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| DC 欄位 | 值 | 語言 |
|---|---|---|
| dc.contributor.advisor | 游文岳 | zh_TW |
| dc.contributor.advisor | Wen-Yuen Yu | en |
| dc.contributor.author | 許冠博 | zh_TW |
| dc.contributor.author | Guan-Bo Syu | en |
| dc.date.accessioned | 2024-03-17T16:17:18Z | - |
| dc.date.available | 2024-03-18 | - |
| dc.date.copyright | 2024-03-16 | - |
| dc.date.issued | 2024 | - |
| dc.date.submitted | 2024-02-15 | - |
| dc.identifier.citation | [1] T. B, In: Proceedings of 8th International Congress on Catalysis.Vol. 1. Weinheim: Verlag Chemie, I‐7 (1984).
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Stere, Promoting effect of Au on Pd/TiO2 catalyst for the selective catalytic reduction of NOx by H2, Catalysis Today, 332 (2019) 69-75. [59] C.N. Costa, A.M. Efstathiou, Transient Isotopic Kinetic Study of the NO/H2/O2 (Lean de-NOx) Reaction on Pt/SiO2 and Pt/La−Ce−Mn−O Catalysts, The Journal of Physical Chemistry B, 108 (2004) 2620-2630. [60] L. Li, L. Qu, J. Cheng, J. Li, Z. Hao, Oxidation of nitric oxide to nitrogen dioxide over Ru catalysts, Applied Catalysis B: Environmental, 88 (2009) 224-231. [61] R.S.o.C.F. Division, Journal of the Chemical Society: Faraday transactions, The Society.1995. [62] D. Cui, Y. Li, K. Pan, J. Liu, Q. Wang, M. Liu, P. Cao, J. Dan, B. Dai, F. Yu, NO hydrogenation to NH3 over FeCu/TiO2 catalyst with improved activity, Frontiers of Chemical Science and Engineering, 17 (2023) 1973-1985 | - |
| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/92236 | - |
| dc.description.abstract | 氮氧化合物（NOx）是空氣中污染的來源，可能引起多種環境問題，包括光化學煙霧、酸雨、PM2.5和霧霾的形成。為了應對這些環境的挑戰，傳統上使用選擇性催化還原（SCR）反應將NOx轉化為無害的N2。與此同時，氨氣（NH3）作為合成含氮化合物的重要化學品，近來更成為氫儲存的載體。然而，NH3通常需要在高壓和高溫的條件下從N2和H2中合成（即Haber-Bosch製程）。為了解決與NOx（環境問題）和NH3（能源問題）相關的挑戰，我們提出了一種催化反應，可以在相對溫和的條件下將NO和H2轉化為NH3。以含浸法合成的2 wt% Pd/TiO2-R、2 wt% Rh/TiO2-R和2 wt% Ru/TiO2-R觸媒皆能在300℃達到NO轉化率約100%，值得注意的是，2Pd/TiO2-R相較2Rh/TiO2-R和2Ru/TiO2-R表現出更高的反應活性以及約95%的NH3選擇率。我們也透過程序升溫系列實驗得知，觸媒之反應活性與選擇率和NO的解離式吸附比例、H2與NH3在觸媒表面吸附能力強度息息相關，為了深入了解2Pd/TiO2-R觸媒上由NO和H2進行NH3合成的催化機制，包括NO和H2的活化過程，我們也進行了原位紅外光譜實驗，並發現了最容易反應之NO吸附型態為Pd-NO。這項研究有望為發展更有效地NOx轉化和NH3合成方法提供新的洞察。 | zh_TW |
| dc.description.abstract | Nitrogen oxides (NOx) serve as sources of air pollution, potentially leading to various environmental issues, including photochemical smog, acid rain, PM2.5, and haze formation. To address these environmental challenges, the traditional approach involves using Selective Catalytic Reduction (SCR) to convert NOx into harmless N2. Ammonia (NH3), an essential chemical for synthesizing nitrogen-containing compounds, has recently gained prominence as a carrier for hydrogen storage. However, the synthesis of NH3 typically requires harsh conditions, involving high pressure and temperature, through the Haber-Bosch process. In order to tackle challenges related to NOx (environment) and NH3 (energy), we propose a catalytic reaction capable of converting NO and H2 into NH3 under relatively mild conditions. There are three catalysts, 2 wt% Pd/TiO2-R, 2 wt% Rh/TiO2-R, and 2 wt% Ru/TiO2-R which synthesized by the impregnation method, achieved approximately 100% NO conversion at 300°C. It is noteworthy that 2Pd/TiO2-R exhibited higher reaction activity and around 95% NH3 selectivity compared to 2Rh/TiO2-R