Ozone-Activated Nanoporous Gold: A Stable and Storable Material for Catalytic Oxidation

Personick, Michelle L.; Zugic, Branko; Biener, Monika M.; Biener, Juergen; Madix, Robert J.; Friend, Cynthia M.

doi:10.1021/acscatal.5b00330

Ozone-Activated Nanoporous Gold: A Stable and Storable Material for Catalytic Oxidation

Journal Article · Thu May 28 00:00:00 EDT 2015 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.5b00330· OSTI ID:1413171

Personick, Michelle L. ^[1]; Zugic, Branko ^[1]; Biener, Monika M. ^[2]; Biener, Juergen ^[2]; Madix, Robert J. ^[1]; Friend, Cynthia M. ^[1]

Harvard Univ., Cambridge, MA (United States)
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

We report a new method for facile and reproducible activation of nanoporous gold (npAu) materials of different forms for the catalytic selective partial oxidation of alcohols under ambient pressure, steady flow conditions. This method, based on the surface cleaning of npAu ingots with ozone to remove carbon documented in ultrahigh vacuum conditions, produces active npAu catalysts from ingots, foils, and shells by flowing an ozone/dioxygen mixture over the catalyst at 150 °C, followed by a temperature ramp from 50 to 150 °C in a flowing stream of 10% methanol and 20% oxygen. With this treatment, all three materials (ingots, foils, and shells) can be reproducibly activated, despite potential carbonaceous poisons resulting from their synthesis, and are highly active for the selective oxidation of primary alcohols over prolonged periods of time. The npAu materials activated in this manner exhibit catalytic behavior substantially different from those activated under different conditions previously reported. Once activated in this manner, they can be stored and easily reactivated by flow of reactant gases at 150 °C for a few hours. They possess improved selectivity for the coupling of higher alcohols, such as 1-butanol, and are not active for carbon monoxide oxidation. As a result, this ozone-treated npAu is a functionally new catalytic material.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC52-07NA27344; SC0012573

OSTI ID:: 1413171

Report Number(s):: LLNL-JRNL--737631

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 7 Vol. 5; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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36 MATERIALS SCIENCE
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
activation
energy-efficient catalysis
nanoporous gold
ozone
selective oxidation

Ozone-Activated Nanoporous Gold: A Stable and Storable Material for Catalytic Oxidation

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