Atmospheric Modeling

Shaojie Song, Tao Ma, Yuzhong Zhang, Lu Shen, Pengfei Liu, Ke Li, Shixian Zhai, Haotian Zheng, Meng Gao, Jonathan M. Moch, Fengkui Duan, Kebin He, and Michael B. McElroy. 2021. “Global modeling of heterogeneous hydroxymethanesulfonate chemistry.” Atmospheric Chemistry and Physics, 21, 1, Pp. 457–481. Publisher's VersionAbstract
Hydroxymethanesulfonate (HMS) has recently been identified as an abundant organosulfur compound in aerosols during winter haze episodes in northern China. It has also been detected in other regions although the concentrations are low. Because of the sparse field measurements, the global significance of HMS and its spatial and seasonal patterns remain unclear. Here, we modify and add to the implementation of HMS chemistry in the GEOS-Chem chemical transport model and conduct multiple global simulations. The model accounts for cloud entrainment and gas–aqueous mass transfer within the rate expressions for heterogeneous sulfur chemistry. Our simulations can generally reproduce quantitative HMS observations from Beijing and show that East Asia has the highest HMS concentration, followed by Europe and North America. The simulated HMS shows a seasonal pattern with higher values in the colder period. Photochemical oxidizing capacity affects the competition of formaldehyde with oxidants (such as ozone and hydrogen peroxide) for sulfur dioxide and is a key factor influencing the seasonality of HMS. The highest average HMS concentration (1–3 µg m−3) and HMS ∕ sulfate molar ratio (0.1–0.2) are found in northern China in winter. The simulations suggest that aqueous clouds act as the major medium for HMS chemistry while aerosol liquid water may play a role if its rate constant for HMS formation is greatly enhanced compared to cloud water.
Haikun Wang, Xiaojing He, Xinyu Liang, Ernani F. Choma, Yifan Liu, Li Shan, Haotian Zheng, Shaojun Zhang, Chris Nielsen, Shuxiao Wang, Ye Wu, and John Evans. 2020. “Health benefits of on-road transportation pollution control programs in China.” Proceedings of the National Academy of Sciences, 117, 41, Pp. 25370-25377. 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, 12, 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.
China’s CO2 peak before 2030 implied from diverse characteristics and growth of cities
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, 7, 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, August, 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.
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 SunderlandGordon 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

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, 6, 8, Pp. 473-478. 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.
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.

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