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Title: Catalytically active Au-O(OH) x- species stabilized by alkali ions on zeolites and mesoporous oxides

Abstract

Here we report that the addition of alkali ions (sodium or potassium) to gold on KLTL-zeolite and mesoporous MCM-41 silica stabilizes mononuclear gold in Au-O(OH) x-(Na or K) ensembles. This single-site gold species is active for the low-temperature (<200°C) water-gas shift (WGS) reaction. Unexpectedly, gold is thus similar to platinum in creating –O linkages with more than eight alkali ions and establishing an active site on various supports. The intrinsic activity of the single-site gold species is the same on irreducible supports as on reducible ceria, iron oxide, and titania supports, apparently all sharing a common, similarly structured gold active site. This finding paves the way for using earth-abundant supports to disperse and stabilize precious metal atoms with alkali additives for the WGS and potentially other fuel-processing reactions.

Authors:
 [1];  [2];  [1];  [2];  [3];  [4];  [5];  [6];  [2];  [1]
  1. Tufts Univ., Medford, MA (United States). Dept. of Chemical and Biological Engineering
  2. Univ. of Wisconsin, Madison, WI (United States). Dept. of Chemical and Biological Engineering
  3. Louisiana State Univ., Baton Rouge, LA (United States). Dept. of Chemical Engineering
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
  5. Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division
  6. Univ. of Sydney, NSW (Australia). School of Chemical and Biomolecular Engineering
Publication Date:
Research Org.:
Univ. of Wisconsin, Madison, WI (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
Contributing Org.:
EMSL; the Center for Nanoscale Materials at Argonne National Laboratory (ANL); the CNMS at ORNL; and the National Energy Research Scientific Computing Center (NERSC)
OSTI Identifier:
1398777
Grant/Contract Number:  
FG02-05ER15731; FG02-05ER15730; AC02-06CH11357; AC02-05CH11231
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Science
Additional Journal Information:
Journal Volume: 346; Journal Issue: 6216; Journal ID: ISSN 0036-8075
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Yang, Ming, Li, Sha, Wang, Yuan, Herron, Jeffrey A., Xu, Ye, Allard, Lawrence F., Lee, Sungsik, Huang, Jun, Mavrikakis, Manos, and Flytzani-Stephanopoulos, Maria. Catalytically active Au-O(OH)x- species stabilized by alkali ions on zeolites and mesoporous oxides. United States: N. p., 2014. Web. doi:10.1126/science.1260526.
Yang, Ming, Li, Sha, Wang, Yuan, Herron, Jeffrey A., Xu, Ye, Allard, Lawrence F., Lee, Sungsik, Huang, Jun, Mavrikakis, Manos, & Flytzani-Stephanopoulos, Maria. Catalytically active Au-O(OH)x- species stabilized by alkali ions on zeolites and mesoporous oxides. United States. doi:10.1126/science.1260526.
Yang, Ming, Li, Sha, Wang, Yuan, Herron, Jeffrey A., Xu, Ye, Allard, Lawrence F., Lee, Sungsik, Huang, Jun, Mavrikakis, Manos, and Flytzani-Stephanopoulos, Maria. Thu . "Catalytically active Au-O(OH)x- species stabilized by alkali ions on zeolites and mesoporous oxides". United States. doi:10.1126/science.1260526. https://www.osti.gov/servlets/purl/1398777.
@article{osti_1398777,
title = {Catalytically active Au-O(OH)x- species stabilized by alkali ions on zeolites and mesoporous oxides},
author = {Yang, Ming and Li, Sha and Wang, Yuan and Herron, Jeffrey A. and Xu, Ye and Allard, Lawrence F. and Lee, Sungsik and Huang, Jun and Mavrikakis, Manos and Flytzani-Stephanopoulos, Maria},
abstractNote = {Here we report that the addition of alkali ions (sodium or potassium) to gold on KLTL-zeolite and mesoporous MCM-41 silica stabilizes mononuclear gold in Au-O(OH)x-(Na or K) ensembles. This single-site gold species is active for the low-temperature (<200°C) water-gas shift (WGS) reaction. Unexpectedly, gold is thus similar to platinum in creating –O linkages with more than eight alkali ions and establishing an active site on various supports. The intrinsic activity of the single-site gold species is the same on irreducible supports as on reducible ceria, iron oxide, and titania supports, apparently all sharing a common, similarly structured gold active site. This finding paves the way for using earth-abundant supports to disperse and stabilize precious metal atoms with alkali additives for the WGS and potentially other fuel-processing reactions.},
doi = {10.1126/science.1260526},
journal = {Science},
number = 6216,
volume = 346,
place = {United States},
year = {Thu Nov 27 00:00:00 EST 2014},
month = {Thu Nov 27 00:00:00 EST 2014}
}

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Cited by: 137 works
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Works referenced in this record:

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