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Mesoporous TiO2-BiOBr Microspheres with Tailorable Adsorption Capacities for Photodegradation of Organic Water Pollutants: Probing Adsorption-Photocatalysis Synergy by Combining Experiments and Kinetic Modeling
摘要： Understanding adsorption-photocatalysis synergy helps advance solar-driven photodegradation of organic wastewater pollutants. To evaluate the synergy, mesoporous TiO2(amorphous)-BiOBr microspheres were facilely synthesized as model photocatalysts and characterized by XRD, SEM, TEM/HRTEM, XPS, nitrogen adsorption-desorption, UV-vis DRS, photoluminescence, and FTIR. The characterizations and photodegradation tests suggested that the composites had both adsorption sites and photocatalysis sites on BiOBr phase, while homogeneously distributed TiO2 in BiOBr microplates tailored the size of BiOBr crystallites. Accordingly, surface areas of the composites spanned from 22 to 155 m2/g and adsorption capacities for methyl orange (MO) ranged from 16 to 54 mg/g, controlled by the TiO2 content. In addition to experiments, kinetic modeling that combined adsorption with photocatalysis was developed and aided elucidating the synergy and quantitatively evaluating the composites with extracted rate constants from experimental data. The rate constant of the composite (Ti/Bi = 0.6) was calculated to be 3 times that of the pure BiOBr. Though adsorption promoted MO photodegradation, the capacity of the composite for MO adsorption and photodegradation decreased dramatically during the cycling tests. Nevertheless, this problem did not happen during photodegradation of rhodamine B and phenol on the composite and photodegradation of MO on pure BiOBr. This was explained by possible accumulation of degradation intermediates on the composite surface. This study provides a useful approach to investigate the adsorption-photocatalysis synergy from the perspectives of experiments and kinetic modeling and implies the necessity of scrutinizing the adverse effects of high levels of adsorption on recyclability of the photocatalysts.
关键词： Organic pollutants photodegradation,Kinetic modeling,TiO2-BiOBr microspheres,Tailorable adsorption capacities,Adsorption-photocatalysis synergy
更新于2025-11-14 17:03:37
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Removal of tetracycline by BiOBr microspheres with oxygen vacancies: Combination of adsorption and photocatalysis
摘要： Oxygen vacancy-containing BiOBr microspheres with dual functions of adsorption-photocatalysis were synthesized by a simple solvothermal method. The as-prepared samples were characterized by X-ray diffraction (XRD), field-emission scanning electron microscopy (FESEM), X-ray photoelectron spectroscopy (XPS), electron paramagnetic resonance spectroscopy (EPR) and UV–vis diffuse reflectance spectroscopy (DRS). BiOBr microspheres with oxygen vacancies exhibited a higher adsorptive and photocatalytic activity for the removal of tetracycline (TC) than that of defect-deficient BiOBr microspheres. After adsorption for 30 min and visible light irradiation for 90 min, about 94 % of TC was removed by oxygen vacancy-containing BiOBr microspheres, and TC removal efficiency performed effectively in a wide pH range from 3.1 to 11.00. Almost all inorganic anions, such as Cl?, SO2?4, PO3?4, CO2?3 and NO?3, inhibited the removal of TC by BiOBr microspheres and their inhibition effects followed the order of PO3?4 > SO2?4 > CO2?3 > Cl? > NO?3. The surface hydroxyl groups had no effect on TC adsorption, and the adsorption of TC on BiOBr was mainly through the anion exchange process. The existence of oxygen vacancies facilitated the generation of superoxide radicals (O2??), which were the dominant reactive oxygen species for TC degradation in BiOBr suspension. The adsorptive and photocatalytic performance of oxygen vacancy-containing BiOBr decreased to different degrees after three cycles mainly due to the formation of surface complex.
