臺灣博碩士論文加值系統

摘要 I
Abstract III
致謝 V
目錄 VII
表目錄 IXX
圖目錄 X
第一章 緒論 1
1-1 研究動機 1
1-2 研究目的及內容 2
第二章 文獻回顧 3
2-1 高級氧化處理法 3
2-1.1 光催化(Photocatalysis) 3
2-2 偶氮染料 4
2-3 氧化銅鉍(CuBi2O4)特性及合成方法 8
2-3.1 CuBi2O4之金屬氧化物複合觸媒 11
2-4 磷酸銀(Ag3PO4)特性及合成方法 17
2-4.1 Ag3PO4之金屬氧化物複合觸媒 19
第三章 實驗方法 22
3-1 研究架構 22
3-2 藥品及儀器 24
3-3 實驗流程及變因 26
3-3.1 觸媒命名 26
3-4 物性分析 45
3-4.1 X光繞射分析儀(X-Ray Diffraction, XRD) 45
3-4.2 紫外-可見光光譜儀(Ultraviolet-Visible Spectroscopy, UV-vis) 46
3-4.3 X射線光電子能譜(X-Ray Photoelectron Spectroscopy, XPS) 46
3-4.4 比表面積分析儀(Brunauer-Emmett-Teller, BET) 47
3-4.5 掃描式電子顯微鏡(Scanning Electron Microscope, SEM) 48
3-4.6 穿透式電子顯微鏡(Transmission Electron Microscope, TEM) 49
3-4.7 粒徑分析儀(Particle Size Analyzer) 49
3-4.8 界達電位儀(Zeta Potential) 49
3-4.9 感應耦合電漿發射光譜儀(Inductively Coupled Plasma Optical Emission Spectrometry, ICP-OES) 50
3-4.10 光激螢光分光光譜儀(Photoluminescence, PL) 50
3-5 光催化活性實驗 50
3-5.1 直接光解實驗 52
3-5.2 暗吸附實驗 52
3-5.3 紫外光實驗 53
3-5.4 可見光實驗 53
3-5.5 pH效應實驗 54
3-5.6 活性物種捕捉實驗 54
3-5.7 重複再使用實驗 55
3-5.8 金屬溶出實驗 55
3-5.9 太陽光光催化實驗 55
3-5.10 反應動力學模擬 56
第四章 結果與討論 57
4-1 觸媒樣品 57
4-2 表面特性分析 58
4-2.1 晶相分析 58
4-2.2 掃描式電子顯微鏡分析 65
4-2.3 穿透式電子顯微鏡分析 73
4-2.4 電子-電洞對再結合率分析 78
4-2.5 表面電性分析 79
4-2.6 觸媒光譜吸收範圍及能隙值分析 81
4-2.7 元素組成與鍵結分析 83
4-2.8 比表面積及孔徑分析 93
4-3 光催化活性實驗結果 93
4-3.1 直接光解 93
4-3.2 Ag3PO4光催化實驗結果 94
4-3.3 CuBi2O4光催化實驗結果 99
4-3.4 一步驟溶劑熱法光催化實驗結果 102
4-3.5 一步驟水熱法光催化實驗結果 103
4-3.6 二步驟光催化實驗結果 107
4-3.7 觸媒物理混合光催化實驗結果 109
4-3.8 觸媒再現性實驗 110
4-3.9 觸媒重複再使用實驗 110
4-3.10 pH效應實驗 113
4-3.11 金屬溶出實驗 114
4-3.12 太陽光實驗 116
4-3.13 活性物種捕捉實驗 119
4-3.14 觸媒光催化反應動力學模擬 121
4-4 光催化觸媒反應機制 123
4-5 光催化實驗後觸媒表面分析 125
4-5.1 反應後晶相分析 125
4-5.2 反應後掃描式電子顯微鏡分析 129
4-5.3 反應後穿透式電子顯微鏡分析 142
4-5.4 反應後回收後觸媒比表面積分析 150
第五章 結論與建議 151
5-1 結論 151
5-2 建議 152
參考文獻 153

Abdulkarem, A. M., Li, J., Aref, A. A., Ren, L., Elssfah, E. M., Wang, H., Ge, Y., & Yu, Y. (2011). CuBi2O4 single crystal nanorods prepared by hydrothermal method: growth mechanism and optical properties. Materials Research Bulletin, 46, 1443-1450.

