Benzenepoly(carboxylic acid)s as Exclusive Intrinsic Markers to Assess Riverine Export of Dissolved Black Carbon.

Landscape fires annually generate large quantities of black carbon. The water-soluble fraction of black carbon (i.e., dissolved black carbon/DBC) is an important constituent of the dissolved organic carbon (DOC) pool, playing a crucial role in the global budget of refractory carbon and climate change. A key challenge in constraining the flux and fate of riverine DBC is to develop targeted and accurate quantification methods. Herein, we report that benzenepentacarboxylic acid (B5CA) intrinsically present in DBC can be used as an exclusive and holistic marker (representing both condensed aromatics and less-/nonaromatic fractions) for DBC quantification. B5CA was universally detected in water extractions of biochar and fire-affected soils with relatively large abundance but not produced by nonthermogenic processes. It has good mobility in the environment as it is not readily precipitated by cations or adsorbed by common geosorbents. B5CA also represents the recalcitrant components of DBC with excellent stability against photodegradation and biodegradation. Applying B5CA as the DBC marker in surface waters of the Changjiang River (i.e., the third largest river in the world), we calculate the DBC concentration in the downstream Changjiang River to be 4.8 ± 5.5% of the DOC flux. Our work provides a simple and reliable approach for the accurate quantification and source tracking of DBC in the soil and aquatic carbon pools.

The contributions of individual countries and regions to the global radiative forcing.

Knowing the historical relative contribution of greenhouse gases (GHGs) and short-lived climate forcers (SLCFs) to global radiative forcing (RF) at the regional level can help understand how future GHGs emission reductions and associated or independent reductions in SLCFs will affect the ultimate purpose of the Paris Agreement. In this study, we use a compact Earth system model to quantify the global RF and attribute global RF to individual countries and regions. As our evaluation, the United States, the first 15 European Union members, and China are the top three contributors, accounting for 21.9 ± 3.1%, 13.7 ± 1.6%, and 8.6 ± 7.0% of global RF in 2014, respectively. We also find a contrast between developed countries where GHGs dominate the RF and developing countries where SLCFs including aerosols and ozone are more dominant. In developing countries, negative RF caused by aerosols largely masks the positive RF from GHGs. As developing countries take measures to improve the air quality, their negative contributions from aerosols will likely be reduced in the future, which will in turn enhance global warming. This underlines the importance of reducing GHG emissions in parallel to avoid any detrimental consequences from air quality policies.

Divergent Energy-Climate Nexus in the Global Fuel Combustion Processes.

Fuel combustion provides basic energy for the society but also produces CO2 and incomplete combustion products that threaten human survival, climate change, and global sustainability. A variety of fuels burned in different facilities expectedly have distinct impacts on climate, which remains to be quantitatively assessed. This study uses updated emission inventories and an earth system model to evaluate absolute and relative contributions in combustion emission-associated climate forcing by fuels, sectors, and regions. We showed that, from 1970 to 2014, coal burned in the energy sector and oil used in the transportation sector contributed comparable energies consumed (24 and 20% of the total) but had distinct climate forcing (1 and 40%, respectively). Globally, coal burned for energy production had negative impacts on climate forcing but positive effects in the residential sector. In many developing countries, coal combustion in the energy sector had negative radiative forcing (RF) per unit energy consumed due to insufficient controls on sulfur and scattering aerosol levels, but oils in the transportation sector had high positive RF values. These results had important implications on the energy transition and emission reduction actions in response to climate change. Distinct climate efficiencies of energies and the spatial heterogeneity implied differentiated energy utilization strategies and pollution control policies by region and sector.

The contribution of China's emissions to global climate forcing.

