Abstract. Emission inventories for major reactive tropospheric CI species (particulate CI, HC1, C1NO2, CH3CI, CHCI3, CH3CCI3, C2C14, C2HC13, CH2C12, and CHCIF2) were integrated across source types (terrestrial biogenic and oceanic emissions, sea-salt production and dechlorination, biomass burning, industrial emissions, fossil-fuel combustion, and incineration). Composite emissions were compared with known sinks to assess budget closure; relative contributions of natural and anthropogenic sources were differentiated. Model calculations suggest that conventional acid-displacement reactions involving Sov)+O3, S(Iv)+ H202, and H2SO4 and HNO3 scavenging account for minor fractions of sea-salt dechlorination globally. Other important chemical pathways involving sea-salt aerosol apparently produce most volatile chlorine in the troposphere. The combined emissions of CH3CI from known sources account for about half of the modeled sink, suggesting fluxes from known sources were unde:estimated, the OH sink was overestimated, or significant unidentified sources exist. Anthropogenic activities (primarily biomass burning) contribute about half the net CH3CI emitted from known sources. Anthropogenic emissions account for only about 10% of the modeled CHCl3 sink. Although poorly constrained, significant fractions of tropospheric CH2C12 (25%), C2HC13 (10%), and C2C14 (5%) are emitted from the surface ocean; the combined contributions of C2C14 and C2HC13 from all natural sources may be substantially higher than the estimated oceanic flux.

Abstract. Much if not all of the chlorine present in fossil fuels is released into the atmosphere as hydrogen chloride (HC1) and chloromethane (CH3C1, methyl chloride). The chlorine content of oilbased fuels is so low that these sources can be neglected, but coal combustion provides significant releases. On the basis of national statistics for the quantity and quality of coal burned during 1990 in power and heat generation, industrial conversion and residential and commercial heating, coupled with information on the chlorine contents of coals, a global inventory of national HC1 emissions from this source has been constructed. This was combined with an estimate of the national emissions of HC1 from waste combustion (both large-scale incineration and trash burning) which was based on an estimate of the global quantity released from this source expressed per head of population. Account was taken of reduced emissions where flue gases were processed, for example to remove sulphur dioxide. The HC1 emitted in 1990, comprising 4.6 + 4.3 Tg C1 from fossil fuel and 2 + 1.9 Tg C1 from waste btmmtg, was spatially distributed using available information on point sources such as power generation utilities and population density by default. Also associated with these combustion sources are chloromethane emissions, calculated to be 0.075 q-0.07 Tg as C1 (equivalent) from fossil fuels and 0.032 q-0.023 Tg C1 (equivalent) from waste combustion. These were distributed spatially exactly as the HC1 emissions, and a further 0.007 Tg C1 in chloromethane from industrial process activity was distributed by point sources.

The identified emissions of the title compounds come predominantly from their use in industrial and commercial processes. Trichloroethene and tetrachloroethene have also been found as byproducts of gasoline and coal combustion; these sources were also considered but shown to be insignificant compared with industrial releases. Global emissions during 1990, amounting to 0.241±0.013 Tg of trichloroethene, 0.366±0.020 Tg of tetrachloroethene, and 0.583±0.032 Tg of dichloromethane (0.195±0.010, 0.313±0.017, and 0.487±0.027 Tg as chlorine, respectively) have been assigned to individual countries and thence to a 1° latitude × 1° longitude grid based on a combination of three data sets: regional sales data that were available on a continental scale; economic activity in the form of national Gross Domestic Products; and the population distribution within each country. For those countries where they were available, data for the quantities and locations of reported emissions were also incorporated. Uncertainty in the distributed emissions is ±4% relative to countries with the largest emissions. The results, which are complementary to the marine fluxes and releases from biomass burning reported by Khalil et al [this issue] and Lobert et al [this issue], respectively, are recorded here as maps and are also available from the Global Emissions Inventory Activity web site at http://groundhog.sprl.umich.edu/geia/rcei. While the industrial regions of North America, Europe, and Japan are the largest sites of anthropogenic emissions, there are also significant sources in the developing nations of Asia; in contrast, anthropogenic emissions within the southern hemisphere are much smaller and more widely dispersed. The total emissions of dichloromethane appear to match the observed atmospheric concentrations, but about 25% of the flux of tetrachloroethene calculated from observations remains unaccounted, and significant extra emissions of trichloroethene are necessary to effect a balance. The known sources have been examined thoroughly in this work, and so it is reasonably certain that the additional emissions are not a deliberate result of human activity; however, there is no means of discriminating their origin unequivocally, and the missing quantities may be inadvertent byproducts of anthropogenic activities.

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Mercury is a persistent, bioaccumulative toxin. Although

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An analysis of the energy return on investment (EROI) of natural gas obtained from horizontal, hydraulically fractured wells in the Marcellus Shale was conducted using net external energy ratio methodology and available data and estimates of energy inputs and outputs. Used as sources of input data were estimates of carbon dioxide and nitrogen oxides emitted from the gas extraction processes, as well as fuel-use reports from industry and other sources. Estimates of quantities of materials used and the associated embodied energy as well as other energy-using steps were also developed from available data. Total input energy was compared with the energy expected to be made available to end users of the natural gas produced from a typical Marcellus well. The analysis indicates that the EROI of a typical well is likely between 64:1 and 112:1, with a mean of approximately 85:1. This range assumes an estimated ultimate recovery (EUR) of 3.0 billion cubic feet (Bcf) per well. EROI values are directly proportionate to EUR values. If the EUR is greater or lesser than 3 Bcf, the EROI would be proportionately higher or lower. EROI is also sensitive to the energy used or embedded in gathering and transmission pipelines and associated infrastructure and energy used for their construction, energy consumed in well drilling and well completion, and energy used for wastewater treatment.