aromatic hydrocarbons (PAHs) were quantified by gas chromatography with ion trap mass spectrometric detection (GC/IT-MS) in selected ion monitoring mode. Particulate matter concentration was determined gravimetrically. In a second experiment, a 300 mg h -1 commercial ozone generator was operated during 1 h, one day after smoke was generated, to evaluate the remediation of THS by ozonation. VOCs and volatile carbonyls were analyzed before and after ozonation. Extracts from fabrics that were exposed in the chamber before and after ozonation as surrogates for indoor furnishings were analyzed by GC/IT-MS, and aerosol size distribution was studied with a scanning mobility particle sizer. Ozone concentration was measured with a photometric detector. An estimated 175 mg ozone reacted with THS after 1 h of treatment, corresponding to 58% of the total O 3 released during that period. Fabric-bound nicotine was depleted after ozonation, and the surface concentration of PAHs adsorbed to fabric specimens decreased by an order of magnitude due to reaction with ozone, reaching pre-smoking levels. These results suggest that ozonation has the potential to remove harmful THS chemicals from indoor surfaces. However, gas phase concentrations of volatile carbonyls, including formaldehyde, acetaldehyde and acetone were higher immediately after ozonation. Ultrafine particles (UFP, in most cases with size <60 nm) were a major ozonation byproduct. UFP number concentrations peaked shortly after ozonation ended, and remained at higher-than background levels for several hours. Based on these results, minimum re-entry times after ozone treatment were predicted for different indoor scenarios. Clearly defining re-entry times can serve as a practical measure to prevent acute exposures to ozone and harmful ozonation byproducts after treatment. This study evaluated potential benefits and risks associated with THS remediation using ozone, providing insights into this technology.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Reducing Long‐Standing Surface Ozone Overestimation in Earth System Modeling by High‐Resolution Simulation and Dry Deposition Improvement

The overestimation of surface ozone concentration in low‐resolution global atmospheric chemistry and climate models has been a long‐standing issue. We first update the ozone dry deposition scheme in both high‐ (0.25°) and low‐resolution (1°) Community Earth System Model (CESM) version 1.3 runs, by adding the effects of leaf area index and correcting the sunlit and shaded fractions of stomatal resistances. With this update, 5‐year‐long summer simulations (2015–2019) using the low‐resolution CESM still exhibit substantial ozone overestimation (by 6.0–16.2 ppbv) over the U.S., Europe, eastern China, and ozone pollution hotspots. The ozone dry deposition scheme is further improved by adjusting the leaf cuticle conductance, reducing the mean ozone bias by 19%, and increasing the model resolution further reduces the ozone overestimation by 43%. We elucidate the mechanism by which model grid spacing influences simulated ozone, revealing distinctive pathways in urban versus rural areas. In rural areas, grid spacing mainly affects daytime ozone levels, where additional NO x emissions from nearby urban areas result in an ozone boost and overestimation in low‐resolution simulations. In contrast, over urban areas, daytime ozone overestimation follows a similar mechanism due to the influence of volatile organic compounds from surrounding rural areas. However, nighttime ozone overestimation is closely linked to weakened NO titration owing to the redistribution of urban NO x to rural areas. Additionally, stratosphere‐troposphere exchange may also contribute to reducing ozone bias in high‐resolution simulations, warranting further investigation. This optimized high‐resolution CESM may enhance understanding of ozone formation mechanisms, sources, and changes in a warming climate.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Adrenal Stress Hormone Regulation of Hepatic Homeostatic Function After an Acute Ozone Exposure in Wistar-Kyoto Male Rats

Ozone-induced lung injury, inflammation, and pulmonary/hypothalamus gene expression changes are diminished in adrenalectomized (AD) rats. Acute ozone exposure induces metabolic alterations concomitant with increases in epinephrine and corticosterone. We hypothesized that adrenal hormones are responsible for observed hepatic ozone effects, and in AD rats, these changes would be diminished. In total, 5–7 days after sham (SH) or AD surgeries, male Wistar-Kyoto rats were exposed to air or 0.8-ppm ozone for 4 h. Serum samples were analyzed for metabolites and liver for transcriptional changes immediately post-exposure. Ozone increased circulating triglycerides, cholesterol, free fatty-acids, and leptin in SH but not AD rats. Ozone-induced inhibition of glucose-mediated insulin release was absent in AD rats. Unlike diminution of ozone-induced hypothalamus and lung mRNA expression changes, AD in air-exposed rats (AD-air/SH-air) caused differential hepatic expression of ~1000 genes. Likewise, ozone in AD rats caused differential expression of ~1000 genes (AD-ozone/AD-air). Ozone-induced hepatic changes in SH rats reflected enrichment for pathways involving metabolic processes, including acetyl-CoA biosynthesis, TCA cycle, and sirtuins. Upstream predictor analysis identified similarity to responses produced by glucocorticoids and pathways involving forskolin. These changes were absent in AD rats exposed to ozone. However, ozone caused unique changes in AD liver mRNA reflecting activation of synaptogenesis, neurovascular coupling, neuroinflammation, and insulin signaling with inhibition of senescence pathways. In these rats, upstream predictor analysis identified numerous microRNAs likely involved in glucocorticoid insufficiency. These data demonstrate the critical role of adrenal stress hormones in ozone-induced hepatic homeostasis and necessitate further research elucidating their role in propagating environmentally driven diseases.

