ChemInform Abstract: Atmospheric Sulfidation of Copper Single Crystals.

Graedel, T. E.; Franey, J. P.; Kammlott, G. W.; Vandenberg, J. M.; Key, P. L.

doi:10.1002/chin.198743025

Cited by 5 publications

(12 citation statements)

References 1 publication

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“…Table I. The In and Al are thought to form vacancy traps that could slow the sulfidation reaction by limiting the Cu permeability and thus influence the supply of Cu (9). Resistance changes in the meander lines were monitored, in-situ, as a function of exposure time to a 50 ppb H 2 S, 80% RH, air environment at 35ºC.…”

Section: Methodsmentioning

confidence: 99%

“…The mechanisms for this Cu 2 S growth is clearly more complex than the simple model proposed by Graedel [9] for atmospheric sulfidation of Cu single crystals.…”

mentioning

confidence: 86%

“…In general, the goal of previous investigators was to characterize and mitigate any detrimental corrosion effects. Contrary to the corrosion processes that occur on many engineering alloys in which localized attack is prevalent, corrosion of copper has been typically viewed as a "relatively simple" uniform phenomenon [1,[6][7][8][9] (modeled pictorially in figure 3.1) with the following processes proposed by Graedel and co-workers [6,7]:…”

Section: General Copper Sulfidation Behaviormentioning

confidence: 99%

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Mechanisms of Atmospheric Copper Sulfidation and Evaluation of Parallel Experimentation Techniques

Barbour¹,

Sullivan²,

Campin³

et al. 2002

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A physics-based understanding of material aging mechanisms helps to increase reliability when predicting the lifetime of mechanical and electrical components. This report examines in detail the mechanisms of atmospheric copper sulfidation and evaluates new methods of parallel experimentation for high-throughput corrosion analysis. Often our knowledge of aging mechanisms is limited because coupled chemical reactions and physical processes are involved that depend on complex interactions with the environment and component functionality. Atmospheric corrosion is one of the most complex aging phenomena and it has profound consequences for the nation's economy and safety. Therefore, copper sulfidation was used as a test-case to examine the utility of parallel experimentation. Through the use of parallel and conventional experimentation, we measured: (1) the sulfidation rate as a function of humidity, light, temperature and O 2 concentration; (2) the primary moving species in solid state transport; (3) the diffusivity of Cu vacancies through Cu 2 S; (4) the sulfidation activation energies as a function of relative humidity (RH); (5) the sulfidation induction times at low humidities; and (6) the effect of light on the sulfidation rate. Also, the importance of various sulfidation mechanisms was determined as a function of RH and sulfide thickness. Different models for sulfidation-reactor geometries and the sulfidation reaction process are presented.

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Section: Methodsmentioning

confidence: 99%

“…The mechanisms for this Cu 2 S growth is clearly more complex than the simple model proposed by Graedel [9] for atmospheric sulfidation of Cu single crystals.…”

mentioning

confidence: 86%

Section: General Copper Sulfidation Behaviormentioning

confidence: 99%

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Mechanisms of Atmospheric Copper Sulfidation and Evaluation of Parallel Experimentation Techniques

Barbour¹,

Sullivan²,

Campin³

et al. 2002

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“…Copper is widely used in a number of critical electrical applications, and the problem and study of copper corrosion is a major area of research [1][2][3][4][5][6][7][8]. Previous researchers have studied the sulfidation of copper using SO 2 and H 2 S gas and found that these reactants interact at the wateroxide interface, possibly at copper oxide grain boundaries [5,[9][10].…”

Section: Background On Copper Sulfidationmentioning

confidence: 99%

“…Previous researchers have studied the sulfidation of copper using SO 2 and H 2 S gas and found that these reactants interact at the wateroxide interface, possibly at copper oxide grain boundaries [5,[9][10]. Solid-state diffusion of copper through Cu 2 O is thought to control the nucleation and initial Cu 2 S island growth on Cu 2 O -in the case of exposure to H 2 S gas -and copper-sulfite and copper-sulfate formation -in the case of exposure to SO 2 gas [5][6]. Also, for both H 2 S and SO 2 exposure, the rate of sulfidation can be controlled by the supply of corroding gas to the surface [4][5][11][12].…”

Section: Background On Copper Sulfidationmentioning

confidence: 99%

The effects of varying humidity on copper sulfide film formation.

