Chapter 6 Conclusion and Future Work
6.2 R ECOMMENDATIONS FOR F UTURE W ORK
i. To adjust the temperatures in PAC system with Rh catalyst for much better reforming selectivity.
ii. To change the ratio of water mixed ethanol to solve the Ni0.35Mg2.65FeO4.5
catalyst is worse in WGS reaction.
iii. To design the MGAD for the shorter residence time of PAC with gliding at higher air flow rate. The detailed design and simulate has been done and showed in Appendix B.
iv. To raise the catalyst reforming temperature for confirm the highest selectivity Ni0.35Mg2.65FeO4.5.
v. To exchange the sequence between plasma and catalyst in PAC system for investigation on the variation.
vi. To combine the plasma with other non-noble catalyst, which has better selectivity and simultaneously is low cost.
vii. To investigate that the effect of gaps between two electrodes in gliding arc plasma for hydrogen production.
viii. To analyze the chemical reaction in plasma alone, catalyst alone, and PAC reforming.
34
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42
Appendix A.
Discussion of Gliding Arc in Tornado (GAT)
To built gliding arc in tornado (GAT) reactor, there are still a lot of details need to be concerned. For gliding arc plasma reactor, the evolution of gliding arc plasma starts at the shortest distance (usually 2-5 mm)
[A. Fridman et al., 2005, Z. Bo et al., 2007]
between two diverging electrodes when applied voltage reaches the breakdown voltage value. Immediately after breakdown, the spark channel is formed crossing the gap between the blades. However, the GA system is a two-dimensional (2D) electrode geometry causing low gas residence time in the reactor. The purpose of GAT system [A. Fridman et
al., 2005] is used to solve the above-mentioned drawbacks. Therefore, the GAT develop
those advantages, which include: a cylindrical three-dimensional (3D) geometry which is called reverse vortex flow (Tornado), higher residence time than traditional GA.
The electrodes of GAT include three parts (In Figure Appendix A. 1. (a)): 1. The spiral electrode which is set and designed to harmony with the flow field shaped into tornado. 2. Circular electrode which consists of a circular electrode as anode at the top.
Additionally, we hope to get the reverse vortex flow, so the GAT chamber is equipped with swirl generator (In Figure Appendix A. 1. (b)). The new gliding arc reactor using a
43
reverse vortex flow in a cylindrical chamber is called gliding arc in tornado (GAT) that contains the advantages and overcome the disadvantage of the traditional GA. The PAC system with GAT in some literatures
[Nongnuch Rueangjitt, 2011] shows the excellent
residence time and near-perfect thermal insulation for the reactor chamber because of the fiercely forced convection. However, the applications of GAT always is used very high flow rate (>10slm) to push the arc along the spiral electrode in the literature surveys[Liang Yu et al., 2011; Alexander F. Gutsol, 2011]. Furthermore, the results of the
simulate flow field (Figure Appendix A. 2), which show most gases fast exhaust through the outlet in GAT system , caused the most fuels to be squandered. Figure Appendix A. 3 and table Appendix A. 1 show the simulate model and conditions, respectively.
44
Appendix B.
Discussion of Magnetic Gliding Arc Discharge (MGAD)
The reactor of MGAD (in (Figure Appendix B. 1) is combined the magnetic around the grounded electrode with the stainless steel of power electrode which is anodic cylinder with spiral. The based principle is Ampere force which is comprised by I (Current through the conductor) cross V (Strength of magnetic force). A reactor of MAGD was built with dc power supply by S. P. Gangoli
[S.P. Gangoli et al., 2010].
Futhremore, the simulate MGAD has been accomplished in the model showed in Figure
Appendix B. 2 and conditions at table Appendix B. 1. In the simulation, the fuel via
tangentially inlet, which let the gases pass through more paths, is injected to reactor and go through the plasma region. And then the results showed that MGAD possesses more excellent residence time than gliding arc because of lower flow velocity over plasma region in figure Appendix B. 3 (MGAD with 0.58 m/s, GA with ~20 m/s). However, the ethanol and water are very possible to condense at the wall without plasma region because of the closed room temperature, design carefully for this problem.
45
Appendix C.
Hydrogen Reduction Furnace
The traditional reduction method of combines the catalyst boat with the quartz of thick diameter at high temperature 600 ℃ and hydrogen mass flow rate of 200 SCCM in 6 hours. However, this reduction method waste a lot of costs because in base of
hydrodynamics most hydrogen doesn’t contact with the catalyst. For frequently using the furnace to manufacture catalyst in study, this squander should be ameliorated as soon as possible. Therefor, the new reduction furance has been design and accomplished in this study.
