Date of Award

2026

Document Type

Open Access Dissertation

Degree Name

Doctor of Philosophy in Chemical Engineering (PhD)

Administrative Home Department

Department of Chemical Engineering

Advisor 1

Yixin Liu

Committee Member 1

Michael M. Mullins

Committee Member 2

Lei Pan

Committee Member 3

Kathryn A. Perrine

Abstract

Metal-oxide gas sensors remain essential for environmental monitoring, industrial safety, and emerging smart-infrastructure applications. However, their widespread deployment is constrained by persistent challenges in selectivity, humidity tolerance, and long-term stability. Harsh operating environments, characterized by fluctuating humidity, interfering gas mixtures, and variable temperatures, can destabilize surface states and disrupt charge-transfer pathways, leading to signal drift and reduced sensing reliability. Emerging applications of gas sensing require trace-level detection, regardless of environmental operating conditions. Addressing these limitations requires a deeper understanding of how defect chemistry, heterojunction formation, and surface-state engineering collectively govern gas-sensing behavior. This dissertation advances understanding through two complementary research directions. The first explores p-type and mixed-phase architectures that leverage heterojunction-driven sensitization. Electrospun ZnO/CoMoO4/ZnCo2O4 composite nanofibers achieved ~ 50 times increase in n-butanol sensing compared to pristine ZnCo2O4 spinel. Also, 250 ppb n-butanol detection was achieved with a Limit of Detection (LOD) of 29 ppb. This illustrates how interconnected n–p–p junctions, catalytic transition-metal sites, and high-surface-area nanostructured morphologies synergistically amplify sensing responses while accelerating surface reaction kinetics. The second research direction investigates rare earth– doped SnO₂, focusing on how Sm³⁺ induced trap states influence electronic structure and sensing performance. Ultra-trace H2 detection at 25 ppb was demonstrated with a calculated LOD of 4.5 ppb. To further enhance humidity tolerance, Sm3+ and Tb3+ co-doping was examined for its effects on defect chemistry and electronic structure. Although co-doping improved gas sensitivity, only modest improvements in humidity tolerance were observed, ultimately identifying Tb-doped SnO2 as the most stable sensing configuration under humid conditions. Tb3+ strengthened metal-oxygen bonding, thereby improving the humidity resilience. Collectively, these studies demonstrate that engineered interfaces, whether through dopant-induced defect modulation or deliberate heterojunction design, play a central role in achieving reliable sensing under real-world conditions. By comparing rare-earth-modified SnO2 with advanced p-type materials, this dissertation establishes a unified framework linking defect chemistry, surface energetics, and interfacial charge transport to improved environmental stability and selectivity in metal-oxide gas sensors.

Available for download on Tuesday, April 13, 2027

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