Origins of formaldehyde in a mountainous background atmosphere of southern China.

Formaldehyde (HCHO) is one of the key indicators of severe photochemical pollution and strong atmospheric oxidation capacity in southern China. However, current information on the origins of regional HCHO and the impacts of polluted air masses remains scarce and unclear. In this study, an intensive observation of HCHO was conducted at a mountainous background site in southern China during typical photochemical pollution episodes. The concentrations of HCHO reached up to 6.14 ppbv and averaged at 2.68 ± 1.11 ppbv. Source appointment using a photochemical age-based parameterization method revealed significant contributions of secondary formation (50 %) and biomass burning (42 %). Meanwhile, under the influence of the East Asian Winter Monsoon, polluted air masses from central and western China can significantly increase the regional HCHO levels. The simulation results adopting the Rapid Adaptive Optimization Model for Atmospheric Chemistry model further demonstrated that the intrusion of active anthropogenic pollutants (e.g., small-molecule alkenes) can accelerate the net production rate of HCHO, particularly through BVOC-oxidation pathways. This study suggests a potential enhanced mechanism of HCHO production resulting from anthropogenic-biogenic interactions. It highlights that polluted air masses carrying abundant HCHO from upwind areas may facilitate severe photochemical pollution in the Greater Bay Area.

Underestimated contribution of open biomass burning to terpenoid emissions revealed by a novel hourly dynamic inventory.

Terpenoids play a crucial role in atmospheric chemistry, contributing significantly to the formation of ozone and secondary organic aerosol. However, the accurate quantification of terpenoid emissions from biomass burning is currently lacking, leading to underestimated air quality impacts. This study developed a near real-time hourly open biomass burning (OBB) emission inventory named OBEIC, which incorporated geostationary and polar-orbiting satellite fire radiative power. The OBEIC inventory provided emission estimates of 69 terpenoids, categorized into four groups, at an hourly resolution. Monoterpenes were the dominant contributors to the total emissions, accounting for 58 % of the total terpenoid emissions from OBB. Notably, only 24 % of the total monoterpenes emitted from OBB were accounted for by α-pinene and ß-pinene, indicating the importance of quantifying emissions of other monoterpene species such as limonene and camphene. Additionally, oxygenated terpenoids, which were previously overlooked, contribute to 20 % of total terpenoid emissions from OBB. Diurnally, the emissions of terpenoids were primarily concentrated during the daytime (61 %); however, this study revealed the significance of nighttime emissions (39 %) as well. When compared to the biogenic and anthropogenic emissions, OBB made substantial contributions to nighttime isoprene (99.8 %), monoterpene (66.8 %), and sesquiterpene (61.7 %) emissions where OBB occurs (in 3 km range), suggesting its significant role in nighttime secondary pollutant formation. The methodology developed in this study has the potential to reduce uncertainties in OBB emissions estimation.

Photochemical loss with consequential underestimation in active VOCs and corresponding secondary pollutions in a petrochemical refinery, China.

The photochemical loss of volatile organic compounds (VOCs) significantly alters the capturing source profiles in high-reactivity VOC species and results in an underestimation of secondary pollutants such as ozone (O3) and secondary organic aerosol (SOA). Utilising speciated VOC data from large petrochemical refineries, the research assesses the photochemical loss of various VOC species. Air samples from multiple sites revealed over 99 VOCs, with initial concentrations estimated via a photochemical age-based parameterisation method. The comparative analysis of initial and measured VOC values provided insights into the VOCs' photochemical degradation during transport. Findings highlight that the average photochemical loss of total VOCs (TVOCs) across different refinery process areas varied between 4.9 and 506.8 ppb, averaging 187.5 ± 128.7 ppb. Alkenes dominated the consumed VOCs at 83.1 %, followed by aromatic hydrocarbons (9.3 %), alkanes (6.1 %), and oxygenated VOCs (OVOCs) at 1.6 %. The average consumption-based ozone formation potential (OFP) and SOA formation potential (SOAP) were calculated at 1767.3 ± 1251.1 ppb and 2959.6 ± 2386.3 ppb, respectively. Alkenes, primarily isoprene, 1,3-butadiene, and acetylene, were the most significant contributors to OFP, ranging from 19.9 % to 95.5 %. Aromatic hydrocarbons, predominantly monocyclic aromatics like toluene, xylene, styrene, and n-dodecane, were the primary contributors to SOAP, accounting for 5.0 % to 81.3 %. This research underscores the significance of considering photochemical losses in VOCs for accurate secondary pollution assessment, particularly in high-reactivity VOC species. It also provides new detection methods and accurate data for the characterization, source analysis and chemical conversion of volatile organic compounds in the petroleum refining industry.

