Microfluidic chip-based one-step fabrication of an artificial photosystem I for photocatalytic cofactor regeneration

Huang, Xiaowen; Liu, Jian; Yang, Qingjing; Liu, Yang; Zhu, Yujiao; Li, Tenghao; Tsang, Yuen Hong; Zhang, Xuming

doi:10.1039/c6ra21390a

Cited by 31 publications

(33 citation statements)

References 45 publications

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“…Subsequently,t he solar energy is stored as the chemical "currency" NADH that is able to power various enzyme-mediated synthetic processes. [49] Herein, GDH, aN ADH-powered enzyme,w as taken as an example to catalyze the chemical transformation of a-ketoglutarate to lglutamate.T he photogenerated hole was consumed by TEOA, which was used as as acrificial electron donor. The NADH regeneration efficiency of TP-COF was evaluated by monitoring the characteristic 340 nm absorbance of NADH by using the UV/Vis spectrophotometer (Figure 3a).…”

Section: Angewandte Chemiementioning

confidence: 99%

Fully Conjugated Two‐Dimensional sp²‐Carbon Covalent Organic Frameworks as Artificial Photosystem I with High Efficiency

et al. 2019

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The synthesis of fully conjugated sp 2 -carbon covalent organic frameworks (COF) is extremely challenging given the difficulty of the formation of very stable carbon-carbon double bonds (-C=C-). Here,w er eport the successful preparation of a2 DC OF (TP-COF) based on triazine as central planar units bridged by sp 2 -carbon linkers through the -C = Ccondensation reaction. High-resolution-transmission electron microscopy( HRTEM) clearly confirmed the tessellated hexagonal pore structure with ap ore center-to-center distance of 2nm. Powder X-rayd iffraction (PXRD) together with structural simulations revealed an AA stacking mode of the obtained layered structure.T P-COF turned out to be an excellent semiconductor material with aL UMO energy of À3.23 eV and aband gap of 2.36 eV.Excitingly,this novel sp 2carbon conjugated TP-COF exhibited unprecedented coenzyme regeneration efficiency and can significantly boost the coenzyme-assisted synthesis of l-glutamate to arecord-breaking 97 %yield within 12 minutes.Long-range p-conjugated two-dimensional (2D) materials have received considerable attention in recent years and present ar ange of unique advantages over traditional polymeric materials. [1][2][3][4][5][6][7] In particular, the topological arrangement of aromatic units propagating in two spatial directions equips them with superior (photo-)electronic and magnetic properties. [8][9][10] However,t he delicate control over specific arrangements of functional units to obtain highly ordered 2D materials is still ag reat challenge. [11][12][13][14] Covalent organic frameworks (COFs) take advantage of the structural selfhealing properties stemming from dynamic covalent bond formation. [15][16][17][18][19][20][21] This advancement has made it possible to synthesize well-defined 2D structures with diverse functionalities.A mong all synthetic strategies of COFs,t he most frequently used dynamic covalent-bond-formations trategies are the Schiff base condensation reaction and the boronate ester bond formation. Despite the fact that the extended pconjugation can propagate through the -N = C-double bonds in the Schiff base structure,t he imine-linkage displays relatively poor stability and weak electron delocalization. To overcome this limitation, researchers have been actively exploring new reactions to construct fully conjugated COFs with an optimal electron delocalization. [22][23][24][25][26][27][28] However,examples of fully conjugated imine-free COFs with sp 2 -carbon double bond structures are still rare because it is extremely difficult to form -C = C-bonds via reversible coupling reactions and simultaneously gain the desired conjugation as well as the refined crystallinity within the COF structure.Recently, Jiang et al. and Feng et al. successfully constructed conjugated 2D COFs bearing -C = C-linkage by using Knoevenagel polycondensation. [29][30][31][32] Ther eported sp 2 -carbon linked 2D COFs were demonstrated to have excellent electrochemical and charge-transfer properties.Thee nhanced electron delocalization of sp 2...

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Section: Angewandte Chemiementioning

confidence: 99%

Fully Conjugated Two‐Dimensional sp²‐Carbon Covalent Organic Frameworks as Artificial Photosystem I with High Efficiency

et al. 2019

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“…Scheme b illustrates the proposed catalytic process of TP‐COF acting as a central photocatalyst in the artificial PSI system: TP‐COF collects solar energy in the form of electrons excited by light, followed by the regeneration of NADH from NAD + through the electron mediator [Cp*Rh(bpy)(H)] + ( M , in abbreviation). Subsequently, the solar energy is stored as the chemical “currency” NADH that is able to power various enzyme‐mediated synthetic processes . Herein, GDH, a NADH‐powered enzyme, was taken as an example to catalyze the chemical transformation of α‐ketoglutarate to l ‐glutamate.…”

Section: Methodsmentioning

confidence: 99%

Fully Conjugated Two‐Dimensional sp²‐Carbon Covalent Organic Frameworks as Artificial Photosystem I with High Efficiency

