Single cobalt atom anchored on carbon nitride with well-defined active sites for photo-enzyme catalysis

Wang, Xinyang; Hu, Wenjuan; Yang, Lijun; Liu, Jian

doi:10.1016/j.nanoen.2020.104750

Cited by 90 publications

(78 citation statements)

References 35 publications

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“…Inspirited by mono‐nuclear metalloenzyme and its metal–N–C‐based active sites, recently, Liu et al made an updated attempt to anchor Co single atom onto the 2D g‐C 3 N 4 nanosheets through crystal‐assisted confinement pyrolysis. [ 70 ] The obtained nanoflake material, named Co 1 /CN, showed very high efficiency for photochemical NADH regeneration. Spherical aberration corrected high‐angle annular dark field‐scanning transmission electron microscopy and X‐ray absorption fine structure spectroscopy indicated the atomic dispersion of Co atoms among its structure (Figure 7B).…”

Section: G‐c3n4‐based Photocatalystsmentioning

confidence: 99%

Bioinspired NADH Regeneration Based on Conjugated Photocatalytic Systems

et al. 2020

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Cofactors, such as nicotinamide adenine dinucleotide (NADH) or its phosphorylated derivative (NADPH), are playing essential roles in redox enzymatic catalysis because of their indispensable roles as biological hydride sources. However, due to its stoichiometric consumption, economic and efficient regeneration for NADH is of great importance for both in vivo and in vitro applications. Inspired by natural photosynthesis, photocatalytic NADH regeneration has drawn increasing attention, resulting from its mild reaction conditions and excellent biocompatibility with enzymes. Currently, various heterogeneous photocatalysts, such as conjugated small molecules, graphitic carbon nitride, carbon‐based materials, and organic polymers, are reported as promising candidates for photocatalytic NADH regeneration due to their outstanding advantages of low cost, high chemical stability, limited toxicity, and molecularly tunable optoelectronic properties. Herein, the key advances of conjugated photocatalytic systems for NADH regeneration are summarized, accompanied with their strengths and limitations. Finally, an outlook is tentatively attempted about the further developments of conjugated polymers–based NADH regeneration as well as integrated photoenzymatic catalysis.

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Section: G‐c3n4‐based Photocatalystsmentioning

confidence: 99%

Bioinspired NADH Regeneration Based on Conjugated Photocatalytic Systems

et al. 2020

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“…NAD(P)H is a cofactor in enzymatic reduction and the regeneration of NAD(P)H is essential for the practical application of reductive enzymes. [25][26][27][28][29][30][31][32][33][34] According to previous reports, HPB could be excited by visible light to form HPB* with reductive potential more negative than [Cp*Rh(bpy)H 2 O] 2þ , thus, it is possible for nTp-TTA/POM-x to drive the photocatalytic NAD þ reduction with cascade electron relay on the basis of energy diagram ( Figure 3A). [14] The photocatalytic NADH regeneration was used as a model reaction to test the catalytic performance of nTp-TTA/POM-x with [Cp*Rh(bpy)H 2 O] 2þ as electron mediator and TEOA as hole sacrificial reagent using Xe lamp (λ ≥ 420 nm) ( Table 1).…”

Section: Pw 12 O 40mentioning

confidence: 99%

Fabrication of NanoCOF/Polyoxometallate Composites for Photocatalytic NADH Regeneration via Cascade Electron Relay

Liu

Wang

et al. 2020

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Covalent organic frameworks (COFs) are novel crystalline polymers with a unique designable feature at molecular level via weaving chemistry. [1,2] 2D COFs with a variety of ordered π systems provide a desirable platform for developing visible-light responsive photocatalysts for solar energy storage and conversion and have already shown potential applications in photocatalytic water splitting, CO 2 reduction, and organic synthesis. [3-11] In regardless of suitable bandgap and band structure, COFs in most cases afforded very low quantum efficiency in photocatalysis. Considering that the separation and transportation of the photogenerated charges is the key step in photosynthesis, the fast extraction of photogenerated electrons confined in π orbitals of COFs is very important for efficient photosynthesis. In natural photosynthesis, the photogenerated holes and electrons are spacially separated in PS II (catalyze H 2 O oxidation to H þ and O 2) and PS I (photoenzymatic reduction of NAD(P) þ to NAD(P)H). [12] The excited electrons are transferred from PS II to PS I through multistep with the assistance of mediators to inhibit the charge recombination. Inspired by natural photosynthesis, the utilization of an electron mediator is an efficient strategy to enhance the charge separation of COFs for efficient artificial photosynthesis. A good electron mediator should possess redox potentials alignment with the band structure of COFs and the properties of easy electron acception and donation. Polyoxometallates (POMs) could be reduced to heteropolyblue (HPB) via accepting electrons. [13] More interestingly, HPB can be excited by visible and near-infrared light at about 700 nm via intervalence charge transfer to regain the energy that is lost in the reduction process and the excited HPB* facilely denotes electrons to electron acceptors, e.g., H þ , O 2 , and metal complexes to drive the photocatalytic reductive reactions. Previous studies showed that the photocatalytic activity of semiconductors, e.g., C 3 N 4 , TiO 2 were greatly promoted by coupling with POM in photocatalytic CO 2 reduction, water oxidation, and organic pollutants removal due to the enhanced charge separation. [14-17] Though POM is a good candidate as electron mediator and electron storage tank, the coupling of COFs and POM has not been reported yet for artificial photosynthesis as far as we know, possibly related with the difficulty in hybridizing of the POM and COFs. Herein, we report the fabrication of nanoCOF/POM composites for the first time by simply mixing the cetyltrimethylammonium bromide/sodium dodecyl sulfate (CTAB/SDS, molar ratio of 97/3) micelle stabilized nanoCOF colloid solution with Na 3 PW 12 O 40 (Scheme 1). NanoCOF/POM composites possess visible-light responsive properties inherited from nanoTp-TTA COF (synthesized using 1,3,5-triformylphloroglucinol and 4,4 0 ,4 00-(1,3,5-triazine-2,4,6-triyl)trianiline as precursors). The transfer of photogenerated electrons from nanoTp-TTA COF to

