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1.
Sci Total Environ ; 925: 171488, 2024 May 15.
Article in English | MEDLINE | ID: mdl-38462000

ABSTRACT

This study addresses significant knowledge gaps in understanding the complex interplay between atmospheric chemistry and synoptic conditions. Using emerging machine learning techniques-Boosted Regression Trees (BRTs) and Random Forest (RF) models-we investigate the influence of synoptic conditions on pollutant levels. Several BRTs and RF models are developed to estimate surface concentrations of ozone (O3), nitrogen dioxide (NO2), and formaldehyde (HCHO). By considering a range of algorithmic structures and explanatory variables for each pollutant, the research aims to identify the most skillful predictive approaches and influential factors governing pollutant levels. The design seeks to highlight key determinants of concentration patterns without constraining the investigation to pre-defined model structures or explanatory variable sets. Introducing a novel methodology, Correlation Coefficient Differential Evaluation (C2DE), we quantitatively assess the influence of explanatory variables. C2DE reveals significant contributions from spatial variables (i.e., trajectory clusters at varying altitudes), formaldehyde to nitrogen dioxide ratio (FNR), and meteorological parameters. Specifically, spatial variables contribute approximately 28 % to O3 concentrations, while the FNR accounts for around 5.2-9.8 % of the overall influence. For NO2 and HCHO, spatial variables contribute around 26.5 % and 32.1 %, respectively. Moreover, when considering the combined influence of meteorological parameters, these collectively explain about 45.34 %, 35.31 %, and 45.41 % of the variations in O3, NO2, and HCHO concentrations, respectively. Thus, C2DE provides valuable insights into the relative contributions of these factors, aiding in the comprehensive evaluation of air quality dynamics. This underscores the need for a multifaceted approach to comprehending and effectively addressing air pollution before devising its control strategies.

2.
J Environ Sci (China) ; 141: 151-165, 2024 Jul.
Article in English | MEDLINE | ID: mdl-38408816

ABSTRACT

In this study, a hybrid model, the convolutional neural network-support vector regression model, was adopted to achieve prediction of the NO2 profile in Nanjing from January 2019 to March 2021. Given the sudden decline in NO2 in February 2020, the contribution of the Coronavirus Disease-19 (COVID-19) lockdown, Chinese New Year (CNY), and meteorological conditions to the reduction of NO2 was evaluated. NO2 vertical column densities (VCDs) from January to March 2020 decreased by 59.05% and 32.81%, relative to the same period in 2019 and 2021, respectively. During the period of 2020 COVID-19, the average NO2 VCDs were 50.50% and 29.96% lower than those during the pre-lockdown and post-lockdown periods, respectively. The NO2 volume mixing ratios (VMRs) during the 2020 COVID-19 lockdown significantly decreased below 400 m. The NO2 VMRs under the different wind fields were significantly lower during the lockdown period than during the pre-lockdown period. This phenomenon could be attributed to the 2020 COVID-19 lockdown. The NO2 VMRs before and after the CNY were significantly lower in 2020 than in 2019 and 2021 in the same period, which further proves that the decrease in NO2 in February 2020 was attributed to the COVID-19 lockdown. Pollution source analysis of an NO2 pollution episode during the lockdown period showed that the polluted air mass in the Beijing-Tianjin-Hebei was transported southwards under the action of the north wind, and the subsequent unfavorable meteorological conditions (local wind speed of < 2.0 m/sec) resulted in the accumulation of pollutants.


