大气中CO2含量的增加速率已经超过了自然界所能吸收的速度,并逐步影响到全球气候变暖。利用模型模拟分析已经成为一个重要的工具用以深入对碳循环的理解。本文使用2008~2010年的生物模型SiB3(Simple Biosphere version 3)与优化后的CT20...大气中CO2含量的增加速率已经超过了自然界所能吸收的速度,并逐步影响到全球气候变暖。利用模型模拟分析已经成为一个重要的工具用以深入对碳循环的理解。本文使用2008~2010年的生物模型SiB3(Simple Biosphere version 3)与优化后的CT2016(Carbon Tracker 2016)陆地生态系统碳通量驱动GEOS-Chem大气化学传输模型模拟全球CO2浓度。通过分析模拟CO2浓度的空间分布与季节变化,加深对全球碳源汇分布特点的理解,探究陆地生态系统碳通量不确定性对模拟结果的影响,进而认识陆地生态系统碳通量反演精度提升的重要性。SiB3与优化后的CT2016陆地生态系统碳通量都具有明显的季节变化,但在欧洲地区碳源汇的表现相反,其全球总量与空间分布也存在极大的不确定性。模拟CO2浓度结果表明:在人为活动较少地区,陆地生态系统碳通量对近地面CO2浓度空间分布起主导作用,尤其在南半球和欧洲地区模拟浓度有明显差异,且两种模拟结果的季节差异依赖于陆地生态系统碳通量的季节变化。将模拟结果与9个观测站点资料进行对比,以期选用合适的陆地生态系统碳通量来提升GEOS-Chem模拟CO2浓度的精度。实验结果表明:两种模拟结果均能较好的模拟CO2浓度的季节变化及其峰谷值,但CT2016模拟的CO2浓度在多数站点处更接近观测资料,模拟准确性更高。展开更多
The 2019 Refinement to the 2006 IPCC Guidelines for National Greenhouse Gas Inventories added the method of assimilating atmospheric CO_(2) concentrations to invert carbon sources and sinks;however,many global carbon ...The 2019 Refinement to the 2006 IPCC Guidelines for National Greenhouse Gas Inventories added the method of assimilating atmospheric CO_(2) concentrations to invert carbon sources and sinks;however,many global carbon inversion models are not publicly available.In addition,our regional assimilation inversion system,CCMVS-R(China Carbon Monitoring,Verification and Supporting for Regional),needs a global carbon inversion model with higher assimilation efficiency to provide boundary conditions.Here,an inversion model based on the global atmospheric chemistry model GEOS-Chem and a more accurate and easier-to-implement ensemble square root Kalman filter(EnSRF)algorithm is constructed and used to infer global and China's carbon fluxes in 2019.Atmospheric CO_(2) concentrations from ObsPack sites and five additional CO_(2) observational sites from China's Greenhouse Gas Observation Network(CGHGNET)were used for data assimilation to improve the estimate.The inverted annual global terrestrial and oceanic carbon uptake is 2.12 and 2.53 Pg C per year,respectively,accounting for 21.1%and 25.1%of global fossil fuel CO_(2) emissions.The remaining 5.41 Pg C per year in the atmosphere is consistent with the global atmospheric CO_(2) growth rates of 5.44 Pg C per year reported by the National Oceanic and Atmospheric Administration(NOAA),showing that the inversion model can provide a reasonable estimate of global-scale natural carbon sinks.The inverted terrestrial carbon sink of China is 0.37 Pg C per year,accounting for approximately 13%of China's fossil CO_(2) emissions.展开更多
We used the global atmospheric chemical transport model,GEOS-Chem,to simulate the spatial distribution and seasonal variation of surface-layer methane (CH4) in 2004,and quantify the impacts of individual domestic so...We used the global atmospheric chemical transport model,GEOS-Chem,to simulate the spatial distribution and seasonal variation of surface-layer methane (CH4) in 2004,and quantify the impacts of individual domestic sources and foreign transport on CH4 concentrations over China.Simulated surface-layer CH4 concentrations over China exhibit maximum concentrations in summer and minimum concentrations in spring.The annual mean CH4 concentrations range from 1800 ppb over western China to 2300 ppb over the more populated eastern China.Foreign emissions were found to have large impacts on CH4 concentrations over China,contributing to about 85% of the CH4 concentrations over western China and about 80% of those over eastern China.The tagged simulation results showed that coal mining,livestock,and waste are the dominant domestic contributors to CH4 concentrations over China,accounting for 36%,18%,and 16%,respectively,of the annual and national mean increase in CH4 concentration from all domestic emissions.Emissions from rice cultivation were found to make the largest contributions to CH4 concentrations over China in the summer,which is the key factor that leads to the maximum seasonal mean CH4 concentrations in summer.展开更多
