La2O2CO3 Encapsulated La2O3 Nanoparticles Supported on Carbon as Superior Electrocatalysts for Oxygen Reduction Reaction

材料科学 氧还原反应 纳米颗粒 氧气 电催化剂 碳纤维 化学工程 无机化学 纳米技术 物理化学 电化学 电极 化学 复合数 工程类 复合材料 有机化学
作者
Weiwei Gu,Jingjun Liu,Mingan Hu,Feng Wang,Ye Song
出处
期刊:ACS Applied Materials & Interfaces [American Chemical Society]
卷期号:7 (48): 26914-26922 被引量:93
标识
DOI:10.1021/acsami.5b06100
摘要

Constructing nanoscale hybrid materials with unique interfacial structures by using various metal oxides and carbon supports as building blocks are of great importance to develop highly active, economical hybrid catalysts for oxygen reduction reaction (ORR). In this work, La2O2CO3 encapsulated La2O3 nanoparticles on a carbon black (La2O2CO3@La2O3/C) were fabricated via chemical precipitation in an aqueous solution containing different concentrations of cetyltrimethyl ammonium bromide (CTAB), followed by calcination at 750 °C. At a given CTAB concentration 24.8 mmol/L, the obtained lanthanum compound nanoparticles reach the smallest particle size (7.1 nm) and are well-dispersed on the carbon surface. X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) results demonstrate the formation of La2O2CO3 located on the surface of La2O3 nanoparticles in the hybrid. The synthesized La2O2CO3@La2O3/C hybrid exhibits a significantly enhanced electrocatalytic activity in electrocatalysis experiments relative to pure La2O3, La2O2CO3, and carbon in an alkaline environment, by using the R(R)DE technique. Moreover, its long-term stability also outperforms that obtained by commercial Pt/C catalysts (E-TEK). The exact origin of the fast ORR kinetics is mainly ascribed to the La2O2CO3 layer sandwiched at the interface of carbon and La2O3, which contributes favorable surface-adsorbed hydroxide (—OH–ad) substitution and promotes active oxygen adsorption at the interfaces. The unique covalent —C—O—C(═O)—O—La—O— bonds, formed at the interfaces between La2O2CO3 and carbon, can act as active sites for the improved ORR kinetics over this hybrid catalyst. Therefore, the fabrication of lanthanum compound-based hybrid material with an unique interfacial structure maybe open a new way to develop carbon-supported metal oxides as next-generation of ORR catalysts.
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