Development of efficient oxidation catalysts with cheap oxidants

2016 Fiscal Year Final Research Report

• Project/Area Number: 26630414
• Research Category: Grant-in-Aid for Challenging Exploratory Research
• Allocation Type: Multi-year Fund
• Research Field: Catalyst/Resource chemical process
• Research Institution: Doshisha University
• Principal Investigator: Kodera Masahito 同志社大学, 理工学部, 教授 (00183806)
• Project Period (FY): 2014-04-01 – 2017-03-31
• Keywords: 可溶性メタンモノオキシゲナーゼ / 酸素分子活性化 / 安価な酸化剤 / カルボキシル基含有二核化配位子 / アルカン水酸化 / カルボキシラト基の効果 / A/K比 / 触媒回転数

Outline of Final Research Achievements

Soluble methane monooxygenases (sMMO) are nonheme diiron enzymes that catalyze oxidation of various organic compounds. Diiron centers of sMMO are coordinated by two imidazole donors of His residues and by four carboxylate donors of Glu residues. In this study we synthesized four different carboxylate-rich dinucleating ligands, 1,2-bis(N-benzyl-2-amino- methyl-6-pyridyl)ethane-N,N’-diglycine (H2Lgly), 1,2-bis(6-aminomethyl-2-pyridyl)ethane-N,N’-di- (norleucine) (H2Lnle), 1,2-bis(6-aminomethyl-2-pyridyl)ethane-N,N’-di(N-methylnorleucine) (H2LMenle), 1,2-bis(N-(9-anthracene)-2-aminomethyl-6-pyridyl)ethane (H2Lanthracenegly). These ligands form diiron complexes, which rapidly and efficiently catalyzed the oxidation of alkanes with m-CPBA as an oxidant to show high A/K ratio, large turnover number, large turnover frequency in the catalytic oxidations. These are attained by the carboxylate-rich coordination environment.

Free Research Field

生物無機化学　bioinorganic chemistry