Cd Single Atom as an Electron Mediator in an S‐Scheme Heterojunction for Artificial Photosynthesis of H₂O₂

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

Published: Feb. 13, 2025

Abstract Developing conductor‐mediated S‐scheme heterojunction photocatalysts imitating natural photosynthetic systems emerges as a promising approach to hydrogen peroxide (H 2 O ) production. However, achieving precise coupling between two semiconductors with charge shuttle and modulating the interfacial interactions still remain significant bottleneck. Herein, we propose catalyst architecture Cd single atom mediated formed by interfacing CdS TiO nanoparticles. This exhibits an H production rate high 60.33 µmol g −1 min under UV–vis light irradiation, which is attributed efficient transport at interface of thanks S‐scheme. In‐situ X‐ray photoelectron spectroscopy (XPS) electron spin resonance (ESR) spin‐trapping tests confirm transfer route. Femtosecond transient absorption (fs‐TA) other ex‐situ characterizations further corroborate across interface. work offers new perspective on constructing atoms heterojunctions enhance photocatalytic performance.

Language: Английский

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Asymmetric CuS₁N₄ as Axial Polarization Site Trigger Rapid Charge Transport Channels for Boosting Photosynthesis of Ammonia

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

Published: Jan. 10, 2025

Abstract Effective photogenerated charge transfer and utilization have been regarded as a critical factor for achieving highly efficient photosynthesis of ammonia. However, the lacks necessary driving force in many catalysts limit directly transfer. In this work, Cu porphyrin‐based monoatomic layer (PML‐Cu) is modified on face‐centered cubic structured defective CdIn 2 S 4 via solvothermal reaction, with strong coupled interfacial Cu─S bond constructed. Owing to formation axial CuS 1 N polarization site, local asymmetric configuration can be created between PML‐Cu form potential difference, inducing rapid transport from bond. Meantime, electron‐enriched site beneficial stabilization * NHOH intermediate state, then lowering NHO→ rate‐limiting step energy barrier. Benefiting these features, PML‐Cu/CdIn exhibit good NH 3 generation rate 1979.0 µmol g −1 h , apparent quantum efficiency 8.56% at 380 nm 7.40% 450 nm, respectively. This work provides an accessible pathway designing coupling boost photocatalysis.

Language: Английский

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Modulating Yeager Adsorption Configuration of O₂ Through Cd Doping in Zn₃In₂S₆ for Photosynthesis of H₂O₂

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

Published: Oct. 14, 2024

Abstract The photocatalytic oxygen reduction reaction (ORR) is a key pathway for producing hydrogen peroxide (H 2 O ). While most previous studies have focused on the two‐step 2e − ORR process, one‐step two‐electron route offers thermodynamic and kinetic advantages that can significantly enhance activity selectivity. In this study, photocatalyst design reported by incorporating cadmium into vacancy‐rich Zn 3 S 6 (Cd‐S V /ZIS). This catalyst enables H production via process without use of sacrificial agents, achieving high yield 39.42 µmol g −1 min under UV–vis light irradiation, outperforming ZIS‐based photocatalysts. Theoretical simulations experimental results demonstrate Cd doping improves carrier kinetics catalyst, broadens its absorption range, promotes Yeager adsorption configuration , leading to highly active selective generation. study provides insights efficient photocatalysts production.

Language: Английский

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Novel cocatalyst MnCo2S4 based on Zn3In2S6 for enhanced photocatalytic hydrogen production and ranitidine degradation

Journal of Alloys and Compounds, Journal Year: 2024, Volume and Issue: 1004, P. 175941 - 175941

Published: Aug. 10, 2024

Language: Английский

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Twin S‐Scheme Heterojunction ZnO/UiO‐66‐NH₂@ZnIn₂S₄ Rhombic Octahedra for Efficient Photocatalytic H₂ Evolution

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

Published: March 3, 2025

Abstract Amid increasing fossil energy scarcity, a key solution is using solar to split water into hydrogen (H 2 ). However, single photocatalysts face limitations of low utilization rate and rapid carrier recombination, so constructing novel composite promising solution. Here, ZnO/UiO‐66‐NH @ZnIn S 4 (ZUN@ZIS) catalyst with twin S‐scheme heterojunction constructed for the first time, in which ZnIn (ZIS) nanosheets are grown situ on surface (ZUN) rhombic octahedra. Under irradiation visible light without help any co‐catalyst, H evolution prepared ZUN@ZIS‐20 5.05 mmol g −1 h , 3.7, 2.1 46 times higher than that ZIS, UiO‐66‐NH /ZIS (UN/ZIS) ZUN, respectively. Moreover, synergistic effect resulting ZUN@ZIS facilitates provision efficient channels carrier/mass transfer ensures structural stability. Various experimental characterizations theoretical calculations confirm by ZUN ZIS can facilitate easy separation photogenerated carriers. This study has developed new idea multi‐heterojunction photocatalysts, provided valuable reference development photocatalysis technology.

