Selective Hydrogenation of Acetylene Over Gold Nanoparticles Supported on CeO2 Pretreated Under Different Atmospheres

Selective Hydrogenation of Acetylene Over Gold Nanoparticles Supported on CeO2 Pretreated Under Different Atmospheres
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不同气氛下CeO2负载金纳米粒子对乙炔的选择性加氢

DOI:
10.1007/s10562-018-2628-5
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发表时间:
2018-12
期刊:
影响因子:
2.8
通讯作者:
Qi Caixia
Qi Caixia
中科院分区:
化学4区
文献类型:
--
作者:
Peng Shuang;Sun Xun;Sun Libo;Zhang Miao;Zheng Yuhua;Su Huijuan;Qi Caixia

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负载型金催化剂是一种高效的乙炔选择加氢催化剂。研究表明,氧化铈等可还原材料由于其独特的还原态和氧化态之间的电荷转移,可能会影响催化性能。然而,它在催化性能中的作用仍然存在激烈的争论。本文分别在空气和氢气气氛下制备了不同形貌的CeO 2负载Au催化剂,并对催化剂进行了乙炔选择加氢性能评价。在空气中还原的Au/CeO 2催化剂,无论是棒状(简称R)还是多面体(简称P),其催化性能均优于在H2气氛中还原的催化剂。Au/CeO 2(R)-空气催化剂表现出最好的性能。在300 °C时,C_2H_2转化率约为Au/CeO_2(R)-H_2催化剂的3倍。拉曼光谱和XPS分析表明,催化剂的活性与氧空位浓度有关,其缺陷特征与预处理气氛有关。本文的研究不仅加深了对催化剂缺陷特征对催化性能影响的认识,而且为通过控制预处理气氛制备高效的多相金/铈催化剂提供了可能。
AbstractSupported gold catalysts are highly efficient for selective hydrogenation of acetylene. It has been shown that reducible materials such as ceria may influence the catalytic performance due to its unique charge shift between reduced and oxidized state. However, its role in catalytic performance remains fiercely debated. In this paper, differently morphological CeO2supported Au catalysts were prepared with pretreatment under air and H2atmospheres respectively, and evaluated for selective hydrogenation of acetylene. No matter with rod (abbreviated as R) or polyhedral (abbreviated as P) shape, the catalysts of Au/CeO2reduced in air exhibits better catalytic performance than that in H2atmosphere. The Au/CeO2(R)-air catalyst shows the best performance. The C2H2conversion is about three times of that over the catalyst of Au/CeO2(R)-H2at 300 °C. The Raman result and XPS analysis clearly showed a dependence of catalytic activity on the oxygen vacancy concentration of catalysts, revealing the correlation between its defect features and pretreatment atmosphere. Our report not only deepens the knowledge of catalytic performance affected by defect features of catalyst but also provides a possibility for the efficient heterogeneous gold/ceria catalysts by controlling the pretreatment atmosphere.Graphical Abstract
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影响因子: 12.9
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