(304b) Nanoparticle Proximity Controls Selectivity in Benzaldehyde Hydrogenation
AIChE Annual Meeting
2024
2024 AIChE Annual Meeting
Catalysis and Reaction Engineering Division
Catalyst Design, Synthesis, and Characterization VI: Environments Around Active Sites
Tuesday, October 29, 2024 - 12:48pm to 1:06pm
Disentangling the effects of nanoparticle proximity and size on thermal
catalytic performance is challenging with traditional synthetic methods.
Here we adapt a modular raspberry-colloid-templating approach to tune the
average interparticle distance of PdAu alloy nanoparticles, while preserving
all other physicochemical characteristics, including nanoparticle size. By
controlling the metal loading and placement of pre-formed nanoparticles
within a 3D macroporous SiO2 support and using the hydrogenation of
benzaldehyde to benzyl alcohol and toluene as the probe reaction, we report
that increasing the interparticle distance (from 12 to 21 nm) substantially
enhances selectivity towards benzyl alcohol (from 54% to 99%) without
compromising catalytic performance. Combining electron tomography,
kinetic evaluation and simulations, we show that interparticle distance
modulates the local benzyl alcohol concentration profile between active
sites, consequently affecting benzyl alcohol readsorption, which promotes
hydrogenolysis to toluene. Our results illustrate the relevance of proximity
effects as a mesoscale tool to control the adsorption of intermediates and,
hence, catalytic performance.
catalytic performance is challenging with traditional synthetic methods.
Here we adapt a modular raspberry-colloid-templating approach to tune the
average interparticle distance of PdAu alloy nanoparticles, while preserving
all other physicochemical characteristics, including nanoparticle size. By
controlling the metal loading and placement of pre-formed nanoparticles
within a 3D macroporous SiO2 support and using the hydrogenation of
benzaldehyde to benzyl alcohol and toluene as the probe reaction, we report
that increasing the interparticle distance (from 12 to 21 nm) substantially
enhances selectivity towards benzyl alcohol (from 54% to 99%) without
compromising catalytic performance. Combining electron tomography,
kinetic evaluation and simulations, we show that interparticle distance
modulates the local benzyl alcohol concentration profile between active
sites, consequently affecting benzyl alcohol readsorption, which promotes
hydrogenolysis to toluene. Our results illustrate the relevance of proximity
effects as a mesoscale tool to control the adsorption of intermediates and,
hence, catalytic performance.
Disentangling the effects of nanoparticle proximity and size on thermal
catalytic performance is challenging with traditional synthetic methods.
Here we adapt a modular raspberry-colloid-templating approach to tune the
average interparticle distance of PdAu alloy nanoparticles, while preserving
all other physicochemical characteristics, including nanoparticle size. By
controlling the metal loading and placement of pre-formed nanoparticles
within a 3D macroporous SiO2 support and using the hydrogenation of
benzaldehyde to benzyl alcohol and toluene as the probe reaction, we report
that increasing the interparticle distance (from 12 to 21 nm) substantially
enhances selectivity towards benzyl alcohol (from 54% to 99%) without
compromising catalytic performance. Combining electron tomography,
kinetic evaluation and simulations, we show that interparticle distance
modulates the local benzyl alcohol concentration profile between active
sites, consequently affecting benzyl alcohol readsorption, which promotes
hydrogenolysis to toluene. Our results illustrate the relevance of proximity
effects as a mesoscale tool to control the adsorption of intermediates and,
hence, catalytic performance.
catalytic performance is challenging with traditional synthetic methods.
Here we adapt a modular raspberry-colloid-templating approach to tune the
average interparticle distance of PdAu alloy nanoparticles, while preserving
all other physicochemical characteristics, including nanoparticle size. By
controlling the metal loading and placement of pre-formed nanoparticles
within a 3D macroporous SiO2 support and using the hydrogenation of
benzaldehyde to benzyl alcohol and toluene as the probe reaction, we report
that increasing the interparticle distance (from 12 to 21 nm) substantially
enhances selectivity towards benzyl alcohol (from 54% to 99%) without
compromising catalytic performance. Combining electron tomography,
kinetic evaluation and simulations, we show that interparticle distance
modulates the local benzyl alcohol concentration profile between active
sites, consequently affecting benzyl alcohol readsorption, which promotes
hydrogenolysis to toluene. Our results illustrate the relevance of proximity
effects as a mesoscale tool to control the adsorption of intermediates and,
hence, catalytic performance.