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Materials Chemistry A Journal of Materials Chemistry A PAPER Novel Ag3PO4/CeO2 composite with high efficiency and stability for photocatalytic applications† Cite this: J. Mater. Chem. A,2014,2, 1750 Zheng-Mei Yang, Gui-Fang Huang,* Wei-Qing Huang,* Jia-Mou Wei, Xin-Guo Yan, Yue-Yang Liu, Chao Jiao, Zhuo Wan and Anlian Pan A novel Ag3PO4/CeO2 composite was fabricated by in situ wrapping CeO2 nanoparticles with Ag3PO4 through a facile precipitation method. The photocatalytic properties of Ag3PO4/CeO2 were evaluated by the photocatalytic degradation of MB and phenol under visible light and UV light irradiation. The photocatalytic activity of the composite is much higher than that of pure Ag3PO4 or CeO2. The rate constant of MB degradation over Ag3PO4/CeO2 is more than 2 times and 20 times than those of pure Ag3PO4 and CeO2 under visible light irradiation, respectively. The Ag3PO4/CeO2 composite photocatalyst also shows higher photocatalytic activity for the colorless phenol degradation compared to pure Ag3PO4. Moreover, the Ag3PO4/CeO2 sample has almost no loss of photocatalytic activity after five recycles under the irradiation of visible light and UV light, indicating that the composite has good photocatalytic stability. The excellent photocatalytic activity of the Ag3PO4/CeO2 composite is closely related to the fast Received 23rd October 2013 transfer and efficient separation of electron–hole pairs at the interfaces of the two semiconductors Accepted 5th November 2013 derived from the matching band positions between CeO2 and Ag3PO4. This newly constructed Ag3PO4/ DOI: 10.1039/c3ta14286h CeO2 composite, with promising and fascinating visible light-driven photocatalytic activity as well as www.rsc.org/MaterialsA good stability, could find potential applications in environmental purification and solar energy conversion. 1. Introduction dyes. The coupled semiconductor with a narrow band gap usually acts as a visible light sensitizer, and the photogenerated Semiconductor-based photocatalysis is a promising avenue to electrons or holes excited by visible light irradiation will trans- 21 ffi solve the worldwide energy shortage and environmental pollu- fer to the CeO2. Thus the high e ciency of the interfacial tion using the abundant solar light.1–7 Of the well-known pho- charge transfer as well as the stronger visible light absorption tocatalysts, cerium dioxide (CeO2), as a fascinating rare earth capacity results in the enhanced activity of the composite – material, has attracted much attention owing to its high activity, photocatalysts.21 25 However, the limited photocatalytic activity low cost and environmentally friendly properties.8–11 It shows is still a barrier for practical applications. Therefore, seeking an promising photoactivity for the degradation of organic pollut- appropriate sensitizer to form CeO2-based composites is a ants and water splitting for hydrogen generation.12 Neverthe- highly crucial task for achieving superior photocatalytic activity. 26,27 less, pristine CeO2 can only be excited by ultraviolet light (UV) Recently, Bi et al. have presented pioneering work on because of its wide band gap (about 3.2 eV), limiting its further exploring the photocatalytic properties of Ag3PO4, which 13 application in the visible light region. In order to highly utilize exhibits extremely high photooxidative capabilities for O2 solar energy, various methods, such as doping, noble metal evolution from water and the decomposition of organic dyes deposition and forming composites, have been designed to under visible-light irradiation. For example, the photo- enhance the absorption of CeO2 photocatalysts in the visible degradation rate of organic dyes over Ag3PO4 is dozens of times 14–17 light region. Among them, the most effective strategy is the faster than the rate over BiVO4 and commercial TiO2ÀxNx. coupling of two semiconductors, CeO2 and another semi- Moreover, most interestingly, this novel photocatalyst can 18 ffi conductor, to form a composite. So far, various CeO2-based achieve a quantum e ciency of up to 90% at wavelengths 14 composites with a visible light response, such as Cu2O–CeO2, greater than 420 nm, which is signi cantly higher than the 15 19 20 26–28 Bi2O3–CeO2, ZnO–CeO2 and BiVO4–CeO2, have been previously reported values. This nding potentially opens an reported to be efficient for the photodecomposition of organic avenue for solving the current energy crisis and environmental problems using the abundant solar light. Unfortunately, the low Department of Applied Physics, Key Laboratory for Micro-Nano Physics and Technology structural stability of pure Ag3PO4 strongly limits its practical of Hunan Province, Hunan University, Changsha 410082, China. E-mail: guang@ environmental applications. hnu.edu.cn; [email protected]; [email protected] Considering the unique photocatalytic activity and its † Electronic supplementary information (ESI) available. See DOI: limitations, coupling Ag3PO4 with other photocatalysts could be 10.1039/c3ta14286h 1750 | J. Mater. Chem. A,2014,2,1750–1756 This journal is © The Royal Society of