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Numerical simulation of atomic layer deposition for thin deposit formation in a mesoporous substrate |
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| Authors: | Liwei Zhuang Peter Corkery Dennis T. Lee Seungjoon Lee Mahdi Kooshkbaghi Zhen-liang Xu Gance Dai Ioannis G. Kevrekidis Michael Tsapatsis |
| Affiliation: | 1. School of Chemical Engineering, East China University of Science and Technology, Shanghai, China;2. Department of Chemical and Biomolecular Engineering, Johns Hopkins University, Baltimore, Maryland, USA Institute for NanoBio Technology, Johns Hopkins University, Baltimore, Maryland, USA Contribution: Formal analysis, Investigation, Methodology, Validation, Writing - original draft, Writing - review & editing;3. Department of Chemical and Biomolecular Engineering, Johns Hopkins University, Baltimore, Maryland, USA;4. Program in Applied and Computational Mathematics, Princeton University, Princeton, New Jersey, USA;5. School of Chemical Engineering, East China University of Science and Technology, Shanghai, China Contribution: Formal analysis;6. Department of Chemical and Biomolecular Engineering, Johns Hopkins University, Baltimore, Maryland, USA Contribution: Validation, Writing - review & editing |
| Abstract: | ZnO deposition in porous γ-Al2O3 via atomic layer deposition (ALD) is the critical first step for the fabrication of zeolitic imidazolate framework membranes using the ligand-induced perm-selectivation process (Science, 361 (2018), 1008–1011). A detailed computational fluid dynamics (CFD) model of the ALD reactor is developed using a finite-volume-based code and validated. It accounts for the transport processes within the feeding system and reaction chamber. The simulated precursor spatiotemporal profiles assuming no ALD reaction were used as boundary conditions in modeling diethylzinc reaction/diffusion in porous γ-Al2O3, the predictions of which agreed with experimental electron microscopy measurements. Further simulations confirmed that the present deposition flux is much less than the upper limit of flux, below which the decoupling of reactor/substrate is an accurate assumption. The modeling approach demonstrated here allows for the design of ALD processes for thin-film membrane formation including the synthesis of metal–organic framework membranes. |
| Keywords: | atomic layer deposition computational fluid dynamics membrane zeolitic imidazolate framework, zinc oxide |