Sources of elevated organic acids in the mountainous background atmosphere of southern China.

Formic acid (FA) and acetic acid (AA) are pivotal organic acids in the troposphere, significantly influencing atmospheric chemistry. However, their abundance and sources in the mountainous background atmosphere remain underexplored. We undertook continuous measurements of FA and AA in Nanling mountains, southern China, during autumn 2020 using a high-resolution time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS). Both acids registered higher concentrations than in other global high-altitude or forested locations, averaging at 0.89 (max: 3.91) and 0.95 (max: 3.52) ppbv for FA and AA, respectively. High concentrations of FA and AA in this forested background area arose from secondary formation and biomass burning, collectively contributing 71 % to 89 %. During episodes, FA and AA concentrations surged 2-3 times, owing to the enhanced atmospheric oxidation capacity. The secondary FA production was predominantly due to isoprene oxidation among the VOC precursors studied. However, observed inconsistencies between calculated and actual FA concentrations suggest overlooked precursors or mechanisms warranting further investigation. Our findings can enhance the understanding of organic acid characteristics and the interplay of biogenic and anthropogenic sources in the background atmosphere.

Emission characteristics of carbonyl compounds from open burning of typical subtropical biomass in South China.

Open biomass burning (OBB) is one of the largest primary emission sources for atmospheric carbonyl compounds, key precursors for ozone and secondary organic aerosol pollution. To clarify the carbonyl emissions, the comprehensive characteristics of C1-C10 carbonyl compounds from open burning of seven typical subtropical biomass in China were investigated in this study, which included subtropical plants and agricultural residues. Total 27 carbonyl compounds were detected. The total EFs were 2824 mg kg-1 with 95% confidence interval (CI) [2418, 3322] for burning subtropical plants and 4080 mg kg-1 with 95% CI [3446, 4724] for burning agriculture residues, respectively. The EFs were 2-3 orders of magnitude larger than previous values in China. Aliphatic aldehydes were the largest group of carbonyl groups, with acetaldehyde, as the most abundant carbonyl species (about 30% contribution). Formaldehyde, acetone, acrolein, glyoxal, methylglyoxal, butanone, isovaleraldehyde, and m-tolualdehyde were also found to be abundant and varying with the types of biomass burnt. Formaldehyde emission ratios to acetonitrile and CO were lower than those in previous studies both for burning plants and agricultural residues. There were significant variabilities in the emission ratios and factors among different types of OBBs. Strong positive correlations were found between carbonyl emissions and CO emissions and water content in biomass; furthermore, total carbonyl concentrations measured in the flaming stage were higher than those in the smoldering one. This study provides important fundamental measurement data on carbonyl emissions from burning typical subtropical plants and agricultural residues, which will help improve the quality of emission inventories and better understand the potential impacts of OBB on regional air quality in southern China.

The anthropogenic effects on organic matter in sediment core based on Bayesian mixing model: a case study of Daya Bay.

