Controlling hot electron flux and catalytic selectivity with nanoscale metal-oxide interfaces

Si Woo Lee, Jong Min Kim, Woonghyeon Park, Hyosun Lee, Gyu Rac Lee, Yousung Jung (), Yeon Sik Jung () and Jeong Young Park ()
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Si Woo Lee: Institute for Basic Science (IBS)
Jong Min Kim: Korea Advanced Institute of Science and Technology (KAIST)
Woonghyeon Park: Korea Advanced Institute of Science and Technology (KAIST)
Hyosun Lee: Institute for Basic Science (IBS)
Gyu Rac Lee: Korea Advanced Institute of Science and Technology (KAIST)
Yousung Jung: Korea Advanced Institute of Science and Technology (KAIST)
Yeon Sik Jung: Korea Advanced Institute of Science and Technology (KAIST)
Jeong Young Park: Institute for Basic Science (IBS)

Nature Communications, 2021, vol. 12, issue 1, 1-11

Abstract: Abstract Interaction between metal and oxides is an important molecular-level factor that influences the selectivity of a desirable reaction. Therefore, designing a heterogeneous catalyst where metal-oxide interfaces are well-formed is important for understanding selectivity and surface electronic excitation at the interface. Here, we utilized a nanoscale catalytic Schottky diode from Pt nanowire arrays on TiO2 that forms a nanoscale Pt-TiO2 interface to determine the influence of the metal-oxide interface on catalytic selectivity, thereby affecting hot electron excitation; this demonstrated the real-time detection of hot electron flow generated under an exothermic methanol oxidation reaction. The selectivity to methyl formate and hot electron generation was obtained on nanoscale Pt nanowires/TiO2, which exhibited ~2 times higher partial oxidation selectivity and ~3 times higher chemicurrent yield compared to a diode based on Pt film. By utilizing various Pt/TiO2 nanostructures, we found that the ratio of interface to metal sites significantly affects the selectivity, thereby enhancing chemicurrent yield in methanol oxidation. Density function theory (DFT) calculations show that formation of the Pt-TiO2 interface showed that selectivity to methyl formate formation was much larger in Pt nanowire arrays than in Pt films because of the different reaction mechanism.

Date: 2021
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DOI: 10.1038/s41467-020-20293-y

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