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原子层沉积法制备高比表面积 LaFeO 负载的热稳定性提高的智能 Pd 催化剂。

Smart Pd Catalyst with Improved Thermal Stability Supported on High-Surface-Area LaFeO Prepared by Atomic Layer Deposition.

机构信息

Department of Chemical and Biomolecular Engineering , University of Pennsylvania , 34th Street , Philadelphia , Pennsylvania 19104 , United States.

Department of Chemical and Pharmaceutical Sciences, ICCOM-CNR, Consortium INSTM , University of Trieste , via L. Giorgieri 1 , 34127 Trieste , Italy.

出版信息

J Am Chem Soc. 2018 Apr 11;140(14):4841-4848. doi: 10.1021/jacs.7b12900. Epub 2018 Mar 27.

Abstract

The concept of self-regenerating or "smart" catalysts, developed to mitigate the problem of supported metal particle coarsening in high-temperature applications, involves redispersing large metal particles by incorporating them into a perovskite-structured support under oxidizing conditions and then exsolving them as small metal particles under reducing conditions. Unfortunately, the redispersion process does not appear to work in practice because the surface areas of the perovskite supports are too low and the diffusion lengths for the metal ions within the bulk perovskite too short. Here, we demonstrate reversible activation upon redox cycling for CH oxidation and CO oxidation on Pd supported on high-surface-area LaFeO, prepared as a thin conformal coating on a porous MgAlO support using atomic layer deposition. The LaFeO film, less than 1.5 nm thick, was shown to be initially stable to at least 900 °C. The activated catalysts exhibit stable catalytic performance for methane oxidation after high-temperature treatment.

摘要

自再生或“智能”催化剂的概念是为了缓解高温应用中负载金属颗粒粗化的问题而开发的,它涉及在氧化条件下将大金属颗粒重新分散到钙钛矿结构的载体中,然后在还原条件下将其解吸为小金属颗粒。不幸的是,由于钙钛矿载体的表面积太低,体相钙钛矿中的金属离子扩散长度太短,因此再分散过程在实践中似乎不起作用。在这里,我们证明了在使用原子层沉积技术在多孔 MgAlO 载体上制备的具有高表面积 LaFeO 上负载的 Pd 进行 CH 氧化和 CO 氧化的氧化还原循环中的可逆活化。厚度小于 1.5nm 的 LaFeO 薄膜至少在 900°C 下是稳定的。经高温处理后,活化催化剂在甲烷氧化中表现出稳定的催化性能。

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