Systematic monitoring of the fluctuations in atmospheric SO2 oxidation efficiency—measured as a molar ratio of SO42- to total SOx (SOx=SO2+SO42-), referred as S-ratio—have been performed during a major long range pl...Systematic monitoring of the fluctuations in atmospheric SO2 oxidation efficiency—measured as a molar ratio of SO42- to total SOx (SOx=SO2+SO42-), referred as S-ratio—have been performed during a major long range plume transport to northeast India (Shillong: 25.67°N, 91.91°E, 1064 m ASL) in March 2009. Anomalously low S-ratios (median, 0.03) were observed during the episode—associated with a cyclonic circulation—and the SO42- and SO2 exhibited unusual features in the ‘relative phase’ of their peaks. During initial days, when SO2 levels were dictated by the long range influx, the SO42- and SO2 variabilities were in anti-phase—for the differing mobility/loss mechanisms. When SO2 levels were governed by the boundary layer diurnality in the latter days, the anti-phase is explained by a ‘depleted OH level’—major portion being consumed in the initial period by the elevated SO2 and other pollutants. Simulations with a global 3D chemical transport model, GEOS-Chem (v8-03-01), also indicated ‘suppressed oxidation conditions’—with characteristic low S-ratios and poor phase agreements. The modelled OH decreased steadily from the initial days, and OH normalized to SO2—referred as OHspecific—was consistently low during the ‘suppressed S-ratio period’. Further, the geographical distribution of modelled OH showed a pronounced minimum over the region surrounding (20°N, 95°E) spanning parts of northeast India and the adjacent regions to the southeast of it—prevalent throughout the year, though the magnitude and the area of influence have a seasonality to it—with significant implications for reducing the oxidizing power of the regional atmosphere. A second set of measurements during January 2010—when prominent long range transports were absent—exhibited no anomalies, and the S-ratios were well within the acceptable limits (median, 0.32). This work highlights the GEOS-Chem model skill in simulating/detecting the ‘transient fluctuations’ in the oxidation efficiency, down to a regional scale.展开更多
Ambient sulphur dioxide (SO2) measurements have been performed at a high altitude site in the semi arid region of western India, Gurushikhar, Mt. Abu (24.6°N, 72.7°E, 1680 m ASL), during different sampling p...Ambient sulphur dioxide (SO2) measurements have been performed at a high altitude site in the semi arid region of western India, Gurushikhar, Mt. Abu (24.6°N, 72.7°E, 1680 m ASL), during different sampling periods span over Sep-Dec 2009 and Feb-Mar 2010. A global three dimensional chemical transport Model, GEOS-Chem, (v8-03-01) is employed to generate the SO2 profile for the entire region for the different sampling months which in turn is used to explain the major features in the measured SO2 spectra via correlating with HYSPLIT generated wind back trajectories. The mean SO2 concentrations recorded at the sampling site varied for the different sampling periods (4.3 ppbv in Sep-Oct 2009, 3.4 ppbv in Nov 2009, 3.5 ppbv in Dec 2009, 7.7 ppbv in Feb 2010 and 9.2 ppbv in Mar 2010) which were found to be strongly influenced by long range transport from a source region surrounding 30°N, 75°E—the one projected with the highest SO2 concentration in the GEOS-Chem generated profiles for the region—lying only a few co-ordinates away. A diurnal cycle of SO2 concentration exists throughout the sampling periods, with the greatest day-night changes observed during Feb and Mar 2010, barely detectable during Sep-Oct 2009, and intermediate values for Nov and Dec 2009 which are systematically studied using the time series PBL height and OH radical values from the GEOS-Chem model. During the sampling period in Nov 2009, a plume transport to the sampling site also was detected when a major fire erupted at an oil depot in Jaipur (26.92°N, 75.82°E), located few co-ordinates away. Separate runs of the model, performed to study the long range transport effects, show a drop in the SO2 levels over the sampling region in the absence of transport, throughout the year with Jan to Apr seen to be influenced the lowest by long range transport while Jul and Dec influenced the highest.展开更多
