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1.
Nat Commun ; 12(1): 5092, 2021 08 24.
Artigo em Inglês | MEDLINE | ID: mdl-34429430

RESUMO

Development of a versatile, sustainable and efficient photosynthesis system that integrates intricate catalytic networks and energy modules at the same location is of considerable future value to energy transformation. In the present study, we develop a coenzyme-mediated supramolecular host-guest semibiological system that combines artificial and enzymatic catalysis for photocatalytic hydrogen evolution from alcohol dehydrogenation. This approach involves modification of the microenvironment of a dithiolene-embedded metal-organic cage to trap an organic dye and NADH molecule simultaneously, serving as a hydrogenase analogue to induce effective proton reduction inside the artificial host. This abiotic photocatalytic system is further embedded into the pocket of the alcohol dehydrogenase to couple enzymatic alcohol dehydrogenation. This host-guest approach allows in situ regeneration of NAD+/NADH couple to transfer protons and electrons between the two catalytic cycles, thereby paving a unique avenue for a synergic combination of abiotic and biotic synthetic sequences for photocatalytic fuel and chemical transformation.


Assuntos
Etanol/química , Fotossíntese/fisiologia , Luz Solar , Catálise , Corantes , Elétrons , Hidrogênio/química , Hidrogenase/química , Cinética , Ligantes , Simulação de Acoplamento Molecular
2.
Nat Commun ; 11(1): 2903, 2020 06 09.
Artigo em Inglês | MEDLINE | ID: mdl-32518257

RESUMO

Direct transfer of protons and electrons between two tandem reactions is still a great challenge, because overall reaction kinetics is seriously affected by diffusion rate of the proton and electron carriers. We herein report a host-guest supramolecular strategy based on the incorporation of NADH mimics onto the surface of a metal-organic capsule to encapsulate flavin analogues for catalytic biomimetic monooxygenations in conjunction with enzymes. Coupling an artificial catalysis and a natural enzymatic catalysis in the pocket of an enzyme, this host-guest catalyst-enzyme system allows direct proton and electron transport between two catalytic processes via NADH mimics for the monooxygenation of both cyclobutanones and thioethers. This host-guest approach, which involves the direct coupling of abiotic and biotic catalysts via a NADH-containing host, is quite promising compared to normal catalyst-enzyme systems, as it offers the key advantages of supramolecular catalysis in integrated chemical and biological synthetic sequences.


Assuntos
Biomimética , Oxigênio/química , Catálise , Domínio Catalítico , Cristalografia por Raios X , Transporte de Elétrons , Enzimas/química , Ligação de Hidrogênio , Íons , Cinética , Ligantes , NAD/química , Solventes/química , Zinco/química
3.
Chem Commun (Camb) ; 55(59): 8524-8527, 2019 Jul 18.
Artigo em Inglês | MEDLINE | ID: mdl-31257393

RESUMO

By incorporating 1,2-benzenedithiol as a chelator to construct cobalt dithiolene species, two negatively charged redox-active metal-organic hosts were obtained. By taking advantage of electrostatic interactions, cationic Ru-based photosensitizers were constrained to improve photoinduced electron transfer processes for efficient photocatalytic proton reduction.

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