Abstract
To assess the chemical reactivity, toxicity, and mobility of pollutants in the environment, knowledge of their species distributions is critical. Because their direct measurement is often infeasible, speciation modeling is widely adopted. Mercury (Hg) is a representative pollutant for which study of its speciation benefits from modeling. However, Hg speciation modeling is often hindered by a lack of reliable thermodynamic constants. Although computational chemistry (e.g., density functional theory [DFT]) can generate these constants, methods for directly coupling DFT and speciation modeling are not available. Here, we combine computational chemistry and continuum-scale modeling with curated online databases to ameliorate the problem of unreliable inputs to Hg speciation modeling. Our AQUA-MER databases and web server (https://aquamer.ornl.gov) provides direct speciation results by combining web-based interfaces to a speciation calculator, databases of thermodynamic constants, and a computational chemistry toolkit to estimate missing constants. Although Hg is presented as a concrete use case, AQUA-MER can also be readily applied to other elements.
Original language | English |
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Pages (from-to) | 147-155 |
Number of pages | 9 |
Journal | Journal of Computational Chemistry |
Volume | 41 |
Issue number | 2 |
DOIs | |
State | Published - Jan 15 2020 |
Funding
The authors thank Dr. Liyuan Liang for valuable discussions. This work was conducted jointly at the University of Tennessee, Knoxville and Oak Ridge National Laboratory (ORNL) and was supported by Grant DE-SC0016478 from the United States (US) Department of Energy (DOE) Office of Science, Biological and Environmental Research, Subsurface Biogeochemical Research. ORNL is managed by UT-Battelle LLC for the US DOE under Contract DE-AC05-00OR22725. This work used resources of the Compute and Data Environment for Science (CADES) at Oak Ridge National Laboratory. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan).
Keywords
- aqueous speciation modeling
- mercury speciation
- multiscale modeling
- online computational chemistry toolkit
- thermodynamic constants