Ambient SO2 concentration at a high rain fall site, Shillong (25.67oN, 91.91oE, 1064 m ASL), located in North-East India, was measured during March 2009 and January 2010 with the aim to understand the effect of long r...Ambient SO2 concentration at a high rain fall site, Shillong (25.67oN, 91.91oE, 1064 m ASL), located in North-East India, was measured during March 2009 and January 2010 with the aim to understand the effect of long range transport of pollutants from North-East Asia on the ambient SO2 levels at this relatively clean site. The concentrations recorded during the former sampling period were very high (Max: 262.3 ppb)—which decayed down gradually towards the end the sampling period—whereas those during the latter sampling period were well within the acceptable limits (Max: 29.7 ppb). This elevated SO2 concentrations during March 2009 is proposed to have association with a major cold air outbreak and an associated cyclone preceding one of the dust storm events reported in China, and a resultant sudden change in wind trajectory leading to the long range transport of pollutants to the sampling site. The argument is formulated on the basis of the back trajectory analysis performed using HYSPLIT for the month of March 2009—the plots clearly showed a drastic change in wind trajectories between 8th and 15th of March 2009 wherein the winds traveled over some of the highly polluted regions such as the Perm region of Russia—and on the results from model runs performed using the global 3-D model of tropospheric chemistry, GEOS-Chem (v8-03-01)—it clearly showed the tropospheric SO2 over Perm region in Russia peaking during Nov, Dec, Jan, Feb and Mar every year, possibly due to central heating. The observation of long range transport of SO2 from the highly industrialized areas of Perm in Russia to North-East India during dust storm events has important implications to the present understanding on its relative contribution to the Asian pollutant outflow to the Pacific during spring as the GEOS-Chem model runs also showed regions in and around Russia with relatively high concentrations of atmospheric NOx, Peroxyacetyl Nitrate, Lumped Peroxypropionyl Nitrate, HNO3, HNO4,C3H8, C2H6, SO4, NH4, Inorganic Sulphur Nitrates and Lumped Alkyl Nitrate.展开更多
Spatiotemporal patterns of column-averaged dry air mole fraction of CO2(XCO2)have not been well characterized on a regional scale due to limitations in data availability and precision.This paper addresses these issues...Spatiotemporal patterns of column-averaged dry air mole fraction of CO2(XCO2)have not been well characterized on a regional scale due to limitations in data availability and precision.This paper addresses these issues by examining such patterns in China using the long-term mapping XCO2 dataset(2009-2016)derived from the Greenhouse gases Observing SATellite(GOSAT).XCO2 simulations are also constructed using the high-resolution nested-grid GEOS-Chem model.The following results are found:Firstly,the correlation coefficient between the anthropogenic emissions and XCO2 spatial distribution is nearly zero in summer but up to 0.32 in autumn.Secondly,on average,XCO2 increases by 2.08 ppm every year from2010 to 2015,with a sharp increase of 2.6 ppm in 2013.Lastly,in the analysis of three typical regions,the GOSAT XCO2 time series is inbetter agreement with the GEOS-Chem simulation of XCO2 in the Taklimakan Desert region(the least difference with bias 0.65±0.78 ppm),compared with the northern urban agglomerationregion(-1.3±1.2 ppm)and the northeastern forest region(-1.4±1.4 ppm).The results are likely attributable to uncertainty in both the satellite-retrieved XCO2 data and the model simulation data.展开更多
The gaseous or particulate forms of divalent mercury(HgⅡ) significantly impact the spatial distribution of atmospheric mercury concentration and deposition flux(FLX). In the new nested-grid GEOS-Chem model, we try to...The gaseous or particulate forms of divalent mercury(HgⅡ) significantly impact the spatial distribution of atmospheric mercury concentration and deposition flux(FLX). In the new nested-grid GEOS-Chem model, we try to modify the HgⅡ gas-particle partitioning relationship with synchronous and hourly observations at four sites in China. Observations of gaseous oxidized Hg(GOM), particulate-bound Hg(PBM), and PM 2.5 were used to derive an empirical gas-particle partitioning coefficient as a function of temperature( T) and organic aerosol(OA) concentrations under different relative humidity(RH). Results showed that with increasing RH, the dominant process of HgⅡ gas-particle partitioning changed from physical adsorption to chemical desorption. And the dominant factor of HgⅡ gas-particle partitioning changed from T to OA