Author ORCID Identifier

https://orcid.org/0009-0009-6217-3357

Semester

Spring

Date of Graduation

2026

Document Type

Dissertation

Degree Type

PhD

College

Statler College of Engineering and Mineral Resources

Department

Chemical and Biomedical Engineering

Committee Chair

Fernando V Lima

Committee Co-Chair

Wenyuan Li

Committee Member

Yuhe Tian

Committee Member

Edward M. Sabolsky

Committee Member

Sai Pushpitha Vudata

Abstract

The global imperative to decarbonize energy systems has intensified research into sustainable hydrogen production pathways, as hydrogen emerges as a critical energy carrier for sectors difficult to electrify directly. Among water electrolysis technologies, solid oxide electrolyzer cells operating at elevated temperatures offer the highest theoretical efficiency by utilizing thermal energy to reduce electrical energy requirements, yet comprehensive frameworks integrating electrochemical modeling with process operability analysis and techno-economic optimization remain scarce in the literature. This dissertation develops a process systems framework for proton-conducting solid oxide electrolyzer cells that bridges the gap between fundamental electrochemical phenomena and industrial-scale process economics. At the cell level, a comprehensive electrochemical model is developed incorporating the dusty gas model for multicomponent gas transport in porous electrodes, capturing the current density-voltage characteristics through reversible potential, activation overpotentials, ohmic losses, and concentration overpotentials. The validated cell model is integrated into a systematic process operability analysis using the Opyrability Python package, enabling quantification of operational flexibility through input-output mapping and identification of optimal operating conditions via Nonlinear programming-based optimization. At the system level, an industrial-scale process flowsheet is developed in AVEVA Process Simulation for hydrogen production at 50,000 kg/day capacity. The techno-economic analysis framework combines sequential quadratic optimization with Monte Carlo simulation for rigorous uncertainty quantification, while environmental sustainability is evaluated using the GREENSCOPE methodology. The electrochemical model demonstrates strong predictive capability with an R-squared of 0.96 when validated against experimental measurements across multiple operating temperatures. The operability analysis yields an operability index of 61.64% under specified production targets, with optimal conditions identified at 0.5 A/cm2 current density and 935 K temperature. Techno-economic optimization yields a evelized cost of hydrogen of $1.81/kg at favorable electricity prices, representing a 63.4% reduction from the DOE H2A process. Monte Carlo analysis indicates electricity price as the dominant cost driver, providing guidance for technology deployment priorities. Sustainability assessment yields a global warming potential of 2.11 kg CO2-eq/kg hydrogen, representing a 78.9% reduction compared to conventional steam methane reforming. The integrated process systems framework demonstrates that high-temperature solid oxide electrolysis represents a technically viable and economically competitive pathway for sustainable hydrogen production when coupled with low-cost renewable electricity. The substantial environmental benefits, combined with favorable economics below established cost targets, position this technology for commercial deployment and provide systematic tools for guiding strategic investment decisions in the transition toward a sustainable hydrogen economy.

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