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完整後設資料紀錄
DC 欄位 | 值 | 語言 |
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dc.contributor.advisor | 萬本儒(Ben-Zu Wan) | |
dc.contributor.author | Yi-Hsiu Chen | en |
dc.contributor.author | 陳怡秀 | zh_TW |
dc.date.accessioned | 2021-06-15T12:26:34Z | - |
dc.date.available | 2019-08-31 | |
dc.date.copyright | 2016-08-31 | |
dc.date.issued | 2016 | |
dc.date.submitted | 2016-08-10 | |
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dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/49944 | - |
dc.description.abstract | 本研究以氯化金酸為前驅物的奈米金擔載於HY型(proton type)沸石來製備Au/Y觸媒,用於催化室溫下的一氧化碳氧化反應。研究分為三部分,第一部分,探討表面修飾對於沸石表面電位的影響。由於沸石的isoelectric point (IEP)為小於pH 3左右,在中性環境下表面電位為負,因此不適用於擔載同樣帶負電荷的金化合物於沸石擔體上,然而,透過在硝酸鈉溶液中的表面修飾程序,沸石的表面電位可由負變正。因此,在第二部分的研究中,就以氯化金酸為前驅物的奈米金擔載其上,探討擔體的表面電位改變,對於奈米金的載負以及催化活性的影響。由研究結果發現,隨著表面電位由負變正,金的擔載量隨之提升,此外,由於金顆粒小同時擔載位置接近外表面,因此具有較佳的催化活性。另一方面,透過降低金溶液的pH值至2.6,亦可使表面電位由負變正,然而,低pH下金化合物的氯殘留量較高,因而對觸媒的催化活性造成負面影響。總結而言,在接近中性環境下(pH 6),將奈米金擔載於經過表面修飾的HY上,具有最佳的催化一氧化碳氧化反應活性。在本研究第三部分,則探討水氣對Au/Y觸媒催化活性的影響。由實驗結果發現,在完全隔絕水氣的環境下,Au/Y幾乎沒有活性,顯示水氣對催化活性的必要性。透過改變水氣含量,探討反應溫度攝氏25度時濕度對催化活性的影響,已結論出相對濕度為30 %時,Au/Y觸媒具有較佳的活性。 | zh_TW |
dc.description.abstract | Nanogold derived from chloroauric acid (HAuCl4) were deposited onto proton-type zeolite Y (HY) for catalyzing CO oxidation around room temperature. Three subjects were studied in this research. In the first part, the effect of surface modification on surface charge of proton-type zeolite Y (HY) was investigated. Owing to the negative zeta potential in neutral aqueous solution close to neutral, zeolite Y is not suitable for supporting negative-charge gold complexes. Nevertheless, the process of surface modification in NaNO3 solutions, with solution pH adjusted to 6 by NaOH(aq), was found able to reverse the zeta potential of HY to positive. In the second part of this study, the effect of surface charge of zeolite supports on the Au loading and catalytic activity was investigated. Positive correlation was observed between the surface charge and Au loading. For modified HY with positive surface charge, the supported gold species were with smaller sizes and finer dispersion. Through ESCA analyses, most of them were deposited near the exterior surface, which enables less resistance in mass transfer for CO oxidation. They possessed catalytic activity superior to those supported on HY without any surface modification. On the other hand, via lowering the solution pH to 2.6 (near IEP of zeolite supports), the surface charge can be reversed to positive as well. However, more residual Cl remained inside the catalysts. Moreover, gold species were deeply deposited inside the cages of HY. The as-prepared Au/Y possessed almost no catalytic activity. In summary, it is recommended to prepare Au/Y in aqueous solution at pH 6, with surface modified HY with positive surface charges. In the third part of this study, the effect of moisture on the catalytic activity of Au/Y was investigated. The results demonstrate that moisture is indispensable for Au/Y to maintain high catalytic activity. Under a relative humidity at ca. 30 % at 25 °C, Au/Y catalysts can perform the best activity in this research. | en |
dc.description.provenance | Made available in DSpace on 2021-06-15T12:26:34Z (GMT). No. of bitstreams: 1 ntu-105-D99524011-1.pdf: 4801457 bytes, checksum: 1c4ff5171f7f458e1cc86cb834b82da7 (MD5) Previous issue date: 2016 | en |
dc.description.tableofcontents | Abstract III
