Photocatalysis coupling hydrogen peroxide synthesis and in-situ radical transform for tetracycline degradation

Xu, Zaixiang; Gong, Si-Yan; Ji, Wenkai; Zhang, Shijie; Bao, Zhikang; Zhao, Zijiang; Zhong, Xing; Hu, Zhong‐Ting; Wang, Jianguo

doi:10.1016/j.cej.2022.137009

Cited by 20 publications

(4 citation statements)

References 71 publications

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“…To gain a deeper insight into the regeneration kinetics, an electrostatic interaction-controlled reaction process was proposed, as depicted in Figure a. Given the confirmed incorporation of potassium ions into the carbon nitride matrix, when ionCN is dispersed in a solution, the surface K ions tend to dissolve in water, forming colloidal particles with negative ζ-potential . Compared to the original ionCN-0.2, the catalyst recovered after M adsorption in solution, showing a significant decrease in the K signal (Figure S17a).…”

Section: Resultsmentioning

confidence: 99%

“…Given the confirmed incorporation of potassium ions into the carbon nitride matrix, when ionCN is dispersed in a solution, the surface K ions tend to dissolve in water, forming colloidal particles with negative ζpotential. 16 Compared to the original ionCN-0.2, the catalyst recovered after M adsorption in solution, showing a significant decrease in the K signal (Figure S17a). The extent of K ion incorporation into the surface of carbon nitride directly correlates with the negative potential in the solution, as confirmed by ζ-potential testing.…”

Section: Kinetic Analysis and Mechanism Investigationmentioning

confidence: 97%

“…Enhancing the intermolecular electrostatic interactions is a possible solution. Previous studies have addressed the selectivity challenges by introducing a metal complex, [Cp*Rh(bpy)H 2 O] 2+ (denoted as M ), into the reaction system as an electron and proton mediator, to achieve nearly 100% production of 1,4-NAD(P)H. − Therefore, when using this reaction system containing M , the reaction system involves molecules with different charges, including NAD with a negative charge, M with a positive charge, and carbon nitride exhibits tunable negative ζ-potential . Thus, it is a feasible method to adjust the electrostatic interaction between different molecules in the system.…”

Section: Introductionmentioning

confidence: 99%

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Regeneration of NAD(P)H and its Analogues by Photocatalysis with Ionized Carbon Nitride

Xu,

Zhou,

Chen

et al. 2024

ACS Catal.

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The regeneration of NAD(P)H and its analogues is crucial for biocatalytic processes. However, despite the efficiency of enzymatic catalysis in regenerating NAD(P)H, the sustainability of enzymes is often compromised, particularly under extreme catalytic conditions. Moreover, artificial cofactors may present advantages in certain reactions due to their stability and versatility, yet the substrate specificity of enzymes poses significant challenges to their regeneration through the enzymatic method. Therefore, it is imperative to develop a highly stable regeneration method that can be adapted to both natural and artificial cofactors. In this work, employing potassium-ion-doped carbon nitride (ionCN-0.2) as a catalyst not only achieves high-efficiency photocatalytic regeneration of NAD(P)H, comparable to that of glucose dehydrogenase (GDH), but also a remarkable ability to regenerate nicotinamide analogues. This enhanced performance stems from the tunable negative ζ-potential, which effectively adsorbs the positively charged [Cp*Rh(bpy)H 2 O] 2+ mediator, resulting in enhanced regeneration kinetics of the nicotinamide moiety. The catalyst demonstrates superior performance compared to the reported systems; the optimal regeneration rate reaches 0.55 mmol L −1 g cat −1 min −1 and approaches enzymatic regeneration efficiency. Expanding the reaction conditions to a wider temperature and pH range also confirms the effectiveness and sufficient stability of this photocatalytic system, offering a promising strategy for stable cofactor regeneration in biocatalytic processes.

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Section: Resultsmentioning

confidence: 99%

Section: Kinetic Analysis and Mechanism Investigationmentioning

confidence: 97%

Section: Introductionmentioning

confidence: 99%

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Regeneration of NAD(P)H and its Analogues by Photocatalysis with Ionized Carbon Nitride

Xu,

Zhou,

Chen

et al. 2024

ACS Catal.