Subject(s)
Air Pollutants , Air Pollution , COVID-19 , Humans , COVID-19/epidemiology , Air Pollutants/analysis , Nitrogen Dioxide/analysis , Environmental Monitoring , Communicable Disease Control , Air Pollution/analysis , China/epidemiology , Particulate Matter/analysis
3.
Talanta ; 270: 125524, 2024 Apr 01.
Article in English | MEDLINE | ID: mdl-38128285

ABSTRACT

A newly constructed thermal dissociation cavity ring-down spectrometer (TD-CRDS) for the simultaneous measurement of ambient total peroxy nitrates (ΣPNs, RO2NO2), total alkyl nitrates (ΣANs, RONO2), and NO2 was presented in this work. ΣPNs and ΣANs were detected as NO2 with the CRDS instrument after thermal dissociation. PNs and ANs completely dissociated at 180 °C and 360 °C, with conversion efficiencies of 96 % and 99 %, respectively. The effects of NO2 and NO on measurement in different temperatures and two types of thermal dissociation inlet (TDI) were further explored. The influence of ambient NO2 and NO on PNs and ANs in the improved TDI (TDI-2) was significantly improved. To further enhance the measurement accuracy, the consistency of the observed NO2 in the three channels was tested, which achieved good agreement. The detection limits of the TD-CRDS instrument for NO2, ΣPNs, and ΣANs were determined as 6.5, 6.8, and 8.6 pptv (10 s, 1σ), respectively. Observations of PNs and ANs were conducted in a suburban site in Hefei, China, from September 2-30, 2021, using the TD-CRDS instrument, and the consecutive time series of PNs and ANs were derived, verifying the capability of the TD-CRDS instrument for continuous field observations of ΣPNs and ΣANs.

4.
Sensors (Basel) ; 23(12)2023 Jun 16.
Article in English | MEDLINE | ID: mdl-37420809

ABSTRACT

Formaldehyde (HCHO) is a tracer of volatile organic compounds (VOCs), and its concentration has gradually decreased with the reduction in VOC emissions in recent years, which puts forward higher requirements for the detection of trace HCHO. Therefore, a quantum cascade laser (QCL) with a central excitation wavelength of 5.68 µm was applied to detect the trace HCHO under an effective absorption optical pathlength of 67 m. An improved, dual-incidence multi-pass cell, with a simple structure and easy adjustment, was designed to further improve the absorption optical pathlength of the gas. The instrument detection sensitivity of 28 pptv (1σ) was achieved within a 40 s response time. The experimental results show that the developed HCHO detection system is almost unaffected by the cross interference of common atmospheric gases and the change of ambient humidity. Additionally, the instrument was successfully deployed in a field campaign, and it delivered results that correlated well with those of a commercial instrument based on continuous wave cavity ring-down spectroscopy (R2 = 0.967), which indicates that the instrument has a good ability to monitor ambient trace HCHO in unattended continuous operation for long periods of time.


Subject(s)
Formaldehyde , Lasers, Semiconductor , Incidence , Gases , Spectrum Analysis
5.
Sci Total Environ ; 901: 165828, 2023 Nov 25.
Article in English | MEDLINE | ID: mdl-37506914

ABSTRACT

Air pollutants represent an environmental and health risk, and the methods for their effective assessment are of the greatest importance. The MAX-DOAS method is a reliable retrieval algorithm, enabling a vertical gas profile analysis. However, the current MAX-DOAS retrieval algorithm heavily relies on the a priori profile, limiting its accuracy. To address this issue, we introduced a novel MAX-DOAS trace gas profile inversion algorithm called McPrA, which is less dependent on the a priori profile. It employs the Monte Carlo method to resolve the problem of optimal estimation of trace gases. The gas vertical column density is obtained from the air mass factor calculated by SCIATRAN. Afterward, the trace gas vertical distribution is retrieved by combining the weight function with the a priori profile. A normalization process is also included to improve the matching of the weight function and the a priori profile. The McPrA algorithm enables greater flexibility in grid modification to achieve a higher vertical resolution of up to 50 m, while sensitivity experiments contribute to determining the optimal configuration of retrieval parameters, with a degree of freedom of over 3.0. Comparative verification experiments indicate that the McPrA algorithm accurately retrieves gas profiles, with a correlation coefficient of over 0.89 for NO2 in the first layer compared to in situ data. Furthermore, comparisons with WRF-Chem and the simulation of synthetic data demonstrate the effectiveness of the McPrA algorithm in accurately retrieving gas profiles.