Knowledge of the contribution that individual countries have made to global radiative forcing is important to the implementation of the agreement on "common but differentiated responsibilities" reached by the United Nations Framework Convention on Climate Change. Over the past three decades, China has experienced rapid economic development, accompanied by increased emission of greenhouse gases, ozone precursors and aerosols, but the magnitude of the associated radiative forcing has remained unclear. Here we use a global coupled biogeochemistry-climate model and a chemistry and transport model to quantify China's present-day contribution to global radiative forcing due to well-mixed greenhouse gases, short-lived atmospheric climate forcers and land-use-induced regional surface albedo changes. We find that China contributes 10% ± 4% of the current global radiative forcing. China's relative contribution to the positive (warming) component of global radiative forcing, mainly induced by well-mixed greenhouse gases and black carbon aerosols, is 12% ± 2%. Its relative contribution to the negative (cooling) component is 15% ± 6%, dominated by the effect of sulfate and nitrate aerosols. China's strongest contributions are 0.16 ± 0.02 watts per square metre for CO2 from fossil fuel burning, 0.13 ± 0.05 watts per square metre for CH4, -0.11 ± 0.05 watts per square metre for sulfate aerosols, and 0.09 ± 0.06 watts per square metre for black carbon aerosols. China's eventual goal of improving air quality will result in changes in radiative forcing in the coming years: a reduction of sulfur dioxide emissions would drive a faster future warming, unless offset by larger reductions of radiative forcing from well-mixed greenhouse gases and black carbon.

Energy and air pollution benefits of household fuel policies in northern China.

In addition to many recent actions taken to reduce emissions from energy production, industry, and transportation, a new campaign substituting residential solid fuels with electricity or natural gas has been launched in Beijing, Tianjin, and 26 other municipalities in northern China, aiming at solving severe ambient air pollution in the region. Quantitative analysis shows that the campaign can accelerate residential energy transition significantly, and if the planned target can be achieved, more than 60% of households are projected to remove solid fuels by 2021, compared with fewer than 20% without the campaign. Emissions of major air pollutants will be reduced substantially. With 60% substitution realized, emission of primary PM2.5 and contribution to ambient PM2.5 concentration in 2021 are projected to be 30% and 41% of those without the campaign. With 60% substitution, average indoor PM2.5 concentrations in living rooms in winter are projected to be reduced from 209 (190 to 230) µg/m3 to 125 (99 to 150) µg/m3 The population-weighted PM2.5 concentrations can be reduced from 140 µg/m3 in 2014 to 78 µg/m3 or 61 µg/m3 in 2021 given that 60% or 100% substitution can be accomplished. Although the original focus of the campaign was to address ambient air quality, exposure reduction comes more from improved indoor air quality because ∼90% of daily exposure of the rural population is attributable to indoor air pollution. Women benefit more than men.

Updated Global Black Carbon Emissions from 1960 to 2017: Improvements, Trends, and Drivers.

Accurate estimation of black carbon (BC) emissions is essential for assessing the health and climate impact of this pollutant. Past emission inventories were associated with high uncertainty due to data limitations, and recent information has provided a unique updating opportunity. Moreover, understanding the drivers that cause temporal emission changes is of research value. Here, we update the global BC emission estimates using new data on the activities and emission factors (EFs). The new inventory covers 73 detailed sources at 0.1° × 0.1° spatial resolution and monthly temporal resolution from 1960 to 2017. The estimated annual emissions were 32% higher than the average of several previous inventories, which was primarily due to field-measured EFs for residential stoves and differentiated EFs for motor vehicles. In addition, the updated emissions show an inverse U-shaped temporal trend, which was mainly driven by the interaction between the positive effects of population growth, per capita energy consumption, and vehicle fleet and the negative effects of residential energy switching, stove upgrading, phasing out of beehive coke ovens, and reduced EFs for vehicles and industrial processes. Urbanization caused a significant increase in urban emissions accompanied by a more significant decline in rural emissions.

Direct and Inverse Reduced-Form Models for Reciprocal Calculation of BC Emissions and Atmospheric Concentrations.

