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| ???org.dspace.app.webui.jsptag.ItemTag.dcfield??? | Value | Language |
|---|---|---|
| dc.contributor.advisor | 吳紀聖 | |
| dc.contributor.author | Sheng-Hung Yu | en |
| dc.contributor.author | 游勝閎 | zh_TW |
| dc.date.accessioned | 2021-06-16T10:14:21Z | - |
| dc.date.available | 2014-08-25 | |
| dc.date.copyright | 2013-08-25 | |
| dc.date.issued | 2013 | |
| dc.date.submitted | 2013-08-19 | |
| dc.identifier.citation | 1. Yoshida, H., Heterogeneous Photocatalytic Conversion of Carbon Dioxide. 2011: p. 531-559.
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Chen, Photocatalytic reduction of carbon dioxide on NiO/InTaO4 under visible light irradiation. Catalysis Communications, 2007. 8(10): p. 1546-1549. 69. Lee, W.-H., et al., A novel twin reactor for CO2 photoreduction to mimic artificial photosynthesis. Applied Catalysis B: Environmental, 2013. 132-133: p. 445-451. 70. Guan, G., T. Kida, and A. Yoshida, Reduction of carbon dioxide with water under concentrated sunlight using photocatalyst combined with Fe-based catalyst. Applied Catalysis B: Environmental, 2003. 41(4): p. 387-396. 71. Zhang, Q., et al., Visible light responsive iodine-doped TiO2 for photocatalytic reduction of CO2 to fuels. Applied Catalysis A: General, 2011. 400(1-2): p. 195-202. | |
| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/60256 | - |
| dc.description.abstract | 由於人類經濟活動不斷的發展並且無節制地排放二氧化碳，導致大氣中的二氧化碳濃度持續增加、溫室效應增強造成全球暖化。二氧化碳回收再利用不僅可以解決全球暖化的危機，還可以帶來可觀的經濟價值。
本研究主要分為兩部分: (1) 合成可見光光觸媒 GaN:ZnO與觸媒分析 (2) 測試GaN:ZnO 光催化能力。以固態熔融法在氨氣的環境下鍛燒氧化鎵與氧化鋅至1123K能夠合成出可見光光觸媒GaN:ZnO，由UV-Vis圖得知該觸媒可以吸收的波段達到可見光的範圍，能隙為2.6eV，由EDS與XRD圖的結果可以判斷是否成功合成出GaN:ZnO，最後再由TEM與XPS來確認附載共觸媒與其價態。 經過光觸媒反應發現共觸媒附載GaN:ZnO具有兩種能力: (1) 還原二氧化碳 (2)產氫。具有雙種功能的觸媒可大幅度提升光觸媒反應的光亮子效率。本實驗除了製備雙功觸媒之外，額外的還發現了一個有趣的現象，還原二氧化碳與產氫具有相輔相成的功能。 當以GaN:ZnO產氫時，可以利用所產生的氫氣進行二氧化碳氫化反應來製造碳氫化合物，而氫化反應的吉布士自由能為負值，其所代表的意義是該反應為自發性反應，能使反應較容易進行。此外反應中被氫化的二氧化碳所產生的甲醇，其扮演的腳色為犧牲試劑並捕捉電子以進行光催化反應。因此，由氫化二氧化碳與甲醇當犧牲試劑所產生的循環可以提升光催化反應的效率，而其效率值超越現有可見光光觸媒所能達到的效率，在可見光的照射下，氫氣、甲烷、甲醇、甲醛的產率分別為 3.16, 1.12, 2.24, 0.312, μmol/h/g，此外一氧化碳也是其中的產物，而光電子效率為 0.0245%。 | zh_TW |
| dc.description.abstract | Global warming has become a major environmental issue to be considered in the 21th century. One possible solution of global warming is the reduction of carbon dioxide. The reduction of carbon dioxide could not only solve the crisis of global warming, but provide a high economic value. Carbon dioxide could be reduced to useful chemicals such as methane, methanol, and other hydrocarbons.
