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模拟碳酸酐酶的活性中心结构,以三(取代吡唑基)硼氢根[Tp~(R,R~1)]~-为配体,合成了一系列金属配合物Tp~(R,R~1)MX[R=Ph,2＇—thie(2＇—噻吩基),Me;R~1=Ph,2＇—thie,Me;M=Co,Ni,Cu,Zn,Cd;X=Cl,NO_3,CH_3COO]共13个,均经元素分析,IR,~1HNMR谱表征.选取其中5个有代表性的配合物,采用Stopped-flow技术,研究了模型物催化CO_2可逆水合反应的动力学,结果表明具备酶促反应动力学的一般特征.详细考察了溶液pH值、模型物的结构(尤其是中心金属离子的电子结构)、浓度对该反应的影响,得出一些重要的结果.计算出该反应有、无催化剂时的活化能,从本质上阐明了反应活化能降低是模型物加速反应的根本原因.
A series of metal complexes Tp ~ (R, R ~ 1) MX [R = Ph, 2’-thie (2’-thienyl), Me; R ~ 1 = Ph, 2’-thie, Me; M = Co, Ni, Cu, Zn, Cl, NO_3 and CH_3COO] were characterized by elemental analysis, IR and 1HNMR spectra, respectively. Five representative complexes were selected and the kinetics of catalytic CO 2 reversible hydration reaction was studied by using Stopped-flow technique The results showed that it has the general characteristics of enzymatic reaction kinetics.We investigated in detail the effects of the solution pH, the structure of the model compounds (especially the electronic structure of the central metal ion) and the concentration on the reaction, and obtained some important results. The activation energy of the reaction with and without the catalyst was calculated. It was clarified that the decrease of activation energy was the fundamental reason for the accelerated reaction of the model substance.