Atmospheric black carbon (BC) concentrations are governed by both emissions and meteorological conditions. Distinguishing these effects enables quantification of the effectiveness of emission mitigation actions by excluding meteorological effects. Here, we develop reduced-form models in both direct (RFDMs) and inverse (RFIMs) modes to estimate ambient BC concentrations. The models were developed based on outputs from multiyear simulations under three conditional scenarios with realistic or fixed emissions and meteorological conditions. We established a set of probabilistic functions (PFs) to quantify the meteorological influences. A significant two-way linear relationship between multiyear annual emissions and mean ambient BC concentrations was revealed at the grid cell scale. The correlation between them was more significant at grid cells with high emission densities. The concentrations and emissions at a given grid cell are also significantly correlated with emissions and concentrations of the surrounding areas, respectively, although to a lesser extent. These dependences are anisotropic depending on the prevailing winds and source regions. The meteorologically induced variation at the monthly scale was significantly higher than that at the annual scale. Of the major meteorological parameters, wind vectors, temperature, and relative humidity were found to most significantly affect variation in ambient BC concentrations.

Coal Is Dirty, but Where It Is Burned Especially Matters.

Coal abatement actions for pollution reduction often target total coal consumption. The health impacts of coal uses, however, vary extensively among sectors. Here, we modeled the sectorial contributions of coal uses to emissions, outdoor and indoor PM2.5 (particulate matter with an aerodynamic diameter of less than 2.5 mm) concentrations, exposures, and health outcomes in China from 1970 to 2014. We show that in 2014, residential coal accounted for 2.9% of total energy use but 34% of premature deaths associated with PM2.5 exposure, showing that effects were magnified substantially along the causal path. The number of premature deaths attributed to unit coal consumption in the residential sector was 40 times higher than that in the power and industrial sectors. Emissions of primary PM2.5 were more important than secondary aerosol precursors in terms of health consequences, and indoor exposure accounted for 97% and 91% of total premature deaths attributable to PM2.5 from coal combustion in 1974 and 2014, respectively. Our assessment raises a critical challenge in the switching of residential coal uses to effectively mitigate PM2.5 exposure in the Chinese population.

Spatially Resolved Emission Factors to Reduce Uncertainties in Air Pollutant Emission Estimates from the Residential Sector.

The residential sector is a major source of air pollutant emission inventory uncertainties. A nationwide field emission measurement campaign was conducted in rural China to evaluate the variabilities of realistic emission factors (EFs) from indoor solid fuel combustion. For a total of 1313 burning events, the overall average EFs (±standard deviation) of PM2.5 were 8.93 ± 6.95 and 7.33 ± 9.01 g/kg for biomass and coals, respectively, and 89.3 ± 51.2 and 114 ± 87 g/kg for CO. Higher EFs were found from burning of uncompressed straws, while lower EFs were found from processed biomass pellets, coal briquettes, and relatively clean anthracite coals. Modified combustion efficiency was found to be the most significant factor associated with variations in CO EFs, whereas for PM2.5, fuel and stove differences determined its variations. Weak correlations between PM2.5 and CO indicated high uncertainties in using CO as a surrogate for PM2.5. EFs accurately fit log-normal distributions, and obvious spatial heterogeneity was observed attributed to different fuel-stove combinations across the country. Emission estimation variabilities, which are determined by the interquartile ranges divided by the median values, were notably reduced when spatially resolved EFs were adopted in the inventory.

Health effects of banning beehive coke ovens and implementation of the ban in China.

Environmental legislation and proper implementation are critical in environmental protection. In the past, beehive coke ovens (BCOs) were popular in China, resulting in enormous emissions of benzo[a]pyrene (BaP), a common indicator of carcinogenic polycyclic aromatic hydrocarbons. BCOs were banned by the Coal Law in 1996. Although BCO numbers have declined since the ban, they were not eliminated until 2011 due to poor implementation. Here, we present the results of a quantitative evaluation of the health effects of historical BCO operation, the health benefits of the ban, and the adverse impacts of the poor implementation of the ban. With only limited official statistics available, historical and geospatial data about BCOs were reconstructed based on satellite images. Emission inventories of BaP from BCOs were compiled and used to model atmospheric transport, nonoccupational population exposure, and induced lung cancer risk. We demonstrated that more than 20% of the BaP in ambient air was from BCOs in the peak year. The cumulative nonoccupational excess lung cancer cases associated with BaP from BCOs was 3,500 (±1,500) from 1982 to 2015. If there was no ban, the cases would be as high as 9,290 (±4,300), indicating the significant health benefits of the Coal Law. On the other hand, if the ban had been fully implemented immediately after the law was enforced in 1996, the cumulative cases would be 1,500 (±620), showing the importance of implementing the law.

