复合纳米Fe2O3/TiO2可见光催化降解邻甲酚溶液的研究

以复合纳米Fe2O3／TiO2作为催化剂,日光色镝灯为光源,研究了邻甲酚溶液的可见光降解。考察了催化剂制备方法、催化剂使用量、溶液pH、催化剂重复使用等条件对可见光降解的影响。实验结果表明,1％Fe2O3／TiO2（n）对邻甲酚溶液的可见光降解效果最优,比Ti02（p25）的降解率提高了2．6倍。在实验条件下,可见光降解3h,邻甲酚溶液的浓度去除率达95．4％,TOC去除率为72．3％。在较宽的浓度范围内,邻甲酚的反应服从一级动力学反应方程,随着浓度的增大,反应速率常数不断降低。     

Room-temperature solid phase surface engineering of BiOI sheets stacking g-C3N4 boosts photocatalytic reduction of Cr(VI)

Cr(VI)-based compounds pollution have attracted global concern due to serious harm to humans and environment. Hence, it is crucial to exploit an effective technique to eliminate Cr(VI) in water. Herein, we in-situ grown BiOI on graphitic carbon nitride to prepare the BiOI/g-C3N4 (BCN) direct Z-scheme heterojunction by solid phase engineering method at room temperature. Experimental result shown the photocatalytic activity of pure BiOI were obviously enhanced by constructing Z-scheme BCN heterostructure, and BCN-3 heterostructure exhibited the optimal photocatalytic degradation of RhB with 98％yield for 2.5 h and reduction of Cr(VI) with more than 99％yield for 1.5 h at pH=2. Stability test shows BCN-3 still kept more than 98％reduction efficiency after 6 cycles. In addition, we also studied the reduction mechanism that shown the ·O2-radicals essentially helped to reduce the Cr(VI) in aqueous solution under illumination, verified the direct Z-scheme charge transfer path by X-ray photoelectron spectroscopy (XPS) and the free radical trapping experiment. The work open a new way for rationally designing photo-catalyst heterostructure to reduce Cr(VI) to Cr(III).     

Selective oxidation of benzyl alcohols to benzoic acid catalyzed by eco-friendly cobalt thioporphyrazine catalyst supported on silica-coated magnetic nanospheres

A novel magnetically recoverable thioporphyrazine catalyst (CoPz(S-Bu)8/SiO2@Fe3O4) was prepared by immobilization of the cobalt octkis(butylthio) porphyrazine complex (CoPz(S-Bu)8) on silica-coated magnetic nanospheres (SiO2@Fe3O4). The composite CoPz(S-Bu)8/SiO2@Fe3O4 appeared to be an active catalyst in the oxidation of benzyl alcohol in aqueous solution using hydrogen peroxide (H2O2) as oxidant under Xe-lamp irradiation, with 36.4% conversion of benzyl alcohol, about 99% selectivity for benzoic acid and turnover number (TON) of 61.7 at ambient temperature. The biomimetic catalyst CoPz(S-Bu)8 was supported on the magnetic carrier SiO2@Fe3O4 so as to suspend it in aqueous solution to react with substrates, utilizing its lipophilicity. Meanwhile the CoPz(S-Bu)8 can use its unique advantages to control the selectivity of photocatalytic oxidation without the substrate being subjected to deep oxidation. The influence of various reaction parameters on the conversion rate of benzyl alcohol and selectivity of benzoic acid was investigated in detail. Moreover, photocatalytic oxidation of substituted benzyl alcohols was obtained with high conversion and excellent selectivity, specifically conversion close to 70%, selectivity close to 100% and TON of 113.6 for para-position electron-donating groups. The selectivity and eco-friendliness of the biomimetic photocatalyst give it great potential for practical applications.     

地表水中典型全氟化合物的污染特性及降解机理研究

全氟化合物(PFCs)因其在环境介质中的稳定性、持久性和生物累积性,引起全球的广泛研究.基于对地表水中全氟化合物污染分布特性相关资料的分析,得出地表水中全氟化合物主要以PFOS和PFOA的形式存在.文章阐述了紫外光催化降解地表水中典型全氟化合物过程中不同催化剂的降解机制.总结了光催化降解的一般过程以及不同研究方法的基础技术的优缺点,提出了作者对地表水中典型全氟化合物降解技术的发展方向的看法.     

Photocatalytic degradation of phenol on different phases of TiO(2) particles in aqueous suspensions under UV irradiation

Photocatalytic degradation of phenol on different phases of TiO₂ particles was examined under 400-W UV irradiation. The effects of various operating parameters including TiO₂ dosage, solution pH (4–10), and initial phenol concentration (0.13–1.05 mM) on phenol degradation were investigated. Three forms of TiO₂ photocatalysts such as pure anatase phase, pure rutile phase, and the mixed phase were prepared by sol-gel method and followed annealing at different temperatures. The annealing temperature used were 500 °C, 700 °C and 900 °C for pure anatase phase, the mixed phase, and pure rutile phase, respectively. It was shown that pure anatase TiO₂ exhibited higher photocatalytic activity than the physical mixture of pure anatase and rutile TiO₂. Moreover, the TiO₂ particle with a specific fraction of mixed anatase and rutile phases exhibited better performance than pure anatase TiO₂. Finally, the degradation rate could be satisfactorily fitted by a pseudo-first-order kinetic model.     

