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Materials Chemistry and Physics 126 (2011) 847–852 Contents lists available at ScienceDirect Materials Chemistry and Physics journal homepage: www.elsevier.com/locate/matchemphys Enhanced photocatalytic activity of flowerlike Cu2 O/Cu prepared using solvent-thermal route Bo Zhou a , Hongxia Wang b , Zhiguo Liu a,∗ , Yanqiang Yang a , Xiqiang Huang a , Zhe Lü a , Yu Sui a,c , Wenhui Su a,c a b c Center for Condensed Matter Science and Technology, Department of Physics, Harbin Institute of Technology, Harbin 150080, PR China College of Chemistry & Chemical Engineering, Harbin Normal University, Harbin 150025, PR China International Center for Materials Physics, Academia Sinica, Shenyang 110015, PR China a r t i c l e i n f o Article history: Received 9 April 2009 Received in revised form 8 November 2010 Accepted 13 December 2010 Keywords: Nanocomposite materials Chemical synthesis Electron microscopy Heterostructures a b s t r a c t Cu2 O/Cu nanocomposites (NCs) with flowerlike nano-architecture were prepared using template-free stepwise solvent-thermal synthesis route with Cu(NO3 )2 ·3H2 O as a precursor. With the precursor concentration increasing gradually from 0.01 to 0.1 M, the morphology of the NCs evolves from nano-flower to microsphere. The content of Cu in the NCs can be easily controlled by adjusting the concentration of precursor and synthesis time. Using photocatalytic degradation of monoazo dye Procion Red MX-5B (PR) and phenol as the probe molecules under visible-light illumination, we have investigated the influence of Cu on the photocatalytic activity of Cu2 O. When the content of Cu lies in the range of 27–71 wt%, the samples exhibit higher photocatalytic performance, indicating that these flowerlike Cu2 O/Cu NCs are promising candidates for pollutant processing. © 2010 Elsevier B.V. All rights reserved. 1. Introduction Environmental protection calls for efficient ways and means to process waste and emissions, e.g., polluted water, which provides the impetus for sustained fundamental and applied researches in the field of environmental remediation. Semiconductor-based photocatalysts [1] have attracted much attention because of their low cost, cleanliness, high stability, and easy availability. TiO2 and ZnO are the most commonly used photocatalysts, however, they need to be activated by ultraviolet (UV) light because of their broad band gap (3.0–3.2 eV), hence only less than 5% solar energy can be utilized [2–5]. On the contrary, cuprous oxide (Cu2 O), with a direct band gap of ca. 2.2 eV, could be activated by visible light, making it a promising candidate for better utilization of solar energy, e.g., solar energy conversion [6], photocatalytic degradation of organic pollutants [7] and decomposition of water into O2 and H2 [8]. Nevertheless, a pure-phase semiconductor exhibits very low quantum efficiency due to the quick recombination of photoelectrons and holes. An efficient way to improve the quantum efficiency is to add noble metal (e.g., Ag, Au, Cu and Pt) into metal oxide, because the quick transfer of the photogenerated electrons by the metal can prevent the recombination. As a result, the ∗ Corresponding author. Tel.: +86 451 86402772; fax: +86 451 86418440. E-mail addresses: zhoubo [email protected], [email protected] (Z. Liu). 0254-0584/$ – see front matter © 2010 Elsevier B.V. All rights reserved. doi:10.1016/j.matchemphys.2010.12.030 metal/semiconductor heterostructures exhibit an excellent photocatalytic activity [9–15]. Therefore, it is highly desirable to develop a synthetic route for the production of metal/metal oxide composites. On the other hand, the activity of a catalyst also depends on its structural parameters, such as geometry and morphology. Nanoparticles [16,17] and porous/hollow structures [18–20] effectively increase the area of surface and interface, which enhances not only the adsorption and desorption of reactants (or products), but also light harvesting, thereby improves the catalytic activity. In the past decade, much efforts have