Details
| Originalsprache | Englisch |
|---|---|
| Seiten (von - bis) | 6073–6083 |
| Seitenumfang | 11 |
| Fachzeitschrift | ACS Sustainable Chemistry and Engineering |
| Jahrgang | 6 |
| Ausgabenummer | 5 |
| Frühes Online-Datum | 22 März 2018 |
| Publikationsstatus | Veröffentlicht - 7 Mai 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.
ASJC Scopus Sachgebiete
- Chemie (insg.)
- Umweltwissenschaften (insg.)
- Umweltchemie
- Chemische Verfahrenstechnik (insg.)
- Energie (insg.)
- Erneuerbare Energien, Nachhaltigkeit und Umwelt
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in: ACS Sustainable Chemistry and Engineering, Jahrgang 6, Nr. 5, 07.05.2018, S. 6073–6083.
Publikation: Beitrag in Fachzeitschrift › Artikel › Forschung › 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, F.
AU - Bahnemann, D.W.
AU - Patrocinio, A.O.T.
N1 - Funding information: In Brazil, this work was supported by Fundaca? õ de Amparo à Pesquisa do Estado de Minas Gerais (FAPEMIG, PPM-00220-17), Conselho Nacional de Desenvolvimento Cientifí co e Tecnologicó (CNPq) and Coordenaca? õ de Aperfeico? amento de Pessoal de Nive? Superior (CAPES). The authors are also thankful to the Grupo de Materiais Inorganicos do Triangulo (GMIT), a research group supported by FAPEMIG (APQ-00330-14). A.O.T.P. is thankful to Alexander von Humboldt Foundation for the fellowship in Germany.
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 and Engineering
JF - ACS Sustainable Chemistry and Engineering
SN - 2168-0485
IS - 5
ER -