Toxicology↗
DOE OSTI2022

Ozone depletion in the Arctic and Antarctic stratosphere induced by wildfire smoke

Abstract. A record-breaking stratospheric ozone loss was observed over the Arctic and Antarctica in 2020. Strong ozone depletion occurred over Antarctica in 2021 as well. The ozone holes developed in smoke-polluted air. In this article, the impact of Siberian and Australian wildfire smoke (dominated by organic aerosol) on the extraordinarily strong ozone reduction is discussed. The study is based on aerosol lidar observations in the North Pole region (October 2019–May 2020) and over Punta Arenas in southern Chile at 53.2∘ S (January 2020–November 2021) as well as on respective NDACC (Network for the Detection of Atmospheric Composition Change) ozone profile observations in the Arctic (Ny-Ålesund) and Antarctica (Neumayer and South Pole stations) in 2020 and 2021. We present a conceptual approach on how the smoke may have influenced the formation of polar stratospheric clouds (PSCs), which are of key importance in the ozone-depleting processes. The main results are as follows: (a) the direct impact of wildfire smoke below the PSC height range (at 10–12 km) on ozone reduction seems to be similar to well-known volcanic sulfate aerosol effects. At heights of 10–12 km, smoke particle surface area (SA) concentrations of 5–7 µm2 cm−3 (Antarctica, spring 2021) and 6–10 µm2 cm−3 (Arctic, spring 2020) were correlated with an ozone reduction in terms of ozone partial pressure of 0.4–1.2 mPa (about 30 % further ozone reduction over Antarctica) and of 2–3.5 mPa (Arctic, 20 %–30 % reduction with respect to the long-term springtime mean). (b) Within the PSC height range, we found indications that smoke was able to slightly increase the PSC particle number and surface area concentration. In particular, a smoke-related additional ozone loss of 1–2 mPa (10 %–20 % contribution to the total ozone loss over Antarctica) was observed in the 14–23 km PSC height range in September–October 2020 and 2021. Smoke particle number concentrations ranged from 10 to 100 cm−3 and were about a factor of 10 (in 2020) and 5 (in 2021) above the stratospheric aerosol background level. Satellite observations indicated an additional mean column ozone loss (deviation from the long-term mean) of 26–30 Dobson units (9 %–10 %, September 2020, 2021) and 52–57 Dobson units (17 %–20 %, October 2020, 2021) in the smoke-polluted latitudinal Antarctic belt from 70–80∘ S.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Disentangling the chemistry and transport impacts of the quasi-biennial oscillation on stratospheric ozone

The quasi-biennial oscillation (QBO) in tropical winds perturbs stratospheric ozone throughout much of the atmosphere via changes in transport of ozone and other trace gases, as well as via temperature changes, both of which alter ozone chemistry. Attributing these causes of QBO–ozone variability may provide insights into model-to-model differences that contribute to ozone simulation. Here we develop a novel metric of steady-state ozone (SSO) to separate these effects: SSO calculates the local steady-state response of ozone due to the changes in temperature, chemical species, and overhead ozone column; the response due to circulation change is presumed when SSO shows no response. It is applied to the nudged Department of Energy's Energy Exascale Earth System Model version 2 (E3SMv2) with interactive ozone chemistry to demonstrate its validity. The E3SMv2 simulations nudged to reanalysis data produced reasonable wind and ozone patterns, especially in the tropics. Consistent with previous studies, we find clear demarcations with pressure. Ozone perturbations in the upper stratosphere (<6 hPa) are predicted by temperature changes; those between 6 and 20 hPa are predicted by NO y changes, and those in the lower stratosphere show no temperature or NO y response and are presumably driven by circulation changes. These results are important for diagnosing model-to-model discrepancy in QBO–ozone response and enhancing the reliability of ozone projections.