Sediment is an important carrier of evidence about environmental evolution which receives huge volumes of organic material originated from both anthropogenic and natural sources. In this study, based on sedimentary chronology, the vertical trends of particle size distribution, total organic carbon (TOC), total nitrogen (TN), and their stable isotopes (δ13C, δ15N) in the sediment core of the nuclear power sea in southwest Daya Bay were analyzed, and the distribution characteristics and contribution ratios of different sources of organic matter in the sedimentary environment over the past 70 years were resolved using a Bayesian mixing model (MixSIAR). TOC, TN, δ13C, and δ15N ranged from 0.89 to 1.56%, 0.09 to 0.2%, - 22.3 to - 20.6‰, and 4.38 to 6.51‰, respectively. The organic matter in the sediment is controlled by a mixture of terrestrial input and marine autochthonous, the proportion of organic matter from terrestrial sources increases, while that from marine sources decreases in the sediment core, which persists from 1960 to 2000, yet organic matter from marine sources still dominates. The first signs of increased primary productivity occurred in 1960, and it was primarily due to agricultural activity. After the 1980s, the rapid increase in population around Daya Bay, the construction of nuclear power plants, the rise of aquaculture, and the quick expansion of industrial bases were all major factors that changed the ecological environment of Daya Bay.

Mortality Risk and Burden From a Spectrum of Causes in Relation to Size-Fractionated Particulate Matters: Time Series Analysis.

BACKGROUND: There is limited evidence regarding the adverse impact of particulate matters (PMs) on multiple body systems from both epidemiological and mechanistic studies. The association between size-fractionated PMs and mortality risk, as well as the burden of a whole spectrum of causes of death, remains poorly characterized. OBJECTIVE: We aimed to examine the wide range of susceptible diseases affected by different sizes of PMs. We also assessed the association between PMs with an aerodynamic diameter less than 1 µm (PM1), 2.5 µm (PM2.5), and 10 µm (PM10) and deaths from 36 causes in Guangzhou, China. METHODS: Daily data were obtained on cause-specific mortality, PMs, and meteorology from 2014 to 2016. A time-stratified case-crossover approach was applied to estimate the risk and burden of cause-specific mortality attributable to PMs after adjusting for potential confounding variables, such as long-term trend and seasonality, relative humidity, temperature, air pressure, and public holidays. Stratification analyses were further conducted to explore the potential modification effects of season and demographic characteristics (eg, gender and age). We also assessed the reduction in mortality achieved by meeting the new air quality guidelines set by the World Health Organization (WHO). RESULTS: Positive and monotonic associations were generally observed between PMs and mortality. For every 10 µg/m3 increase in 4-day moving average concentrations of PM1, PM2.5, and PM10, the risk of all-cause mortality increased by 2.00% (95% CI 1.08%-2.92%), 1.54% (95% CI 0.93%-2.16%), and 1.38% (95% CI 0.95%-1.82%), respectively. Significant effects of size-fractionated PMs were observed for deaths attributed to nonaccidental causes, cardiovascular disease, respiratory disease, neoplasms, chronic rheumatic heart diseases, hypertensive diseases, cerebrovascular diseases, stroke, influenza, and pneumonia. If daily concentrations of PM1, PM2.5, and PM10 reached the WHO target levels of 10, 15, and 45 µg/m3, 7921 (95% empirical CI [eCI] 4454-11,206), 8303 (95% eCI 5063-11,248), and 8326 (95% eCI 5980-10690) deaths could be prevented, respectively. The effect estimates of PMs were relatively higher during hot months, among female individuals, and among those aged 85 years and older, although the differences between subgroups were not statistically significant. CONCLUSIONS: We observed positive and monotonical exposure-response curves between PMs and deaths from several diseases. The effect of PM1 was stronger on mortality than that of PM2.5 and PM10. A substantial number of premature deaths could be preventable by adhering to the WHO's new guidelines for PMs. Our findings highlight the importance of a size-based strategy in controlling PMs and managing their health impact.

Tibetan Plateau is vulnerable to aromatic-related photochemical pollution and health threats: A case study in Lhasa.