关键词： Mechanism,Photocatalysis,Oxygen vacancy,Adsorption,BiOBr microspheres,Tetracycline
更新于2025-09-23 15:23:52
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Synthesis and photocatalytic activity of BiOBr hierarchical structures constructed by porous nanosheets with exposed (110) facets
摘要： BiOBr hierarchical structures were successfully synthesized through a solvothermal process assisted with citric acid using methanol as a solvent. The as-synthesized BiOBr hierarchical structures have diameters of ca. 1 μm, and assembled by numerous porous nanosheets with exposed (110) facets. Results indicated that the crystal growth and morphology structures of BiOBr were significantly influenced by the amount of citric acid, the solvothermal time and the solvent used in reaction. In addition, the as-synthesized BiOBr hierarchical structures exhibited high photocatalytic activity on the degradation of methyl orange under either UV light or simulated sunlight illumination, due to the larger specific surface area and unique hierarchical structures assembled by numerous BiOBr porous nanosheets.
关键词： photocatalytic,citric acid,hierarchical structures,solvothermal,BiOBr
更新于2025-09-23 15:22:29
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Improved Solar Energy Photoactivity over Defective BiOBr Ultrathin Nanosheets towards Pollutants Removal and Oxygen Evolution
摘要： Defective BiOBr nanosheets with ultrathin thickness and surface confined pits have been synthesized through a dual control of cetyltrimethyl ammonium bromide (CTAB) and polyvinyl pyrrolidone (PVP). The photocatalytic activity of the obtained defective BiOBr nanosheets was evaluated for the removal of rhodamine B (RhB), ciprofloxacin (CIP) and oxygen evolution from water. The as-prepared defective BiOBr nanosheets displayed significantly increased activity for pollutant degradation and oxygen evolution. The enhanced photocatalytic activity was ascribed to the improved light harvesting, suppression of charge recombination, and an increase in the number of active sites for photocatalytic reaction. The electronic structure of the defective BiOBr ultrathin nanosheets with confined pits has been tuned and thus varied the photocatalytic mechanism for pollutant degradation. The active species have changed from hole for BiOBr nanoplates to superoxide radical (O2??) and hole for defective BiOBr nanosheets determined by ESR analysis and trapping experiments.
关键词： Ultrathin nanosheets,Solar energy,Defects,BiOBr,Photocatalytic
更新于2025-09-23 15:21:21
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Largea??Scale Ultrathin 2D Widea??Bandgap BiOBr Nanoflakes for Gatea??Controlled Deepa??Ultraviolet Phototransistors
摘要： Ternary two-dimensional (2D) semiconductors with controllable wide bandgap, high ultraviolet (UV) absorption coefficient, and critical tuning freedom degree of stoichiometry variation have a great application prospect for UV detection. However, as-reported ternary 2D semiconductors often possess a bandgap below 3.0 eV, which must be further enlarged to achieve comprehensively improved UV, especially deep-UV (DUV), detection capacity. Herein, sub-one-unit-cell 2D monolayer BiOBr nanoflakes (≈0.57 nm) with a large size of 70 μm are synthesized for high-performance DUV detection due to the large bandgap of 3.69 eV. Phototransistors based on the 2D ultrathin BiOBr nanoflakes deliver remarkable DUV detection performance including ultrahigh photoresponsivity (Rλ, 12739.13 A W?1), ultrahigh external quantum efficiency (EQE, 6.46 × 106%), and excellent detectivity (D*, 8.37 × 1012 Jones) at 245 nm with a gate voltage (Vg) of 35 V attributed to the photogating effects. The ultrafast response (τrise = 102 μs) can be achieved by utilizing photoconduction effects at Vg of ?40 V. The combination of photocurrent generation mechanisms for BiOBr-based phototransistors controlled by Vg can pave a way for designing novel 2D optoelectronic materials to achieve optimal device performance.
