Controlling the Effect of Slug-to-Slug Variation on the Crystal Size Distribution of Perovskite QDs: A CFD-Based Approach
- Type: Conference Presentation
- Conference Type: AIChE Annual Meeting
- Presentation Date: November 10, 2021
- Duration: 21 minutes
- Skill Level: Intermediate
- PDHs: 0.50
Despite the intriguing advantages of SFCs, there are still some key issues with the operation of SFCs. For example, previous studies have not accounted for the effect of slug-to-slug (S2S) variation on crystal size distribution (CSD), and the absence of a modeling and control framework for CsPbBr3 QDs made it challenging to fine-tune the QD size distribution.  In response, we have developed a computational fluid dynamics (CFD) model to elucidate the mechanism of slug formation process in a millifluidic SFC, and then combined it with a slug crystallizer model to accurately model QD size distributions and precursor concentration profiles in SFC. Specifically, the slug crystallizer model was constructed by combining a continuum model with a previously developed kinetic Monte Carlo (kMC) model.  Based on the CFD-based multiscale modeling framework (i.e., CFD + continuum + kMC model), an optimal operation problem was formulated to ensure adequate set-point (QD size) tracking, resulting in a narrow CSD. Overall, (a) the proposed multiscale model is in good agreement with the experimental results; (b) the CFD simulation highlights the region in which the SFC should be operated (i.e., stable slug flow regime); and (c) the optimizer is capable of effective simultaneous set-point tracking (QD size) and disturbance rejection (S2S variation) while ensuring a narrow CSD.
In summary, the CFD model was used to identify a stable slug regime and quantify the S2S variation in a millifluidic SFC. Additionally, a dynamic multiscale model for a SFC was developed to describe the temporal evolution of average QD size and CSD. Lastly, an optimization-driven controller scheme was implemented to ensure that the QDs match the industry specifications while maintaining a narrow CSD. Overall, the proposed work is a major leap towards continuous nano-manufacturing of metal halide perovskite QDs, which will be crucial in meeting market demands of the optoelectronics industry in the coming decade.
- Protesescu L, Yakunin S, Bodnarchuk MI, Krieg F, Caputo R, Hendon CH, Yang RX, Walsh A, Kovalenko MV. Nanocrystals of cesium lead halide perovskites (CsPbX3, X= Cl, Br, and I): novel optoelectronic materials showing bright emission with a wide color gamut. Nano Letters. 2015 Jun 10; 15(6):3692-6.
- Pu Y, Cai F, Wang D, Wang JX, Chen JF. Colloidal synthesis of semiconductor quantum dots toward large-scale production: a review. Industrial & Engineering Chemistry Research. 2018 Feb 14; 57(6):1790-802.
- AbdelâLatif K, Epps RW, Kerr CB, Papa CM, Castellano FN, Abolhasani M. Facile roomâtemperature anion exchange reactions of inorganic perovskite quantum dots enabled by a modular microfluidic platform. Advanced Functional Materials. 2019 Jun; 29(23):1900712.
- Rasche ML, Jiang M, Braatz RD. Mathematical modeling and optimal design of multi-stage slug-flow crystallization. Computers & Chemical Engineering. 2016 Dec 5; 95:240-8.
- Sitapure N, Epps R, Abolhasani M, Kwon JS. Multiscale modeling and optimal operation of millifluidic synthesis of perovskite quantum dots: towards size-controlled continuous manufacturing. Chemical Engineering Journal. 2020 Dec 7:127905.
|AIChE Member Credits||0.5|
|AIChE Graduate Student Members||Free|
|AIChE Undergraduate Student Members||Free|