Mayer¹,

Missert²,

Barbour³

et al. 2004

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Detailed experiments involving extensive high resolution transmission electron microscopy (TEM) revealed significant microstructural differences between Cu sulfides formed at low and high relative humidity (RH). It was known from prior experiments that the sulfide grows linearly with time at low RH up to a sulfide thickness approaching or exceeding one micron, while the sulfide initially grows linearly with time at high RH then becomes sub-linear at a sulfide thickness less than about 0.2 microns, with the sulfidation rate eventually approaching zero. TEM measurements of the Cu 2 S morphology revealed that the Cu 2 S formed at low RH has large sized grains (75 to greater than 150 nm) that are columnar in structure with sharp, abrupt grain boundaries. In contrast, the Cu 2 S formed at high RH has small equiaxed grains of 20 to 50 nm in size. Importantly, the small grains formed at high RH have highly disordered grain boundaries with a high concentration of nano-voids. Two-dimensional diffusion modeling was performed to determine whether the existence of localized source terms at the Cu/Cu 2 S interface could be responsible for the suppression of Cu sulfidation at long times at high RH. The models indicated that the existence of static localized source terms would not predict the complete suppression of growth that was observed. Instead, the models suggest that the diffusion of Cu through Cu 2 S becomes restricted during Cu 2 S formation at high RH. The leading speculation is that the extensive voiding that exists at grain boundaries in this material greatly reduces the flux of Cu between grains, leading to a reduction in the rate of sulfide film formation. These experiments provide an approach for adding microstructural information to Cu sulfidation rate computer models. In addition to the microstructural studies, new micro-patterned test structures -4 -were developed in this LDRD to offer insight into the point defect structure of Cu 2 S and to permit measurement of surface reaction rates during Cu sulfidation. The surface reaction rate was measured by creating micropatterned Cu lines of widths ranging from 5 microns to 100 microns. When sulfidized, the edges of the Cu lines show greater sulfidation than the center, an effect known as microloading. Measurement of the sulfidation profile enables an estimate of the ratio of the diffusivity of H 2 S in the gas phase to the surface reaction rate constant, k. Our measurements indicated that the gas phase diffusivity exceeds k by more than 10, but less than 100. This is consistent with computer simulations of the sulfidation process. Other electrical test structures were developed to measure the electrical conductivity of Cu 2 S that forms on Cu. This information can be used to determine relative vacancy concentrations in the Cu 2 S layer as a function of RH. The test structures involved micropatterned Cu disks and thin films, and the initial measurements showed that the electrical approach is feasible for point defect studies in Cu 2 S.

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Commentary: From Mindmeld to Mindset: Negotiating the Information Minefield in Developing Countries

Adamu

2002

Bul. Am. Soc. Info. Sci. Tech.

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ChemInform Abstract: Atmospheric Sulfidation of Copper Single Crystals.

Abstract: (100), (110), and (111) single crystals of Cu and polycrystalline copper have been exposed to a controlled test atmosphere containing low concentrations of H2S, designed to simulate atmospheric sulfidation.

Cited by 5 publications

References 1 publication

Mechanisms of Atmospheric Copper Sulfidation and Evaluation of Parallel Experimentation Techniques

Mechanisms of Atmospheric Copper Sulfidation and Evaluation of Parallel Experimentation Techniques

The effects of varying humidity on copper sulfide film formation.

Commentary: From Mindmeld to Mindset: Negotiating the Information Minefield in Developing Countries

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