Distinguishing Emission-Associated Ambient Air PM2.5 Concentrations and Meteorological Factor-Induced Fluctuations.

Although PM2.5 (particulate matter with aerodynamic diameters less than 2.5 µm) in the air originates from emissions, its concentrations are often affected by confounding meteorological effects. Therefore, direct comparisons of PM2.5 concentrations made across two periods, which are commonly used by environmental protection administrations to measure the effectiveness of mitigation efforts, can be misleading. Here, we developed a two-step method to distinguish the significance of emissions and meteorological factors and assess the effectiveness of emission mitigation efforts. We modeled ambient PM2.5 concentrations from 1980 to 2014 based on three conditional scenarios: realistic conditions, fixed emissions, and fixed meteorology. The differences found between the model outputs were analyzed to quantify the relative contributions of emissions and meteorological factors. Emission-related gridded PM2.5 concentrations excluding the meteorological effects were predicted using multivariate regression models, whereas meteorological confounding effects on PM2.5 fluctuations were characterized by probabilistic functions. When the regression models and probabilistic functions were combined, fluctuations in the PM2.5 concentrations induced by emissions and meteorological factors were quantified for all model grid cells and regions. The method was then applied to assess the historical and future trends of PM2.5 concentrations and potential fluctuations on global, national, and city scales. The proposed method may thus be used to assess the effectiveness of mitigation actions.

Global forest carbon uptake due to nitrogen and phosphorus deposition from 1850 to 2100.

Spatial patterns and temporal trends of nitrogen (N) and phosphorus (P) deposition are important for quantifying their impact on forest carbon (C) uptake. In a first step, we modeled historical and future change in the global distributions of the atmospheric deposition of N and P from the dry and wet deposition of aerosols and gases containing N and P. Future projections were compared between two scenarios with contrasting aerosol emissions. Modeled fields of N and P deposition and P concentration were evaluated using globally distributed in situ measurements. N deposition peaked around 1990 in European forests and around 2010 in East Asian forests, and both increased sevenfold relative to 1850. P deposition peaked around 2010 in South Asian forests and increased 3.5-fold relative to 1850. In a second step, we estimated the change in C storage in forests due to the fertilization by deposited N and P (∆Cν dep ), based on the retention of deposited nutrients, their allocation within plants, and C:N and C:P stoichiometry. ∆Cν dep for 1997-2013 was estimated to be 0.27 ± 0.13 Pg C year-1 from N and 0.054 ± 0.10 Pg C year-1 from P, contributing 9% and 2% of the terrestrial C sink, respectively. Sensitivity tests show that uncertainty of ∆Cν dep was larger from P than from N, mainly due to uncertainty in the fraction of deposited P that is fixed by soil. ∆CPdep was exceeded by ∆CNdep over 1960-2007 in a large area of East Asian and West European forests due to a faster growth in N deposition than P. Our results suggest a significant contribution of anthropogenic P deposition to C storage, and additional sources of N are needed to support C storage by P in some Asian tropical forests where the deposition rate increased even faster for P than for N.

Spatial and Temporal Trends in Global Emissions of Nitrogen Oxides from 1960 to 2014.

