气候变化领域集成服务门户(CCPortal): In-cloud processing as a possible source of isotopically light iron from anthropogenic aerosols: New insights from a laboratory study

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DOI	10.1016/j.atmosenv.2021.118505
	In-cloud processing as a possible source of isotopically light iron from anthropogenic aerosols: New insights from a laboratory study
	Mulholland D.S.; Flament P.; de Jong J.; Mattielli N.; Deboudt K.; Dhont G.; Bychkov E.
发表日期	2021
ISSN	1352-2310
卷号	259
英文摘要	Wet atmospheric deposition can account for up to 50% of the total iron input to surface waters, so establishing the extent to which kinetic and equilibrium isotope effects can influence aerosol soluble δ56Fe values is imperative to trace and constrain aerosol sources using Fe isotopes and to understand the differences found between δ56Fe values for bulk and soluble phases of aerosols. In this context, changes in iron solubility and isotopic composition of dissolved Fe during simulated atmospheric processing of industrial ash was investigated. Kinetic and equilibrium experiments were performed under UV/VIS light using ash from a Fe–Mn alloy metallurgical plant and a synthetic solution that mimics cloud water chemistry. The nature of the Fe species of the industrial ash was investigated by Mössbauer Spectroscopy, whereas ash and dissolved δ56Fe values were measured by MC-ICP-MS. Mössbauer Spectroscopy revealed that α-hematite, magnetite, and poorly crystallized manganoferrite nanoparticles are the main Fe species. In the early-stage dissolution (until 60 min) a Fe isotope fractionation (Δ56Fesolution-bulk ash) of −0.284 ± 0.103‰ was found at the minimum contact time evaluated herein (i.e., 5 min) due to kinetic isotopic effects. In the late-stage dissolution (after 60 min) a Δ56Fesolution-ash of 0.227 ± 0.091‰ was found due to equilibrium isotopic effects. The kinetic isotope effect within one ash surface monolayer was modeled with an enrichment factor (ε) of −1‰ in 56Fe/54Fe ratio. Iron fractional dissolution undergone during different atmospheric processing time scales may release Fe with contrasted isotope compositions to solution, changing the original soluble Fe isotope signature (which is linked to its source). This might be especially important when the dissolution process goes from kinetic to near-equilibrium conditions, in which higher amounts of Fe are progressively released from ash surface. © 2021 Elsevier Ltd
关键词	Aerosol Cloud processing Iron dissolution Iron isotope Iron oxide Isotope fractionation
语种	英语
scopus关键词	Aerosols; Atmospheric chemistry; Deposition; Dissolution; Hematite; Iron alloys; Kinetics; Magnetite; Manganese alloys; Meteorological problems; Nucleation; Anthropogenic aerosols; Cloud processing; Fe isotopes; Fe species; In-cloud processing; Iron dissolution; Iron isotopes; Isotope fractionation; Laboratory studies; Mossbauer; Isotopes; ferric oxide; ferrite; iron; isotope; magnetite; manganese; manganoferrite; nanoparticle; unclassified drug; aerosol; anthropogenic effect; atmospheric deposition; isotopic analysis; isotopic composition; laboratory method; nanoparticle; reaction kinetics; solubility; surface water; air analysis; Article; ash; atmosphere; chemical composition; cloud; concentration (parameter); contact time; dissolution; equilibrium constant; fractionation; inductively coupled plasma mass spectrometry; kinetics; leaching; metal industry; metallurgy; Mossbauer spectroscopy; secondary organic aerosol; simulation; solubility; surface property; ultraviolet visible spectroscopy
来源期刊	ATMOSPHERIC ENVIRONMENT
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/248365
作者单位	Laboratoire de Physico-Chimie de l'Atmosphère, Université du Littoral Côte d'Opale, Dunkerque, France; Laboratoire G-Time, Université Libre de Bruxelles (ULB), Brussels, Belgium; Laboratório de Análises Ambientais – Química Ambiental, Universidade Federal do Tocantins, Gurupi, Tocantins, Brazil
推荐引用方式 GB/T 7714	Mulholland D.S.,Flament P.,de Jong J.,et al. In-cloud processing as a possible source of isotopically light iron from anthropogenic aerosols: New insights from a laboratory study[J],2021,259.
APA	Mulholland D.S..,Flament P..,de Jong J..,Mattielli N..,Deboudt K..,...&Bychkov E..(2021).In-cloud processing as a possible source of isotopically light iron from anthropogenic aerosols: New insights from a laboratory study.ATMOSPHERIC ENVIRONMENT,259.
MLA	Mulholland D.S.,et al."In-cloud processing as a possible source of isotopically light iron from anthropogenic aerosols: New insights from a laboratory study".ATMOSPHERIC ENVIRONMENT 259(2021).