Structural bases for the catalytic mechanism of Ni-containing carbon monoxide dehydrogenases
Structural bases for the catalytic mechanism of Ni-containing carbon monoxide dehydrogenases
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DOI：
10.1039/b508403b
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发表时间：
2005-01-01
影响因子：
4
通讯作者：
Fontecilla-Camps, JC
中科院分区：
文献类型：
--
作者：
Volbeda, A;Fontecilla-Camps, JC
最近，我们对一氧化碳脱氢酶催化C簇结构/功能关系的理解取得了重大进展。已经报道了这种酶的几种结构，其中一些具有非常高的分辨率。然而，一个经常出现的问题是每个结构内以及不同X射线模型之间的高度不均匀性。在这里，我们试图将结构数据与多年来收集的丰富的光谱和生物化学信息联系起来。因此，我们提出了一个催化循环，这是符合观察和立体化学。我们还给出了替代方案的一个最困难的方面的周期，即，位置的两个电子在最减少状态的C-集群。
Significant progress has been made recently in our understanding of the structure/function relationships of the catalytic C-cluster of carbon monoxide dehydrogenases. Several structures of this enzyme have been reported, some of them at very high resolution. One recurrent problem, however, is the high degree of heterogeneity within each structure, as well as between the different X-ray models. Here, we have tried to relate the structural data with the wealth of spectroscopic and biochemical information gathered over many years. As a result, we propose a catalytic cycle that is consistent with both observations and stereochemistry. We also give alternatives to one of the most difficult aspects of the cycle, namely, the location of the two electrons in the most reduced state of the C-cluster.