been devoted to the shape-controlled synthesis of Cu2 O micro- and nanocrystals, such as nanowires [21], nanocubes [22], hollow spheres [23], and mesoporous nanoflowers [24]. To the best of our knowledge, few results were reported on the synthesis and photocatalytic property of Cu2 O/Cu NCs. In order to develop an efficient photocatalyst that can sufficiently utilize solar energy, Cu2 O/Cu NCs were prepared in this study. The in situ synthesis of Cu2 O/Cu NCs was developed with a template-free stepwise solvent-thermal route to control its morphology and phase composition. The effect of reaction time and precursor concentration on its phase composition and morphology, and the effect of the content of Cu in composite Cu2 O/Cu photocatalysts on photocatalytic activity was investigated. The flowerlike Cu2 O/Cu NCs show high photocatalytic activity, indicating their potential applications in the future. 848 B. Zhou et al. / Materials Chemistry and Physics 126 (2011) 847–852 Table 1 Experimental conditions, phase composition and characterized parameters of different samples, where SBET , dP and VP are specific surface area, pore diameter and pore volume, respectively. 2.1. Preparation of Cu2 O/Cu nanoflowers Cu2 O/Cu nanoflowers were synthesized using Cu(NO3 )2 ·3H2 O as the precursor by a typical two-step method similar to Ref. [25]. Cu(NO3 )2 ·3H2 O was dissolved in an organic solvent N,N-dimethylformamide (DMF) with a concentration range of 0.01–0.1 M. 35 mL of this transparent blue solvent was sealed in a Teflon-lined stainless steel autoclave with a capacity of 50 mL, and heated at 150 ◦ C for 24 h in electric oven, and then further heated at 180 ◦ C for 8–26 h. The autoclave was slowly cooled down to room temperature in the oven. The precipitation was separated from the solution by centrifugation, then washed with alcohol for several times, and finally dried at 70 ◦ C for 5 h in a vacuum oven. The denotations of samples prepared at different conditions are shown in Table 1. 2.2. Characterization The samples were characterized by X-ray powder diffraction (XRD) using a Rigaku 12 kW X-ray diffractometer with Cu K␣ radiation ( = 0.15418 nm). Their morphology and size distribution were determined by a JEM-S4800 field-emission scanning electron microscope (FESEM) operated at 15 kV. N2 adsorption–desorption isotherms were obtained using a Quantachrome Autosorb1 apparatus. Barret–Joyner–Halenda (BJH) method was employed to determine the pore diameter (dP ) and pore volume (VP ). The specific surface area (SBET ) was calculated using the Brunauer–Emmett–Teller (BET) method. 2.3. Adsorption and photocatalytic activity The adsorption behavior and photocatalytic activity of the Cu2 O/Cu NCs were evaluated by the degradation of the solution of monoazo dye Procion Red MX5B (PR, Aldrich) and phenol at a concentration of 10 mg L−1 . 0.030 g Cu2 O/Cu NC powder was dispersed in a 50 mL probe molecular aqueous solution. Before illumination, the suspension was stirred in dark for more than 120 min to achieve an adsorption/desorption equilibrium of organic molecules on the surface of Cu2 O/Cu NCs. The photocatalytic reaction was carried out at room temperature by using a 40 W tungsten lamp as a visible-light source. At different time intervals during the experiment, 5 mL of solution was sampled for analysis. After centrifugation at 11,000 rpm for 10 min, the absorbance of solution was measured using a UV–visible spectrophotometer. 3. Results and discussion 3.1. Phase composition Fig. 1 shows the XRD patterns of a series of samples prepared with different precursor concentrations at 180 ◦ C for 24 h. All the samples are found to be composite materials, which are characterized by the two sets of diffraction peaks, i.e., Cu2 O (space group Pn3m; a0 = 0.4252 nm; JCPDS 05-0667) and cubic Cu (space group Fm3m; a0 = 0.3613 nm; JCPDS 04-0836). With increasing precursor concentration, the relative intensity of Cu2 O (1 1 1) peak increases, indicating the higher content of Cu2 O in the NCs. The mass fraction of Cu2 O in the NCs can be calculated using the relative ratio [26]: ICu2 O(1 1 1) ICu2 O(1 1 1) + ICu(1 1 1) 16.4 16.9 9.6 4.2 5.5 29.1 8.6 12.2 12.5 1.888 3.774 3.704 3.750 3.748 1.888 3.774 2.993 2.143 0.0156 0.0152 0.0106 0.0048 0.0052 0.0334 0.0096 0.0111 0.0117 where ICu2 O(1 1 1) and ICu(1 1 1) are the height of the characteristic diffraction peaks of Cu2 O (1 1 1) and Cu (1 1 1) planes, respectively. The content of Cu2 O increases from 29 wt% to 89 wt% when the precursor concentration increases from 0.01 M to 0.1 M, as shown in Table 1. 