Table of contents V List of Figures IX Lists of Tables XV Chapter 1. Reversal of zeta potential of proton-type zeolite Y after surface modification in sodium ion aqueous solutions 1 1.1 Introduction 1 1.2 Experimental 4 1.2.1 Surface modification of Y-type zeolites in NaNO3(aq) solutions 4 1.2.2 Characterizations 5 1.2.3 Adsorption of Cr(VI) in aqueous solutions 7 1.3 Results and Discussion 7 1.3.1 Effect of surface modifications in NaNO3(aq) solutions at pH 6 on zeta potentials of HY-1 and NaY-1 7 1.3.2 ESCA analyses of exterior-surface compositions of HY-1 and NaY-1 and the derivatives 10 1.3.3 Analyses of ESCA Al(2p) and Si(2p) spectra of NaY-1, NaY-S-1, HY-1 and HY-SPH-1 12 1.3.4 Analyses of bulk structure of NaY-1, HY-1 and the derivatives by using XRD and 27Al MAS solid-state NMR 15 1.3.5 Effect of Al/Si ratios of HY on zeta potentials after surface modifications in NaNO3(aq) solutions at pH 6 20 1.3.6 Zeta potentials of HY after surface modifications in NaNO3(aq) solutions without pH adjustments or directly dispersed in NaCl(aq) solutions 23 1.3.7 Application of the surface modified HY-1 for adsorption of Cr(VI) pollutants in aqueous solutions 26 1.4 Conclusions 30 Chapter 2. Effects of surface charge of proton-type zeolite Y on the loading of AuCl4- -derived complexes and Activity of Au/Y in low-temperature CO oxidation 32 2.1 Introduction 32 2.2. Experimental 36 2.2.1 surface modification of HY zeolite 36 2.2.2 Preparation of Au/Y catalysts 37 2.2.3 Activity test of CO oxidation 39 2.2.4. Characterizations 40 2.3 Results 42 2.3.1 Deposition of AuCl4-- derived gold complexes onto modified HY with various Al/Si weight ratios 42 2.3.1.1 characterizations of fresh Au/Y 42 2.3.1.2 CO oxidation tests and characterizations of reacted Au/Y 47 2.3.2 Deposition of AuCl4--derived gold complexes onto zeolite supports of same parent HY but prepared via different procedures 53 2.3.2.1 Au loading analyses 53 2.3.2.2 Elementary analyses over bulk catalysts and exterior surface 59 2.3.2.3 HRTEM characterizations 61 2.3.2.4 Analyses of residual chloride 64 2.3.2.5 CO oxidation tests of fresh Au/Y and pretreatment with 10 vol % H2/N2 flows at 400 K 67 2.4 Discussion 72 2.4.1 Gold loading mechanisms 72 2.4.2 CO oxidation reactivity and comparison with literature works 78 2.5 Conclusions 84 Chapter 3. Effects of moisture on Au/Y in low-temperature CO oxidation 87 3.1 Introduction 87 3.2 Experimental 90 3.2.1 Preparation of Au/Y catalysts 90 3.2.2 Activity test of CO oxidation 91 3.2.3 Characterizations 92 3.3 Results and Discussion 93 3.3.1 N2 pretreatment 93 3.3.2 CO oxidation with or without moisture under a high space velocity 98 3.3.3 Effects of moisture contents 106 3.4 Conclusions 117 Chapter 4 Conclusions 119 References 121 | |
dc.language.iso | en | |
dc.title | Au/Y觸媒應用於室溫一氧化碳氧化反應 | zh_TW |
dc.title | Proton-type Zeolite Y Supported Gold Catalysts for Room-temperature CO Oxidation | en |
dc.type | Thesis | |
dc.date.schoolyear | 104-2 | |
dc.description.degree | 博士 | |
dc.contributor.oralexamcommittee | 徐治平(Jyh-Ping Hsu),吳紀聖(Chi-Sheng Wu),鄭淑芬(Soofin Cheng),牟中原(Chung Yuan Mou),林昇佃(Shawn D. Lin) | |
dc.subject.keyword | Au/Y觸媒,表面修飾程序,表面電位,水氣,一氧化碳氧化反應, | zh_TW |
dc.subject.keyword | Au/Y,CO oxidation,surface modification,surface charge,moisture, | en |
dc.relation.page | 131 | |
dc.identifier.doi | 10.6342/NTU201602095 | |
dc.rights.note | 有償授權 | |
dc.date.accepted | 2016-08-10 | |
dc.contributor.author-college | 工學院 | zh_TW |
dc.contributor.author-dept | 化學工程學研究所 | zh_TW |
顯示於系所單位: | 化學工程學系 |
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