超小奈米鈀金屬於二維與三維結構中孔洞矽材以及中孔洞碳氮材在有機催化反應之應用

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林家榕(Chia-Jung Lin) 查詢紙本館藏

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論文名稱

超小奈米鈀金屬於二維與三維結構中孔洞矽材以及中孔洞碳氮材在有機催化反應之應用
(Ultrasmall Palladium Nanoparticles Confined in 2D-3D Mesoporous Silica and Mesoporous Carbon Nitride for the Catalytic Organic Reaction)

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摘要(中)

本論文主要分為兩大部分，在第一部分研究中，超小奈米鈀金屬還原在中孔洞材料之二維結構SBA-15以及三維結構KIT-6之中，利用化學還原劑使金屬還原速率上升，並藉由和SBA-15以及KIT-6表面原有的羥基，使離子鈀金屬能快速平均分散並負載在SBA-15以及KIT-6孔洞之中並還原奈米鈀金屬顆粒。由於SBA-15以及KIT-6具有高比表面積以及良好的孔洞體積，故使用SBA-15以及KIT-6作為載體可以提高奈米鈀金屬分散率和負載率從而提高催化活性。本實驗將製成的Pd(x)@SBA-15以及Pd(x)@KIT-6應用在催化苯乙烯氫化反應當中，分別探討二維結構以及三維結構、不同氫供體以及不同溶劑對催化活性之影響。經過一系列的研究使用Pd(30)@KIT-6作為催化劑去進行催化苯乙烯氫化反應，其轉換頻率（TOF）高達363 h-1。在這項研究中，Pd(30)@KIT-6展示了其用於催化苯乙烯氫化是高活性催化劑。
在第二部分研究中，通過奈米模鑄法(Nanocasting)合成出中孔洞碳氮材料（MUFC），並將奈米鈀金屬顆粒負載在MUFC上作為催化觸媒。藉由MUFC上不僅可以利用有缺陷的C-N位點和氮間隙可以很均勻分散鈀金屬顆粒，且由於其具有鹼性的含氮位點可有效促進反應進行，從而提高催化活性。本實驗將Pd(x)@MUFC應用在催化苯甲醇氧化反應當中，分別探討不同載體、不同溶劑以及不同鹼添加試劑對催化活性之影響。在催化苯甲醇氧化反應的研究中Pd(30)@MUFC表現出很高的催化活性，其轉換頻率（TOF）高達750 h-1。在這項研究中，Pd(30)@MUFC展示了其用於催化苯甲醇氧化反應中是高前景催化劑。

摘要(英)

This study consists of two main parts. In the first part, the Palladium nanoparticles (Pd NPs) with a particle size of 2-3nm are successfully confined within the 2D mesoporous silica SBA-15 and the 3D mesoporous silica KIT-6. Under the wet impregnation process, SBA-15 and KIT-6 were immersed in Pd2+ precursor and adsorbed into the pores, then. The mixture chemically reduced by reagent containing NaBH4 and NH3BH3 to obtain Pd(x)@SBA-15 and Pd(x)@KIT-6. It was found that the use of SBA-15 and KIT-6 support can highly enhance the dispersion and efficiency due to the high surface area and large pore volume. In addition, SBA-15 and KIT-6 with the pore size of 9.09 nm and 9.56 nm, respectively, may effectively confine the Pd NPs and subsequently avoid the aggregation. According to the X-ray diffraction pattern and TEM image, it can be confirmed that the particle size of Pd NPs is about 2-3 nm and highly dispersed without aggregation. The Pd(x)@SBA-15 and Pd(x)@KIT-6 exhibited superior catalytic activity and chemoselectivity for the catalytic transfer hydrogenation of styrene under mild conditions with formic acid and ammonium formate as a hydrogen donor. Among all the as-prepared catalysts, the Pd(30)@KIT-6 exhibited the highest turnover frequency (TOF) of 363 h-1. In addition, Pd(30)@KIT-6 exhibited an excellent high stability after five successive cycles without significant loss of its catalytic activity.
In the second part of study, heteroatom doped carbon materials have received considerable attention in the field of catalysis. Herein, we report a catalyst made of palladium nanoparticles (Pd NPs) supported on mesoporous nitrogen-doped carbon (MUFC), Pd@MUFC. The use of the mixture of melamine-urea-formaldehyde as a precursor and the mesoporous silica SBA-15 as a hard template afforded a high-nitrogen-content mesoporous carbon material that showed high activity in stabilizing Pd NPs. The N-doped mesoporous carbon, MUFC, can provide a large surface area to adsorb the reductant and substrate, and enhance the accessibility of the active sites of the Pd NPs in the catalytic reaction process. When Pd@MUFC was applied as catalyst in the catalytic aerobic oxidation of benzyl alcohol, it achieved conversion rate and selectivity of 99.9% within 30 minutes. Among all the as-prepared catalysts, the Pd(30)@MUFC exhibited the highest turnover frequency of 750 h-1. The remarkable catalytic activity for the benzyl alcohol oxidation can be attributed to the ultra-small Pd NPs confined in the hexagonal N-doped carbonaceous MUFC.