6.
Opt Express ; 31(2): 2602-2620, 2023 Jan 16.
Article in English | MEDLINE | ID: mdl-36785270

ABSTRACT

This paper investigates a method for measuring SO2 concentration using Fabry-Perot interferometer correlation spectroscopy. In this method, the experimental system is designed as a separated beam, with the beam entering the F-P cavity at two incidence angles simultaneously to match the peak and valley positions of the SO2 absorption cross-section. The system achieves a 2σ detection limit of 28.2 ppm·m(15 cm) at a sampling frequency of 10 Hz. An outfield comparison experiment with the differential optical absorption spectroscopy method shows good agreement for the simultaneous measurement of SO2 concentration from sulfur combustion, with a correlation coefficient of R2 = 0.93. This study introduces a non-dispersive, highly accurate, and fast gas detection technique.

7.
J Environ Sci (China) ; 123: 235-254, 2023 Jan.
Article in English | MEDLINE | ID: mdl-36521987

ABSTRACT

Abrupt air pollution accidents can endanger people's health and destroy the local ecological environment. The appropriate emergency response can minimize the harmful effects of accidents and protect people's lives and property. This paper provides an overview of the key emergency response technologies for abrupt air pollution accidents around the globe with emphasis on the major achievements that China has obtained in recent years. With decades of effort, China has made significant progress in emergency monitoring technologies and equipment, source estimation technologies, pollutant dispersion simulation technologies and others. Many effective domestic emergency monitoring instruments (e.g., portable DOAS/FT-IR systems, portable FID/PID systems, portable GC-MS systems, scanning imaging remote sensing systems, and emergency monitoring vehicles) had been developed which can meet the demands for routine emergency response activities. A monitoring layout technique combining air dispersion simulation, fuzzy comprehensive evaluation, and a post-optimality analysis was proposed to identify the optimal monitoring layout scheme under the constraints of limited monitoring resources. Multiple source estimation technologies, including the forward method and the inversion method, have been established and evaluated under various scenarios. Multi-scale dynamic pollution dispersion simulation systems with high temporal and spatial resolution were further developed. A comprehensive emergency response platform integrating database support, source estimation, monitoring schemes, fast monitoring of pollutants, pollution predictions and risk assessment was developed based on the technical idea of "source identification - model simulation - environmental monitoring" dynamic interactive feedback. It is expected that the emergency response capability for abrupt air pollution accidents will gradually improve in China.


Subject(s)
Air Pollutants , Air Pollution , Environmental Pollutants , Humans , Spectroscopy, Fourier Transform Infrared , Air Pollution/analysis , Environmental Monitoring/methods , Accidents , China , Air Pollutants/analysis
8.
J Environ Sci (China) ; 123: 41-53, 2023 Jan.
Article in English | MEDLINE | ID: mdl-36522002

ABSTRACT

Accurate monitoring of the atmospheric environment and its evolution are important for understanding the sources, chemical mechanisms, and transport processes of air pollution and carbon emissions in China, and for regulatory and control purposes. This study gives an overview of atmospheric environment monitoring technology and equipment in China and summarizes the major achievements obtained in recent years. China has made great progress in the development of atmospheric environment monitoring technology and equipment with decades of effort. The manufacturing level of atmospheric environment monitoring equipment and the quality of products have steadily improved, and a technical & production system that can meet the requirements of routine monitoring activities has been initiated. It is expected that domestic atmospheric environment monitoring technology and equipment will be able to meet future demands for routine monitoring activities in China and provide scientific assistance for addressing air pollution problems.


