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The g-C3N4/NaTaO3 composite showed the enhanced photocatalytic activity for degradation of rhodamine B dye (Rh

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P-94 2014년도 한국표면공학회 추계학술대회 논문집 g-C3N4/NaTaO3 복합체의 제조 및 태양광 조사 하에서의 광촉매 특성 평가

Preparation and characterization of g-C3N4/NaTaO3 composite and their photocatalytic activity under simulated solar light

박지수a*, 김태호b, 조용현c, 이수완d

a*선문대학교 나노화학과(E-mail:jisu0519@naver.com), b선문대학교 정보디스플레이학과, c선문대학교 재료금속공학과,

d선문대학교 환경생명화학공학과

초 록: This Paper reports the photocatalytic activity of g-C3N4/NaTaO3 hybrid composite photocatalysts synthesized by ball-mill method. The g-C3N4 and NaTaO3 were individually prepared by Solid state reaction and microwave hydrothermal process, respectively. The g-C3N4/NaTaO3 composite showed the enhanced photocatalytic activity for degradation of rhodamine B dye (Rh. B) under simulated solar light irradiation. The results revealed that the band-gap energy absorption edge of hybrid composite samples was shifted to a longer wavelength as compared to NaTaO3 and the 50 wt%

g-C3N4/NaTaO3 hybrid composite exhibited the highest percentage (99.6 %) of degradation of Rh. B and the highest reaction rate constant (0.013 min-1) in 4 h which could be attributed to the enhanced absorption of the hybrid composite photocatalyst in the UV-Vis region. Hence, these results suggest that the g-C3N4/NaTaO3 hybrid composite exhibits enhanced photocatalytic activity for the degradation of rhodamine B under simulated solar light irradiation in comparison to the commercial NaTaO3.

1. 서론

In recent year, semiconductor photocatalysts have been attracted much attention because of their high photocatalytic activity, high stability, non-toxicity and environmentally-harmonious characteristics.1-3 TiO2 photocatalysts are presently the most actively and widely investigated for applications that can effectively address environmental pollution.4-6 Recently, NaTaO3 has been used as a photocatalyst for water splitting and environmental remediation under UV light irradiation due to its physical, chemical and structural properties.7-9 Moreover, NaTaO3 has favorable band edge potentials and delocalized nature of photoexcited electrons which are primary reasons for higher efficiency.10-12 Recent studies have shown that the photocatalytic activities of doping rare-earth and hybrid composite into the perovskite type alkali tantalates have been significantly improved. These coupling of different semiconductor photocatalysts may increase the photocatalytic efficiency by enhancing the charge separation and extending the photo-formed electron.hole pairs under irradiation.

2. 본론

In this study, the microwave hydrothermal synthesis was used to prepare NaTaO3 and then g-C3N4 was prepared by solid state reaction. Finally, g-C3N4/NaTaO3 hybrid composite were prepared by ball-mill method. The photocatalytic activity of the g-C3N4/NaTaO3 composite was performed by degradation of Rh B dye in aqueous solution under simulated solar light irradiation. Figure 1 shows the XRD patterns of the g-C3N4/NaTaO3 composite with various g-C3N4 amounts with a range of g-C3N4 content from 0 wt% to 50 wt%. The monoclinic phase NaTaO3 has been obtained by microwave hydrothermal method at 180 ℃ for 8 h. These characteristic reflections can be readily indexed as the cubic phase (100), (110), (111), (020), (102), (211) and (220) planes, according to (JCPDS#742477). In the XRD patterns of g-C3N4/NaTaO3 composites, no change was observed in the crystal structure of NaTaO3 but a new peak was appeared at 27.4 °. The inset of Figure 1 shows a magnified image of the diffraction peaks for the (002) plane of g-C3N4. The peak at 27.4 °, could be indexed to graphitic materials as the (002) peak, which is attributed to the interplanar striking of the aromatic compound.

Moreover, intensity of this diffraction peaks was increased with increasing content of g-C3N4. The schematic of the charge separation and transport of photoinduced charge carrier at the interface of the g-C3N4/NaTaO3 composite under simulated solar light is shown in Figure 2. The photoinduced holes migrate from NaTaO3 to the valence band (VB) of g-C3N4 which supresses the recombination of photoinduced electron.hole pairs. In addition, g-C3N4 and surface in g-C3N4/NaTaO3 hybrid composite can act as electron traps and prevents the recombination of the electron-hole pairs.

These facts together could be attributed for the enhanced photocatalytic activity of the g-C3N4/NaTaO3 composite.

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Figure 1. XRD patterns of photocatalysts: (a) NaTaO3, (b) 10 wt% g-C3N4/NaTaO3, (c) 30 wt% g-C3N4/NaTaO3 and (d) 50 wt% g-C3N4/NaTaO3. The inset shows the magnification of the diffraction peaks around 27 °.

h+ Solar light

h+ e- e-

NaTaO3 (4.12 eV)

g-C3N4 (2.74 eV) O(H2/H+)

O2 O2-

H2O OH- Oxidation

CB

VB

CB

VB

Figure 2. Schematic illustrating the mechanism of degradation of dye by g-C3N4/NaTaO3 under solar light irradiation.

3. 결론

Solar-light-responsive g-C3N4/NaTaO3 hybrid composite was successfully prepared by the ball-mill method. Diffuse reflectance UV-vis spectra of 50 wt% g-C3N4/NaTaO3 composite revealed the lowest band gap energy of about 2.81 eV.

The highest efficiency was observed for 50 wt% g-C3N4/NaTaO3 hybrid composite. The enhanced photocatalytic performance could be attributed to synergistic effects of band gap lowering, photoinduced electron-hole pair at the interface and the larger surface area of the g-C3N4/NaTaO3 hybrid composite photocatalysts which promote the migration effciency of electron.hole pairs leading to enhanced photocatalytic degradation of Rh. B dye under simulated solar light irradiation.

참고문헌

1. I. Sopyan, M. Watanabe, S. Murasawa, K. Hashimoto, and A. Fujishima, J. Photochem. Photobiol. A: Chem. 98, 79 (1996).

2. A. Fujishima, T. N. Rao, and D. A. Tryk, J. Photochem. Photobiol. C: Photochem. Rev. 1, 1 (2000).

3. Y. Paz, Z. Luo, L. Rabenberg, and A. Heller, J. Mater. Res. 10, 2842 (1995).

4. M. R. Hoffmann, S. T. Martin, W. Choi, and D. W. Bahnemann, Chem. Rev. 95, 69 (1995).

5. A. Heller, Acc. Chem. Res. 14, 154 (1981).

6. M. Anpo and Y. Kubokawa, Res. Chem. Intermed. 8, 105 (1987).

7. H. Kato and A. Kudo, Chem. Phys. Lett. 295, 487 (1998).

8. A. Kudo and H. Kato, Chem. Phys. Lett. 331, 373 (2000).

9. A. Kudo, H. Kato, and I. Jsuji, Chem. Lett. 33, 1534 (2004).

10. H. Kato and A. Kudo, J. Phys. Chem. B 105, 4285 (2001).

11. C. C.Hu, C. C. Tsai, andH. Teng, J. Am. Ceram. Soc. 92, 460 (2009).

12. A. Yamakata, T. Ishibashi, H. Kato, A. Kudo, and H. Onishi, J. Phys. Chem. B 107, 14383 (2003).

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