臺灣博碩士論文加值系統

The use of palladium membranes for industrial applications has gained much interest as of late. The purification of hydrogen through palladium (Pd) membranes has therefore been proposed as a viable solution to traditional separation methods. It is believed that hydrogen permeation can be enhanced when coupled with a vacuum at the permeate side. This study was divided into two parts.
The first part of the study focuses on the effects of various vacuum degrees applied to the permeate side of the Pd membrane, where the results under normal operation were compared to that without a vacuum. The feed gas used for experiments consists of a mixture of hydrogen (70 vol%) and nitrogen (30 vol%). Three membrane operating temperatures (320, 350, and 380 °C), four pressure differences (2, 3, 4, and 5atm) across the membrane, and four vacuum degrees (-15, -30, -45, and -53 kPa) applied to the permeate side are considered. For the three operating temperatures, the best improvements in the performance of hydrogen permeation are at 320 and 350 °C when a -53 kPa vacuum is applied, resulting in 79.4% and 79.1% improvements, respectively, compared to normal operations. Increasing temperatures leads to an increase in H2 permeation both with and without a vacuum; however, best performances of H2 permeation are observed in cases without a vacuum.
In the second part, the effect of different degrees of vacuum pressures on H2 permeation through a high-perm selectivity Pd membrane in different binary gas mixtures was investigated and compared to those without vacuum. Three feed gases were used containing three different H2 concentrations, which were 90, 70, and 50 vol% for each gas mixture. Hydrogen permeation rates were studied at 320, 350, and 380 °C under vacuum pressures ranging between 0 to -60 kPa. It was found that an increase in vacuum degree intensified H2 permeation. However, best performance improvements were observed at lower H2 concentrations, lower temperatures, and also at lower vacuum pressures for all gas mixtures. The highest performance improvement of 88.83% was with the gas mixture containing 50% H2 at 320 °C with a -15 kPa vacuum pressure. However, from an efficiency point of view, lower temperatures and vacuum pressures were preferred for all the gas mixtures, since the best improvements in H2 permeations under those conditions. This would minimize the overall energy requirements of the system for H2 purification. Activation Energies were also relatively lower for conditions with a vacuum for all gas mixtures.

Abstract i
Acknowledgements iii
Table of Contents iv
List of Tables vi
List of Figures vii
Nomenclature x
Chapter 1. Introduction 1
1.1 Background 1
1.2 Motivation and objectives 4
1.3 Schematics of experimental procedures 5
Chapter 2. Literature Review 7
2.1 Gas mixtures 7
2.2 Activation energy 8
2.3 Vacuum technologies 8
Chapter 3. Methodology 13
3.1 Membrane tubes 13
3.2 Experimental set up 15
3.3 Operating conditions 20
3.3.1 Experiment 1 20
3.3.2 Experiment 2 21
3.4 Experimental procedure 22
3.5 Mechanism for hydrogen transport through the Pd membrane 24

Chapter 4. Results and Discussion 26
4.1 H2 permeation enhancements in membrane 1 of gas mixture: 70%H2+30%N2 under various vacuum pressures 26
4.1.1 The effect of vacuum on hydrogen permeation 26
4.1.2 Effect of membrane temperature 33
4.1.3 Permeance and concentration polarization 36
4.1.4 Permeance mechanism of a vacuum 40
4.2 H2 permeation enhancements in membrane 2 of three different gas mixtures with different H2 concentrations under various vacuum pressures 41
4.2.1 Influence of vacuum on hydrogen permeation 41
4.2.2 Hydrogen permeation improvement under different vacuum degrees …................................................................................... 49
4.2.3 Effect of membrane temperature 53
4.2.4 Pressure exponent 56
4.2.5 Activation energy 62
Chapter 5. Conclusions and Future Work 68
5.1 Conclusions 68
5.2 Future works 69
Appendix A. Reproducible data of the first study 71
Appendix B. Reproducible data of the second study 72
References 75
自述 84

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