Partial oxidation of methane with Cu–Zn–Al catalyst in a dielectric barrier discharge

Chemical Engineering & Processing

Antonius Indarto, Dae Ryook Yang, Jelliarko Palgunadi, Jae-Wook Choi,
Hwaung Lee, Hyung Keun Song

Chemical Engineering and Processing, 2008, 47(1): 780-786

Abstract:
A series of methanol synthesis catalyst containing Cu–Zn–Al (CZA) were prepared by co-precipitation method and applied for partial oxidation of methane into methanol using dielectric barrier discharge (DBD). The methanol synthesis process was occurred at ambient temperature and atmospheric pressure. In our experiment, CZA showed a high catalytic activity to increase the production of methanol. The methanol selectivity of CZA-assisted plasma process was twice higher than that of non-catalytic plasma process. The addition of other metals on CZA catalyst also produced a significant effect on the methanol production and it was found that yttrium could the best addition metal compared to Pt, Fe, and Ni. Instead of methanol, the reaction products of plasma reactions were dominated by H2, CO, CO2, C2 and water. The optimum methanol selectivity reached 27% when 3% yttrium metal was doped over CZA.

Keywords: Methane oxidation; Methanol synthesis; Dielectric barrier discharge; Cu–Zn–Al; Heterogeneous catalyst 

© 2007 Published by Elsevier B.V
 

Decomposition of CCl4 and CHCl3 on gliding arc plasma

Journal of Environmental Science

Antonius Indarto, Jae-Wook Choi, Hwaung Lee, Hyung-Keun Song

Journal of Environmental Sciences, 2006, 18(1): 83 – 89

Abstract:
Decomposition of chlorinated hydrocarbons, CCl4 and CHCl3, in gliding plasma was examined. The effects of initial concentrations, total gas flow rates, and power consumption have been investigated. The conversion result was relatively high. It reached 80% for CCl4 and 97% for CHCl3. Using atmospheric air as the carrier gas, the plasma reaction occurred at exothermic reaction and the main products were CO2, CO, and Cl2. Transformation into CCl4 was also detected for CHCl3 decomposition reaction. The conversion of CCl4 and CHCl3 were increased with the increasing applied frequency and decreasing total gas flow rate.

Keywords: plasma-gliding arc, CCl4, CHCl3, decomposition reaction

Discharge characteristics of a gliding-arc plasma in chlorinated methanes diluted in atmospheric air

Plasma Devices and Operations

Antonius Indarto, Jae-Wook Choi, Hwaung Lee, Hyung Keun Song, Nowarat Coowanitwong

Plasma Devices and Operations, 14(1), 15 – 26

Abstract:
Plasma processing of the chloromethane compounds (methylene chloride (CH2Cl2), chloroform (CHCl3) and carbon tetrachloride (CCl4)) diluted in atmospheric air using a gliding arc has been studied. Various injected initial chloromethane concentrations, total gas flow rates and power frequencies were used as the variables to investigate the discharge characteristics. This paper evaluates the phenomenon of chloromethane processing by gliding-arc plasma.

Keywords: Plasma; Gliding arc; Chloromethanes; Alternating-current waveform; Equilibrium voltage; Voltage breakdown

Treatment of CCl4 and CHCl3 emission in a gliding-arc plasma

Plasma Devices and Operations


Antonius Indarto; Jae-wook Choi; Hwaung Lee; Hyung Keun Song

Plasma Devices and Operations, 14(1), 1 – 14
Abstract:

The decomposition of the chlorinated hydrocarbons CCl4 and CHCl3 in a gliding-arc plasma was examined. The effects of initial concentrations, total gas flow rates and power consumption were investigated. The conversion of the hydrocarbons mentioned above was relatively high. It could reach 80% for CCl4 and 97% for CHCl3. In atmospheric air as a carrier gas, the reaction was exothermic, and the main products were CO2, CO and Cl2. The transformation into CCl4 was also detected for the decomposition reaction of CHCl3. The conversion of these compounds increased with increasing frequency of power supplied and decreasing total gas flow rate.

Keywords: Plasma; Gliding arc; CCl4; CHCl3; Decomposition reaction

Kinetic of CO2 Reduction by Gliding Arc Plasma

Asian Journal of Water, Environmental and Pollution

Antonius Indarto

Asian Journal of Water, Environment and Pollution, 2007, 4(1): 191-194

Abstract:

Decomposition of carbon dioxide (CO2) by gliding arc plasma was examined. The plasma device consisted of two triangular stainless steel plates. The gas entered through a nozzle tube from the upstream cylinder reactor and exit at a downstream of the reactor. The effect of total gas flow rates have been used to study the chemical process reaction in gliding plasma system. The model of active-chemical kinetic of CO2 decomposition was developed to investigate the pathways of plasma reactions. Experimental results indicate the conversion of CO2 reached 18% at the total gas flow rate of 1.5 × 10-5 m3s-1 and produced CO and O2 as the final products.

Keywords: Plasma, gliding arc, CO2, kinetic reaction, decomposition

Effect of additive gases on methane conversion using gliding arc discharge

Energy

Antonius Indarto, Jae-Wook Choi, Hwaung Lee, and Hyung Keun Song

Energy, 2006, 31(14): 2986-2995

Abstract:
Methane conversion using gliding arc plasma has been studied. The process was conducted at atmospheric pressure. Four kinds of additive gases—helium, argon, nitrogen, and CO2—were used to investigate their effects on methane conversion, as well as product selectivity, and discharged power. Methane conversion was increased with the increasing concentration of helium, argon, and nitrogen in the feed gas but decreased when CO2 concentration increased. Qualitatively, hydrogen and acetylene were the major gas products. No liquid product was produced.