concentrations. We thus improved the simulated OA concentration field by introducing intermediate-volatility and semi-volatile organic compounds(I/SVOCs) emission inventory into the model framework and refining the volatile distributions of I/SVOCs according to new filed tests in the recent literatures. Finally, normalized mean biases(NMBs) of monthly gaseous element mercury(GEM), GOM, PBM, WFLX were reduced from-33%–29%, 95%–300%, 64%–261%, 117%–122% to-13%–0%,-20%–80%,-31%–50%,-17%–23%. The improved model explains 69%–98% of the observed atmospheric Hg decrease during 2013–2020 and can serve as a useful tool to evaluate the effectiveness of the Minamata Convention on Mercury.展开更多
基金partially supported by the National Key Research and Development Program of China [grant number 2016YFA0600203]the National Natural Science Foundation of China [grant number 41575100]
基金financially supported by the General Project of Top-Design of Mlti-Scale Nature-Social Models,Data Support and Decision Support System for NSFC Carbon Neutrality Major Project and the Basic Scientific Research Fund of the Chinese Academy of Meteorological Sciences(2021Z014)。
文摘The 2019 Refinement to the 2006 IPCC Guidelines for National Greenhouse Gas Inventories added the method of assimilating atmospheric CO_(2) concentrations to invert carbon sources and sinks;however,many global carbon inversion models are not publicly available.In addition,our regional assimilation inversion system,CCMVS-R(China Carbon Monitoring,Verification and Supporting for Regional),needs a global carbon inversion model with higher assimilation efficiency to provide boundary conditions.Here,an inversion model based on the global atmospheric chemistry model GEOS-Chem and a more accurate and easier-to-implement ensemble square root Kalman filter(EnSRF)algorithm is constructed and used to infer global and China's carbon fluxes in 2019.Atmospheric CO_(2) concentrations from ObsPack sites and five additional CO_(2) observational sites from China's Greenhouse Gas Observation Network(CGHGNET)were used for data assimilation to improve the estimate.The inverted annual global terrestrial and oceanic carbon uptake is 2.12 and 2.53 Pg C per year,respectively,accounting for 21.1%and 25.1%of global fossil fuel CO_(2) emissions.The remaining 5.41 Pg C per year in the atmosphere is consistent with the global atmospheric CO_(2) growth rates of 5.44 Pg C per year reported by the National Oceanic and Atmospheric Administration(NOAA),showing that the inversion model can provide a reasonable estimate of global-scale natural carbon sinks.The inverted terrestrial carbon sink of China is 0.37 Pg C per year,accounting for approximately 13%of China's fossil CO_(2) emissions.
基金supported by the Chinese Academy of Sciences Strategic Priority Research Program (Grant No. XDA05100503)the National Natural Science Foundation of China (Grant Nos. 40825016 and 41021004)
文摘We used the global atmospheric chemical transport model,GEOS-Chem,to simulate the spatial distribution and seasonal variation of surface-layer methane (CH4) in 2004,and quantify the impacts of individual domestic sources and foreign transport on CH4 concentrations over China.Simulated surface-layer CH4 concentrations over China exhibit maximum concentrations in summer and minimum concentrations in spring.The annual mean CH4 concentrations range from 1800 ppb over western China to 2300 ppb over the more populated eastern China.Foreign emissions were found to have large impacts on CH4 concentrations over China,contributing to about 85% of the CH4 concentrations over western China and about 80% of those over eastern China.The tagged simulation results showed that coal mining,livestock,and waste are the dominant domestic contributors to CH4 concentrations over China,accounting for 36%,18%,and 16%,respectively,of the annual and national mean increase in CH4 concentration from all domestic emissions.Emissions from rice cultivation were found to make the largest contributions to CH4 concentrations over China in the summer,which is the key factor that leads to the maximum seasonal mean CH4 concentrations in summer.
基金This study was supported by the National Key Research and Development Program of China[grant numbers 2020YFA0607803 and 2019YFA0606800]the National Natural Science Foundation of China[grant number 41975159].
