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제125회 대한화학회 학술발표회 및 총회 Computational Understanding of Electrocatalytic Selective CO2 Conversion to Formic acid with Amine-tethered Manganese Bipyridine Catalyst

등록일
2020년 2월 4일 16시 43분 31초
접수번호
0276
발표코드
ELEC.P-894 이곳을 클릭하시면 발표코드에 대한 설명을 보실 수 있습니다.
발표시간
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발표형식
포스터
발표분야
Electrochemistry
저자 및
공동저자
Dasol Cho, Mu-Hyun Baik1,*
Department of chemistry, Korea Advanced Institute of Science and Technology, Korea
1Chemistry, Korea Advanced Institute of Science and Technology, Korea
Electrocatalysis for CO2 conversion to other C1 or Cn product is regarded as the one of the promising solution to cope with increasing CO2 concentration in earth for decades. Starting with Lehn's rhenium bipyridine system, so many researches has continued to develop a catalytic system showing the efficient transformation of CO2 to CO which would be a key feedstock of Fischer-Tropsch process. However, recently, the transformation of CO2 to formate/formic acid is of great interest with its usage as an energy carrier or as a hydrogen storage material. We developed a first high efficient electrocatalytic homogeneous system for CO2 to formate/formic acid conversion by constructing the secondary coordination sphere of a tethered amine group to general manganese bipyridine catalyst. This system shows a high efficiency as a conversion catalyst with showing a maximum turnover frequency of up to 5500 and working at an overpotential of 300 mV~630 mV. Mechanistically, the rule of the amine is demonstrated as a Brønsted base catalyst and H+-transfer mediator. The key intermediate is determined by cyclic voltammetry, 1H NMR, DFT calculations, and infrared spectroelectrochemistry.

Reference
Magnus H. Rønne, Dasol Cho, Monica R. Madsen, Joakim B. Jakobsen, Seunghwan Eom, Émile Escoudé, Hans Christian D. Hammershøj, Dennis U. Nielsen, Steen U. Pedersen, Mu-Hyun Baik*, Troels Skrydstrup*, Kim Daasbjerg*, Ligand Controlled Product Selectivity in the Electrochemical Carbon Dioxide Reduction Using Manganese Bipyridine Catalysts, J. Am. Chem. Soc. 2020, accepted

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