# Atmospheric Transport and Chemistry Modeling

Meng Gao, Zirui Liu, Bo Zheng, Dongsheng Ji, Peter Sherman, Shaojie Song, Jinyuan Xin, Cheng Liu, Yuesi Wang, Qiang Zhang, Jia Xing, Jingkun Jiang, Zifa Wang, Gregory R. Carmichael, and Michael B. McElroy. 2021. “China's emission control strategies have suppressed unfavorable influences of climate on wintertime PM2.5 concentrations in Beijing since 2002.” Atmospheric Chemistry and Physics, 20, 3, Pp. 1497–1505. Publisher's VersionAbstract
Severe wintertime PM2.5 pollution in Beijing has been receiving increasing worldwide attention, yet the decadal variations remain relatively unexplored. Combining field measurements and model simulations, we quantified the relative influences of anthropogenic emissions and meteorological conditions on PM2.5 concentrations in Beijing over the winters of 2002–2016. Between the winters of 2011 and 2016, stringent emission control measures resulted in a 21 % decrease in mean mass concentrations of PM2.5 in Beijing, with 7 fewer haze days per winter on average. Given the overestimation of PM2.5 by the model, the effectiveness of stringent emission control measures might have been slightly overstated. With fixed emissions, meteorological conditions over the study period would have led to an increase in haze in Beijing, but the strict emission control measures have suppressed the unfavorable influences of the recent climate. The unfavorable meteorological conditions are attributed to the weakening of the East Asia winter monsoon associated particularly with an increase in pressure associated with the Aleutian Low.
X. Lu, L. Zhang, T. Wu, M. S. Long, J. Wang, D.J. Jacob, F. Zhang, J. Zhang, S. D. Eastham, L. Hu, L. Zhu, X. Liu, and M Wei. 2020. “Development of the global atmospheric general circulation-chemistry model BCC-GEOS-Chem v1.0: model description and evaluation.” Geoscientific Model Development, 13, 9, Pp. 3817–3838. Publisher's VersionAbstract
Chemistry plays an indispensable role in investigations of the atmosphere; however, many climate models either ignore or greatly simplify atmospheric chemistry, limiting both their accuracy and their scope. We present the development and evaluation of the online global atmospheric chemical model BCC-GEOS-Chem v1.0, coupling the GEOS-Chem chemical transport model (CTM) as an atmospheric chemistry component in the Beijing Climate Center atmospheric general circulation model (BCC-AGCM). The GEOS-Chem atmospheric chemistry component includes detailed troposphericHOx–NOx–volatile organic compounds–ozone–bromine–aerosol chemistry and online dry and wet deposition schemes. We then demonstrate the new capabilities of BCC-GEOS-Chem v1.0 relative to the base BCC-AGCM model through a 3-year (2012–2014) simulation with anthropogenic emissions from the Community Emissions Data System (CEDS) used in the Coupled Model Intercomparison Project Phase 6 (CMIP6). The model captures well the spatial distributions and seasonal variations in tropospheric ozone, with seasonal mean biases of 0.4–2.2 ppbv at 700–400 hPa compared to satellite observations and within 10 ppbv at the surface to 500 hPa compared to global ozonesonde observations. The model has larger high-ozone biases over the tropics which we attribute to an overestimate of ozone chemical production. It underestimates ozone in the upper troposphere which is likely due either to the use of a simplified stratospheric ozone scheme or to biases in estimated stratosphere–troposphere exchange dynamics. The model diagnoses the global tropospheric ozone burden, OH concentration, and methane chemical lifetime to be 336 Tg, 1.16×106 molecule cm−3, and 8.3 years, respectively, which is consistent with recent multimodel assessments. The spatiotemporal distributions of NO2, CO, SO2, CH2O, and aerosol optical depth are generally in agreement with satellite observations. The development of BCC-GEOS-Chem v1.0 represents an important step for the development of fully coupled earth system models (ESMs) in China.
Haikun Wang, Xiaojing He, Xinyu Liang, Ernani F. Choma, Yifan Liu, Li Shan, Haotian Zheng, Shaojun Zhang, Chris P. Nielsen, Shuxiao Wang, Ye Wu, and John S. Evans. 2020. “Health benefits of on-road transportation pollution control programs in China.” Proceedings of the National Academy of Sciences, Sept 2020, 201921271. Publisher's VersionAbstract
