Thomas John Meurig, Williams Robert J P
Department of Materials Science, University of Cambridge, Cambridge CB2 3QZ, UK.
Philos Trans A Math Phys Eng Sci. 2005 Apr 15;363(1829):765-91; discussion 1035-40. doi: 10.1098/rsta.2004.1534.
In this introductory paper, we endeavour to bridge the gaps that currently exist between the three main subdivisions of catalysis: enzymatic, homogeneous and heterogeneous. Hitherto, there has been a tendency for each of these three divisions to grow separately using their own concepts, phrases and techniques. However, there is much that unites them, not least the notion of the catalytically active site and, in particular, its often unusual (constrained) state of electronic or atomic environmental disposition. We identify many points of similarity between, for example, the mode of action of, metalloenzymes on the one hand and the recent generation of transition metal ions embedded within nanoporous (usually siliceous) solids on the other. Useful unifying principles emerge from considerations of free-energy/reaction-coordinate plots. We present a number of tabulations and comparisons designed to facilitate the understanding of the mode of operation of existing, and the performance of new, catalysts. In doing so, we have drawn on our own work as well as that of others, including contributions that are to be found in this volume, with the intention of covering the great variety of catalytic phenomena.
在这篇介绍性论文中，我们努力弥合目前催化作用的三个主要分支——酶催化、均相催化和多相催化之间存在的差距。迄今为止，这三个分支各自倾向于使用自己的概念、术语和技术独立发展。然而，它们之间有很多共通之处，尤其是催化活性位点的概念，特别是其通常不寻常的（受限的）电子或原子环境分布状态。我们发现了许多相似之处，例如，一方面是金属酶的作用方式，另一方面是最近在纳米多孔（通常为硅质）固体中嵌入的过渡金属离子。从自由能/反应坐标图的考虑中得出了有用的统一原理。我们提供了一些表格和比较，旨在促进对现有催化剂的作用方式以及新型催化剂性能的理解。在此过程中，我们借鉴了自己以及他人的工作，包括本卷中的相关贡献，目的是涵盖各种各样的催化现象。