Anthropogenic aromatics play a key role in photochemical pollution and pose a serious threat to human health. Current knowledge on source characteristics of aromatics in the urban region of the Tibetan Plateau (TP), the "Third Pole" and ecologically sensitive area, remains limited. In this study, an intensive observation of 17 aromatic hydrocarbons was conducted in Lhasa, the cultural and economic center of TP, during the second Tibetan Plateau Scientific Expedition and Research in summer 2020. The results showed that the average concentration of aromatics in Lhasa (7.6 ± 7.4 ppbv) was unexpectedly higher than those in megacities such as Beijing, Shanghai, and Guangzhou. Tripled concentrations and corresponding ozone formation potential during pollution episodes were recorded. Further source apportionment using positive matrix factorization revealed that solvent usage (60.0 %) was the dominant source, which may be due to the extremely low atmospheric pressure. Vehicle exhaust (15.4 %), industrial emissions (12.8 %), fuel evaporation (6.2 %), and burning emissions (5.7 %) were also important sources. The concentration weighted trajectory analysis revealed that the observed high levels of aromatics were mainly driven by local anthropogenic emissions, rather than the regional transport by the Indian summer monsoon. Long-term exposure to aromatics in Lhasa was assessed to pose carcinogenic risks to the population, with the risks of benzene and ethylbenzene 5 times the criteria. Our results suggest that, given the magnified emissions of aromatics in this extreme environment (low atmospheric pressure and strong solar radiation), the implementation of targeted pollution controls is urgently needed to mitigate the aromatic-related photochemical pollution and health threats in TP.

Anthropogenic pollutants induce enhancement of aerosol acidity at a mountainous background atmosphere in southern China.

Aerosol acidity plays a crucial role in atmospheric physicochemical processes, climate change and human health, particularly in the formation of secondary organic aerosols (SOA). However, understanding the characteristics and driving factors of aerosol acidity in background mountains has been limited. In this study, we conducted intensive field measurements in the Nanling mountains during the dry and wet seasons to analyze aerosol pH characteristics and their driving factors using sensitivity tests. The mean aerosol pH in the background mountains was found to be 2.68 ± 0.55, with values ranging from 0.38 to 4.44, significantly lower than predicted values in northern China. Sensitivity tests revealed that aerosol acidity in the background atmosphere was more responsive to dominant chemical species (T-NH3 (= NH4+ + NH3) and SO42-) rather than relative humidity and temperature. Additionally, we observed that sulfate and ammonium, transported occasionally by dryer northern air masses, had a substantial impact on decreasing aerosol pH at the site. Similar to the southeastern United States, NH4+/NH3 also dominated the total buffer capacity of aerosol acidity in the Nanling mountains. The strong aerosol acidity in this area is expected to have adverse effects on regional air quality and climate by enhancing SOA formation and regulating the dry deposition of inorganic reactive nitrogen.

A vehicle-mounted dual-smog chamber: Characterization and its preliminary application to evolutionary simulation of photochemical processes in a quasi-realistic atmosphere.

Smog chambers are the effective tools for studying formation mechanisms of air pollution. Simulations by traditional smog chambers differ to a large extent from real atmospheric conditions, including light, temperature and atmospheric composition. However, the existing parameters for mechanism interpretation are derived from the traditional smog chambers. To address the gap between the traditional laboratory simulations and the photochemistry in the real atmosphere, a vehicle-mounted indoor-outdoor dual-smog chamber (JNU-VMDSC) was developed, which can be quickly transferred to the desired sites to simulate quasi-realistic atmosphere simultaneously in both chambers using "local air". Multiple key parameters of the smog chamber were characterized in the study, demonstrating that JNU-VMDSC meets the requirements of general atmospheric chemistry simulation studies. Additionally, the preliminary results for the photochemical simulations of quasi-realistic atmospheres in Pearl River Delta region and Nanling Mountains are consistent with literature reports on the photochemistry in this region. JNU-VMDSC provides a convenient and reliable experimental device and means to study the mechanism of atmospheric photochemical reactions to obtain near-real results, and will make a great contribution to the control of composite air pollution.