關鍵字(中)

★ 鈀奈米金屬
★ 催化反應
★ 有序中孔洞矽材
★ 中孔洞碳氮材料

關鍵字(英)

★ Catalyst

論文目次

中文摘要 I
ABSTRACT III
謝誌 V
目錄 VII
圖目錄 XI
表目錄 XX
第一章序論 1
第壹部分鈀金屬在中孔洞矽材催化苯乙烯氫化反應 1
1-1 中孔洞二氧化矽 1
1-1-1中孔洞材料之介紹 1
1-1-2中孔洞二氧化矽合成方法 4
1-1-3軟性模板-微胞結構 5
1-2 二維及三維中孔洞二氧化矽 9
1-2-1二維與三維的差異 9
1-2-2二維結構SBA-15 10
1-2-3三維結構KIT-6 11
1-3 鈀金屬催化苯乙烯氫化反應 12
1-3-1不飽和碳氫化合物的氫化反應 12
1-3-2金屬催化苯乙烯氫化反應機制介紹 13
1-3-3奈米金屬鈀催化苯乙烯氫化反應文獻回顧 15
第貳部分鈀金屬在中孔洞碳氮材催化苯甲醇氧化反應 20
1-4 有序中孔洞碳氮材 20
1-4-1奈米模鑄法(Nanocasting)合成機制 22
1-4-2奈米模鑄法合成有序中孔洞碳氮材之發展 23
1-5 鈀金屬催化苯甲醇氧化反應 30
1-5-1苯甲醛介紹 30
1-5-2金屬催化苯甲醇氧化機制介紹 31
1-5-3奈米金屬鈀催化苯甲醇氧化反應文獻回顧 33
1-5-4催化劑載體的表面酸鹼性對催化性能的影響 38
1-6 研究動機與目的 41
第二章實驗部分 43
2-1 實驗藥品 43
2-2 鈀金屬催化苯乙烯氫化反應實驗 45
2-2-1二維結構p6mm中孔洞矽材SBA-15合成 45
2-2-2三維立方體Ia3d中孔洞矽材KIT-6合成 46
2-2-3以PdCl2做為前驅物還原至SBA-15與KIT-6之中 47
2-2-3.1利用雙還原劑化學還原法 47
2-2-4利用Pd(x)@SBA-15與Pd(x)@KIT-6催化苯乙烯氫化實驗 49
2-2-5催化苯乙烯氫化重複使用實驗 50
2-3 鈀金屬催化苯甲醇氧化反應實驗 51
2-3-1奈米模鑄法合成中孔洞碳氮材MUFC 51
2-3-2以PdCl2做為前驅物還原至MUFC之中 52
2-3-3利用Pd(x)@MUFC催化苯甲醇氧化實驗 53
2-3-4 Pd(x)@MUFC催化苯甲醇氧化重複實驗 54
2-4 實驗設備 55
2-4-1實驗合成設備 55
2-4-2實驗鑑定儀器 55
第三章結果與討論 57
第壹部分鈀金屬在中孔洞矽材催化苯乙烯氫化反應 57
3-1 Pd(x)@SBA-15以及Pd(x)@KIT-6材料系列 57
3-1-1基本性質鑑定 57
3-1-1.1 SAXRD繞射圖譜 57
3-1-1.2 WAXRD繞射圖譜 61
3-1-1.3等溫氮氣吸脫附 63
3-1-1.4 SEM影像 69
3-1-1.5 TEM圖像 72
3-1-1.6 XPS結果分析 82
3-1-2鈀催化苯乙烯氫化實驗 85
3-1-2.1 Pd(x)@SBA-15催化苯乙烯氫化反應 85
3-1-2.2 Pd(x)@KIT-6催化苯乙烯氫化反應 87
3-1-2.3不同材料對催化苯乙烯氫化反應之比較 89
3-1-2.4不同氫供體對催化苯乙烯氫化反應之比較 91
3-1-2.5 不同溶劑對催化苯乙烯氫化反應之比較 93
3-1-2.6催化不同烯烴之氫化反應 96
3-1-3 Pd(30)@KIT-6催化苯乙烯氫化反應重複利用之實驗 98
3-1-3.1 Pd(30)@KIT-6 5th回收利用 98
3-1-3.2 Pd(30)@KIT-6 5th XRD繞射圖譜 100
3-1-3.3 Pd(30)@KIT-6 5th的TEM圖譜 101
第貳部分鈀金屬在中孔洞碳氮材催化苯甲醇氧化反應 103
3-2 Pd(x)@MUFC材料系列 103
3-2-1基本性質鑑定 103
3-2-1.1 SAXRD繞射圖譜 103
3-2-1.2 WAXRD繞射圖譜 105
3-2-1.3等溫氮氣吸脫附 106
3-2-1.4 SEM影像 110
3-2-1.5 TEM影像 112
3-2-1.6元素分析以及XPS電子能譜 118
3-2-1.7拉曼光譜分析 125
3-2-2鈀催化苯甲醇氧化反應實驗 126
3-2-2.1 Pd(x)@MUFC催化苯甲醇氧化反應 126
3-2-2.2不同材料對催化苯甲醇氧化反應之比較 128
3-1-3.3不同溶劑對催化苯甲醇氧化反應之比較 132
3-1-3.4不同鹼試劑對催化苯甲醇氧化反應之比較 134
3-1-3.5催化不同醇類之氧化反應 137
3-2-3 Pd(30)@MUFC催化苯甲醇氧化反應重複利用之實驗 139
3-2-3.1 Pd(30)@MUFC 5th 回收利用產氫 139
3-2-3.2 Pd(30)@MUFC 5th XRD繞射圖譜 141
3-2-3.3 Pd(30)@MUFC 5th TEM圖 142
第四章結論 144
第五章參考文獻 146

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指導教授

高憲明

審核日期

2019-7-23

推文