Probing Functional Groups at the Gas–Aerosol Interface Using Heterogeneous Titration Reactions: A Tool for Predicting Aerosol Health Effects?

Setyan, Ari; Sauvain, Jean‐Jacques; Guillemin, Michel; Riediker, Michael; Demirdjian, Benjamin; Rossi, Michel J.

doi:10.1002/cphc.201000490

Cited by 27 publications

(29 citation statements)

References 74 publications

(120 reference statements)

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“…Ozone is a strong oxidizing agent which has been applied as a probe gas for reducing functional groups on various solid substrates (e.g., Setyan et al, , ; Tapia et al, , ), and we similarly attribute its uptake on the glass and ash material to adsorption on reducing surface sites (Maters et al, ). These sites may include oxygen deficiencies in the anionic oxide (O 2− ) network at the solid‐gas interface (Diebold, ) and transition metal atoms (e.g., Fe) in their lower valence state (e.g., Fe 2+ ) present in varying abundance on the aluminosilicate samples (Maters et al, ).…”

Section: Discussionmentioning

confidence: 99%

Reactive Uptake of Sulfur Dioxide and Ozone on Volcanic Glass and Ash at Ambient Temperature

et al. 2017

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The atmospheric impacts of volcanic ash from explosive eruptions are rarely considered alongside those of volcanogenic gases/aerosols. While airborne particles provide solid surfaces for chemical reactions with trace gases in the atmosphere, the reactivity of airborne ash has seldom been investigated. Here we determine the total uptake capacity (NiM) and initial uptake coefficient (γM) for sulfur dioxide (SO2) and ozone (O3) on a compositional array of volcanic ash and glass powders at ~25°C in a Knudsen flow reactor. The measured ranges of NiSO2 and γSO2 (1011–1013 molecules cm−2 and 10−3–10−2) and NiO3 and γO3 (1012–1013 molecules cm−2 and 10−3–10−2) are comparable to values reported for mineral dust. Differences in ash and glass reactivity toward SO2 and O3 may relate to varying abundances of, respectively, basic and reducing sites on these materials. The typically lower SO2 and O3 uptake on ash compared to glass likely results from prior exposure of ash surfaces to acidic and oxidizing conditions within the volcanic eruption plume/cloud. While sequential uptake experiments overall suggest that these gases do not compete for reactive surface sites, SO2 uptake forming adsorbed S(IV) species may enhance the capacity for subsequent O3 uptake via redox reaction forming adsorbed S(VI) species. Our findings imply that ash emissions may represent a hitherto neglected sink for atmospheric SO2 and O3.

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Section: Discussionmentioning

confidence: 99%

Reactive Uptake of Sulfur Dioxide and Ozone on Volcanic Glass and Ash at Ambient Temperature

et al. 2017

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“…Unless otherwise noted, all materials of commercial origin have been used as received. 16 . This sample has been called "Diesel TPG".…”

Section: Source Of Materialsmentioning

confidence: 99%

“…We hereby propose a direct gas-phase titration technique with the following advantages: (a) it enables the use of MS-based techniques sensitive to less than one per cent of a molecular monolayer; (b) the low sample mass requirement in the range of one mg or so directly enables the investigation of ambient aerosol samples or from smog chambers; (c) the present approach emphasizes the measurement of interfacial or subsurface physical and chemical properties of nanoparticles not easily performed by spectroscopic methods, especially when molecular information is required. Setyan et al 16 have recently successfully used this technique for the investigation of aerosols sampled in the field.…”

Section: Introductionmentioning

confidence: 99%

The use of heterogeneous chemistry for the characterization of functional groups at the gas/particle interface of soot and TiO2 nanoparticles

Setyan

Sauvain

Rossi

2009

Phys. Chem. Chem. Phys.

