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.

Impact of the initial hydrophilic ratio on black carbon aerosols in the Arctic.

Black carbon (BC) contributes to patterns of Arctic warming, yet the initial hydrophilic ratio (IHR) of BC emitted from various sources and its impact on Arctic BC remain uncertain. With the use of a tagged tracer method of BC implemented in the global chemistry transport model GEOS-Chem, IHRs were partitioned into 7 BC combustion source categories according to the PKU-BC-v2 emission inventory. The results show that as the IHR increased, the concentration of BC decreased globally. The impact on Arctic BC was mainly reflected in the vertical profile and the burden rather than at the surface. Specifically, the greatest impact of IHR on Arctic BC appeared in summer, with the largest perturbation appearing at an altitude of approximately 600 hPa, reaching 8%. This change in BC vertical profile was mainly caused by the IHR change of wildfire combustion in Russia (44%) and Canada (51%), and the emissions from these two regions were also the two most important contributors to the BC concentration and burden in the middle and lower Arctic atmosphere in summer. In the other three seasons, anthropogenic combustion sources (oil, coal, and biomass) in East Asia, Russia, and Europe accounted for 19-40%, 14-28%, and 7-23%, respectively, of the monthly BC burden. Emissions from Russia were the most important contributor (27-43%) to the monthly BC surface concentration. Due to the large adjustment in IHR from 20% to 70%, biomass burning in Europe was shown to be the dominant contributor causing both burden (39%) and surface concentration (88%) changes in all seasons except summer.

Source identification of particulate phosphorus in the atmosphere in Beijing.

We tracked atmospheric phosphorus (P) in suspended particulate matter (PM) from a site in Beijing, China over a three-year period and found a new relationship between plants and atmospheric P. Concentrations of total phosphorus (TP) in the atmosphere during plant growing seasons were 2.5 times those observed in other months and levels of organic phosphorus (OP) were 3.9 times as high. TP and OP increases during growing seasons were much more significant in PM with diameters of over 2.5 µm (PM>2.5). PM collected during growing seasons included high levels of P but less nitrogen than that in primary biogenic aerosol particles (PBAPs) and differed from other emission sources such as combustion emissions and dust. A time series of OP concentrations in the atmosphere shows a time lag relative to Normalized Difference Vegetation Index (NDVI) data with high levels found during early growing periods and much lower levels found during flourishing periods. Thus, we find that plants contribute to atmospheric P and especially to OP rather than to PBAP levels.

Graphene oxide-induced formation of a boron-doped iron oxide shell on the surface of NZVI for enhancing nitrate removal.

The surface products have a significant influence on the reactivity of zero-valent iron-based materials. Although the enhancing effect of graphene on the reactivity of nanoscale zero-valent iron (NZVI)/graphene composites have been confirmed, the effect of graphene on the formation of surface products of NZVI is not well understood. In order to assess the effect of graphene on the structural of the outer iron oxide layers of NZVI, the NZVI was pre-oxidized by graphene oxide (ONZVI-GO). Compared with the NZVI oxidized by O2 (ONZVI-O2), ONZVI-GO was shown to be effective at NO3- removal with a high efficiency over a wide range of initial pH values. The results from characterization showed that GO could induce the formation of a tight iron oxide shell with dense spinel structures. The boron introduced during the preparation of NZVI was doped into iron oxides on the surface of ONZVI-GO. The B-O in adsorbed borate was transformed to B-B/B-Fe in the lattice structure of iron oxides, causing the formation of highly electron-deficient Lewis acid sites on the surface of ONZVI-GO, which could effectively gather NO3- and OH-, leading to the higher efficiency removal of NO3- than ONZVI-O2 over a wide range of initial pH values. This study provides new insight into the interaction between graphene and the surface species of NZVI.

An inter-comparative evaluation of PKU-FUEL global SO2 emission inventory.

PKU-FUEL is a recently developed gridded global emission inventory for multiple air pollutants that uses a bottom-up approach. The inventory includes data collected monthly for the period of 1960 to 2014 and at a 0.1° × 0.1° latitude/longitude resolution. In an effort to evaluate and improve this emission inventory, the PKU-FUEL Sulfur Dioxide (SO2) emission inventory was compared to other currently available and widely used global SO2 emission inventories constructed based on bottom-up and top-down approaches, including CEDS and OMI-HTAP. While PKU-FUEL is capable of capturing SO2 emissions across the globe and particularly in Asia, it misses 41 industrial point sources globally, accounting for 9.3% of Ozone Monitoring Instrument (OMI) remote sensing-measured industrial point sources. Most of these missing point sources are identified in Latin America, the Middle East (~60%), and some remote places. To improve the PKU-FUEL SO2 inventory, we applied OMI-measured emissions to sources missing from PKU-FUEL. GEOS-Chem model simulations were performed to evaluate original and improved PKU-FUEL SO2 inventories against measured SO2 concentrations across the world. Results were further compared to GEOS-Chem modeled SO2 concentrations using the CEDS inventory. We show that the modeled SO2 concentrations determined using both CEDS and improved PKU-FUEL inventories to a large extent corroborate sampled data and that the improved PKU-FUEL performs better for those regions lacking monitoring data.