Chemistry 2014 Paper Journal of Materials Chemistry A regarded as a good strategy to design efficient and stable pho- 2.3 Photocatalytic activity test tocatalysts. Moreover, beneting from the relatively small band The photocatalytic behavior for the degradation of methylene gap (the indirect and direct band gaps are 2.36 eV and 2.43 eV, À1 blue (MB, 10 mg L , 80 mL) with 30 mg of the photocatalysts 29 respectively), Ag3PO4 is an ideal candidate to be a sensitizer (CeO2,Ag3PO4 or Ag3PO4/CeO2) under irradiation was explored. which absorbs visible light to improve the photocatalytic A low-power 5 W compact uorescent lamp equipped with a UV activity in the composite system. In this paper, we report a facile cutoff lter (l > 400 nm) and a 300 W UV lamp were chosen as process to synthesize a newly constructed Ag PO /CeO 3 4 2 the visible light and UV light source, respectively. Prior to composite by an in situ precipitation method. The results show irradiation, solutions suspended with photocatalysts were that the novel composite photocatalyst displays much higher sonicated in the dark for 10 min to ensure the adsorption– activity than that of single Ag PO or CeO under the irradiation 3 4 2 desorption equilibrium of MB on the surface of the photo- of visible light as well as UV light. Moreover, the prepared catalysts. During irradiation, the samples were withdrawn at Ag PO /CeO composite shows good stability. This work 3 4 2 regular time intervals and centrifuged to remove the catalysts. provides a possible way to develop new visible light-responsive The photodegradation efficiency was monitored by measuring photocatalysts with excellent activity and good stability, thus the absorbance of the solution samples at its characteristic meeting the requirements of future environmental and energy absorption wavelength of 663 nm (MB) with a UV-Vis spectro- technologies. photometer at room temperature. To further investigate the visible light photocatalytic activity, a colorless compound, phenol, was also chosen as a model 2. Experimental section pollutant since phenol shows no absorption in the visible 2.1 Photocatalyst synthesis region. A 55 W compact uorescent lamp equipped with a UV cutoff lter (l > 400 nm) was used as the light source. The visible CeO2 nanoparticles were synthesized by the low-temperature light photocatalytic activity of the Ag PO or Ag PO /CeO solution combustion method using citric acid as the fuel, 3 4 3 4 2 samples for the degradation of phenol was tested with a UV-Vis followed by annealing at 500 C. The preparation of the spectrophotometer. Ag3PO4/CeO2 composite structures was carried out by an in situ precipitation method. All of the reagents were of analytical grade and used without further purication. In a 3. Results and discussion typical synthesis process, 0.1 g of as-prepared CeO2 nano- 3.1 Morphology and structure characterization of catalyst particles were dispersed in 150 mL deionized water and sonicated for 30 minutes. Immediately aer sonication, SEM was used to investigate the morphology and size of the À1 AgNO3 aqueous solution (100 mL, 0.012 mol L ) was added prepared samples. The typical SEM images of pure CeO2,Ag3PO4 to the white CeO2 dispersed solution, followed by magnetic and the Ag3PO4/CeO2 composite are displayed in Fig. 1. The À1 stirring. Na2HPO4 aqueous solution (200 mL, 0.003 mol L ) morphology of pure CeO2 (Fig. 1(a)) shows spherical-shaped was then added dropwise, accompanied with thorough stir- nanoparticles with diameters of about 40 nm, whereas pure ring until the color of the solution changed from white to Ag3PO4 (Fig. 1(b)) is found to consist of agglomerated grains yellow. The precipitate was centrifuged and washed several composed of irregular particles with approximately 200 nm times with deionized water and absolute ethanol, and dried dimensions. The SEM image in Fig. 1(c) and the TEM observation at 60 C. For comparison, Ag3PO4 particles were also prepared under the same conditions without the presence of CeO2 nanoparticles. 2.2 Characterization The crystallographic structures of the samples were charac- terized by power X-ray diffraction (XRD, Siemens D-5000 diffractometer with Cu Ka irradiation) and high-resolution transmission electron microscopy (HRTEM, FEI Tecai F20). The morphological details of the prepared samples were pro- bed by eld emission scanning electron microscopy (FESEM, S-4800) and TEM. The optical absorption spectra of the samples were recorded using a UV-Vis spectrometer (UV-2450, Shimadzu). The Brunauer–Emmett–Teller (BET) specic surface area of the samples was analyzed by nitrogen adsorp- tion using a Micromeritics ASAP 2020 nitrogen adsorption apparatus. The photophysics of the excited states generated by absorption was investigated by surface photovoltage spec- Fig. 1 SEM images of (a) CeO2, (b) Ag3PO4, (c) Ag3PO4/CeO2 troscopy (SPS) measurements. composite, and (d) HRTEM image of the Ag3PO4/CeO2 composite. This journal is © The Royal Society of Chemistry 2014 J. Mater. Chem. A,2014,2,1750–1756 | 1751 Journal of Materials Chemistry A Paper shown in the inset of Fig.
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