Artificial Photocatalytic System Using Polydiacetylene-(-NH-phen)Ru(bpy)2 for Cofactor Regeneration and CO2 Reduction
- 등재 SCIE, SCOPUS
- 발행기관 American Chemical Society
- 발행년도 2016
- 총서유형 Journal
- URI http://www.dcollection.net/handler/ewha/000000140572
- 본문언어 영어
- Published As http://dx.doi.org/SCI
- Published As SCIE
- Published As SCOPUS
- 저작권 이화여자대학교 논문은 저작권에 의해 보호받습니다.
초록/요약
(Chemical Equation Presented) For the practical use of a photobioreactor for artificial photosynthesis, efficient visible light-absorbing materials have to link reduction and oxidation catalysts for an efficient energy flow. As a step toward this goal of an NADH regeneration system and enzymatic production of solar fuels from CO2, we report the synthesis of a new polydiacetylene compound that is covalently connected with [Ru(phen-NH2) (bpy)2]2+ (bpy =2,2′-bipyridine, phen =1,10-phenonthroline-5-amine). The [(bpy)2Ru(phen-NH-)]-polydiacetylene absorbed a wide range of visible light because of the presence of two chromophores, the Ru complex and polydiacetylene. The polyacetylene backbone was converted from blue to red by conformational changes under the catalytic reaction conditions in a buffer solution. The electron transfer from the photoexcited [Ru(phen)(bpy)2]2+ to the polydiacetylene backbone was observed. In a visible light-driven photocatalytic NAD+ reduction by (cyclopentadienyl)Rh(bpy)(H2O)2+ with [(bpy)2Ru(phen-NH-)]-polydiacetylene, NADH was regenerated, and the reactivity using Ru(bpy)2(phen-NH)-polydiacetylene was enhanced relative to control experiments using only [Ru(phen)(bpy)2]2+ or polydiacetylene. The consecutive carbon dioxide reduction coupled with formate dehydrogenase was carried out to utilize the in situ photoregenerated NADH catalytically. The catalytic condition using [(bpy)2Ru(phen-NH-)]-polydiacetylene also showed much higher reactivity than the controls. © 2016 American Chemical Society.
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