Artificial Photocatalytic System Using Polydiacetylene-(-NH-phen)Ru(bpy)(2) for Cofactor Regeneration and CO2 Reduction

作者：Kim Soojin; Lee Songyi; Anjong Tikum Florence; Jang Ha Yoon; Kim Ji Yeong; Lee Chiho; Park Sungnam; Lee Hye Jin^*; Yoon Juyoung; Kim Jinheung

来源：Journal of Physical Chemistry C, 2016, 120(50): 28407-28414.

DOI：10.1021/acs.jpcc.6b08532

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)(2)Ru(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 [ku(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),Ru(phen-NH)]-polydiacetylene, NADH was regenerated, and the reactivity using Ru(bpy),(phen-NH)-polydiacetyleue 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),Ru(phen-NH)]-polydiacetylene also showed much higher reactivity than the controls.

• 出版日期2016-12-22