Ananyev G M, Zaltsman L, Vasko C, Dismukes G C
Princeton University Department of Chemistry, Hoyt Laboratory, Princeton, NJ 09544, USA.
Biochim Biophys Acta. 2001 Jan 5;1503(1-2):52-68. doi: 10.1016/s0005-2728(00)00215-2.
At the request of the organizer of this special edition, we have attempted to do several things in this manuscript: (1) we present a mini-review of recent, selected, works on the light-induced inorganic biogenesis (photoactivation), composition and structure of the inorganic core responsible for photosynthetic water oxidation; (2) we summarize a new proposal for the evolutionary origin of the water oxidation catalyst which postulates a key role for bicarbonate in formation of the inorganic core; (3) we summarize published studies and present new results on what has been learned from studies of 'inorganic mutants' in which the endogenous cofactors (Mn(n+), Ca2+, Cl-) are substituted; (4) the first DeltapH changes measured during the photoactivation process are reported and used to develop a model for the stepwise photo-assembly process; (5) a comparative analysis is given of data in the literature on the kinetics of substrate water exchange and peroxide binding/dismutation which support a mechanistic model for water oxidation in general; (6) we discuss alternative interpretations of data in the literature with a view to forecast new avenues where progress is needed.
应本特刊组织者的要求，我们在本稿件中尝试做了几件事：（1）我们对近期精选的关于光诱导无机生物合成（光激活）、负责光合水氧化的无机核心的组成和结构的研究进行了简要综述；（2）我们总结了关于水氧化催化剂进化起源的一项新提议，该提议假定碳酸氢盐在无机核心形成中起关键作用；（3）我们总结了已发表的研究，并展示了从对内源辅因子（Mn(n+)、Ca2+、Cl-）被取代的“无机突变体”研究中所获得的新结果；（4）报告了光激活过程中首次测量到的ΔpH变化，并用于建立逐步光组装过程的模型；（5）对文献中关于底物水交换动力学以及过氧化物结合/歧化的数据进行了比较分析，这些数据总体上支持水氧化的机理模型；（6）我们讨论了文献数据的其他解释，以期预测需要取得进展的新途径。