基金supported by the National Basic Research Program of China[973 program,grant number 2014CB441202]the Strategic Priority Research Program of the Chinese Academy of Sciences[grant number XDA05100503]the National Natural Science Foundation of China[grant numbers 41021004,41475137,and 91544219]
文摘Systematic monitoring of the fluctuations in atmospheric SO2 oxidation efficiency—measured as a molar ratio of SO42- to total SOx (SOx=SO2+SO42-), referred as S-ratio—have been performed during a major long range plume transport to northeast India (Shillong: 25.67°N, 91.91°E, 1064 m ASL) in March 2009. Anomalously low S-ratios (median, 0.03) were observed during the episode—associated with a cyclonic circulation—and the SO42- and SO2 exhibited unusual features in the ‘relative phase’ of their peaks. During initial days, when SO2 levels were dictated by the long range influx, the SO42- and SO2 variabilities were in anti-phase—for the differing mobility/loss mechanisms. When SO2 levels were governed by the boundary layer diurnality in the latter days, the anti-phase is explained by a ‘depleted OH level’—major portion being consumed in the initial period by the elevated SO2 and other pollutants. Simulations with a global 3D chemical transport model, GEOS-Chem (v8-03-01), also indicated ‘suppressed oxidation conditions’—with characteristic low S-ratios and poor phase agreements. The modelled OH decreased steadily from the initial days, and OH normalized to SO2—referred as OHspecific—was consistently low during the ‘suppressed S-ratio period’. Further, the geographical distribution of modelled OH showed a pronounced minimum over the region surrounding (20°N, 95°E) spanning parts of northeast India and the adjacent regions to the southeast of it—prevalent throughout the year, though the magnitude and the area of influence have a seasonality to it—with significant implications for reducing the oxidizing power of the regional atmosphere. A second set of measurements during January 2010—when prominent long range transports were absent—exhibited no anomalies, and the S-ratios were well within the acceptable limits (median, 0.32). This work highlights the GEOS-Chem model skill in simulating/detecting the ‘transient fluctuations’ in the oxidation efficiency, down to a regional scale.
文摘Ambient sulphur dioxide (SO2) measurements have been performed at a high altitude site in the semi arid region of western India, Gurushikhar, Mt. Abu (24.6°N, 72.7°E, 1680 m ASL), during different sampling periods span over Sep-Dec 2009 and Feb-Mar 2010. A global three dimensional chemical transport Model, GEOS-Chem, (v8-03-01) is employed to generate the SO2 profile for the entire region for the different sampling months which in turn is used to explain the major features in the measured SO2 spectra via correlating with HYSPLIT generated wind back trajectories. The mean SO2 concentrations recorded at the sampling site varied for the different sampling periods (4.3 ppbv in Sep-Oct 2009, 3.4 ppbv in Nov 2009, 3.5 ppbv in Dec 2009, 7.7 ppbv in Feb 2010 and 9.2 ppbv in Mar 2010) which were found to be strongly influenced by long range transport from a source region surrounding 30°N, 75°E—the one projected with the highest SO2 concentration in the GEOS-Chem generated profiles for the region—lying only a few co-ordinates away. A diurnal cycle of SO2 concentration exists throughout the sampling periods, with the greatest day-night changes observed during Feb and Mar 2010, barely detectable during Sep-Oct 2009, and intermediate values for Nov and Dec 2009 which are systematically studied using the time series PBL height and OH radical values from the GEOS-Chem model. During the sampling period in Nov 2009, a plume transport to the sampling site also was detected when a major fire erupted at an oil depot in Jaipur (26.92°N, 75.82°E), located few co-ordinates away. Separate runs of the model, performed to study the long range transport effects, show a drop in the SO2 levels over the sampling region in the absence of transport, throughout the year with Jan to Apr seen to be influenced the lowest by long range transport while Jul and Dec influenced the highest.
