Abstract. The seasonal evolution of O3 and its photochemical production regime in a polluted region of eastern China between 2014 and 2017 has been investigated using observations. We used tropospheric ozone (O3), carbon monoxide (CO), and formaldehyde (HCHO, a marker of VOCs (volatile organic compounds)) partial columns derived from high-resolution Fourier transform spectrometry (FTS); tropospheric nitrogen dioxide (NO2, a marker of NOx (nitrogen oxides)) partial column deduced from the Ozone Monitoring Instrument (OMI); surface meteorological data; and a back trajectory cluster analysis technique. A broad O3 maximum during both spring and summer (MAM/JJA) is observed; the day-to-day variations in MAM/JJA are generally larger than those in autumn and winter (SON/DJF). Tropospheric O3 columns in June are 1.55×1018 molecules cm−2 (56 DU (Dobson units)), and in December they are 1.05×1018 molecules cm−2 (39 DU). Tropospheric O3 columns in June were ∼50 % higher than those in December. Compared with the SON/DJF season, the observed tropospheric O3 levels in MAM/JJA are more influenced by the transport of air masses from densely populated and industrialized areas, and the high O3 level and variability in MAM/JJA is determined by the photochemical O3 production. The tropospheric-column HCHO∕NO2 ratio is used as a proxy to investigate the photochemical O3 production rate (PO3). The results show that the PO3 is mainly nitrogen oxide (NOx) limited in MAM/JJA, while it is mainly VOC or mixed VOC–NOx limited in SON/DJF. Statistics show that NOx-limited, mixed VOC–NOx-limited, and VOC-limited PO3 accounts for 60.1 %, 28.7 %, and 11 % of days, respectively. Considering most of PO3 is NOx limited or mixed VOC–NOx limited, reductions in NOx would reduce O3 pollution in eastern China.
Abstract. A ground-based high-resolution Fourier transform spectrometer (FTS) station has been established in Hefei, China to remotely measure CO 2 , CO and other greenhouse gases based on near-infrared solar absorption spectra. Total column measurements of atmospheric CO 2 and CO were successfully obtained from July 2014 to April 2016. The spectra collected with an InSb detector in the first year were compared with those collected by an InGaAs detector from July 2015, demonstrating that InGaAs spectra have better signal-to-noise ratios and rms of spectral fitting residuals relative to InSb spectra. Consequently, the measurement precision of the retrieved XCO 2 and XCO for InGaAs spectra is superior to InSb spectra, with about 0.04 and 0.09 % for XCO 2 , and 1.07 and 2.00 % for XCO within clear-sky days respectively. Daily and monthly averages of columnaveraged dry air mole fraction of CO 2 show a clear seasonal cycle, while the daily and monthly averages of XCO displayed no seasonal variation. Also, we analysed the relationship of the anomalies of XCO and XCO 2 , found that the correlations are only observable for individual days, and the data under different prevailing wind conditions during the observations displayed weak correlation. The observations based on the high-resolution FTS were also compared with the temporally coinciding measurements taken with a low-resolution solar FTS instrument, the EM27/SUN. Ratioing the daily averaged XCO 2 of EM27 and FTS gives an overall calibration factor of 0.996 ± 0.001. We also compared ground-based observations from the Tsukuba TCCON station with our observations, the results showing that the variation in phase and seasonal amplitude of XCO 2 are similar to our results, but the variation of XCO in Tsukuba is quite different from our data in Hefei. To further evaluate our retrieved data, we made use of satellite measurements. The direct comparison of our observations with the Greenhouse Gases Observing Satellite (GOSAT) data shows good agreement of daily median XCO 2 , with a bias of −0.52 ppm and standard deviation of 1.63 ppm. The correlation coefficient (R 2 ) is 0.79 for daily median XCO 2 between our FTS and GOSAT observations. Daily median Orbiting Carbon Observatory 2 (OCO-2) data produce a positive bias of 0.81 ppm and standard deviation of 1.73 ppm relative to our ground-based data. Our daily median XCO 2 also show strong correlation with OCO-2 data, with correlation coefficient (R 2 ) of 0.83. Although there were a limited number of data during the observations due to instrument downtime and adverse weather, the results confirm the suitability of the observatory for ground-based long-term measurements of greenhouse gases with high precision and
