scholarly journals Controlling the Optical and Catalytic Properties of Artificial Metalloenzyme Photocatalysts Using Chemogenetic Engineering

2021 ◽  
Author(s):  
Yasmine S. Zubi ◽  
Bingqing Liu ◽  
Yifan Gu ◽  
Dipankar Sahoo ◽  
Jared Lewis
Keyword(s):  
Energy Transfer ◽  
Visible Light ◽  
Catalytic Properties ◽  
Photophysical Properties ◽  
Organic Transformations ◽  
Polypyridyl Complexes ◽  
Transfer Processes ◽  
Pyridine Ligands ◽  
Artificial Metalloenzymes ◽  
Artificial Metalloenzyme

Visible light photocatalysis enables a broad range of organic transformations that proceed via single electron or energy transfer. Metal polypyridyl complexes are among the most commonly employed visible light photocatalysts. The photophysical properties of these complexes have been extensively studied and can be tuned by modifying the substituents on the pyridine ligands. On the other hand, ligand modifications that enable substrate binding to control reaction selectivity remain rare. Given the exquisite control that enzymes exert over electron and energy transfer processes in nature, we envisioned that artificial metalloenzymes (ArMs) created by incorporating Ru(II) polypyridyl complexes into a suitable protein scaffold could provide a means to control photocatalyst properties. This study describes approaches to create covalent and non-covalent ArMs from a variety of Ru(II) polypyridyl cofactors and a prolyl oligopeptidase scaffold. A panel of ArMs with enhanced photophysical properties were engineered, and the nature of the scaffold/cofactor interactions in these systems was investigated. These ArMs provided higher yields and rates than Ru(Bpy)32+ for the reductive cyclization of dienones and the [2+2] photocycloaddition between C-cinnamoyl imidazole and 4-methoxystyrene, suggesting that protein scaffolds could provide a means to improve the efficiency of visible light photocatalysts.

scholarly journals Controlling the Optical and Catalytic Properties of Artificial Metalloenzyme Photocatalysts Using Chemogenetic Engineering

2022 ◽  
Author(s):  
Yasmine S Zubi ◽  
Bingqing Liu ◽  
Yifan Gu ◽  
Dipankar Sahoo ◽  
Jared C Lewis
Keyword(s):  
Energy Transfer ◽  
Visible Light ◽  
Catalytic Properties ◽  
Single Electron ◽  
Visible Light Photocatalysis ◽  
Organic Transformations ◽  
Polypyridyl Complexes ◽  
Artificial Metalloenzyme

Visible light photocatalysis enables a broad range of organic transformations that proceed via single electron or energy transfer. Metal polypyridyl complexes are among the most commonly employed visible light photocatalysts....

Intramolecular energy transfer and photoisomerization in stilbene dendrimers

2017 ◽  
Vol 95 (9) ◽  
pp. 1013-1023 ◽  
Author(s):  
Masahiro Taima ◽  
Yuka Ishida ◽  
Tatsuo Arai
Keyword(s):  
Energy Transfer ◽  
Energy Harvesting ◽  
Photophysical Properties ◽  
Intersystem Crossing ◽  
Intramolecular Energy Transfer ◽  
The Core ◽  
Transfer Processes ◽  
Trans Isomerization ◽  
Photophysical Processes ◽  
In Cis

Stilbene dendrimers with energy harvesting chromophores, such as naphthalene and benzophenone, have been prepared and their photochemical and photophysical properties have been examined. These dendrimers underwent trans–cis mutual photoisomerization on excitation of the core stilbene or the peripheral naphthalene and benzophenone chromophores through several energy transfer processes, and photophysical processes such as intersystem crossing finally resulted in cis-trans isomerization of the core stilbene.

Synergistic combination of visible-light photo-catalytic electron and energy transfer facilitating multicomponent synthesis of β-functionalized α,α-diarylethylamines

2019 ◽  
Vol 55 (45) ◽  
pp. 6405-6408 ◽  
Author(s):  
Yanan Wu ◽  
Yipin Zhang ◽  
Mingjie Jiang ◽  
Xunqing Dong ◽  
Hitesh B. Jalani ◽  
...  
Keyword(s):  
Energy Transfer ◽  
Visible Light ◽  
Multicomponent Synthesis ◽  
Transfer Processes ◽  
Synthetic Strategy ◽  
Synergistic Combination

A synthetic strategy which takes advantage of the synergistic combination of electron and energy transfer processes using only one photocatalyst has been developed for the multicomponent synthesis of the α,α-diarylalkylamine skeleton.

