Population and hierarchy of active species in gold iron oxide catalysts for carbon monoxide oxidation.

Population and hierarchy of active species in gold iron oxide catalysts for carbon monoxide oxidation.
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DOI:
10.1038/ncomms12905
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发表时间:
2016-09-27
影响因子:
16.6
通讯作者:
Kiely, Christopher J.
Kiely, Christopher J.
中科院分区:
综合性期刊1区
文献类型:
--
作者:
He, Qian;Freakley, Simon J.;Edwards, Jennifer K.;Carley, Albert F.;Borisevich, Albina Y.;Mineo, Yuki;Haruta, Masatake;Hutchings, Graham J.;Kiely, Christopher J.

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低温一氧化碳氧化负载型金催化剂中活性物种的身份仍然是一个悬而未决的争论。随着大量的实验证据支持金纳米粒子或亚纳米金物种具有活性的理论,最近有人提出应该存在大小依赖的活性等级。本文研究了共沉淀法和沉积沉淀法制备的Au/FeOx材料在热处理后的不同催化行为。排除任何支持的影响后,在不同的催化剂中的金粒子的粒度分布定量研究使用像差校正扫描透射电子显微镜(STEM)。开发了一种计数方案,以从HAADF-STEM图像中揭示真实的粒度分布,该图像可靠地包括所有存在的金物质。与催化结果的各种金物种存在的人口的相关性表明,一个大小依赖的活性层次必须存在于Au/FeOx催化剂。低温一氧化碳氧化负载型金催化剂中活性物种的身份仍然是一个悬而未决的问题。在这里,作者研究了在不同条件下制备的负载型催化剂的催化行为,并将各种物种的数量与活性相关联。
The identity of active species in supported gold catalysts for low temperature carbon monoxide oxidation remains an unsettled debate. With large amounts of experimental evidence supporting theories of either gold nanoparticles or sub-nm gold species being active, it was recently proposed that a size-dependent activity hierarchy should exist. Here we study the diverging catalytic behaviours after heat treatment of Au/FeOx materials prepared via co-precipitation and deposition precipitation methods. After ruling out any support effects, the gold particle size distributions in different catalysts are quantitatively studied using aberration corrected scanning transmission electron microscopy (STEM). A counting protocol is developed to reveal the true particle size distribution from HAADF-STEM images, which reliably includes all the gold species present. Correlation of the populations of the various gold species present with catalysis results demonstrate that a size-dependent activity hierarchy must exist in the Au/FeOx catalyst. The identity of active species in supported gold catalysts for low-temperature carbon monoxide oxidation remains an open question. Here, the authors look at the catalytic behaviours of supported catalysts prepared under different conditions and correlate the populations of various species with activity.
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