Air Pollution, Greenhouse Gases & Climate

In Press
Hewen Zhou, Qing Yang, Pietro Bartocci, Francesco Fantozzi, Ondřej Mašek, Foster A. Agblevor, Zhiyu Wei, Haiping Yang, Hanping Chen, Xi Lu, Guoqing Chen, Chuguang Zheng, Chris P. Nielsen, and Michael B. McElroy. In Press. “Prospective contributions of biomass pyrolysis to China’s 2050 carbon reduction and renewable energy goals.” Nature Communications.
2020
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, 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.
Haotian Zheng, Shaojie Song, Golam Sarwar, Masao Gen, Shuxiao Wang, Dian Ding, Xing Chang, Shuping Zhang, Jia Xing, Yele Sun, Dongsheng Ji, Chak Chan, Jian Gao, and Michael B. McElroy. 2020. “Contribution of Particulate Nitrate Photolysis to Heterogeneous Sulfate Formation for Winter Haze in China.” Environmental Science & Technology Letters , 7, 9, Pp. 632–638. Publisher's VersionAbstract
Nitrate and sulfate are two key components of airborne particulate matter (PM). While multiple formation mechanisms have been proposed for sulfate, current air quality models commonly underestimate its concentrations and mass fractions during northern China winter haze events. On the other hand, current models usually overestimate the mass fractions of nitrate. Very recently, laboratory studies have proposed that nitrous acid (N(III)) produced by particulate nitrate photolysis can oxidize sulfur dioxide to produce sulfate. Here, for the first time, we parameterize this heterogeneous mechanism into the state-of-the-art Community Multi-scale Air Quality (CMAQ) model and quantify its contributions to sulfate formation. We find that the significance of this mechanism mainly depends on the enhancement effects (by 1–3 orders of magnitude as suggested by the available experimental studies) of nitrate photolysis rate constants in aerosol liquid water compared to that in the gas phase. Comparisons between model simulations and in-situ observations in Beijing suggest that this pathway can explain about 15% (assuming an enhancement factor (EF) of 10) to 65% (assuming EF = 100) of the model–observation gaps in sulfate concentrations during winter haze. Our study strongly calls for future research on reducing the uncertainty in EF.
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.
Archana Dayalu, J. William Munger, Yuxuan Wang, Steven C. Wofsy, Yu Zhao, Thomas Nehrkorn, Chris P. Nielsen, Michael B. McElroy, and Rachel Chang. 2020. “Evaluating China's anthropogenic CO2 emissions inventories: a northern China case study using continuous surface observations from 2005 to 2009.” Atmospheric Chemistry and Physics. Publisher's VersionAbstract
China has pledged reduction of carbon dioxide (CO2) emissions per unit of gross domestic product (GDP) by 60 %–65 % relative to 2005 levels, and to peak carbon emissions overall by 2030. However, the lack of observational data and disagreement among the many available inventories makes it difficult for China to track progress toward these goals and evaluate the efficacy of control measures. To demonstrate the value of atmospheric observations for constraining CO2 inventories we track the ability of CO2 concentrations predicted from three different CO2 inventories to match a unique multi-year continuous record of atmospheric CO2. Our analysis time window includes the key commitment period for the Paris Agreement (2005) and the Beijing Olympics (2008). One inventory is China-specific and two are spatial subsets of global inventories. The inventories differ in spatial resolution, basis in national or subnational statistics, and reliance on global or China-specific emission factors. We use a unique set of historical atmospheric observations from 2005 to 2009 to evaluate the three CO2 emissions inventories within China's heavily industrialized and populated northern region accounting for ∼33 %–41 % of national emissions. Each anthropogenic inventory is combined with estimates of biogenic CO2 within a high-resolution atmospheric transport framework to model the time series of CO2 observations. To convert the model–observation mismatch from mixing ratio to mass emission rates we distribute it over a region encompassing 90 % of the total surface influence in seasonal (annual) averaged back-trajectory footprints (L_0.90 region). The L_0.90 region roughly corresponds to northern China. Except for the peak growing season, where assessment of anthropogenic emissions is entangled with the strong vegetation signal, we find the China-specific inventory based on subnational data and domestic field studies agrees significantly better with observations than the global inventories at all timescales. Averaged over the study time period, the unscaled China-specific inventory reports substantially larger annual emissions for northern China (30 %) and China as a whole (20 %) than the two unscaled global inventories. Our results, exploiting a robust time series of continuous observations, lend support to the rates and geographic distribution in the China-specific inventory Though even long-term observations at a single site reveal differences among inventories, exploring inventory discrepancy over all of China requires a denser observational network in future efforts to measure and verify CO2 emissions for China both regionally and nationally. We find that carbon intensity in the northern China region has decreased by 47 % from 2005 to 2009, from approximately 4 kg of CO2 per USD (note that all references to USD in this paper refer to USD adjusted for purchasing power parity, PPP) in 2005 to about 2 kg of CO2 per USD in 2009 (Fig. 9c). However, the corresponding 18 % increase in absolute emissions over the same time period affirms a critical point that carbon intensity targets in emerging economies can be at odds with making real climate progress. Our results provide an important quantification of model–observation mismatch, supporting the increased use and development of China-specific inventories in tracking China's progress as a whole towards reducing emissions. We emphasize that this work presents a methodology for extending the analysis to other inventories and is intended to be a comparison of a subset of anthropogenic CO2 emissions rates from inventories that were readily available at the time this research began. For this study's analysis time period, there was not enough spatially distinct observational data to conduct an optimization of the inventories. The primary intent of the comparisons presented here is not to judge specific inventories, but to demonstrate that even a single site with a long record of high-time-resolution observations can identify major differences among inventories that manifest as biases in the model–data comparison. This study provides a baseline analysis for evaluating emissions from a small but important region within China, as well a guide for determining optimal locations for future ground-based measurement sites.
