Synergetic Effect of Heterojunction and Sulfur Vacancy on ZnIn2S4/CeO2 to Enhance the Photocatalytic Performance of 5‐Hydroxymethylfurfural into 2,5‐Diformylfuran DOI
Yue Wang, Huai Liu,

Tianping Lv

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 18, 2024

Abstract The efficient separation of photocarriers and facile generation superoxide radicals are crucial for enhancing the performance photocatalysts in selectively photo‐oxidizing 5‐hydroxymethylfurfural (HMF) into 2,5‐diformylfuran (DFF). Herein, a ZnIn 2 S 4 /CeO composite with S‐scheme heterojunction sulfur vacancies (S V ) is successfully developed through one‐step hydrothermal method. optimal catalyst ‐ZnIn exhibits excellent catalytic activity 100% conversion HMF 96.1% selectivity DFF 80 min under ambient conditions, production rate up to 952.6 µmol g −1 h . Intriguingly, remains significant even when concentration increased from 8 100 mм. Experimental theoretical investigations discover that synergistic effect contribute activation oxygen, which facilitate radicals, thus boosting oxidation reactions.

Language: Английский

Tracking Charge Dynamics in a Silver Single-Atom Catalyst During the Light-Driven Oxidation of Benzyl Alcohol to Benzaldehyde DOI Creative Commons

Areti Moutsiou,

Andrea Olivati,

Luis A. Cipriano

et al.

ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 5601 - 5613

Published: March 21, 2025

Understanding charge transfer in light-driven processes is crucial for optimizing the efficiency and performance of a photocatalyst, as directly influences separation migration photogenerated carriers determines overall reaction rate product formation. However, achieving this understanding remains challenging context single-atom photocatalysis. This study addresses gap investigates an Ag-based catalyst (Ag1@CNx) photocatalytic oxidation benzyl alcohol to benzaldehyde. Comprehensive characterization was conducted using battery diffractive, textural, spectroscopic, microscopic methods, confirming crystallinity, porosity, elemental composition, atomic dispersion silver atoms. material displayed efficient selective Density functional theory calculations were used rationalize structure elucidate mechanism, unveiling role holes lowering energy barriers. Time-resolved transient spectroscopic studies monitor dynamics charges reaction, revealing lifetimes behaviors excited states within catalyst. Specifically, introduction atoms led significant enhancement state lifetime, which favors hole-transfer presence alcohol. indicated that photoexcited effectively transferred reactant, thereby driving process oxygen. These mechanistic insights are pivotal spectroscopically elucidating mechanism can be practically applied design photocatalysts more rationally, targeting materials combine both rapid reductive quenching metal.

Language: Английский

Citations

0
Semiartificial Photoelectrochemistry for CO2-Mediated Enantioselective Organic Synthesis DOI Creative Commons
Tessel Bouwens, Samuel J. Cobb, Celine W. S. Yeung

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: April 15, 2025

Photoelectrochemical (PEC) cells are under intensive development for the synthesis of solar fuels, but CO2 reduction typically only results in simple building blocks such as HCOO-. Here, we demonstrate that CO2-converting PEC can drive integrated enzymatic domino catalysis to produce chiral organic molecules by using CO2/HCOO- a sustainable redox couple. First, establish semiartificial electrode consisting three enzymes co-immobilized on high surface area based carbon felt covered mesoporous indium tin oxide (ITO) coating. When applying mild cathodic potential (-0.25 V vs reversible hydrogen (RHE)), is reduced HCOO- W-formate dehydrogenase (FDHNvH) from Nitratidesulfovibrio vulgaris Hildenborough, which then enables NAD+ NADH an NAD+-cofactor-dependent formate Candida boidinii (FDHCB). Subsequently, alcohol (ADH) uses generated cycling reduce acetophenone 1-phenylethanol good enantiomeric excess (93%) and conversion yields (38%). Depending specific ADH (ADHS or ADHR), either (S)- (R)-1-phenylethanol be synthesized at pH 6 20 °C. To illustrate energy utilization, integrate nanoconfined with platform semiconductor photocathode allow enantioselective (at +0.8 RHE) fuel device. This proof-of-principle demonstration shows concepts devices artificial photosynthesis readily translated precise biocatalysis, including production light.

Language: Английский

Citations

0
Research and significance of Electroenzymatic conversion of carbon dioxide DOI Creative Commons

Xiaowen Yu

Applied and Computational Engineering, Journal Year: 2025, Volume and Issue: 123(1), P. 248 - 254

Published: Jan. 7, 2025

The concentration of carbon dioxide in the atmosphere is increasing, leading to a rising demand for its conversion. It growing (CO2) conversion that drives research into various innovative technologies. There are many existing methods catalytic dioxide, such as electrocatalysis and chemical catalysis. However, each technology has own sets advantages disadvantages. Among these, electro-catalytic combining enzymatic catalysis electrocatalysis, stands out potential provide efficient clean solutions. Writing relevant literature review meaningful this context. This article commences by examining electron transfer mechanisms between NAD(P)H-independent NAD(P)H-dependent redox enzymes electrodes, with aim exploring efficiencies electrocatalytic systems In addition, an discussed, which notable successfully developing new electro-enzyme coupling pathway. innovation enhances high activity NADH enzyme, providing pathway environmentally friendly utilization. process capable synthesizing high-value chemicals while minimizing environmental impact.

Language: Английский

Citations

0
Recent Advances in Desulfurization of VOSCs: Multiple Catalysts and Coupling Enzymes DOI
Rui Tian, Shiying Fan, Xinyong Li

et al.

ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 4331 - 4349

Published: Feb. 26, 2025

Language: Английский

Citations

0
Rh-functionalized Imino-pyridine Covalent Organic Framework Assembled on Ti3C2Tx (MXene) for Efficient NADH Regeneration and Photoenzymatic CO2 Reduction DOI

Hailong Zheng,

Zhipeng Huang,

Ping Wei

et al.

ACS Sustainable Chemistry & Engineering, Journal Year: 2025, Volume and Issue: unknown

Published: March 4, 2025

Nicotinamide adenine dinucleotide (NADH) regeneration is crucial for sustainable enzymatic CO2 reduction. In this study, Ti3C2Tx (MXene) and [Cp*Rh(bpy)(H2O)]2+ (labeled as [Cp*Rh]) were sequentially assembled onto imino-pyridine structured covalent organic frameworks (TD-COF) to construct Rh@TDM photocatalysts with dual cocatalyst. The photoelectrochemical tests temperature-dependent photoluminescence spectra suggest that the synergistic effect of incorporation [Cp*Rh] immobilization enables a reduction in exciton binding energy promotes carrier transfer. Consequently, optimized [email protected] photocatalyst achieves 95.0% NADH yield, significantly higher than TD-COF free (32.7%). Additionally, modification strategy applied also enhances selectivity 1,4-NADH. Therefore, turnover frequency 1,4-NADH 1.06 h–1, which 7.1 times (0.15 h–1). Subsequently, photoenzymatic cascade catalytic system, obtained remarkable formate generation rate 2137.7 μmol g–1 h–1. This work not only provides novel example using COF containing an structure immobilize but reveals synergetic MXene facilitates These findings offer new insights opportunities design application artificial systems

Language: Английский

Citations

0
Photocatalytic Reduction of Levulinic Acid to γ-Valerolactone on Non-noble Metal Bi2S3 Catalysts under Mild Reaction Conditions DOI

Wenjing An,

Weiping Yang,

Shi Li-qing

et al.

ACS Sustainable Chemistry & Engineering, Journal Year: 2025, Volume and Issue: unknown

Published: March 25, 2025

Language: Английский

Citations

0
Embedding Tandem Built‐in Electric Fields within Hollow Architectures for Enhanced Photothermal Effect in Alcohol Oxidation Coupled with H2 Production DOI

Yi‐Wen Han,

Yuxin Zhang, Lei Ye

et al.

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: April 1, 2025

Abstract Rationally designing nanostructures based on a comprehensive understanding of structure‐property relationships is instrumental in enhancing the photothermal effect. Here, general two‐stage morphology‐structure‐control strategy presented to construct tandem built‐in electric fields (BIEFs) embedded hollow bifunctional photocatalysts (Sv‐chalcogenide nanocage/NiCo 2 S 4 heterojunctions, Sv represents sulfur vacancies, chalcogenides include ZnIn , CdS, CdIn ). This involves fabricating polyhedral cages via constraint epitaxy and embedding BIEFs (consisting intra‐component inter‐component BIEF) within nanocages through defect‐mediated heterocomponent anchorage. The resulting nanoreactors synergize multilight scattering/reflection with directional charge‐transfer boost photocarrier dynamics by stimulating plentiful carrier generation driving continuous localization delocalized‐electron transportation. Subsequently, localized surface plasmon resonance (LSPR)‐induced photogenerated electron excitation continuously collaborates intrinsic for hot generation, thus improving Heterojunctions efficient regulation optimize pivotal intermediate adsorption/activation selective alcohol oxidation coupled H evolution, delivering unprecedented reactivity broad substrate compatibility. study provides programmable framework structurally architectures, elucidating substantial impact morphology‐structure control molecular catalytic behavior.

Language: Английский

Citations

0
Modern organic transformations: heterogeneous thermocatalysis or photocatalysis? DOI
Ning Zhang, Wanbing Gong, Yujie Xiong

et al.

Chemical Society Reviews, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

This review presents the working principles, advantages and disadvantages of heterogeneous thermo- photocatalysis in organic transformations, outlines related applications advancements photocatalytic transformations.

Language: Английский

Citations

0
Highly efficient photoenzymatic CO2 reduction dominated by 2D/2D MXene/C3N5 heterostructured artificial photosynthesis platform DOI
Fengyi Yang,

Pengye Zhang,

Jiafu Qu

et al.

Journal of Colloid and Interface Science, Journal Year: 2024, Volume and Issue: 678, P. 1121 - 1131

Published: Aug. 22, 2024

Language: Английский

Citations

3
Synergetic Effect of Heterojunction and Sulfur Vacancy on ZnIn2S4/CeO2 to Enhance the Photocatalytic Performance of 5‐Hydroxymethylfurfural into 2,5‐Diformylfuran DOI
Yue Wang, Huai Liu,

Tianping Lv

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 18, 2024

Abstract The efficient separation of photocarriers and facile generation superoxide radicals are crucial for enhancing the performance photocatalysts in selectively photo‐oxidizing 5‐hydroxymethylfurfural (HMF) into 2,5‐diformylfuran (DFF). Herein, a ZnIn 2 S 4 /CeO composite with S‐scheme heterojunction sulfur vacancies (S V ) is successfully developed through one‐step hydrothermal method. optimal catalyst ‐ZnIn exhibits excellent catalytic activity 100% conversion HMF 96.1% selectivity DFF 80 min under ambient conditions, production rate up to 952.6 µmol g −1 h . Intriguingly, remains significant even when concentration increased from 8 100 mм. Experimental theoretical investigations discover that synergistic effect contribute activation oxygen, which facilitate radicals, thus boosting oxidation reactions.

Language: Английский

Citations

2