TY - JOUR
T1 - Atomic Layer Deposition Overcoating Improves Catalyst Selectivity and Longevity in Propane Dehydrogenation
AU - Lu, Zheng
AU - Tracy, Ryon W.
AU - Abrams, M. Leigh
AU - Nicholls, Natalie L.
AU - Barger, Paul T.
AU - Li, Tao
AU - Stair, Peter C.
AU - Dameron, Arrelaine A.
AU - Nicholas, Christopher P.
AU - Marshall, Christopher L.
N1 - Funding Information:
This work was supported by the U.S. Department of Energy’s Office of Energy Efficiency and Renewable Energy (EERE) under the Advanced Manufacturing Office Next Generation R&D Projects award number DE-EE0008328. The views expressed herein do not necessarily represent the views of the U.S. Department of Energy or the United States Government. Additional support was received in-kind from Honeywell UOP and Forge Nano.
PY - 2020/12/4
Y1 - 2020/12/4
N2 - Propylene, a precursor for commodity chemicals and plastics, is produced by propane dehydrogenation (PDH). An increase in PDH yield via added catalyst activity, lifetime, or selectivity represents significant energy and economic savings. Using Pt dispersed on Al2O3 extrudate supports as a commercially relevant model system, we demonstrate that atomic layer deposition (ALD) metal oxide overcoats, used to tailor metal-active sites, can increase PDH yield and selectivity. We investigate the interplay of Pt loading, ALD overcoat thickness, and Al2O3 support surface area on PDH activity, selectivity, and catalyst stability to show that applying a 6-8 Å thick layer of Al2O3 on low-surface area Al2O3 supports of ∼90 m2/g surface area yields the optimal combination of stability and activity, while increasing propylene selectivity from 91 to 96%. Increased stability upon steaming deactivation occurs because the Al2O3 overcoat prevents the Pt nanoparticles from sintering. We speculate that the ALD overcoat selectively binds to the undercoordinated sites on the Pt nanoparticles, while leaving the more selective terrace sites available for dehydrogenation.
AB - Propylene, a precursor for commodity chemicals and plastics, is produced by propane dehydrogenation (PDH). An increase in PDH yield via added catalyst activity, lifetime, or selectivity represents significant energy and economic savings. Using Pt dispersed on Al2O3 extrudate supports as a commercially relevant model system, we demonstrate that atomic layer deposition (ALD) metal oxide overcoats, used to tailor metal-active sites, can increase PDH yield and selectivity. We investigate the interplay of Pt loading, ALD overcoat thickness, and Al2O3 support surface area on PDH activity, selectivity, and catalyst stability to show that applying a 6-8 Å thick layer of Al2O3 on low-surface area Al2O3 supports of ∼90 m2/g surface area yields the optimal combination of stability and activity, while increasing propylene selectivity from 91 to 96%. Increased stability upon steaming deactivation occurs because the Al2O3 overcoat prevents the Pt nanoparticles from sintering. We speculate that the ALD overcoat selectively binds to the undercoordinated sites on the Pt nanoparticles, while leaving the more selective terrace sites available for dehydrogenation.
KW - atomic layer deposition
KW - extruded platinum catalyst
KW - overcoating effects
KW - propane dehydrogenation
UR - http://www.scopus.com/inward/record.url?scp=85096622886&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85096622886&partnerID=8YFLogxK
U2 - 10.1021/acscatal.0c03391
DO - 10.1021/acscatal.0c03391
M3 - Article
AN - SCOPUS:85096622886
VL - 10
SP - 13957
EP - 13967
JO - ACS Catalysis
JF - ACS Catalysis
SN - 2155-5435
IS - 23
ER -