Ir-Catalysed Nitrous oxide (N2O) Decomposition: Effect of Ir Particle Size and Metal-Support Interactions

Ir-Catalysed Nitrous oxide (N2O) Decomposition: Effect of Ir Particle Size and Metal-Support Interactions
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DOI:
10.1007/s10562-017-2233-z
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发表时间:
2018-01-01
期刊:
影响因子:
2.8
通讯作者:
Lambert, R. M.
Lambert, R. M.
中科院分区:
化学4区
文献类型:
--
作者:
Yentekakis, I. V.;Goula, G.;Lambert, R. M.

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研究了负载在. -研究了Al_2O_3、8mol%Y_2O_3稳定的ZrO_2(YSZ)、10mol%Gd_2O_3掺杂的CeO_2(GDC)和80wt%Al_2O_3 - 10wt%CeO_2 - 10wt%ZrO_2(ACZ)对它们在氧化条件下的稳定性、金属-载体相互作用和催化分解N_2O活性的影响。具有中等或高氧离子不稳定性的载体(GDC和ACZ)有效地稳定了Ir纳米颗粒以防止烧结,与提供可忽略的或低氧离子不稳定性的载体(γ-Al 2 O3和YSZ)形成鲜明对比。周转频率的研究,使用尺寸控制的Ir颗粒表现出较强的结构敏感性,脱N2 O催化剂有利于大的催化剂颗粒。虽然金属Ir显示出一定的脱N2 O活性,但IrO 2更活跃,可能在反应条件下作为铱颗粒上的表面覆盖层存在。在GDC和ACZ的情况下,通过支持物的O2-反向溢出,铱纳米颗粒表面上的有效双层[O delta--delta(+)](Ir)导致支持物诱导的周转率改变是显着的。图形摘要[GRAPHICS]。
The effect of the morphology of Ir particles supported on.-Al2O3, 8 mol% Y2O3-stabilized -ZrO2 (YSZ), 10 mol%Gd2O3-doped CeO2 (GDC) and 80 wt%Al2O3-10 wt%CeO2-10 wt%ZrO2 (ACZ) on their stability on oxidative conditions, the associated metal-support interactions and activity for catalytic decomposition of N2O has been studied. Supports with intermediate or high oxygen ion lability (GDC and ACZ) effectively stabilized Ir nanoparticles against sintering, in striking contrast to supports offering negligible or low oxygen ion lability (gamma-Al2O3 and YSZ). Turnover frequency studies using size-controlled Ir particles showed strong structure sensitivity, de-N2O catalysis being favoured on large catalyst particles. Although metallic Ir showed some de-N2O activity, IrO2 was more active, possibly present as a superficial overlayer on the iridium particles under reaction conditions. Support-induced turnover rate modifications, resulted from an effective double layer [O delta--delta(+)](Ir) on the surface of iridium nanoparticles, via O2- backspillover from the support, were significant in the case of GDC and ACZ.Graphical Abstract[GRAPHICS].