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| Content Provider | Springer Nature Link |
|---|---|
| Author | Singireddy, Soujanya Gordon, Alexander D. Smirv, Alexander Vance, Michael A. Schoonen, Martin A. A. Szilagyi, Robert K. Strongin, Daniel R. |
| Copyright Year | 2012 |
| Abstract | An important constraint on the formation of the building blocks of life in the Hadean is the availability of small, activated compounds such as ammonia (NH$_{3}$) relative to its inert dinitrogen source. Iron-sulfur particles and/or mineral surfaces have been implicated to provide the catalytic active sites for the reduction of dinitrogen. Here we provide a combined kinetic, spectroscopic, and computational modeling study for an alternative source of ammonia from water soluble nitrogen oxide ions. The adsorption of aqueous nitrite (NO 2 − ) and nitrate (NO 3 − ) on pyrite (FeS$_{2}$) and subsequent reduction chemistry to ammonia was investigated at 22°C, 70°C, and 120°C. Batch geochemical and in situ Attenuated Total Reflection – Fourier Transform Infrared (ATR-FTIR) spectroscopy experiments were used to determine the reduction kinetics to NH$_{3}$ and to elucidate the identity of the surface complexes, respectively, during the reaction chemistry of NO 2 − and NO 3 − . Density functional theory (DFT) calculations aided the interpretation of the vibrational data for a representative set of surface species. Under the experimental conditions used in this study, we detected the adsorption of nitric oxide (NO) intermediate on the pyrite surface. NH$_{3}$ production from NO 2 − occurred at 70 and 120°C and from NO 3 − occurred only at 120°C. |
| Starting Page | 275 |
| Ending Page | 294 |
| Page Count | 20 |
| File Format | |
| ISSN | 01696149 |
| Journal | Origins of Life and Evolution of Biospheres |
| Volume Number | 42 |
| Issue Number | 4 |
| e-ISSN | 15730875 |
| Language | English |
| Publisher | Springer Netherlands |
| Publisher Date | 2012-05-06 |
| Publisher Place | Dordrecht |
| Access Restriction | Subscribed |
| Subject Keyword | Pyrite Nitrite Nitrate Ammonia Nitric oxide DFT ATR-FTIR Biochemistry Life Sciences Astrophysics and Astroparticles Astronomy, Observations and Techniques Earth Sciences |
| Content Type | Text |
| Resource Type | Article |
| Subject | Medicine Ecology, Evolution, Behavior and Systematics Space and Planetary Science |
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