Jiexiang Xia

Preparation of sphere-like g-C3N4/BiOI photocatalysts via a reactable ionic liquid for visible-light-driven photocatalytic degradation of pollutants

Novel sphere-like g-C3N4/BiOI composite photocatalysts were prepared by a one-pot EG-assisted solvothermal process in the presence of reactable ionic liquid 1-butyl-3-methylimidazolium iodine ([Bmim]I). The nanostructured heterojunction was formed with g-C3N4 covering the surface of BiOI microspheres uniformly. Multiple techniques were applied to investigate the structure, morphology and photocatalytic properties of as-prepared samples. During the reactive process, the ionic liquid acted as solvent, reactant, template and dispersing agent at the same time, leading to g-C3N4 being uniformly dispersed on the sphere-like BiOI surface. Three different types of dyes rhodamine B (RhB), methylene blue (MB), methyl orange (MO) were chosen as model pollutants to evaluate the photocatalytic activity of g-C3N4/BiOI composite. The as-prepared g-C3N4/BiOI composite exhibited much higher photocatalytic activity than the pure BiOI. At the same time, colourless endocrine disrupting chemical bisphenol A (BPA) and phenols 4-chlorophenol (4-CP) were chosen to further evaluate the photocatalytic activity of g-C3N4/BiOI composite. The g-C3N4/BiOI composite also exhibited much higher photocatalytic activity than the pure BiOI, which showed a broad spectrum of photocatalytic degradation activities. The results indicated that the formed heterojunction of g-C3N4 covers the BiOI microspheres contributed to improved electron–hole separation and enhancement in photocatalytic activity. A photocatalytic mechanism of g-C3N4/BiOI composites is also proposed.

Self-Assembly and Enhanced Photocatalytic Properties of BiOI Hollow Microspheres via a Reactable Ionic Liquid

BiOI uniform flowerlike hollow microspheres with a hole in its surface structures have been successfully synthesized through an EG-assisted solvothermal process in the presence of ionic liquid 1-butyl-3-methylimidazolium iodine ([Bmim]I). The as-prepared samples were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), energy-dispersive X-ray spectroscopy (EDS), nitrogen sorption, and diffuse reflectance spectroscopy (DRS). A possible formation mechanism for the growth of hollow microspheres was discussed. During the reactive process, ionic liquid not only acted as solvents and templates but also as an I source for the fabrication of BiOI hollow microspheres and was vital for the structure of hollow microspheres. Additionally, we evaluated the photocatalytic activities of BiOI on the degradation of methyl orange (MO) under visible light irradiation and found that as-prepared BiOI hollow microspheres exhibited higher photocatalytic activity than BiOI nanoplates and TiO(2) (Degussa, P25) did. On the basis of such analysis, it can be assumed that the enhanced photocatalytic activities of BiOI hollow microspheres could be ascribed to its energy band structure, high BET surface area, high surface-to-volume ratios, and light absorbance.

Commercially available molybdic compound-catalyzed ultra-deep desulfurization of fuels in ionic liquids

A simple liquid–liquid extraction and catalytic oxidative desulfurization (ECODS) system composed of molybdic compound, 30% H2O2 and 1-butyl-3-methylimidazolium tetrafluoroborate ([bmim]BF4) has been found suitable for the ultra-deep removal of dibenzothiophene (DBT) in model oil. The precatalyst of molybdic compound was oxidized with H2O2 to form peroxomolybdic compound, which was soluble in ionic liquid and dissolved in oil. The sulfur-containing compounds, such as benzothiophene (BT), DBT and 4,6-dimethyldibenzothiophene (4,6-DMDBT), in model oil were extracted into ionic liquid phase and oxidized to their corresponding sulfones by peroxomolybdic compound. In the case of the system containing model oil (DBT), H2O2, Na2MoO4·2H2O and [bmim]BF4, extraction and catalytic oxidation increased the sulfur removal to 99.0%, which was remarkably superior to mere solvent extraction with IL (13.6%) or catalytic oxidation without IL (4.1%). The desulfurization system could be recycled five times with very little decrease in activity.

One-pot synthesis of visible-light-driven plasmonic photocatalyst Ag/AgCl in ionic liquid.

Plasmonic photocatalyst Ag/AgCl was prepared by in situ hydrothermal method with the contribution of 1-octyl-3-methylimidazolium chloride ([Omim]Cl), in which the [Omim]Cl ionic liquid acted not only as a precursor but also as a reducing reagent in the process of formation of Ag⁰. The samples were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), diffuse reflectance spectroscopy (DRS), X-ray photoelectron spectroscopy (XPS), and thermogravimetric and differential scanning calorimetry (TG-DSC). The photocatalytic activity of the composites were evaluated by degradation of methyl orange (MO) under visible light irradiation. The experimental results showed that the high activity and stability of Ag/AgCl photocatalysts under visible-light irradiation were due to their localized surface plasmon resonance (LSPR). Based on the characterization of the structure and photocatalytic performance, the LSPR was determined by synergetic effect of many factors, such as particle size of metallic Ag, contents of the Ag⁰ nanoparticles, and the extent of metallic Ag dispersing. A photocatalytic mechanism of the Ag/AgCl photocatalyst was also proposed.