High contribution of new particle formation to ultrafine particles in four seasons in an urban atmosphere in south China.

Ultra fine particles (UFP) cover the size range of both nucleation mode particles (NUC, Dp < 25 nm) and Aitken mode particles (AIT, 25 nm < Dp < 100 nm), and play important roles in radiative forcing and human health. In this study, we identified new particle formation (NPF) events and undefined events, explored their potential formation mechanism, and quantified their contributions to UFP number concentration (NUFP) in urban Dongguan of the Pearl River Delta (PRD) region. Field campaigns were carried out in four seasons in 2019 to measure particle number concentration in the size range of 4.7-673.2 nm, volatile organic compounds (VOCs), gaseous pollutants, chemical compositions in PM2.5, and meteorological parameters. The frequency of the occurrence of NPF, as indicated by a significant increase in NUC number concentration (NNUC), was 26 %, and that of the undefined event, as indicated by substantial increases in NNUC or AIT number concentration (NAIT), was 32 % during the whole campaign period. The NPF events mainly occurred in autumn (with a frequency of 59 %) and winter (33 %) and only occasionally in spring (4 %) and summer (4 %). On the contrary, the frequencies of the undefined events were higher in spring (52 %) and summer (38 %) than in autumn (19 %) and winter (22 %). The burst periods of the NPF events mainly occurred before 11:00 Local Time (LT), while those of the undefined events mainly occurred after 11:00 LT. Accompanied to NPF events were low concentrations of VOCs and high concentrations of O3. The undefined events by NUC or AIT were associated with the upwind transport of newly formed particles. Source apportionment analysis suggested that NPF and undefined events were the largest contributor to NNUC (51 ± 28 %), NAIT (41 ± 26 %), and NUFP (45 ± 27 %), while coal combustion and biomass burning, and traffic emission were the second largest contributor to NNUC (22 ± 20 %) and NAIT (39 ± 28 %), respectively.

Anthropogenic Pollutants Induce Changes in Peroxyacetyl Nitrate Formation Intensity and Pathways in a Mountainous Background Atmosphere in Southern China.

Mountainous background areas are typically considered to have a clean atmosphere where peroxyacetyl nitrate (PAN) can be decomposed. This study demonstrated that PAN was photochemically formed with a simulated production rate of 0.28 ± 0.06 ppbv h-1 in the Nanling mountains (1690 m a.s.l.) of South China and that net PAN formation was dependent on both volatile organic compounds (VOCs) and NOx precursors (transition regime). In contrast to dominated acetaldehyde oxidation in previous urban and rural research, PAN at Nanling was primarily formed by methylglyoxal (38%), acetaldehyde (28%), radicals (20%), and other oxygenated volatile organic compounds (OVOCs) (13%). Moreover, when polluted air masses invaded the Nanling mountains, the PAN production rate was altered, primarily because anthropogenic aromatics intensified PAN formation via the oxidized pathways of methylglyoxal, other OVOCs, and radicals. Finally, net PAN formation at Nanling reduced the hydroxyl radical level by consuming NOx, impaired local radical cycling, and thereby suppressed local O3 production. This suppressing effect was exacerbated on polluted days. The findings of this study deepen our understanding of PAN photochemistry and the impact of anthropogenic intrusions on the background atmosphere of mountainous regions.

Fine particulate pollution driven by nitrate in the moisture urban atmospheric environment in the Pearl River Delta region of south China.

