Walton, Amber [Univ. of Minnesota, Minneapolis, MN (United States)] (ORCID:0000000306001613)

DOE OSTI2024

Alumina–Titania Nanolaminate Condensers for Hot Programmable Catalysis

Nanolaminates composed of thin alternating layers of Al2O 3 and TiO 2 (ATO) were engineered by using atomic layer deposition as the dielectric material for a Pt-on-carbon catalytic condenser. Investigation assessed synthesis parameters including the deposition temperature, Al 2 O 3 and TiO 2 layer thicknesses, total number of layers, and a capping Al 2 O 3 layer on the maximum charge accumulation in the Pt catalyst. The highest capacitance ATO configuration demonstrated a specific capacitance of ∼1200 nF/cm 2 with working voltages of ±5 V, enabling the storage of 4 × 10 13 electrons or holes per cm 2 at room temperature. The ATO devices exhibited enhanced capacitance at elevated temperatures of up to 400 °C, suggesting the suitability of these materials for high-temperature applications. Adsorption of carbon monoxide on the Pt/C-ATO device characterized by grazing incidence infrared spectroscopy showed changes in the surface binding energy of 13.1 ± 0.8 kJ/mol for an applied external voltage bias of ±1 V.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Fabrication of Large-Area Metal-on-Carbon Catalytic Condensers for Programmable Catalysis

Catalytic condensers stabilize charge on either side of a high-k dielectric film to modulate the electronic states of a catalytic layer for the electronic control of surface reactions. Here, carbon sputtering provided for fast, large-scale fabrication of metal–carbon catalytic condensers required for industrial application. Carbon films were sputtered on HfO 2 dielectric/p-type Si with different thicknesses (1, 3, 6, and 10 nm), and the enhancement of conductance and capacitance of carbon films was observed upon increasing the carbon thickness following thermal treatment at 400 °C. After Pt deposition on the carbon films, the Pt catalytic condenser exhibited a high capacitance of ∼210 nF/cm 2 that was maintained at a frequency ∼1000 Hz, satisfying the requirement for a dynamic catalyst to implement catalytic resonance. Temperature-programmed desorption of carbon monoxide yielded CO desorption peaks that shifted in temperature with the varying potential applied to the condenser (−6 or +6 V), indicating a shift in the binding energy of carbon monoxide on the Pt condenser surface. A substantial increase in capacitance (∼2000 nF/cm 2 ) of the Pt-on-carbon devices was observed at elevated temperatures of 400 °C that can modulate ∼10% of charge per metal atom when 10 V potential was applied. A large catalytic condenser of 42 cm 2 area Pt/C/HfO 2 /Si exhibited a high capacitance of 9393 nF with a low leakage current/capacitive current ratio (<0.1), demonstrating the practicality and versatility of the facile, large-scale fabrication method for metal–carbon catalytic condensers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