In this research, co-catalyst loaded GaN:ZnO is found to have the ability to perform both photocatalytic reduction of carbon dioxide and produce hydrogen (water splitting) simultaneously. Having the duel functions ability gives the advantages of increasing the conversion of solar energy. An interesting phenomena found while performing photocatalytic reaction of duel function catalyst is that providing the ability of water splitting, carbon dioxide reduction ability is enhanced through the hydrogenation of CO2 [1] through the produced hydrogen. For the reaction in the hydrogenation of carbon dioxide to produce hydrocarbons, the change of Gibbs energy becomes a negative value meaning that the reaction is favorable and is spontaneous. Furthermore, the as produced methanol acted as an electron trap for the enhancement of hydrogen production [2]. Therefore the efficiency of the photocatalyst introduced in this research is higher than recent developed visible light catalyst. The result of Ni/NiO-GaN:ZnO showed a yield of 3.16, 1.12, 2.24, 0.312 μmol/h/g of hydrogen, methane, methanol, formaldehyde respectively. | en |
| dc.description.provenance | Made available in DSpace on 2021-06-16T10:14:21Z (GMT). No. of bitstreams: 1 ntu-102-R00524094-1.pdf: 5449921 bytes, checksum: fc97f27909b5d2ffecaee4c080051583 (MD5) Previous issue date: 2013 | en |
| dc.description.tableofcontents | Acknowledgement I
Abstract (Chinese) III Abstract V Table of Contents VII List of Figures XII 1. Introduction 1 1.1 Background 2 1.2 Research Motivations 3 1.3 Research Goals 4 2. Literature Review 4 2.1 Background of photocatalysis 4 2.2 Introduction of GaN:ZnO 7 2.2.1 Structure and Characteristics 10 2.2.2 Co-catalyst loading 13 2.2.3 Water splitting ability 14 2.3 Background of Carbon Dioxide 19 2.3.1 Chemical and physical properties 19 2.3.2 Reduction of Carbon Dioxide through photocatalytic reaction 21 2.3.3 Hydrogenation of Carbon Dioxide 26 3. Experimental Method 33 3.1 Materials and Apparatus 33 3.1.1 Chemicals 33 3.1.2 Apparatus 35 3.2 Preparation of Photocatalysts 36 3.2.1 GaN:ZnO Photocatalyst preparation Setup 36 3.2.2 Solid State Fusion Method 42 3.2.3 Loading co-catalyst 43 3.2.3.1 Co-catalyst loading Setup 43 3.2.3.2 Incipient wetness impregnation method 46 3.3 Photocatalyst Characterization 49 3.3.1 X-Ray Diffraction (XRD) 49 3.3.2 UV – Visible Spectrum (UV-VIS)2 51 3.3.3 Energy Dispersive Spectrometer (EDS)2 53 3.3.4 X-Ray Photoelectron Spectrometer (XPS)2 55 3.3.5 Field Emission Scanning Electron Microscopy (SEM)2 56 3.3.6 Transmission electron microscopy (TEM) 57 3.3.7 Photoluminescence (PL) 58 3.3.8 Gas Chromatography Instrument (GC-FID, GC-TCD) 59 3.4 Analysis of Formaldehyde 61 3.4.1 Calibration Curve 63 3.4.2 Formaldehyde Calibration 63 3.5 Photocatalytic Reaction 65 3.5.1 Gas Chromatography Detection Conditions 65 3.5.1.1 FID detector 65 3.5.2 Reaction System 73 3.5.2.1 Slurry batch reactor 74 3.5.2.2 Light sources 76 3.5.2.3 Reduction of carbon dioxide and hydrogen production 76 3.5.3 Calibration Curve 78 3.5.3.1 Hydrogen Calibration 78 3.5.3.2 Methane Calibration 80 3.5.3.3 Carbon Monoxide Calibration 81 3.5.3.4 Methanol Calibration 83 4. Results and Discussion 84 4.1 Catalyst characterization and Analysis 84 4.1.1 X-Ray Diffraction (XRD) 84 4.1.2 UV – Visible Spectrum (UV-VIS) 86 4.1.3 Field Emission Scanning Electron Microscopy (SEM) 88 4.1.4 Energy Dispersive Spectrometer (EDS) 89 4.1.5 X-Ray Photoelectron Spectrometer (XPS) 92 4.1.6 Transmission electron microscopy (TEM) 93 4.1.7 Photoluminescence (PL) 95 4.2 Catalyst preparation with different precursors 97 4.3 Photocatalytic reduction of Carbon Dioxide 99 4.3.1 Blank Experiment 100 4.3.2 Results over different conditions: Addition of H2, NaOH, NaCl 101 4.3.3 Photocatalytic reaction over several metal/metal oxide loadings .103 4.3.3.1 Photocatalytic reaction over Ni/NiO / GaN:ZnO 103 4.3.3.2 Photocatalytic reaction over low activity co-catalyst 110 4.4 Quantum Efficiency 110 4.5 Comparison with current references 116 5. Twin Reactor 118 5.1 Experimental conditions 118 5.2 Experimental Result 120 6. Conclusions and Future Advices 123 6.1 Conclusions 123 6.2 Future Advices 124 References 126 Appendices 132 Autobiography 136 | |
| dc.language.iso | zh-TW | |
| dc.subject | 氫化二氧化碳 | zh_TW |
| dc.subject | 單反應器 | zh_TW |
| dc.subject | 可見光光觸媒 | zh_TW |
| dc.subject | GaN:ZnO | zh_TW |
| dc.subject | 產氫 | zh_TW |
| dc.subject | Visible light | en |
| dc.subject | Photocatalyst | en |
| dc.subject | CO2 reduction | en |
| dc.subject | Water splitting | en |
| dc.subject | GaN:ZnO | en |
| dc.title | 可見光雙功觸媒氫化二氧化碳與產氫反應 | zh_TW |
| dc.title | Duel function visible light photocatalyst in hydrogenation of carbon dioxide via hydrogen production. | en |
| dc.type | Thesis | |
| dc.date.schoolyear | 101-2 | |
| dc.description.degree | 碩士 | |
| dc.contributor.oralexamcommittee | 林欣瑜,萬本如 | |
| dc.subject.keyword | 可見光光觸媒,氫化二氧化碳,產氫,GaN:ZnO,單反應器, | zh_TW |
| dc.subject.keyword | Visible light,GaN:ZnO,Photocatalyst,Water splitting,CO2 reduction, | en |
| dc.relation.page | 136 | |
| dc.rights.note | 有償授權 | |
| dc.date.accepted | 2013-08-19 | |
| dc.contributor.author-college | 工學院 | zh_TW |
| dc.contributor.author-dept | 化學工程學研究所 | zh_TW |
| Appears in Collections: | 化學工程學系 | |
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