Semester of Graduation

Summer 2026

Degree

Master of Science in Chemical Engineering (MSChE)

Department

Cain Department of Chemical Engineering

Document Type

Thesis

Abstract

Fossil fuel combustion remains the dominant source of anthropogenic CO₂ emissions, necessitating clean energy carriers compatible with existing infrastructure. Hydrogen is a promising candidate given its gravimetric energy density of 120 MJ/kg, nearly three times that of gasoline and its water-only combustion product, though low volumetric energy density and flammability complicate storage and transport. Formic acid and sodium formate are attractive liquid organic hydrogen carriers due to their low toxicity and 4.38 wt.% hydrogen storage capacity via HCOOH → CO₂ + H₂. Palladium-based nanoparticle catalysts enable on-demand hydrogen generation from formate at ambient conditions, yet Pd's high cost, CO poisoning susceptibility, and poor nanoparticle–support adhesion limit practical deployment. Alloying Pd with earth abundant nickel improves activity and stability through geometric strain effects and d-band center shifts that optimize intermediate binding energies while suppressing CO adsorption. Here we report the first synthesis of bimetallic PdNi nanoparticle catalysts on carboxyl functionalized carbon nanotube (CNT) bucky paper supports via pulsed laser irradiation. Precursor salts are deposited by incipient wetness impregnation with pH-controlled Strong Electrostatic Adsorption and subsequently decomposed by 1064 nm pulsed laser irradiation without stabilizing agents, chemical reductants, or post-synthesis thermal treatment. Electron microscopy confirms uniform nanoparticle distribution, and energy dispersive spectroscopy verifies homogeneous alloy composition across all formulations. In sodium formate dehydrogenation, PdNi 70:30 and PdNi 60:40 achieve H₂ concentrations of 100 and 70 µmol/L, respectively, versus 20 µmol/L for monometallic Pd/C, demonstrating that Ni alloying substantially enhances both activity and Pd utilization. Catalysts sustained hydrogen production for 33 hours and retained activity over four reuse cycles, establishing pulsed laser synthesis as a viable additive-free route to high-performance bimetallic formate dehydrogenation catalysts.

Date

6-26-2026

Committee Chair

McPeak, Kevin M.

LSU Acknowledgement

1

LSU Accessibility Acknowledgment

1

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Available for download on Monday, June 25, 2029

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