Accelerating Small Electron Polaron Dissociation and Hole Transfer at Solid-Liquid Interface for Enhanced Heterogeneous Photoreaction.

In a photocatalysis process, quick charge recombination induced by small electron polarons in a photocatalyst and sluggish kinetics of hole transfer at the solid-liquid interface have greatly limited photocatalytic efficiency. Herein, we demonstrate hydrated transition metal ions as mediators that can simultaneously accelerate small electron polaron dissociation (via metal ion reduction) and hole transfer (through high-valence metal production) at the solid-liquid interface for improved photocatalytic pollutant degradation. Fe, by virtue of its excellent redox ability as a homogeneous mediator, enables the BiVO photocatalyst to achieve drastically increased photocatalytic degradation performance, up to 684 times that without Fe.

Efficient photocatalytic in-situ Fenton degradation of 2,4-dichlorophenol via anthraquinone-modified carbon nitride for 2e oxygen reduction.

Constructing a photocatalytic in-situ Fenton system (PISFs) is a promising strategy to address the need for continuous hydrogen peroxide (HO) addition and the low efficiency of HO activation for hydroxyl radical generation in the traditional Fenton reaction. In this study, we constructed a photocatalytic in-situ Fenton system using anthraquinone-modified carbon nitride (AQ-CN) for efficient pollutant degradation. The resultant AQ-CN not only enhanced the production of HO but also increased the generation of hydroxyl radical (·OH).

Tandem Proton Transfer in Carboxylated Supramolecular Polymer for Highly Efficient Overall Photosynthesis of Hydrogen Peroxide.

Proton supply is as critical as O activation for artificial photosynthesis of hydrogen peroxide (HO) via two-electron oxygen reduction reaction (2e ORR). However, proton release via water dissociation is frequently hindered because of the sluggish water oxidation reaction (WOR), extremely limiting the efficiency of photocatalytic HO production. To tackle this challenge, carboxyl-enriched supramolecular polymer (perylene tetracarboxylic acid-PTCA) is elaborately prepared by molecular self-assembly for overall photosynthesis of HO.

Tandem Fields Facilitating Directional Carrier Migration in Van der Waals Heterojunction for Efficient Overall Piezo-Synthesis of HO.

Piezo-synthesis of HO utilizing sustainable mechanical energy as well as earth-abundant water and oxygen is a green, cost-effective, and promising approach. However, achieving simultaneous two-electron water oxidation reaction (2e WOR) and two-electron oxygen reduction reaction (2e ORR) faces huge challenges due to insufficient synergistic active sites and slow/messy carrier transfer. Herein, a novel 2D/2D van der Waals heterojunction consisting of BiOIO and carbon nitride (BIO/CN) is elaborately designed for highly efficient overall HO piezo-synthesis.

single iron atom doping on BiWO monolayers triggers efficient photo-fenton reaction.

Developing an efficient photocatalytic system for hydrogen peroxide (HO) activation in Fenton-like processes holds significant promise for advancing water purification technologies. However, challenges such as high carrier recombination rates, limited active sites, and suboptimal HO activation efficiency impede optimal performance. Here we show that single-iron-atom dispersed BiWO monolayers (SIAD-BWOM), designed through a facile hydrothermal approach, can offer abundant active sites for HO activation.

Triggering Dual Two-electron Pathway for H O Generation by Multiple [Bi-O] Interlayers in Ultrathin Bi O Cl towards Efficient Piezo-self-Fenton Catalysis.

Piezo-self-Fenton system (PESF) has been emerging as a promising water treatment technology but suffering from unsatisfied H O production efficiency. Herein, we rationally design a Bi O Cl piezo-catalyst with multiple [Bi-O] interlayers towards highly efficient H O production. The introduction of [Bi O ] layers initiates dual two-electron pathway for H O generation by altering the interlayer properties.

Environmental energy enhanced solar-driven evaporator with spontaneous internal convection for highly efficient water purification.

Solar-driven interfacial evaporation for water purification is limited by the structural design of the solar evaporator and, more importantly, by the inability to separate the water from volatile organic compounds (VOCs) present in the water source. Here, we report a three-dimensional (3D) bifunctional evaporator based on N-doped carbon (CoNC/CF), which enables the separation of fresh water from VOCs by activating PMS during the evaporation process with a VOC removal rate of 99%. There is abundant van der Waals interaction between peroxymonosulfate (PMS) and CoNC/CF, and pyrrolic N is confirmed as the active site for binding phenol, thus contributing to the separation of phenol from water.