Figure appendix C. 1 shows interior structure of the new reduction furance in
detail. First, the vertically stainless flow channel with the thin grill sieve is fixed on thepedestal. And then, the catalyst is placed on the sieve in an quartz with 41 mm of inner diameter around high temperature 650 (℃). Finally, the hydrogen goes through the
catalyst and carries out the O atoms to accomplish the hydrogen reduction.
Table appendix C. 1 and figure appendix C. 3 shows the detailed test conditions and the
appearance construction respectively. In the preliminary test using Ni0.35Mg2.65FeO4.5
catalyst, the successful outcomes shows that the new system economize on hydrogen mass flow very well rate during the reducion process (figure appendix C. 2).
46
Table 1.1:
Properties of ethanol steam reforming with different noble metal catalysts.47
Table 1.2: P
roperties of ethanol steam reforming with different non-noble metal catalysts.48
1. C: conversion rate 2. S: selectivity 3. E: efficiency
Table 1.3: Summary of important features, experiments and parameters for plasma alone
reforming.49
1. C: conversion rate 2. S: selectivity 3. E: efficiency
Table 1.4: Summary of important features, experiments and parameters for PAC.
50
Author Phase Power generator Power input
Y. Kusano
et al.
(2008)
AC
Power supply (Generator 6030. SOFTAL Electronic
GmbH, Germany).
DC Power supply (Universal Voltronics, Inc.)
Input voltage: 10 kV
Pulse modulator (Kurita Seisakusho Co., Ltd., 6 kW)
Slide regulator (Matsunaga Seisakusho, S3-2413, 5.2
kVA)
High-voltage transformer (Kurita Seisakusho Co., Ltd.,
250/12 kV)
Input power: 300 W
Pulse frequency: 15-20 kHz
Pulse width: 1.6-2.8 μs
Table 1.4: Summary of plasma power input type.
51
Reforming Fuel C/O Ratio Catalyst
Plasma
Table 3.1: Test Condition of gliding arc, catalyst(Rh/CeO
2/Al2O3), PAC with gliding arcreforming
Table 3.2: Test Conditions of catalyst (Ni0.35Mg2.65FeO4.5), PAC with gliding
reforming
52
Air Flow Rate
Compositions
0.5 SLM
H
2, CO
2, CO, CH
4,C
2H
4(trace), C
2H
6(trace), H
2O, EtOH
1.0 SLM
H
2, CO
2, CO, CH
4, H
2O, EtOH
1.5 SLM
H
2, CO
2, CO, CH
4, H
2O, EtOH
2.0 SLM
H
2, CO
2, CO, CH
4, H
2O, EtOH
Table 5.1: The composition after the plasma reactor at a C/O ratio of 0.7 at different air
flow rates.53
The Simulate conditions in GAT
Parameter Range
MFR (SLM) 2
IA(°) 0°-30°
B.C Outlet：101,300 Pa = 1 atm
Wall：Stationary Wall
I.C 101,300 Pa = 1 atm
Gravity ( ) -9.8
Number of Mesh 500,000
Number of Iterations 2,000
1. MFR: Mass Flow Rate 2. IA: Injected Angle 3. B.C.: Boundary Conditions 4. I.C.: Initial Condition
Table Appendix A. 1: The parameters for simulation of gliding arc in tornado.
54
The Simulate conditions in MGAD
Parameter Range
MFR (SLM) 2
B.C Outlet：101,300 Pa = 1 atm
Wall：Stationary Wall
I.C 101,300 Pa = 1 atm
Gravity ( ) -9.8
Number of Mesh 500,000
Number of Iterations 2,000
1. MFR: Mass Flow Rate 2. IA: Injected Angle 3. B.C.: Boundary Conditions 4. I.C.: Initial Condition
Table Appendix B. 1: The parameters for simulation of magnetic gliding arc
discharge.
55
Test Reduction Time (hr) H2 Flow Rate (SCCM)
Furnace Temperature (℃)
Sample 1 5 50 650
Sample 2 2 30 650
Sample 3 0.5 30 650
Table Appendix C. 1: The parameters for testing the reduciton furnace.
56
FIGURE
Figure 1.1: Sketch of the typical test arrangement for ethanol reformer (left) and the SOFC
(right) at CGET of NCTU.
