Simultaneously Utilizing Excited Holes and Electrons for Piezoelectric-Enhanced Photoproduction of H₂O₂ from S-Scheme 2D S-Doped VO_x/g-C₃N₄ Nanostructures

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(22), P. 29421 - 29438

Published: May 22, 2024

2D/2D step-scheme (S-scheme) piezo-photocatalysts for the production of fine chemicals, such as hydrogen peroxide (H2O2), have attracted significant attention global scientists owing to efficiency in utilizing surface piezoelectric effects from 2D materials overcome rapid charge recombination photocatalytic processes. In this research, we reported fabrication S-doped VOx deposited on g-C3N4 produce H2O2 via piezo-photocatalytic process with high yields at 20.19 mmol g–1 h–1, which was 1.75 and 4.87 times higher than that solely piezo-catalytic generation. The finding pointed out adding sulfur (S) can help improve catalytic outcomes by modifying electronic properties pristine VOx. addition, when coupled g-C3N4, presence S limits formation graphene VOx/g-C3N4 composites, causing shielding pushing cascade reactions toward water generation materials. Besides, research also sheds light transport between S-VOx under irradiation how composites work trigger H2O2. composite systems enhances transfer two semiconductors strengthening internal electric fields (IEF) drive electrons moving one direction, demonstrated density functional theory (DFT) calculations. Moreover, significantly relies reduction oxygen generate oxygenic radical species sites. Meanwhile, provides oxidative sites oxidize molecules directly or indirectly O2, will further participate final products. This study confirms validation S-scheme piezo-photocatalysts, thus encouraging developing heterojunction efficiency, be used practical conditions.

Language: Английский

---

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

---

Assembling Graphene Quantum Dots on Aminophenol-formaldehyde Resin towards Efficient Artificial Photocatalytic Hydrogen Peroxide Synthesis

Journal of Materials Chemistry A, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

Assembling GQDs on APF resin could improve separation and transfer efficiency of photogenerated electrons for H 2 O synthesis.

Language: Английский

---

Piezoelectrical Hydrogel Containing Cationic Vacancies Bismuth Sulfide with Enhanced Sonodynamic/Nanozyme Activity for Synergistic Killing Bacteria and Boosting Osteoblast Differentiation

Journal of Materials Chemistry B, Journal Year: 2025, Volume and Issue: 13(10), P. 3420 - 3436

Published: Jan. 1, 2025

A piezoelectric nanozyme is a novel biomaterial with the integration of piezoelectricity and activity that has capability killing bacteria promoting cell responses under mechanical stimulus exhibits great prospects in tissue regeneration. Herein, bismuth sulfide (BS) cationic vacancies (VBS) was synthesized, which enhanced activities compared BS. Moreover, hydrogel VBS phenylboronic acid grafted sodium alginate-arginine (VBS-PSA) prepared. Triggered by ultrasound (US) high power (>0.5 W cm-2), VBS-PSA produces large amount reactive oxygen species (ROS) through both piezoelectricity-enhanced sonodynamic efficiency peroxidase-like (POD-like) activity, thereby displaying powerful antibacterial capability. However, low-power US (≤0.5 effect generates electrical signals significantly stimulate osteoblast (proliferation differentiation) enhance catalase-like (CAT-like) for scavengers ROS generation oxygen, creating favorable microenvironment growth. Our study presents strategy to apply hydrogels enhancing synergistically kill responses. The would have potential repair infected bone defects.

Language: Английский

---

Microwave–Driven Interface Engineering Enhancing Electron Flow for Highly Efficient Solar NO Oxidation over rGO-Integrated NH₂-MIL125(Ti)/TiO₂

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

Published: March 1, 2025

Interface design plays a pivotal role in developing high-performance photocatalysts for NO oxidation. In this work, hierarchical rGO-integrated NH2-MIL125(Ti)/TiO2 photocatalyst was constructed using combined liquid-phase and solid-phase microwave synthesis approach. The process enabled the precise deposition of NH2-MIL125(Ti) on graphene oxide (GO), forming strong interfacial bonds, while thermal shock (SMTS) transformed GO into rGO induced formation TiO2 nanoparticles. This structure established an efficient electron transport pathway, promoting charge separation directional transfer to activate O2 generate superoxide radicals (•O2–) as primary reactive species. resulting achieved remarkable oxidation performance, with 81.2% removal efficiency NO3– selectivity 98.5% under simulated sunlight. study highlights potential microwave–driven interface engineering innovative environmentally sustainable applications.

