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http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/80460完整後設資料紀錄
| DC 欄位 | 值 | 語言 |
|---|---|---|
| dc.contributor.advisor | 徐治平(Jyh-Ping Hsu) | |
| dc.contributor.author | Yu-Jen Lee | en |
| dc.contributor.author | 李友仁 | zh_TW |
| dc.date.accessioned | 2022-11-24T03:07:06Z | - |
| dc.date.available | 2022-02-21 | |
| dc.date.available | 2022-11-24T03:07:06Z | - |
| dc.date.copyright | 2022-02-21 | |
| dc.date.issued | 2022 | |
| dc.date.submitted | 2022-01-01 | |
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| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/80460 | - |
| dc.description.abstract | "金屬有機骨架 (MOF) 為一群以過渡金屬離子為核心，有機分子為配位基團的固態晶體。 MOF 多半具有中孔徑的特性，且其孔隙內通常具有巨大的表面積。 雖然眾多有關於MOF的特性已經被廣泛研究，MOF被親核基團攻擊的機制，以及被攻擊後產生的多孔材料的性質則依舊不清楚。 本論文首先回顧於水中穩定的MOF之研究，以及其初步應用。 對水穩定的MOF具有從水溶液中吸附分子的潛力。 我們已經成功製備並分析其中一類鋯金屬為核心的MOF，UiO-66 和 UiO-66-NH2。 有鑑於UiO-66 和 UiO-66-NH2對磷酸的吸附力大幅優於市面上的吸附劑，在此研究中合成的UiO-66 和 UiO-66-NH2 首次被用於從極強酸性 (pH < -1) 的溶液中吸附磷酸。使用朗謬爾方程式做回歸後，其在25 oC廢棄混合酸，硝酸-磷酸-醋酸混合物，以及重量百分率85% 磷酸中，對磷酸之最大吸附量 (qmax) 分別為 3360, 8510 和 4790 mg-H3PO4/g。 吸附過磷酸之UiO-66/UiO-66-NH2，其磷與鋯的比例為6.2‒13.5，可能的原因為高濃度的磷酸堆積在UiO-66 的表面，形成一個類似聚磷酸的結構，並以氫鍵作為連結。 當MOF被浸泡於無機酸溶液中，質子與親核基團均有可能攻擊MOF，並破壞其晶體結構。本論文首次發現在極強酸性溶液中，親核基團，而非質子，會取代晶體中原有之有機配基，而破壞晶體之結構，肇因於親核基團為強路易斯鹼，和四價鋯具有強親和力。 MOF受攻擊後所產生的不定型中孔徑固體，若其沒有完全溶解，亦可以用於吸附劑。 由於這些不定型中孔徑固體，對於二價銅離子以及親核基團的吸附能力，與固體的晶體結構與內表面積並無明顯關聯，其吸附力可能為摻於固體內之親核基團所提供。 根據上述的發現，我們使用了UiO-66以合成對pH、溫度，以及親核基團穩定的不定型固體。 此固體由 UiO-66 浸泡於10或50 mM 磷酸中得到，並以1 M 鹽酸/1 M 氫氧化鈉進行再處理。 無經酸鹼再處理之固體則作為對照。 這些無配基的官能基團，以及磷酸根，可以做為吸附鉛離子的活性位置。 綜上所述，本論文提升了我們對親核基團攻擊UiO-66的認知，並提出了高效轉化UiO-66成為穩定性高的不定型多孔固體之方法。此類固體有被使用於極端環境中的能力。 " | zh_TW |
| dc.description.provenance | Made available in DSpace on 2022-11-24T03:07:06Z (GMT). No. of bitstreams: 1 U0001-2411202112575600.pdf: 4766230 bytes, checksum: 51d9685bcf5b52e281d107c4d749be37 (MD5) Previous issue date: 2022 | en |
| dc.description.tableofcontents | "Acknowledgements .....i Abstract .....ii 摘要 .....iv Contents .....vi List of Figures .....ix List of Tables .....xii Chapter 1 Introduction .....1 Chapter 2 Literature review .....3 2.1 General .....3 2.2 Chemically Stable MOF .....6 2.2.1 Water-stable MOF .....6 2.2.2 pH stable MOF .....7 2.3 Water-stable zirconium(Zr)-based MOF .....14 2.4 MOF under modification .....18 2.5 MOF as adsorbent .....18 2.5.1 Use with anionic adsorbates .....18 2.5.2 Use with cationic or neutral adsorbates .....22 2.5.3 Use of MOF in extremely acidic solution as adsorbent .....23 2.5.3.1 Recovery of resources from extremely acidic mix .....23 2.5.3.2 Stability of UiO-66 as adsorbents in waste mixed acids .....24 2.6 Phosphorus .....26 2.7 Nature of nucleophile and reaction with MOF .....27 2.8 Main theme of this work .....27 Chapter 3 