ACS Earth and Space Chemistry

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ISSN / EISSN : 2472-3452 / 2472-3452
Published by: American Chemical Society (ACS) (10.1021)
Total articles ≅ 1,045
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Shuzhen Chen, , Fabrizio Orlando, Jacinta Edebeli, Xiangrui Kong, Huanyu Yang, Anthony Boucly, Pablo Corral Arroyo, ,
ACS Earth and Space Chemistry; https://doi.org/10.1021/acsearthspacechem.1c00233

Abstract:
The reaction of ozone with sea-salt derived bromide is relevant for marine boundary layer atmospheric chemistry. The oxidation of bromide by ozone is enhanced at aqueous interfaces. Ocean surface water and sea spray aerosol are enriched in organic compounds, which may also have a significant effect on this reaction at the interface. Here, we assess the surface propensity of cationic tetrabutylammonium at the aqueous liquid–vapor interface by liquid microjet X-ray photoelectron spectroscopy (XPS) and the effect of this surfactant on ozone uptake to aqueous bromide solutions. The results clearly indicate that the positively charged nitrogen group in tetrabutylammonium (TBA), along with its surface activity, leads to an enhanced interfacial concentration of both bromide and the bromide ozonide reaction intermediate. In parallel, off-line kinetic experiments for the same system demonstrate a strongly enhanced ozone loss rate in the presence of TBA, which is attributed to an enhanced surface reaction rate. We used liquid jet XPS to obtain detailed chemical composition information from the aqueous-solution–vapor interface of mixed aqueous solutions containing bromide or bromide and chloride with and without TBA surfactant. Core level spectra of Br 3d, C 1s, Cl 2p, N 1s, and O 1s were used for this comparison. A model was developed to account for the attenuation of photoelectrons by the carbon-rich layer established by the TBA surfactant. We observed that the interfacial density of bromide is increased by an order of magnitude in solutions with TBA. The salting-out of TBA in the presence of 0.55 M sodium chloride is apparent. The increased interfacial bromide density can be rationalized by the association constants for bromide and chloride to form ion-pairs with TBA. Still, the interfacial reactivity is not increasing simply proportionally with the increasing interfacial bromide concentration in response to the presence of TBA. The steady state concentration of the bromide ozonide intermediate increases by a smaller degree, and the lifetime of the intermediate is 1 order of magnitude longer in the presence of TBA. Thus, the influence of cationic surfactants on the reactivity of bromide depends on the details of the complex environment at the interface.
Luke T. Townsend, Gina Kuippers, Jonathan R. Lloyd, , Christopher Boothman, , ,
ACS Earth and Space Chemistry; https://doi.org/10.1021/acsearthspacechem.1c00126

Abstract:
Globally, the need for radioactive waste disposal and contaminated land management is clear. Here, gaining an improved understanding of how biogeochemical processes, such as Fe(III) and sulfate reduction, may control the environmental mobility of radionuclides is important. Uranium (U), typically the most abundant radionuclide by mass in radioactive wastes and contaminated land scenarios, may have its environmental mobility impacted by biogeochemical processes within the subsurface. This study investigated the fate of U(VI) in an alkaline (pH ∼9.6) sulfate-reducing enrichment culture obtained from a high-pH environment. To explore the mobility of U(VI) under alkaline conditions where iron minerals are ubiquitous, a range of conditions were tested, including high (30 mM) and low (1 mM) carbonate concentrations and the presence and absence of Fe(III). At high carbonate concentrations, the pH was buffered to approximately pH 9.6, which delayed the onset of sulfate reduction and meant that the reduction of U(VI)(aq) to poorly soluble U(IV)(s) was slowed. Low carbonate conditions allowed microbial sulfate reduction to proceed and caused the pH to fall to ∼7.5. This drop in pH was likely due to the presence of volatile fatty acids from the microbial respiration of gluconate. Here, aqueous sulfide accumulated and U was removed from solution as a mixture of U(IV) and U(VI) phosphate species. In addition, sulfate-reducing bacteria, such as Desulfosporosinus species, were enriched during development of sulfate-reducing conditions. Results highlight the impact of carbonate concentrations on U speciation and solubility in alkaline conditions, informing intermediate-level radioactive waste disposal and radioactively contaminated land management.
Tao Wang, Qixin Wu, Zhuhong Wang, Gang Dai, Huipeng Jia, Shilin Gao
ACS Earth and Space Chemistry; https://doi.org/10.1021/acsearthspacechem.1c00238

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Mengke Wang, Ziting Zhang, Yinghui Wang, Xiaohan Mo, Qiang Zhang, Peng Zhang, Gege Yin, Liping Li, Senhao Wang, Jiangming Mo, et al.
ACS Earth and Space Chemistry; https://doi.org/10.1021/acsearthspacechem.1c00243

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Ying Lin, Nanping Wu, Kaiwen Ta, Amaelle Landais, Xiaotong Peng
ACS Earth and Space Chemistry; https://doi.org/10.1021/acsearthspacechem.1c00187

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Paul R. Tumminello, Reece C. James, Samantha Kruse, Allison Kawasaki, Adam Cooper, Isis Guadalupe-Diaz, Karen Lopo Zepeda, Daniel R. Crocker, Kathryn J. Mayer, Jonathan S. Sauer, et al.
ACS Earth and Space Chemistry; https://doi.org/10.1021/acsearthspacechem.1c00186

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, Sarrah M. Dunham-Cheatham, Beatriz Ferreira Araujo, Olivier Magand, Jennie L. Thomas, Foteini Baladima, Katrine Aspmo Pfaffhuber, Torunn Berg, , Jiaoyan Huang, et al.
ACS Earth and Space Chemistry; https://doi.org/10.1021/acsearthspacechem.1c00299

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