臺灣博碩士論文加值系統

雙氧水在工業上非常廣用,為具有價值之化學品,其需求量近來日益增加。本研究以修飾還原氧化石墨烯擔載之鈀金(PdAu)奈米觸媒, 並利用直接合成法於室溫室壓條件下合成雙氧水。

首先製備各種不同PdAu組成之奈米觸媒,承載於還原氧化石墨 烯上,並以XRD, SEM, TEM, Raman, FTIR與電化學分析做鑑定。研 究結果發現以組成為Pd07Au03之奈米觸媒展現出對雙氧水產生有最 佳之活性,此可歸因於其具有較佳之雙金屬合金程度。接著將氧化石 墨烯做磺化(sulfonation)處理,並承載Pd07Au03之奈米觸媒於其上;結 果發現雙氧水產生的活性更進一步的提昇。

本研究成功地在室溫室壓條件下以修飾還原氧化石墨烯擔載之 PdAu奈米觸媒製備高產量之雙氧水。發展之PdAu奈米觸媒系統為 新穎且具有吸引力之提昇雙氧水產量之策略。

Hydrogen Peroxide is a valuable chemical with wide spread uses in industry; its demand is recently increasing due to its utilization. The modified reduced graphene oxide supported PdAu nanocatalysts were prepared for direct synthesis of hydrogen peroxide at ambient conditions in this work.

The various atomic ratios of PdAu nanocatalysts on reduced graphene oxides were synthesized and characterized by XRD, SEM, TEM, Raman, FTIR and electrochemical analysis. It is found that the Pd07Au03 nanocatalyst shows the highest productivity of hydrogen peroxide due to its higher alloying extent. The graphene oxides were further modified by sulfonation. The results indicate the productivity can be further improved when Pd07Au03 nanocatalysts were prepared on the modified reduced graphene oxide. The high productivity of hydrogen peroxide was successfully achieved on the developed PdAu/mrGO nanocatalysts at ambient conditions. The method developed for preparation of PdAu nanocatalysts on modified reduced graphene oxide opens a new and interesting direction for increasing productivity hydrogen peroxide.

ABSTRACT I
CHAPTER I 1
INTRODUCTION 1
1.1. General aspects and application of H2O2 1
1.2. The production of H2O2 5
1.3. Direct synthesis of H2O2 9
1.4. Drawback in the catalytic direct synthesis of H2O2 11
CHAPTER II 14
LITERATURE REVIEW &; OBJECTIVE 14
2.1. Catalysts used in the direct synthesis of H2O2 from H2 and O2 14
2.1.1 Direct synthesis of H2O2 by bimetallic alloy Pd-Au/C 16
2.1.2 Reduced graphene oxide support of Pd-Au nanoparticles for direct synthesis H2O2 17
2.1.3 Synthesis of graphite oxide support 19
2.2. Synthesis of alloy &; core-shell bimetallic Pd-Au/rGO 20
2.3. X-ray absorption spectroscopy (XAS) [23] 24
2.4. Electrochemical measurement 27
2.4.1 Electrochemical measurement of H2O2 detection with RDE 27
2.4.2 Linear sweep voltammetry (LSV) 28
2.4.3 Cyclic Voltammogram 31
2.4.4 Chronoamperometry 32
2.5. Research challenge 34
2.6. Research Objective 34
CHAPTER III 35
EXPERIMENTAL AND INSTRUMENTAL SETUP 35
3.1. Materials 35
3.2. Preparation of bimetallic catalyst Pd-Au/reduced graphene oxide and modified functional group of reduced graphene oxide. 35
3.3. Synthesis of graphite oxide 36
3.4. Synthesis of bimetallic PdAu/rGO in oil bath 38
3.5. Synthesis of modified reduced graphene oxide (mrGO) 39
3.6. Synthesis of PdAu catalyst supported on modified reduced graphene oxide (mrGO) 41
3.7. Instrumentation 43
3.7.1 X-Ray diffraction (XRD) 43
3.7.2. Transmission electron microscopy (TEM) 45
3.7.3. Field emission scanning electron microscope (FESEM) 46
3.7.4. Fourier transforms infrared spectroscopy (FTIR) 48
3.7.5. RAMAN spectroscopy 48
3.7.6. Electrochemical measurement test 50
CHAPTER IV 52
RESULTS AND DISCUSSION 52
4.1. Synthesis of graphite oxide 52
4.1.1 X-ray diffraction of graphite oxide 52
4.1.2 SEM of reduced graphene oxide 53
4.2. Synthesis of Pd-Au/reduced graphene oxide 54
4.2.1 XRD of PdAu/rGO 55
4.2.2 X-ray adsorption of PdAu/rGO 57
4.2.3 TEM images of PdAu/rGO 59
4.2.4 Electrochemical measurement 62
4.3. Synthesis of Pd-Au/modified reduced graphene oxide 68
4.3.1 XRD of modified reduced graphene oxide 68
4.3.2 Electrochemical measurement of Pd-Au/modified rGO 70
4.4. Comparison between PdAu/rGO and PdAu/mrGO 72
4.4.1 Raman Spectroscopy 72
4.4.2 Performance of PdAu/rGO and PdAu/mrGO 74
4.5. Comparison of our result with literature 75
CHAPTER V 78
CONCLUSION 78

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