Experimental .....29 3.1 UiO-66 synthesis and sample preparation .....29 3.2 Adsorption Tests .....31 3.3 Instrumental analysis .....33 3.3.1 pH determination .....3 3.3.2 Ion chromatography (IC) .....33 3.3.3 Powder X-ray diffraction (XRD) .....34 3.3.4 Fourier-transform infrared (FTIR) spectrometry .....34 3.3.5 Nuclear magnetic resonance (NMR) analysis .....34 3.3.6 Zeta potential determination .....34 3.3.7 Scanning electron microscopy (SEM) .....35 3.3.8 Thermogravimetric analysis (TGA) .....35 Chapter 4 Results and discussion .....36 4.1 Characterization of the synthesized UiO-66 salts .....36 4.2 Adsorption of phosphoric acid from extremely acidic solution .....40 4.2.1 General .....40 4.2.2 Adsorption from extremely acidic solutions .....40 4.2.3 Discussion .....44 4.2.4 Summary .....51 4.3 Impact of nucleophiles on UiO-66 stability .....52 4.3.1 General .....52 4.3.2 Tests with mixed acids .....52 4.3.3 Stability of UiO-66 in nucleophile solutions with different pH .....60 4.3.4 Pivotal study of adsorption of cation – Use Cu2+ as an example .....60 4.3.5 Pivotal study of adsorption of anions .....64 4.3.6 XRD patterns and zeta potential analysis of modified UiO-66 .....66 4.3.7 Effects of nucleophile on structures of UiO-66 .....79 4.3.8 Summary .....83 4.4 Making stable amorphous matrix from UiO-66 template .....84 4.4.1 General .....84 4.4.2 Effects of acid, base treatment .....84 4.4.2.1 XRD pattern .....85 4.4.2.2 FTIR spectrum .....88 4.4.2.3 TGA test .....91 4.4.2.4 Zeta potential test .....93 4.4.2.5 XPS test .....97 4.4.2.6 Adsorption of lead .....100 4.4.3 Discussion .....102 4.4.4 Summary .....104 Chapter 5 Prospects and challenge .....105 Chapter 6 Conclusions .....109 References .....111 Appendices .....126" | |
| dc.language.iso | en | |
| dc.subject | 親核基團 | zh_TW |
| dc.subject | 金屬有機骨架 | zh_TW |
| dc.subject | 吸附劑 | zh_TW |
| dc.subject | 不定型固體 | zh_TW |
| dc.subject | Amorphous | en |
| dc.subject | Adsorbent | en |
| dc.subject | Nucleophile | en |
| dc.subject | Metal-organic framework | en |
| dc.title | 使用受親核基團攻擊之金屬有機骨架UiO-66為水溶液中吸附劑 | zh_TW |
| dc.title | Nucleophile Attacked Metal Organic Framework UiO-66 with Its Use as Adsorbent in Aqueous Solutions | en |
| dc.date.schoolyear | 110-1 | |
| dc.description.degree | 博士 | |
| dc.contributor.oralexamcommittee | 王大銘(Hsin-Tsai Liu),諶玉真(Chih-Yang Tseng),張嘉修,曾琇瑱 | |
| dc.subject.keyword | 金屬有機骨架,不定型固體,吸附劑,親核基團, | zh_TW |
| dc.subject.keyword | Metal-organic framework,Amorphous,Adsorbent,Nucleophile, | en |
| dc.relation.page | 128 | |
| dc.identifier.doi | 10.6342/NTU202104489 | |
| dc.rights.note | 同意授權(限校園內公開) | |
| dc.date.accepted | 2022-01-03 | |
| 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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