Language: Английский

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Molecularly Tunable Donor–Acceptor Integrated Carbon Nitride for Sunlight‐Driven H₂O₂ Synthesis: Mechanism and Performance Insights

Small, Journal Year: 2025, Volume and Issue: unknown

Published: March 16, 2025

Abstract Graphite phase carbon nitride (CN) emerges as a promising catalyst for sunlight‐driven H 2 O synthesis owing to its merits of stable physicochemical properties, distinctive electronic structure, adjustable bandgap, etc., yet poor charge behavior, especially high carrier recombination and low migration rate, limit photocatalytic activity. Herein, molecularly tunable donor‐acceptor (D‐A) integrated CN is fabricated via cytosine doping combined with molten salt‐assisted calcination. The utilized achieves the highest H₂O₂ yield 8.07 mmol g −1 h , which exceeds initial by factor 40.4, surpassing numerous reported CN‐based photocatalysts. Series characterizations/tests (e.g., transient absorption, steady‐state SPV spectra, KPFM) theoretical calculations HOMO/LUMO, adsorption energy) confirm that incorporation K + ‐C≡N pyrimidine ring disrupts symmetry establishes D‐A significantly augmenting separation photogenerated charges. capture experiment rotating disk electrode test affirm two‐step single electron oxygen reduction pathway occurs in process synthesis. This work offers novel approaches profound revelations development

Language: Английский

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Assembling Heterojunction Zn_0.75Cd_0.25Se–CdS Quantum Dot Aerogels for Enhanced Photocatalytic CO₂ Methanation

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

Published: March 16, 2025

Abstract Heterojunction engineering into quantum dot (QD) assemblies has emerged as an effective approach to optimize photocatalytic systems through enhanced charge separation and extended light‐harvesting capabilities. Nevertheless, fabricating QD heterojunctions with robust interfacial coupling remains challenging due stringent morphological lattice matching constraints. Here, a class of atomically fused ZnCdSe–CdS aerogels tailored heterointerfaces is reported for superior solar‐driven CO 2 reduction. The high compatibility between ZnCdSe CdS enables seamless heterojunction formation strong electronic coupling, while strategic Cd doping in ZnSe extends optical absorption maximize solar utilization. optimized exhibit exceptional photoreduction activity, achieving CH 4 production rate 240 µmol g⁻ 1 h⁻ 87% selectivity apparent yield (AQY) 1.2% under visible light. Combined spectroscopic characterization density functional theory (DFT) simulations elucidate that suppressed carrier recombination at the engineered interface serves key mechanistic determinant performance. This work establishes universal platform designing interfacial‐engineered aerogels, advancing their applicability high‐efficiency fuel generation systems.

Language: Английский

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Construction of Hierarchical 2D-3D@3D Zn3In2S6@CdS Photocatalyst for Boosting Degradation of an Azo Dye

Molecules, Journal Year: 2025, Volume and Issue: 30(7), P. 1409 - 1409

Published: March 21, 2025

Herein, flower-like Zn3In2S6 (ZIS3) crystallites were grown onto acorn leaf-like CdS assemblies via a two-step hydrothermal approach. Under visible light irradiation, the Zn3In2S6-enriched heterostructures demonstrated an enhanced azo-dye degradation rate, with majority of organic analyte (Orange G) being degraded within 60 min. In contrast, CdS-enriched hybrids showed poor photocatalytic performance. The optimized hybrid containing nominal content 4 wt% was characterized by various physicochemical techniques, such as XRD, SEM, XPS and Raman. analysis that electron density around Zn sites in slightly increased, implying certain charge migration pattern. Complementary information from scavenging experiments suggested hydroxy radicals not exclusive transient responsible for oxidative azo-dye. This research provides new about development metal chalcogenide-based efficient pollutant degradation.

Language: Английский

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Fabrication of In-doped CdSe/Zn3In2S6 type II heterojunction composite for efficient photocatalytic hydrogen evolution

Separation and Purification Technology, Journal Year: 2024, Volume and Issue: unknown, P. 129907 - 129907

Published: Sept. 1, 2024

Language: Английский

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ZnIn2S4 nanosheets with tunable dual vacancies for efficient sacrificial-agent-free H2O2 photosynthesis

Inorganic Chemistry Frontiers, Journal Year: 2024, Volume and Issue: 11(23), P. 8383 - 8391

Published: Jan. 1, 2024

ZnIn 2 S 4 nanosheets with tunable concentration of dual vacancies were prepared. Introducing effectively promotes photocarrier separation, facilitates O adsorption, and inhibits H decomposition by increasing hydrophilicity.

Language: Английский

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