The quantification of nitrogen oxide (NOx) emissions is critical for air quality modeling. Based on updated fuel consumption and emission factor databases, a global emission inventory was compiled with high spatial (0.1° × 0.1°), temporal (monthly), and source (87 sources) resolutions for the period 1960 to 2014. The monthly emission data have been uploaded online ( http://inventory.pku.edu.cn ), along with a number of other air pollutant and greenhouse gas data for free download. Differences in source profiles, not global total quantities, between our results and those reported previously were found. There were significant differences in total and per capita emissions and emission intensities among countries, especially between the developing and developed countries. Globally, the total annual NOx emissions finally stopped increasing in 2013 after continuously increasing over several decades, largely due to strict control measures taken in China in recent years. Nevertheless, the peak year of NOx emissions was later than for many other major air pollutants. Per capita emissions, either among countries or over years, follow typical inverted U-shaped environmental Kuznets curves, indicating that the emissions increased during the early stage of development and were restrained when socioeconomic development reached certain points. Although the trends are similar among countries, the turning points of developing countries appeared sooner than those of developed countries in terms of development status, confirming late-move advantages.

Exposure to ambient black carbon derived from a unique inventory and high-resolution model.

Black carbon (BC) is increasingly recognized as a significant air pollutant with harmful effects on human health, either in its own right or as a carrier of other chemicals. The adverse impact is of particular concern in those developing regions with high emissions and a growing population density. The results of recent studies indicate that BC emissions could be underestimated by a factor of 2-3 and this is particularly true for the hot-spot Asian region. Here we present a unique inventory at 10-km resolution based on a recently published global fuel consumption data product and updated emission factor measurements. The unique inventory is coupled to an Asia-nested (∼50 km) atmospheric model and used to calculate the global population exposure to BC with fully quantified uncertainty. Evaluating the modeled surface BC concentrations against observations reveals great improvement. The bias is reduced from -88% to -35% in Asia when the unique inventory and higher-resolution model replace a previous inventory combined with a coarse-resolution model. The bias can be further reduced to -12% by downscaling to 10 km using emission as a proxy. Our estimated global population-weighted BC exposure concentration constrained by observations is 2.14 µg⋅m(-3); 130% higher than that obtained using less detailed inventories and low-resolution models.

Direct Energy Consumption Associated Emissions by Rural-to-Urban Migrants in Beijing.

Hundreds of millions of rural residents have migrated to cities in China in recent years. Different lifestyles and living conditions lead to substantial changes in their household energy. Here, we present the result of a survey on direct household energy use of low-skilled rural-to-urban migrants in Beijing. The migrants moved up the energy ladder immediately after arriving in the city by replacing biomass fuels with coal, electricity, and liquefied petroleum gas. After the original shift, pattern of household energy use by the migrants has not changed much over decades, likely due to the long-existing household registration system (Hukou). As a result, the mix of energy types used by the rural-to-urban migrants were different from those by long-term urban residents, although total quantities were similar. Shifting from biomass fuels to coal, the migrants emitted 2.4 times more non-neutral CO2 than rural residents and 14% more than urban residents. The migration also resulted in significant increase in emissions of SO2 and mercury but dramatic decreases in some incomplete combustion products including particulate matter. All these changes have significant implication on air quality, health, and climate considering the scale of urbanization in China.

Influence of anthropogenic aerosol deposition on the relationship between oceanic productivity and warming.

Satellite data and models suggest that oceanic productivity is reduced in response to less nutrient supply under warming. In contrast, anthropogenic aerosols provide nutrients and exert a fertilizing effect, but its contribution to evolution of oceanic productivity is unknown. We simulate the response of oceanic biogeochemistry to anthropogenic aerosols deposition under varying climate from 1850 to 2010. We find a positive response of observed chlorophyll to deposition of anthropogenic aerosols. Our results suggest that anthropogenic aerosols reduce the sensitivity of oceanic productivity to warming from -15.2 ± 1.8 to -13.3 ± 1.6 Pg C yr-1 °C-1 in global stratified oceans during 1948-2007. The reducing percentage over the North Atlantic, North Pacific, and Indian Oceans reaches 40, 24, and 25%, respectively. We hypothesize that inevitable reduction of aerosol emissions in response to higher air quality standards in the future might accelerate the decline of oceanic productivity per unit warming.

A new high-resolution N2O emission inventory for China in 2008.