Exfoliated graphene-like carbon nitride in organic solvents: enhanced photocatalytic activity and highly selective and sensitive sensor for the detection of trace amounts of Cu2+

Due to their unprecedented electronic, surface and optical properties, the atomic-thick graphene-like materials have aroused great interest. Compared with the bulk counterparts, the graphene-like material can not only enhance the internal properties, but also gives rise to new promising properties. Herein, the graphene-like carbon nitride (graphene-like C3N4) was synthesized via liquid exfoliation from the bulk graphitic carbon nitride (g-C3N4) in 1,3-butanediol (1,3-BUT) for the first time. And the graphene-like C3N4 was characterized by X-ray diffraction (XRD), atomic force microscopy (AFM), transmission electron microscopy (TEM), thermogravimetric analysis (TG), and X-ray photoelectron spectroscopy (XPS). The obtained graphene-like C3N4 exhibited a two-dimensional thin-layer structure with about 3–6 atoms thickness, a high specific surface area of 32.54 m2 g−1, increased photocurrent responses, improved electron transport ability and enhanced photocatalytic activity. The photocatalytic reaction for the organic dye methylene blue (MB) by the graphene-like C3N4 followed first-order kinetics. Moreover, the graphene-like C3N4 exhibited a higher apparent rate of 0.1262 min−1, which was 3.1 times higher than that of the bulk g-C3N4 (0.0409 min−1). The enhanced photocatalytic reaction was due to a high specific surface area and a larger bandgap (by 0.14 eV). The yield of the graphene-like C3N4 was up to ∼0.35 mg mL−1. Moreover, the graphene-like C3N4 had a new property that it could be used as the sensor for trace amounts of Cu2+ determination, so the graphene-like C3N4 is a new but promising candidate for heavy metal ions (Cu2+) determination in water environment. Photoelectrochemical selective sensing of trace amounts of Cu2+ was also discussed.

Facile fabrication of the visible-light-driven Bi2WO6/BiOBr composite with enhanced photocatalytic activity

Novel Bi2WO6/BiOBr composite photocatalysts were prepared by a one-pot EG-assisted solvothermal process in the presence of reactable ionic liquid 1-hexadecyl-3-methylimidazolium bromide ([C16mim]Br). Multiple techniques, such as X-ray diffraction (XRD), X-ray photoemission spectroscopy (XPS), scanning electron microscopy (SEM), transmission electron microscopy (TEM), energy dispersive X-ray spectrometry (EDS), Fourier transform infrared spectroscopy (FT-IR), UV-vis diffuse reflection spectroscopy (DRS), photoluminescence (PL), photocurrent and electrochemical impedance spectroscopy (EIS) were applied to investigate the structures, morphology and photocatalytic properties of as-prepared samples. Compared with bare Bi2WO6 and BiOBr, the Bi2WO6/BiOBr composites exhibited significantly enhanced photocatalytic activity for rhodamine B (RhB) degradation under visible light irradiation. The 50 at% Bi2WO6/BiOBr showed the highest photocatalytic activity under visible light irradiation, which was about 26.6 times and 1.8 times than that of the bare Bi2WO6 and BiOBr, respectively. The Bi2WO6/BiOBr composites also exhibited enhanced photocatalytic activity for bisphenol A (BPA) and methylene blue (MB) degradation under visible light irradiation. The results of PL, photocurrent and EIS indicated that Bi2WO6 and BiOBr could combine well to form a heterojunction structure which facilitated electron–hole separation, and led to the increasing photocatalytic activity. On the basis of the experimental results and estimated energy band positions, the mechanism of enhanced photocatalytic activity was proposed.

