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研究生：	吳昆翰 Wu, Kwun-Han
論文名稱：	高低聚物氮化碳複合結構之高效率水分解產氫機制探討 Oligomer-Polymer Carbon Nitride Composites as Effective Photocatalysts for Hydrogen Production from Water Decomposition
指導教授：	鄧熙聖 Teng, Hsi-Sheng
學位類別：	碩士 Master
系所名稱：	工學院 - 化學工程學系 Department of Chemical Engineering
論文出版年：	2016
畢業學年度：	104
語文別：	中文
論文頁數：	115
中文關鍵詞：	氮化碳、氮化碳高分子、氮化碳低聚物、光催化、分解水、產氫
外文關鍵詞：	Carbon Nitride, Melem Oligomer, Oligomer and Polymer Composites, Water splitting, Hydrogen generation
相關次數：	點閱：91 下載：2
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氫氣能源是最環保乾淨的替代能源之一，利用太陽光作能量來源達成光催化水分解產氫更可以實現能源永續的理想。石磨相氮化碳高分子是近七年來最受矚目的光觸媒之一，隨著研究程度逐漸深入，人們發現完全聚縮合的氮化碳並無可測量的光催化產氫效果，不完全聚縮合的氮化碳高分子卻擁有可觀的產氫能力，推測此效果與被視為缺陷的胺基有關，最新的研究更是利用特殊分離技術與合成方法將氮化碳低聚物從高分子的領域獨立分開討論，並且明確指出低聚物因為具有更多胺基的裸露而在動力學上更適合發生還原反應而產氫，然而氮化碳低聚物卻因為量子效應的關係使得能隙較同種類高分子來得更大，導致光催化效果在熱力學上不滿足。本研究開發出一個創意性十足的工法合成出氮化碳的高、低聚物複合材料，經過各項儀器的分析與檢驗之後，吾人大膽斷定此複合材料完美利用了低聚物更多胺基裸露的優點，並且保留了高分子本身在熱力學上可以吸收更長波長光的優勢。除此之外，複合結構的出現增加了光生電子電洞的分離率，分開的電子電洞各自被導出材料表面發生表面的反應。改質前後的樣品產氫效能可以相差十倍以上，對於氮化碳這項材料而言，本研究除了更進一步證明了胺基在產氫應用上的地位之外，同時也開創了另一個對學術界影響重大的研究方向。

The effectiveness of melon chain termination, amine groups, on photocatalytic activity attracted people to study the melem monomer and its condensates recently. Melem oligomers has been announced an active phase of “carbon nitride” owing to more amino-group exposure. Based on the advantages of exposure of amines, we here figure out a brand-new fashion to fabricate the composite of melem oligomer and carbon nitride polymer. The unique combination of distinct phases extended the optical absorption range of our material to longer wavelength, and highly improves its charge separation rate. The H2 evolution rate of this oligomer-polymer composite is 10 times higher than polymeric carbon nitride made from urea. This study re-emphasizes the crucial role of melem derivatives on photocatalysis.

總目錄
中文摘要	..........................	I
Abstract..........................	II
誌謝	..........................	XII
本文目錄	..........................	XIV
表目錄	..........................	XVII
圖目錄	..........................	XVIII
本文目錄
第一章	緒論.................1
	1-1 	前言.............1
	1-2 	Fujishima-Honda effect.......2
	1-3	半導體簡介...........3
   1-3-1原子的電子軌域與能階...........3
   1-3-2價帶與導帶的形成.............5
   1-3-3半導體的定義.............7
   1-3-4本質半導體與外質半導體...........8
   1-3-5費米能階(Fermi-level)...........10
	1-4	半導體光觸媒催化原理.........13
   1-4-1光催化分解水之應用與反應機制........15
   1-4-2共觸媒的角色.............17
   1-4-3犧牲試劑工作原理.............18
	1-5	光觸媒分解水反應器.........19
	1-6	研究動機.............21
第二章	文獻回顧...............22
	2-1	半導體光觸媒的發展：金屬氧化物......22
	2-2	氮化碳的發展與應用..........26
	2-3	類石墨相氮化碳高分子的結構與性質.....30
	2-4	類石墨相氮化碳高分子的改質與多樣性.....33
   2-4-1能隙的縮減與能帶位置遷移工程.........33
   2-4-2比表面積的拓展..............35
   2-4-3光生電子電洞再結合的減少...........37
   2-4-4氮化碳高分子於光催化之其他改質與突破.......38
	2-5	本研究於類石墨相氮化碳高分子的改質設計....39
第三章	實驗方法與儀器原理介紹...........40
	3-1 	藥品、材料與儀器設備.........40
   3-1-1 藥品與材料...............40
   3-1-2 儀器與實驗設備.............41
	3-2 	實驗步驟............42
   3-2-1 氮化碳高分子奈米層製備..........42
   3-2-2 高溫熱裂解處理.............44
   3-2-3 溫氮空缺的修補.............46
   3-2-3 白金(Pt)共觸媒之負載...........48
	3-3 	系統架設與光源測量簡介........49
   3-3-1懸浮式上照反應器與分解水系統.........49
   3-3-2氣相層析儀簡介..............51
   3-3-3上照燈源強度測定與量子產率計算.........52
	3-4	分析儀器原理簡介..........54
   3-4-1 X光繞射儀..............54
   3-4-2 X光光電子能譜儀............58
   3-4-3傅立葉轉換紅外光譜儀............60
   3-4-4紫外-可見光分光光度計...........62
   3-4-5光至螢光光譜儀..............64
   3-4-6熱重分析儀..............64
   3-4-7氮氣吸脫附儀..............65
   3-4-8元素分析儀..............67
   3-4-9掃描式與穿透式電子顯微鏡...........68
   3-4-10半導體-電解質之介面分析...........72
第四章	結果與討論..............75
	4-1 	XRD圖譜及結構分析..........76
	4-2	XPS圖譜分析與反應機制探討.......79
	4-3	FT-IR吸收光譜分析..........81
	4-4	TGA結果之討論............83
	4-5	EA結果之討論...........85
	4-6	DRS探究能隙與半導體性質.........87
	4-7	材料之電子結構的分析..........89
	4-8	PL光譜分析.............91
	4-9	SEM與TEM之發現...........93
	4-10	產氫效能之成果發表.......100
第五章	結論...........102
	5-1	結論..........102
	5-2	未來建議..........102
參考文獻...........103
                                    

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