关键词： monolayer BiOBr,deep UV phototransistors,wide-bandgap semiconductors,high gain
更新于2025-09-23 15:19:57
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Enhanced UV-Vis-NIR activated photocatalytic activity from Fe <sup>3+</sup> -doped BiOBr:Yb <sup>3+</sup> /Er <sup>3+</sup> upconversion nanoplates: synergistic effect and mechanism insight
摘要： Upconversion (UC) materials are recognized as promising candidates to harvest solar energy for photocatalysis. In this work, a simple strategy for simultaneously enhancing the UC luminescence and photocatalytic efficiency of BiOBr:Yb3+/Er3+ nanoplates through Fe3+ ion doping is reported. Compared to the Fe3+-free sample, the UC emission intensity was significantly enhanced through tailoring of the crystal symmetry by Fe3+ ions. Experiment and DFT calculations reveal that the introduction of Fe3+ ions resulted in the formation of an impurity energy level, extending to the light absorption region. As expected, the Fe3+-doped BiOBr:Yb3+/Er3+ nanoplates exhibit a wide photoresponse from the UV to NIR regions, good stability, and obviously enhanced photocatalytic activities compared with the BiOBr:Yb3+/Er3+ nanoplates in the degradation of RhB. The boosted photocatalytic activity can be attributed to the synergic effect of the efficient utilization of UC luminescence and Fe3+ doping, where Fe3+ doping could improve the light harvesting capacity, enhance the separation efficiency of electron and hole (e?/h+) pairs, and promote the production of highly oxidative species. This work not only provides a promising system for the efficient utilization of solar light, but also offers a feasible guideline for the further design of broad-spectrum active photocatalysts.
关键词： Enhanced UV-Vis-NIR activated photocatalytic activity,mechanism insight,Fe3+-doped BiOBr:Yb3+/Er3+ upconversion nanoplates,synergistic effect
更新于2025-09-19 17:15:36
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Fabrication of vessel–like biochar–based heterojunction photocatalyst Bi2S3/BiOBr/BC for diclofenac removal under visible LED light irradiation: Mechanistic investigation and intermediates analysis
摘要： In this work, a novel, economical and effective vessel–like biochar–based photocatalyst Bi2S3/BiOBr/BC was synthesized by a facile one–pot solvothermal method for the first time. A series of characterization analyses demonstrated the successful preparation of photocatalyst Bi2S3/BiOBr/BC. Furthermore, diclofenac (DCF) as the target contaminant was applied to elucidate the enhanced photocatalytic performance (93.65%, 40 min) under energy–saving visible LED light irradiation. Comparison experiments among different photocatalysts and photoelectrochemical tests results illustrated that excellent photocatalytic performance of Bi2S3/BiOBr/BC 10% might be attributed to the electrons transfer of biochar and higher charge separation efficiency of heterojunction structure. Besides, lower electrical energy per order value indicated photocatalyst/visible LED light system was more energy–saving. Proper photocatalyst dosage (0.6 g/L) and relatively acidic water environment (pH=5.0) would be beneficial to DCF photodegrdation by Bi2S3/BiOBr/BC. Good reusability and stability of Bi2S3/BiOBr/BC were verified via five consecutive recycle experiments. Furthermore, the role of active species was determined through trapping experiments and ·O2– and h+ dominated the photodegradation reaction to mineralize DCF molecules. Eleven main intermediates and four possible photodegradation pathways were proposed by HRMS analysis. Accordingly, photocatalyst Bi2S3/BiOBr/BC would provide potential technical support for emerging pollutant removal in water matrix.
