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Photolysis of Frozen Iodate Salts As a Source of Active Iodine in the Polar Environment

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Photolysis of Frozen Iodate Salts As a Source of Active Iodine in the Polar Environment Atmos. Chem. Phys., 16, 12703–12713, 2016 www.atmos-chem-phys.net/16/12703/2016/ doi:10.5194/acp-16-12703-2016 © Author(s) 2016. CC Attribution 3.0 License. Photolysis of frozen iodate salts as a source of active iodine in the polar environment Óscar Gálvez1,a, M. Teresa Baeza-Romero2, Mikel Sanz2,b, and Alfonso Saiz-Lopez3 1Departamento de Física Molecular, Instituto de Estructura de la Materia, IEM-CSIC, 28006 Madrid, Spain 2Escuela de Ingeniería Industrial, Universidad de Castilla-La Mancha, 45071 Toledo, Spain 3Department of Atmospheric Chemistry and Climate, Institute of Physical Chemistry Rocasolano, CSIC, 28006 Madrid, Spain anow at: Departamento de Física Interdisciplinar, Facultad de Ciencias, Universidad Nacional de Educación a Distancia, 28040 Madrid, Spain bnow at: Institute of Physical Chemistry Rocasolano, CSIC, 28006 Madrid, Spain Correspondence to: Óscar Gálvez ([email protected], [email protected]) Received: 15 September 2015 – Published in Atmos. Chem. Phys. Discuss.: 15 October 2015 Revised: 22 September 2016 – Accepted: 26 September 2016 – Published: 12 October 2016 Abstract. Reactive halogens play a key role in the oxida- 1 Introduction tion capacity of the polar troposphere. However, sources and mechanisms, particularly those involving active iodine, are still poorly understood. In this paper, the photolysis of an Atmospheric iodine compounds are present in the marine atmospherically relevant frozen iodate salt has been experi- and polar boundary layers (Saiz-Lopez et al., 2012), where mentally studied using infrared (IR) spectroscopy. The sam- they play a relevant role in catalytic ozone destruction (Saiz- ples were generated at low temperatures in the presence of Lopez et al., 2007b; Read et al., 2008), and they could also different amounts of water. The IR spectra have confirmed be involved in new particle formation in the polar environ- that, under near-ultraviolet–visible (UV–Vis) radiation, io- ment (Allan et al., 2015; Roscoe et al., 2015). Moreover, in date is efficiently photolysed. The integrated IR absorption the polar atmosphere, iodine has also been suggested as one coefficient of the iodate anion on the band at 750 cm−1 has of the possible sinks of gaseous elemental mercury (Calvert been measured to be A D 9.8 ± 0.5 × 10−17 cm molecule−1. and Lindberg, 2004; Saiz-Lopez et al., 2008). The photolysis rate of the ammonium iodate salt was mea- Although the concentration of atmospheric iodine is sured by monitoring the decay of ammonium or iodate IR highly variable at different regions, ground- (Frieß et al., bands (1430 and 750 cm−1 respectively) in the presence of a 2001; Saiz-Lopez et al., 2007b; Atkinson et al., 2012) and solar simulator. The absorption cross section of the liquid so- satellite-based instrumentation (Saiz-Lopez et al., 2007a; lutions of ammonium iodate at wavelengths relevant for the Schönhardt et al., 2008) measurements have confirmed re- troposphere (250 to 400 nm) has been obtained and used to markably high concentrations (up to 20 pptv) of IO in coastal estimate the photolytic quantum yield for the frozen salt. Fi- Antarctica. Nevertheless, the sources and mechanisms of io- nally, using an atmospheric model, constrained with the ex- dine emissions from ice remain poorly understood (Saiz- perimental data, we suggest that the photolysis of iodate in Lopez et al., 2015; Kim et al., 2016). frozen salt can potentially provide a pathway for the release Apart from observations of gaseous iodine species, differ- of active iodine to the polar atmosphere. ent studies have conducted analysis of the iodine fraction in rainwater (Laniewski et al., 1999) and aerosols (Baker et al., 2000). In all of them, iodine concentrations are considerably enriched over seawater, and an appreciable fraction of sol- − − uble iodine species like I and IO3 is observed, although − − the mechanism determining the I = IO3 ratio is still unclear. Published by Copernicus Publications on behalf of the European Geosciences Union. 12704 Ó. Gálvez et al.: Photolysis of frozen iodate salts as a source of active iodine − Thus, for example since IO3 has been considered an inert in- have followed, and more details of these calculations are organic iodine species, and therefore a sink molecule in the given in the next section. atmospheric iodine cycle, model calculations (Pechtl et al., − 2006) suggest that IO3 should accumulate in marine aerosol. iii. Moreover, ammonium iodate is expected to be an abun- However, several field campaigns (Baker, 2004; Gilfedder et dant iodate salt in the atmosphere, since ammonium al., 2008) have revealed that the iodide = iodate ratio is rather concentrations are high in some environments, and it − variable in aerosol, showing significant I concentration. could be deposited into the ice as large fluxes of iodi- − A