Regional land use change and ecological security are important fields and have been popular issues in global change research in recent years. Regional habitat quality is also an important embodiment of the service function and health of ecosystems. Taking Shiyan City of Hubei Province as an example, the spatiotemporal differences in habitat quality in Shiyan City were evaluated using the habitat quality module of the InVEST model and GIS spatial analysis method based on DEM and land use data from 2000, 2005, 2010, 2015, and 2020. According to the habitat quality index values, the habitats were divided into four levels indicating habitat quality: I (very bad), II (bad), III (good), and IV (excellent), and the topographic gradient effect of habitat quality was studied using the topographic position index. The results show the following. (1) The habitat quality of Shiyan City showed relatively high and obvious spatial heterogeneity overall and, more specifically, was high in the northwest and southwest, moderate in the center, and low in the northeast. The higher quality habitats (levels III, IV) were mainly distributed in mountain and hill areas and water areas, while those with lower quality habitats (levels I, II) were mainly distributed in agricultural urban areas. (2) From 2000 to 2020, the overall average habitat quality of Shiyan City first increased, then decreased, and then increased again. Additionally, the habitat area increased with an improvement in the level. There was a trend in habitat transformation moving from low to high quality level, showing a spatial pattern of “rising in the southwest and falling in the northeast”. (3) The habitat quality in the water area and woodland area was the highest, followed by grassland, and that of cultivated land was the lowest. From 2000 to 2020, the habitat quality of cultivated land, woodland, and grassland decreased slightly, while the habitat quality of water increased significantly. (4) The higher the level of the topographic position index, the smaller the change range of land use types with time. The terrain gradient effect of habitat quality was significant. With the increase in terrain level, the average habitat quality correspondingly improved, but the increasing range became smaller and smaller. These results are helpful in revealing the spatiotemporal evolution of habitat quality caused by land use changes in Shiyan City and can provide a scientific basis for the optimization of regional ecosystem patterns and land use planning and management, and they are of great significance for planning the rational and sustainable use of land resources and the construction of an ecological civilization.
Abstract. The major air pollutant emissions have decreased and the overall air quality has substantially improved across China in recent years as a consequence of active clean air policies for mitigating severe air pollution problems. As key precursors of formaldehyde (HCHO) and ozone (O3), the volatile organic compounds (VOCs) in China are still increasing because current clean air policies lack mitigation measures for VOCs. In this study, we mapped the drivers of HCHO variability over eastern China using ground-based high-resolution Fourier transform infrared (FTIR) spectrometry and GEOS-Chem model simulation. Diurnal, seasonal, and interannual variability of HCHO over eastern China was investigated and hydroxyl (OH) radical production from HCHO was evaluated. The relative contributions of emitted and photochemical sources to the observed HCHO were analysed by using ground level carbon monoxide (CO) and Ox (O3 + nitrogen oxide (NO2)) as tracers for emitted and photochemical HCHO, respectively. Contributions of various emission sectors and geographical transport to the observed HCHO summertime enhancements were determined by using a GEOS-Chem tagged-tracer simulation. The tropospheric HCHO volume mixing ratio (VMR) reached a maximum monthly mean value of (1.1 ± 0.27) ppbv in July and a minimum monthly mean value of (0.4 ± 0.11) ppbv in January. The tropospheric HCHO VMR time series from 2015–2019 shows a positive trend of (1.43 ± 0.14) % per yr. The photochemical HCHO is the dominant source of atmospheric HCHO over eastern China for most of the year (68.1 %). In the studied years, the HCHO photolysis was an important source of OH radical over eastern China during all sunlight hours of both summer and winter days. The anthropogenic emissions (fossil fuel + biofuel emissions) accounted for 31.96 % and the natural emissions (biomass burning + biogenic) accounted for 48.75 % of HCHO summertime enhancements. The observed HCHO summertime enhancements were largely attributed to the emissions within China (76.92 %), where eastern China dominated the contribution (46.24 %). The increased trend in HCHO in recent years was largely attributed to the increase in the HCHO precursors such as CH4 and nonmethane VOCs (NMVOCs). This study can provide an evaluation of recent VOC emissions and regional photochemical capacity in China. In addition, this study is also important for regulatory and control purposes and will help to improve urban air quality and contribute to the formation of new Chinese clean air policies in the future.
