Following the Evolution of Ru/Activated Carbon Catalysts during the Decomposition-Reduction of the Ru(NO)(NO3)3 Precursor

被引:19
作者
Garcia-Garcia, Francisco R. [1 ]
Fernandez-Garcia, Marcos [2 ]
Newton, Mark A. [3 ]
Rodriguez-Ramos, Inmaculada [2 ]
Guerrero-Ruiz, Antonio [1 ]
机构
[1] Unidad Asociada UNED CSIC, Fac Ciencias, Dept Quim Inorgan & Quim Tecn, Grp Diseno & Aplicac Catalizadores Heterogeneos, C Senda del Rey 9, Madrid, Spain
[2] CSIC, Inst Catalisis & Petr Quim, Madrid 28049, Spain
[3] European Synchrotron Radiat Facil, F-38043 Grenoble, France
关键词
carbon; reduction; ruthenium; supported catalysts; X-ray absorption spectroscopy; NI BIMETALLIC CATALYSTS; AMMONIA DECOMPOSITION; SURFACE-CHEMISTRY; RU CATALYSTS; ACTIVE-CARBON; HYDROGEN; RUTHENIUM; GENERATION; DIOXIDE; SITES;
D O I
10.1002/cctc.201300065
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Oxygen surface groups, which are typically present on the surface of activated carbon, have a decisive effect on the achieved dispersion of active phases, which affects the electronic properties of the surface sites and stabilizes the materials against sintering phenomena. Therefore, the desorption of oxygen surface groups during the decomposition-reduction of the metal salt precursors of the fresh carbon-based catalysts can lead to surface reconstruction of the metal nanoparticles, which can significantly affect their catalytic activity. In this work, the oxidation states of Ru atoms supported on both an activated carbon thermally treated during the reduction process. The precursor to prepare these catalysts is Ru(No)(NO3)(3). The main results were obtained by using in situ x-ray absorption near-edge structure analysis of the Ru K-edge under conditions comparable to the temperature-programmed reduction experiments. The different reduction mechanism observed in each of the catalysts, of a multistep nature if oxygen surface groups are present and single-step in the case of clean graphitic surfaces, differences in both the final Ru oxidation state and the main cause of the five-times higher catalytic activity observed in the presence of the catalyst without surface oxygen groups for the NH3 decomposition reaction.
引用
收藏
页码:2446 / 2452
页数:7
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