Journal
NANO LETTERS
Volume 16, Issue 10, Pages 6644-6649Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.6b03395
Keywords
platinum-based catalyst; nanocage; Pt-Ag alloy; oxygen reduction reaction; density functional theory
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Funding
- Georgia Tech
- DOE-BES (Office of Chemical Sciences) [DE-FG02-05ER15731]
- Graduate Research Fellowship award from National Science Foundation [DGE-1148903]
- Georgia Tech-ORNL Fellowship
- DOE Office of Biological and Environmental Research at Pacific Northwest National Laboratory
- Center for Nanoscale Materials at Argonne National Laboratory
- DOE [DE-AC02-06CH11357]
- National Energy Research Scientific Computing Center (NERSC), a DOE Office of Science User Facility by DOE [DE-AC02-05CH11231]
- UW-Madison Center for High Throughput Computing (CHTC)
- UW-Madison
- Advanced Computing Initiative
- Wisconsin Alumni Research Foundation
- Wisconsin Institutes for Discovery
- National Science Foundation
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Engineering the elemental composition of metal nano crystals offers an effective strategy for the development of catalysts Or electrocatalysts with greatly enhanced activity. Herein, we report the synthesis of Pt-Ag, alloy nanocages with an outer edge length of 18 nm and a wall thickness of about 3 nm. Such nanocages with a composition of Pt19Ag81 could be readily prepared in one step through the galvanic replacement reaction between Ag nanocubes and a Pt(II) precursor. After 10 090 cycles of potential cycling in the range of 0.60-1.0 V as in an accelerated durability test, the composition of the nanocages changed to Pt56Ag44, together with a specific activity of 1.23 mA cm(-2) toward oxygen reduction, which was 3.3 times that of a state-of-the-art commercial Pt/C catalyst (0.37 mA cm(-2)) prior to durability testing. Density functional theory calculations attributed the increased activity to the stabilization of the transition state for breaking the O-O bond in molecular oxygen. Even after 30 000 cycles of potential cycling) the Mass activity of the nanocages only dropped from 0.64 to 0.33 A mg(Pt)(-1), which was still about two times that of the pristine Pt/C catalyst (0.19 A mg(Pt)(-1)).
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