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研究生:張又中
研究生(外文):Yu-Chung Chang
論文名稱:官能基調變氧化石墨烯之二氧化碳光催化之研究
論文名稱(外文):Modulation on the surface functionalities of GOx for CO2 photoreduction
指導教授:王丞浩
指導教授(外文):Chen-Hao Wang
口試委員:林麗瓊陳貴賢鍾博文林昇佃
口試委員(外文):Li-Chyong LinKuei-Hsien ChenPo-Wen ChungShawn-D Lin
口試日期:2020-01-21
學位類別:博士
校院名稱:國立臺灣科技大學
系所名稱:材料科學與工程系
學門:工程學門
學類:材料工程學類
論文種類:學術論文
論文出版年:2020
畢業學年度:108
語文別:英文
論文頁數:90
中文關鍵詞:二氧化碳還原光觸媒氧化石墨烯
外文關鍵詞:CO2 reductionPhotocatalystGraphene oxide
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本研究利用官能基調變氧化石墨烯作為可見光驅動的無金屬碳基觸媒進行二氧化碳還原光催化。為了瞭解氧化石墨烯表面上之含氧官能基在進行二氧化碳光催化石所扮演的腳色,本研究利用管狀高溫爐在氬氣環境升溫超過600度將含氧官能基從氧化石墨烯(As-GO)表面移除,通過此步驟可以得到表面官能基主要為羥基(-OH)的改質氧化石墨烯(M-GO),改質氧化石墨烯在二氧化碳光催化的效能在碳氫化合物的產量得到效能增長。透過反向滴定法測得各氧化官能基在氧化石墨烯及改質氧化石墨烯上的比例,進一步使用鹼基將官能基中和並測量二氧化碳光催化產率;在此一結果上可以證明羥基(-OH)是二氧化碳光催化的主導官能基。
This work demonstrates a metal-free photocatalyst for visible-light-driven CO2 redaction via a selective-functional-group of graphene oxide (GO) by rapid annealing process under the Ar environment. The oxygenated group of GO facilitates CO2 photoreduction reaction; however, the primary function of oxygen contained groups is still not clear. In this study, as-prepared graphene (As-GO) and modified graphene oxide (M-GO) have been investigated for CO2 reduction. Mostly, the oxygen functional groups on the GO’s basal plane have been removed as the temperature exceeds 400 oC, but the hydroxyl functional groups persistently bond strongly with carbon, especially localized on the edge side of graphene oxide. The M-GO optimized by the treated temperature performs a higher CO2 reduction reaction (CO2RR), promoting the yield of hydrocarbon products during the reaction process. The Boehm titration and surface neutralization graphene oxide were done for the investigation of the oxygen-containing functional group's contribution.
摘要 I
Abstract II
Acknowledgment III
Contents IV
Lists of Figures VI
Lists of Tables X
Chapter 1 Introduction 1
1-1 Globe Warming and CO2 Property 1
1-2 CO2 Utilization and Strategies 1
1-3 Photocatalytic CO2 reduction 4
1-4 Thermodynamics of CO2 Conversion 11
1-5 Challenges for CO2 Photoreduction 13
1-6 Graphene Oxide as Photocatalysts 16
1-7 Characteristic of Oxygen Containing Functional Groups via Boehm Titration 18
1-8 CO2 Adsorption Ability of Various Oxygen Containing Functional Groups on Graphene Oxide Surface 21
Chapter 2 Motivation 26
2-1 Narrow Band Gap Graphene Oxide for CO2 Photoreduction 26
2-2 Investigation of Functional Groups Contribution for CO2 Photoreduction 27
Chapter 3 Experimental and Instrumental Setup 29
3-1 Materials 29
3-2 Synthesis of Graphene Oxide (As-GO) 29
3-3 Synthesis of Modified Graphene Oxide 30
3-4 Boehm Titration and Surface Neutralized GO 31
3-5 UV-visible Absorption Measurement 33
3-6 Raman Spectroscopy, Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS-FTIR) and X-ray Diffraction Pattern 34
3-7 X-ray Photoelectron Spectroscopy, Ultraviolet Photoelectron Spectroscopy (UPS) and X-ray Absorption Spectroscopy (XAS) measurement 35
3-8 Gas Chromatography Measurement 37
3-9 Photocatalytic CO2 Reduction Experiment 38
3-10 Standard Calibration Curves and Blank CO2 Photoreduction Measurement 40
3-11 Solar Spectrum and Quantum Efficiency Calculation 43
3-12 Wavelength Dependent, Power Dependent, and Relative Humidity CO2 Conversion Measurement 45
Chapter 4 Results and Discussions 47
4-1 Characterization of Graphene Oxide 47
4-2 Surface Neutralization of Graphene Oxide for CO2 Photoreduction Conversion Measurement 58
4-3 Environmental Influence of CO2 Photoreduction 64
Chapter 5 Conclusion 69
Reference 70
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