(2jy) Tuning the Interface for Carbon Dioxide Removal Chemistries with First Principles Computational Methods

Research Interests:
Climate change demands varied approaches to meet the necessarily aggressive goals set in 2018
to avoid a global climate disaster and one of these approaches must be carbon dioxide removal
(CDR). First principles atomic scale methods, including density functional theory (DFT), have
contributed heavily to other sustainable technologies (e.g., water splitting and energy storage)
but are relatively underutilized in carbon capture. Furthermore, computational materials design
has slowed somewhat in its ability to provide truly novel, predictive insights into the material or
surface properties required to carry out target chemistries. One reason for this computational
stagnation is that we have explored to near completion the easily accessible phase space of bulk
materials and their low energy surfaces exposed to vacuum. On the other hand, computational
efforts continue to improve at complementing experiments by explaining observed phenomena
at the atomic level. I aim to leverage this strength immediately by providing collaborative
assistance to experimentalists working in the CDR space while simultaneously working to
improve computational predictivity by exploring more complex (realistic) models. Realistic
chemistry takes place at an interface (often a solid-gas or solid-liquid interface) and first
principles methods including DFT have only just begun to explicitly query this highly complex
space.

My research will explore the fundamentals of explicit solid-liquid/gas interface modeling using
my background in carbon mineralization and physics-based electronic structure model derivation.
My research will target three main areas: 1) carbon mineralization at the surface-water interface
of structurally simple to model Ca and Mg containing minerals and find surface driven
mechanistic insights into the dissolution processes that are necessary for high carbonation
reaction conversions; 2) physics-informed model construction to understand and describe how
perturbations to the electronic structure of the surface in the presence of explicit liquid layers
result in changes to the adsorption energies of critical reaction intermediates; and 3) developing
a novel computational framework for the prediction of expected material surface faceting and
adsorbate coverage in the presence of different liquid/gas compositions at the interface. With
respect to Task 3, if models do not accurately capture the true surface composition and
coordination under reaction conditions, then the results will always be suspect. This is a crucial

area for modeling to focus on in the immediate future regardless of the presence or absence of
explicit interfacial models. This research plan will address the need for more realistic first
principles computational models. Most importantly, the research will be applied in the CDR space,
and experimental collaborations will provide relevance to the computational data in a field that
desperately needs to succeed in the coming decades for us to have a chance against the worst
effects of climate change.

Teaching Interests:
My unconventional background spending four years as a process engineer in industry has
prepared me to effectively combine practice with theory in teaching application-focused courses
like process control, design, health and safety, etc. Furthermore, my PhD training has reinforced
theoretical concepts especially with respect to thermodynamics, kinetics, and physical chemistry
and I would be well positioned to teach these as well. Finally, I am interested in designing courses
that expose students to computational science and its application to sustainable chemistries.

In addition to working as a teaching assistant for three semesters, I have given six guest lectures
across three different undergraduate and graduate chemical engineering courses while a PhD
student and mentored four undergraduate students in research. These students have gone on to
win poster awards and four of them are planning to apply to graduate school in chemical
engineering. I am a passionate mentor first and I believe that this is the role of an educator: to
build students up to their potential rather than break them down and show them their limits.

Keywords:
Interfacial Phenomena, Catalysis, Carbon Management