Spencer Michael George, Sacchi Marco, Allam Jeremy, Silva S R P
Quantum Biology Doctoral Training Centre, University of Surrey, GuildfordGU2 7XH, U.K.
Advanced Technology Institute, University of Surrey, GuildfordGU2 7XH, U.K.
ACS Omega. 2022 Nov 1;7(45):41304-41313. doi: 10.1021/acsomega.2c05065. eCollection 2022 Nov 15.
Porphyrin-nanocarbon systems were used to generate a photocatalyst for the control of rhodamine B and rhodamine 6G photodegradation. Carboxylic functionalized multi-walled carbon nanotubes (-MWCNTs) were decorated by two different porphyrin moieties: 5-(4-aminophenyl)-10,15,20-(triphenyl)porphyrin (a-TPP) with an amine linker and 5-(4-carboxyphenyl)-10,15,20-(triphenyl)porphyrin (c-TPP) with a carboxyl linker to the -MWCNT, respectively, with their photocatalyst performances investigated. The optical properties of the mixed nanocomposite materials were investigated to reveal the intrinsic energy levels and mechanisms of degradation. The charge-transfer states of the -MWCNTs were directly correlated with the performance of the complexes as well as the affinity of the porphyrin moiety to the -MWCNT anchor, thus extending our understanding of energy-transfer kinetics in porphyrin-CNT systems. Both a-TPP and c-TPP -MWCNT complexes offered improved photocatalytic performance for both RhB and Rh6G compared to the reference -MWCNTs and both porphyrins in isolated form. The photocatalytic performance improved with higher concentration of -MWCNTs in the complexed sample, indicating the presence of greater numbers of -H/-OH groups necessary to more efficient photodegradation. The large presence of the -H/-OH group in the complexes was expected and was related to the functionalization of the -MWCNTs needed for high porphyrin attachment. However, the photocatalytic efficiency was affected at higher -MWCNT concentrations due to the decomposition of the porphyrins and changes to the size of the CNT agglomerates, thus reducing the surface area of the reactant. These findings demonstrate a system that displays solar-based degradation of rhodamine moieties that are on par, or an improvement to, state-of-the-art organic systems.
卟啉-纳米碳体系被用于制备一种光催化剂,以控制罗丹明B和罗丹明6G的光降解。羧基官能化的多壁碳纳米管(-MWCNTs)用两种不同的卟啉部分进行修饰:分别通过胺连接基与-MWCNT相连的5-(4-氨基苯基)-10,15,20-(三苯基)卟啉(a-TPP)和通过羧基连接基与-MWCNT相连的5-(4-羧基苯基)-10,15,20-(三苯基)卟啉(c-TPP),并对它们的光催化剂性能进行了研究。对混合纳米复合材料的光学性质进行了研究,以揭示其本征能级和降解机制。-MWCNTs的电荷转移态与配合物的性能以及卟啉部分与-MWCNT锚定基团的亲和力直接相关,从而扩展了我们对卟啉-CNT体系中能量转移动力学的理解。与参考-MWCNTs以及分离形式的两种卟啉相比,a-TPP和c-TPP-MWCNT配合物对RhB和Rh6G均表现出更好的光催化性能。配合物样品中-MWCNTs浓度越高,光催化性能越好,这表明存在更多数量的-H/-OH基团,这些基团对于更有效的光降解是必需的。配合物中大量存在-H/-OH基团是预期的,并且与高卟啉附着所需的-MWCNTs的功能化有关。然而,在较高的-MWCNT浓度下,由于卟啉的分解和CNT团聚体尺寸的变化,光催化效率受到影响,从而降低了反应物的表面积。这些发现证明了一种基于太阳能降解罗丹明部分的体系,该体系与现有有机体系相当或有所改进。