Multi-heteroatom-doping promotes molecular oxygen activation on polymeric carbon nitride for simultaneous generation of HO and degradation of oxcarbazepine.

Simultaneously realizing the efficient generation of HO and degradation of pollutants is of great significance for environmental remediation. However, most polymeric semiconductors only show moderate performance in molecular oxygen (O) activation due to the sluggish electron-hole pair dissociation and charge transfer dynamics. Herein, we develop a simple thermal shrinkage strategy to construct multi-heteroatom-doped polymeric carbon nitride (K, P, O-CN).

n→π* Electron Transitions and Directional Charge Migration Synergistically Promoting O Activation and Holes Utilization on Carbon Nitride for Efficiently Photocatalytic Degradation of Organic Contaminants.

Stimulating electron transitions and promoting exciton dissociation are crucial for improving the photocatalytic performance of polymeric carbon nitride (CN) yet still challenging. Herein, a novel CN with C dopant and asymmetric structure (CC-UCN ) is ingeniously synthesized. The obtained CC-UCN not only reinforces the intrinsic π→π* electron transitions, but also successfully awakens additional n→π* electron transitions.

Simultaneously Achieving Fast Intramolecular Charge Transfer and Mass Transport in Holey D-π-A Organic Conjugated Polymers for Highly Efficient Photocatalytic Pollutant Degradation.

Simultaneously realizing efficient intramolecular charge transfer and mass transport in metal-free polymer photocatalysts is critical but challenging for environmental remediation. Herein, we develop a simple strategy to construct holey polymeric carbon nitride (PCN)-based donor-π-acceptor organic conjugated polymers via copolymerizing urea with 5-bromo-2-thiophenecarboxaldehyde (PCN-5B2T D-π-A OCPs). The resultant PCN-5B2T D-π-A OCPs extended the π-conjugate structure and introduced abundant micro-, meso-, and macro-pores, which greatly promoted intramolecular charge transfer, light absorption, and mass transport and thus significantly enhanced the photocatalytic performance in pollutant degradation.

Highly efficient removal of organic contaminant with wide concentration range by a novel self-cleaning hydrogel: Mechanism, degradation pathway and DFT calculation.

A novel carbon nitride based self-cleaning hydrogel photocatalyst (KI-PCN gel, potassium and iodine co-doped carbon nitride confined in alginate) has been successfully constructed by a facile method. Fabricated photocatalyst showed enhanced synergistic adsorption-photocatalytic degradation property on a high concentration of methylene blue (HMB) because of enhanced carrier separation efficiency and improved light adsorption capacity of KI-PCN. As expected, the KI-PCN gel showed the highest apparent rate constant value K =0.

Regulating directional transfer of electrons on polymeric g-CN for highly efficient photocatalytic HO production.

Graphite carbon nitride (g-CN) has been widely used in various photocatalytic reactions due to its higher thermodynamic stability and better electronic properties compared to g-CN. However, it is still challenging to endow g-CN with high performance on photocatalytic hydrogen peroxide (HO) production. Herein, potassium and iodine are co-doped into g-CN (g-CN-K, I) for photocatalytic production of HO with high efficiency.

Understanding the mechanism of interfacial interaction enhancing photodegradation rate of pollutants at molecular level: Intermolecular π-π interactions favor electrons delivery.

Uncovering the interaction between photocatalyst and reaction substrate as well as subsequent electron transfer process is critical to achieve high-performance photodegradation of pollutants. Herein, based on the reduced density gradient (RDG) method, we visualize the simulation of the π-π interactions between photocatalyst (g-CN) and pollutant molecule (flumequine, FLU). Results revealed that π-π interactions between g-CN and FLU favor electrons delivery, resulting in enhanced charge separation efficiency and direct hole oxidation of FLU.

Iodide-Induced Fragmentation of Polymerized Hydrophilic Carbon Nitride for High-Performance Quasi-Homogeneous Photocatalytic H O Production.

