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

Soojin Kim, Songyi Lee, Tikum Florence Anjong, Ha Yoon Jang, Ji Yeong Kim, Chiho Lee, Sungnam Park, Hye Jin Lee, Juyoung Yoon, Jinheung Kim

Research output: Contribution to journalArticlepeer-review

15 Scopus citations

Abstract

(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.

Original languageEnglish
Pages (from-to)28407-28414
Number of pages8
JournalJournal of Physical Chemistry C
Volume120
Issue number50
DOIs
StatePublished - 22 Dec 2016

Bibliographical note

Funding Information:
This work was supported by the New & Renewable Energy Core Technology Program of the Korea Institute of Energy Technology Evaluation and Planning (KETEP) which was granted financial resources from the Ministry of Trade, Industry & Energy, Republic of Korea (20153030031720, to H.L.) and the National Research Foundation of Korea's (NRF) grant funded by the Korean government (MEST) (NRF-2016R1A2B4012488, to J.K.).

Publisher Copyright:
© 2016 American Chemical Society.

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