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Title: Dynamic restructuring drives catalytic activity on nanoporous gold–silver alloy catalysts

Abstract

Bimetallic, nanostructured materials hold promise for improving catalyst activity and selectivity, yet little is known about the dynamic compositional and structural changes that these systems undergo during pretreatment that leads to efficient catalyst function. Here we use ozone-activated silver–gold alloys in the form of nanoporous gold as a case study to demonstrate the dynamic behaviour of bimetallic systems during activation to produce a functioning catalyst. We show that it is these dynamic changes that give rise to the observed catalytic activity. Advanced in situ electron microscopy and X-ray photoelectron spectroscopy are used to demonstrate that major restructuring and compositional changes occur along the path to catalytic function for selective alcohol oxidation. Transient kinetic measurements correlate the restructuring to three types of oxygen on the surface. The direct influence of changes in surface silver concentration and restructuring at the nanoscale on oxidation activity is demonstrated. Finally, our results demonstrate that characterization of these dynamic changes is necessary to unlock the full potential of bimetallic catalytic materials.

Authors:
; ; ; ; ; ORCiD logo; ; ; ;
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States); Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1438304
Alternate Identifier(s):
OSTI ID: 1414360; OSTI ID: 1472028
Report Number(s):
BNL-205660-2018-JAAM; LLNL-JRNL-739604
Journal ID: ISSN 1476-1122; TRN: US1800690
Grant/Contract Number:  
SC0012704; SC0012573; AC52-07NA27344; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Nature Materials
Additional Journal Information:
Journal Volume: 16; Journal Issue: 5; Journal ID: ISSN 1476-1122
Publisher:
Springer Nature - Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 77 NANOSCIENCE AND NANOTECHNOLOGY; Bimetallic catalyst; catalyst activity; selectivity; nanoporous gold; environmental transmission electron microscopy; X-ray photoelectron spectroscopy; alcohol oxidation

Citation Formats

Zugic, Branko, Wang, Lucun, Heine, Christian, Zakharov, Dmitri N., Lechner, Barbara A. J., Stach, Eric A., Biener, Juergen, Salmeron, Miquel, Madix, Robert J., and Friend, Cynthia M. Dynamic restructuring drives catalytic activity on nanoporous gold–silver alloy catalysts. United States: N. p., 2016. Web. doi:10.1038/nmat4824.
Zugic, Branko, Wang, Lucun, Heine, Christian, Zakharov, Dmitri N., Lechner, Barbara A. J., Stach, Eric A., Biener, Juergen, Salmeron, Miquel, Madix, Robert J., & Friend, Cynthia M. Dynamic restructuring drives catalytic activity on nanoporous gold–silver alloy catalysts. United States. doi:10.1038/nmat4824.
Zugic, Branko, Wang, Lucun, Heine, Christian, Zakharov, Dmitri N., Lechner, Barbara A. J., Stach, Eric A., Biener, Juergen, Salmeron, Miquel, Madix, Robert J., and Friend, Cynthia M. Mon . "Dynamic restructuring drives catalytic activity on nanoporous gold–silver alloy catalysts". United States. doi:10.1038/nmat4824. https://www.osti.gov/servlets/purl/1438304.
@article{osti_1438304,
title = {Dynamic restructuring drives catalytic activity on nanoporous gold–silver alloy catalysts},
author = {Zugic, Branko and Wang, Lucun and Heine, Christian and Zakharov, Dmitri N. and Lechner, Barbara A. J. and Stach, Eric A. and Biener, Juergen and Salmeron, Miquel and Madix, Robert J. and Friend, Cynthia M.},
abstractNote = {Bimetallic, nanostructured materials hold promise for improving catalyst activity and selectivity, yet little is known about the dynamic compositional and structural changes that these systems undergo during pretreatment that leads to efficient catalyst function. Here we use ozone-activated silver–gold alloys in the form of nanoporous gold as a case study to demonstrate the dynamic behaviour of bimetallic systems during activation to produce a functioning catalyst. We show that it is these dynamic changes that give rise to the observed catalytic activity. Advanced in situ electron microscopy and X-ray photoelectron spectroscopy are used to demonstrate that major restructuring and compositional changes occur along the path to catalytic function for selective alcohol oxidation. Transient kinetic measurements correlate the restructuring to three types of oxygen on the surface. The direct influence of changes in surface silver concentration and restructuring at the nanoscale on oxidation activity is demonstrated. Finally, our results demonstrate that characterization of these dynamic changes is necessary to unlock the full potential of bimetallic catalytic materials.},
doi = {10.1038/nmat4824},
journal = {Nature Materials},
number = 5,
volume = 16,
place = {United States},
year = {2016},
month = {12}
}

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Works referenced in this record:

The Active Site of Methanol Synthesis over Cu/ZnO/Al2O3 Industrial Catalysts
journal, April 2012


Selectivity Control in Gold-Mediated Esterification of Methanol
journal, May 2009

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