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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