3.2. Structure and morphology Fig. 2 shows the relationship between the morphology and the precursor concentration. At low precursor concentration of 0.01 M (S1, Fig. 2a) and 0.02 M (S2, Fig. 2b), flowerlike morphology is formed, whose “petals” are approximately 300–500 nm long and 30–70 nm wide (the inset of Fig. 2a). At the concentration of 0.03 M (S3), the petals become shorter and smaller and some of them even aggregate into spheres of 500–800 nm in diameter (Fig. 2c). When the precursor concentration increases to 0.05 M (S5), the products become cubes or octohedra with a few small nanobelts standing on them, whose edge length is 500–800 nm (Fig. 2d). No flowerlike structures can be seen at the precursor concentration of 0.1 M (S10, Fig. 2e), while the mixture of large porous spheres and octahedra appears instead. The spheres are of about 10 m in diameter, whereas the octahedra are relatively small, with an edge length of 300–600 nm. Highly magnified SEM images of S10 are shown in Fig. 2f. The broken spherical particle (the inset at the top left corner of Fig. 2f) indicates that the big spherical assemblies are not hollow, and the other magnified image of the surface of sphere (at the right bottom corner of Fig. 2f) indicates a mesoporous structure. It can be concluded that the precursor concentration has a significant effect on the morphology of the products. This concentration-dependent self-assembly allows S10 20 A: Cu2O B: Cu A (311) 2. Experimental 29 46 72 81 89 100 73 44 15 S5 S3 S2 S1 30 40 50 B (220) 71 54 28 19 11 – 27 56 85 VP (cm3 g−1 ) A (220) 24 24 24 24 24 8 14 24 26 dP (nm) B (200) 0.01 0.02 0.03 0.05 0.1 0.01 0.01 0.01 0.01 SBET (m2 g−1 ) A (200) S1 (S 1-24) S2 S3 S5 S10 S1-8 S1-14 S1-20 S1-26 Cu2 O (wt%) B (111) Cu (wt%) A (111) Secondary reaction time (h) A (110) Precursor concentration (M) Relative Intensiy (arb.units) Sample 60 70 o 2θ ( ) (1) Fig. 1. XRD patterns of S1, S2, S3, S5 and S10. 80 B. Zhou et al. / Materials Chemistry and Physics 126 (2011) 847–852 849 Fig. 2. FESEM images of Cu2 O/Cu NCs prepared at different precursor concentrations: (a) 0.01 M, (b) 0.02 M, (c) 0.03 M, (d) 0.05 M and (e) 0.1 M. (f) Enlarged images of (e). The inset of (a) is a magnified image. The inset on the top left of (f) shows a broken spherical particle, and the other one at the bottom shows a highly magnified image of the surface of a sphere. selective synthesis of nano-flowerlike architectures or mesoporous spheres by changing precursor concentration, which is of great importance for designing catalysts with high activity. When the reaction time was prolonged from 8 h to 26 h at the second step (180 ◦ C), the flowerlike structure obtained at 0.01 M exhibits little change on morphology (Fig. 3) even though its phase composition is changed (Table 1). As calculated from XRD results (Fig. 4), the corresponding content of Cu increases from 27 wt% to 85 wt% when the time increases from 14 h (S1-14) to 26 h (S1-26). In the experiments, DMF acts as the reducing agent. As described by Zeng et al. [25,27], solid CuO forms only after reaction for 1.5–2 h at 150 ◦ C, then it is reduced to Cu2 O, and further reduced into metal Cu after longer reaction. Moreover, the physical and chemical processes can be accelerated at higher processing temperature. The redox chemical process can be described as follows: HCON(CH3 )2 + H2 O → HCOOH + NH(CH3 )2 (2) Cu2+ + H2 O + 2NH(CH3 )2 → CuO + 2NH(CH3 )2+ (3) CuO + HCOOH → Cu2 O + H2 O + CO2 (4) Cu2 O + HCOOH → Cu + H2 O + CO2 (5) In fact, formic acid HCOOH in Eq. (2) is generated through hydrolysis of DMF, and acts as a reducing agent. The small amount of water comes from the starting regent Cu(NO3 )2 ·3H2 O. The reaction time plays a crucial role on the ratio of Cu2 O to Cu in the NCs. Therefore, by controlling the reaction time at the second step, the phase composition of the products can be adjusted without changing the morphology. 