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Design of Hollow Sphere MCM-22 Zeolites with Short Diffusion Length for Enhanced Aromatization Performance and Regeneration Capability

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Abstract in English vii
Abstract in Korean ix
List of Figures xii
List of Tables xvi

1 Introduction 1

2 Experimental Section 12
2.1 Synthesis of carbon sphere templates 12
2.1.1 Synthesis of carbon sphere 12
2.1.2 Synthesis of silica-coated carbon sphere 12
2.1.3 Synthesis of Alumina-coated carbon sphere 13
2.2 Synthesis of the MCM-22 catalysts 14
2.2.1 Synthesis of the original MCM-22 and
the two types of thin MCM-22 14
2.2.2 Synthesis of HS-MCM-22 zeolites with CS-Si templates- 15

2.2.3 Synthesis of HS-MCM-22 zeolite with CS-Al template 17
2.3 Catalyst characterization 19
2.4 Catalytic activity tests 21
2.5 Evaluation of acetylene Adsorption properties of zeolite catalysts
22
2.6 Evaluation of benzene desorption properties of zeolite catalysts- 23

3 Results and discussion 25
3.1 Effects of acid sites on thin MCM-22 zeolite catalysts
and their catalytic applications for acetylene aromatization 25
3.1.1 Structural properties of zeolite catalysts 25
3.1.2 Textural and acidic properties of catalysts 35
3.1.3 Catalytic performance on the aromatization of acetylene 41
3.1.4 Possibility of coke removal 50
3.2 Design of hollow sphere MCM-22 zeolite with minimal
extraframework Al and its enhanced aromatization
and regeneration capability 54
3.2.1 Development of thickness-controlled hollow sphere-type
MCM-22 catalyst particles 54

3.2.2 Analysis of zeolite framework, acid sites,
and extraframework aluminum 65
3.2.3 Evaluation of catalytic performance through aromatization
reaction of acetylene 74
3.2.4 Regeneration of spent catalysts and evaluation of second
reaction over regenerated catalysts 81
3.3 Behaviors of acetylene adsorption and benzene desorption
over hollow sphere MCM-22 catalyst for aromatization 90
3.3.1 Microscopic images and textural properties 90
3.3.2 Acid sites and framework/extra-framework aluminum species
96
3.3.3 Acetylene adsorption and benzene desorption tests 106

4 Conclusions 116
4.1 Effects of acid sites on thin MCM-22 zeolite catalysts
and their catalytic applications for acetylene aromatization 117
4.2 Design of hollow sphere MCM-22 zeolite with minimal
extraframework Al and its enhanced aromatization
and regeneration capability 118

4.3 Behaviors of acetylene adsorption and benzene desorption
over hollow sphere MCM-22 catalyst for aromatization 120

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