Removal of elemental mercury by photocatalytic oxidation over La2O3/Bi2O3 composite

La₂O₃/Bi₂O₃ photocatalysts were prepared by impregnation of Bi₂O₃ with an aqueous solution of lanthanum precursor followed by calcination at different temperatures. The composite materials were used for the first time for the photocatalytic removal of Hg⁰ from a simulated flue gas under UV light irradiation. The results showed that the sample containing 6 wt.% La₂O₃ and calcined at 500°C has the highest dispersion of the active sites, which was promoted by the strong interaction with the support (i.e., the formation of Bi-O-La species). Since they are fully accessible on the surface, the material also exhibits excellent optical properties while the heterojunction formed in La₂O₃/Bi₂O₃ promotes the separation and migration of photoelectron-hole pairs and thus Hg⁰ oxidation efficiency is enhanced. The effects of the various factors (e.g., the reaction temperature and composition of the simulated flue gas (i.e., O₂, NO, H₂O, and SO₂)) on the efficiency of the Hg⁰ photocatalytic oxidation were investigated. The results demonstrated that O₂ and SO₂ enhanced the efficiency of the reaction while the reaction temperature, NO, and H₂O had an inhibitory effect.     

Inactivation of bacteria by sun light in a solar reactor with Immobilised TiO2

The photocatalytical inactivation of bacteria (Escherichia coli, Staphylococcus epidermidis,...) in the flow‐through plate solar reactor by sunlight was investigated. The low stability of bacteria in the reactor was attributed to bacteria sensitivity to mixing and/or gas bubbling. Sunlight inactivation proceeds with sufficient rate even under cloudy conditions.     

铁离子掺杂TiO2薄膜光催化降解无水肼废水的研究

研究Fe^3＋掺杂的TiO2薄膜对无水脐废水光催化降解作用,考察了影响Fe^3＋掺杂的TiO2薄膜光催化降解无水肼废水的效果的相关因素,结果表明：当Fe^3＋掺杂TiO2薄膜的摩尔分数为0．5％,煅烧温度为500℃,煅烧时间为3h,并且无水肼废水为中性或弱碱性,催化降解温度在30℃左右时,Fe^3＋掺杂的TiO2薄膜的催化效果最好。     

HAP/UV催化降解活性艳蓝K-3R的研究

用化学沉淀法合成羟基磷灰石(HAP),并用XRD、SEM、FT-IR对其进行分析。以活性艳蓝K-3R为降解底物,研究HAP对其光催化降解性能。探讨了HAP煅烧温度、通气量、投加量、初始浓度等因素对光催化降解活性艳蓝K-3R效果的影响。研究表明化学沉淀法合成的HAP粒度均匀,HAP对活性艳蓝的吸附作用较强,30min之内即能达到吸附平衡,其对初始浓度为100mg/L的活性艳蓝的吸附率可达17.5%。适当的煅烧有利于提高HAP的催化活性,以200℃煅烧2h最佳。在投加量为4g/L,鼓气量为300L/h和pH=6的试验条件下,HAP(200℃)对初始浓度为100mg/L的活性艳蓝K-3R 3h的降解率达68%。降解反应动力学研究表明,HAP/UV光催化降解活性艳蓝K-3R的过程符合Langmuir-Hinshel-wood一级动力学方程,降解速率常数k随着活性艳蓝K-3R浓度的增大而减小。     

Photocatalytic decomposition of acrylonitrile with N–F codoped TiO2/SiO2 under simulant solar light irradiation

The solid acid catalyst, N–F codoped TiO₂/SiO₂ composite oxide was prepared by a sol–gel method using NH₄F as nitrogen and fluorine source. The prepared materials were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), UV–Visible diffuse reflectance spectroscopy (UV–Vis), ammonia adsorption and temperature-programmed desorption (NH₃-TPD), in situ Fourier transform infrared spectroscopy (FT-IR) and N₂ physical adsorption isotherm. The photocatalytic activity of the catalyst for acrylonitrile degradation was investigated under simulant solar irradiation. The results showed that strong Lewis and Brønsted acid sites appear on the surface of the sample after N–F doping. Systematic investigation showed that the highest photocatalytic activity for acrylonitrile degradation was obtained for samples calcined at 450°C with molar ratio (NH₄F to Ti) of 0.8. The degradation ratio of 71.5% was achieved with the prepared catalyst after 6-min irradiation, demonstrating the effectiveness of photocatalytic degradation of acrylonitrile with N–F codoped TiO₂/SiO₂ composite oxide. The photocatalyst is promising for application under solar light irradiation. Moreover, the intermediates generated after irradiation were verified by gas chromatography–mass spectrometry (GC–MS) analysis and UV–Vis spectroscopy to be simple organic acids with lower toxicity, and the degradation pathway was also proposed for acrylonitrile degradation with the prepared catalyst.