期刊
NANO LETTERS
卷 16, 期 10, 页码 6644-6649出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.6b03395
关键词
platinum-based catalyst; nanocage; Pt-Ag alloy; oxygen reduction reaction; density functional theory
类别
资金
- 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
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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