Abroshan, E., Farhadi, S., & Zabardasti, A. (2018). Novel magnetically separable Ag3PO4/MnFe2O4 nanocomposite and its high photocatalytic degradation performance for organic dyes under solar-light irradiation. Solar Energy Materials and Solar Cells, 178, 154-163.

Chen, M., Yang, Q., Li, L., Liu, M., Xiao, P., & Zhang, M. (2016). Solid-state synthesis of CuBi2O4/MWCNT composites with enhanced photocatalytic activity under visible light irradiation. Materials Letters, 171, 255-258.

Choi, Y. H., Kim, D. H., & Hong, S. H. (2018). Gas sensing properties of p-type CuBi2O4 porous nanoparticulate thin film prepared by solution process based on metal-organic decomposition. Sensors and Actuators B: Chemical, 268, 129-135.

Choi, Y. H., Yang, K. D., Kim, D. H., Nam, K. T., & Hong, S. H. (2017). p-type CuBi2O4 thin films prepared by flux-mediated one-pot solution process with improved structural and photoelectrochemical characteristics. Materials Letters, 188, 192-196.

Deng, Y., Chen, Y., Chen, B., & Ma, J. (2013). Preparation, characterization and photocatalytic activity of CuBi2O4/NaTaO3 coupled photocatalysts. Journal of Alloys and Compounds, 559, 116-122.

Deng, M., & Huang, Y. (2020). The phenomena and mechanism for the enhanced adsorption and photocatalytic decomposition of organic dyes with Ag3PO4/graphene oxide aerogel composites. Ceramics International, 46, 2565-2570.

Dissanayake, M., Liyanage, N., Herath, C., Rathnayake, S., & Fernando, E. (2021). Mineralization of persistent azo dye pollutants by a microaerophilic tropical lake sediment mixed bacterial consortium. Environmental Advances, 3, 100038.

Do, D. D., Do, H. D., & Nicholson, D. (2010). A computer appraisal of BET theory, BET surface area and the calculation of surface excess for gas adsorption on a graphite surface. Chemical Engineering Science, 65, 3331-3340.

Fan, X. Y., Wu, Z. G., Yan, P. X., Geng, B. S., Li, H. J., Li, C., & Zhang, P. J. (2008). Fabrication of well-ordered CuO nanowire arrays by direct oxidation of sputter-deposited Cu3N film. Materials Letters, 62, 1805-1808.

Gao, H., Wang, F., Wang, S., Wang, X., Yi, Z., & Yang, H. (2019). Photocatalytic activity tuning in a novel Ag2S/CQDs/CuBi2O4 composite: synthesis and photocatalytic mechanism. Materials Research Bulletin, 115, 140-149.

Guo, J., Shi, H., Huang, X., Shi, H., & An, Z. (2018). AgCl/Ag3PO4: a stable Ag-based nanocomposite photocatalyst with enhanced photocatalytic activity for the degradation of parabens. Journal of Colloid and Interface Science, 515, 10-17.

Huang, S., Xu, Y., Zhou, T., Xie, M., Ma, Y., Liu, Q., Jing, L., Xu, H., & Li, H. (2018). Constructing magnetic catalysts with in-situ solid-liquid interfacial photofenton-like reaction over Ag3PO4@NiFe2O4 composites. Applied Catalysis B: Environmental, 225, 40-50.

Jin, S., Hao, H., Gan, Y., Guo, W., Li, H., Hu, X., Hou, H., Zhang, G., Yan, S., Gao, W., & Liu, G. (2017). Preparation and improved photocatalytic activities of Ho3+/Yb3+ co-doped Bi2MoO6. Materials Chemistry and Physics, 199, 107-112.

Karunakaran, C., Kalaivani, S., & Vinayagamoorthy, P. (2014). Optical, electrical and visible light-photocatalytic properties of hydrothermally synthesized amorphous BiVO4 nanoparticles, Materials Letters, 122, 21-24.

Katsumata, H., Hayashi, T., Taniguchi, M., Suzuki, T., & Kaneco, S. (2015). AgI/Ag3PO4 hybrids with highly efficient visible-light driven photocatalytic activity. Materials Research Bulletin, 63, 116-122.

