In this short review, we provide an account of a number of computational studies of catalytic reaction mechanisms carried out in our groups. We focus in particular on studies in which we came to realize during the course of the investigation that the active catalytic species was a bimetallic complex, rather a monometallic one as previously assumed. In some cases, this realization was in part prompted by experimental observations, but careful exploration based on computation of the speciation of the metal precursor also provided a powerful guide: it is often possible to predict that bimetallic species (intermediates or transition states) lie lower in free energy than a priori competitive monometallic species. In this sense, we argue that in organometallic catalysis, the rule whereby “two is better than one” turns out to be relevant much more often than one might expect.

在这篇简短的评论中，我们提供了对我们小组中进行的催化反应机制的许多计算研究的说明。我们特别关注在调查过程中我们意识到活性催化物质是双金属的研究复杂的，而不是之前假设的单金属。在某些情况下，这种认识部分是由实验观察促成的，但基于金属前体物种形成计算的仔细探索也提供了强有力的指导：通常可以预测双金属物种（中间体或过渡态）位于较低的位置在自由能方面比先验的竞争性单金属物种。从这个意义上说，我们认为在有机金属催化中，“两个比一个更好”的规则比人们预期的更相关。