Details
| Original language | English |
|---|---|
| Pages (from-to) | 6073–6083 |
| Number of pages | 11 |
| Journal | ACS Sustainable Chemistry & Engineering |
| Volume | 6 |
| Issue number | 5 |
| Early online date | 22 Mar 2018 |
| Publication status | Published - 7 May 2018 |
Abstract
Immobilization of Re(I) CO 2 reduction photocatalysts on metal oxide surfaces is an interesting approach to improve their stability and recyclability. In this work, we describe the photocatalytic activity of two Re(I) complexes (fac-[Re(NN)(CO) 3(Cl)], NN = 4,4'-dicarboxylic acid-2,2'-bipyridine, 1, or 5,6-dione-1,10-phenantroline, 2) on the surface of hexaniobate nanoscrolls. After adsorption, the turnover number for CO production (TON CO) in DMF/TEOA of 1 was increased from 9 to 58, which is 20% higher than that observed on TiO 2, being among the highest reported values for a Re(I)-based photocatalyst under visible light irradiation without any sensitizer. The complex 2 is inactive in solution under visible-light irradiation, but it has a TON CO of 35 when immobilized on hexaniobate nanoscrolls. Transient absorption spectroscopy studies reveal that the slow back-electron transfer and the higher reducing power of the hexaniobate conduction-band electrons play a major role for the photocatalytic process. The results provide new insights concerning the role of the metal oxide substrate on Re(I)-based molecular systems for CO 2 reduction.
Keywords
- Re(I)-based molecular catalysts, layered materials, photocatalytic CO reduction, transient absorption spectroscopy
ASJC Scopus subject areas
- Chemistry(all)
- Environmental Science(all)
- Environmental Chemistry
- Chemical Engineering(all)
- Energy(all)
- Renewable Energy, Sustainability and the Environment
Sustainable Development Goals
Cite this
- Standard
- Harvard
- Apa
- Vancouver
- BibTeX
- RIS
In: ACS Sustainable Chemistry & Engineering, Vol. 6, No. 5, 07.05.2018, p. 6073–6083.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
T1 - Photocatalytic CO2 Reduction by Re(I) Polypyridyl Complexes Immobilized on Niobates Nanoscrolls
AU - Faustino, L.A.
AU - Souza, B.L.
AU - Nunes, B.N.
AU - Duong, A.-T.
AU - Sieland, Fabian
AU - Bahnemann, Detlef W.
AU - Patrocinio, A.O.T.
N1 - © 2018 American Chemical Society
PY - 2018/5/7
Y1 - 2018/5/7
N2 - Immobilization of Re(I) CO 2 reduction photocatalysts on metal oxide surfaces is an interesting approach to improve their stability and recyclability. In this work, we describe the photocatalytic activity of two Re(I) complexes (fac-[Re(NN)(CO) 3(Cl)], NN = 4,4'-dicarboxylic acid-2,2'-bipyridine, 1, or 5,6-dione-1,10-phenantroline, 2) on the surface of hexaniobate nanoscrolls. After adsorption, the turnover number for CO production (TON CO) in DMF/TEOA of 1 was increased from 9 to 58, which is 20% higher than that observed on TiO 2, being among the highest reported values for a Re(I)-based photocatalyst under visible light irradiation without any sensitizer. The complex 2 is inactive in solution under visible-light irradiation, but it has a TON CO of 35 when immobilized on hexaniobate nanoscrolls. Transient absorption spectroscopy studies reveal that the slow back-electron transfer and the higher reducing power of the hexaniobate conduction-band electrons play a major role for the photocatalytic process. The results provide new insights concerning the role of the metal oxide substrate on Re(I)-based molecular systems for CO 2 reduction.
AB - Immobilization of Re(I) CO 2 reduction photocatalysts on metal oxide surfaces is an interesting approach to improve their stability and recyclability. In this work, we describe the photocatalytic activity of two Re(I) complexes (fac-[Re(NN)(CO) 3(Cl)], NN = 4,4'-dicarboxylic acid-2,2'-bipyridine, 1, or 5,6-dione-1,10-phenantroline, 2) on the surface of hexaniobate nanoscrolls. After adsorption, the turnover number for CO production (TON CO) in DMF/TEOA of 1 was increased from 9 to 58, which is 20% higher than that observed on TiO 2, being among the highest reported values for a Re(I)-based photocatalyst under visible light irradiation without any sensitizer. The complex 2 is inactive in solution under visible-light irradiation, but it has a TON CO of 35 when immobilized on hexaniobate nanoscrolls. Transient absorption spectroscopy studies reveal that the slow back-electron transfer and the higher reducing power of the hexaniobate conduction-band electrons play a major role for the photocatalytic process. The results provide new insights concerning the role of the metal oxide substrate on Re(I)-based molecular systems for CO 2 reduction.
KW - Re(I)-based molecular catalysts
KW - layered materials
KW - photocatalytic CO reduction
KW - transient absorption spectroscopy
UR - http://www.scopus.com/inward/record.url?scp=85046826377&partnerID=8YFLogxK
U2 - 10.1021/acssuschemeng.7b04713
DO - 10.1021/acssuschemeng.7b04713
M3 - Article
VL - 6
SP - 6073
EP - 6083
JO - ACS Sustainable Chemistry & Engineering
JF - ACS Sustainable Chemistry & Engineering
SN - 2168-0485
IS - 5
ER -