Subject(s)
Air Pollutants , Air Pollution , Environmental Monitoring , Air Pollution/prevention & control , Air Pollution/analysis , China , Technology , Air Pollutants/analysis
9.
Sci Total Environ ; 849: 157749, 2022 Nov 25.
Article in English | MEDLINE | ID: mdl-35926628

ABSTRACT

To explore the impact of open straw burning on air quality in the Yangtze River Delta (YRD) and surrounding areas, three key cities in the YRD, namely Hefei, Nanjing, and Shanghai, were selected to observe changes in aerosol characteristics. Based on Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) observations from May to June 2021, the spatial-temporal distribution and potential sources of aerosol were studied. During the observation period, aerosol optical depth (AOD) in Shanghai was 55.15 % and 29.50 % higher than that in Hefei and Nanjing, respectively. For Shanghai, aerosols accumulated at night, and the aerosol extinction could reach 1.3 km-1 in the morning. The aerosol variations in Hefei and Nanjing were consistent due to the relative conformity of the surrounding environmental conditions (R = 0.84). The vertical distribution of aerosol in all three cities had the same Gaussian shape. The aerosol lifted layers in Nanjing and Shanghai were higher than that in Hefei, with heights of 0.2-0.8 km and 0.2-0.6 km, respectively. The averaged aerosol extinctions for these two cities were 0.34 km-1 and 0.49 km-1, respectively. Pollution source analysis was conducted based on wind field trajectory, satellite observation, and model simulation, taking Hefei as the recipient. The results showed that western Shandong Province, northern Anhui Province, northern Jiangxi Province, central Jiangsu Province, and the central YRD were the most important aerosols sources for Hefei. The contributions of central and southern Jiangsu Province were significantly higher than those of other potential sources, with a WCWTAOD (Meteoinfo concentration weight trajectory) between 1.2 and 3.0. The influence of fine particles produced by open biomass burning inside the YRD was significantly higher than that outside the region (outside contribution: 36.6 %). Regarding the influence between YRD cities, more aerosols were transported from Shanghai to Hefei and Nanjing, with similar transport contributions between Nanjing and Hefei.


Subject(s)
Air Pollutants , Air Pollution , Aerosols/analysis , Air Pollutants/analysis , Air Pollution/analysis , China , Environmental Monitoring/methods , Particulate Matter/analysis , Seasons
10.
Sci Total Environ ; 838(Pt 1): 155924, 2022 Sep 10.
Article in English | MEDLINE | ID: mdl-35577098

ABSTRACT

Atmospheric oxidation is a driving force of complex air pollution, and accurate hydroxyl radical (OH) measurement is helpful in investigating the radical-cored photooxidation mechanism in the troposphere. A self-developed laser-induced fluorescence instrument by the Anhui Institute of Optics Fine Mechanics, Chinese Academy of Sciences (AIOFM-LIF), was able to measure OH concentration with high sensitivity and good time resolution, and a detection limit of 1.7 × 105 cm-3 (1σ, 30 s). A long-period, multi-level intercomparison of hydroxyl radical (OH) measurements between AIOFM-LIF and PKU-LIF (the Peking University laser-induced fluorescence system) was conducted in Chengdu, China. The measurement between two instruments was in excellent agreement in the 5-min time resolution. Linear regression analysis reported a linear slope of 0.96 with a 0.68 × 106 cm-3 offset, and the correlation coefficient R2 was 0.85. The overall linearity with only a slight offset indicated a negligible influence on OH measurement. No noticeable artifacts from ozonolysis were observed under the condition of high ozone and ozonolysis-related compound concentrations. In addition to the subtraction of background signal through wavelength modulation, the dynamic correction on ozone photolysis interference ensured high intercomparison quality in both relatively constant and rapidly varying periods. Based on the reliability of OHAIOFM and OHPKU, comparisons under different oxidation-related species (NOx, VOCs, O3, PM2.5) levels and typical scenarios (rich-BVOC and high-reactivity) were carried out to evaluate the performance under complex atmospheres. A slightly higher drift was observed in a certain scenario, but the general data variability due to environmental changes did not affect the measurement accuracy. The intercomparison demonstrated that both systems are able to achieve reliable OH data under typical conditions of complex atmospheric pollution in China. Additional improvements are necessary for future intercomparisons in order to enhance the confidence in OH detection accuracy.