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Peter Sherman, Eli Tziperman, Clara Deser, and Michael B. McElroy. 2020. “Historical and future roles of internal atmospheric variability in modulating summertime Greenland Ice Sheet melt.” Geophysical Research Letters, 47, 6. Publisher's VersionAbstract
Understanding how internal atmospheric variability affects Greenland Ice Sheet (GrIS) summertime melting would improve understanding of future sea level rise. We analyze the Community Earth System Model Large Ensemble (CESM‐LE) over 1951‐2000 and 2051‐2100. We find that internal variability dominates the forced response on short timescales (~20 years) and that the area impacted by internal variability grows in the future, connecting internal variability and climate change. Unlike prior studies, we do not assume specific patterns of internal variability to affect GrIS melting, but derive them from Maximum Covariance Analysis. We find that the North Atlantic Oscillation (NAO) is the major source of internal atmospheric variability associated with GrIS melt conditions in CESM‐LE and reanalysis, with the positive phase (NAO+) linked to widespread cooling over the ice sheet. CESM‐LE and CMIP5 project an increase in the frequency of NAO+ events, suggesting a negative feedback to the GrIS under future climate change.
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Xueli Zhao, Xiaofang Wu, Chenghe Guan, Rong Ma, Chris P. Nielsen, and Bo Zhang. 2020. “Linking agricultural GHG emissions to the global trade network.” Earth's Future, 8, 3. Publisher's VersionAbstract
As part of the climate policy to meet the 2‐degrees Celsius (2 °C) target, actions in all economic sectors, including agriculture, are required to mitigate global greenhouse gas (GHG) emissions. While there has been an ever‐increasing focus on agricultural greenhouse gas (AGHG) emissions, limited attention has been paid to their economic drivers in the globalized world economy and related mitigation potentials. This paper makes a first attempt to trace AGHG emissions via global trade networks using a multi‐regional input‐output model and a complex network model. Over one third of global AGHG emissions in 2012 can be linked with products traded internationally, of which intermediate trade and final trade contribute 64.2% and 35.8%, respectively. Japan, the USA, Germany, the UK, and Hong Kong are the world's five largest net importers of embodied emissions, while Ethiopia, Australia, Pakistan, India and Argentina are the five largest net exporters. Some hunger‐afflicted developing countries in Asia and Africa are important embodied emission exporters, due to their large‐scale exports of agricultural products. Trade‐related virtual AGHG emission transfers shape a highly heterogenous network, due to the coexistence of numerous peripheral economies and a few highly‐connected hub economies. The network clustering structure is revealed by the regional integration of several trading communities, while hub economies are collectors and distributors in the global trade network, with important implications for emission mitigation. Achieving AGHG emission reduction calls for a combination of supply‐ and demand‐side policies covering the global trade network.