Xie, Jinbo [Lawrence Livermore National Laboratory↗
DOE OSTI2022

Quantifying contributions of ozone changes to global and arctic warming during the second half of the twentieth century

Ozone is the third most important greenhouse gas in driving global warming, mainly due to increased tropospheric ozone. About 50% of the growth of global tropospheric ozone since preindustrial time occurred during 1955–2005, with continued growth since then. Furthermore, this study quantifies the relative contributions of ozone changes during 1955–2005 to total observed global and Arctic climate changes by comparing CESM1 historical simulations with all anthropogenic and natural radiative forcings including realistic ozone changes, and with the same forcings except with constant ozone or well-mixed greenhouse gases (WMGHG). Results indicate that ozone changes during 1955–2005 have strongly enhanced the downwelling longwave flux and increased net shortwave flux at the surface, and thus significantly contributed about 0.15 °C of global mean surface warming, roughly 21%, 26% and 16% of the observed, all-forcing and WMGHG-driven trends, respectively. In the Arctic in the same period, corresponding ozone-driven warming was about 0.63 °C, roughly 48%, 40% and 25% of the same three trends. During 1979–2005, these ozone changes have markedly added about 0.25 × 10 6 km 2 to the decrease in the Arctic sea ice extent (SIE), or roughly 25%, 48%, and 40% of the same three trends. Considering that the ozone-driven radiative forcing of about 0.22 (0.06) W·m –2 in 1955–2005 (1979–2005) was about 12% (6%) of the corresponding WMGHG forcing, ozone changes had contributed disproportionately to global and Arctic warming and Arctic sea ice decline during the second half of the twentieth century. Tropospheric ozone has shown relatively steady growth since 2006 and might have significantly contributed recent observed warming over the global and the Arctic.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

The contribution of the neuroendocrine system to adaption after repeated daily ozone exposure in rats

Ozone-induced lung injury/inflammation dissipates despite continued exposure for 3 or more days; however, the mechanisms of adaptation/habituation remain unclear. Since ozone effects are mediated through adrenal-derived stress hormones, which also regulate longevity of centrally-mediated stress response, we hypothesized that ozone-adaptation is linked to diminution of neuroendocrine stress-axes activation and glucocorticoid levels. Male Wistar-Kyoto-rats (12-week-old) were injected with vehicle or a therapeutically-relevant dexamethasone dose (0.01-mg/kg/day; intraperitoneal) for 1-month to determine if suppression of glucocorticoid signaling was linked to adaptation. Vehicle- and dexamethasone-treated rats were exposed to air or 0.8-ppm ozone, 4 h/day × 2 or 4 days to assess the impacts of acute exposure and adaptation, respectively. Dexamethasone reduced thymus and spleen weights, circulating lymphocytes, corticosterone and increased insulin. Ozone increased lavage-fluid protein and neutrophils and decreased circulating lymphocytes at day-2 but not day-4. Ozone-induced hyperglycemia, glucose intolerance and inhibition of beta-cell insulin release occurred at day-1 but not day-3. Ozone depleted circulating prolactin, thyroid-stimulating hormone, and luteinizing-hormone at day-2 but not day-4, suggesting central mediation of adaptation. Adrenal epinephrine biosynthesis gene, Pnmt, was up-regulated after ozone exposure at both timepoints. However, genes involved in glucocorticoid biosynthesis were up-regulated after day-2 but not day-4, suggesting that acute 1- or 2-day ozone-mediated glucocorticoid increase elicits feedback inhibition to dampen hypothalamic stimulation of ACTH release in response to repeated subsequent ozone exposures. Although dexamethasone pretreatment affected circulating insulin, lymphocytes and adrenal genes, it had modest effect on ozone adaptation. In conclusion, ozone adaptation likely involves lack of hypothalamic response due to reduced availability of circulating glucocorticoids.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2022

Disentangling the mechanism of temperature and water vapor modulation on ozone under a warming climate