Subject(s)
Air Pollutants , Air Pollution , Ozone , Air Pollutants/analysis , Air Pollution/analysis , Atmosphere/analysis , Humans , Hydroxyl Radical , Ozone/analysis , Reproducibility of Results
11.
J Environ Sci (China) ; 114: 297-307, 2022 Apr.
Article in English | MEDLINE | ID: mdl-35459493

ABSTRACT

To investigate nitrous acid (HONO) levels and potential HONO sources above crop rotation fields. The HONO fluxes were measured by the aerodynamic gradient (AG) method from 14 December 2019 to 2 January 2020 over an agricultural field in the Huaihe River Basin. The ambient HONO levels were measured at two different heights (0.15 and 1.5 m), showing a typical diurnal cycle with low daytime levels and high nighttime levels. The upward HONO fluxes were mostly observed during the day, whereas deposition dominated at night. The diurnal variation of HONO flux followed solar radiation, with a noontime maximum of 0.2 nmol/(m2∙sec). The average upward HONO flux of 0.06 ± 0.17 nmol/(m2∙sec) indicated that the agricultural field was a net source for atmospheric HONO. The higher HONO/NO2 ratio and NO2-to-HONO conversion rate close to the surface suggested that nocturnal HONO was formed and released near the ground. The unknown HONO source was derived from the daytime HONO budget analysis, with an average strength of 0.31 ppbV/hr at noontime. The surface HONO flux, which was highly correlated with the photolysis frequency J(NO2) (R2 = 0.925) and the product of J(NO2) × NO2 (R2 = 0.840), accounted for ∼23% of unknown daytime HONO source. The significant correlation between HONO fluxes and J(NO2) suggests a light-driven HONO formation mechanism responsible for the surface HONO flux during daytime.


Subject(s)
Nitrogen Dioxide , Rivers , China , Nitrogen Dioxide/analysis , Nitrous Acid/analysis , Photolysis
12.
J Environ Sci (China) ; 114: 376-390, 2022 Apr.
Article in English | MEDLINE | ID: mdl-35459501

ABSTRACT

Comprehensive observations of the nocturnal atmospheric oxidation of NO3 and N2O5 were conducted at a suburban site in Changzhou in the YRD using cavity ring-down spectroscopy (CRDS) from 27 May to 24 June, 2019. High concentrations of NO3 precursors were observed, and the nocturnal production rate of NO3 was determined to be 1.7 ± 1.2 ppbv/hr. However, the nighttime NO3 and N2O5 concentrations were relatively low, with maximum values of 17.7 and 304.7 pptv, respectively, illustrating the rapid loss of NO3 and N2O5. It was found that NO3 dominated the nighttime atmospheric oxidation, accounting for 50.7%, while O3 and OH only contributed 34.1% and 15.2%, respectively. For the reactions of NO3 with volatile organic compounds (VOCs), styrene was found to account for 60.3%, highlighting its dominant role in the NO3 reactivity. In general, the contributions of the reactions between NO3 and VOCs and the N2O5 uptake to NO3 loss were found to be about 39.5% and 60.5%, respectively, indicating that N2O5 uptake also played an important role in the loss of NO3 and N2O5, especially under the high humidity conditions in China. The formation of nitrate at night mainly originated from N2O5 uptake, and the maximum production rate of NO3- reached 6.5 ppbv/hr. The average NOx consumption rate via NO3 and N2O5 chemistry was found to be 0.4 ppbv/h, accounting for 47.9% of the total NOx removal. The predominant roles of NO3 and N2O5 in nitrate formation and NOx removal in the YRD region was highlighted in this study.