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“…However, the high cost of NADH and the stoichiometric consumption of NADH in the oxidoreductase catalysis entail the economic, environment-friendly methods for NADH regeneration. [4][5][6] Continuing efforts have been devoted to in situ NADH regeneration from oxidized counterpart by enzymatic, [1,6] chemical, [7] electrochemical, [8] and photochemical [9] routes.…”

Section: Introductionmentioning

confidence: 99%

“…However, the high cost of NADH and the stoichiometric consumption of NADH in the oxidoreductase catalysis entail the economic, environment‐friendly methods for NADH regeneration. [ 4–6 ] Continuing efforts have been devoted to in situ NADH regeneration from oxidized counterpart by enzymatic, [ 1,6 ] chemical, [ 7 ] electrochemical, [ 8 ] and photochemical [ 9 ] routes. Light‐driven NADH regeneration by semiconductor photocatalysis is very promising, and a lot of photocatalysts, such as g‐C 3 N 4 , [ 6 ] metal–organic frameworks, [ 10,11 ] and covalent organic frameworks, [ 12,13 ] have been reported for fulfilling such purpose.…”

Section: Introductionmentioning

confidence: 99%

“…Photoenzyme catalysis of artificial photosynthesis is one of the promising strategies for accomplishing the goal. [1][2][3] In the enzyme involved artificial photosynthesis, one of the key steps is nicotinamide adenine dinucleotide (NADH) regeneration, which serves as hydrogen donor in the redox process. However, the high cost of NADH and the stoichiometric consumption of NADH in the oxidoreductase catalysis entail the economic, environment-friendly methods for NADH regeneration.…”

Section: Introductionmentioning

confidence: 99%

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Investigation of Water‐Stable Perovskite DMASnI_xBr_3−x for Photoenzyme Catalysis in Aqueous Solution

Lin

Xiao

et al. 2020

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The impressive optoelectronic performances of hybrid perovskites have attracted enormous interests. However, the moisture sensitivity of these materials hampers their practical applications. Herein, the lead‐free perovskites of DMASnIxBr3−x (DMA = CH3NH2CH3+) crystals as photocatalysts for nicotinamide adenine dinucleotide (NADH) regeneration in aqueous solution are engineered. The very high NADH yield (≈100%) is achieved for all the DMASnIxBr3−x crystals with tunable bandgaps, which is further coupled with formate dehydrogenase for the production of 320 μM formic acid from CO2. The density functional theory (DFT) calculations further shed light on the intrinsic water‐stable mechanism of DMASnI3 perovskite, which is ascribed to the higher water surface adsorption energy, the higher water osmotic energy barrier, and the smaller intralayer spacing inside DMASnI3 structures by comparing with Pb‐based counterpart. The work can provide new prospects for designing water‐stable hybrid perovskites and further broaden their photocatalytic and optoelectronic applications.

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Single cobalt atom anchored on carbon nitride with well-defined active sites for photo-enzyme catalysis

Cited by 90 publications

References 35 publications

Bioinspired NADH Regeneration Based on Conjugated Photocatalytic Systems

Bioinspired NADH Regeneration Based on Conjugated Photocatalytic Systems

Fabrication of NanoCOF/Polyoxometallate Composites for Photocatalytic NADH Regeneration via Cascade Electron Relay

Investigation of Water‐Stable Perovskite DMASnI_xBr_3−x for Photoenzyme Catalysis in Aqueous Solution

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Single cobalt atom anchored on carbon nitride with well-defined active sites for photo-enzyme catalysis

Cited by 90 publications

References 35 publications

Bioinspired NADH Regeneration Based on Conjugated Photocatalytic Systems

Bioinspired NADH Regeneration Based on Conjugated Photocatalytic Systems

Fabrication of NanoCOF/Polyoxometallate Composites for Photocatalytic NADH Regeneration via Cascade Electron Relay

Investigation of Water‐Stable Perovskite DMASnIxBr3−x for Photoenzyme Catalysis in Aqueous Solution

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Investigation of Water‐Stable Perovskite DMASnI_xBr_3−x for Photoenzyme Catalysis in Aqueous Solution