Abstract
Improving the use of platinum in propane dehydrogenation catalysts is a crucial aspect to increasing the efficiency and sustainability of propylene production. A known and practiced strategy involves incorporating more abundant metals in supported platinum catalysts, increasing its activity and stability while decreasing the overall loading. Here, using colloidal techniques to control the size and composition of the active phase, we show that Pt/Cu alloy nanoparticles supported on alumina (Pt/Cu/Al2O3) displayed elevated rates for propane dehydrogenation at low temperature compared to a monometallic Pt/Al2O3 catalyst. We demonstrate that the enhanced catalytic activity is correlated with a higher surface Cu content and formation of a Pt-rich core and Cu-rich shell that isolates Pt sites and increases their intrinsic activity. However, rates declined on stream because of dynamic metal diffusion processes that led to a more uniform alloy structure. This transformation was only partially inhibited by adding excess hydrogen to the feed stream. Instead, cobalt was introduced to provide trimetallic Pt/Cu/Co catalysts with stabilized surface structure and stable activity and higher rates than the original Pt/Cu system. The structure-activity relationship insights in this work offer improved knowledge of propane dehydrogenation catalyst development featuring reduced Pt loadings and notable thermal stability for propylene production.
| Original language | English |
|---|---|
| Pages (from-to) | 30966-30975 |
| Number of pages | 10 |
| Journal | Journal of the American Chemical Society |
| Volume | 146 |
| Issue number | 45 |
| DOIs | |
| State | Published - Nov 13 2024 |
Funding
This research was mainly supported by funding from the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science Program to the SUNCAT Center for Interface Science and Catalysis. Additional support was provided by the American Chemical Society, Petroleum Research Fund, New Directions Award. Part of this work was performed at the Stanford Nanoshared Facilities (SNSF), supported by the National Science Foundation under Award ECCS-2026822. Marco Gigantino is acknowledged for help with TGA data collection. Use of the Microscopy Instrumentation at the Center for Nanophase Materials Science, Oak Ridge National Laboratory was supported by the U.S. Department of Energy, Office of Science and managed by UT-Battelle. This research used resources of the Stanford Synchrotron Radiation Lightsource. Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract DE-AC02-76SF00515. Co-ACCESS, part of the SUNCAT Center for Interface Science and Catalysis, is supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Chemical Sciences, Geosciences and Biosciences Division. Special thanks to Basic Energy Science Program at PNNL for access to perform some of the CO-DRIFTS measurements.
| Funders | Funder number |
|---|---|
| Basic Energy Sciences | |
| American Chemical Society Petroleum Research Fund | |
| U.S. Department of Energy | |
| Catalysis Science Program | |
| Office of Science | |
| Chemical Sciences, Geosciences, and Biosciences Division | |
| National Science Foundation | ECCS-2026822 |
| National Science Foundation | |
| UT-Battelle | DE-AC02-76SF00515 |
| UT-Battelle |