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用于低温下甲醇选择性气相氧化偶联的纳米多孔金催化剂。

Nanoporous gold catalysts for selective gas-phase oxidative coupling of methanol at low temperature.

机构信息

Institute of Applied and Physical Chemistry, Universität Bremen, Bremen 28359, Germany.

出版信息

Science. 2010 Jan 15;327(5963):319-22. doi: 10.1126/science.1183591.

Abstract

Gold (Au) is an interesting catalytic material because of its ability to catalyze reactions, such as partial oxidations, with high selectivities at low temperatures; but limitations arise from the low O2 dissociation probability on Au. This problem can be overcome by using Au nanoparticles supported on suitable oxides which, however, are prone to sintering. Nanoporous Au, prepared by the dealloying of AuAg alloys, is a new catalyst with a stable structure that is active without any support. It catalyzes the selective oxidative coupling of methanol to methyl formate with selectivities above 97% and high turnover frequencies at temperatures below 80 degrees C. Because the overall catalytic characteristics of nanoporous Au are in agreement with studies on Au single crystals, we deduced that the selective surface chemistry of Au is unaltered but that O2 can be readily activated with this material. Residual silver is shown to regulate the availability of reactive oxygen.

摘要

金(Au)是一种有趣的催化材料,因为它能够在低温下以高选择性催化反应,如部分氧化;但 Au 的 O2 离解概率低限制了其应用。通过使用负载在合适氧化物上的 Au 纳米颗粒可以克服这一问题,但后者容易烧结。通过脱合金 AuAg 合金制备的纳米多孔 Au 是一种具有稳定结构的新型催化剂,无需任何载体即可表现出活性。它在低于 80°C 的温度下催化甲醇选择性氧化偶联生成甲酸甲酯,选择性高于 97%,周转频率高。由于纳米多孔 Au 的整体催化特性与 Au 单晶的研究结果一致,我们推断 Au 的选择性表面化学性质没有改变,但可以通过这种材料容易地激活 O2。残留的银被证明可以调节活性氧的可用性。

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