Zhao

Liu

et al. 2019

Angewandte Chemie

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The synthesis of fully conjugated sp2‐carbon covalent organic frameworks (COF) is extremely challenging given the difficulty of the formation of very stable carbon‐carbon double bonds (‐C=C‐). Here, we report the successful preparation of a 2D COF (TP‐COF) based on triazine as central planar units bridged by sp2‐carbon linkers through the ‐C=C‐ condensation reaction. High‐resolution‐transmission electron microscopy (HRTEM) clearly confirmed the tessellated hexagonal pore structure with a pore center‐to‐center distance of 2 nm. Powder X‐ray diffraction (PXRD) together with structural simulations revealed an AA stacking mode of the obtained layered structure. TP‐COF turned out to be an excellent semiconductor material with a LUMO energy of −3.23 eV and a band gap of 2.36 eV. Excitingly, this novel sp2‐carbon conjugated TP‐COF exhibited unprecedented coenzyme regeneration efficiency and can significantly boost the coenzyme‐assisted synthesis of l‐glutamate to a record‐breaking 97 % yield within 12 minutes.

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“…Optofluidic reactors have intrinsic merits, such as fine flow control, large surface-to-volume ratio, and direct delivery of light to the reaction surface, making them natural photoreactors for photocatalysis [7][8][9][10]. Some studies showed microfluidic methods for achieving good degradation efficiency of polluted water [11][12][13][14].…”

Section: Introductionmentioning

confidence: 99%

“…In this work, we reported a paper-based photocatalyst immobilization method to solve the "coffee ring" problem. A mesoporous graphite carbon nitride (mpg-C 3 N 4 ) was chosen to be the photocatalyst, because it has been proven to be a good photocatalyst material in both others' works and our previous work [9,[20][21][22][23][24][25]. Experiments on photo-degradation of methylene blue were adopted to test the effect of both coffee ring and paper-based methods.…”

Section: Introductionmentioning

confidence: 99%

Paper-based Photocatalysts Immobilization without Coffee Ring Effect for Photocatalytic Water Purification

Lin

Huang

et al. 2020

Micromachines

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Photocatalytic water purification is important for the degradation of organic pollutants, attracting intensive interests. Photocatalysts are preferred to be immobilized on a substrate in order to reduce the laborious separation and recycling steps. To get uniform irradiation, the photocatalysts are preferred to be even/uniform on the substrate without aggregation. Generally, the “coffee ring effect” occurs on the substrate during solvent evaporation, unfortunately resulting in the aggregation of the photocatalysts. This aggregation inevitably blocks the exposure of active sites, reactant exchange, and light absorption. Here, we reported a paper-based photocatalyst immobilization method to solve the “coffee ring” problem. We also used a “drop reactor” to achieve good photocatalytic efficiency with the advantages of large surface area, short diffusion lengths, simple operation, and uniform light absorption. Compared with the coffee ring type, the paper-based method showed higher water purification efficiency, indicating its potential application value in the future.

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Microfluidic chip-based one-step fabrication of an artificial photosystem I for photocatalytic cofactor regeneration

Abstract: We report a one-step strategy for the formation of an artificial photosystem I, with an enhanced coenzyme regeneration rate.

Cited by 31 publications

References 45 publications

Fully Conjugated Two‐Dimensional sp²‐Carbon Covalent Organic Frameworks as Artificial Photosystem I with High Efficiency

Fully Conjugated Two‐Dimensional sp²‐Carbon Covalent Organic Frameworks as Artificial Photosystem I with High Efficiency

Fully Conjugated Two‐Dimensional sp²‐Carbon Covalent Organic Frameworks as Artificial Photosystem I with High Efficiency

Paper-based Photocatalysts Immobilization without Coffee Ring Effect for Photocatalytic Water Purification

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Microfluidic chip-based one-step fabrication of an artificial photosystem I for photocatalytic cofactor regeneration

Abstract: We report a one-step strategy for the formation of an artificial photosystem I, with an enhanced coenzyme regeneration rate.

Cited by 31 publications

References 45 publications

Fully Conjugated Two‐Dimensional sp2‐Carbon Covalent Organic Frameworks as Artificial Photosystem I with High Efficiency

Fully Conjugated Two‐Dimensional sp2‐Carbon Covalent Organic Frameworks as Artificial Photosystem I with High Efficiency

Fully Conjugated Two‐Dimensional sp2‐Carbon Covalent Organic Frameworks as Artificial Photosystem I with High Efficiency

Paper-based Photocatalysts Immobilization without Coffee Ring Effect for Photocatalytic Water Purification

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Fully Conjugated Two‐Dimensional sp²‐Carbon Covalent Organic Frameworks as Artificial Photosystem I with High Efficiency

Fully Conjugated Two‐Dimensional sp²‐Carbon Covalent Organic Frameworks as Artificial Photosystem I with High Efficiency

Fully Conjugated Two‐Dimensional sp²‐Carbon Covalent Organic Frameworks as Artificial Photosystem I with High Efficiency