Subject(s)
Nitrates , Rivers , China , Environmental Monitoring , Nitrates/analysis , Nitrogen Oxides/chemistry
13.
Anal Chim Acta ; 1200: 339607, 2022 Apr 01.
Article in English | MEDLINE | ID: mdl-35256149

ABSTRACT

Constructing a highly sensitive and selective electrochemical interface is of great significance for the effective detection of Hg2+ in water and biological samples. Herein, Co3O4 nanopolyhedron (NP) anchored on nitrogen-doped reduced graphene oxide (N-RGO) is utilized as the electrode material for the detection of Hg2+ in the range of 0.1 µM-1.0 µM, with high sensitivity (1899.70 µA µM-1 cm-2) and low detection limits (0.03 µM) in natural water. Moreover, the Co3O4-NP/N-RGO modified electrode possesses reasonable anti-interference ability for Hg2+ in the presence of inorganic ions and glucose, which is the basis of its good response to trace Hg2+ in serum. Besides, combined with X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) calculations, the electron transfer tendency is revealed. Additionally, combined with the electron state density of Co-p, it is speculated that Co3+ is an optimum active site for catalytic reaction. The above results elucidate an electrochemically sensitive interface is constructed to realize the efficient detection of Hg2+, which provides some theoretical guidance for the development of electrochemical sensors.


Subject(s)
Graphite , Mercury , Cobalt , Electrochemical Techniques/methods , Graphite/chemistry , Oxides
14.
Angew Chem Int Ed Engl ; 61(21): e202201638, 2022 May 16.
Article in English | MEDLINE | ID: mdl-35275427

ABSTRACT

OH radicals in the air maintain the oxidizing power of the troposphere. A conventional view is that particulate matter (PM) in the atmosphere is a major sink of OH radicals, thereby lowering the oxidizing power of atmosphere in the event of high-level PM. By contrary, our joint experimental/theoretical study reveals a new mechanism for the generation of gaseous OH radicals by carbonaceous soot particles. We show that water and O2 react on carbonaceous surfaces and give rise to gaseous OH radicals under irradiation. With ample delocalized π electrons, carbonaceous surfaces enable the easy desorption of hydroxyl groups to produce gaseous OH radicals, evidenced by direct observation of the steady generation of OH radicals on a carbonaceous surface. Our results reveal a new chemical mechanism for the production of OH radicals.

15.
Natl Sci Rev ; 9(2): nwab103, 2022 Feb.
Article in English | MEDLINE | ID: mdl-35145701

ABSTRACT

Smog chamber experimental systems, which have been widely used in laboratory simulation for studying atmospheric processes, are comprehensively reviewed in this paper. The components, development history, main research topics and main achievements of smog chambers are introduced. Typical smog chambers in the world, including their volumes, wall materials, light sources and features, are summarized and compared. Key factors of smog chambers and their influences on the simulation of the atmospheric environment are discussed, including wall loss, wall emission and background pollutants. The features of next-generation smog chambers and their application prospect in future studies of the atmospheric environment are also outlined in this paper.

16.
Sci Total Environ ; 823: 153425, 2022 Jun 01.
Article in English | MEDLINE | ID: mdl-35090930

ABSTRACT

The research on the mechanism of combined air pollution in the Yangtze-Huaihe region, which is characterized by unique meteorological and geographical conditions and pollution emission characteristics, is still insufficient. We performed an experiment on key pollutants and an ozone formation study in Hefei, which is a pivotal city in the Yangtze-Huaihe region, from September 1 to 20, 2020. The aerosols retrieved via two-dimensional Multi-axis Differential Optical Absorption Spectroscopy (2D-MAX-DOAS) with a Boltzmann-shaped a priori profile had the best agreement with the results of Light Detection and Ranging (LIDAR) and sun-photometer measurements among the three typical a priori profiles (Gaussian, Boltzmann, and exponential shapes). The correlation coefficients of the near-surface gas concentrations retrieved using both 2D-MAX-DOAS and in situ measurements were 0.86 (NO2) and 0.61 (HCHO). The high NO2 and HCHO concentrations were observed at azimuths of 180° and 315° at heights of 0.8-1.5 km, and they may have been emitted by aircrafts. Importantly, the ratio of HCHO to NO2 during a typical pollution episode revealed that the factors controlling the O3 formation changed with altitude: VOCs (surface) to NOx (0.4 km) to transition (1.0 km) to VOCs (1.6 km). Moreover, the effect of VOCs on the O3 generation was stronger than that of NOx, especially in the downtown area of Hefei. When the ratio of HCHO to NO2 was 3.55-7.46, the ozone concentration in Hefei could be controlled well, especially at the optimal value of 5.50.