and 2Ru/TiO2-R. Through temperature programmed experiments, we discovered that the catalytic activity and selectivity are closely linked to the dissociative adsorption ratio of NO, and the surface adsorption strength of H2 and NH3 on the catalyst surface. To gain a deeper understanding of the catalytic mechanism of NH3 synthesis from NO and H2 on the 2Pd/TiO2-R catalyst, including the activation processes of NO and H2, we conducted in-situ infrared spectroscopy experiments. We found the most reactive NO adsorption form was identified as Pd-NO. This research holds the potential to provide new insights for the development of more effective methods for NOx conversion and NH3 synthesis. | en |
| dc.description.provenance | Submitted by admin ntu (admin@lib.ntu.edu.tw) on 2024-03-17T16:17:18Z No. of bitstreams: 0 | en |
| dc.description.provenance | Made available in DSpace on 2024-03-17T16:17:18Z (GMT). No. of bitstreams: 0 | en |
| dc.description.tableofcontents | 口試委員審定書 i
誌謝 ii 摘要 iii ABSTRACT iv 目錄 iv 圖目錄 viii 表目錄 xi 第一章 緒論 1 1-1 研究背景—氨氣生成 1 1-1-1 氨氣生成技術歷史及面臨挑戰 1 1-1-2 氨氣經濟價值及益處 4 1-1-3 氨氣生成觸媒 6 1-2 研究背景—氮氧化合物 9 1-2-1 氮氧化合物對於環境之影響 9 1-2-2 去除氮氧化合物之技術 10 1-2-3 氫氣選擇性催化還原反應 12 1-3 研究目標 16 第二章 實驗方法 17 2-1 實驗藥品與氣體鋼瓶 17 2-1-1 實驗藥品 17 2-1-2 實驗氣體鋼瓶 17 2-2 觸媒製備 18 2-3 催化反應系統 20 2-3-1 反應系統架設 20 2-3-2 氨氣生成催化測試 21 2-3-3產物鑑定—質譜儀 22 2-4 觸媒鑑定 28 2-4-1 X光繞射儀 (XRD) 28 2-4-2 穿透式電子顯微鏡 (TEM) 29 2-4-3 氫氣程溫還原分析 (H2-TPR) 30 2-4-4 氫氣、氨氣程溫脫附分析(H2-TPD & NH3-TPD) 32 2-4-5 一氧化氮程序升溫表面反應 (NO-TPSR) 34 2-4-6 氫氣脈衝化學吸附分析 (H2 pulse chemisorption) 35 2-4-7 傅立葉紅外線光譜儀 (FT-IR) 37 第三章 結果與討論 40 3-1反應熱力學 40 3-1-1熱力學數據蒐集 40 3-1-2 平衡常數結果 43 3-1-3 平衡濃度分析 45 3-2 Pd, Rh & Ru擔載於TiO2觸媒對催化反應之影響 47 3-2-1 一氧化氮去除率 47 3-2-2 氨氣選擇率 49 3-2-3 穩定度測試 51 3-2-4 與NO + H2 + O2反應的比較 53 3-2-5 Pd擔載量之影響 56 3-3 Pd, Rh & Ru擔載於TiO2觸媒物理及化學性質鑑定 58 3-3-1 晶體結構分析 58 3-3-2 表面形貌分析 60 3-3-3 觸媒還原性質分析 62 3-3-4 金屬分散度分析 64 3-4 Pd, Rh & Ru擔載於TiO2觸媒反應機制探討 66 3-4-1 一氧化氮於觸媒表面之吸附現象 66 3-4-2 氫氣於觸媒表面之吸附現象 69 3-4-3 氨氣於觸媒表面之吸附現象 72 3-4-4 一氧化氮與氫氣生成氨氣之反應機制 75 第四章 結論 84 第五章 未來展望 85 APPENDIX 86 REFERENCE 88 | - |
| dc.language.iso | zh_TW | - |
| dc.subject | NH3生成 | zh_TW |
| dc.subject | NO移除 | zh_TW |
| dc.subject | 程序升溫 | zh_TW |
| dc.subject | 原位紅外線光譜 | zh_TW |
| dc.subject | in-situ FTIR | en |
| dc.subject | NH3 synthesis | en |
| dc.subject | NO removal | en |
| dc.subject | temperature programmed | en |
| dc.title | 應用Pd/TiO2, Rh/TiO2以及Ru/TiO2觸媒催化一氧化氮氫化生成氨氣 | zh_TW |
| dc.title | Ammonia Synthesis from Hydrogenation of Nitric Oxide over Pd/TiO2, Rh/TiO2 and Ru/TiO2 Catalysts | en |
| dc.type | Thesis | - |
| dc.date.schoolyear | 112-1 | - |
| dc.description.degree | 碩士 | - |
| dc.contributor.oralexamcommittee | 林昇佃;林錕松;林亮毅 | zh_TW |
| dc.contributor.oralexamcommittee | Shawn D. Lin;Kuen-Song Lin;Liang-Yi Lin | en |
| dc.subject.keyword | NH3生成,NO移除,程序升溫,原位紅外線光譜, | zh_TW |
| dc.subject.keyword | NH3 synthesis,NO removal,temperature programmed,in-situ FTIR, | en |
| dc.relation.page | 93 | - |
| dc.identifier.doi | 10.6342/NTU202400564 | - |
| dc.rights.note | 同意授權(限校園內公開) | - |
| dc.date.accepted | 2024-02-16 | - |
| dc.contributor.author-college | 工學院 | - |
| dc.contributor.author-dept | 化學工程學系 | - |
| dc.date.embargo-lift | 2029-01-01 | - |
| 顯示於系所單位： | 化學工程學系 | |
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