To identify potential sources of fine particles (PM2.5, with aerodynamic diameter (Da) ≤ 2.5 µm) in urban Dongguan of south China, a comprehensive campaign was carried out in the whole 2019. Hourly PM2.5 and its dominant chemical components including organic carbon (OC), elemental carbon (EC), water-soluble inorganic ions (WSIIs) and thirteen elements were measured using online instruments. Gaseous pollutants including NH3, HNO3, NO2, NO and O3 and meteorological parameters were also synchronously measured. PM2.5 was dominated by carbonaceous aerosols in summer and by WSIIs in the other seasons. PM2.5 and its dominant chemical components mostly peaked around noon (10:00-14:00 LST). Furthermore, high PM2.5 levels during the daytime were closely related with the increased NO3- levels. The high mass concentrations of NO3- in urban Dongguan during the daytime were likely related with regional transport of NO3- from suburban Dongguan, which was originated from the reaction between NO2 and O3 under the moisture condition during the nighttime. Seven major source factors for PM2.5 including secondary sulfate, ship emission, traffic emission, secondary nitrate, industrial processes, soil dust and coal combustion were identified by positive matrix factorization (PMF) analysis, which contributed 26 ± 14%, 16 ± 16%, 16 ± 10%, 14 ± 11%, 12 ± 11%, 8 ± 6% and 8 ± 6%, respectively, to annual PM2.5 mass concentration. Although secondary sulfate contributed much more than secondary nitrate to PM2.5 on annual basis, the latter exceeded the former source factor when daily PM2.5 mass concentration was higher than 60 µg m-3, indicating the critical role nitrate played in PM2.5 episode events.

Atmospheric concentrations and sources of black carbon over tropical Australian waters.

Black carbon (BC) aerosols significantly contribute to radiative budgets globally, however their actual contributions remain poorly constrained in many under-sampled ocean regions. The tropical waters north of Australia are a part of the Indo-Pacific warm pool, regarded as a heat engine of global climate, and are in proximity to large terrestrial sources of BC aerosols such as fossil fuel emissions, and biomass burning emissions from northern Australia. Despite this, measurements of marine aerosols, especially BC remain elusive, leading to large uncertainties and discrepancies in current chemistry-climate models for this region. Here, we report the first comprehensive measurements of aerosol properties collected over the tropical warm pool in Australian waters during a voyage in late 2019. The non-marine related aerosol emissions observed in the Arafura Sea region were more intense than in the Timor Sea marine region, as the Arafura Sea was subject to greater continental outflows. The median equivalent BC (eBC) concentration in the Arafura Sea (0.66 µg m-3) was slightly higher than that in the Timor Sea (0.49 µg m-3). Source apportionment modelling and back trajectory analysis and tracer studies consistently suggest fossil fuel combustion eBC (eBCff) was the dominant contributor to eBC across the entire voyage region, with biomass burning eBC (eBCbb) making significant additional contributions to eBC in the Arafura Sea. eBCff (possibly from ship emissions or oil and gas rigs and their associated activities) and cloud condensation nuclei (CCN) were robustly correlated in the Timor Sea data, whereas eBCbb positively correlated to CCN in the Arafura Sea, suggesting different sources and atmospheric processing pathways occurred in these two regions. This work demonstrates the substantial impact that fossil fuel and biomass burning emissions can have on the composition of aerosols and cloud processes in the remote tropical marine atmosphere, and their potentially significant contribution to the radiative balance of the rapidly warming Indo-Pacific warm pool.

The effect of a single escalating dose of long-acting recombinant human follicle-stimulating hormone Fc fusion protein (KN015) on healthy, pituitary-suppressed women: first-in-human and randomized study on its pharmacokinetics, pharmacodynamics, and tolerability.