3.3. N2 adsorption–desorption Fig. 5 shows the N2 adsorption–desorption isotherm of S1, which is representative for all the flowerlike samples. The isotherm exhibits type IV hystersis, indicating S1 is porous. The corresponding parameters are listed in Table 1. As shown in the inset of Fig. 5, the pore size of S1 ranges from 3 to 15 nm, which can be attributed to the aggregation of primary nanoparticles. 850 B. Zhou et al. / Materials Chemistry and Physics 126 (2011) 847–852 Fig. 3. SEM images of flowerlike Cu2 O/Cu NCs obtained in a 0.01 M Cu(NO3 )2 ·3H2 O solution at 180 ◦ C for (a) 8 h, (b) 14 h, (c) 20 h and (d) 26 h. 3.4. Photocatalytic activity 12 dv/dD (cm3/g/nm) 10 Volume (cm 3/g) Fig. 6 shows the absorption spectra of PR solution with the presence of S1 at different visible light irradiation times. The strong absorption peak that lies at about 512 nm is selected to monitor the photocatalytic degradation process. With longer irradiation time, this characteristic peak becomes weaker. No new adsorption peaks appear, and no obvious shift of the characteristic peak is observed, indicating the degradation of PR. After the irradiation time of 60 min, PR is completely decolorized. Shown in Fig. 7 is the photocatalytic activity of S1, S2, S3, S5 and S10, which is characterized by the initial concentration (C0 ) and the concentrations at different time intervals (C). Without catalyst, PR cannot be degraded under visible-light irradiation, whereas 0.0003 8 0.0002 0.0001 0.0000 6 0 5 10 15 20 Pore Diameter (nm) Adsorption 4 Desorption 2 0 0.0 0.2 0.4 0.6 0.8 1.0 A: Cu2O Fig. 5. N2 adsorption–desorption BET isotherms of sample S1. The inset shows the pore size distribution. B (220) B (200) B (111) S1-26 B: Cu 0.14 S1-24 Absorbance A (311) A (220) A (200) A (111) S1-14 S1-8 0 min 0.12 S1-20 A (110) Relative Intensiy (arb.units) Relative Pressure (P/P0) PR 0.10 0.08 0.06 20 min 40 min 0.04 0.02 60 min 0.00 20 30 40 50 60 70 80 o 2θ ( ) Fig. 4. The XRD patterns of the flowerlike Cu2 O/Cu NCs. The Cu (2 2 0) is marked by the dashed line. 400 500 600 700 800 Wavelength (nm) Fig. 6. Absorption spectra of PR solution with the presence of S1. B. Zhou et al. / Materials Chemistry and Physics 126 (2011) 847–852 (a) 1.0 0.6 0.4 Irradiation 0 min Absorbance C/C0 0.8 Phenol 0.6 Without catalyst S1 S2 S3 S5 S10 851 20 0.4 40 60 0.2 80 100 0.2 120 0.0 0.0 240 0 20 40 60 80 100 260 Irradiation time (min.) 280 300 320 340 Wavelength (nm) 120 (b) 1.0 Fig. 7. Relative concentration (C/C0 ) of PR versus time under visible-light irradiation with S1, S2, S3, S5 and S10 as photocatalysts. it can be easily decolorized with the presence of Cu2 O/Cu NCs. Among these NCs, the performance of S10 is relatively low, while S1 exhibits the highest performance. As shown in Table 1, the specific surface areas of S10 and S1 are 5.5 m2 g−1 and 16.9 m2 g−1 , respectively. It is generally accepted that the catalytic process is closely related to the adsorption and desorption of molecules on the surface of the catalyst [28]. The large specific surface area of S1 enhances its adsorption ability and consists in its high performance. It should also be noted that the mass ratio of Cu2 O to Cu in the NCs plays an important role on the photocatalytic activity. The photocatalytic activities of S1-8, S1-14, S1-20, S1-24 (S1) and S1-26 are shown in Fig. 8, which possess flowerlike morphology and different contents of Cu (Table 1). At an irradiation time of 120 min, PR is completely degraded with the presence of S1-14, S1-20 and S124. On the contrary, the photocatalytic performances of S1-8 (pure Cu2 O) and S1-26 (with a high Cu content) are relatively low. As shown in Figs. 7 and 8, within the first 20 min of irradiation, a very high rate of dye degradation is observed, namely, more than 90% for Cu2 O/Cu NCs. In fact, the absorption of PR lies in the range of 440–580 nm with max = 512 nm. With the presence of PR, a large amount of light becomes inaccessible to catalyst particles [29,30]. A possible mechanism for the photocatalytic process can be described as follows. The electrons are injected from photoexcited PR molecules to the conduction band of Cu2 O, and the adsorbed O2 can scavenge the injected electrons, which prevents the recombination, hence the degradation of the electron-deficient PR is ensured. 