Subject(s)
Air Pollutants , Ozone , Air Pollutants/analysis , China , Environmental Monitoring/methods , Nitrogen Dioxide/analysis , Ozone/analysis
17.
Sci Total Environ ; 804: 149680, 2022 Jan 15.
Article in English | MEDLINE | ID: mdl-34509838

ABSTRACT

NO3 radicals can clean the atmospheric primary contaminants during the night. However, it can also effect the formation of secondary organic aerosol (SOA) and nitrate, which may worsen air quality. We report field observations of NO3 radicals with a home-made long path differential optical absorption spectroscopy (LP-DOAS) at a rural site in the polluted North China Plain in the summer of 2014. The detection limit (1σ) of NO3 with 3.4 km optical path was 3.4 ppt. The observed mean NO3 mixing ratios were 21 ppt with the maximum value of 104 ppt. The average calculated production rates and steady state lifetime of NO3 were 952 ppt/h and 103 s, respectively. The increase of both PM2.5 (>60 µg/m3) and RH (>60%) would result in an increase of the loss of NO3. The proportion of indirect losses rise with the increase of RH (>50%). The fitting kNO3 ranged from 0.0018 to 0.012 s-1 while γN2O5 was 0.0012 to 0.072. The ratios of direct loss ranged from 20.95% to 90.36% with an average of 56.81% during the campaign.


Subject(s)
Air Pollutants , Particulate Matter , Air Pollutants/analysis , China , Environmental Monitoring , Particulate Matter/analysis , Spectrum Analysis
18.
Sci Total Environ ; 810: 152275, 2022 Mar 01.
Article in English | MEDLINE | ID: mdl-34902401

ABSTRACT

A continuous wintertime observation of ambient OH and HO2 radicals was first carried out in Shanghai, in 2019. This effort coincided with the second China International Import Expo (CIIE), during which strict emission controls were implemented in Shanghai, resulting in an average PM2.5 concentration of less than 35 µg/m3. The self-developed instrument based on the laser-induced fluorescence (LIF) technique reported that the average OH radical concentration at noontime (11:00-13:00) was 2.7 × 106 cm-3, while the HO2 concentration was 0.8 × 108 cm-3. A chemical box model utilizing the Regional Atmospheric Chemical Mechanism 2 (RACM2), which is used to simulate pollutant reactions and other processes in the troposphere and which incorporates the Leuven isoprene mechanism (LIM1), reproduced the OH concentrations on most days. The HO2 concentration was underestimated, and the observed-to-modelled ratio demonstrated poor performance by the model, especially during the elevated photochemistry period. Missing primary peroxy radical sources or unknown behaviors of RO2 for high-NOx regimes are possible reasons for the discrepancy. The daytime ROx production was controlled by various sources. HONO photolysis accounted for more than one half (0.83 ppb/h), and the contribution from formaldehyde, OVOCs and ozone photolysis was relatively similar. Active oxidation paths accelerated the rapid ozone increase in winter. The average ozone production rate was 15.1 ppb/h, which is comparable to that of a Beijing suburb (10 ppb/h for the 'BEST-ONE') but much lower than that of Beijing's center (39 ppb/h in 'PKU' and 71 ppb/h in 'APHH') in wintertime. Cumulative local ozone based on observed peroxy radicals was five times higher than the value simulated by the current model due to the underprediction of HO2 and RO2 under the high-NOx regime. This analysis provides crucial information for subsequent pollution control policies in Shanghai.


