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研究生: 簡理軒
Chien, Li-Hsuan
論文名稱: 硫化亞銅修飾二硫化錫形成奈米異質結構來提升光催化二氧化碳還原效率之研究
Cu2-xS decorated SnS2 for enhanced photocatalytic CO2 reduction by forming nanoscale heterostructure
指導教授: 陳家俊
Chen, Chia-Chun
陳貴賢
Chen, Kuei-Hsien
林麗瓊
Chen, Li-Chyong
學位類別: 碩士
Master
系所名稱: 化學系
Department of Chemistry
論文出版年: 2018
畢業學年度: 106
語文別: 中文
論文頁數: 99
中文關鍵詞: 硫化亞銅二硫化錫異質結構二氧化碳還原
英文關鍵詞: Cu2-xS, SnS2, CO2 reduction, heterostructure
DOI URL: http://doi.org/10.6345/THE.NTNU.DC.038.2018.B05
論文種類: 學術論文
相關次數: 點閱:160下載:17
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  • 本研究利用人造光合成作用系統將二氧化碳還原轉換成碳氫化合物,作為未來新興的替代性能源,以期改善愈趨被重視的環境及能源議題,本研究以溶劑熱法合成二硫化錫與硫化亞銅,由於兩種材料的能隙大小與位置能讓二氧化碳還原反應發生,並以異質接面方式混合兩種半導體材料,有效的將激發後所產生的電子與電洞分離,並降低電子電洞輻射復合的現象,使其有較多的激子能夠飄移至材料表面進行二氧化碳還原反應;在本研究中,首先就材料的晶體結構、成份比例及元素、光學性質等特性分析,再利用氣相層析,發現二硫化錫與硫化亞銅分別能產出乙醛及甲醇,兩者材料在二氧化碳還原上具有不同之特性,經由混合兩材料形成異質結構,發現能產出乙醛與大量的乙醇,並有效地提高光化學量子轉換效率,可達到約0.048%,且乙醇是能作為燃料的碳氫化合物,最後藉由改變兩種材料的混合比例來優化反應效率,在不同比例下,本研究發現以0.5:1的比例混合硫化亞銅與二硫化錫,相較於其他比例,光化學量子轉換效率能提高至0.072%,從此研究,能證明利用p-n異質接面結構方法,能有效提高光觸媒在二氧化碳還原反應上的效率。

    Formation of hydrocarbon from carbon dioxide via artificial photosynthesis is a new and developing alternative energy for solving the environmental energy issue which has gradually been emphasized seriously. We prepare the SnS2 and Cu2S by solvothermal method. The band gap and position of these two materials are suitable for photocatalytic CO2 reduction. We hybrid these two materials to be the heterojunction structure. By this modification, it can effectively separate the electron-hole pairs and suppress the charge recombination. There are more carriers which can diffuse to the surface and involve in CO2 reduction. At first, we analyze the crystal structure, composition and element, optical property. Then we detect the photocatalytic efficiency by gas chromatography. The SnS2 and Cu2S can produce the acetaldehyde and methanol respectively. They have different selectivity on CO2 reduction. After hybridization of these two materials and forming the heterostructure, it can produce the acetaldehyde and a lot of ethanol. The quantum efficiency is effectively increased and up to 0.058%. The ethanol is a well hydrocarbon as the fuel. At the last, we try to optimize the system by tuning the ratio of these two materials. When the ratio of these two material is 0.5:1, it has the highest quantum efficiency and up to 0.072%. By this study, the p-n junction structure can effectively enhance the photocatalytic CO2 reduction.

    致謝 I 中文摘要 III Abstract IV 目錄 VI 圖目錄 IX 表目錄 XIII 第一章 緒論 1 1-1 前言 1 1-2 研究動機與目的 3 第二章 文獻回顧 5 2-1 硫化亞銅(Cu2S)半導體材料性質 5 2-2 二硫化錫(SnS2)半導體材料性質 9 2-3 溶劑熱法 (Solvothermal method) 14 2-4 二氧化碳還原技術發展 17 2-4-1 金屬氧化物觸媒系統 23 2-4-2 金屬硫化物觸媒系統 27 2-4-3 半導體複合材料觸媒系統 28 第三章 實驗設備與方法 33 3-1 儀器設備 33 3-2 實驗藥品與器材 34 3-3 實驗步驟 35 3-3-1 二硫化錫(SnS2) 35 3-3-2 硫化亞銅(Cu2S) 35 3-3-3 硫化亞銅/二硫化錫混合物(Cu2S/SnS2) 36 3-4 實驗方法 37 3-4-1 溶劑熱法(Solvothermal method)合成 37 3-4-2 離心法(Centrifugation)合成粉末 38 3-5 材料鑑定與分析 39 3-5-1 場發射掃描式電子顯微鏡 (Field-Emission Scanning Electron Microscope, FE-SEM) 39 3-5-2 X光繞射儀 (X-ray Diffraction, XRD) 40 3-5-3 拉曼振動光譜儀 (Raman Spectrum, Raman) 41 3-5-4 穿透式電子顯微鏡 (Transmission Electron Microscope, TEM) 43 3-5-5 能量色散X射線光譜(Energy Dispersive Spectroscopy, EDS) 44 3-5-6 紫外-可見光光譜儀 (UV-Visible Spectroscopy) 45 3-5-7 紫外光電子能譜(Ultraviolet Photoelectron Spectroscopy, UPS) 46 3-5-8 X射線光電子能譜儀(X-ray Photoelectron Spectroscopy, XPS) 48 3-6 二氧化碳還原系統 50 第四章 實驗結果與討論 53 4-1 SnS2與Cu2S與Cu2S/SnS2的性質分析 53 4-1-1 SnS2的表面輪廓與成分分析 55 4-1-2 SnS2的晶體結構分析 56 4-1-3 不同環境下成長之Cu2S的表面輪廓與成分分析 58 4-1-4 不同環境下成長之Cu2S的晶體結構分析 59 4-1-5 Cu2S/SnS2異質結構的表面輪廓與成分分析 64 4-1-6 Cu2S/SnS2異質結構的晶體結構分析 65 4-1-7 元素分析 69 4-1-8 光學性質分析 71 4-2 利用GC-FID測量光觸媒效率 76 4-2-1 Cu2S、SnS2與Cu2S/SnS2的生成產物與產量比較 77 4-2-2 量子轉換效率比較 79 4-3 最佳化Cu2S及SnS2比例下所合成之混合相Cu2S/SnS2 80 4-3-1 不同比例之Cu2S與SnS2之混合相Cu2S/SnS2的晶體分析 81 4-3-2 不同比例之Cu2S與SnS2之混合相Cu2S/SnS2的生成產物與產量比較 83 4-3-3 量子轉換效率比較 86 第五章 結論 87 第六章 參考資料 88

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