scholarly journals Pyrene-based metal–organic framework NU-1000 photocatalysed atom-transfer radical addition for iodoperfluoroalkylation and (Z)-selective perfluoroalkylation of olefins by visible-light irradiation

RSC Advances ◽  
2018 ◽  
Vol 8 (57) ◽  
pp. 32610-32620 ◽  
Author(s):  
Tiexin Zhang ◽  
Pengfang Wang ◽  
Zirui Gao ◽  
Yang An ◽  
Cheng He ◽  
...  
Keyword(s):  
Energy Transfer ◽  
Visible Light ◽  
Visible Light Irradiation ◽  
Metal Organic Framework ◽  
Radical Addition ◽  
Light Irradiation ◽  
Atom Transfer ◽  
Transfer Processes ◽  
Atom Transfer Radical Addition ◽  
Metal Organic

Iodoperfluoroalkylation or (Z)-selective perfluoroalkylation of olefins is mediated through energy transfer processes by using pyrene-based MOF NU-1000 under visible-light irradiation.

Synthesis, electrochemistry, spectroscopy and photophysical properties of a series of meso-phenylpyridylporphyrins with one to four pyridyl rings coordinated to [Ru(bipy)2Cl]+ groups

2002 ◽  
Vol 06 (01) ◽  
pp. 33-42 ◽  
Author(s):  
Fábio M. Engelmann ◽  
Pellegrino Losco ◽  
Herbert Winnischofer ◽  
Koiti Araki ◽  
Henrique E. Toma
Keyword(s):  
Energy Transfer ◽  
Quantum Yield ◽  
Electrochemical Behavior ◽  
Fluorescence Quantum Yield ◽  
Photophysical Properties ◽  
Intramolecular Energy Transfer ◽  
Porphyrin Ring ◽  
Transfer Processes ◽  
Redox Pair ◽  
Mlct State

A series of meso-phenylpyridylporphyrins and their respective supermolecular species obtained by the coordination of [ Ru ( bipy )2 Cl ]+ groups to the pyridyl substituents was synthesized and characterized. Their spectroscopic and electrochemical behavior were similar to that observed for the meso-tetra(4-pyridyl)porphyrin derivative, but the redox potential of the Ru (III/II) redox pair was about 70 mV more negative. The porphyrin centered fluorescence quantum yield exhibited a linear decrease as a function of the number of pyridyl substituents on the porphyrin ring. Efficient intramolecular energy transfer processes from the 3 MLCT state of the ruthenium complexes to the porphyrin center were observed at 77K in ethanol glass.

Application of singlet energy transfer in triplet state formation: broadband visible light-absorbing triplet photosensitizers, molecular structure design, related photophysics and applications

2015 ◽  
Vol 3 (34) ◽  
pp. 8735-8759 ◽  
Author(s):  
Xiaoneng Cui ◽  
Caishun Zhang ◽  
Kejing Xu ◽  
Jianzhang Zhao
Keyword(s):  
Molecular Structure ◽  
Energy Transfer ◽  
Visible Light ◽  
Triplet State ◽  
State Formation ◽  
Photophysical Properties ◽  
Structure Design

The molecular structure design, photophysical properties and the application of the broadband visible light-absorbing triplet photosensitizers are summarized.

Luminescence Properties and Energy Transfer Processes in Fluorescent and Phosphorescent Tris(Phenylquinoxaline)

1999 ◽  
Vol 598 ◽  
Author(s):  
Sylke Blumstengel ◽  
Elio Colabella ◽  
Riccardo Tubino ◽  
M. Jandke ◽  
P. Strohriegl
Keyword(s):  
Energy Transfer ◽  
Electron Transport ◽  
Photophysical Properties ◽  
Red Light ◽  
Dipole Interaction ◽  
Transport Layer ◽  
Electron Transport Layer ◽  
Efficient Energy Transfer ◽  
Guest Molecules ◽  
Transfer Processes

ABSTRACTWe have studied the photophysical properties and energy transfer processes in tris(phenylquinoxalines ) (TPQ). TPQs emit blue fluorescence with a maximum at 2.9 eV as well as green phosphorescence at 2.2 eV. When doped with a phosphorescent dye efficient energy transfer takes place from the excited singlet and triplet state of the TPQ host to the guest molecules. The mechanism of energy transfer can be understood in the frame of Förster's theory of dipole-dipole interaction. Besides the interesting photophysical properties, TPQs are also very efficient electron transport materials. Red light-emitting diodes utilizing doped TPQ as emitter and electron transport layer have been prepared and electroluminescence properties investigated.

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