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Plasma Enhanced Dry Reforming of Propane to Syngas over Ni-CeO_2/γ-AI_2O_3 Catalysts in DBD Reactor

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Abstract
Syngas (a mixture of CO and H_2) production from dry reforming of propane (DRP) over Ni-based catalyst has attained huge interests in the production of value-added oxygenated chemicals and high tech industrial applications as an environment-friendly process. A coaxial dielectric barrier discharge (DBD) reactor has been developed for DRP over Ni-CeO_2-γ/Al_2O_3 catalyst with 4 wt.% of cerium and nickel metals (2 wt% each). In addition, plasma-catalytic DRP has been carried out with the thermally and plasma-reduced Ni-CeO_2-γ/Al_2O_3 catalysts using the reactant ratio of C_3H_8/CO_2 at 1/3 at a total flow rate of 300 ml min^-^1. After general calcination in air, the Ni-CeO_2-γ/Al_2O_3 catalysts were reduced by thermal and plasma-assisted process in H_2/Ar atmosphere. The catalytic activities for DRP were evaluated at 500-600°C. Thermally and plasma-reduced (H_2 and plasma-assisted) catalysts' properties before and after DRP reactions were investigated using XRD, TEM, FE-SEM, temperature programmed reduction (H_2-TPR) techniques, temperature programmed desorption (H_2-TPD, CO_2-TPD) and Raman spectroscopy. The Ni-CeO_2-γ/Al_2O_3 catalyst prepared by plasma reduction exhibited better catalytic performance towards H_2 production, compared with thermally reduced catalysts, which is attributed to the nickel particles' nanoconfinement within the interaction between the support and favorable metal-support as a result of plasma-assisted reduction mechanism. One of the main concerns regarding the DRP process is catalyst deactivation due to excess amount of carbon deposition. The plasma-reduced Ni-CeO_2-γ/Al_2O_3 catalyst for the DRP process exhibited long term stability at 600°C for anti-sintering and coke resistance with high reactivity and durability without severe deactivation as a potential catalyst.
Author(s)
라미야술타나
Issued Date
2018
Awarded Date
2018. 2
Type
Dissertation
URI
http://dcoll.jejunu.ac.kr/jsp/common/DcLoOrgPer.jsp?sItemId=000000008467
Alternative Author(s)
Lamia, Sultana
Affiliation
제주대학교 일반대학원
Department
대학원 에너지응용시스템학부
Table Of Contents
TABLE OF CONTENTS I
LIST OF FIGURES IV
LIST OF TABLES VII
ABSTRACT
CHAPTER I 1
INTRODUCTION 1
1.1 Brief introduction from literature review 1
1.2 Objectives 2
1.3 Significance of Dry Reforming Research 3
1.4.The Scope of Research 3
CHAPTER II 4
LITERATURE REVIEW 4
2.1 Historical Background 4
2.2 Propane 7
2.2.1 Physical Properties 8
2.2.2 Chemical Properties 8
2.3 Carbon Dioxide 8
2.3.1 Physical Properties 9
2.3.2 Chemical Properties 9
2.4 Industrial Application of Syngas 9
2.5 Types of Reforming Technology 11
2.5.1 Steam Reforming 11
2.5.2 Dry Reforming Technologies 12
2.5.3 Tri Reforming 13
2.5.4 Auto-thermal Reforming 15
2.5.5 Partial Oxidation Using Oxygen (POX) 16
2.5.6 Thermo-catalytic Decomposition of Methane 17
2.6 Thermo-dynamical Study 17
2.7 Overview of Plasma Technology 18
2.7.1 Plasma 18
2.7.2 Classification of Plasma 19
2.7.3 Generation of Non-Thermal Plasma by Electric Fields 20
2.7.3.1 Corona Discharges 23
2.7.3.2 Glow Discharge 24
2.7.3.3 Gliding Arc Discharges 25
2.7.3.4 Atmospheric Pressure Plasma Jet 26
2.7.3.5 Radio Frequency Discharges 27
2.7.3.6 Microwave Discharges 28
2.7.3.7 Dielectric Barrier Discharges 28
CHAPTER III 30
EXPERIMENTAL METHODS 30
3.1 Experimental Overview 30
3.2 Catalyst preparation 31
3.3 Experimental Setup and Characterization of Reaction Performance 33
CHAPTER IV 36
RESULTS AND DISCUSSION
4.1 Characterization of the catalyst before reaction 36
4.1.1 TEM analysis 36
4.1.2 SEM analysis 38
4.1.3 Powder X-ray diffraction 39
4.1.4 Raman Spectral Study 41
4.1.5 TPR analysis 42
4.1.5.1 H_2-TPR analysis 43
4.2 Chemical Characterization of the Active Sites 44
4.2.1 TPD analysis 44
4.2.1.1 H_2-TPD analysis 44
4.2.1.2 CO_2-TPD analysis 46
4.3 Dry Reforming of Propane 47
4.3.1 Best Catalytic Performance with Applied Voltage in DRP 50
4.4 Characterization of the catalyst after reaction 52
4.4.1 SEM analysis 52
4.4.2 Raman spectroscopy 53
4.4.3 TPO analysis 55
CHAPTER V 57
CONCLUSION AND FUTURE DIRECTIONS
5.1 Conclusions 57
5.2-5.3 Future works and references 58
Degree
Master
Publisher
제주대학교 일반대학원
Citation
라미야술타나. (2018). Plasma Enhanced Dry Reforming of Propane to Syngas over Ni-CeO_2/γ-AI_2O_3 Catalysts in DBD Reactor
Appears in Collections:
Faculty of Applied Energy System > Energy and Chemical Engineering
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