Nucleation and growth: models for faceted and layered materials

Weatherspoon, Howard Bernard

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https://hdl.handle.net/2142/129435 Copy

Description

Title

Nucleation and growth: models for faceted and layered materials

Author(s)

Weatherspoon, Howard Bernard

Issue Date

2025-04-24

Director of Research (if dissertation) or Advisor (if thesis)

Peters, Baron

Doctoral Committee Chair(s)

Peters, Baron

Committee Member(s)

• Kenis, Paul
• Yang, Hong
• Statt, Antonia

Department of Study

Chemical & Biomolecular Engr

Discipline

Chemical Engineering

Degree Granting Institution

University of Illinois Urbana-Champaign

Degree Name

Ph.D.

Degree Level

Dissertation

Keyword(s)

• Nucleation and growth
• magic-sized clusters, covalent organic frameworks
• population balance equations

Abstract

This dissertation presents the development of mechanistic models to describe the nucleation and growth kinetics of various nanoparticle systems. Nucleation and the subsequent growth processes govern the outcomes of nanoparticle formation; however, the kinetics are complicated because numerous processes, pathways, and components are involved. To address this, we integrate classical and nonclassical nucleation theories (CNT and NCNT) with thermodynamic and kinetic modeling tools to predict particle size distributions, nucleation rates, and yield. A phenomenological free energy model incorporating atomistic interactions and Becker–Döring theory is developed to describe the layer-by-layer growth of tetrahedral magic-sized clusters (MSCs), a class of semiconductor nanocrystals, which is poorly captured by traditional CNT model due to their non-spherical geometry and discrete growth. We also present population balance models for covalent organic frameworks (COFs), accounting for multilayer growth via a two-step nucleation process involving crystallization and polymerization. These models include analytical and numerical solutions that track monomer concentration, induction time, and yield as functions of time. The population balance approach incorporates templated nucleation and lateral growth for multilayer COF formation. Altogether, these models link molecular-scale interactions and thermodynamic driving forces with macroscopic synthesis outcomes, offering a quantitative framework for predicting and controlling nanoparticle properties such as size and aspect ratio. This work bridges experimental observations with predictive modeling, enabling the optimization of nanoparticle and COF synthesis for applications ranging from optoelectronics to membrane separations.

Graduation Semester

2025-05

Type of Resource

Thesis

Handle URL

https://hdl.handle.net/2142/129435

Copyright and License Information

Copyright 2025 Howard Weatherspoon

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