Figure 1.2: The basic reaction of ethanol steam reforming [Vizcaino et al., 2007].
57
Fig. 1.3: Comparisons of yields for non-thermal (new plasmatron) and thermal (old
plasmatron) plasmas [G. Petipas, et al., 2007].
Fig. 1.4: The comparison between different plasma reactors [G. Petipas, et al., 2007].
58
Figure 1.5: An energy diagram indicating the standard enthalpy (△H°) and free energy
changes (△G°) in kJ/mol for the reactions in a renewable energy cycle operating between CO2 and biomass [L. D. Schmidt, et al., 2004].
Figure 1.6: Typical arrangement of instrumentation for PAC system [Y. C. Yang et al.,
2009].
59
Figure 2.1: Schematic of gliding arc reactor. [A. Fridman et al., 2002].
60
Figure 2.2: (a) voltage waveform of gliding arc prduction; (b) current waveform of gliding
arc production [Antonius I. et al., 2006].
Figure 3.1: The experimental arrangement of PAC system.
61
Figure 3.2: Gas Chromatograph.
62
Figure 3.3: The self-designed gliding arc reactor.
Figure 3.4: PVM500 plasma driver
63
Figure 3.5: The MFC and liquid pump.
Figure 3.6: The fuel Injections
64
Figure 3.7: The furnaces for heating system
Figure 3.8: The Rh catalyst setup procedure.
65
Figure 3.9: The Ni
0.35Mg2.65FeO4.5catalyst setup procedureFigure 3.9: High-voltage probe.
66
Figure 3.10: Rogowski coil and Oscilloscope.
67
Figure 4.1: The visualization of gliding arc discharge. The parameters: air flow rate is 1..5
SLM; The plasma power from power supply is 223 W with 20 kHz
68
Figure 4.2: The visualization of comparison of the gliding arc with C/O ratio or not.
69
Figure 4.3: The elecreical properties- I-V wave form.
70
Figure 5.1: The conversion rate, S
H2 and SCO2 versus the C/O ratio with plasma alone.71
Figure 5.2: The conversion rate, S
H2 and SCO2 as functions of the air flow rate with plasma alone at a C/O ratio of 0.7.72
Figure 5.3: S
H2, SH2O and SCH4 as functions of the air flow rate with plasma alone at a C/O ratio of 0.7.73
Figure 5.4: S
CO2, SCO and SCH4 as functions of the air flow rate with plasma alone at a C/O ratio of 0.7.74
Figure 5.5: The conversion rate, hydrogen selectivity and carbon dioxide selectivity as
functions of the air flow rate with catalyst alone.
75
Figure 5.6: The conversion rate, hydrogen selectivity and carbon dioxide selectivity as
functions of the catalyst temperature with catalyst alone. (Ni0.35Mg2.65FeO4.5)
76
Figure 5.7: The conversion rate, hydrogen and carbon dioxide selectivity as a function air
flow rate for the cases of PAC with Rh catalyst.
77
Figure 5.8: The comparison of conversion rate between catalyst reforming and PAC
reforming using Ni0.35Mg2.65FeO4.5 catalyst.
78
Figure 5.9: The comparison of hydrogen selectivity between catalyst reforming and PAC
reforming using Ni0.35Mg2.65FeO4.5 catalyst.
79
Figure Appendix A. 1: GAT system in a cylindrical (a) a cross-sectional view (b) Top
view of swirl generator [Alexander Fridman, 2009].
80
(a)
(b)
Figure Appendix A. 2: The vector in air flow rate (a). The injection of vector in 0°
injected angle (b). The injection of vector in 30° injected angle
81
Figure Appendix A. 3: The simulate model in GAT system.
82
Figure Appendix B. 1: Composition of MGAD system (1) inner electrode (power cathode)
(2) outer anodic electrode (ground) (3) wire attached to inner electrode (4) magnet (5) the arc motion between two electrodes [S.P. Gangoli, et al., 2010].
83
Figure Appendix B. 3: The simulate model in MGAD system. Diameter of injection is
2mm; diameter of outlet is 4mm; diameter and length of model is 30mm and 100mm, respectively; and Gap between electrodes is 2mm;
84
Figure Appendix B. 3: The simulation of MGAD reactor. Flow velocity of z axial
direction at the plasma region.
85
Figure Appendix C. 1: The interior structure of reduction furance.
86
Figure Appendix C. 2: The apperance constructure of reduction furance.
87