Model systems for flavoenzyme activity: Relationships between cofactor structure, binding and redox properties
Model systems for flavoenzyme activity: Relationships between cofactor structure, binding and redox properties
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DOI：
10.1021/ja036940b
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发表时间：
2003-12-24
影响因子：
15
通讯作者：
Rotello, VM
中科院分区：
文献类型：
--
作者：
Legrand, YM;Gray, M;Rotello, VM
合成了一系列带有吸电子和供电子取代基的黄素。测定了这些黄素在非极性溶剂中的电化学性质。二氨基吡啶 (DAP) 受体对这些黄素的识别以及该受体对黄素氧化还原电位的影响也得到了量化。结果发现，DAP-黄素结合亲和力以及 DAP 结合和未结合黄素的还原电位 (E-1/2) 与线性自由能关系 (LFER) 导出的函数密切相关。这些结果为非生物和酶系统的电子相互作用和氧化还原态特定相互作用提供了洞察和预测能力。
A series of flavins were synthesized bearing electron-withdrawing and -donating substituents. The electrochemical properties of these flavins in a nonpolar solvent were determined. The recognition of these flavins by a diamidopyridine (DAP) receptor and the effect this receptor has on flavin redox potential was also quantified. It was found that the DAP-flavin binding affinity and the reduction potentials (E-1/2) for both the DAP-bound and unbound flavins correlated well with functions derived from linear free energy relationships (LFERs). These results provide insight and predictive capability for the interplay of electronics and redox state-specific interactions for both abiotic and enzymatic systems.