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The surface behavior of mercury on iron systems
KTH, School of Industrial Engineering and Management (ITM), Materials Science and Engineering, Materials Process Science.
KTH, School of Information and Communication Technology (ICT), Material Physics, Material Physics, MF.
KTH, School of Industrial Engineering and Management (ITM), Materials Science and Engineering, Materials Process Science.
KTH, School of Industrial Engineering and Management (ITM), Materials Science and Engineering, Materials Process Science.
2006 (English)In: Metallurgical and materials transactions. B, process metallurgy and materials processing science, ISSN 1073-5615, E-ISSN 1543-1916, Vol. 37, no 6, 1049-1056 p.Article in journal (Refereed) Published
Abstract [en]

Thermal desorption Auger electron spectroscopy (TDAES) was used to investigate the circumstances under which mercury is adsorbed on the surface of iron in the temperature interval of 85 to 298 K. The effects of chlorine and oxygen modifications on the iron surface have also been investigated within the same temperature interval. It was seen that chlorine reduced the adsorption of mercury on polycrystalline iron at 85 K, as did oxygen. On the clean iron system at 298 K, only one monolayer (ML) of mercury adsorbed. The physisorption of mercury on chlorine and oxygen layers at low temperatures (LTs) is discussed in combination with the calculated activation energies of desorption, as well as the factors affecting the mechanism of adsorption at room temperature.

Place, publisher, year, edition, pages
2006. Vol. 37, no 6, 1049-1056 p.
Keyword [en]
atmospheric mercury, chemisorption, speciation, films
National Category
Metallurgy and Metallic Materials
Identifiers
URN: urn:nbn:se:kth:diva-16221DOI: 10.1007/BF02735027ISI: 000242967000023Scopus ID: 2-s2.0-33846199496OAI: oai:DiVA.org:kth-16221DiVA: diva2:334263
Note
QC 20100525Available from: 2010-08-05 Created: 2010-08-05 Last updated: 2017-12-12Bibliographically approved
In thesis
1. Towards Abatement of Selected Emissions from Metals Manufacturing
Open this publication in new window or tab >>Towards Abatement of Selected Emissions from Metals Manufacturing
2010 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Although the metallurgical industry has made great strides in the reduction of unwanted emissions to the atmosphere as a result of production processes, significant challenges still exist. From a global perspective, even large reductions in emissions per produced ton become immaterial when considering that the total world production of metals continues to increase. Two such particularly hazardous emissions are sulfur dioxide, primarily from copper ore roasting, and mercury, which has had increasing emissions from the steel industry in recent years. Both pollutants have severe consequences for the environment and also for human health. The primary motivations of this work have hence been: (1). to study sulfate formation on soot from sulfur dioxide emissions reacting with ozone and H2O in the vapor phase and (2). to study factors involving the behavior of mercury adsorption on metal surfaces involved in steelmaking, in order to further the understanding of select emissions from scrap-based steelmaking.

Gas phase experiments were conducted to examine the heterogeneous oxidation of sulfur dioxide on soot in the presence of ozone and water vapor. The sulfur dioxide oxidation into sulfate was quantified using a particle-into-liquid sampler coupled with ion chromatography to measure the sulfate formation at atmospheric pressure. Water vapor, ozone and sulfur dioxide concentrations were controlled.

Due to the ozone oxidation, multilayer adsorption of sulfur dioxide on soot, as well as sulfate formation and physisorption on secondary surface layer sites were observed. The exposure also caused the soot to become hydrophilic, due to the sulfur dioxide adsorption and also likely the formation of carboxyl groups on the surface. No significant increase in sulfate formation was observed at ozone concentrations above 1000 ppm.

The effects of common surface contaminants such as oxygen and chlorine were examined on the metal surfaces, as well as the impact of changes in temperature, with controlled conditions using thermal desorption auger electron spectroscopy. It was established that low temperatures (82 K through 111 K) were conducive to mercury adsorption, wherein physisorption and subsequent lateral mercury interactions in mercury adlayers occurred. Chlorine appeared to favor mercury uptake, as determined by the increased mercury coverage at low temperatures on polycrystalline iron, copper and zinc. Oxygen, however, was found to be an inhibitor of mercury, most notably at room temperature.