Keywords: Methane conversion; Plasma; Gliding arc discharge; Additive gas

© 2006 Published by Elsevier B.V

Partial Oxidation of Methane with Sol-Gel Fe/Hf/YSZ Catalyst in Dielectric Barrier Discharge: Catalyst Activation by Plasma

Journal of Rare Earths

Antonius Indarto, Jae-Wook Cho, Hwaung Lee, Hyung Keun Song, and Jelliarko Palgunadi

Journal of Rare Earths, 2006, 24(5): 513-518

Abstract:

A 1% Fe-30% Hf over yttria-stabilized zirconia catalyst in combination with novel plasma-assisted activation techniques for a direct partial oxidation of methane to methanol was tested using dielectric barrier discharge plasma at ambient temperature and atmospheric pressure. However, instead of methanol, the reaction products were dominated by H2, CO, CO2, C2, and H2O. A catalytically activated plasma process increased the production of methanol compared with a noncatalytic plasma process. The maximum selectivity of methanol production was achieved using a catalyst that was treated at higher applied power.

Keywords: methane oxidation; dielectric barrier discharge; catalyst; plasma activation; rare earths

Methane Conversion Using Dielectric Barrier Discharge: Comparison with Thermal Process and Catalyst Effects

Journal of Natural Gas Chemistry

Antonius Indarto, Jae-Wook Choi, Hwaung Lee and Hyung Keun Song

Journal of Natural Gas Chemistry, 2006, 15(2): 87-92

Abstract:

The direct conversion of methane using a dielectric barrier discharge has been experimentally studied. Experiments with different values of flow rates and discharge voltages have been performed to investigate the effects on the conversion and reaction products both qualitatively and quantitatively. Experimental results indicate that the maximum conversion of methane has been 80% at an input flow rate of 5 ml/min and a discharge voltage of 4 kV. Experimental results also show that the optimum condition has occurred at a high discharge voltage and higher input flow rate. In terms of product distribution, a higher flow rate or shorter residence time can increase the selectivity for higher hydrocarbons. No hydrocarbon product was detected using the thermal method, except hydrogen and carbon. Increasing selectivity for ethane was found when Pt and Ru catalysts presented in the plasma reaction. Hydrogenation of acetylene in the catalyst surface could have been the reason for this phenomenon as the selectivity for acetylene in the products was decreasing.

Key words: plasma; dielectric barrier discharge; thermal process; methane conversion; catalyst

Advanced VOCs decomposition method by gliding arc plasma

Chemical Engineering Journal 

Short communication

Antonius Indarto, Dae Ryook Yang, Che Husna Azhari, Wan Hanna Wan Mohtar, Jae-Wook Choi, Hwaung Lee and Hyung Keun Song

Chemical Engineering Journal, 131 (1-3), 337-341

Abstract:

The decomposition of a series of volatile organic compounds (VOCs) has been carried out by gliding arc, a new-interest type of plasma technology in our laboratory. The operation of gliding arc was done at ambient temperature and normal pressure. Feed compositions were containing 0.1–0.5% of aromatic VOCs and 1–8% of chlorinated VOCs diluted in atmospheric air and total flow rates were varied from 3 to 5 L/min. Significant conversions (>50%) of VOCs with high destruction efficiency have been achieved in gliding arc plasma.

Keywords: Plasma; Gliding arc; Decomposition reaction; Aromatic VOCs; Chlorinated VOCs

Dispersion force

Dispersion force?

Currently, dispersion forces calculation is becoming hot and challenging topic in computational chemistry. Although many scientific papers have been published but none of them represent the clear definition and explanation about this phenomena. Dispersion force is a non-covalent bond intermolecule interaction. This kind of interaction is quite important and we can find in many areas, such as DNA stacking, interaction of  graphite layers, molecular recognation behavior, and so on. This kind interaction is usually existed in the ring-type molecules which contain pi bonding system. It is weak long-range attractive force between molecule and exist even without charge or with permanent charge. It is known as a complicated quantum system.

In order to approach the complexcity of dispersion system, people tried first to use the simpler configuration. In aromatic pi-ring interaction, we can devide into three non-covalent bond that usually exsist: pi-cation, pi-hydrogen, and pi-pi type. Among these, pi-cation bond has the largest energy which is around 10-35 kcal/mol and the others two has lower at 2-4 kcal/mol. The pi-pi bond will be stronger in the bigger molecules as this bond was occured among electron in the pi system of two moieties.
Computation calculation

How to calculate it? It is rather tricky ways. Different from the common method, the calculation to find it slightly different from the others computational calculation. It probably there is no perfect method or function that addrest directly to this issue. Usually people will use point-to-point calculation, means that you calculate the optimized structure and corrected by counter-poise calculation. It is because when you calculate one moeity, you will use another function of the other moieties to calculate it. Counter-poise calculation will calculate the current moiety and give ‘zero’ for the other functions.

Phyrene dimers

Simple HF calculation is not applicable for this case as the function has ‘too little’ describing this interaction. Common density functional theory (DFT) is also give a little un-corrected value. So, 2nd order Moller-Plesset (MP2) could be nice combined with moderat basis sets, eg. 6-31G(d), 6-31G*, 6-31+G*. MP2 is known to be overestimate the real value, means produce more negative value interm of correlation energy compared to couple-clusters method CCSD but it require less computational time. Just to give an imagination for how long to do the calculation, for dimers phyrene, using home PC-spect, I spent one week long only for the optimization!!!!

If you want to know detail about this, you can read the review paper about dispersion forces. Please klik this paper to download it.