关键词： Diclofenac,Photocatalytic mechanism,Bi2S3/BiOBr/BC,Visible LED light,Degradation pathway
更新于2025-09-19 17:13:59
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Facile constructing plasmonic Z-scheme Au NPs/g-C3N4/BiOBr for enhanced visible light photocatalytic activity
摘要： A novel ternary Au NPs/g-C3N4/BiOBr Z-scheme heterojunction composite was fabricated through hydrothermal and in-situ reduction method, and characterized by X-ray diffraction, X-ray photoelectron spectroscopy, transmission electron microscopy, ultraviolet-visible diffuse reflection spectroscopy and photoluminescence emission spectroscopy. The photocatalytic activity was evaluated by the degradation of phenol under visible-light irradiation. It was found that Au NPs/g-C3N4/BiOBr showed enhanced photocatalytic activity, which is 3-fold higher than g-C3N4 and 2.5-fold higher than BiOBr. This could be attributed to the effective separation of photogenerated electron-hole pairs, narrowed band gap (2.10 eV) and surface plasmon resonance (SPR).
关键词： Au NPs/g-C3N4/BiOBr,Z-scheme,phenol,visible-light photocatlysis,plasmon
更新于2025-09-12 10:27:22
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BiOBr/Ag6Si2O7 heterojunctions for enhancing visible light catalytic degradation performances with a sequential selectivity enabled by dual synergistic effects
摘要： Efficient separation of photogenerated electron-hole pairs is always one of the key factors boosting visible light photodegradation efficiency. Till now, there are few reports on the synergistic competitive consumption of photogenerated active species and the synergistic adsorption of organic contaminants to promote the performance of a designed heterojunction. Herein, we design and construct a novel BiOBr/Ag6Si2O7 heterojunction with the dual synergistic effects towards methylene blue (MB) and methyl orange (MO). The dual synergistic effects could avoid the combination of photogenerated h+/e? pairs, improve the adsorption efficiency, and even regulate the photodegradation efficiency. Thus, for an aqueous mixture of MB and MO, the BiOBr/Ag6Si2O7 photocatalyst exhibits largely improved adsorption capacities of the dyes by a multi-layer adsorption mode. Moreover, the photocatalyst could further promote the photodegradation rate of MO while slow that of MB due to the competitive consumption of photogenerated active species, showing a sequential selectivity phenomenon. Thanks to the dual synergistic effects, the adsorption capacity of MO increases 1379% higher than that of neat MO solution, and the photodegradation time decrease from 30 to 12 min with a rate constant of 0.22 min?1, 38% higher than that of neat MO solution.
关键词： BiOBr,Silver silicates,Visible light photodegradation,Heterojunctions,Photocatalysts
更新于2025-09-11 14:15:04
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Enhanced photocatalytic activity and stability of AgBr/BiOBr/graphene heterojunction for phenol degradation under visible light
摘要： In this work, we have reported synthesis of AgBr/BiOBr photocatalyst supported on graphene (Gr) using facile precipitation method. AgBr/BiOBr/Gr was characterized using various spectral techniques like FESEM, TEM, XRD, FTIR, XPS, Raman and PL analyses. AgBr/BiOBr/Gr had improved visible light absorption. PL studies indicated the reduction in recombination of photogenerated electron hole pair of AGBr/BiOBr/Gr. AFM analysis con?rmed the thickness of AGBr/BiOBr/Gr was less than 8.0 nm. The higher dispersibility of photocatalyst was ascertained by Tyndall effect. AgBr/BiOBr/Gr photocatalyst was effectively used for the photodegradation of phenol from simulated water. The phenol degradation process was remarkably in?uenced by adsorption process. The concurrent adsorption and photocatalytic was effective for degradation of phenol. The phenol was completely mineralized into CO2 and H2O in 6 h. The degradation process followed pseudo ?rst order kinetics. The results con?rmed that integration of AgBr/BiOBr with graphene caused an increase in photocatalytic activity due to reduced recombination of photogenerated electron hole pair and electron sink behavior of graphene for photogenerated electrons of BiOBr. AgBr/BiOBr/Gr photocatalyst displayed signi?cant stability and recyclability for ten catalytic cycles.
关键词： Enhanced photocatalytic activity,Recyclability,Phenol degradation,Graphene,AgBr/BiOBr,Heterojunction formation
更新于2025-09-11 14:15:04