China started to implement comprehensive measures to mitigate traffic pollution at the end of 1990s, but the comprehensive effects, especially on ambient air quality and public health, have not yet been systematically evaluated. In this study, we analyze the effects of vehicle emission control measures on ambient air pollution and associated deaths attributable to long-term exposures of fine particulate matter (PM2.5) and O3 based on an integrated research framework that combines scenario analysis, air quality modeling, and population health risk assessment. We find that the total impact of these control measures was substantial. Vehicular emissions during 1998–2015 would have been 2–3 times as large as they actually were, had those measures not been implemented. The national population-weighted annual average concentrations of PM2.5 and O3 in 2015 would have been higher by 11.7 μg/m3 and 8.3 parts per billion, respectively, and the number of deaths attributable to 2015 air pollution would have been higher by 510 thousand (95% confidence interval: 360 thousand to 730 thousand) without these controls. Our analysis shows a concentration of mortality impacts in densely populated urban areas, motivating local policymakers to design stringent vehicle emission control policies. The results imply that vehicle emission control will require policy designs that are more multifaceted than traditional controls, primarily represented by the strict emission standards, with careful consideration of the challenges in coordinated mitigation of both PM2.5 and O3 in different regions, to sustain improvement in air quality and public health given continuing swift growth in China’s vehicle population.
Shaojie Song, Athanasios Nenes, Meng Gao, Yuzhong Zhang, Pengfei Liu, Jingyuan Shao, Dechao Ye, Weiqi Xu, Lu Lei, Yele Sun, Baoxian Liu, Shuxiao Wang, and Michael B. McElroy. 2019. “Thermodynamic modeling Suggests declines in water uptake and acidity of inorganic aerosols in Beijing winter haze events during 2014/2015–2018/2019.” Environmental Science & Technology Letters, 6, Pp. 752-760. Publisher's VersionAbstract
During recent years, aggressive air pollution mitigation measures in northern China have resulted in considerable changes in gas and aerosol chemical composition. But it is unclear whether aerosol water content and acidity respond to these changes. The two parameters have been shown to affect heterogeneous production of winter haze aerosols. Here, we performed thermodynamic equilibrium modeling using chemical and meteorological data observed in urban Beijing for four recent winter seasons and quantified the changes in the mass growth factor and pH of inorganic aerosols. We focused on high relative humidity (>60%) conditions when submicron particles have been shown to be in the liquid state. From 2014/2015 to 2018/2019, the modeled mass growth factor decreased by about 9%–17% due to changes in aerosol compositions (more nitrate and less sulfate and chloride), and the modeled pH increased by about 0.3–0.4 unit mainly due to rising ammonia. A buffer equation is derived from semivolatile ammonia partitioning, which helps understand the sensitivity of pH to meteorological and chemical variables. The findings provide implications for evaluating the potential chemical feedback in secondary aerosol production and the effectiveness of ammonia control as a measure to alleviate winter haze.
S.J. Song, M. Gao, W.Q. Xu, Y.L. Sun, D.R. Worsnop, J.T. Jayne, Y.Z. Zhang, L. Zhu, M. Li, Z. Zhou, C.L. Cheng, Y.B. Lv, Y. Wang, W. Peng, X.B. Xu, N. Lin, Y.X. Wang, S.X. Wang, J. W. Munger, D. Jacob, and M.B. McElroy. 2019. “Possible heterogeneous hydroxymethanesulfonate (HMS) chemistry in northern China winter haze and implications for rapid sulfate formation.” Atmospheric Chemistry and Physics, 19, Pp. 1357-1371. Publisher's VersionAbstract
The chemical mechanisms responsible for rapid sulfate production, an important driver of winter haze formation in northern China, remain unclear. Here, we propose a potentially important heterogeneous hydroxymethanesulfonate (HMS) chemical mechanism. Through analyzing field measurements with aerosol mass spectrometry, we show evidence for a possible significant existence in haze aerosols of organosulfur primarily as HMS, misidentified as sulfate in previous observations. We estimate that HMS can account for up to about one-third of the sulfate concentrations unexplained by current air quality models. Heterogeneous production of HMS by SO2 and formaldehyde is favored under northern China winter haze conditions due to high aerosol water content, moderately acidic pH values, high gaseous precursor levels, and low temperature. These analyses identify an unappreciated importance of formaldehyde in secondary aerosol formation and call for more research on sources and on the chemistry of formaldehyde in northern China winter.
Haikun Wang, Xi Lu, Yu Deng, Yaoguang Sun, Chris P. Nielsen, Yifan Liu, Ge Zhu, Maoliang Bu, Jun Bi, and Michael B. McElroy. 2019. “China’s CO2 peak before 2030 implied from diverse characteristics and growth of cities.” Nature Sustainability, 2, Pp. 748–754. Publisher's VersionAbstract