Effect of northern boreal forest fires on PAH fluctuations across the arctic.

Polycyclic aromatic hydrocarbons (PAHs) are formed by the incomplete combustion of fossil fuels and forest or biomass burning. PAHs undergo long-range atmospheric transport, as evidenced by in situ observations across the Arctic. However, monitored atmospheric concentrations of PAHs indicate that ambient PAH levels in the Arctic do not follow the declining trend of worldwide anthropogenic PAH emissions since the 2000s, suggesting missing sources of PAHs in the Arctic or other places across the Northern Hemisphere. To trace origins and causes for the increasing trend of PAHs in the Arctic, the present study reconstructed PAH emissions from forest fires in the northern boreal forest derived by combining forest carbon stocks and MODIS burned area. We examined the statistical relationships of forest biomass, MODIS burned area, emission factors, and combustion efficiency with different PAH congeners. These relationships were then employed to construct PAH emission inventories from forest biomass burning. We show that for some PAH congeners, for example, benzo[a]pyrene (BaP)-the forest-fire-induced air emissions are almost one order of magnitude higher than previous emission inventories in the Arctic. A global-scale atmospheric chemistry model, GEOS-Chem, was used to simulate air concentrations of BaP, a representative PAH congener primarily emitted from biomass burning, and to quantify the response of BaP to wildfires in the northern boreal forest. The results showed that BaP emissions from wildfires across the northern boreal forest region played a significant role in the contamination and interannual fluctuations of BaP in Arctic air. A source-tagging technique was applied in tracking the origins of BaP pollution from different northern boreal forest regions. We also show that the response of BaP pollution at different Arctic monitoring sites depends on the intensity of human activities.

Missed atmospheric organic phosphorus emitted by terrestrial plants, part 2: Experiment of volatile phosphorus.

The emission and deposition of global atmospheric phosphorus (P) have long been considered unbalanced, and primary biogenic aerosol particles (PBAP) and phosphine (PH3) are considered to be the only atmospheric P sources from the ecosystem. In this work, we found and quantified volatile organic phosphorus (VOP) emissions from plants unaccounted for in previous studies. In a greenhouse in which lemons were cultivated, the atmospheric total phosphorus (TP) concentration of particulate matter (PM) was 41.8% higher than that in a greenhouse containing only soil, and the proportion of organic phosphorus (OP) in TP was doubled. 31P nuclear magnetic resonance tests (31P-NMR) of PM showed that phosphate monoesters were the main components contributed by plants in both the greenhouse and at an outside observation site. Atmospheric gaseous P was directly measured to be 1-2 orders of magnitude lower than P in PM but appeared to double during plant growing seasons relative to other months. Bag-sampling and gas chromatography mass spectrometry (GCMS) tests showed that the gaseous P emitted by plants in the greenhouse was triethyl phosphate. VOP might be an important component of atmospheric P that has been underestimated in previous studies.

The potential water-food-health nexus in urban China: A comparative study on dietary changes at home and away from home.

In China, urbanization strengthens the water-food-health nexus by driving dietary changes both at home and away from home (AFH). However, few studies have compared the effects of dining location on water footprint generation and/or linked such habits to the prevalence of non-communicable diseases (NCDs), such as hypertension, diabetes, asthma, myocardial infarction, stroke and cancer. Here, household survey data were used to develop a multiple-component urbanization sequence, on which the diet-related water footprint was quantified and the mechanisms under the water-food-health nexus were explored. Significant dietary changes due to urbanization have occurred at home (instead of AHF), and increases or decreases in various food groups are stratified across dining locations. Log mean Divisia index decomposition shows that the diet-structure effect outweighing the intake effect dominates the water footprint changes during China's urbanization. Animal products contribute 92(94)% of the diet-structure effect on net water footprint growth at home(AFH); in contrast, vegetal foods dominate the intake effect, contributing 67(49)%. The at-home water footprint ratio of animal products to vegetal foods is highly related to the prevalence of diabetes, hypertension, cancer, and asthma, and reaching statistical significance. Two urbanization components, namely housing situation and community diversity, serve as the key drivers of water-food-health nexus enhancement in urbanized China. Due to the complexity of water-food-health links, nexus thinking is needed to benefit human health and diet-related water consumption; besides, it may be reasonable to expand current dimension of food-energy-water nexus topic to include health issues.