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硅基负载金铜纳米粒子催化剂的合成及其对 CO 氧化反应预处理条件的影响。

Synthesis of silica supported AuCu nanoparticle catalysts and the effects of pretreatment conditions for the CO oxidation reaction.

机构信息

Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA.

出版信息

Phys Chem Chem Phys. 2011 Feb 21;13(7):2571-81. doi: 10.1039/c0cp01859g. Epub 2011 Jan 18.

Abstract

Supported gold nanoparticles have generated an immense interest in the field of catalysis due to their extremely high reactivity and selectivity. Recently, alloy nanoparticles of gold have received a lot of attention due to their enhanced catalytic properties. Here we report the synthesis of silica supported AuCu nanoparticles through the conversion of supported Au nanoparticles in a solution of Cu(C(2)H(3)O(2))(2) at 300 °C. The AuCu alloy structure was confirmed through powder XRD (which indicated a weakly ordered alloy phase), XANES, and EXAFS. It was also shown that heating the AuCu/SiO(2) in an O(2) atmosphere segregated the catalyst into a Au-CuO(x) heterostructure between 150 °C to 240 °C. Heating the catalyst in H(2) at 300 °C reduced the CuO(x) back to Cu(0) to reform the AuCu alloy phase. It was found that the AuCu/SiO(2) catalysts were inactive for CO oxidation. However, various pretreatment conditions were required to form a highly active and stable Au-CuO(x)/SiO(2) catalyst to achieve 100% CO conversion below room-temperature. This is explained by the in situ FTIR result, which shows that CO molecules can be chemisorbed and activated only on the Au-CuO(x)/SiO(2) catalyst but not on the AuCu/SiO(2) catalyst.

摘要

担载金纳米粒子由于其极高的反应活性和选择性,在催化领域引起了极大的兴趣。最近,由于其增强的催化性能,金合金纳米粒子受到了广泛关注。在这里,我们通过在 300°C 的 Cu(C2H3O2)2 溶液中转化担载的 Au 纳米粒子,报告了通过在 300°C 的 Cu(C2H3O2)2 溶液中转化担载的 Au 纳米粒子合成二氧化硅担载的 AuCu 纳米粒子。通过粉末 XRD(表明存在弱有序合金相)、XANES 和 EXAFS 证实了 AuCu 合金结构。还表明,在 O2 气氛中加热 AuCu/SiO2 会将催化剂在 150°C 至 240°C 之间分离成 Au-CuO(x) 异质结构。在 300°C 的 H2 中加热催化剂可将 CuO(x) 还原回 Cu(0)以重新形成 AuCu 合金相。发现 AuCu/SiO2 催化剂对于 CO 氧化没有活性。但是,需要各种预处理条件才能形成高活性和稳定的 Au-CuO(x)/SiO2 催化剂,以在室温以下实现 100% CO 转化率。这可以通过原位 FTIR 结果得到解释,该结果表明只有在 Au-CuO(x)/SiO2 催化剂上,CO 分子才能被化学吸附和活化,而在 AuCu/SiO2 催化剂上则不能。

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