Direct, Soft Chemical Route to Mesoporous Metallic Lead Ruthenium Pyrochlore and Investigation of its Electrochemical Properties

被引:19
作者
Oh, Si Hyoung [1 ,2 ]
Adams, Brian D. [1 ]
Lee, Boeun [2 ]
Nazar, Linda F. [1 ]
机构
[1] Univ Waterloo, Dept Chem, Waterloo, ON N2L 3G1, Canada
[2] Korea Inst Sci & Technol, Seoul, South Korea
关键词
NONAQUEOUS LI-O-2 BATTERIES; LITHIUM-OXYGEN BATTERIES; OXIDE PYROCHLORES; MESOSTRUCTURED MATERIALS; FUEL-CELLS; TIN OXIDE; REDUCTION; ELECTRODE; ELECTROCATALYSIS; PB2RU2O6.5;
D O I
10.1021/cm5034904
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Mesoporous, nanocrystalline metallic lead ruthenium oxide (a pyrochlore) was syntheSized through the formation of a mesostructured cohydroxide network via liquid crystal templating, and subsequent soft chemical oxidation that Crystallizes the oxide at low temperature. The stable S+I- interaction chemistry responsible for the templating methodology is elucidated. The formation of a disordered mesopotous structure with a pore volume of 0.18 cm(3)/g and walls comprised of nanocrystallites was confirmed by X-ray diffraction and conductivity, N-2 isotherm measurements, and TEM observations. The resistivity of mesopotous oxide at room temperature was 0:046 Omega.cm, only 2 orders of magnitude less than the single crystal; value, and one of the only two porous metallic oxides that are known to date. The electrocatalytic properties Of this material for oxygen reduction and evolution in aqueous and nonaqueous media were evaluated by cyclic vatarnmetry, chronoariaperometty, and linear sweep vdltarninetry. These techniques show that the synthesized pyttichlore lowers the overall oxidation voltage by 0.7 relative to carbon m nonaqueous, Li+ containing electrolyte. This is the result of its ability to both completely oxidize Li2O2 (at a relatively low potential) and electrocatalytically oxidize all known side products formed from electrolyte decomposition in the Li-O-2 battery. This further helps to explain the nature of "electrOcatalysis" in this system.
引用
收藏
页码:2322 / 2331
页数:10
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