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Synthesis of Ceria-Zirconia Nanocrystals with Improved Microstructural Homogeneity and Oxygen Storage Capacity by Hydrolytic Sol-Gel Process in Coordinating Environment

机译:协同环境下水解溶胶-凝胶法合成具有改善的微结构同质性和储氧能力的氧化铈-锆纳米晶

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摘要

Ceria-zirconia solid solution nanocrystals, (1 - x)CeO_(2-x)ZrO_2, 0 ≤ x ≤ 1, are prepared by sol-gel processing in dodecylamine of solutions obtained by forced hydrolysis of inorganic salts. The as-prepared nanoparticles have a ceria cubic structure, up to x = 0.35, or are amorphous. Heat-treatment is carried out at temperatures ranging from 500 to 800 ℃, the latter temperature begin suitable to obtain solid solutions throughout the composition range. For all the heating temperatures and x values, the fluorite cubic structure of pure CeO_2 transforms to a mixture (c) of the cubic c and tetragonal t" phases for x = 0.35, and to tetragonal t phase only for x = 0.8 at 650 ℃, x = 0.65 at 800 ℃, and, to a very limited extent, x = 0.5 at 1000 °C. No evidence is obtained at low x values of the t phase, which is detrimental to the oxygen storage capacity. Prolonged heating at 1000 ℃ demonstrates that only for x = 0.65 a limited separation of CeO_2-rich nanocrystals occurs. The samples undergo the same transition without simultaneous occurrence of different phases, apart for the two mentioned limited cases. This result is attributed to the intimate mixing of the metal cations even in the early stages of processing. In as-prepared samples the Zr distribution becomes inhomo-geneous when going from x = 0.2 to x = 0.35, but no early phase separations appear. The oxygen storage capacity is favorably influenced by the persistence of the cubic c phase.
机译:氧化铈-氧化锆固溶体纳米晶体(1-x)CeO_(2-x)ZrO_2,0≤x≤1,是通过在十二烷基胺中通过溶胶-凝胶工艺制备的,该溶液通过无机盐的强力水解而制得。所制备的纳米颗粒具有二氧化铈立方结构,最高x = 0.35,或者是无定形的。热处理在500至800℃的温度范围内进行,后者温度开始适合于在整个组成范围内获得固溶体。对于所有加热温度和x值,x = 0.35时,纯CeO_2的萤石立方结构转变为立方c和四方t“相的混合物(c),在650℃时仅x = 0.8时转变为四方t相。 ,在800℃时x = 0.65,在非常有限的程度上,在1000°C时x = 0.5。在低的t相x值下没有得到证据,这不利于储氧量。在1000℃下长时间加热℃表明,仅当x = 0.65时,富CeO_2纳米晶体才发生有限的分离;样品经历了相同的转变而没有同时出现不同的相,这是上述两种有限的情况,这是由于金属的充分混合造成的。在制备的样品中,Zr分布从x = 0.2变为x = 0.35时,Zr分布变得不均质,但没有出现早期相分离现象。立方度ase。

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  • 来源
    《Advanced Functional Materials》 |2012年第13期|p.2867-2875|共9页
  • 作者单位

    Consiglio Nazionale delle Ricerche - Istituto per la Microelettronica e Microsistemi (C.N.R.-I.M.M.), via Monteroni, 1-73100 Lecce, Italy;

    Catalonia Institute for Energy Research IREC c/Jardins de les Dones de Negre 1, 08930-Sant Adria del Besos, Barcelona, Spain;

    M2E-IN2UB-XaRMAE Departament d'Electronica Universitat de Barcelona C. Marti I Franques 1, 08028 Barcelona, CAT, Spain;

    M2E-IN2UB-XaRMAE Departament d'Electronica Universitat de Barcelona C. Marti I Franques 1, 08028 Barcelona, CAT, Spain;

    Catalonia Institute for Energy Research IREC c/Jardins de les Dones de Negre 1, 08930-Sant Adria del Besos, Barcelona, Spain;

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