OBJECTIVE: KN015 is a long-acting, recombinant human follicle-stimulating hormone Fc fusion protein that induces follicle development. This first-in-human study evaluated the effect of KN015 on healthy, pituitary-suppressed women and examined its pharmacokinetics, pharmacodynamics, and tolerability. METHODS: This phase I study was a double-blind, randomized, and placebo-controlled design with a single ascending dose (20, 40, and 60 µg, respectively). RESULTS: After subcutaneous administration of a single dose, the maximum serum KN015 concentrations reached 1.57, 2.78, and 3.62 ng/mL, respectively, after baseline adjustment. Over this dose range, the median Tmax occurred at 240-312 h, and the half-life (t½) was 752-1160 h. Dose proportionality was shown across the studied dose range. In most subjects, follicular growth was observed, and the number and diameter of the follicles increased with an increasing dose. In the 40-µg and 60-µg groups, the mean numbers of follicles with a diameter of ≥17 mm were 3 and 4, respectively. There was no significant difference in adverse events between the KN015 and placebo groups. KN015 antibody was not detected in any of the dosage groups. CONCLUSION: The administration of a single ascending dose of KN015 was tolerated and able to induce follicular growth. TRIAL REGISTRATION: This trial is registered at the Chinese Clinical Trials website (http://www.chinadrugtrials.org.cn/index.html # CTR20160741) and ClinicalTrials.gov (https://clinicaltrials.gov/ # NCT03192527).

Anthropogenic impacts on the temporal variation of heavy metals in Daya Bay (South China).

A detailed study of a sediment core from Daya Bay (South China) has revealed three stages of heavy metal deposition over the past century. Prior to the 1980s, heavy metal concentrations were low with limited influence by human activities. From the 1980s to 2000, metal pollution intensified, and anthropogenic activities, such as oil and petrochemical industries, and fuel combustion, had the greatest direct influence on Hg, Ni, Pb, and Zn concentrations, whereas atmospheric deposition and mariculture were also contributors to the continued increase in Cr, Cu, Pb, Zn, and Ni. Since the year 2000, heavy metal concentration has declined and stabilized. It is noteworthy that anthropogenic input of Cu and Pb is ongoing and may result in a moderate pollution risk. Both modified pollution index (MPI) and modified ecological risk (MRI) consistently indicate that the ecological risk in terms of heavy metals in Daya Bay has remained moderate over the past 70 years.

Interactive Effects Between Temperature and PM2.5 on Mortality: A Study of Varying Coefficient Distributed Lag Model - Guangzhou, Guangdong Province, China, 2013-2020.

Introduction: There is a large body of epidemiological evidence showing significantly increased mortality risks from air pollution and temperature. However, findings on the modification of the association between air pollution and mortality by temperature are mixed. Methods: We used a varying coefficient distributed lag model to assess the complex interplay between air temperature and PM2.5 on daily mortality in Guangzhou City from 2013 to 2020, with the aim of establishing the PM2.5-mortality association at different temperatures and exploring synergetic mortality risks from PM2.5 and temperature on vulnerable populations. Results: We observed near-linear concentration-response associations between PM2.5 and mortality across different temperature levels. Each 10 µg/m³ increase of PM2.5 in low, medium, and high temperature strata was associated with increments of 0.73% [95% confidence interval (CI): 0.38%, 1.09%], 0.12% (95% CI: -0.27%, 0.52%), and 0.46% (95% CI: 0.11%, 0.81%) in non-accidental mortality, with a statistically significant difference between low and medium temperatures (P=0.02). There were significant modification effects of PM2.5 by low temperature for cardiovascular mortality and among individuals 75 years or older. Conclusions: Low temperatures may exacerbate physiological responses to short-term PM2.5 exposure in Guangzhou, China.

Open biomass burning emissions and their contribution to ambient formaldehyde in Guangdong province, China.