Subject(s)
Ozone , China , Formaldehyde , Oxidation-Reduction , Ozone/analysis , Photolysis
19.
J Environ Sci (China) ; 107: 1-13, 2021 Sep.
Article in English | MEDLINE | ID: mdl-34412773

ABSTRACT

Atmospheric aerosols have effects on atmospheric radiation assessments, global climate change, local air quality and visibility. In particular, aerosols are more likely transformed and accumulated in winter. In this paper, we used the Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) instrument to study the characteristics of aerosol type and contributions of PM2.5 chemical components to aerosol extinction (AE), vertical distribution of aerosols, and source. From December 30, 2018 to January 27, 2019, we conducted MAX-DOAS observations on Sanmenxia. The proportion of PM2.5 to PM10 was 69.48%-95.39%, indicating that the aerosol particles were mainly fine particles. By analyzing the ion data and modifying Interagency Monitoring of Protected Visual Environments (IMPROVE) method, we found that nitrate was the largest contributor to AE, accounting for 31.51%, 28.98%, and 27.95% of AE on heavily polluted, polluted, and clean days, respectively. NH4+, OC, and SO42- were also major contributors to AE. The near-surface aerosol extinction retrieved from MAX-DOAS measurement the PM2.5 and PM10 concentrations measured by an Unmanned Aerial Vehicle (UAV) have the same trend in vertical distribution. AE increased about 3 times from surface to 500 m. With the backward trajectory of the air mass during the haze, we also found that the continuous heavy pollution was mainly caused by transport of polluted air from the northeast, then followed by local industrial emissions and other sources of emissions under continuous and steady weather conditions.


Subject(s)
Air Pollutants , Aerosols/analysis , Air Pollutants/analysis , Environmental Monitoring , Particulate Matter/analysis , Spectrum Analysis
20.
Sci Total Environ ; 772: 144829, 2021 Jun 10.
Article in English | MEDLINE | ID: mdl-33578154

ABSTRACT

This study reports on the first continuous measurements of ambient OH and HO2 radicals at a suburban site in Chengdu, Southwest China, which were collected during 2019 as part of a comprehensive field campaign 'CompreHensive field experiment to explOre the photochemical Ozone formation mechaniSm in summEr - 2019 (CHOOSE-2019)'. The mean concentrations (11:00-15:00) of the observed OH and HO2 radicals were 9.5 × 106 and 9.0 × 108 cm-3, respectively. To investigate the state-of-the-art chemical mechanism of radical, closure experiments were conducted with a box model, in which the RACM2 mechanism updated with the latest isoprene chemistry (RACM2-LIM1) was used. In the base run, OH radicals were underestimated by the model for the low-NO regime, which was likely due to the missing OH recycling. However, good agreement between the observed and modeled OH concentrations was achieved when an additional species X (equivalent to 0.25 ppb of NO mixing ratio) from one new OH regeneration cycle (RO2 + X â†’ HO2, HO2 + X â†’ OH) was added into the model. Additionally, in the base run, the model could reproduce the observed HO2 concentrations. Discrepancies in the observed and modeled HO2 concentrations were found in the sensitivity runs with HO2 heterogeneous uptake, indicating that the impact of the uptake may be less significant in Chengdu because of the relatively low aerosol concentrations. The ROx (= OH + HO2 + RO2) primary source was dominated by photolysis reactions, in which HONO, O3, and HCHO photolysis accounted for 34%, 19%, and 23% during the daytime, respectively. The efficiency of radical cycling was quantified by the radical chain length, which was determined by the NO to NO2 ratio successfully. The parameterization of the radical chain length may be very useful for the further determinations of radical recycling.

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