Luận án Research into TiO₂/ac, TiO₂/go synthesis and coating on cordierite ceramic applied as catalysts for photodegradation of methyl orange and phenol

on the more easily destroyed organic molecule MO demonstrated that the addition of GO to TiO2 catalysts did not increase their activity in visible light. Catalysts based on synthesized TiO2 displayed less activity than ZnO based cunder visible light illumination. The findings are agreed with previous studies [160, 181,182]. Summary: The synthesis of TiO2-based photocatalysts by various methods, such as solgel, hydrothermal, and precipitation, revealed that the synthesis technique effects photocatalytic activity mostly owing to changes in surface area and pore size. TiO2 generated by hydrothermal synthesis contains a large surface area and adequate pore size, and hence displayed the best activity for the degradation of MO and phenol under UV light. Due to phenol's more stable structure, its degradation was more difficult than that of MO (lower degradation and longer reaction time), but with optimum amount of added H2O2 (4 mmol/l) and a low phenol concentration (10 ppm), more than 80 percent of phenol was degraded after 240 minutes of reaction. The Langmuir-Hinshelwood kinetic model was also used to compare the rate of phenol degradation reaction on different catalysts and conditions [175]. The results presented in the results tables show the agreement of all the photocatalytic processes of the samples with the applied model. The reaction rate constants corresponding to the catalytic process of each sample are listed in Table fom 3.9 to 3.12. Under UV light, catalyst P123-C25-450 has the highest rate constant of 0.0027 compared to the other two catalyst samples. The initial concentration of phenol greatly affects the reaction rate. At 10 ppm, the rate constant reaches 0.0071, more than twice as much as at 30 ppm (0.0027). At phenol concentrations of 30 ppm and optimal H2O2 content (4 ppm), catalyst P123-c25-450 gives results of up to 0.0079. GO is found to speed up the processing of phenol catalyst GO-ZnO with a rate constant of up to 0.0107 in the visible light range. It also shows that the process parameters are a very important part of figuring out how well a photocatalyst is synthesized. However, the attempt to shift phenol photodegradation to the visible light range by making a TiO2–GO composite failed despite the success of the same manufacturing technique for ZnO–GO. 115 CHAPTER 4: CONCLUSIONS AND RECOMENDATONS 1.Precipitation and hydrothermal methods were used to synthesize the Nano TiO2 catalysts. Many characterization methods of material structure and morphology as well as synthesis parameters have been measured, researched, and optimized (substance structure, calcination temperature, citric acid amount, substance removal methods, etc.). The photodegradation is evaluated by the photochemical reaction to degrade the agent methyl orange in solution (MO). The results showed that the catalyst made by the hydrothermal method P123-C25-450 worked the best. After 60 minutes of lighting by the UVC 254 NM-100W lamp, 98% of the MO had been broken down (MO concentration was 20 ppm). 