Sources and budgets for CO and O-3 in the northeastern Pacific during the spring of 2001: Results from the PHOBEA-II Experiment

Abstract. Ground and airborne measurements of CO, ozone, and aerosols were obtained in th

Vertical distribution of mercury, CO, ozone, and aerosol scattering coefficient in the Pacific Northwest during the spring 2006 INTEX‐B campaign

Peer Reviewedhttp://deepblue.lib.umich.edu/bitstream/2027.42/94827/1/jgrd14532.pd

Mercury sources to Lake Ozette and Lake Dickey : highly contaminated remote coastal lakes, Washington State, USA

Author Posting. © The Author(s), 2009. This is the author's version of the work. It is posted here by permission of Springer for personal use, not for redistribution. The definitive version was published in Water, Air, & Soil Pollution 208 (2009): 275-286, doi:10.1007/s11270-009-0165-y.Mercury concentrations in largemouth bass and mercury accumulation rates in age-dated sediment cores were examined at Lake Ozette and Lake Dickey in Washington State. Goals of the study were to compare concentrations in fish tissues at the two lakes with lakes in a larger statewide dataset and evaluate factors influencing lake loading at Ozette and Dickey, which may include: catchment disturbances, coastal mercury cycling, and the role of trans-Pacific Asian mercury. Mercury fish tissue concentrations at the lakes were among the highest recorded in Washington State. Wet deposition and historical atmospheric monitoring from the area show no indication of enhanced deposition from Asian sources or coastal atmospheric processes. Sediment core records from the lakes displayed rapidly increasing sedimentation rates coinciding with commercial logging. The unusually high mercury flux rates and mercury tissue concentrations recorded at Lake Ozette and Lake Dickey appear to be associated with logging within the catchments

Observations of Reactive Gaseous Mercury in the Free Troposphere at the Mount Bachelor Observatory

We measured gaseous elemental mercury (GEM), particulate mercury (PHg), and reactive gaseous mercury (RGM), along with CO, ozone, and aerosol scatter at the Mount Bachelor Observatory (2.7 km above sea level), Oregon, from May to August 2005. The mean mercury concentrations (at standard conditions) were 1.54 ng/m3 (GEM), 5.2 pg/m3 (PHg), and 43 pg/m3 (RGM). RGM enhancements, up to 600 pg/m3, occurred at night and were linked to a diurnal pattern of upslope and downslope flows that mixed in boundary layer air during the day and free tropospheric air at night. During the night, RGM was inversely correlated (P < 0.0001) with CO (r = −0.36), GEM (r = −0.73), and H2O (r = −0.44), was positively correlated with ozone (r = 0.38), and could not be linked to recent anthropogenic emissions from local sources or long-range transport. Principal component analysis and a composite of change in RGM versus change in GEM during RGM enhancements indicate that a nearly quantitative shift in speciation is associated with increases in ozone and decreases in water vapor and CO. This argues that high concentrations of RGM are present in the free troposphere because of in situ oxidation of GEM to RGM. A global chemical transport model reproduces the RGM mean and diurnal pattern but underestimates the magnitude of the largest observed enhancements. Since the only modeled, in situ RGM production mechanisms are oxidation of GEM by ozone and OH, this implies that there are faster reaction rates or additional RGM production mechanisms in the free troposphere.Earth and Planetary SciencesEngineering and Applied Science

Use of a global model to understand speciated atmospheric mercury observations at five high-elevation sites

