Tailoring nanopore formation in atomic layer deposited ultrathin films

S. Karwal, T. Li, A. Yanguas-Gil, C.P. Canlas, Y. Lei, A.U. Mane, J.A. Libera, S. Seifert, R.E. Winans, J.W. Elam

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Abstract

Selectivity is a critical attribute of catalysts used in manufacturing of essential and fine chemicals. An excellent way to induce selectivity in catalysts is by using ultrathin films with tailored nanoporosity. For instance, nanopores can be created in atomic layer deposition (ALD) ultrathin over-coatings on supported metal nanoparticles by subjecting the coatings to high temperature annealing. These nanopores expose the active surface of the underlying metal nanoparticles. The dimensions of these nanopores can be tuned to impart shape selectivity: only reactants or products with a specific size or shape can fit inside the pore. In this work, the authors explore the underlying mechanism driving nanopore formation in ALD films. Ultrathin films of ALD TiO2 (∼2.5 nm thick) and ALD Al2O3 (∼4.9 nm thick) were deposited on nonporous γ-Al2O3 nanoparticles. The pore formation and evolution were monitored in situ during thermal annealing using small-angle x-ray scattering (SAXS), and the crystallinity was monitored by in situ x-ray diffraction. A correlation between the nanopore formation and amorphous to crystalline phase transitions in the ALD layers was observed. The authors hypothesize that the pores form through the relaxation of stress induced by densification of the ALD films during the phase transitions. The authors developed a mathematical model to evaluate this hypothesis and found remarkable agreement between the model and the SAXS measurements.

Original languageEnglish
Article number01A103
Number of pages7
JournalJournal of Vacuum Science and Technology A: Vacuum, Surfaces, and Films
Volume36
Issue number1
DOIs
Publication statusPublished - 1 Jan 2018

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Nanopores
Atomic layer deposition
Ultrathin films
atomic layer epitaxy
Catalyst selectivity
Metal nanoparticles
selectivity
x ray scattering
porosity
X rays
nanoparticles
Phase transitions
Scattering
Annealing
coatings
catalysts
Coatings
Catalysts
annealing
densification

Cite this

Karwal, S. ; Li, T. ; Yanguas-Gil, A. ; Canlas, C.P. ; Lei, Y. ; Mane, A.U. ; Libera, J.A. ; Seifert, S. ; Winans, R.E. ; Elam, J.W. / Tailoring nanopore formation in atomic layer deposited ultrathin films. In: Journal of Vacuum Science and Technology A: Vacuum, Surfaces, and Films. 2018 ; Vol. 36, No. 1.
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Karwal, S, Li, T, Yanguas-Gil, A, Canlas, CP, Lei, Y, Mane, AU, Libera, JA, Seifert, S, Winans, RE & Elam, JW 2018, 'Tailoring nanopore formation in atomic layer deposited ultrathin films', Journal of Vacuum Science and Technology A: Vacuum, Surfaces, and Films, vol. 36, no. 1, 01A103. https://doi.org/10.1116/1.5003360

Tailoring nanopore formation in atomic layer deposited ultrathin films. / Karwal, S.; Li, T.; Yanguas-Gil, A.; Canlas, C.P.; Lei, Y.; Mane, A.U.; Libera, J.A.; Seifert, S.; Winans, R.E.; Elam, J.W.

In: Journal of Vacuum Science and Technology A: Vacuum, Surfaces, and Films, Vol. 36, No. 1, 01A103, 01.01.2018.

Research output: Contribution to journalArticleAcademicpeer-review

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