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

Abstract

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-treatedmore » npAu is a functionally new catalytic material.« less

Authors:
 [1];  [1];  [2];  [2];  [1];  [1]
  1. Harvard Univ., Cambridge, MA (United States)
  2. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Energy Frontier Research Centers (EFRC) (United States). Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1413171
Report Number(s):
LLNL-JRNL-737631
Journal ID: ISSN 2155-5435
Grant/Contract Number:  
AC52-07NA27344; SC0012573
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 5; Journal Issue: 7; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; activation; energy-efficient catalysis; nanoporous gold; ozone; selective oxidation

Citation Formats

Personick, Michelle L., Zugic, Branko, Biener, Monika M., Biener, Juergen, Madix, Robert J., and Friend, Cynthia M. Ozone-Activated Nanoporous Gold: A Stable and Storable Material for Catalytic Oxidation. United States: N. p., 2015. Web. doi:10.1021/acscatal.5b00330.
Personick, Michelle L., Zugic, Branko, Biener, Monika M., Biener, Juergen, Madix, Robert J., & Friend, Cynthia M. Ozone-Activated Nanoporous Gold: A Stable and Storable Material for Catalytic Oxidation. United States. doi:10.1021/acscatal.5b00330.
Personick, Michelle L., Zugic, Branko, Biener, Monika M., Biener, Juergen, Madix, Robert J., and Friend, Cynthia M. Thu . "Ozone-Activated Nanoporous Gold: A Stable and Storable Material for Catalytic Oxidation". United States. doi:10.1021/acscatal.5b00330. https://www.osti.gov/servlets/purl/1413171.
@article{osti_1413171,
title = {Ozone-Activated Nanoporous Gold: A Stable and Storable Material for Catalytic Oxidation},
author = {Personick, Michelle L. and Zugic, Branko and Biener, Monika M. and Biener, Juergen and Madix, Robert J. and Friend, Cynthia M.},
abstractNote = {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.},
doi = {10.1021/acscatal.5b00330},
journal = {ACS Catalysis},
issn = {2155-5435},
number = 7,
volume = 5,
place = {United States},
year = {2015},
month = {5}
}

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Cited by: 27 works
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Works referencing / citing this record:

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  • Barroo, Cédric; Moors, Matthieu; Visart de Bocarmé, Thierry
  • Catalysis Science & Technology, Vol. 7, Issue 22
  • DOI: 10.1039/c7cy00994a

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  • Barroo, Cédric; Akey, Austin J.; Bell, David C.
  • Applied Sciences, Vol. 9, Issue 13
  • DOI: 10.3390/app9132721

Aerobic Methanol Oxidation over Unsupported Nanoporous Gold: The Influence of an Added Base
journal, May 2019

  • Lackmann, Anastasia; Mahr, Christoph; Rosenauer, Andreas
  • Catalysts, Vol. 9, Issue 5
  • DOI: 10.3390/catal9050416