© 2015 Author(s). Atmospheric mercury (Hg) measurements using the Tekran® analytical system from five high-elevation sites (1400-3200 m elevation), one in Asia and four in the western US, were compiled over multiple seasons and years, and these data were compared with the GEOS-Chem global model. Mercury data consisted of gaseous elemental Hg (GEM) and "reactive Hg" (RM), which is a combination of the gaseous oxidized (GOM) and particulate bound ( < 2.5 μm) (PBM) fractions as measured by the Tekran® system. We used a subset of the observations by defining a "free tropospheric" (FT) data set by screening using measured water vapor mixing ratios. The oxidation scheme used by the GEOS-Chem model was varied between the standard run with Br oxidation and an alternative run with OH-O 3 oxidation. We used this model-measurement comparison to help interpret the spatio-temporal trends in, and relationships among, the Hg species and ancillary parameters, to understand better the sources and fate of atmospheric RM. The most salient feature of the data across sites, seen more in summer relative to spring, was that RM was negatively correlated with GEM and water vapor mixing ratios (WV) and positively correlated with ozone (O 3 ), both in the standard model and the observations, indicating that RM was formed in dry upper altitude air from the photo-oxidation of GEM. During a free tropospheric transport high RM event observed sequentially at three sites from Oregon to Nevada, the slope of the RM/GEM relationship at the westernmost site was-1020 ± 209 pg ng -1 , indicating near-quantitative GEM-to-RM photochemical conversion. An improved correlation between the observations and the model was seen when the model was run with the OH-O3 oxidation scheme instead of the Br oxidation scheme. This simulation produced higher concentrations of RM and lower concentrations of GEM, especially at the desert sites in northwestern Nevada. This suggests that future work should investigate the effect of Br-and O 3 -initiated gas-phase oxidation occurring simultaneously in the atmosphere, as well as aqueous and heterogeneous reactions to understand whether there are multiple global oxidants for GEM and hence multiple forms of RM in the atmosphere. If the chemical forms of RM were known, then the collection efficiency of the analytical method could be evaluated better.Taiwan. Environmental Protection Administratio

Total and Monomethyl Mercury in Fog Water from the Central California Coast

[1] Total mercury (HgT) and monomethyl mercury (MMHg) concentrations in fog collected from 4 locations in and around Monterey Bay, California during June-August of 2011 were 10.7 ± 6.8 and 3.4 ± 3.8 ng L−1respectively. In contrast, mean HgT and MMHg concentrations in rain water from March-June, 2011 were 1.8 ± 0.9 and 0.1 ± 0.04 ng L−1 respectively. Using estimates of fog water deposition from 6 sites in the region using a standard fog water collector (SFC), depositions of HgT and MMHg via fog were found to range from 42–4600 and 14–1500 ng m−2 y−1, which accounted for 7–42% of HgT and 61–99% of MMHg in total atmospheric deposition (fog, rain, and dry deposition), estimated for the coastal area. These initial measurements suggest that fog precipitation may constitute an important but previously overlooked input of MMHg to coastal environments. Preliminary comparisons of these data with associated chemical, meteorological and oceanic data suggest that biotically formed MMHg from coastal upwelling may contribute to the MMHg in fog water

Nested-grid simulation of mercury over North America

We have developed a new nested-grid mercury (Hg) simulation over North America with a 1/2° latitude by 2/3° longitude horizontal resolution employing the GEOS-Chem global chemical transport model. Emissions, chemistry, deposition, and meteorology are self-consistent between the global and nested domains. Compared to the global model (4° latitude by 5° longitude), the nested model shows improved skill at capturing the high spatial and temporal variability of Hg wet deposition over North America observed by the Mercury Deposition Network (MDN) in 2008–2009. The nested simulation resolves features such as higher deposition due to orographic precipitation, land/ocean contrast and and predicts more efficient convective rain scavenging of Hg over the southeast United States. However, the nested model overestimates Hg wet deposition over the Ohio River Valley region (ORV) by 27%. We modify anthropogenic emission speciation profiles in the US EPA National Emission Inventory (NEI) to account for the rapid in-plume reduction of reactive to elemental Hg (IPR simulation). This leads to a decrease in the model bias to −2.3% over the ORV region. Over the contiguous US, the correlation coefficient (<i>r</i>) between MDN observations and our IPR simulation increases from 0.60 to 0.78. The IPR nested simulation generally reproduces the seasonal cycle in surface concentrations of speciated Hg from the Atmospheric Mercury Network (AMNet) and Canadian Atmospheric Mercury Network (CAMNet). In the IPR simulation, annual mean gaseous and particulate-bound Hg(II) are within 140% and 11% of observations, respectively. In contrast, the simulation with unmodified anthropogenic Hg speciation profiles overestimates these observations by factors of 4 and 2 for gaseous and particulate-bound Hg(II), respectively. The nested model shows improved skill at capturing the horizontal variability of Hg observed over California during the ARCTAS aircraft campaign. The nested model suggests that North American anthropogenic emissions account for 10–22% of Hg wet deposition flux over the US, depending on the anthropogenic emissions speciation profile assumed. The modeled percent contribution can be as high as 60% near large point sources in ORV. Our results indicate that the North American anthropogenic contribution to dry deposition is 13–20%

