Amorphous Alumina Coatings on Glass Bottles Using Direct Liquid Injection MOCVD for Packaging Applications

Etchepare, Pierre-Luc; Vergnes, Hugues; Samélor, Diane; Sadowski, Daniel C.; Brasme, Caroline; Caussat, Brigitte; Vahlas, Constantin

doi:10.4028/www.scientific.net/ast.91.117

Cited by 10 publications

(12 citation statements)

References 21 publications

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“…In view of their injection in the process chamber, both ATI and DMAI are dissolved in anhydrous cyclohexane. 19,20,24 For DMAI, the O/Al ratio is equal to 1 (O/Al = 3 for ATI) and for this reason an additional oxygen source (H 2 O or O 2 ) is required for the CVD of alumina from this precursor (O/Al = 1.5 in alumina). 17,18 The experimental protocols used for each process are presented in detail in the corresponding references and the process conditions are summarized in Table 1.…”

Section: Sample Preparationmentioning

confidence: 99%

Atomic scale structure of amorphous aluminum oxyhydroxide, oxide and oxycarbide films probed by very high field²⁷Al nuclear magnetic resonance

Baggetto

Sarou‐Kanian

Florian

et al. 2017

Phys. Chem. Chem. Phys.

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The atomic scale structure of aluminum in amorphous alumina films processed by direct liquid injection chemical vapor deposition from aluminum tri-isopropoxide (ATI) and dimethyl isopropoxide (DMAI) is investigated by solid-state Al nuclear magnetic resonance (SSNMR) using a very high magnetic field of 20.0 T. This study is performed as a function of the deposition temperature in the range 300-560 °C, 150-450 °C, and 500-700 °C, for the films processed from ATI, DMAI (+HO), and DMAI (+O), respectively. While the majority of the films are composed of stoichiometric aluminum oxide, other samples are partially or fully hydroxylated at low temperature, or contain carbidic carbon when processed from DMAI above 500 °C. The quantitative analysis of the SSNMR experiments reveals that the local structure of these films is built from AlO, AlO, AlO and Al(O,C) units with minor proportions of the 6-fold aluminum coordination and significant amounts of oxycarbides in the films processed from DMAI (+O). The aluminum coordination distribution as well as the chemical shift distribution indicate that the films processed from DMAI present a higher degree of structural disorder compared to the films processed from ATI. Hydroxylation leads to an increase of the 6-fold coordination resulting from the trend of OH groups to integrate into AlO units. The evidence of an additional environment in films processed from DMAI (+O) by Al SSNMR and first-principle NMR calculations on AlC and AlOC crystal structures supports that carbon is located in Al(O,C) units. The concentration of this coordination environment strongly increases with increasing process temperature from 600 to 700 °C favoring a highly disordered structure and preventing from crystallizing into γ-alumina. The obtained results are a valuable guide to the selection of process conditions for the CVD of amorphous alumina films with regard to targeted applications.

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Section: Sample Preparationmentioning

confidence: 99%

Atomic scale structure of amorphous aluminum oxyhydroxide, oxide and oxycarbide films probed by very high field²⁷Al nuclear magnetic resonance

Baggetto

Sarou‐Kanian

Florian

et al. 2017

Phys. Chem. Chem. Phys.

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“…Films composed of a-Al 2 O 3 are selected for this purpose due to their excellent barrier and anti-corrosion properties [19][20][21][22] and high optical transmission [23]. They compete with silica based coatings which also present excellent barrier properties, although limited durability [24].…”

Section: Introductionmentioning

confidence: 99%

Modeling a MOCVD process to apply alumina films on the inner surface of bottles

Etchepare¹,

Vergnes²,

Samélor³

et al. 2015

Surface and Coatings Technology

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a b s t r a c tDeposition inside a cavity with a narrow neck, i.e. a hollow body, is a challenge, in particular for the supply and the evacuation of the reactive phase and of the effluents through the same entrance. High gradients (pressure, velocity, species concentrations) and important convective mechanisms related to the impacting jet of the gaseous phase on the bottom inner wall of the cavity are created in that region. Given the increasing number of experimental parameters, modeling helps efficient process optimization with better understanding of physical and chemical phenomena occurring inside the hollow body. This study presents a numerical modeling using the CFD code Fluent to simulate a direct liquid injection metalorganic chemical vapor deposition of amorphous alumina coatings from aluminum tri-isopropoxide (ATI) on the inner walls of a glass bottle. The model is used to predict local profiles of gas velocity, temperature and species concentrations into the reactor as well as local growth rate based on an apparent heterogeneous kinetic law of ATI decomposition. Comparison with experimental thickness profiles allows validating the model and leads to a better insight in the phenomena which impact film thickness inhomogeneity along the inner surface. The model contributes to the improvement of the reactor configuration by increasing the distance between nozzle and bottle and the outlet section of the nozzle.