Li, N., Miao, S., Zheng, X., Lai, J., Lv, S., Gu, X., Zhang, M., Yang, J., & Cui, S. (2019). Construction of Ag3PO4/BiNbO4 heterojunction photocatalysts with high activity for rhodamine B removal under simulated sunlight irradiation. Ceramics International, 45, 24260-24268.

Li, Q., Wang, F., Hua, Y., Luo, Y., Liu, X., Duan, G., & Yang, X. (2017). Deposition-precipitation preparation of Ag/Ag3PO4/WO3 nanocomposites for efficient visible-light degradation of rhodamine B under strongly acidic/alkaline conditions. Journal of Colloid and Interface Science, 506, 207-216.

Liang, C., Zhang, L., Guo, H., Niu, C. G., Wen, X. J., Tang, N., Liu, H. Y., Yang, Y. Y., Shao, B. B., & Zeng, G. M. (2019). Photo-removal of 2,2’4,4’-tetrabromodiphenyl ether in liquid medium by reduced graphene oxide bridged artificial z-scheme system of Ag@Ag3PO4/g-C3N4. Chemical Engineering Journal, 361, 373-386.

Liu, W., Shen, J., Yang, X., Liu, Q., & Tang, H. (2018). Dual Z-scheme g-C3N4/Ag3PO4/Ag2MoO4 ternary composite photocatalyst for solar oxygen evolution from water splitting. Applied Surface Science, 456, 369-378.

Luna-Sanguino, G., Tolosana-Moranchel, A., Carbajo, J., Pascual, L., Rey, A., Faraldos, M., & Bahamonde, A. (2020). Role of surrounding crystallization media in TiO2 polymorphs coexistence and the effect on AOPs performance. Molecular Catalysis, 493, 111059.

Luo, J., Zhou, X., Ning, X., Zhan, L., Huang, L., Cai, Q., Li, S., & Sun, S. (2018). Enhancing visible-light photocatalytic performance and stability of Ag3PO4 nanoparticles by coupling with hierarchical flower-like In2S3 microspheres. Materials Research Bulletin, 100, 102-110.

Ma, D., Wu, J., Gao, M., Xin, Y., Ma, T., & Sun, Y. (2016). Fabrication of z-scheme g- C3N4/RGO/Bi2WO6 photocatalyst with enhanced visible-light photocatalytic activity. Chemical Engineering Journal, 290, 136-146.

Ma, P., Yu, Y., Xie, J., & Fu, Z. (2017). Ag3PO4/CuO composites utilizing the synergistic effect of photocatalysis and Fenton-like catalysis to dispose organic pollutants. Advanced Powder Technology, 28, 2797-2804.

Mei, J., Zhang, D., Li, N., Zhang, M., Gu, X., Miao, S., Cui, S., & Yang, J. (2018). The synthesis of Ag3PO4/g-C3N4 nanocomposites and the application in the photocatalytic degradation of bisphenol A under visible light irradiation. Journal of Alloys and Compounds, 749, 715-723.

Mu, Z., Hua, J., Tammina, S. K., & Yang, Y. (2019). Visible light photocatalytic activity of Cu, N co-doped carbon dots/Ag3PO4 nanocomposites for neutral red under green LED radiation. Colloids and Surfaces A, 578, 123643.

Muthukrishnaraj, A., Vadivel, S., Made Joni, I., & Balasubramanian, N. (2015). Development of reduced graphene oxide/CuBi2O4 hybrid for enhanced photocatalytic behavior under visible light irradiation. Ceramics International, 41, 6164-6168.

Najafian, H., Manteghi, F., Beshkar, F., & Salavati-Niasari, M. (2019). Fabrication of nanocomposite photocatalyst CuBi2O4/Bi3ClO4 for removal of acid brown 14 as water pollutant under visible light irradiation. Journal of Hazardous Materials, 361, 210-220.

Nakabayashi, Y., Nishikawa, M., & Nosaka, Y. (2014). Fabrication of CuBi2O4 photocathode through novel anodic electrodeposition for solar hydrogen production. Electrochimica Acta, 125, 191-198.