In this study, the characterization of Hydrogen Chloride (HCl) seasonal variations and inter-annual linear trend are presented for the first time over the polluted region at Hefei (117°10’E, 31°54’N), China. The time series of HCl were retrieved by the mid-infrared (MIR) solar spectra recorded by the ground-based high-resolution Fourier transform infrared spectroscopy (FTIR) between July, 2015 and April, 2019. The magnitude of HCl reaches a peak in January (2.70 ± 0.16) × 1015 molecules*cm-2 and a minimum in September (2.27 ± 0.09) × 1015 molecules*cm-2. The four-year time series of HCl total column show a negative linear trend of (-1.83 ± 0.13) %. The FTIR data are compared with GEOS-Chem data in order to evaluate the performance of the GEOS-Chem model to simulate HCl. In general, total column FTIR data and GEOS-Chem model data are in a good agreement with a correlation coefficient of 0.82. GEOS-Chem model data present a good agreement with FTIR data in seasonal variation and inter-annul trend. The maximum differences occur in January and April with mean differences of 4%-6%. We also present HCl time series observed by 6 NDACC stations (Bremen, Toronto, Rikubetsu, Izana, Reunion.maido, Lauder) in low-middle-latitude sites of the northern and southern hemispheres and Hefei stations in order to investigate the seasonal and annual trends of HCl in low-middle-latitude sites. The HCl total column at the northern hemisphere stations reached the maximum in the late winter or early spring and the minimum in the early winter or late autumn. In general, the seasonal variations of HCl over Hefei is similar to that in other northern hemisphere mid-latitude FTIR stations.
Abstract. The major air pollutant emissions have decreased, and the overall air quality has substantially improved across China in recent years as a consequence of active clean air policies for mitigating severe air pollution problems. As key precursors of formaldehyde (HCHO) and ozone (O3), the volatile organic compounds (VOCs) in China are still increasing due to the lack of mitigation measures for VOCs. In this study, we investigated the drivers of HCHO variability from 2015 to 2019 over Hefei, eastern China, by using ground-based high-resolution Fourier transform infrared (FTIR) spectroscopy and GEOS-Chem model simulation. Seasonal and interannual variabilities of HCHO over Hefei were analyzed and hydroxyl (OH) radical production rates from HCHO photolysis were evaluated. The relative contributions of emitted and photochemical sources to the observed HCHO were analyzed by using ground-level carbon monoxide (CO) and Ox (O3 + nitrogen oxide (NO2)) as tracers for emitted and photochemical HCHO, respectively. Contributions of emission sources from various categories and geographical regions to the observed HCHO summertime enhancements were determined by using a series of GEOS-Chem sensitivity simulations. The column-averaged dry air mole fractions of HCHO (XHCHO) reached a maximum monthly mean value of 1.1 ± 0.27 ppbv in July and a minimum monthly mean value of 0.4 ± 0.11 ppbv in January. The XHCHO time series from 2015 to 2019 over Hefei showed a positive change rate of 2.38 ± 0.71 % per year. The photochemical HCHO is the dominant source of atmospheric HCHO over Hefei for most of the year (68.1 %). In the studied years, the HCHO photolysis was an important source of OH radicals over Hefei during all sunlight hours of both summer and winter days. The oxidations of both methane (CH4) and nonmethane VOCs (NMVOCs) dominate the HCHO production over Hefei and constitute the main driver of its summertime enhancements. The NMVOC-related HCHO summertime enhancements were dominated by the emissions within eastern China. The observed increasing change rate of HCHO from 2015 to 2019 over Hefei was attributed to the increase in photochemical HCHO resulting from increasing change rates of both CH4 and NMVOC oxidations, which overwhelmed the decrease in emitted HCHO. This study provides a valuable evaluation of recent VOC emissions and regional photochemical capacity in China. In addition, understanding the sources of HCHO is a necessary step for tackling air pollution in eastern China and mitigating the emissions of pollutants.
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