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“…Solar-driven H 2 O 2 production offers several distinct advantages over the traditional anthraquinone method, such as high efficiency, low cost, and less pollution . On the other hand, solar-driven H 2 O 2 production also could be used for organic pollutant degradation . Generally, the photocatalytic generation of H 2 O 2 involves O 2 reduction reaction (O 2 RR) or H 2 O oxidation reaction (WOR) .…”

Section: Introductionmentioning

confidence: 99%

Photocatalytic Hydrogen Peroxide Production by a Mixed Ligand-Functionalized Uranyl–Organic Framework

Wang,

Li,

Wei

et al. 2024

ACS Omega

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Hydrogen peroxide (H 2 O 2 ) production driven by solar energy has received enormous attention due to its high efficiency, low cost, and environmental friendliness characteristics. Searching for new photocatalytic materials for H 2 O 2 production is one of the most important targets. In this work, a new three-dimensional (3D) uranyl−organic framework material was constructed with mixed ligands via a solvothermal reaction and used for photocatalytic H 2 O 2 production. The mixed ligand strategy not only benefits the construction of a 3D uranyl−organic framework but also introduces strong photon absorption groups into the framework. The thiophene and pyridine rings in the framework enhance photon absorption and carrier transfer. In addition, with the assistance of the hydrogen abstraction reaction of uranyl centers, the H 2 O 2 production rate reaches 345 μmol h −1 g −1 . This study provides a new blueprint for exploring the artificial photosynthesis of H 2 O 2 through uranium-based metal−organic frameworks.

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Assembly of Amorphizing Porous Bimetallic Metal‐Organic Frameworks Spheres with Zn─O─Fe Cluster and Coordination Deficiency via Ligand Competition for Efficient Electro‐Fenton Catalysis

Xu,

Teng,

et al. 2024

Adv Funct Materials

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Electro‐Fenton process stands out as a highly promising approach for generating reactive oxygen‐containing radicals to address the escalating issue of environmental pollution. However, the long‐term goal of application necessitates ongoing pursuit of high‐quality catalysts with both sufficient activity and stability. Herein, a general route is reported for large‐scale synthesis of amorphizing porous bimetallic metal‐organic framework (MOF) spheres with Zn─O─Fe structure and coordination deficiency through facile and low‐cost synthesis of ligand competition. Assisted by a coordination modulator, deprotonation of terephthalic acid is accelerated and rapid synthesis of amorphous bimetallic MOF spheres is successfully achieved at room temperature. As inactive metal Zn is introduced into metal clusters of MOFs, the cycling efficiency of Fe3+/Fe2+ is improved and a secondary building unit of Zn─O─Fe is constructed, greatly accelerating electron conduction rate. Compared to crystalline spindle cMIL‐88B(Fe2Zn) by traditional solvothermal route, amorphous aMIL‐88B(Fe2Zn) has a unique spherical porous structure with larger surface area, higher conductivity, and more exposed active sites. Endowed with unique textural and surface chemistry, aMIL‐88B(Fe2Zn) exhibits superior catalytic activity in the degradation of refractory organic pollutants. The progress offers a feasible way to rational design of iron‐based hybrid MOF materials with tunable structures and enhance properties for various applications.

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Photocatalysis coupling hydrogen peroxide synthesis and in-situ radical transform for tetracycline degradation

Cited by 20 publications

References 71 publications

Regeneration of NAD(P)H and its Analogues by Photocatalysis with Ionized Carbon Nitride

Regeneration of NAD(P)H and its Analogues by Photocatalysis with Ionized Carbon Nitride

Photocatalytic Hydrogen Peroxide Production by a Mixed Ligand-Functionalized Uranyl–Organic Framework

Assembly of Amorphizing Porous Bimetallic Metal‐Organic Frameworks Spheres with Zn─O─Fe Cluster and Coordination Deficiency via Ligand Competition for Efficient Electro‐Fenton Catalysis

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