Temperature and water vapor have been considered as important factors affecting ozone concentrations, however, their synergistic effect on ozone, as well as its response to a warming climate remains unclear. Here, numerical experiments with different combinations of climate and emissions highlighted opposite changes of annual ozone over the contiguous U.S. under scenarios with high vs. low ozone precursor emissions in the future with warming. Comparing the occurrence of heat waves on higher vs. lower ozone days, we found significant suppression of the heat wave exacerbation of ozone by anthropogenic emissions reductions. Variations of ozone with temperature (T) and water vapor (Q) over the western U.S. and southeastern U.S. in the simulations are clearly revealed through the construction of an O 3 -T-Q diagram. Based on the diagram, we further identified a T-dominant regime at higher temperatures where ozone increases with temperature increase, and a Q-dominant regime at lower temperatures where ozone decreases with temperature increase due to the negative effect of water vapor. With larger anthropogenic emission reductions, ozone may increase at a lower rate with temperature in the T-dominant regime, or even decrease with temperature in the Q-dominant regime. Our results show that with large emission reductions, substantial ozone pollution due to warming and increasing heat waves may be counteracted by water vapor, partly turning the ‘climate penalty’ on ozone into ‘climate benefit’. Hence controlling anthropogenic emissions may be an increasingly important strategy in a warmer and wetter climate to improve air quality and public health.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

The Role and Lifetime of Dissociative Heterogeneous Processes in Improving Simulated Ozone on Mars

Abstract Ozone simulated in Mars Global Climate Models (MGCMs) is used to assess the underlying chemistry occurring in the atmosphere. Currently, ozone total column abundance (TCA) is under‐predicted in MGCMs by up to 120%, implying missing or inaccurate chemistry in models. Heterogeneous reactions of hydroxyl radicals (HO X ) have been offered as an explanation for some of this bias, because they cause ozone to increase at locations where it's currently under‐predicted. We use four simulations to compare modeled ozone TCA with observations from the UVIS spectrometer aboard the ExoMars Trace Gas Orbiter to improve the representation of heterogeneous processes and their impact on ozone. We use a gas‐phase only run, a dissociative scheme, an adsorbed HO X retention scheme, and a hybrid scheme that combines the dissociative mechanism with the retention of HO X on water ice. We find retention of HO X is dependent on water ice sublimation, and ozone abundance increases when water ice persists for longer periods (1–20 sols). Over time, the loss of HO X causes a depletion in H 2 O 2 concentration (HO X reservoir), and thus allows ozone concentration to increase. When adsorbed HO X are desorbed and dissociate into other by‐products, HO X are not immediately available to destroy ozone. This results in larger ozone concentrations than if desorbed HO X are released directly back into their gaseous states. When using the hybrid scheme, ozone TCA is increased up to 50% where the ozone deficit is greatest, demonstrating the best agreement with observations, and implying that HO X radicals are both retained when adsorbed and dissociate.

Brown, M. A. J.↗
DOE OSTI2024

Unique impacts of strong and westward-extended western Pacific subtropical high on ozone pollution over eastern China

As a subtropical anticyclonic high-pressure system that typically forms over the northwestern Pacific Ocean in summer, the Western Pacific subtropical high (WPSH) affects meteorological conditions and ozone pollution in China. The relationship between maximum daily 8-h average ozone (MDA8 O 3 ) concentrations and the extremely strong and westward-extended WPSH occurred in 2022 is investigated using observations, reanalysis data and GEOS-Chem model simulations. The intensity of WPSH has a significant positive correlation with MDA8 O3 over southern China during July-August in 2022, with a correlation coefficient of +0.44, but the correlation is negative (–0.40) in northern China. During the strong WPSH days, MDA8 O 3 increased by 16.5µgm -3 (16.4% relative to July-August average) over southern China and decreased by 19.0µgm -3 (14.5%) in northern China compared to the weak WPSH days. The unique dipole pattern in the relationship between ozone levels and the WPSH in 2022 exhibited a contrast to that during 2015–2021. The difference is primarily due to the extremely strong WPSH intensity and its unusual westward expansion in 2022. In this case, an anomalous anticyclone at 500 hPa dominates over southern China, which creates conditions conducive for ozone formation and accumulation. The anticyclone weakened horizontal winds and reduced the dispersion of ozone, alongside a high temperature and low relative humidity, which favored the chemical production of ozone. In contrast, abnormal northerly winds enhanced ozone diffusion in northern China and the low temperature reduced ozone chemical production. Here, this study reveals the mechanism for the significant impact of strong and westward-extended WPSH on ozone concentrations over China, emphasizing the role of the WPSH location in modulating meteorology and ozone levels.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Ozonized biochar filtrate effects on the growth of Pseudomonas putida and cyanobacteria Synechococcus elongatus PCC 7942

