From the Sabatier principle to a predictive theory of transition-metal heterogeneous catalysis
From the Sabatier principle to a predictive theory of transition-metal heterogeneous catalysis
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DOI：
10.1016/j.jcat.2014.12.033
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发表时间：
2015-08-01
影响因子：
7.3
通讯作者：
Norskov, Jens K.
中科院分区：
文献类型：
--
作者：
Medford, Andrew J.;Vojvodic, Aleksandra;Norskov, Jens K.
我们讨论了三个概念，使人们有可能发展一个定量的理解过渡金属催化的趋势：标度关系，活动地图，和d带模型。标度关系是不同吸附物种（包括过渡态）的表面键能之间的相关性;它们开启了将决定完全催化反应速率的许多参数映射到几个描述符上的可能性。所得的活性图可以被视为经典Sabatier原理的定量实施，该原理指出存在最佳“键强度”，其定义了给定反应的最佳催化剂。在现代版本中，标度关系决定了相关的“键强度”，并且这些描述符可以测量或计算的事实使其成为催化的定量理论，可以通过对新催化剂的具体预测进行实验测试。因此，该模型的定量方面提供了新的可能性，在催化剂的设计。最后，d带模型提供了一个理解的尺度关系和变化的催化活性方面的过渡金属表面的电子结构。(C)由Elsevier Inc.出版。
We discuss three concepts that have made it possible to develop a quantitative understanding of trends in transition-metal catalysis: scaling relations, activity maps, and the d-band model. Scaling relations are correlations between surface bond energies of different adsorbed species including transition states; they open the possibility of mapping the many parameters determining the rate of a full catalytic reaction onto a few descriptors. The resulting activity map can be viewed as a quantitative implementation of the classical Sabatier principle, which states that there is an optimum "bond strength" defining the best catalyst for a given reaction. In the modern version, the scaling relations determine the relevant "bond strengths" and the fact that these descriptors can be measured or calculated makes it a quantitative theory of catalysis that can be tested experimentally by making specific predictions of new catalysts. The quantitative aspect of the model therefore provides new possibilities in catalyst design. Finally, the d-band model provides an understanding of the scaling relations and variations in catalytic activity in terms of the electronic structure of the transition-metal surface. (C) 2015 Published by Elsevier Inc.