The ability of P(V) phthalocyanines (Pcs) for efficient singlet oxygen (SO) generation was demonstrated for the first time by the example of unsubstituted and α- and β-octabutoxy-substituted P(V)Pcs with hydroxy, methoxy and phenoxy ligands in the apical positions of the octahedral P centre. Variation of substituents in Pc ring and P(V) axial ligands allows careful tuning of photophysical and photochemical properties. Indeed, a combination of BuO groups in the β-positions of the Pc ring and PhO groups as axial ligands provides significant SO generation quantum yields up to 90%; meanwhile, the values of SO generation quantum yields for others investigated compounds vary from 27 to 55%. All the complexes, except α-substituted P(V)Pc, demonstrate fluorescence with moderate quantum yields (10-16%). The introduction of electron-donating butoxy groups, especially in the α-position, increases the photostability of P(V)Pcs. Moreover, it has been shown in the example of β-BuO-substituted P(V) that the photostability depends on the nature of axial ligands and increases in the next row: OPh < OMe < OH. The presence of oxy/hydroxy axial ligands on the P(V) atom makes it possible to switch the photochemical and photophysical properties of P(V)Pcs by changing the acidity of the media.
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http://dx.doi.org/10.3390/molecules28031094 | DOI Listing |
J Comput Chem
January 2025
Department of Mechanical Engineering, Texas Tech University, Lubbock, Texas, USA.
Multi-copper oxidases (MCOs) are enzymes of significant interest in biotechnology due to their efficient catalysis of oxygen reduction to water, making them valuable in sustainable energy production and bio-electrochemical applications. This study employs time-dependent density functional theory (TDDFT) to investigate the electronic structure and spectroscopic properties of the Type 1 (T1) copper site in Azurin, which serves as a model for similar sites in MCOs. Four model complexes of varying complexity were derived from the T1 site, including 3 three-coordinate models and 1 four-coordinate model with axial methionine ligation, to explore the impact of molecular branches and axial coordination.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
Qingdao University of Science and Technology, college of materials science and engineering, Zhengzhou Road 53#, 266042, Qingdao, CHINA.
The catalytic efficiency of natural enzymes depends on the precise electronic interactions between active centers and cofactors within a three-dimensional (3D) structure. Single-atom nanozymes (SAzymes) attempt to mimic this structure by modifying metal active sites with molecular ligands. However, SAzymes struggle to match the catalytic efficiency of natural enzymes due to constraints in active site proximity, quantity, and the inability to simulate electron transfer processes driven by internal electronic structures of natural enzymes.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
Nagoya University: Nagoya Daigaku, Department of Chemistry, Graduate School of Science, Furo-cho, Chikusa-ku, 464-8602, Nagoya, JAPAN.
A new series of metal-organic nanotubes was constructed through one-dimensional assembly using molecular triangles or molecular squares composed of paddlewheel dirhodium complexes and bidentate axial ligands. The metal-organic nanotubes were significantly different from conventional solid metal-organic framework (MOF) motifs. They exhibit good solubility owing to the branched side chains at their periphery and demonstrate high orientation capabilities in thin films owing to their anisotropic structure.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
Lanzhou University, College of chemistry and chemical engineering, Lanzhou, CHINA.
Imperfections in metal halide perovskites, such as those induced by light exposure or thermal stress, compromise device performance and stability. A key challenge is immobilizing volatile iodine produced by iodide oxidation and regenerating impurities like elemental lead and iodine. Here, we address this by integrating a redox-active supramolecular assembly of nickel octaethylporphyrin into perovskite film, functioning as both an immobilizer and redox shuttle.
View Article and Find Full Text PDFAdv Mater
December 2024
Tianjin Key Lab for Rare Earth Materials and Applications, Center for Rare Earth and Inorganic Functional Materials, School of Materials Science and Engineering, National Institute for Advanced Materials, Nankai University, Tianjin, 300350, China.
Currently, there are still obstacles to rationally designing the ligand fields to activate rare-earth (RE) elements with satisfactory intrinsic electrocatalytic reactivity. Herein, axial coordination strategies and nanostructure design are applied for the construction of La single atoms (La-Cl SAs/NHPC) with satisfactory oxygen reduction reaction (ORR) activity. The nontrivial LaNCl motifs configuration and the hierarchical porous carbon substrate that facilitates maximized metal atom utilization ensure high half-wave potential (0.
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