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제123회 대한화학회 학술발표회, 총회 및 기기전시회 안내 Synthesis of Model Complex of [NiFe]-Carbon Monoxide Dehydrogenase Active Site using Aromatic Spacer

2019년 2월 12일 23시 02분 51초
INOR.P-85 이곳을 클릭하시면 발표코드에 대한 설명을 보실 수 있습니다.
4월 18일 (목요일) 11:00~12:30
Inorganic Chemistry
저자 및
Seungjin Song, Junhyeok Seo*
Department of Chemistry, Gwangju Institute of Science and Technology, Korea
Carbon monoxide dehydrogenase (CODH) is a family of enzymes, that promotes the conversion of CO to CO2. The enzymes are categorized as [NiFe]- and [MoCu]-CODH according to the metal ions in the active sites. The [NiFe]-CODH, functioning under anaerobic conditions, is known to be also active for the reversible CO2 reduction. According to the X-ray crystal structure, the enzyme active site contains a Ni(II) ion in the square planar geometry and a high-spin Fe(II) in the tetrahedral coordination. In particular, as seen in another X-ray crystal structure of the ‘Ni-C(O)O-Fe’ moiety, the FeS cluster maintains the Ni and Fe centers by 2.87 Å. The interstitial distance seems essential for the interaction of the CO2 molecule with the ‘frustrated’ Lewis pair of the Ni and Fe centers. Since the time that the crystal structure of the enzyme active site is known, many structural analogues have been synthesized by others; however, so far known models never showed the enzyme-like reactivity with CO2 or CO. We synthesize model complexes of the [NiFe]-CODH active site to understand the structural meaning of the active site, and furthermore develop the small molecular catalysts for the CO2 reduction. Currently, we model the Ni active center by a Ni-pincer complex, and then conjugate a high spin Fe(II) complex using aromatic spacers. The molecular framework would likely position the Ni/Fe active centers closely to capture CO2, and the synthesized model complexes are tested for the reduction of CO2.