Formaldehyde (HCHO) plays a vital role in atmospheric chemistry and O3 formation. Open biomass burning (OBB) is considered to be an important source of HCHO; however, its quantitative contribution to ambient HCHO remains poorly understood due to the lack of reliable high-resolution emission inventories. In this study, a satellite-based method coupled with local emission factors was developed to estimate the hourly primary emissions of HCHO and volatile organic compound (VOC) precursors from OBB in Guangdong (GD) Province of southern China. Furthermore, the contribution of OBB to ambient HCHO was quantified using the Community Multi-scale Air Quality model. The results suggested that in average OBB emissions contributed 5293 tons of primary HCHO per year, accounting for ~14% of the total anthropogenic HCHO emissions in GD. The ambient HCHO concentration ranged from 0.3 ppbv to 8.7 ppbv during normal days, and from 8 ppbv to 45 ppbv in downwind area during OBB impacted days. The monthly contribution of OBB to local HCHO levels reached up to 50% at locations with frequent fires and over 70% during a forest fire event. Ambient HCHO was heavily affected by primary OBB emissions near the source region and by the oxidation of OBB-emitted VOCs in the downwind area. Secondary HCHO formation from OBB emissions was enhanced during photochemical pollution episodes, especially under conditions of high O3 and low NOx. OBB-emitted ethene was identified as the most important VOC precursor of HCHO and contributed to the formation of ~50% of the secondary HCHO. The HCHO formation potential of cropland fires was 26% higher than that of forest fires. Our results suggest that OBB can elevate ambient HCHO levels significantly. Thus, strict control policies on OBB should be implemented, especially for open burning agricultural residues in upwind areas on serious photochemical pollution days.

Rapid increase in atmospheric glyoxal and methylglyoxal concentrations in Lhasa, Tibetan Plateau: Potential sources and implications.

Glyoxal (Gly) and methylglyoxal (Mgly) are the intermediate products of several volatile organic compounds (VOCs) as well as the precursors of brown carbon and may play key roles in photochemical pollution and regional climate change in the Tibetan Plateau (TP). However, their sources and atmospheric behaviors in the TP remain unclear. During the second Tibetan Plateau Scientific Expedition and Research in the summer of 2020, the concentrations of Gly (0.40 ± 0.30 ppbv) and Mgly (0.57 ± 0.16 ppbv) observed in Lhasa, the most densely populated city in the TP, had increased by 20 and 15 times, respectively, compared to those measured a decade previously. Owing to the strong solar radiation, secondary formations are the dominant sources of both Gly (71%) and Mgly (62%) in Lhasa. In addition, primary anthropogenic sources also play important roles by emitting Gly and Mgly directly and providing abundant precursors (e.g., aromatics). During ozone pollution episodes, local anthropogenic sources (industries, vehicles, solvent usage, and combustion activities) contributed up to 41% and 45% in Gly and Mgly levels, respectively. During non-episode periods, anthropogenic emissions originating from the south of Himalayas also have non-negligible contributions. Our results suggest that in the previous decade, anthropogenic emissions have elevated the levels of Gly and Mgly in the TP dramatically. This study has important implications for understanding the impact of human activities on air quality and climate change in this ecologically fragile area.

Accelerated toluene degradation over forests around megacities in southern China.

Toluene is a typical anthropogenic pollutant that has profound impacts on air quality, climate change, and human health, but its sources and sinks over forests surrounding megacities remain unclear. The Nanling Mountains (NM) is a large subtropical forest and is adjacent to the Pearl River Delta (PRD) region, a well-known hotspot for toluene emissions in southern China. However, unexpectedly low toluene concentrations (0.16 ± 0.20 ppbv) were observed at a mountaintop site in NM during a typical photochemical period. A backward trajectory analysis categorized air masses received at the site into three groups, namely, air masses from the PRD, those from central China, and from clean areas. The results revealed more abundant toluene and its key oxidation products, for example, benzaldehyde in air masses mixed with urban plumes from the PRD. Furthermore, a more than three times faster degradation rate of toluene was found in this category of air masses, indicating more photochemical consumption in NM under PRD outflow disturbance. Compared to the categorized clean and central China plumes, the simulated OH peak level in the PRD plumes (15.8 ± 2.2 × 106 molecule cm-3) increased by approximately 30% and 55%, respectively, and was significantly higher than the reported values at other background sites worldwide. The degradation of toluene in the PRD plumes was most likely accelerated by increased atmospheric oxidative capacity, which was supported by isoprene ozonolysis reactions. Our results indicate that receptor forests around megacities are not only highly polluted by urban plumes, but also play key roles in environmental safety by accelerating the degradation rate of anthropogenic pollutants.