Top-down constraints on atmospheric mercury emissions and implications for global biogeochemical cycling

We perform global-scale inverse modeling to constrain present-day atmospheric mercury emissions and relevant physiochemical parameters in the GEOS-Chem chemical transport model. We use Bayesian inversion methods combining simulations with GEOS-Chem and ground-based Hg[superscript 0] observations from regional monitoring networks and individual sites in recent years. Using optimized emissions/parameters, GEOS-Chem better reproduces these ground-based observations and also matches regional over-water Hg[superscript 0] and wet deposition measurements. The optimized global mercury emission to the atmosphere is ~ 5.8 Gg yr[superscript −1]. The ocean accounts for 3.2 Gg yr[superscript −1] (55% of the total), and the terrestrial ecosystem is neither a net source nor a net sink of Hg[superscript 0]. The optimized Asian anthropogenic emission of Hg[superscript 0] (gas elemental mercury) is 650–1770 Mg yr[superscript −1], higher than its bottom-up estimates (550–800 Mg yr[superscript −1]). The ocean parameter inversions suggest that dark oxidation of aqueous elemental mercury is faster, and less mercury is removed from the mixed layer through particle sinking, when compared with current simulations. Parameter changes affect the simulated global ocean mercury budget, particularly mass exchange between the mixed layer and subsurface waters. Based on our inversion results, we re-evaluate the long-term global biogeochemical cycle of mercury, and show that legacy mercury becomes more likely to reside in the terrestrial ecosystem than in the ocean. We estimate that primary anthropogenic mercury contributes up to 23 % of present-day atmospheric deposition.National Science Foundation (U.S.). Atmospheric Chemistry Program (1053648

Interdependent Infrastructure as Linked Social, Ecological, and Technological Systems (SETSs) to Address Lock‐in and Enhance Resilience

Traditional infrastructure adaptation to extreme weather events (and now climate change) has typically been techno‐centric and heavily grounded in robustness—the capacity to prevent or minimize disruptions via a risk‐based approach that emphasizes control, armoring, and strengthening (e.g., raising the height of levees). However, climate and nonclimate challenges facing infrastructure are not purely technological. Ecological and social systems also warrant consideration to manage issues of overconfidence, inflexibility, interdependence, and resource utilization—among others. As a result, techno‐centric adaptation strategies can result in unwanted tradeoffs, unintended consequences, and underaddressed vulnerabilities. Techno‐centric strategies that lock‐in today\u27s infrastructure systems to vulnerable future design, management, and regulatory practices may be particularly problematic by exacerbating these ecological and social issues rather than ameliorating them. Given these challenges, we develop a conceptual model and infrastructure adaptation case studies to argue the following: (1) infrastructure systems are not simply technological and should be understood as complex and interconnected social, ecological, and technological systems (SETSs); (2) infrastructure challenges, like lock‐in, stem from SETS interactions that are often overlooked and underappreciated; (3) framing infrastructure with a SETS lens can help identify and prevent maladaptive issues like lock‐in; and (4) a SETS lens can also highlight effective infrastructure adaptation strategies that may not traditionally be considered. Ultimately, we find that treating infrastructure as SETS shows promise for increasing the adaptive capacity of infrastructure systems by highlighting how lock‐in and vulnerabilities evolve and how multidisciplinary strategies can be deployed to address these challenges by broadening the options for adaptation