Language: Английский

---

Radiation‐Synthesized Metal–Organic Frameworks with Ligand‐Induced Lewis Pairs for Selective CO₂ Electroreduction

Small, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 15, 2024

Abstract The electrochemical activation of inert CO 2 molecules through C─C coupling reactions under ambient conditions remains a significant challenge but holds great promise for sustainable development and the reduction emission. Lewis pairs can capture react with , offering novel strategy electrosynthesis high‐value‐added C2 products. Herein, an electron‐beam irradiation is presented rapidly synthesizing metal–organic framework (MOF) well‐defined (i.e., Cu‐ N pyridinic ). synthesized MOFs exhibit total product faradic efficiency 70.0% at −0.88 V versus RHE. In situ attenuated reflection Fourier transform infrared Raman spectra reveal that electron‐deficient acidic Cu sites electron‐rich basic in ligand facilitate targeted chemisorption, activation, conversion molecules. DFT calculations further elucidate electronic interactions key intermediates reaction. work not only advances pair‐site as new platform conversion, also provides pioneering insights into underlying mechanisms irradiated synthesis advanced nanomaterials.

Language: Английский

---

Nitrogen-Doped Carbon Quantum Dots with Photoactivation Properties for Ultraviolet Ray Detection

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(32), P. 42632 - 42640

Published: July 31, 2024

Photoactivation is a phenomenon that could enhance the photoluminescence (PL) and photostability upon UV/vis light exposure, which usually observed in CdSe/ZnS quantum dots (QDs). However, photoactivation has been scarcely reported fluorescent carbon (CQDs). Herein, nitrogen-doped (N-CQDs) were prepared through facile solvothermal approach with naphthalenetracarboxylic dianhydride serine as precursors. Upon simple UV irradiation for 10 min, fluorescence yield (QY) of N-CQDs increase up to 10-fold. Based on this phenomenon, explored an ultraviolet (UV) sensor assess intensity radiation sunlight indirectly evaluate UV-blocking efficiency various sunscreen products. Thus, contribution not only provided insight into developing low-cost detector but also opened door development converse-photobleaching properties.

Language: Английский

---

Integral morphology and structure design of poly (heptazine imide) for efficient utilization of visible light generated charge carriers in proton reduction reactions

Carbon Neutralization, Journal Year: 2024, Volume and Issue: unknown

Published: Aug. 22, 2024

Abstract Sufficient utilization of visible‐light generated charge carriers in proton reduction reactions is great significance for the development effective solar‐fuel technologies. Achieving simultaneous bulk rapid transfer and surface efficient extraction still very challenging. Herein, it found first time ammonium persulfate (APS) can significantly influence polymerization processes C 3 N 4 (CN) from melamine to poly (heptazine imide) (PHI) under oxygen doping etching effect SO 2− . PHI with high crystallinity, porous structure, in‐situ was therefore obtained through one‐step APS‐assisted salt strategy. Benefiting sufficient absorption upshifted conduction band originating regulated electronic structure optimized morphology APS modification, as‐prepared achieved a H 2 evolution activity 3274.23 μmol h −1 g ( λ > 420 nm), which appropriately 148 19 times that conventional crystalline CN. This work opens up new opportunities photocatalysis.

Language: Английский

---

Modulating Quinoline-Linked Covalent Organic Frameworks via Fluorination for Boosting the Photocatalytic Air Reductive H₂O₂ Production

ACS Sustainable Chemistry & Engineering, Journal Year: 2024, Volume and Issue: 12(35), P. 13306 - 13315

Published: Aug. 20, 2024

The intrinsic reversibility and strong polarization of imine linkages limit the application imine-based covalent organic frameworks (COFs) in photocatalysis. Herein, inspired by aza-Diels–Alder cycloaddition reaction, two quinoline-linked fluorinated COFs (termed TTB-TTA-Ph-F TTB-TTA-Ph-3F) are developed based on postsynthetic modification an imine-linked COF (TTB-TTA). simultaneous reversibility-to-irreversibility bond transformation fluorination endow resultant with improved robustness, extended structural conjugation, intriguing optoelectronic properties. introduced fluorine groups change local electronic structures improve charge separation transfer. Benefiting from rational design skeleton, TTB-TTA-Ph-3F exhibits excellent activity, giving a 3496.9 μmol g–1 h–1 photocatalytic H2O2 production rate water air after optimizing modulation.

Language: Английский

---

Harnessing S-scheme junctions for enhanced CO2 photoreduction: molecular bonding of copper(II) complexes onto K-doped polymeric carbon nitride via microwave heating

Rare Metals, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 20, 2024

Language: Английский

---