AGU_Full_Text
Meng Gao, Jinhui Gao, Bin Zhu, Rajesh Kumar, Xiao Lu, Shaojie Song, Yuzhong Zhang, Beixi Jia, Peng Wang, Gufran Beig, Jianlin Hu, Qi Ying, Hongliang Zhang, Peter Sherman, and Michael B. McElroy. 2020. “Ozone pollution over China and India: seasonality and sources.” Atmospheric Chemistry and Physics, 20, 7, Pp. 4399-4414. Publisher's VersionAbstract
A regional fully coupled meteorology–chemistry model, Weather Research and Forecasting model with Chemistry (WRF-Chem), was employed to study the seasonality of ozone (O3) pollution and its sources in both China and India. Observations and model results suggest that O3 in the North China Plain (NCP), Yangtze River Delta (YRD), Pearl River Delta (PRD), and India exhibit distinctive seasonal features, which are linked to the influence of summer monsoons. Through a factor separation approach, we examined the sensitivity of O3 to individual anthropogenic, biogenic, and biomass burning emissions. We found that summer O3 formation in China is more sensitive to industrial and biogenic sources than to other source sectors, while the transportation and biogenic sources are more important in all seasons for India. Tagged simulations suggest that local sources play an important role in the formation of the summer O3 peak in the NCP, but sources from Northwest China should not be neglected to control summer O3 in the NCP. For the YRD region, prevailing winds and cleaner air from the ocean in summer lead to reduced transport from polluted regions, and the major source region in addition to local sources is Southeast China. For the PRD region, the upwind region is replaced by contributions from polluted PRD as autumn approaches, leading to an autumn peak. The major upwind regions in autumn for the PRD are YRD (11 %) and Southeast China (10 %). For India, sources in North India are more important than sources in the south. These analyses emphasize the relative importance of source sectors and regions as they change with seasons, providing important implications for O3 control strategies.
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Jialin Liu, Fangyan Cheng, J. William Munger, Timothy G. Whitby, Peng Jiang, Siyue Chen, Weiwen Ji, and Xiuling Man. 2020. “Precipitation extremes influence patterns and partitioning of evapotranspiration and transpiration in a deciduous boreal larch forest.” Agricultural and Forest Meteorology, 287, 107936. Publisher's VersionAbstract
Ecosystems at the margins of their zone could be amongst the first to experience significant shifts in structure and function. At this site there have already been signs of permafrost degradation and more frequent temperature and precipitation anomalies. The canopy-dominant larch accounted for half the total T fluxes. The remaining 50% was distributed evenly among intermediate and suppressed trees. T is the dominant subcomponent in ET, where overall T/ET varies of 66%–84% depending on precipitation patterns. In dormant and early growing seasons, T still constitutes a majority of ET even though the canopy foliage is not fully developed because cold soil creates a negative soil to air vapor pressure gradient that impedes evaporation. However, in the peak growing season, excess precipitation reduces T while providing sufficient wetness for surface evaporation. ET from standard data product based on MODIS satellite reflectance underestimates tower ET by 17%–29%. Solar-induced chlorophyll fluorescence measured by satellite is well correlated with tower ET (r2 = 0.69–0.73) and could provide a better basis for regional ET extrapolations. Sites along boreal ecotones are critical to observe for signs of shifts in their structure, function, and response to climate anomalies.
2019
Mengyao Han, Bo Zhang, Yuqing Zhang, and Chenghe Guan. 2019. “Agricultural CH4 and N2O emissions of major economies: Consumption- vs. production-based perspectives.” Journal of Cleaner Production, 210, Pp. 276-286. Publisher's VersionAbstract

Agriculture is one of the most important sectors for global anthropogenic methane (CH4) and nitrous oxide (N2O) emissions. While much attention has been paid to production-side agricultural non-CO2 greenhouse gas (ANGHG) emissions, less is known about the emissions from the consumption-based perspective. This paper aims to explore the characteristics of agricultural CH4 and N2O emissions of global major economies by using the latest emission data from the Food and Agriculture Organization Corporate Statistical Database (FAOSTAT) and the recently available global multi-regional input-output model from the World Input-Output Database (WIOD). The results show that in 2014, the 42 major economies together accounted for 60.7% and 65.0% of global total direct and embodied ANGHG emissions, respectively. The consumption-based ANGHG emissions in the US, Japan, and the EU were much higher than their production-based emissions, while the converse was true for Brazil, Australia, and India. The global-average embodied ANGHG emissions per capita was 0.7 t CO2-eq, but major developing countries such as China, India, Indonesia and Mexico were all below this average value. We find that the total transfer of embodied ANGHG emissions via international trade was 622.4 Mt CO2-eq, 11.9% of the global total. China was the largest exporter of embodied ANGHG emissions, while the US was the largest importer. Most developed economies were net importers of embodied emissions. Mexico-US, China-US, China-EU, China-Japan, China-Russia, Brazil-EU, India-EU and India-US formed the main bilateral trading pairs of embodied emission flows. Examining consumption-based inventories can be useful for understanding the impacts of final demand and international trade on agricultural GHG emissions and identifying appropriate mitigation potentials along global supply chains.