2.The TiO2 was modified with activated carbon by the sol-gel method. The parameters of support as the amount as well as the type of activated carbon used, are evaluated. The results showed that the catalyst SG AC1200 TI1/18 has the best degradation efficiency. Similar experiments with samples modified with graphene oxide (GO) support have yielded similar results. SG GO Ti 1/18 also gives the best decomposition optical efficiency. 3. Different amounts of PEG 600 were used to dip coat TiO2/AC catalysts made with sol-gel, hydrothermal, and precipitation methods on cordierite supports. The results show that high PEG Corgel-150 material has the best performance in MO degradation, with a performance of up to nearly 94%. 4.. The TiO2 coating by the chemical vapor deposition (CVD) method on glass, aluminum, and cordierite supports has also been evaluated. The results show that the catalyst coated on the ceramic support is the best at breaking down MO. After 120 minutes of light from a UVC lamp with a wavelength of 254 nm, MO was degraded down by about 52%. 5. The highly active catalyst materials evaluated above, such as P123-C25-450, SG AC 1200 T1/18, have been compared in the phenol photodegradation UV lamp. The P123-C25-450 catalyst has the most effective result with a degradation rate of 45% under research conditions. Preliminary research has compared the ability of GO-TiO2 catalysts, GO-ZnO, and P123-C25-450 to degrade phenol and the kinetics of their processes. 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Nguyễn Trung Hiếu, Phạm Thị Mai Phương, Đào Quốc Tùy, Lê Minh Thắng (2016), “Nghiên cứu ảnh hưởng của chủng loại và hàm lượng than hoạt tính trong vật liệu AC/TiO2 đến quá trình quang phân hủy methyl orange (MO)”, Tạp chí hóa học, số T54 (5e1,2) 1-5 2016, tr. 343-347. 2. Nguyễn Trung Hiếu, Đào Quốc Tùy, Filip Verschaeren, Lê Minh Thắng (2017), “Nghiên cứu ảnh hưởng của chất hoạt động bề mặt và phương pháp tổng hợp đến quá trình tổng hộp xúc tác quang hóa TiO2 trong xử lý methyl da cam (MO)”, Tạp chí Hóa học, số T.55 (2e) 2017, tr. 5-10. 3. Nguyễn Trung Hiếu, Bùi Đức Huy, Le Minh Thắng (2018), “Nghiên cứu hoạt tính của xúc tác TiO2 dạng màng mỏng trên cordierite trong xử lý methyl da cam”, Tạp chí Hóa học, số T.56 (3E12), tr. 198-202. 4. Nguyễn Trung Hiếu, Hoàng Thế Huynh, Trịnh Giang Khánh, Vũ Anh Tuấn, Lê Minh Thắng (2019), “Tổng hợp và đánh giá hoạt tính xúc tác của màng TiO2 trên gốm cordierite trong việc xử lý methyl da cam”, Tạp chí Hóa học, số T.57 (2e12) 1-5, tr. 115-121. 5. Nguyễn Trung Hiếu, Trịnh Huy Quang, Đào Quốc Tùy, Lê Minh Thắng (2019), “Nghiên cứu ảnh hưởng của tỷ lệ grapheme oxide (GO) trong quá trình biến tính xúc tác quang hóa TiO2 bằng phương pháp sol-gel và xử lý methyl da cam (MO)”, Tạp chí Hóa học, số T.57 (2e12) 1-5, tr. 122-127. 6. Trung Hieu Nguyen, Anh Tuan Vu, Van Han Dang, Jeffrey Chi-Sheng Wu, Minh Thang Le (2020), “Photocatalytic Degradation of Phenol and Methyl Orange with Titania-Based Photocatalysts Synthesized by Various Methods in Comparison with ZnO–Graphene Oxide Composite”, Topics in Catalysis, Springer Nature 2020. https://doi.org/10.1007/s11244-020-01361-5 APPENDIX A TiO2/AC composites Calculation Example of Calculation: TiO2/AC at 5%wt: In preparation process 20ml Ti(OCH(CH3)2)4 was used. The synthesis reaction was presented below Ti(OCH(CH3)2)4 information; the