1.0 S1-8 S1-14 C/C0 0.8 S1-20 S1-24 0.6 S1-26 0.4 0.2 0.0 0 20 40 60 80 100 120 Irradiation time (min.) Fig. 8. Relative concentration (C/C0 ) of PR versus time under visible-light irradiation with the presence of flowerlike Cu2 O/Cu NCs possessing different Cu contents. C/C0 0.8 0.6 S1-8 S1-14 S1-20 0.4 S1-24 S1-26 0.2 0 20 40 60 80 100 120 Irradiation time (min) Fig. 9. (a) Absorption spectra of phenol solution with the presence of S1. (b) Relative concentration (C/C0 ) of phenol versus time under visible-light irradiation with the presence of flowerlike Cu2 O/Cu NCs possessing different Cu contents. When 90% of PR is decomposed, the decrease of degradation rate is largely due to the low dye concentration. Phenol is transparency for visible light and very hard to mineralize due to its resonance stability. Shown in Fig. 9(a) are the absorption spectra of phenol solution with the presence of S1. The strong absorption peak at about 269 nm is selected to monitor the photocatalytic degradation process. With longer irradiation time, this characteristic peak becomes weaker and weaker, indicating the degradation of phenol. Fig. 9(b) shows the photocatalytic performance of Cu2 O/Cu NCs, whose Cu contents are different, on the degradation of phenol. Compared with PR, the maximum degradation rate of phenol is only 40% within the first 20 min of irradiation. For pure Cu2 O nanoparticles, only a degradation rate of 15% is observed. Consisted in PR, Cu2 O/Cu NCs exhibit better photocatalytic performance than pure Cu2 O. According to the theory of metal/semiconductor heterostructure catalysis [20,31–33], the photocatalytic activity of semiconductor-based heterostructure depends greatly on the concentration of heterostructure interface and defect, which can increase the separation efficiency of photogenerated electron–hole pairs. The metal on the surface of semiconductor acts as a sink for the electrons, which promotes interfacial charge-transfer kinetics between the metal and semiconductor, improves the separation of photogenerated electron–hole pairs, thus increases photocatalytic activity [31]. In Cu2 O/Cu NCs, the interfaces between Cu and Cu2 O act as the sites where rapid separation of photogenerated electrons and holes occurs. On the other hand, very high content of Cu (S1-26, 85 wt%) does not favor high photocatalytic activity, since Cu becomes recombination centers for electrons and holes instead [34]. Therefore, the mass fraction of Cu in the NCs also 852 B. Zhou et al. / Materials Chemistry and Physics 126 (2011) 847–852 influences photocatalytic activity. However, detailed degradation mechanism has not been clear yet. Further work is needed for better understanding of this issue. 4. Conclusions Flowerlike Cu2 O/Cu photocatalysts have been synthesized by following a two-step solvent-thermal synthesis route without using any templates and additives. The precursor concentration has a strong effect on the microstructure and phase composition of the Cu2 O/Cu NCs. The flowerlike structure is formed in a precursor concentration range of 0.01–0.02 M. The content of Cu increases with increasing reaction time or decreasing precursor concentration. As visible light photocatalysts, Cu2 O/Cu NCs exhibit better photocatalytic performance than the pure-phase Cu2 O. Our stepwise route offers an effective way to control the synthesis of Cu2 O/Cu NCs, and may shed light on the design of other well defined complex nanostructures. 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