Theoretical Descriptors for Electrochemical Devices: Interfaces-Transport

Abstract

Meeting climate targets demands technologies that convert renewable electricity into storable fuels while valorizing CO₂ emissions. Electrochemical routes offer direct pathways but face a critical gap: classical single-site descriptors fail to predict device-level performance, where coverage effects, interfacial microenvironments, and collective transport phenomena dominate. This challenge is intensified by sustainability pressures and upcoming forever chemicals phase-outs that threaten key membrane technologies.

This thesis establishes a descriptor framework that bridges molecular understanding with device performance, systematically advancing from active sites through composite interfaces to collective transport. The approach integrates density-functional theory, ab initio molecular dynamics, and machine-learning simulations in synergy with experiments, applying a consistent methodology across earth-abundant materials spanning the full device architecture—from fuel-forming cathodes (hydrogen evolution reaction (HER) and electrochemical CO₂ reduction reaction) to ion-selective membranes.

This descriptor-driven design uncovers: (i) coverage-dependent adsorbate interactions; (ii) photocatalytic cascades enabling H₂ formation on HER-inactive materials; (iii) MOF linkers tuning CO₂ activation; and (iv) structural-chemical descriptors guiding fluorine-free, high-diffusivity membranes.

By unifying catalyst energetics and membrane transport under a common framework, this work demonstrates how systematic multi-scale design can close the laboratory-to-device gap, delivering sustainable, earth-abundant electrochemical systems and validated principles for their deployment.

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