Polymeric carbon nitride (PCN) as a class of two-electron oxygen reduction reaction (2 e ORR) photocatalyst has attracted much attention for H O production. However, the low activity and inferior selectivity of 2 e ORR greatly restrict the H O production efficiency. Herein, we develop a new strategy to synthesize hydrophilic, fragmented PCN photocatalyst by the terminating polymerization (TP-PCN) effect of iodide ions.

Confinement of ultrasmall CoFeO nanoparticles in hierarchical ZnInS microspheres with enhanced interfacial charge separation for photocatalytic H evolution.

The charge carriers' separation efficiency, light absorption capacity and microstructure of photocatalysts are important factors affecting the photocatalytic performance. Herein, we prepared the hierarchical ZnInS (ZIS) microspheres-confined CoFeO nanoparticles (CFO NPs) p-n junction (CFO/ZIS) with enhanced charge carriers' separation and extensive visible light response. Surprisingly, the 1% CFO/ZIS exhibits the optimal photocatalytic H evolution (PHE) activity, which is about over 3.

Enhanced light utilization efficiency and fast charge transfer for excellent CO photoreduction activity by constructing defect structures in carbon nitride.

Defect structure is one of the crucial factors for enhancing the catalytic activities of photocatalysts. However, rational design and construction of defect structures in catalysts to meet the aim of enhancing photocatalytic performance in a simple and cost-effective way is still a challenge. In this contribution, we report a strategy to construct defect structures in graphitic carbon nitride (g-CN) by simple copolymerizing of urea with polyethyleneimine (PEI).

Precursor-reforming strategy induced g-CN microtubes with spatial anisotropic charge separation established by conquering hydrogen bond for enhanced photocatalytic H-production performance.

Precursor-reforming strategy induced graphitic carbon nitride (g-CN) with different morphologies for enhanced photocatalytic hydrogen (H) evolution activity is highly desirable. Herein, g-CN microtubes (mg-CN) with adjustable closure degree of microtube orifice and spatial anisotropic charge separation are established by conquering hydrogen bond during thermally exfoliate precursor. Compared to the bulk g-CN (bg-CN) and ultrathin g-CN (ug-CN), the tubular structure endows mg-CN with spatial anisotropic charge separation that accelerates transfer of charge carriers.

Yeast-derived carbon sphere as a bridge of charge carriers towards to enhanced photocatalytic activity of 2D/2D CuWS/g-CN heterojunction.

It is very challenging to fabricate novel, high-efficiency photocatalysts with an enhanced visible light absorption capacity, high charge carrier separation efficiency, and large specific surface area. For this purpose, a yeast-derived carbon (YC) sphere was added as a charge carrier bridge to the 2D-2D CuWS/g-CN heterojunction through a facile hydrothermal method. The YC sphere, as a bridge for electrons, is not only advantageous in inhibiting rapid recombination by electrons, but also remarkably enhances the visible light absorption capacity.

A visible-light-driven Z-scheme CdS/BiGeO heterostructure with enhanced photocatalytic degradation of various organics and the reduction of aqueous Cr(VI).

A series of Z-scheme CdS/BiGeO heterostructures were successfully obtained by a simple hydrothermal method. The Z-scheme CdS/BiGeO heterostructures show outstanding photocatalytic performance for degrading the various organic pollutants of the waste water, and for the reduction of aqueous Cr(VI) under visible light. For degradation of 2-Mercaptobenzothiazole (MBT), the Z-scheme 30CdS/BiGeO heterostructure exhibits the superior rate constant, which is about 22.

Visible-light-driven Ag/BiOCl nanocomposite photocatalyst with enhanced photocatalytic activity for degradation of tetracycline.

In this study, a novel Ag/BiOCl photocatalyst has been synthesized by a facile photodeposition process. Its photocatalytic performance was evaluated from the degradation of tetracycline (TC) under visible light irradiation ( > 420 nm). The 1.

Composition dependent magnetic and ferroelectric properties of hydrothermally synthesized GdFeCrO (0.1 ≤ x ≤ 0.9) perovskites.

The hydrothermal synthesis and magnetic, dielectric and ferroelectric property characterization of ABO-perovskite GdFeCrO (0 < x < 1) are reported. The mineralizer KOH plays a critical role in the perovskite structure of the sample. The Fe/Cr ratio of the final crystal is controlled by the alkalinity in the initial reaction mixtures.