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

DOI: 10.1039/D4EY00044G

Authors: Khaled Mohammed (University of Southampton) , Reza Vakili (Queen's University Belfast; Imperial College London) , Donato Decarolis (UK Catalysis Hub, Research Complex at Harwell; Diamond Light Source) , Shaojun Xu (UK Catalysis Hub, Research Complex at Harwell; The University of Manchester) , Luke L. Keenan (Diamond Light Source) , Apostolos Kordatos (University of Southampton) , Nikolay Zhelev (University of Southampton) , Chris K. Skylaris (University of Southampton) , Marina Carravetta (University of Southampton) , Emma K. Gibson (UK Catalysis Hub, Research Complex at Harwell; University of Glasgow) , Haresh Manyar (Queen's University Belfast) , Alexandre Goguet (Queen's University Belfast) , Peter P. Wells (University of Southampton; UK Catalysis Hub, Research Complex at Harwell; Diamond Light Source)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Ees Catalysis

State: Published (Approved)
Published: April 2024
Diamond Proposal Number(s): 28666 , 34632

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 the 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 validated against PdNx samples made via known synthesis methods. . Above 240 ℃, 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.

Subject Areas: Chemistry, Materials, Environment


Instruments: B18-Core EXAFS , I20-EDE-Energy Dispersive EXAFS (EDE)

Added On: 24/04/2024 14:31

Documents:
d4ey00044g.pdf

Discipline Tags:

Earth Sciences & Environment Climate Change Physical Chemistry Catalysis Chemistry Materials Science Nanoscience/Nanotechnology

Technical Tags:

Spectroscopy X-ray Absorption Spectroscopy (XAS) Energy Dispersive EXAFS (EDE)