Molecular Structural Design of Conjugated Microporous Poly(Benzooxadiazole) Networks for Enhanced Photocatalytic Activity with Visible Light

Wang, Zi Jun; Ghasimi, Saman; Landfester, Katharina; Zhang, Kai A. I.

doi:10.1002/adma.201502735

Cited by 256 publications

(165 citation statements)

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“…[28] Ar ecent study on CMPs demonstrated that the geometry design of the 3D polymer network structure played an crucial role in improving the photocatalytic efficiencies of the CMP photocatalysts. [29] Herein, we report am olecular design strategy used to finetune the VB and CB levels within as eries of conjugated microporousp oly(benzochalcogenadiazole) networks by altering the chalcogene moieties in the acceptor,t hat is, the benzochalcogenadiazole unit of the polymer backbone. We show that the Metal-free visible-light photocatalystso ffer ac lean, sustainable solution to many pressing environmental issues.…”

Section: Introductionmentioning

confidence: 99%

Conjugated Microporous Poly(Benzochalcogenadiazole)s for Photocatalytic Oxidative Coupling of Amines under Visible Light

et al. 2015

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Metal-free visible-light photocatalysts offer a clean, sustainable solution to many pressing environmental issues. Herein, we present a molecular design strategy to fine-tune the valence and conduction band levels of a series of conjugated microporous polymer networks based on poly(benzochalcogenadiazole) for heterogeneous photocatalysis. Enhanced photocatalytic efficiency was observed by altering the chalcogene moieties in the electron-accepting benzochalcogenadiazole unit of the polymer backbone structure. Photooxidative coupling of benzylamines was chosen as a model reaction. This design strategy leading to enhanced efficiency could potentially improve a wide range of photoredox reactions.

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Section: Introductionmentioning

confidence: 99%

Conjugated Microporous Poly(Benzochalcogenadiazole)s for Photocatalytic Oxidative Coupling of Amines under Visible Light

et al. 2015

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“…Moreover,w e show that regeneration of NAD + by the photocatalyst nanoparticles can oxidize am odel substrate, in conjunction with the enzymeg lycerol dehydrogenase. [10] This class of metal-free polymer photocatalyst has recently emerged as ap romising alternative to traditional metal-containing catalytic systems, as it has additional features such as high stabilitya nd reusability. [1] Synthetic biology uses artificially designed modules as systems that can reproduce simple cell-like activity and even mimic rudimentary cellular behavior.…”

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confidence: 99%

Polymer‐Based Module for NAD⁺ Regeneration with Visible Light

Chiyin

Silva

et al. 2019

ChemBioChem

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The regeneration of enzymatic cofactors by cell-free synthetic modulesi sak ey step towards producing ap urely synthetic cell. Herein, we demonstrate the regeneration of the enzyme cofactor NAD + by photo-oxidation of NADH under visible-light irradiation by using metal-free conjugated polymer nanoparticles. Encapsulation of the light-activen anoparticles in the lumen of polymeric vesicles produced af ully organic module able to regenerate NAD + in an enzyme-free system.T he polymer compartment conferred physical and chemicala utonomy to the module, allowing the regenerationo fN AD + to occur efficiently,e ven in harshc hemical environments. Moreover,w e show that regeneration of NAD + by the photocatalyst nanoparticles can oxidize am odel substrate, in conjunction with the enzymeg lycerol dehydrogenase. To ensure the longevity of the enzyme, we immobilizedi tw ithin ap rotectives ilica matrix;t his yieldede nzymatic silican anoparticles with enhanced long-term performance and compatibility with the NAD + -regeneration system.The immobilizationo re ncapsulationo ff unctional parts in artificial compartmentsi sapowerful way to create responsive autonomous objects, or functional modules, that displaylocalized input-output properties. [1] Synthetic biology uses artificially designed modules as systems that can reproduce simple cell-like activity and even mimic rudimentary cellular behavior. [2] Some examples include the cell-free synthesis of ATP, [3] cytoskeleton and microtubule reconstitution, [4] self-replication of giant vesicles, [5] and av ariety of compartmentalized biochemical reactions. [6] The cell-free regulation of nicotinamide adenine nucleotide (NAD) coenzymes has been an important target in photocatalysis and functional module design. [7] In cells, NAD coenzymes controlt he flow of electrons in numerous redox transformations involvingo xidoreductases and are key components for the conversion and storageo fe nergy during photosynthesis. Therefore, the ability to control the redox state of NAD in a functional module offers aw ay to simplify and optimize the use of numerous enzymatic redox transformations,m any of them with relevant synthetic applications. [8] Previous work in this area has focused mainly on creating NAD modules containing inorganic photocatalysts, such as TiO 2 and other metal-based nanoparticles, encapsulatedi nt he lumen of lipid vesicles or embedded in solid matrices. [9] To date, most developmentsi nt his area has focusedo nr egenerating NADH through the photocatalytic reduction of NAD + . These metal-based catalysts show high versatility,s electivity, and excellent photocatalytic properties, but they can also suffer from the need for mediators or excitation wavelengths in the UV region, whichc an be harmful to other components in the system.Herein, we report the designo fametal-free, polymer-based NAD module that regenerates NAD + through the nonenzymatic photocatalytic oxidation of NADH by using visiblel ight. Our photocatalyst consisted of conjugated microporous polymer nano...