Carbon Quantum Dots Modified BiOCl Ultrathin Nanosheets with Enhanced Molecular Oxygen Activation Ability for Broad Spectrum Photocatalytic Properties and Mechanism Insight

In this paper, carbon quantum dots (CQDs) modified BiOCl ultrathin nanosheets photocatalyst was synthesized via a facile solvothermal method. The structures, morphologies, optical properties, and photocatalytic properties were investigated in detail. The photocatalytic activity of the obtained CQDs modified BiOCl ultrathin nanosheets photocatalyst was evaluated by the degradation of bisphenol A (BPA) and rhodamine B (RhB) under ultraviolet, visible, and near-infrared light irradiation. The CQDs/BiOCl materials exhibited significantly enhanced photocatalytic performance as compared with pure BiOCl and the 5 wt % CQDs/BiOCl materials displayed the best performance, which showed a broad spectrum of photocatalytic degradation activity. The main active species were determined to be hole and O2•- under visible light irradiation by electron spin resonance (ESR) analysis, XPS valence spectra, and free radicals trapping experiments. The crucial role of CQDs for the improved photocatalytic activity was mainly attributed to the superior electron transfer ability, enhanced light harvesting, and boosted catalytic active sites.

A g-C3N4/BiOBr visible-light-driven composite: synthesis via a reactable ionic liquid and improved photocatalytic activity

g-C3N4/BiOBr composite photocatalysts have been synthesized in the presence of the reactable ionic liquid 1-hexadecyl-3-methylimidazolium bromide ([C16mim]Br). The as-prepared samples were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FT-IR), diffuse reflectance spectroscopy (DRS), photoluminescence (PL) spectroscopy, electrochemical impedance spectroscopy (EIS), and photocurrent analysis. During the reaction process, the ionic liquid [C16mim]Br acted as solvent, reactant, template and dispersing agent at the same time, leading the g-C3N4 to disperse well on the surface of the BiOBr flower-like microspheres. The photocatalytic ability of the as-prepared photocatalysts was evaluated using rhodamine B (RhB) as a target pollutant. The photocatalysts exhibited a significantly enhanced photocatalytic performance in the degradation of RhB. The results of PL, EIS, and photocurrent tests indicated that g-C3N4 combined and dispersed well on the surface of BiOBr which facilitated electron–hole separation, and led to the increased photocatalytic activity. The optimal g-C3N4 content for the photocatalytic activity of the g-C3N4/BiOBr composites was determined. Radical trap experiments certified that the hole was the main reactive species for the photocatalytic degradation of RhB. A possible mechanism of g-C3N4 for the enhancement of visible light performance was proposed.

Reactable ionic liquid-assisted rapid synthesis of BiOI hollow microspheres at room temperature with enhanced photocatalytic activity

BiOI hollow microspheres have been rapidly synthesized through a facile reactable ionic liquid 1-butyl-3-methylimidazolium iodine ([Bmim]I)-assisted microemulsion method at room temperature. The formation mechanism of the BiOI hollow microspheres has been investigated. The BiOI hollow microspheres were formed through self-assembly and inside-out Ostwald ripening growth mechanism. During the reactive process, the ionic liquid, which acts as the solvent, reactant and template at the same time, plays a crucial role on the formation of hollow microspheres. In addition, the influencing factors (such as the reactant, the concentration of ionic liquids and the amount of acetic acid) of the formation of BiOI hollow microsphere have also been explored. The photocatalytic ability of the as-prepared photocatalysts was evaluated using rhodamine B (RhB) as a target pollutant. After systematic characterizations, the relationship between the structure of the photocatalyst and the photocatalytic activities were also discussed in detail. It can be assumed that the enhancing photocatalytic activity of BiOI hollow microspheres could be attributed to the improved light harvesting, shortened diffusion pathways, high BET surface area and faster interfacial charge separation. O2˙− and h+ were the main active species for the photocatalytic degradation of RhB. It is hoped that this rapidly synthetic route at room temperature can be extended to the purposive preparation of other hollow microsphere materials.

Controllable synthesis of Bi4O5Br2 ultrathin nanosheets for photocatalytic removal of ciprofloxacin and mechanism insight

A novel Bi4O5Br2 photocatalyst was prepared via a reactable ionic liquids-assisted solvothermal method accompanied with facile pH control. A Bi4O5Br2 ultrathin nanosheets material with 8 nm thickness could be obtained. The photocatalytic activity of the Bi4O5Br2 ultrathin nanosheets was evaluated with respect to the photo-degradation of colourless antibiotic agent ciprofloxacin (CIP) under visible light irradiation. The results revealed that the Bi-rich Bi4O5Br2 ultrathin nanosheets exhibited higher photocatalytic activity than BiOBr ultrathin nanosheets for the photo-degradation of CIP. The O2˙− anion was determined to be the main active species for the photo-degradation process by ESR. After multiple characterizations, the variable energy band structure was confirmed to be responsible for the enhanced photocatalytic activity. The more negative conduction band (CB) value of Bi4O5Br2 facilitated the formation of more active species, O2˙−. The upshifting of the CB and the wider valence band favor the higher separation efficiency of electron–hole pairs. It was hoped that this architecture of ultrathin 2D inorganic materials with a suitable band gap can be extended to other systems for high-performance photocatalysis applications.