Reply to comment on ''CO oxidation on ruthenium: The nature of the active catalytic surface'' by H. Over, M. Muhler, A.P. Seitsonen
Reply to comment on ''CO oxidation on ruthenium: The nature of the active catalytic surface'' by H. Over, M. Muhler, A.P. Seitsonen
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DOI：
10.1016/j.susc.2007.09.042
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发表时间：
2007-12
期刊：
影响因子：
1.9
通讯作者：
D. Goodman;C. Peden;Mingshu Chen
中科院分区：
文献类型：
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作者：
D. Goodman;C. Peden;Mingshu Chen
我们首先声明，我们的信[1]的前提是强调Peden和Goodman（PG）[2]的早期研究可以完全解释为活性表面是单层氧覆盖的Ru（0001）表面。与作者在其评论中的论点相反，PG [2]实验中讨论的反应条件跨越了375至600 K的温度范围，O2和CO压力范围为0.5至500 Torr，CO/O2比为60至0.03。作者在他们的引言中指出，“只有在高于500 K的温度下，Ru金属才会氧化为RuO 2。在这里，我们不想讨论所有形态的Ru的氧化，而是讨论在Ru（0001）上形成RuO 2所需的特定反应条件，Ru（0001）是PG实验中使用的催化剂，也是我们之前的信[1]的主题。事实上，正如我们在信[1]中指出的那样，奥弗和同事在一项非常明确的工作[3]中表明，在Ru（0001）上形成RuO 2所需的临界条件远远超出了PG实验中使用的温度和氧化学势。根据我们早期的研究[2]和Over及其同事的工作[3]，我们在信中得出结论，在PG实验中，RuO 2不可能形成到任何明显的程度。
We first state that the premise of our Letter [1] was to state emphatically that the early studies of Peden and Goodman (PG) [2] can be entirely explained by and are only consistent with the active surface being a monolayer oxygen-covered Ru(0001) surface. Contrary to the authors’ contention in their Comment, the reaction conditions addressed in the experiments of PG [2] spanned the temperature range 375 to 600 K, a pressure range of O2 and CO pressures from 0.5 to 500 Torr, and CO/O2 ratios from 60 to .03. The authors state in their introduction that “the oxidation of Ru metal takes place to RuO2 only for temperatures higher than 500 K. Here we do not wish to address the oxidation of Ru in all morphologies, but rather the specific reaction conditions required for RuO2 to form on Ru(0001), the catalyst used in the experiments of PG and the subject of our previous Letter [1]. Indeed, as pointed out in our Letter [1], Over and coworkers in a very definitive piece of work [3] showed that the critical conditions required for the formation of RuO2 on Ru(0001) were far outside those used in the experiments of PG with respect to temperature and oxygen chemical potential. Based on our earlier studies [2] and the work of Over and coworkers [3] we concluded in our Letter that RuO2 could not have formed to any appreciable extent in the PG experiments.