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胶体金负载于块状 MnO2 纳米材料上对 CO 的低温氧化:不同氧化锰上的金。

Gold on Different Manganese Oxides: Ultra-Low-Temperature CO Oxidation over Colloidal Gold Supported on Bulk-MnO2 Nanomaterials.

机构信息

Max-Planck-Institut für Kohlenforschung , Kaiser-Wilhelm-Platz 1, 45470 Mülheim an der Ruhr, Germany.

Inorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science, Utrecht University , Universiteitsweg 99, 3584 CG Utrecht, The Netherlands.

出版信息

J Am Chem Soc. 2016 Aug 3;138(30):9572-80. doi: 10.1021/jacs.6b04251. Epub 2016 Jul 20.

Abstract

Nanoscopic gold particles have gained very high interest because of their promising catalytic activity for various chemicals reactions. Among these reactions, low-temperature CO oxidation is the most extensively studied one due to its practical relevance in environmental applications and the fundamental problems associated with its very high activity at low temperatures. Gold nanoparticles supported on manganese oxide belong to the most active gold catalysts for CO oxidation. Among a variety of manganese oxides, Mn2O3 is considered to be the most favorable support for gold nanoparticles with respect to catalytic activity. Gold on MnO2 has been shown to be significantly less active than gold on Mn2O3 in previous work. In contrast to these previous studies, in a comprehensive study of gold nanoparticles on different manganese oxides, we developed a gold catalyst on MnO2 nanostructures with extremely high activity. Nanosized gold particles (2-3 nm) were supported on α-MnO2 nanowires and mesoporous β-MnO2 nanowire arrays. The materials were extremely active at very low temperature (-80 °C) and also highly stable at 25 °C (70 h) under normal conditions for CO oxidation. The specific reaction rate of 2.8 molCO·h(-1)·gAu(-1) at a temperature as low as -85 °C is almost 30 times higher than that of the most active Au/Mn2O3 catalyst.

摘要

纳米金颗粒因其在各种化学反应中表现出的高催化活性而备受关注。在这些反应中,低温 CO 氧化是研究最广泛的反应之一,因为它在环境应用中具有实际意义,并且在低温下具有非常高的活性,这涉及到一些基本问题。负载在氧化锰上的金纳米颗粒属于 CO 氧化的最活跃的金催化剂之一。在各种氧化锰中,MnO2 被认为是最有利于提高金纳米颗粒催化活性的载体。在之前的工作中,已经表明负载在 MnO2 上的金比负载在 Mn2O3 上的金的活性要低得多。与之前的这些研究不同,在对不同的氧化锰负载的金纳米颗粒的综合研究中,我们开发出了一种在 MnO2 纳米结构上具有极高活性的金催化剂。纳米金颗粒(2-3nm)负载在 α-MnO2 纳米线和介孔 β-MnO2 纳米线阵列上。这些材料在非常低的温度(-80°C)下具有极高的活性,并且在正常条件下(25°C)下也具有很高的稳定性,在 CO 氧化反应中可以持续 70 小时。在如此低的温度(-85°C)下,其特定反应速率达到 2.8 molCO·h(-1)·gAu(-1),几乎比最活跃的 Au/Mn2O3 催化剂高 30 倍。

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