recent study has suggested that IO3 anions show a sub- nated compounds have been observed during glacial pe- stantial reactivity in frozen solutions under near-ultraviolet– riods (Spolaor et al., 2013); the presence of ammonium visible (UV–Vis) light irradiation (Spolaor et al., 2013). Dur- ions in ice samples is also expected. Moreover, ammo- − ing the irradiation of IO3 frozen solutions, reactive gaseous nium and iodinated compounds have been detected at iodine species were produced and converted to iodine oxide the same time in melting Arctic sea ice, implying that particles (IOPs) for detection. Inspired by these results, we this salt could be atmospherically relevant (Assmy et have further studied the photostability of iodate frozen salts al., 2013). Note, however, that other salts such as NaIO3 to assess its potential role in iodine emissions to the polar at- or KIO3 would be representative of polar environments mosphere. In this work, we have determined the absorption too, and further experiments using these compounds cross section of the NH4IO3 solution, which has been used should be addressed in the future. to estimate for the first time the absorption cross section and quantum yield of frozen ammonium iodate solutions at wave- Solid samples containing iodate anions were produced lengths relevant for the troposphere, from 250 to 400 nm. through the sudden freezing of droplets of aqueous solutions The product of these two quantities gives us the efficiency of NH4IO3 on a cold Si substrate located inside a vacuum of the photolytic process, but these values should be taken chamber. A detailed description of the experimental setup as a lower limit that needs to be explored in further detail can be found elsewhere (Maté et al., 2009; Gálvez et al., in future laboratory work. This information has been incor- 2010), and only a brief description of the most relevant as- porated into an atmospheric model to assess the potential of pects for the present experiments is given here. The solid iodate photolysis to release reactive iodine to the Antarctic substrate is mounted in a Cu block in contact with a liquid boundary layer during springtime. nitrogen Dewar. The substrate temperature can be controlled with 1 K accuracy between 90 and 300 K. The vacuum cham- ber, which is coupled to a Bruker VERTEX 70 Fourier trans- 2 Experimental methods form infrared spectroscopy (FTIR) spectrometer through a purged pathway, is evacuated with a turbomolecular pump to For the study of the photolysis of iodate salts, we have tested a background pressure of ∼ 10−8 mbar. Transmission spectra several iodated compounds. Firstly, the photolysis of frozen of the samples were recorded, with 2 cm−1 resolution, using solutions of KIO3 was studied, and significant photolysis was an MCT (mercury cadmium telluride) detector refrigerated observed (for more details see the Supplement). However, with liquid nitrogen. Liquid solution droplets from a room − due to the overlapping of the IO3 IR band with water ab- temperature pulsed valve (General Valve, series 9), usually sorption, we studied NH4IO3 for the following reasons: employed for the generation of free jets and molecular beams (Abad et al., 1995), were made to impinge on the cold Si i. As mentioned above, it was not possible to monitor io- substrate placed at ∼ 15–20 mm. When a desired amount of date signal in the presence of high concentrations of wa- sample is on the substrate, this can be rotated to record the IR ter since the infrared iodate band overlaps with water spectra, or to be processed by simulated solar light. A scheme absorptions. The fact that the chosen salt has a cation of the experimental setup is shown in Fig. 1. Solar irradiance C ® like NH4 that presents a band with no interference (and was simulated by a 1000 W LOT Xenon Arc lamp that radi- that it is consumed in a 1 : 1 ratio with iodate; see Sup- ates between around 250 nm and 2.5 µm, although an impor- plement) allowed us to measure the photolysis of iodate tant fraction of the output is given below 900 nm according indirectly as described below. to the supplier of this lamp, where a fairly constant spectral irradiance is obtained between 300 and 900 nm. Power light ii. As far as we know, there is no information in the litera- received on the substrate is measured by a portable thermal ture of the integrated value of the IR absorption coeffi- detector meter, model 407A by Spectra-Physics, which op- cient of the iodate band, and in consequence it was not erates in a wavelength range from 250 nm to 11 µm without possible to directly quantify the amount of iodate in the significant sensitivity variations (less than 3 %). samples. One of the possibilities to solve this problem is UV–Vis spectra of the studied salts were obtained in wa- to use an iodate salt for which the integrated absorption ter solution at different concentrations using both a UV–Vis coefficient of the IR band of the counter-ion was known, Uvikon spectrophotometer 930 from Kontron Instruments like ammonium iodate.
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