China pledges to peak CO2 emissions by 2030 or sooner under the Paris Agreement to limit global warming to 2 °C or less by the end of the century. By examining CO2 emissions from 50 Chinese cities over the period 2000–2016, we found a close relationship between per capita emissions and per capita gross domestic product (GDP) for individual cities, following the environmental Kuznets curve, despite diverse trajectories for CO2 emissions across the cities. Results show that carbon emissions peak for most cities at a per capita GDP (in 2011 purchasing power parity) of around US$21,000 (80% confidence interval: US$19,000 to 22,000). Applying a Monte Carlo approach to simulate the peak of per capita emissions using a Kuznets function based on China’s historical emissions, we project that emissions for China should peak at 13–16 GtCO2 yr−1 between 2021 and 2025, approximately 5–10 yr ahead of the current Paris target of 2030. We show that the challenges faced by individual types of Chinese cities in realizing low-carbon development differ significantly depending on economic structure, urban form and geographical location.
Peter Sherman, Meng Gao, Shaojie Song, Patrick Ohiomoba, Alex Archibald, and Michael B. McElroy. 2019. “The influence of dynamics and emissions changes on China’s wintertime haze.” Journal of Applied Meteorology and Climatology, 58, Pp. 1603-1611. Publisher's VersionAbstract
Haze days induced by aerosol pollution in North and East China have posed a persistent and growing problem over the past few decades. These events are particularly threatening to densely-populated cities such as Beijing. While the sources of this pollution are predominantly anthropogenic, natural climate variations may also play a role in allowing for atmospheric conditions conducive to formation of severe haze episodes over populated areas. Here, an investigation is conducted into the effects of changes in global dynamics and emissions on air quality in China’s polluted regions using 35 simulations developed from the Community Earth Systems Model Large Ensemble (CESM LENS) run over the period 1920-2100. It is shown that internal variability significantly modulates aerosol optical depth (AOD) over China; it takes roughly a decade for the forced response to balance the effects from internal variability even in China’s most polluted regions. Random forest regressions are used to accurately model (R2 > 0.9) wintertime AOD using just climate oscillations, the month of the year and emissions. How different phases of each oscillation affect aerosol loading are projected using these regressions. AOD responses are identified for each oscillation, with particularly strong responses from El Niño-Southern Oscillation (ENSO) and the Pacific Decadal Oscillation (PDO). As ENSO can be projected a few months in advance and improvements in linear inverse modelling (LIM) may yield a similar predictability for the PDO, results of this study offer opportunities to improve the predictability of China’s severe wintertime haze events, and to inform policy options that could mitigate subsequent health impacts.
Yan Zhang, Xin Bo, Yu Zhao, and Chris P. Nielsen. 2019. “Benefits of current and future policies on emissions of China's coal-fired power sector indicated by continuous emission monitoring.” Environmental Pollution, 251, Pp. 415-424. Publisher's VersionAbstract
Emission inventories are critical to understanding the sources of air pollutants, but have high uncertainties in China due in part to insufficient on-site measurements. In this study, we developed a method of examining, screening and applying online data from the country's improving continuous emission monitoring systems (CEMS) to reevaluate a “bottom-up” emission inventory of China's coal-fired power sector. The benefits of China's current national emission standards and ultra-low emission policy for the sector were quantified assuming their full implementation. The derived national average emission factors of SO2, NOx and particulate matter (PM) were 1.00, 1.00 and 0.25 kg/t-coal respectively for 2015 based on CEMS data, smaller than those of previous studies that may not fully recognize improved emission controls in recent years. The annual emissions of SO2, NOx and PM from the sector were recalculated at 1321, 1430 and 334 Gg respectively, 75%, 63% and 76% smaller than our estimates based on a previous approach without the benefit of CEMS data. The results imply that online measurement with proper data screening can better track the recent progress of emission controls. The emission intensity (the ratio of emissions to economic output) of Northwest China was larger than that of other regions, attributed mainly to its less intensive economy and industry. Transmission of electricity to more-developed eastern provinces raised the energy consumption and emissions of less-developed regions. Judged by 95 percentiles of flue-gas concentrations measured by CEMS, most power plants met the current national emission standards in 2015 except for those in Northwest and Northeast China, while plants that met the ultra-low emission policy were much scarcer. National SO2, NOx and PM emissions would further decline by 68%, 55% and 81% respectively if the ultra-low emission policy can be strictly implemented, implying the great potential of the policy for emission abatement.

