Structural selectivity of supported Pd nanoparticles: selective ethanol ammoxidation to acetonitrile

Khaled Mohammed, Reza Vakili, Donato Decarolis, Shaojun Xu, Luke Keenan, Apostolos Kordatos, Nikolay Zhelev, Chris K. Skylaris, Marina Carravetta, Emma K. Gibson, Haresh Manyar, Alexandre Goguet, Peter P. Wells*

*Corresponding author for this work

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Abstract

The need to achieve net zero requires decarbonisation across all areas of our industrialised society, including the production of chemicals. One example is the production of acetonitrile, which currently relies on fossil carbon. Recently, supported Pd nanoparticles have been shown to promote the selective transformation of bio-derived ethanol to acetonitrile. Elsewhere, current research has demonstrated the importance of interstitial structures of Pd in promoting specific transformations. In this study, we demonstrate through a spatially resolved operando energy-dispersive-EXAFS (EDE) technique that selectivity to acetonitrile (up to 99%) is concurrent with the formation of a PdNx phase. This was evidenced from the features observed in the X-ray absorption near edge structure that were validated against PdNx samples made via known synthesis methods. Above 240 °C, the Pd nanoparticles became progressively oxidised which led to the production of unwanted byproducts, primarily CO2. The spatially resolved analysis indicated that the Pd speciation was homogeneous across the catalyst profile throughout the series of studies performed. This work resolved the structural selectivity of Pd nanoparticles that directs ethanol ammoxidation towards acetonitrile, and provides important information on the performance descriptors required to advance this technology.
Original languageEnglish
JournalEES Catalysis
Early online date18 Apr 2024
DOIs
Publication statusEarly online date - 18 Apr 2024

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