Size and composition control of specialty nanocatalysts for sustainability: Fuel cell cathode material and production of sustainable aviation fuel

Sustainable energy technologies are required to reduce greenhouse gas emissions and fulfill growing energy demands. The transition from conventional fossil fuels to renewable-generated energy requires scientific and technical breakthroughs that deliver favorable energy- and cost-efficiency. Noble metal-based catalysts applied to sustainable energy technologies are catalytically reactive but less economical than low-platinum group metal (PGM) and PGM-free nanomaterials. This thesis focuses on (1) platinum-based binary intermetallic nanoparticles for proton exchange membrane fuel cells (PEMFCs) and (2) molybdenum carbide nanocatalysts for the production of sustainable aviation fuel (SAF). Platinum-cobalt (PtCo) intermetallic nanoparticles have been proven to be good substitutions to reduce the amount of precious metal required in PEMFCs. The near-term challenge is to develop a facile and scalable production of PtCo nanoparticles with controlled size and composition to satisfy the needs of heavy-duty PEMFCs. Similarly, molybdenum carbide nanoparticles are reported as promising hydrodeoxygenation (HDO) catalysts to replace platinum and palladium in producing SAF. However, their reported performance is mainly based on pure-phase model compounds such as oleic acid instead of real biofuels. An in-depth investigation of the effects of structural and compositional factors of molybdenum carbides on catalytic properties in real biocrude oils is required. Thus, this thesis is divided into two parts: the first part reports facile synthetic approaches of dense, sub-5 nm Pt-based intermetallic nanoparticles using a dual-ligand metal organic framework as atomically dispersed precursors. Sacrificial metal (zinc) in the precursors were found to contribute to the size control of Pt-based nanoparticles by creating vacancies and facilitating atomic diffusion. The second part of the thesis showcases the excellent HDO activity (~100% deoxygenation efficiency) of supported molybdenum carbide nanocatalysts in food-waste-derived biocrude oils, which were further converted to SAF candidate via distillation. Effects of several key structural and compositional factors, i.e., particle size, Fe loading, and surface oxidation on HDO activity, were also investigated.

Name thesis:degree_name

Ph.D.

Level thesis:degree_level

Dissertation

Discipline thesis:degree_discipline

Chemical Engineering

Grantor

University of Illinois at Urbana-Champaign

Year dc:date

2024

Author dc:creator

• Yu, Siying

Contributors dc:contributor

• Rao, Christopher V.
• Su, Xiao
• Yang, Hong
• Zhang, Yuanhui
• Peters, Baron G.

• Platinum-based Intermetallic Nanoparticles
• Molybdenum Carbide Nanocatalysts
• Sustainable Aviation Fuel

Statement dc:rights

• Copyright 2024 Siying Yu

Language dc:language

en, eng

Handle dc:identifier

https://hdl.handle.net/2142/127470

OAI record oai:identifier

https://www.ideals.illinois.edu/oai-pmh?verb=GetRecord&metadataPrefix=etdms&identifier=oai%3Awww.ideals.illinois.edu%3A2142%2F127470