density is 0.97 kg/l, the molecular weight is 284.26 g/mol. For TiO2, the molecular weight is 80 g/mol. Ti{OCH(CH3)2}4 + 2 H2O → TiO2 + 4 (CH3)2CHOH So, 20ml Ti[OCH(CH3)2]4 can be produced TiO2; 2 2 423 423 /80 1 1 /26.284 /97.020 )( ])([ ])([ 2 TiO TiO CHOCHTi CHOCHTi molg mol mol molg lkgml gTiO   = So the amount of TiO2 = 5.46 g The percent theoretical amount of AC percent in composite catalyst can be computed by 100%   = TX X ACofwt 100 46.5 %5   = X X wt The amount of AC added, X =0.29 g APPENDIX B MO (methyl orange) photodegradation A: methyl orange MO in powder, B experimental setup for full range visible experiment, C MO sampling tube, D: MO absorbance by Avantes Uv-Vis device APPENDIX C Phenol photodegradation a b c d APPENDIX D BET pore results APPENDIX E XRD characterizations Faculty of Chemistry, HUS, VNU, D8 ADVANCE-Bruker - G1-18 00-021-1272 (*) - Anatase, syn - TiO2 - Y: 82.49 % - d x by: 1. - WL: 1.5406 - Tetragonal - a 3.78520 - b 3.78520 - c 9.51390 - alpha 90.000 - beta 90.000 - gamma 90.000 - Body-centered - I41/amd (141) - 4 - 136.313 - I/Ic File: HieuBK G1-18.raw - Type: 2Th/Th locked - Start: 5.000 ° - End: 70.010 ° - Step: 0.030 ° - Step time: 0.3 s - Temp.: 25 °C (Room) - Time Started: 3 s - 2-Theta: 5.000 ° - Theta: 2.500 ° - Chi: 0.00 ° - Phi: 0.00 ° - X: 0.0 m L in ( C p s ) 0 100 200 300 400 500 600 2-Theta - Scale 5 10 20 30 40 50 60 70 d = 3 .5 2 7 d = 2 .3 7 8 d = 1 .8 9 5 d = 1 .6 9 7 d = 1 .6 6 7 d = 1 .4 8 7 Faculty of Chemistry, HUS, VNU, D8 ADVANCE-Bruker - G1-24 00-021-1272 (*) - Anatase, syn - TiO2 - Y: 50.21 % - d x by: 1. - WL: 1.5406 - Tetragonal - a 3.78520 - b 3.78520 - c 9.51390 - alpha 90.000 - beta 90.000 - gamma 90.000 - Body-centered - I41/amd (141) - 4 - 136.313 - I/Ic 1) File: HieuBK G1-24.raw - Type: 2Th/Th locked - Start: 2.000 ° - End: 70.010 ° - Step: 0.030 ° - Step time: 0.3 s - Temp.: 25 °C (Room) - Time Started: 14 s - 2-Theta: 2.000 ° - Theta: 1.000 ° - Chi: 0.00 ° - Phi: 0.00 ° - X: 0.0 Left Angle: 23.540 ° - Right Angle: 26.180 ° - Left Int.: 69.9 Cps - Right Int.: 94.8 Cps - Obs. Max: 25.276 ° - d (Obs. Max): 3.521 - Max Int.: 238 Cps - Net Height: 151 Cps - FWHM: 0.718 ° - Chord Mid.: 25.253 ° - Int. Br L in ( C p s ) 0 100 200 300 400 500 600 2-Theta - Scale 5 10 20 30 40 50 60 70 d = 3 .5 2 0 d = 3 .3 6 0 d = 2 .3 7 8 d = 1 .8 9 0 d = 1 .7 0 0 d = 1 .4 8 1 d = 1 .3 7 0 Faculty of Chemistry, HUS, VNU, D8 ADVANCE-Bruker - G1-4 00-021-1272 (*) - Anatase, syn - TiO2 - Y: 55.67 % - d x by: 1. - WL: 1.5406 - Tetragonal - a 3.78520 - b 3.78520 - c 9.51390 - alpha 90.000 - beta 90.000 - gamma 90.000 - Body-centered - I41/amd (141) - 4 - 136.313 - I/Ic 1) File: HieuBK G1-4.raw - Type: 2Th/Th locked - Start: 2.000 ° - End: 70.010 ° - Step: 0.030 ° - Step time: 0.3 s - Temp.: 25 °C (Room) - Time Started: 14 s - 2-Theta: 2.000 ° - Theta: 1.000 ° - Chi: 0.00 ° - Phi: 0.00 ° - X: 0.0 m Left Angle: 22.820 ° - Right Angle: 27.560 ° - Left Int.: 71.2 Cps - Right Int.: 64.8 Cps - Obs. Max: 25.280 ° - d (Obs. Max): 3.520 - Max Int.: 234 Cps - Net Height: 167 Cps - FWHM: 0.742 ° - Chord Mid.: 25.271 ° - Int. Br L in ( C p s ) 0 100 200 300 400 500 600 2-Theta - Scale 5 10 20 30 40 50 60 70 d = 3 .5 2 0 d = 2 .3 7 4 d = 1 .8 9 1 d = 1 .6 9 8 d = 1 .6 6 4 d = 1 .4 8 2