Atomic Layer Deposition Overcoating Improves Catalyst Selectivity and Longevity in Propane Dehydrogenation

Lu, Zheng; Tracy, Ryon W.; Abrams, M. Leigh; Nicholls, Natalie L.; Barger, Paul T.; Li, Tao; Stair, Peter C.; Dameron, Arrelaine A.; Nicholas, Christopher P.; Marshall, Christopher L.

doi:10.1021/acscatal.0c03391

Atomic Layer Deposition Overcoating Improves Catalyst Selectivity and Longevity in Propane Dehydrogenation

Journal Article · Sun Nov 15 23:00:00 EST 2020 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.0c03391· OSTI ID:1783220

Lu, Zheng ^[1]; Tracy, Ryon W. ^[2]; Abrams, M. Leigh ^[3]; Nicholls, Natalie L. ^[3]; Barger, Paul T. ^[3]; ^[4]; ^[5]; Dameron, Arrelaine A. ^[2]; ^[3]; ^[1]

Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
Forge Nano Inc., Thornton, CO (United States)
Honeywell UOP, Des Plaines, IL (United States). Exploratory Materials and Catalysis Research
Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division; Northern Illinois Univ., DeKalb, IL (United States). Dept. of Chemistry
Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division; Northwestern University, Evanston,(United States). Dept. of Chemistry

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 A thick layer of Al₂O₃ on low-surface area Al₂O₃ supports of similar to 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.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1783220

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 23 Vol. 10; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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