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.
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.
ESTLett paper.pdf
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.

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.
Ying Wang, Bin Chen, Chenghe Guan, and Bo Zhang. 2019. “Evolution of methane emissions in global supply chains during 2000-2012.” Resources, Conservation and Recycling, 150, 104414. Publisher's VersionAbstract
Reduction of methane emissions (CH4) plays an important role in addressing global climate change. Most previous studies have focused on the direct CH4 emissions of economies, but overlooked the upstream CH4 emissions along global supply chains induced by the final consumption of economies. Using a global multi-regional input-output analysis, this study aims to explore the evolution of CH4 emissions embodied in international trade and final consumption in major economies during 2000–2012. The results show that China, the EU, USA, India and Brazil were the top five economies with high volumes of consumption-based CH4 emissions from 2000 to 2012. In particular, China’s consumption-based CH4 emissions showed an observable growth trend, while the EU, the USA and Japan showed a downward trend. It’s estimated that growing amounts of CH4 emissions (i.e., the volume increase from 77.1 Mt in 2000 to 95.9 Mt in 2012) were transferred globally via international trade, primarily as exports from China, Russia and other large developing economies to consumers in major developed economies. Russia–EU, China–USA and China–EU formed the main bilateral trading pairs of embodied emission flows. Further analysis found that per capita consumption-based CH4 emissions was closely related to their per capita GDP. Quantifying the CH4 emissions embodied in trade and final demand of major economies can provide important basis for understanding economy-wide emission drivers to design global and regional CH4 reduction scheme from a consumer perspective.
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.

JAMC paper
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.
ACP paper
Wenjie Tian, Xudong Wu, Rong Ma, and Bo Zhang. 2019. “Quantifying global CH4 and N2O footprints.” Journal of Environmental Management, 251, 109566. Publisher's VersionAbstract
This study aims to quantify global CH4 and N2O footprints in 2012 in terms of 181 economies and 20 world regions based on the official national emission accounts from the UNFCCC database and the global multi-region input-output accounts from the EORA database. Global total CH4 and N2O emissions increased by 15.0% in 2012 compared to 1990, mainly driven by increasing demands of agricultural and energy products. Mainland China, Western Europe, the USA, Southeast Asia and Sub-Saharan Africa were identified as the largest five CH4 footprint contributors (55.6% of the global total), while Mainland China, the USA, Western Europe, Brazil and Sub-Saharan Africa as the largest N2O footprint contributors (59.2% of the global total). In most developed economies, the CH4 and N2O footprints were much higher than their emissions on the production side, but opposite picture is observed in emerging economies. 36.4% and 24.8% of the global CH4 and N2O emissions in 2012 were associated with international trade, respectively. Substantial energy-related CH4 and agricultural CH4 and N2O emissions were transferred from developed countries to developing countries. Several nations within Kyoto targets have reduced their CH4 and N2O emissions significantly between 1990 and 2012, but the generally-believed success is challenged when viewing from the consumption side. Mainland China, Southeast Asia, Sub-Saharan Africa, Brazil, Middle East and India witnessed prominent increase of CH4 and N2O footprints in the same period. The structure and spatial patterns of global CH4 and N2O footprints shed light on the role of consumption-side actions and international cooperation for future non-CO2 GHG emission reduction.
Meng Gao, Peter Sherman, Shaojie Song, Yueyue Yu, Zhiwei Wu, and Michael B. McElroy. 2019. “Seasonal prediction of Indian wintertime aerosol pollution using the Ocean Memory Effect.” Science Advances, 5, 7. Publisher's VersionAbstract
As China makes every effort to control air pollution, India emerges as the world’s most polluted country, receiving worldwide attention with frequent winter (boreal) haze extremes. In this study, we found that the interannual variability of wintertime aerosol pollution over northern India is regulated mainly by a combination of El Niño and the Antarctic Oscillation (AAO). Both El Niño sea surface temperature (SST) anomalies and AAO-induced Indian Ocean Meridional Dipole SST anomalies can persist from autumn to winter, offering prospects for a prewinter forecast of wintertime aerosol pollution over northern India. We constructed a multivariable regression model incorporating El Niño and AAO indices for autumn to predict wintertime AOD. The prediction exhibits a high degree of consistency with observation, with a correlation coefficient of 0.78 (P < 0.01). This statistical model could allow the Indian government to forecast aerosol pollution conditions in winter and accordingly improve plans for pollution control.
Science_Advances_Paper.pdf
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.

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