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“…Covalent organic frameworks (COFs) are highly ordered two-or three-dimensional crystalline polymers [16,17]. These materials specially attract the interest in the area of photochemical hydrogen generation due to high surface area and tuneable pore size, which are essential criteria for heterogeneous catalysis [18].…”

Section: Covalent Organic Frameworkmentioning

confidence: 99%

Visible Light–Driven Hydrogen Production by Carbon based Polymeric Materials

Pati¹,

In²,

Tian³

2018

Visible-Light Photocatalysis of Carbon-Based Materials

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Converting solar energy into storable solar fuels such as H 2 from earth abundant sourcewater-is a nice approach to find the solution of energy crisis and environmental protection. There are two half reactions; first, water oxidation into oxygen and proton and followed by proton reduction led to H 2 evolution from water. After two decades of continuous attempts, there have been several efficient water oxidation photocatalysts introduced, whereas the proton reduction photocatalyst were relatively less explored. Major portion of reported photocatalysts for proton reduction are mainly derived from either noble metals or precious metals. Carbon-based organic photocatalysts have become attractive recently. These organic materials have several advantages like light weight, cheap, well-defined structure-property relationship and the most attractive one is better batch to batch reproducibility. Here, the reported organic photocatalysts and their performance are summarized which in fact help others to get an idea about ongoing progress in this area of research and to understand the basic designing principle for efficient photocatalysts for fuel production.

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Molecular Structural Design of Conjugated Microporous Poly(Benzooxadiazole) Networks for Enhanced Photocatalytic Activity with Visible Light

Cited by 256 publications

References 41 publications

Conjugated Microporous Poly(Benzochalcogenadiazole)s for Photocatalytic Oxidative Coupling of Amines under Visible Light

Conjugated Microporous Poly(Benzochalcogenadiazole)s for Photocatalytic Oxidative Coupling of Amines under Visible Light

Polymer‐Based Module for NAD⁺ Regeneration with Visible Light

Visible Light–Driven Hydrogen Production by Carbon based Polymeric Materials

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Molecular Structural Design of Conjugated Microporous Poly(Benzooxadiazole) Networks for Enhanced Photocatalytic Activity with Visible Light

Cited by 256 publications

References 41 publications

Conjugated Microporous Poly(Benzochalcogenadiazole)s for Photocatalytic Oxidative Coupling of Amines under Visible Light

Conjugated Microporous Poly(Benzochalcogenadiazole)s for Photocatalytic Oxidative Coupling of Amines under Visible Light

Polymer‐Based Module for NAD+ Regeneration with Visible Light

Visible Light–Driven Hydrogen Production by Carbon based Polymeric Materials

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Product

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Polymer‐Based Module for NAD⁺ Regeneration with Visible Light