Synthesis of Metal Complexes that can function in an Aqueous Solution Aiming at Application to Chemical Biology

为了开发适用于化学生物学的仿生金属配合物，我们用新设计的各种配体合成了金属配合物，这些配体专门稳定了溶液中金属配合物的结构。利用金属配合物，我们成功地实现了以下生物学相关功能：（1）模拟可溶性甲烷单加氧酶（sMMO）O_2激活中的P-Q转换，（2）富含羧酸盐的配位环境在O_2激活二铁酶中的作用，以及（3）作为析氧配合物（OEC）的模型，增强钌配合物对水氧化放出O_2的催化活性。在这些系统中，我们发现溶液中功能的最佳结构的稳定会导致功能的增强，这对于开发有效的仿生金属配合物至关重要。

For the purpose of developing bio-inspired metal complexes applicable to chemical biology, we synthesized metal complexes with newly designed various ligands that specifically stabilize the structures of the metal complexes in solution. With the metal complexes, we successfully attained following biologically relevant functions, (1) mimicking P-to-Q conversion in the O_2-activation of soluble methane monooxygenase(sMMO), (2) roles of the carboxylate-rich coordination environment in O_2-activating diiron enzymes, and (3) enhancement of catalytic activity of ruthenium complexes for O_2-evolution by water oxidation as a model of oxygen evolution complex(OEC). In these systems, we found that stabilization of the optimal structures for the functions in solution leads to enhancement of the functionality, essential for developing effective bio-inspired metal complexes.