文摘Ambient SO2 concentration at a high rain fall site, Shillong (25.67oN, 91.91oE, 1064 m ASL), located in North-East India, was measured during March 2009 and January 2010 with the aim to understand the effect of long range transport of pollutants from North-East Asia on the ambient SO2 levels at this relatively clean site. The concentrations recorded during the former sampling period were very high (Max: 262.3 ppb)—which decayed down gradually towards the end the sampling period—whereas those during the latter sampling period were well within the acceptable limits (Max: 29.7 ppb). This elevated SO2 concentrations during March 2009 is proposed to have association with a major cold air outbreak and an associated cyclone preceding one of the dust storm events reported in China, and a resultant sudden change in wind trajectory leading to the long range transport of pollutants to the sampling site. The argument is formulated on the basis of the back trajectory analysis performed using HYSPLIT for the month of March 2009—the plots clearly showed a drastic change in wind trajectories between 8th and 15th of March 2009 wherein the winds traveled over some of the highly polluted regions such as the Perm region of Russia—and on the results from model runs performed using the global 3-D model of tropospheric chemistry, GEOS-Chem (v8-03-01)—it clearly showed the tropospheric SO2 over Perm region in Russia peaking during Nov, Dec, Jan, Feb and Mar every year, possibly due to central heating. The observation of long range transport of SO2 from the highly industrialized areas of Perm in Russia to North-East India during dust storm events has important implications to the present understanding on its relative contribution to the Asian pollutant outflow to the Pacific during spring as the GEOS-Chem model runs also showed regions in and around Russia with relatively high concentrations of atmospheric NOx, Peroxyacetyl Nitrate, Lumped Peroxypropionyl Nitrate, HNO3, HNO4,C3H8, C2H6, SO4, NH4, Inorganic Sulphur Nitrates and Lumped Alkyl Nitrate.
基金supported by the National Key Research and Development Program of China (Grant No. 2016YFA0600303)the Key Deployment Projects of the Chinese Academy of Sciences (Grant No. ZDRWZS-2019-1-3)
文摘Spatiotemporal patterns of column-averaged dry air mole fraction of CO2(XCO2)have not been well characterized on a regional scale due to limitations in data availability and precision.This paper addresses these issues by examining such patterns in China using the long-term mapping XCO2 dataset(2009-2016)derived from the Greenhouse gases Observing SATellite(GOSAT).XCO2 simulations are also constructed using the high-resolution nested-grid GEOS-Chem model.The following results are found:Firstly,the correlation coefficient between the anthropogenic emissions and XCO2 spatial distribution is nearly zero in summer but up to 0.32 in autumn.Secondly,on average,XCO2 increases by 2.08 ppm every year from2010 to 2015,with a sharp increase of 2.6 ppm in 2013.Lastly,in the analysis of three typical regions,the GOSAT XCO2 time series is inbetter agreement with the GEOS-Chem simulation of XCO2 in the Taklimakan Desert region(the least difference with bias 0.65±0.78 ppm),compared with the northern urban agglomerationregion(-1.3±1.2 ppm)and the northeastern forest region(-1.4±1.4 ppm).The results are likely attributable to uncertainty in both the satellite-retrieved XCO2 data and the model simulation data.
基金supported by the National Natural Science Foundation of China (No. 21625701 )the Major State Basic Research Development Program of China ( 973 ) (No. 2013CB430001 )+1 种基金the Youth Project of National Natural Science Foundation of China (No. 21607090 )the Shuimu Tsinghua Scholar Program (No. 2021SM017)。
文摘The gaseous or particulate forms of divalent mercury(HgⅡ) significantly impact the spatial distribution of atmospheric mercury concentration and deposition flux(FLX). In the new nested-grid GEOS-Chem model, we try to modify the HgⅡ gas-particle partitioning relationship with synchronous and hourly observations at four sites in China. Observations of gaseous oxidized Hg(GOM), particulate-bound Hg(PBM), and PM 2.5 were used to derive an empirical gas-particle partitioning coefficient as a function of temperature( T) and organic aerosol(OA) concentrations under different relative humidity(RH). Results showed that with increasing RH, the dominant process of HgⅡ gas-particle partitioning changed from physical adsorption to chemical desorption. And the dominant factor of HgⅡ gas-particle partitioning changed from T to OA concentrations. We thus improved the simulated OA concentration field by introducing intermediate-volatility and semi-volatile organic compounds(I/SVOCs) emission inventory into the model framework and refining the volatile distributions of I/SVOCs according to new filed tests in the recent literatures. Finally, normalized mean biases(NMBs) of monthly gaseous element mercury(GEM), GOM, PBM, WFLX were reduced from-33%–29%, 95%–300%, 64%–261%, 117%–122% to-13%–0%,-20%–80%,-31%–50%,-17%–23%. The improved model explains 69%–98% of the observed atmospheric Hg decrease during 2013–2020 and can serve as a useful tool to evaluate the effectiveness of the Minamata Convention on Mercury.