Journal
CHEMISTRY OF MATERIALS
Volume 23, Issue 6, Pages 1570-1577Publisher
AMER CHEMICAL SOC
DOI: 10.1021/cm1034134
Keywords
electrocatalyst; nanoleaves; Pd-Fe; oxygen reduction; solution phase synthesis; alkaline electrolyte
Funding
- U.S. National Science Foundation [CBET-1032547]
- American Chemical Society
- Office of Basic Energy Sciences, U.S. Department of Energy
- Directorate For Engineering
- Div Of Chem, Bioeng, Env, & Transp Sys [1032547] Funding Source: National Science Foundation
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Novel PdFe-nanoleaves (NLs) have been prepared through a wet chemistry-based solution phase reduction synthesis route. High-resolution transmission electron microscopy (HR-TEM) and scanning transmission electron microscopy (S/TEM) coupled with high-spatial-resolution compositional analysis clearly show that this newly developed structure is assembled from Pd-rich nanowires (Pd-NWs) surrounded by Fe-rich sheets. The Pd-NWs have diameters in the range of 1.8-2.3 nm and large electrochemical surface areas of > 50 m(2)/g. Their length (30-100 nm) and morphology can be tuned by altering the nanostructure synthesis conditions and the Fe amount in the NLs. With increasing Fe content, thinner and longer sheet-enveloped nanowires can be prepared. The side surfaces of Pd-NWs observed by HR-TEM are predominantly Pd(111) facets, while the tips and ends are Pd(110) and Pd(100) facets. By etching away the enveloping Fe-rich sheets using an organic acid, the Pd-rich NWs are exposed on the surfaces of the nanoleaves, and they demonstrate high reactivity toward electrocatalytic reduction of oxygen in a 0.1 M NaOH electrolyte, i.e., a factor of 3.0 increase in the specific activity and a factor of 2.7 increase in the mass activity, compared to a commercial Pt/C catalyst (at 0 V vs. Hg/HgO). The electrocatalytic activity enhancement can be attributed to the unique nanoleave structure, which provides more Pd(111) facets, a large surface area, and more resistance to Pd oxide formation.
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