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Six gases [N(CH(3))(3), NH(2)OH, CF(3)COOH, HCl, NO(2) and O(3)] were selected to probe the surface of seven different types of combustion aerosol samples (amorphous carbon, flame soot) and three types of TiO(2) nanoparticles using heterogeneous, i.e. gas-surface reactions. The gas uptake to saturation of the probes was measured under molecular flow conditions in a Knudsen flow reactor and expressed as a density of surface functional groups on a particular aerosol, namely acidic (carboxylic) and basic (conjugated oxides such as pyrone, N-heterocycle and amine) sites, carbonyl (R(1)-C(O)-R(2)) and oxidizable (olefinic, -OH) groups. The limit of detection was generally well below 1% of a formal monolayer of adsorbed probe gas. With few exceptions most investigated aerosol samples interacted with all probe gases to various extents which points to the coexistence of different functional groups on the same aerosol surface such as acidic and basic groups. Generally, the carbonaceous particles displayed significant differences in surface group density: Printex 60 amorphous carbon had the lowest density of surface functional groups throughout, whereas Diesel soot recovered from a Diesel particulate filter had the largest. The presence of basic oxides on carbonaceous aerosol particles was inferred from the ratio of uptakes of CF(3)COOH and HCl owing to the larger stability of the acetate compared to the chloride counterion in the resulting pyrylium salt. Both soots generated from a rich and a lean hexane diffusion flame had a large density of oxidizable groups similar to amorphous carbon FS 101. TiO(2) 15 had the lowest density of functional groups studied for all probe gases among the three TiO(2) nanoparticles despite the smallest size of its primary particles. The technique used enabled the measurement of the uptake probability of the probe gases on the various supported aerosol samples. The initial uptake probability, gamma(0), of the probe gas onto the supported nanoparticles differed significantly among the various investigated aerosol samples but was roughly correlated with the density of surface groups, as expected.

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“…Ambient particles are associated with a clearly increased risk for cardiovascular and pulmonary morbidity and mortality and the creation of reactive oxygen species (ROS) has repeatedly been proposed to be centrally involved in this response (Brook et 2010). A recent study of workers exposed to diesel exhaust suggested that functional groups such as reactive carbonyls promoted oxidative stress (Setyan et al 2010). Thus, a potential strategy could be to evaluate the types of functional groups that are formed during the degradation of nanomaterials, and to compare them with a (yet to be established) library listing the oxidative stress potential of a wide range of functional groups.…”

Section: Physicochemical and Biological Characteristics Of Nanomaterialsmentioning

confidence: 99%

Biological impact assessment of nanomaterial used in nanomedicine. Introduction to the NanoTEST project

et al. 2013

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Therapeutic nanoparticles (NPs) are used in nanomedicine as drug carriers or imaging agents, providing increased selectivity/specificity for diseased tissues. The first NPs in nanomedicine were developed for increasing the efficacy of known drugs displaying dose-limiting toxicity and poor bioavailability and for enhancing disease detection. Nanotechnologies have gained much interest owing to their huge potential for applications in industry and medicine. It is necessary to ensure and control the biocompatibility of the components of therapeutic NPs to guarantee that intrinsic toxicity does not overtake the benefits. In addition to monitoring their toxicity in vitro, in vivo and in silico, it is also necessary to understand their distribution in the human body, their biodegradation and excretion routes and dispersion in the environment. Therefore, a deep understanding of their interactions with living tissues and of their possible effects in the human (and animal) body is required for the safe use of nanoparticulate formulations. Obtaining this information was the main aim of the NanoTEST project, and the goals of the reports collected together in this special issue are to summarise the observations and results obtained by the participating research teams and to provide methodological tools for evaluating the biological impact of NPs.

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Probing Functional Groups at the Gas–Aerosol Interface Using Heterogeneous Titration Reactions: A Tool for Predicting Aerosol Health Effects?

Cited by 27 publications

References 74 publications

Reactive Uptake of Sulfur Dioxide and Ozone on Volcanic Glass and Ash at Ambient Temperature

Reactive Uptake of Sulfur Dioxide and Ozone on Volcanic Glass and Ash at Ambient Temperature

The use of heterogeneous chemistry for the characterization of functional groups at the gas/particle interface of soot and TiO2 nanoparticles

Biological impact assessment of nanomaterial used in nanomedicine. Introduction to the NanoTEST project

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