還原氧化石墨烯擔載之雙金屬鈀金奈米觸媒於雙氧水綠色生產之應用

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研究生：	黎玉瓊花 Le - Ngoc Quynh Hoa
論文名稱：	還原氧化石墨烯擔載之雙金屬鈀金奈米觸媒於雙氧水綠色生產之應用 Reduced Graphene Oxide supported bimetallic Pd-Au nanocatalysts for green production of Hydrogen Peroxide
指導教授：	黃炳照 Bing-Joe Hwang
口試委員:	周澤川 Tse-Chuan Chou 林智汶 Chi-Wen Lin 周宏隆 Hung-Lung Chou
學位類別：	碩士 Master
系所名稱：	工程學院 - 化學工程系 Department of Chemical Engineering
論文出版年：	2014
畢業學年度：	102
語文別：	英文
論文頁數：	97
中文關鍵詞：	還原氧化石墨烯、雙金屬鈀金奈米、雙氧水
外文關鍵詞：	Reduced Graphene Oxide, bimetallic Pd-Au, Hydrogen Peroxide
相關次數：	點閱：299 下載：3
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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. General aspects and application of H2O2	1
2. The production of H2O2	5
3. Direct synthesis of H2O2	9
4. Drawback in the catalytic direct synthesis of H2O2	11
CHAPTER II	14
LITERATURE REVIEW & OBJECTIVE	14
1. Catalysts used in the direct synthesis of H2O2 from H2 and O2	14
1.1 Direct synthesis of H2O2 by bimetallic alloy Pd-Au/C	16
1.2 Reduced graphene oxide support of Pd-Au nanoparticles for direct synthesis H2O2	17
1.3 Synthesis of graphite oxide support	19
2. Synthesis of alloy & core-shell bimetallic Pd-Au/rGO	20
3. X-ray absorption spectroscopy (XAS) [23]	24
4. Electrochemical measurement	27
4.1 Electrochemical measurement of H2O2 detection with RDE	27
4.2 Linear sweep voltammetry (LSV)	28
4.3 Cyclic Voltammogram	31
4.4 Chronoamperometry	32
5. Research challenge	34
6. Research Objective	34
CHAPTER III	35
EXPERIMENTAL AND INSTRUMENTAL SETUP	35
1. Materials	35
2. Preparation of bimetallic catalyst Pd-Au/reduced graphene oxide and modified functional group of reduced graphene oxide.	35
3.	Synthesis of graphite oxide	36
4.	Synthesis of bimetallic PdAu/rGO in oil bath	38
5.	Synthesis of modified reduced graphene oxide (mrGO)	39
6. Synthesis of PdAu catalyst supported on modified reduced graphene oxide (mrGO)	41
7. Instrumentation	43
7.1 X-Ray diffraction (XRD)	43
7.2. Transmission electron microscopy (TEM)	45
7.3. Field emission scanning electron microscope (FESEM)	46
7.4. Fourier transforms infrared spectroscopy (FTIR)	48
7.5. RAMAN spectroscopy	48
7.6. Electrochemical measurement test	50
CHAPTER IV	52
RESULTS AND DISCUSSION	52
1. Synthesis of graphite oxide	52
1.1 X-ray diffraction of graphite oxide	52
1.2 SEM of reduced graphene oxide	53
2. Synthesis of Pd-Au/reduced graphene oxide	54
2.1 XRD of PdAu/rGO	55
2.2 X-ray adsorption of PdAu/rGO	57
2.3 TEM images of PdAu/rGO	59
2.4 Electrochemical measurement	62
3. Synthesis of Pd-Au/modified reduced graphene oxide	68
3.1 XRD of modified reduced graphene oxide	68
3.2 Electrochemical measurement of Pd-Au/modified rGO	70
4. Comparison between PdAu/rGO and PdAu/mrGO	72
4.1 Raman Spectroscopy	72
4.2 Performance of PdAu/rGO and PdAu/mrGO	74
5. Comparison of our result with literature	75
CHAPTER V	78
CONCLUSION	78

                                

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