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“…[ 20 ] It is recalled that the reactive gas phase was driven with pure N 2 and introduced through a SS nozzle from the upper part of the quartz tube. In this confi guration, the total fl ow rate and the inlet ATI molar fraction were equal to 585 sccm and 1.7 × 10 −3 , respectively.…”

Section: Methodsmentioning

confidence: 99%

“…Interplay between simulation and deposition experiments allowed identifying the process conditions which led to the deposition of transparent coatings with uniform thickness profi le. [ 20,21 ] In a continuation of this theoretical work and of recently published preliminary experimental results, [ 22 ] we report hereafter on the experimental investigation of the process-structure-property relationship of coatings obtained by the DLI-CVD of ATI. First, we focus on the dissolution of ATI, with the aim to establish criteria for the selection of the different solvents and defi ne a priori the most appropriate one.…”

Section: Introductionmentioning

confidence: 99%

Amorphous Alumina Barrier Coatings on Glass: MOCVD Process and Hydrothermal Aging

Etchepare

Baggetto

Vergnes

et al. 2016

Adv Materials Inter

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OATAO is an open access repository that collects the work of Toulouse researchers and makes it freely available over the web where possible. This is an author-deposited version published in : http://oatao.univ-toulouse.fr/ Eprints ID : 15772 [ 9 ] radio frequency magnetron sputtering, [ 2 ] atomic layer deposition, [ 10 ] sol-gel, [ 5 ] and metalorganic chemical vapor deposition (MOCVD). [ 7,[11][12][13] CVD is one of the most attractive techniques for the time effi cient deposition of such coatings on complexin-shape geometries with conformal coverage, i.e., uniform thickness along the surface. Composition, stoichiometry, crystallinity, and microstructure of the material can be adjusted by fi ne tuning of the MOCVD experimental parameters such as reactor design, precursor selection, reactive atmosphere, deposition temperature, and pressure. The MOCVD of alumina from vaporized aluminum tri-isopropoxide (ATI) is very well documented. [ 7,8,[11][12][13][14][15][16] ATI yields amorphous and stoichiometric alumina coatings with a smooth and dense microstructure at 5 Torr in the temperature range 420 to 650 °C. [ 7,8,14,15 ] Higher process temperatures lead to the deposition of nanocrystallized γ -Al 2 O 3 [ 15 ] or to the homogeneous decomposition of ATI, which generates a different microstructure. [ 11 ] The ATI molecule is well described in the literature.[ 17 ] It is sensitive to water vapor and thus it is subjected to ageing upon exposure to ambient atmosphere, which results in its partial or total hydrolysis in nonvolatile compounds, Al(O i Pr) 3− n (OH) n ( n = 1, 2) and Al(OH) 3 , respectively. [ 12,17 ] The precursor is usually melted, maintained in supercooled state, and vaporized with a bubbler.Despite the simplicity and the cost effectiveness of this solution, the use of ATI in the supercooled state has two drawbacks. First, maintaining ATI at the vaporization temperature for a long-period impacts the stability of the molecule and subsequently the coating quality. [ 12 ] Second, it is diffi cult to know exactly the mass fl ow rate of the generated reactive gas. Such poorly controlled transport conditions lead to nonreproducible processes, especially for the present case when low activation energy prevails in the entire temperature range of interest, de facto resulting in mass transport limited process. The direct liquid injection (DLI) technology overcomes these drawbacks with the controlled vaporization of the solution made of ATI dissolved in a carrier solvent. [ 18 ] The DLI of ATI is insuffi ciently documented in the literature. Song et al. [ 19 ] and Krumdieck et al. [ 13 ] implemented the technique in a pulsedpressure MOCVD process. The authors used a solution of ATI in n -octane and in dry toluene, respectively. Coatings obtained

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Amorphous Alumina Coatings on Glass Bottles Using Direct Liquid Injection MOCVD for Packaging Applications

Cited by 10 publications

References 21 publications

Atomic scale structure of amorphous aluminum oxyhydroxide, oxide and oxycarbide films probed by very high field²⁷Al nuclear magnetic resonance

Atomic scale structure of amorphous aluminum oxyhydroxide, oxide and oxycarbide films probed by very high field²⁷Al nuclear magnetic resonance

Modeling a MOCVD process to apply alumina films on the inner surface of bottles

Amorphous Alumina Barrier Coatings on Glass: MOCVD Process and Hydrothermal Aging

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Amorphous Alumina Coatings on Glass Bottles Using Direct Liquid Injection MOCVD for Packaging Applications

Cited by 10 publications

References 21 publications

Atomic scale structure of amorphous aluminum oxyhydroxide, oxide and oxycarbide films probed by very high field27Al nuclear magnetic resonance

Atomic scale structure of amorphous aluminum oxyhydroxide, oxide and oxycarbide films probed by very high field27Al nuclear magnetic resonance

Modeling a MOCVD process to apply alumina films on the inner surface of bottles

Amorphous Alumina Barrier Coatings on Glass: MOCVD Process and Hydrothermal Aging

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Product

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Atomic scale structure of amorphous aluminum oxyhydroxide, oxide and oxycarbide films probed by very high field²⁷Al nuclear magnetic resonance

Atomic scale structure of amorphous aluminum oxyhydroxide, oxide and oxycarbide films probed by very high field²⁷Al nuclear magnetic resonance