Background: Biochar ozonization was previously shown to dramatically increase its cation exchange capacity, thus improving its nutrient retention capacity. The potential soil application of ozonized biochar warrants the need for a toxicity study that investigates its effects on microorganisms. Results: In the study presented here, we found that the filtrates collected from ozonized pine 400 biochar and ozonized rogue biochar did not have any inhibitory effects on the soil environmental bacteria Pseudomonas putida, even at high dissolved organic carbon (DOC) concentrations of 300 ppm. However, the growth of Synechococcus elongatus PCC 7942 was inhibited by the ozonized biochar filtrates at DOC concentrations greater than 75 ppm. Further tests showed the presence of some potential inhibitory compounds (terephthalic acid and p-toluic acid) in the filtrate of non-ozonized pine 400 biochar; these compounds were greatly reduced upon wet-ozonization of the biochar material. Nutrient detection tests also showed that dry-ozonization of rogue biochar enhanced the availability of nitrate and phosphate in its filtrate, a property that may be desirable for soil application. Conclusion: Ozonized biochar substances can support soil environmental bacterium Pseudomonas putida growth, since ozonization detoxifies the potential inhibitory aromatic molecules.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2023

Contrasting changes in ozone during 2019–2021 between eastern and the other regions of China attributed to anthropogenic emissions and meteorological conditions

Ozone pollution is one of the most severe air quality issues in China that poses a serious threat to human health and ecosystems. During 2019–2021, the maximum daily 8-h average ozone concentrations in eastern China (110–122.5°E, 26–42°N) and the rest of China (ROC) show different decreasing patterns, with ozone concentrations in eastern China decreasing by 14.9 μg/m 3 , which is much larger than 4.8 μg/m 3 in ROC. Here, based on two independent methods, the atmospheric chemical transport model (GEOS-Chem) simulations and the machine learning (ML) model (LightGBM) predictions, the reasons for the differences in ozone changes between eastern China and ROC during the warm season (April to September) are investigated. According to the GEOS-Chem (LightGBM) results, changes in the meteorological conditions contributed to an ozone decrease by 7.3 (6.8) μg/m 3 in eastern China due to decreased chemical production and an ozone decrease by 6.8 (7.0) μg/m 3 in ROC attributed to the weakened horizontal and vertical advection. With the influence of meteorological factors excluded, the observations show that changes in anthropogenic emissions resulted in an ozone decrease by 7.6 (8.1) μg/m 3 in eastern China and an ozone increase by 2.0 (2.2) μg/m 3 in ROC, which is primarily induced by the changes in NO x emissions. The surface measurements and satellite retrievals also indicate that the reduction in NO x emissions in ROC is less efficient than that in the more developed eastern China, leading to contrasting changes in ozone concentrations between eastern China and ROC during 2019–2021. In conclusion, our results highlight the critical need to reduce ozone precursor emissions in the rest regions of China apart from eastern China.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Comparing the Effect of Anthropogenically Amplified Halogen Natural Emissions on Tropospheric Ozone Chemistry Between Pre-Industrial and Present-Day

Reactive halogens (X + XO, X = I, Br or Cl) catalytically destroy a fraction of tropospheric ozone under present-day (PD) conditions, however, their distribution and potential impact on tropospheric ozone under pre-industrial (PI) conditions remain largely unexplored. This study uses the Community Atmosphere Model with Chemistry (CAM-Chem) to investigate the effect of anthropogenically amplified natural emissions of halogenated species and their subsequent chemistry on tropospheric ozone under PI and PD atmospheric conditions. Model results show that the global tropospheric ozone depletion due to natural halogens is slightly more sensitive in PI than PD, with percentage changes in tropospheric ozone burden (TOB) of -14.1 ± 0.6% for PI and -12.9 ± 0.6% for PD. Individually, the role of iodine and chlorine in ozone depletion is equivalent in both periods (ΔTOB I : ~-7% and ΔTOB Cl : ~-2.5%), while bromine plays a larger role in PI (ΔTOB Br : -5.5 ± 0.6%) versus PD (ΔTOB Br : -4.3 ± 0.7%). The increase in anthropogenic ozone precursor emissions from PI to PD has amplified the natural emission of inorganic halogens and led to a shift in the partitioning of inorganic halogens from reactive to reservoir species. Consequently, halogen-driven ozone depletion from the surface to the free troposphere is larger in PI than PD. In contrast, in the upper troposphere, the ozone depletion is larger in PD influenced mainly by stratospheric intrusion of reactive halogens from long-lived species. This study highlights the importance of including a complete chemical coupling of natural halogens and atmospheric pollutants in chemistry-climate models to adequately assess their effects on tropospheric ozone in a changing climate.

54 ENVIRONMENTAL SCIENCES↗