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

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.

doi:10.1038/nmat4824

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

Journal Article · Sun Dec 18 23:00:00 EST 2016 · Nature Materials

DOI:https://doi.org/10.1038/nmat4824· OSTI ID:1414360

Zugic, Branko; Wang, Lucun; Heine, Christian; Zakharov, Dmitri N.; Lechner, Barbara A. J.; ; Biener, Juergen; Salmeron, Miquel; Madix, Robert J.; Friend, Cynthia M.

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.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

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

Grant/Contract Number:: SC0012704; SC0012573; AC52-07NA27344; AC02-05CH11231

OSTI ID:: 1414360

Alternate ID(s):: OSTI ID: 1438304
OSTI ID: 1388711
OSTI ID: 1472028

Report Number(s):: BNL--205660-2018-JAAM; LLNL-JRNL--739604

Journal Information:: Nature Materials, Journal Name: Nature Materials Journal Issue: 5 Vol. 16; ISSN 1476-1122

Publisher:: Springer Nature - Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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