Abstract
Ethanol oxidation reaction (EOR) is a key component of direct ethanol fuel cells (DEFCs). However, due to its slow kinetics, EOR remains a significant challenge, leading to an increasing search for low-cost, efficient, and stable catalysts. Herein, palladium (Pd) nanostructured catalysts supported on titanium dioxide (Pd/TiO<sub>2</sub>) and cerium titanate (Pd/Ce<sub>2</sub>Ti<sub>2</sub>O<sub>7</sub>-TiO<sub>2</sub>) were prepared for EOR. The Pd/Ce<sub>2</sub>Ti<sub>2</sub>O<sub>7</sub>-TiO<sub>2</sub> catalyst exhibits superior electroactivity toward the EOR, demonstrating a high mass activity of 2.70 and 2.63-fold relative to Pd/TiO<sub>2</sub> and Pd/C, respectively. The enhanced behavior was attributed to the bifunctional mechanism, improved electron transport, and downshifted d-band center (ε<sub>d</sub>). Density functional theory (DFT) calculations show a higher density of states for Pd/Ce<sub>2</sub>Ti<sub>2</sub>O<sub>7</sub>-TiO<sub>2</sub>,suggesting higher EOR kinetics than the Pd and Pd/TiO<sub>2</sub>, due to its multiorbital (p-d-f) hybridization. The accelerated durability test (ADT) reveals that the Pd/Ce<sub>2</sub>Ti<sub>2</sub>O<sub>7</sub>-TiO<sub>2</sub> catalyst exhibits satisfactory durability, showing an electrochemically active surface area (ECSA) loss of 18.8% compared with the Pd/C catalyst (33.3% loss) after 1000 cycles. Furthermore, the Pd/Ce<sub>2</sub>Ti<sub>2</sub>O<sub>7</sub>-TiO<sub>2</sub> catalyst exhibited a low detection limit of 12.0 μM toward the nonenzymatic amperometric detection of ethanol. Thus, this study demonstrates the promising use of Ce<sub>2</sub>Ti<sub>2</sub>O<sub>7</sub>-TiO<sub>2</sub> as a support for Pd-based catalysts for EOR in DEFCs and a nonenzymatic amperometric sensor.
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- 2025
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Refiloe Modise,
Patrick V. Mwonga,
Jeseelan Pillay
et al.
(2025).
Synergistic Enhancement of Ethanol Oxidation on Pd/Ce <sub>2</sub> Ti <sub>2</sub> O <sub>7</sub> –TiO <sub>2</sub> via Multiorbital (p–d–f) Interactions.
Inorganic Chemistry
.
https://doi.org/10.1021/acs.inorgchem.5c04103
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- DOI
- 10.1021/acs.inorgchem.5c04103