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- Kong, Xiangrui, et al.
(författare)
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A surface-promoted redox reaction occurs spontaneously on solvating inorganic aerosol surfaces
- 2021
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Ingår i: Science. - : American Association for the Advancement of Science (AAAS). - 0036-8075 .- 1095-9203. ; 374:6568, s. 747-
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Tidskriftsartikel (refereegranskat)abstract
- A surface-promoted sulfate-reducing ammonium oxidation reaction was discovered to spontaneously take place on common inorganic aerosol surfaces undergoing solvation. Several key intermediate species-including elemental sulfur (S-0), bisulfide (HS-), nitrous acid (HONO), and aqueous ammonia [NH3(aq)]-were identified as reaction components associated with the solvation process. Depth profiles of relative species abundance showed the surface propensity of key species. The species assignments and depth profile features were supported by classical and first-principles molecular dynamics calculations, and a detailed mechanism was proposed to describe the processes that led to unexpected products during salt solvation. This discovery revealed chemistry that is distinctly linked to a solvating surface and has great potential to illuminate current puzzles within heterogeneous chemistry.
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| 2. |
- Kong, Xiangrui, et al.
(författare)
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Reversibly Physisorbed and Chemisorbed Water on Carboxylic Salt Surfaces under Atmospheric Conditions
- 2020
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Ingår i: Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 124:9, s. 5263-5269
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Tidskriftsartikel (refereegranskat)abstract
- Copyright © 2020 American Chemical Society. The particle-gas interface in aerosol systems is of essential importance because it is here that many key atmospheric processes occur. In this study, we employ ambient pressure X-ray photoelectron spectroscopy (APXPS) to investigate the surface properties and processes of an atmospherically relevant carboxylic salt, sodium acetate, at subdeliquescence conditions. From the depth profiles of the elemental ratios of sodium, oxygen, and carbon, we find that after deliquescence-efflorescence cycles the salt surface is sodium-depleted. The mechanism of the observed depletion is proposed to be (i) the formation of neutral acetic acid in the solution due to the nature of the basic salt; (ii) the selective surface enhancement of neutral molecules under aqueous condition; and (iii) a hypothetical kinetic barrier to re-homogenization due to spatial separation and special local conditions on the surface, resulting in varied local surface composition. When the relative humidity gradually increases and approaches the deliquescence point, both reversible water uptake and reversible surface dissociation are confirmed by near-edge X-ray adsorption fine structure (NEXAFS) spectroscopy at the oxygen K-edge and sodium K-edge, respectively. The solvation of sodium requires a higher relative humidity than needed for water adsorption, which suggests that water molecules are taken up by the surface, but the solvation of the salt surface begins only when sufficient water molecules are present, to facilitate the process. The sodium-depleted surface requires additional adsorbed water to affect and dissolve the sodium ions in deeper regions.
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| 3. |
- Li, Jun, et al.
(författare)
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Hygroscopicity and Ice Nucleation Properties of Dust/Salt Mixtures Originating from the Source of East Asian Dust Storms
- 2022
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Ingår i: Frontiers in Environmental Science. - : Frontiers Media SA. - 2296-665X. ; 10
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Tidskriftsartikel (refereegranskat)abstract
- Dust storms are common meteorological events that occur frequently in the late spring and early summer in arid and semi-arid areas. The resulting lofted dust and salt mixtures can impact atmospheric chemistry and climate systems through the many pathways represented by aerosol-cloud-climate interactions. In this study, dust/salt samples were collected from important sources of the East Asian dust storm, including the Badain Jaran Desert, the Tengger Desert and the Ulan Buh Desert in northwestern China. Ion chromatography (IC) measurements were performed to determine the concentrations of cations and anions. The ionic concentrations, pH and dissolvable fractions of sand samples show a positive correlation, indicating that the dissolved content is rich in alkaline ions. A positive matrix factorization (PMF) receptor model was employed to analyze the IC results, and from the PMF solutions non-obvious connections to local geography emerge. The results of hygroscopic experiments of sand samples which were measured by a vapor sorption analyzer indicate that the hygroscopicity may be related to the soluble content of samples, and the observed hygroscopic behavior can be well described by a thermodynamic model. The morphology of individual particles was chemically mapped by the synchrotron-based scanning transmission X-ray microscopy, and needle-shaped CaCO3 particles were observed to adhere to more irregular high K-containing particles. Moreover, a continuous flow diffusion chamber was used to investigate the ice nucleation abilities of typical salts, with both homogeneous freezing and deposition nucleation being observed. The results indicate that the salts primarily act as cloud condensation nuclei but can also act as ice nucleating particles at low temperatures.
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