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Photocatalytic CO2 Reduction by Re(I) Polypyridyl Complexes Immobilized on Niobates Nanoscrolls
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2018-03-22 00:00:00 , DOI: 10.1021/acssuschemeng.7b04713
Leandro A. Faustino 1 , Breno L. Souza 1 , Barbara N. Nunes 1 , Anh-Thu Duong 2 , Fabian Sieland 2 , Detlef W. Bahnemann 2, 3 , Antonio Otavio T. Patrocinio 1, 2
Affiliation  

Immobilization of Re(I) CO2 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 (TONCO) in DMF/TEOA of 1 was increased from 9 to 58, which is 20% higher than that observed on TiO2, 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 TONCO 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 CO2 reduction.

中文翻译:

固定在铌酸盐纳米卷上的Re(I)聚吡啶配合物对光催化CO 2的还原作用

Re(I)CO 2还原光催化剂固定在金属氧化物表面上是提高其稳定性和可回收性的有趣方法。在这项工作中,我们描述了两种Re(I)配合物(fac- [Re(NN)(CO)3(Cl)],NN = 4,4'-二羧酸-2,2'-联吡啶,己二酸酯纳米卷的表面上的1或5,6-dione-1,10-菲咯啉2)。吸附后,对CO产生的转换数(TON CO在DMF / TEOA)1从9增加到58,这比在TiO观察到的高20%2,是在没有任何敏化剂的可见光照射下,基于Re(I)的光催化剂的最高报告值。络合物2在可见光照射下在溶液中是无活性的,但是当固定在六铌酸盐纳米卷上时其TON CO为35。瞬态吸收光谱研究表明,己二酸酯导带电子的缓慢的背电子转移和较高的还原能力在光催化过程中起主要作用。结果提供了有关金属氧化物基质在基于Re(I)的分子系统中减少CO 2的作用的新见解。
更新日期:2018-03-22
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