Naraginti, S., Yu, Y. Y., Fang, Z., & Yong, Y. C. (2019). Novel tetrahedral Ag3PO4@N-rGO for photocatalytic detoxification of sulfamethoxazole: process optimization, transformation pathways and biotoxicity assessment. Chemical Engineering Journal, 375, 122035.

Oh, W. D., Dong, Z., & Lim, T. T. (2017). Hierarchically-structured Co–CuBi2O4 and Cu–CuBi2O4 for sulfanilamide removal via peroxymonosulfate activation. Catalysis Today, 280, 2-7.

Ouyang, K., Jiang, N., Xue, W., & Xie, S. (2020). Enhanced photocatalytic activities of visible light-responsive Ag3PO4-GO photocatalysts for oxytetracycline hydrochloride degradation. Colloids and Surfaces A, 604, 125312.

Qian, Z., Zhang, J., Wang, C., Chen, H., & Zheng, J. (2021). A novel high-gravity AOP process for enhanced NOx attenuation using alkaline H2O2 as a strong oxidizing reagent: reaction mechanisms and kinetics. Chemical Engineering Journal, 404, 126454.

Ran, R., McEvoy, J. G., & Zhang, Z. (2016). Ag2O/Ag3VO4/Ag4V2O7 heterogeneous photocatalyst prepared by a facile hydrothermal synthesis with enhanced photocatalytic performance under visible light irradiation. Materials Research Bulletin, 74, 140-150.

Sahay, R., Sundaramurthy, J., Suresh Kumar, P., Thavasi, V., Mhaisalkar, S. G., & Ramakrishna, S. (2012). Synthesis and characterization of CuO nanofibers, and investigation for its suitability as blocking layer in ZnO NPs based dye sensitized solar cell and as photocatalyst in organic dye degradation. Journal of Solid State Chemistry, 186, 261-267.

Sangiorgi, N., Aversa, L., Tatti, R., Verucchi, R., & Sanson, A. (2017). Spectrophotometric method for optical band gap and electronic transitions determination of semiconductor materials. Optical Materials, 64, 18–25.

Shao, B., Liu, X., Liu, Z., Zeng, G., Liang, Q., Liang, C., Cheng, Y., Zhang, W., Liu, Y., & Gong, S. (2019). A novel double z-scheme photocatalyst Ag3PO4/Bi2S3/Bi2O3 with enhanced visible-light photocatalytic performance for antibiotic degradation. Chemical Engineering Journal, 368, 730-745.

Shi, W., Guo, F., & Yuan, S. (2017a). In situ synthesis of z-scheme Ag3PO4/CuBi2O4 photocatalysts and enhanced photocatalytic performance for the degradation of tetracycline under visible light irradiation. Applied Catalysis B: Environmental, 209, 720-728.

Shi, Y., Luo, L., Zhang, Y., Chen, Y., Wang, S., Li, L., Long, Y., & Jiang, F. (2017b). Synthesis and characterization of α/β-Bi2O3 with enhanced photocatalytic activity for 17α-ethynylestradiol. Ceramics International, 43, 7627-7635.

Sun, M., Zeng, Q., Zhao, X., Shao, Y., Ji, P., Wang, C., Yan, T., & Du, B. (2017). Fabrication of novel g-C3N4 nanocrystals decorated Ag3PO4 hybrids: enhanced charge separation and excellent visible-light driven photocatalytic activity. Journal of Hazardous Materials, 339, 9-21.

Tahir, M., Tasleem, S., & Tahir, B. (2020). Recent development in band engineering of binary semiconductor materials for solar driven photocatalytic hydrogen production. Hydrogen Energy, 45, 15985-16038.

Tian, J., Yan, T., Qiao, Z., Wang, L., Li, W., You, J., & Huang, B. (2017). Anion-exchange synthesis of Ag2S/Ag3PO4 core/shell composites with enhanced visible and NIR light photocatalytic performance and the photocatalytic mechanisms. Applied Catalysis B: Environmental, 209, 566-578.

Uma, H. B., Ananda, S., & Vijaya Kumar, M. S. (2021). Electrochemical synthesis and characterization of CuO/ZnO/SnO nano photocatalyst: evaluation of its application towards photocatalysis, photo-voltaic and antibacterial properties. Chemical Data Collections, 32, 100658.

