Synergy Between Metal and Molecular Catalysts for (Photo)electrocatalytic 1,4-NADH Regeneration

The Journal of Physical Chemistry C, Journal Year: 2024, Volume and Issue: 128(14), P. 5927 - 5933

Published: April 2, 2024

(Photo)electrocatalytic NAD+ reduction provides a promising approach for 1,4-NADH regeneration, but it remains challenging to achieve both high activity and selectivity. Here, we found prominent synergetic effects between various metals (Cu, Fe, Co, Ni) Rh-based complexes (M M') electrocatalytic reduction, promoting the selectivity simultaneously. Typically, normalized of Cu M coupled system is 15.6 times that M, while alone shows negligible at same potential. Meanwhile, enhanced from 63.3% as 95.3% system. We transfer hydrogen atoms metal electrode complex accelerates formation metal-hydride active species, which catalyzes regioselective production 1,4-NADH. This work universal strategy coupling proton-reduction electrocatalysts molecular catalysts efficient (photo)electrocatalytic 1,4-NAD(P)H regeneration.

Language: Английский

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Photocatalytic Regeneration of Reactive Cofactors with InP Quantum Dots for the Continuous Chemical Synthesis

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(9), P. 6740 - 6748

Published: April 16, 2024

The shuttling of redox-active nicotinamide cofactors between the light and dark cycles is key to continuous production biomass in photosynthesis. replication such processes artificial photosynthetic systems demands fast photoregeneration as well simultaneous integration these into cycle. Here, we report design an system for butanol via constant consumption cofactors, powered by indium phosphide quantum dot (InP QD) photocatalyst alcohol dehydrogenase (ADH) enzyme, respectively. A strong electrostatic attraction oppositely charged InP QDs electron mediators significantly enhanced charge extraction utilization processes, enabling a (∼30 min, with turn over frequency ∼1333 h–1), quantitative (>99%), selective enzymatically active These photoregenerated were further coupled cycle trigger ADH oxidoreductase enzyme butanol, sequential light–dark cycles. amount produced under was higher than stoichiometric limit, proving regeneration cycles, Thus, proper QD-based photocatalytic enzymatic led effective seen

Language: Английский

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Turning the band alignment of carbon dots for visible-light-driven enzymatic asymmetric reduction of aromatic ketone

International Journal of Biological Macromolecules, Journal Year: 2025, Volume and Issue: 295, P. 139444 - 139444

Published: Jan. 5, 2025

Language: Английский

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Bifunctional sludge-derived redox carbon dots with photoelectron storage and delivery properties for ammonia production by photosensitized Shewanella oneidensis MR-1

Bioresource Technology, Journal Year: 2024, Volume and Issue: unknown, P. 131539 - 131539

Published: Sept. 1, 2024

Language: Английский

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Synergistic integration of polysulfobetaine brush-grafted porphyrinic covalent organic frameworks with native enzymes for electrolyte-sensitive aerobic photobiocatalysis

Journal of Materials Chemistry A, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

COFs with polysulfobetaine brushes (TpDh-P) could efficiently regenerate NAD + from NADH under red light. The polysulfobetaines capture and neutralize ROS, protecting native enzymes, modulate oxidation electrolyte-sensitivity.

Language: Английский

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Highly efficient photoenzymatic CO2 reduction via integrated structural design of porphyrin covalent organic framework on Ti3C2T (MXene)

Separation and Purification Technology, Journal Year: 2025, Volume and Issue: unknown, P. 132943 - 132943

Published: April 1, 2025

Language: Английский

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N-Doped Carbon Dots as Electrolytes to Boost Photoelectrochemical Water Oxidation for the Photo-assisted Zinc-Air Battery

Chemical Communications, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

BiVO 4 photoanodes in an N-doped carbon dot solution can dynamically assemble into p–n heterojunctions, achieving enhanced charge separation for water oxidation that significantly reduces the voltage gap photo-assisted zinc–air batteries.

Language: Английский

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Modular design and integrated construction of photosynthetic biohybrids for solar-driven CO2 conversion to chemicals

Coordination Chemistry Reviews, Journal Year: 2025, Volume and Issue: 540, P. 216774 - 216774

Published: May 11, 2025

Language: Английский

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C–C-Coupled Two-Dimensional Conjugated Polymer Nanosheets as Highly Efficient Photocatalysts for NADH Regeneration and Biocatalytic Artificial Photosynthesis

ACS Materials Letters, Journal Year: 2024, Volume and Issue: 6(9), P. 4012 - 4018

Published: July 31, 2024

Two-dimensional (2D) polymers, due to their abundance of active sites and fast charge separation transfer efficiency, have been regarded as ideal candidates for high-performance photocatalysts. However, current 2D polymers suffer from drawbacks harsh preparation conditions, limited thermal/photostability, poor structural diversity. In this work, the C–C-coupled polymer 2D@COP-DBTS was synthesized via isopropanol-assisted exfoliation corresponding layerlike linear polymer. The obtained demonstrates a competitive conversion 60.8% in NADH regeneration. DFT calculations reveals that photocatalyst has strong affinities reactive substrates, guaranteeing quick electron prominent catalytic efficiency. When situ regeneration is combined with formate dehydrogenase, an extremely high amount (572.92 mmol, turnover frequency (TOF) 63500 mmol gcat–1 h–1) accumulated. addition, 0.0351 l-glutamate (TOF 0.488 also 2D@COP-DBTS/glutamate dehydrogenase mixture, indicating feasibility production polymer/enzyme-coupled system.

Language: Английский

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Electron-mediator-free efficient photocatalytic regeneration of coenzyme NAD(P)H via direct electron transfer using ultrathin Bi₂MoO₆ nanosheets

Green Chemistry, Journal Year: 2024, Volume and Issue: 27(3), P. 623 - 632

Published: Nov. 12, 2024

The direct electron transfer mechanism of single-layer Bi 2 MoO 6 ultrathin nanosheets promotes the efficient regeneration photocatalytic coenzyme NAD(P)H.

Language: Английский

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