Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 8, Issue 9, Pages 6011-6018Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.5b11836
Keywords
artificial photosynthesis; carbon dioxide fixation; heterogeneous photocatalysis; light-energy conversion; solar fuels
Funding
- JSPS
- Photon and Quantum Basic Research Coordinated Development Program (MEXT, Japan)
- CREST program (JST)
- Noguchi Institute
- Murata Science Foundation
- Grants-in-Aid for Scientific Research [24107005] Funding Source: KAKEN
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Photocatalytic CO, reduction using hybrids of carbon nitride (C3N4) and a Ru(II) complex under visible light was studied with respect to reaction solvent. Three different Ru(II) complexes, trans(Cl)[Ru(X(2)bpy) (CO)(2)Cl-2] (X(2)bpy = 2,2'-bipyridine with substituents X in the 4-positions, X = COOH, PO3H2, or CH2PO3H2), were employed as promoters and will be abbreviated as RuC (X = COOH), RuP (X = PO3H2), and RuCP (X = CH2PO3H2). When C3N4 modified with a larger amount of RuCP (>7.8 mu mol g(-1)) was employed as a photocatalyst in a solvent having a relatively high donor number (e.g., N,N-dimethylacetamide (DMA), NN-dimethylformamide (DMF), and dimethyl sulfoxide (DMSO)) with the aid of triethanolamine (TEOA) as an electron donor, the hybrid photocatalyst exhibited high performance for CO2 reduction, producing CO and HCOOH with relatively high CO selectivity (40-70%). On the other hand, HCOOH was the major product when RuC/C3N4 or RuP/C3N4 was employed regardless of the loading amount of the Ru(II) complex and the reaction solvent. Results of photocatalytic reactions and UV-visible diffuse reflectance spectroscopy indicated that polymeric Ru species, which were formed in situ from RuCP on C3N4 under irradiation in a solvent having a high donor number, were active catalysts for CO formation. Nonsacrificial CO, reduction using RuP/C3N4 was accomplished in a DMA solution containing methanol as an electron donor, which means that visible light energy was stored as chemical energy in the form of CO and formaldehyde (Delta G degrees = +67.6 kJ mol(-1)). This study demonstrated the first successful example of an energy conversion scheme using carbon nitride through photocatalytic CO2 reduction.
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