April 22 - 26, 2024
Seattle, Washington
May 7 - 9, 2024 (Virtual)

Event Supporters

2024 MRS Spring Meeting
MT01.08.09

Engineering Relative Stability in Four Dimensions with The Generalized Clausius-Clapeyron Relation

When and Where

Apr 25, 2024
4:45pm - 5:00pm
Room 320, Level 3, Summit

Presenter(s)

Co-Author(s)

Jiadong Chen1,Wenhao Sun1

University of Michigan1

Abstract

Jiadong Chen1,Wenhao Sun1

University of Michigan1
Sequential learning algorithms based on Bayesian optimization are routinely being deployed for materials stability optimization in high-parameter spaces. We anticipate these optimization methods would perform better if they were built upon stronger priors, for example, as derived from the fundamental thermodynamics underlying the equilibrium behavior of materials. Here, we present a thermodynamics-based technique to optimize the relative stability of a materials in high-dimensional thermodynamic space, based on a new derivation of a generalized high-dimensional Clausius Clapeyron relation. Using this thermodynamic infrastructure, we design several pathways to enhance the relative acid stability of Mn-oxides versus its dissolved states for potential electrochemical catalyst application. We construct a 4-D Pourbaix diagram with <i>p</i>H, redox potential <i>E</i>, particle radius 1/<i>R</i> and a chemical potential <i>μ</i><sub>K</sub> as axis. By exploring the gradients of the high-dimensional phase boundaries, we derive first-principles insights that nano-sizing (1/R) and certain doping ions (<i>μ</i><sub>K</sub>) can stabilize some metastable Mn-oxides polymorphs,<sub> </sub>where 1/R decreases acid stability and <i>μ</i><sub>K</sub> increases it. Our high-dimensional thermodynamic framework is a general method to engineer relative stability in parameter spaces that leverage multiple forms of thermodynamic work.

Keywords

ion-solid interactions | Mn | phase transformation

Symposium Organizers

Raymundo Arroyave, Texas A&M Univ
Elif Ertekin, University of Illinois at Urbana-Champaign
Rodrigo Freitas, Massachusetts Institute of Technology
Aditi Krishnapriyan, UC Berkeley

Session Chairs

Penghui Cao
Rodrigo Freitas

In this Session