It was surprising to establish that no mercury adsorbed on zinc surfaces at room temperature and only on polycrystalline samples at low temperature. The mercury signal intensity increased up to the limit of the melting temperature for iron systems, on the oxidized copper surface and the polycrystalline zinc surfaces, prior to desorption from the surfaces. It is suggested that this is due to a rearrangement of mercury atoms on the surface at increasing temperatures, whereas at 85 K, mercury adhered to its initial adsorption position. In other words, mercury wet these surfaces on annealing, transitioning from an islanded surface at low temperature to a smooth layer before desorption. Based on these results, it was concluded that the mercury bond to the oxidized surface was weakened compared to clean copper. Furthermore, it is proposed that a surface phase transition occurred on polycrystalline zinc prior to desorption. No such transition was observed on iron.

Activation energies of desorption were calculated for the relevant metal surfaces. It was established that clean iron had the highest activation energy of desorption. The large bond strength between mercury and iron may account for the highest desorption temperature of the iron systems. Zinc and copper had similar activation energies and desorption temperatures, which were respectively lower than that of iron.

X-Ray Photoelectron and Auger Electron Spectroscopy were used to ascertain common surface contamination, i.e. chlorine, oxygen and sulfur, which affected mercury adsorption. Laser Ablation Inductively Coupled Plasma Time of Flight Mass Spectrometry was used to determine the depth of mercury adsorption on the samples. The technique also showed that the samples contained mercury in the surface layers.

Accompanied by the rising demand for metals is the increase in emissions from metals manufacturing. Moreover, it is critical to minimize sulfur dioxide emissions as particulates from soot continue to be released in the atmosphere. For scrap-based steelmaking, monolayer mercury adsorption on clean iron and copper at room temperature are significant results. With the rising use of electronic devices in vehicles, the sorting of scrap becomes increasingly important. Mercury not adsorbing on zinc at room temperature is also of relevance as it disproves the theory of increased mercury adsorption with the increased use of galvanized scrap in summer conditions. However, the low temperature studies showed multilayer adsorption of mercury on iron, zinc and copper, which has relevance for the reported temporal variations of mercury deposition in arctic regions.

Keywords: mercury, iron, zinc, sulfur dioxide, adsorption, pollution, thermal desorption, polycrystalline, surfaces, spectroscopy

Place, publisher, year, edition, pages
Stockholm: KTH, 2010. xiv, 74 p.
Keyword
mercury, zinc, iron, copper, sulfur dioxide, adsorption, pollution, spectroscopy, thermal desorption, polycrystalline, surfaces
National Category
Materials Engineering
Identifiers
urn:nbn:se:kth:diva-26107 (URN)978-91-7415-773-4 (ISBN)
Public defence
2010-11-26, F3, Lindstedtsvägen 26, KTH, Stockholm, 13:00 (English)
Opponent
Supervisors
Note
QC 20120326Available from: 2010-11-16 Created: 2010-11-15 Last updated: 2012-03-27Bibliographically approved
2. Hg metal surfaces: towards Hg abatement in steel plants
Open this publication in new window or tab >>Hg metal surfaces: towards Hg abatement in steel plants
2005 (English)Licentiate thesis, comprehensive summary (Other scientific)
Place, publisher, year, edition, pages
Stockholm: KTH, 2005. 48 p.
Keyword
iron, mercury, zinc, copper, Auger electron spectroscopy, thermal desorption, polycrystalline surfaces, adsorption, X-ray photoelectron spectroscopy, LA-ICP-TOFMS
National Category
Metallurgy and Metallic Materials
Identifiers
urn:nbn:se:kth:diva-4086 (URN)91-7178-233-8 (ISBN)
Presentation
2005-12-08, Sal B2, KTH, Brinellvägen, Stockholm, 10:00
Supervisors
Note
QC 20101220Available from: 2006-08-23 Created: 2006-08-23 Last updated: 2010-12-20Bibliographically approved

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