Abstract
High-temperature operations present a substantial challenge for developing industrial-capable precious metal catalysts (e.g. Pt/alumina), where the scarce metal atoms easily become wasted as sintered nanoparticles. Using fully dispersed precious metal atoms to deliver the catalysis remains an elusive goal. On a widely used La-stabilized alumina support, we find that the atomically dispersed Pt1(II)-Ox- species, rather than the much more visible large metal particles, are the actual catalytic sites for the CO and C3H6 oxidation reactions. Unfortunately, the La dopants in alumina support will not hinder the sintering of the active Pt1(II)-Ox- species. As a natural next step, the Ba-Ox- species were introduced to specifically stabilize the single-atom Pt on the La-stabilized alumina support. By implementing this improved formulation, the atomically dispersed Pt on alumina retains the original full dispersion even after 650 °C hydrothermal aging. Intriguingly, with or without the barium additives and/or sintered platinum particles in the catalysts, the intrinsic activity per Pt atom stays intact. Along with other experimental evidence, this leads to the finding that the single-atom Pt is the true catalytic site for the oxidation of CO and C3H6 in the widely-used Pt/La-Al2O3 material system. This work provides a new perspective for efficient precious metal utilization under demanding catalytic conditions.
Original language | English |
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Pages (from-to) | 327-339 |
Number of pages | 13 |
Journal | Applied Catalysis B: Environmental |
Volume | 244 |
DOIs | |
State | Published - May 5 2019 |
Funding
The work from Tianjin Univ. was supported by the National Key Research and Development Program ( 2017YFC0211002 ), the Science and Technology Program of Tianjin ( 16YFZCSF00290 ), and the grant from GM Global R&D . Microscopy work at ORNL was supported by a Strategic Partnership Project funded by GM Global R&D, and in part by the U.S. Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Office, Propulsion Materials Program. This research used resources of the Advanced Photon Source, a US-DOE Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. The paper is dedicated to celebrating Tom Johnson’ retirement after 40 years’ research work at General Motors Global R&D.
Funders | Funder number |
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DOE Office of Science | |
GM Global R&D | |
Science and Technology Program of Tianjin | 16YFZCSF00290 |
Tianjin Univ. | |
U.S. Department of Energy | |
Office of Energy Efficiency and Renewable Energy | |
Argonne National Laboratory | |
National Basic Research Program of China (973 Program) | 2017YFC0211002 |
Keywords
- Alumina
- Emissions purification
- High-temperature stability
- Platinum
- Single-atom catalyst