(4at) First Principles-Based Multiscale Modeling of Dispersed, Multifunctional Heterogeneous Catalysts in Dynamic Reactive Environments for Decarbonization

As the world’s appetite for commodity and fine chemicals continuously grows, the development of processes for the sustainable and decarbonized production of chemicals and for the remediation of chemical wastes is critical. Dispersed, multifunctional heterogeneous catalysts lie at the heart of these transformations, finding applications in biomass upgrading, shale gas reforming, and plastics upcycling. Periodically operated reactors have been demonstrated to further improve the reactivity and selectivity of these processes. Practically, dispersed catalysts are desirable as they efficiently utilize a large atomic fraction of the precious active component, while the flexibility of multifunctional catalysts allows the user to tailor their composition for the desired application. In recent decades, much attention has been invested to understand the structure of the dispersed active sites, the physicochemical interactions among the active components, and the dynamics of the active site structure and reaction pathways. In my future research, I plan to perform multiscale modeling rooted in first principles simulations to study the structure and reactivity of dispersed and multifunctional heterogeneous catalysts in dynamic reactive environments. Achieving a rigorous, transparent and physics-informed understanding of the catalytic sites forms the foundation for improving catalyst design.

In my doctoral and postdoctoral research, I employed multiscale modeling techniques to understand the structure and reactivity of dispersed and multifunctional heterogeneous catalysts. In my doctoral research, in collaborative works with experimentalists, I used atomistic thermodynamics to describe the structure of the support and active sites of single atom and cluster catalysts and to understand spectroscopic measurements under reactive environmental conditions.^1-4 Further, in collaboration with colleagues, I developed and analyzed detailed microkinetic models to explain the kinetic behavior of (de)hydrogenations reactions occurring over dispersed multi-site catalysts.^4-8 In my current postdoctoral research, I used concepts from stiff kinetic Monte Carlo simulations and dynamical systems theory to analyze and simplify transient kinetic networks.⁹ Additionally, in collaboration with colleagues, I developed physics-informed models to describe interfacial phenomena of prototypical dispersed metal catalysts.^{10, 11} Overall, my research experience has equipped me to explore the complexities of dispersed, multifunctional heterogeneous catalysts using multiscale modeling techniques in a collaborative research environment.

Teaching Interests:

As my background at each level is in chemical engineering, I am prepared to teach the core classes of a chemical engineering curriculum. My research experience makes me best equipped to teach courses in thermodynamics, reaction engineering, and mathematical methods for chemical engineers. In addition, based on my research skillset, I can also develop elective courses in first-principles modeling, heterogeneous catalysis from a theoretical/computational perspective, and numerical modeling using Python.

Throughout my academic journey, I was very lucky to have had teaching opportunities at each stage. As an undergraduate, I served as an apprentice teacher for an introductory course in fluid mechanics, where, with a fellow apprentice teacher, we planned and hosted a weekly problem-solving session and tutored individual students. During my PhD, I worked as a teaching assistant for both an undergraduate course on the thermodynamics of mixtures and a graduate course on statistical thermodynamics. Additionally, I mentored an undergraduate student on performing first-principles calculations and multiple PhD students on microkinetic modeling. Through these experiences, we have authored or contributed to multiple collaborative papers. Finally, as a postdoctoral researcher, I had the opportunity to deliver two lectures on quantum chemical calculations and statistical thermodynamics in a graduate course on reaction kinetics. Overall, my experiences have prepared me to teach and mentor both undergraduate and graduate students.

Selected Publications: (* indicates equal contribution)

1. G. Yan*, Y. Tang*, Y. T. Li*, Y. X. Li, L. Nguyen, T. Sakata, K. Higashi, F. Tao, P. Sautet, Nat. Catal., 2022, 5 (2), 119-127.

2. G. Yan, T. Waehler, R. Schuster, M. Schwarz, C. Hohner, K. Werner, J. Libuda, P. Sautet, J. Am. Chem. Soc., 2019, 141 (14), 5623-5627.

3. G. Yan, P. Sautet, ACS Catal., 2019, 9 (7), 6380-6392. Erratum: 10.1021/acscatal.9b03445.

4. Y. Tang*, G. Yan*, S. Zhang*, L. T. Nguyen*, Y. T. Li, Y. Iwasawa, T. Sakata, C. Andolina, J. C. Yang, P. Sautet, F. Tao, Submitted.

5. N. Marcella*, J. S. Lim*, A. M. PÅ‚onka*, G. Yan*, C. J. Owen, J. E. S. van der Hoeven, A. C. Foucher, H. T. Ngan, S. B. Torrisi, N. S. Marinkovic, E. A. Stach, J. F. Weaver, P. Sautet, B. Kozinsky, A. I. Frenkel, Nat. Commun., 2022, 13 (1), 832.

6. H. T. Ngan, G. Yan, J. E. S. van der Hoeven, R. J. Madix, C. M. Friend, P. Sautet, ACS Catal., 2022, 12 (21), 13321-13333.

7. J. E. S. van der Hoeven, H. T. Ngan, G. Yan, J. Aizenberg, R. J. Madix, P. Sautet, C. M. Friend, J. Phys. Chem. C, 2022, 126 (37), 15710-15723. Erratum: 10.1021/acs.jpcc.2c04982.

8. D. Patel*, G. Giannakakis*, G. Yan*, H. T. Ngan, P. Yu, R. Hannagan, P. Kress, J. Shan, P. Deshlahra, P. Sautet, E. C. H. Sykes, ACS Catal., 2023, 13 (7), 4290-4303.

9. G. Yan, D. G. Vlachos, ACS Catal., 2023, 13(16), 10602-10614.

10. G. Yan*, S. A. Khan*, D. G. Vlachos, Submitted.

11. G. Yan, D. G. Vlachos, Submitted.