The amount and geographic distribution of N2O emissions over China remain largely uncertain. In this study, county-level and 0.1° × 0.1° gridded anthropogenic N2O emission inventories for China (PKU-N2O) in 2008 are developed based on high-resolution activity data and regional emission factors (EFs) and parameters. These new estimates are compared with previous inventories, and with two sensitivity tests: one that uses high-resolution activity data but the default IPCC methodology (S1) and the other that uses regional EFs and parameters but starts from coarser-resolution activity data. The total N2O emissions are 2150 GgN2O/yr (interquartile range from 1174 to 2787 GgN2O/yr). Agriculture contributes 64% of the total, followed by energy (17%), indirect emissions (12%), wastes (5%), industry (2.8%), and wildfires (0.2%). Our national emission total is 17% greater than that of the EDGAR v4.2 global product sampled over China and is also greater than the GAINS-China, NDRC, and S1 estimates by 10%, 50%, and 17%, respectively. We also found that using uniform EFs and parameters or starting from national/provincial data causes systematic spatial biases compared to PKU-N2O. Spatial analysis shows nonlinear relationships between N2O emission intensities and urbanization. Per-capita and per-GDP N2O emissions increase gradually with an increase in the urban population fraction from 0.3 to 0.9 among 2884 counties, and N2O emission density increases with urban expansion.

Quantification of global primary emissions of PM2.5, PM10, and TSP from combustion and industrial process sources.

Emission quantification of primary particulate matter (PM) is essential for assessment of its related climate and health impacts. To reduce uncertainty associated with global emissions of PM2.5, PM10, and TSP, we compiled data with high spatial (0.1° × 0.1°) and sectorial (77 primary sources) resolutions for 2007 based on a newly released global fuel data product (PKU-FUEL-2007) and an emission factor database. Our estimates for developing countries are higher than those previously reported. Spatial bias associated with large countries could be reduced by using subnational fuel consumption data. Additionally, we looked at temporal trends from 1960 to 2009 at country-scale resolution. Although total emissions are still increasing in developing countries, their intensities in terms of gross domestic production or energy consumption have decreased. PM emitted in developed countries is finer owing to a larger contribution from nonindustrial sources and use of abatement technologies. In contrast, countries like China, with strong industry emissions and limited abatement facilities, emit coarser PM. The health impacts of PM are intensified in hotspots and cities owing to covariance of sources and receptors. Although urbanization reduces the per person emission, overall health impacts related to these emissions are heightened because of aggregation effects.

Global mercury emissions from combustion in light of international fuel trading.

The spatially resolved emission inventory is essential for understanding the fate of mercury. Previous global mercury emission inventories for fuel combustion sources overlooked the influence of fuel trading on local emission estimates of many countries, mostly developing countries, for which national emission data are not available. This study demonstrates that in many countries, the mercury content of coal and petroleum locally consumed differ significantly from those locally produced. If the mercury content in locally produced fuels were used to estimate emission, then the resulting global mercury emissions from coal and petroleum would be overestimated by 4.7 and 72%, respectively. Even higher misestimations would exist in individual countries, leading to strong spatial bias. On the basis of the available data on fuel trading and an updated global fuel consumption database, a new mercury emission inventory for 64 combustion sources has been developed. The emissions were mapped at 0.1° × 0.1° resolution for 2007 and at country resolution for a period from 1960 to 2006. The estimated global total mercury emission from all combustion sources (fossil fuel, biomass fuel, solid waste, and wildfires) in 2007 was 1454 Mg (1232-1691 Mg as interquartile range from Monte Carlo simulation), among which elementary mercury (Hg(0)), divalent gaseous mercury (Hg(2+)), and particulate mercury (Hg(p)) were 725, 548, and 181 Mg, respectively. The total emission from anthropogenic sources, excluding wildfires, was 1040 Mg (886-1248 Mg), with coal combustion contributing more than half. Globally, total annual anthropogenic mercury emission from combustion sources increased from 285 Mg (263-358 Mg) in 1960 to 1040 Mg (886-1248 Mg) in 2007, owing to an increased fuel consumption in developing countries. However, mercury emissions from developed countries have decreased since 2000.