Wang, F., Yang, H., & Zhang, Y. (2018a). Enhanced photocatalytic performance of CuBi2O4 particles decorated with Ag nanowires. Materials Science in Semiconductor Processing, 73, 58-66.

Wang, Y., Liu, C., Zhang, Y., Meng, W., Yu, B., Pu, S., Yuan, D., Qi, F., Xu, B., & Chu, W. (2018b). Sulfate radical-based photo-fenton reaction derived by CuBi2O4 and its composites with α-Bi2O3 under visible light irradiation: catalyst fabrication, performance and reaction mechanism. Applied Catalysis B: Environmental, 235, 264-273.

Włodarczyk-Stasiak, M., & Jamroz, J. (2009). Specific surface area and porosity of starch extrudates determined from nitrogen adsorption data. Journal of Food Engineering, 93, 379-385.

Wu, C. H. (2004). Comparison of azo dye degradation efficiency using UV/single semiconductor and UV/coupled semiconductor system. Chemosphere, 57, 601–608.

Xiu, Z., Wu, Y., Hao, X., Lu, Q., & Liu, S. (2014). Graphene oxide wrapped Ag3PO4 sub-micro particles with highly enhanced photocatalytic activity and stability under visible light irradiation. Materials Research Bulletin, 59, 192-198.

Yuan, X., Shen, D., Zhang, Q., Zou, H., Liu, Z., & Peng, F. (2019). Z-scheme Bi2WO6/CuBi2O4 heterojunction mediated by interfacial electric field for efficient visible-light photocatalytic degradation of tetracycline. Chemical Engineering Journal, 369, 292-301.

Yuvaraj, S., Karthikeyan, K., Kalpana, D., Lee, Y. S., & Selvan, R. K. (2016). Surfactant-free hydrothermal synthesis of hierarchically structured spherical CuBi2O4 as negative electrodes for Li-ion hybrid capacitors. Journal of Colloid and Interface Science, 469, 47-56.

Zhang, X. B., Dong, W. Y., & Yang, W. (2013a). Decolorization efficiency and kinetics of typical reactive azo dye RR2 in the homogeneous Fe(II) catalyzed ozonation process. Chemical Engineering Journal, 233, 14-23.

Zhang, Y., Xie, Y., Li, J., Yang, G., Bai, T., & Wang, J. (2013b). Effects of synthetic conditions on the morphology and catalytic properties of hierarchical CuBi2O4 nanoflowers grown by low-temperature solution process. Journal of Alloys and Compounds, 580, 172-175.

Zhang, H., Nengzi, L. C., Li, X., Wang, Z., Li, B., Liu, L., & Cheng, X. (2020a). Construction of CuBi2O4/MnO2 composite as z-scheme photo activator of peroxymonosulfate for degradation of antibiotics. Chemical Engineering Journal, 386, 124011.

Zhang, C., Wang, L., Yuan, F., Meng, R., Chen, J., Hou, W., & Zhu, H. (2020b). Construction of p-n type Ag3PO4/CdWO4 heterojunction photocatalyst for visible-light-induced dye degradation. Applied Surface Science, 534, 147544.

Zhang, J., Yan, M., Yuan, X., Si, M., Jiang, L., Wu, Z., Wang, H., & Zeng, G. (2018). Nitrogen doped carbon quantum dots mediated silver phosphate/bismuth vanadate z-scheme photocatalyst for enhanced antibiotic degradation. Journal of Colloid and Interface Science, 529, 11-22.

Zhang, X., Zhang, C., Yang, Y., Zhang, H., Huang, X., Hang, R., & Yao, X. (2019). Light-assisted rapid sterilization by a hydrogel incorporated with Ag3PO4/MoS2 composites for efficient wound disinfection. Chemical Engineering Journal, 374, 596-604.

Zhu, D. & Zhou, Q. (2019). Action and mechanism of semiconductor photocatalysis on degradation of organic pollutants in water treatment: a review. Environmental Nanotechnology Monitoring & Management, 12, 100255.

林永輝，(2018)三氧化二鉍複合釩酸鹽氧化物為可見光激發觸媒之研究，國立高雄科技大學，碩士論文。