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高活性碳化钨负载型催化剂用于水煤气变换反应。

High activity carbide supported catalysts for water gas shift.

机构信息

Hydrogen Energy Technology Laboratory, University of Michigan, Ann Arbor, Michigan 48109, USA.

出版信息

J Am Chem Soc. 2011 Mar 2;133(8):2378-81. doi: 10.1021/ja110705a. Epub 2011 Feb 3.

Abstract

Nanostructured carbides are refractory materials with high surface areas that could be used as alternatives to the oxide materials that are widely used as support materials for heterogeneous catalysts. Carbides are also catalytically active for a variety of reactions, offering additional opportunities to tune the overall performance of the catalyst. In this paper we describe the synthesis of molybdenum carbide supported platinum (Pt/Mo(2)C) catalysts and their rates for the water gas shift reaction. The synthesis method allowed interaction of the metal precursor with the native, unpassivated support. The resulting materials possessed very high WGS rates and atypical Pt particle morphologies. Under differential conditions, rates for these catalysts were higher than those for the most active oxide-supported Pt catalysts and a commercial Cu-Zn-Al catalyst. Experimental and computational results suggested that active sites on the Pt/Mo(2)C catalysts were located on the perimeter of the Pt particles and that strong interactions between Pt and the Mo(2)C surface gave rise to raft-like particles.

摘要

纳米结构碳化物是具有高表面积的难熔材料,可用作广泛用作多相催化剂载体材料的氧化物材料的替代品。碳化物对于各种反应也具有催化活性,为进一步调整催化剂的整体性能提供了机会。本文介绍了负载型铂碳化钼(Pt/Mo2C)催化剂的合成及其在水煤气变换反应中的速率。该合成方法允许金属前体与原生的、未钝化的载体相互作用。所得到的材料具有非常高的 WGS 速率和典型的 Pt 颗粒形态。在差分条件下,这些催化剂的速率高于最活跃的氧化物负载型 Pt 催化剂和商业 Cu-Zn-Al 催化剂的速率。实验和计算结果表明,Pt/Mo2C 催化剂上的活性位位于 Pt 颗粒的周边,Pt 与 Mo2C 表面之间的强相互作用导致了筏状颗粒。

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