April 8, 2019

March 8, 2019

2019 Mar 07

# China and Asia in a Changing Climate: Natural Science for the Non-Scientist

12:15pm to 1:45pm

## Location:

CGIS South S020, Belfer Case Study Room, 1730 Cambridge St., Cambridge, MA

Panelists:

• Professor John Holdren, Teresa and John Heinz Professor of Environmental Policy, Harvard Kennedy School (HKS) and Department of Earth and Planetary Sciences, Harvard University; Co-Director of Science, Technology, and Public Policy Program, HKS; former Science Advisor to President Barack Obama and former Director of the White House Office of Science and Technology Policy
• Professor Peter Huybers, Department of Earth and Planetary Sciences, Harvard University, and Harvard John A. Paulson School of Engineering and Applied Sciences
• Professor Elsie Sunderland, Gordon McKay Professor of Environmental Chemistry, Harvard John A. Paulson School of Engineering and Applied Sciences and Harvard T.H. Chan School of Public Health
• Professor Steve Wofsy, Abbott Lawrence Rotch Professor of Atmospheric and Environmental Science, Department of Earth and Planetary Sciences, Harvard University, and Harvard John A. Paulson School of Engineering and Applied Sciences

Chair: Professor Mike McElroy, Gilbert Butler Professor of Environmental Studies, Department of Earth and Planetary Sciences, Harvard University, and Harvard John A. Paulson School of Engineering and Applied Sciences; Chair, Harvard-China Project on Energy, Economy and Environment... Read more about China and Asia in a Changing Climate: Natural Science for the Non-Scientist

Peng Jiang, Hongyan Liu, Shilong Piao, Philippe Ciais, Xiuchen Wu, Yi Yin, and Hongya Wang. 2019. “Enhanced growth after extreme wetness compensates for post-drought carbon loss in dry forests.” Nature Communications, 10, 195. Publisher's VersionAbstract
While many studies have reported that drought events have substantial negative legacy effects on forest growth, it remains unclear whether wetness events conversely have positive growth legacy effects. Here, we report pervasive and substantial growth enhancement after extreme wetness by examining tree radial growth at 1929 forest sites, satellite-derived vegetation greenness, and land surface model simulations. Enhanced growth after extreme wetness lasts for 1 to 5 years and compensates for 93 ± 8% of the growth deficit after extreme drought across global water-limited regions. Remarkable wetness-enhanced growths are observed in dry forests and gymnosperms, whereas the enhanced growths after extreme wetness are much smaller in wet forests and angiosperms. Limited or no enhanced growths are simulated by the land surface models after extreme wetness. These findings provide new evidence for improving climate-vegetation models to include the legacy effects of both drought and wet climate extremes.
Jianxiong Sheng, Shaojie Song, Yuzhong Zhang, Ronald G. Prinn, and Greet Janssens-Maenhout. 2019. “Bottom-up estimates of coal mine methane emissions in China: A gridded inventory, emission factors, and trends.” Environmental Science and Technology Letters. Publisher's VersionAbstract
China has large but uncertain coal mine methane (CMM) emissions. Inverse modeling (top-down) analyses of atmospheric methane observations can help improve the emission estimates but require reliable emission patterns as prior information. To serve this urgent need, we developed a high-resolution (0.25° × 0.25°) methane emission inventory for China’s coal mining using a recent publicly available database of more than 10000 coal mines in China for 2011. This number of coal mines is 25 and 2.5 times, respectively, more than the number available in the EDGAR v4.2 and EDGAR v4.3.2 gridded global inventories, which have been extensively used in past inverse analyses. Our inventory shows large differences with the EDGAR v4.2 as well as its more recent version, EDGAR v4.3.2. Our results suggest that China’s CMM emissions have been decreasing since 2012 on the basis of coal mining activities and assuming time-invariant emission factors but that regional trends differ greatly. Use of our inventory as prior information in future inverse modeling analyses can help better quantify CMM emissions as well as more confidently guide the future mitigation of coal to gas in China.
Meng Gao, Yihui Ding, Shaojie Song, Xiao Lu, Xinyu Chen, and Michael B. McElroy. 2018. “Secular decrease of wind power potential in India associated with warming Indian Ocean.” Science Advances, 4, 12. Publisher's VersionAbstract
The Indian government has set an ambitious target for future renewable power generation, including 60 GW of cumulative wind power capacity by 2022. However, the benefits of these substantial investments are vulnerable to the changing climate. On the basis of hourly wind data from an assimilated meteorology reanalysis dataset covering the 1980–2016 period, we show that wind power potential may have declined secularly over this interval, particularly in western India. Surface temperature data confirm that significant warming occurred in the Indian Ocean over the study period, leading to modulation of high pressure over the ocean. A multivariable linear regression model incorporating the pressure gradient between the Indian Ocean and the Indian subcontinent can account for the interannual variability of wind power. A series of numerical sensitivity experiments confirm that warming in the Indian Ocean contributes to subsidence and dampening of upward motion over the Indian continent, resulting potentially in weakening of the monsoonal circulation and wind speeds over India.