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Methane to Liquid Hydrocarbons over Tungsten-ZSM-5 and Tungsten Loaded Cu/ZSM-5 Catalysts

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Journal of Natural Gas Chemistry 2006年第4期15卷 340-347页

作者： Didi Dwi Anggoro nor aishah saidina amin Department of Chemical Engineering University of Diponegoro TembalangSemarang 50239Indonesia Faculty of Chemical and Natural Resources Engineering Universiti Teknologi MalaysiaJohor Bahru 81130Malaysia

Metal containing ZSM-5 can produce higher hydrocarbons in methane oxidation. Many researchers have studied the applicability of HZSM-5 and modify ZSM-5 for methane conversion to liquid hydrocarbons, but their research results still lead to low conversion, low selectivity and low heat resistance. The modified HZSM-5, by loading with tungsten （W）, could enhance its heat resistant performance, and the high reaction temperature （800 ℃） did not lead to a loss of the W component by sublimation. The loading of HZSM-5 with tungsten and copper （Cu） resulted in an increment in the methane conversion as well as CO2 and C5＋ selectivities. In contrast, CO, C2-3 and H2O selectivities were reduced. The process of converting methane to liquid hydrocarbons （C5＋） was dependent on the metal surface area and the acidity of the zeolite. High methane conversion and C5＋ selectivity, and low H20 selectivity are obtained over W/3.0Cu/HZSM.

关键词： methane liquid hydrocarbons HZSM-5 W-ZSM-5 W-Cu/ZSM-5

Screening of MgO- and CeO_2-Based Catalysts for Carbon Dioxide Oxidative Coupling of Methane to C_(2+) Hydrocarbons

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Journal of Natural Gas Chemistry 2004年第1期13卷 23-35页

作者： Istadi nor aishah saidina amin Chemical Reaction Engineering Group(CREG) Faculty of Chemical and Natural Resources EngineeringUnivevsiti Teknologi MalaysiaUTM SkudaiJohor Bahru81310 Malaysia

The catalyst screening tests for carbon dioxide oxidative coupling of methane (CO2-OCM) have been investigated over ternary and binary metal oxide catalysts. The catalysts are prepared by doping MgO- and CeO2-based solids with oxides from alkali (Li2O), alkaline earth (CaO), and transition metal groups (WO3 or MnO). The presence of the peroxide (O2-2) active sites on the Li2O2, revealed by Raman spectroscopy, may be the key factor in the enhanced performance of some of the Li2O/MgO catalysts. The high reducibility of the CeO2 catalyst, an important factor in the CO2-OCM catalyst activity, may be enhanced by the presence of manganese oxide species. The manganese oxide species increases oxygen mobility and oxygen vacancies in the CeO2 catalyst. Raman and Fourier Transform Infra Red (FT-IR) spectroscopies revealed the presence of lattice vibrations of metal-oxygen bondings and active sites in which the peaks corresponding to the bulk crystalline structures of Li2O, CaO, WO3 and MnO are detected. The performance of 5%MnO/15%CaO/CeO2 catalyst is the most potential among the CeO2-based catalysts, although lower than the 2%Li2O/MgO catalyst. The 2%Li2O/MgO catalyst showed the most promising C2+ hydrocarbons selectivity and yield at 98.0% and 5.7%, respectively.

关键词： catalyst screening carbon dioxide oxidative coupling methane ternary metal oxide binary metal oxide MgO CeO2 C2+ hydrocarbons

Co-Generation of C_2 Hydrocarbons and Synthesis Gases from Methane and Carbon Dioxide: a Thermodynamic Analysis

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Journal of Natural Gas Chemistry 2005年第3期14卷 140-150页

作者： Istadi nor aishah saidina amin Chemical Reaction Engineering Group (CREG) Faculty of Chemical and Natural Resources Engineering Universiti Teknologi Malaysia UTM Skudai Johor 81310 Malaysia Chemical Reaction Engineering Group (CREG) Faculty of Chemical and Natural Resources Engineering Universiti Teknologi Malaysia UTM Skudai Johor 81310 Malaysia

This paper deals with thermodynamic chemical equilibrium analysis using the method of direct minimization of Gibbs free energy for all possible CH4 and CO2 reactions. The effects of CO2/CH4 feed ratio, reaction temperature, and system pressure on equilibrium composition, conversion, selectivity and yield were studied. In addition, carbon and no carbon formation regions were also considered at various reaction temperatures and CO2/CH4 feed ratios in the reaction system at equilibrium. It was found that the reaction temperature above 1100 K and CO2/CH4 ratio=1 were favourable for synthesis gas production with H2/CO ratio unity, while carbon dioxide oxidative coupling of methane （CO2 OCM） reaction to produce ethane and ethylene is less favourable thermodynamically. Numerical results indicated that the no carbon formation region was at temperatures above 1000 K and CO2/CH4 ratio larger than 1.

关键词： thermodynamic chemical equilibrium co-generation synthesis gas C2 hydrocarbons Gibbs free energy CH4 C02 carbon

Improved Performance of W/HZSM-5 Catalysts for Dehydroaromatization of Methane

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Journal of Natural Gas Chemistry 2004年第3期13卷 148-159页

作者： nor aishah saidina amin Kusmiyati Department of Chemical Engineering Faculty of Chemical and Natural Resources EngineeringUniversiti Teknologi Malaysia 81310 UTM Skudai Johor Malaysia.Department of Chemical Engineering Faculty of Chemical and Natural Resources EngineeringUniversiti Teknologi Malaysia 81310 UTM Skudai Johor Malaysia.

The dehydroaramatization of methane over W-supported ZSM-5 with varying degrees of Li+ ion-exchanged catalysts was studied with and without oxygen at 1073 K and atmospheric pressure. Catalyst activity and stability were found to be influenced by the catalyst acidity related to Bronsted acid sites and by the presence of oxygen in the feed. The NH3-TPD and FTIR-pyridine results demonstrated that partially exchanged of H+ ions by Li+ into the W/HZSM-5 catalysts could be used to control the amount of strong acid sites on the catalyst surface. Without oxygen, the 3WHLi-Z (5:1) catalyst that has strong acid sites equal to nearly 74% of the original strong acid sites in the parent HZSM-5 exhibited the highest methane conversion and selectivity towards aromatics. However, the catalyst deactivated in a five hour period. In the presence of oxygen, the catalyst activity and stability could be improved further. The results of this study revealed that a suitable amount of strong Bronsted acid sites as well as oxygen addition in the feed increased the catalyst activity and stability. The 3WHLi-Z(5:1) catalyst exhibited improved performance in the dehydroaromatization of methane.

关键词： dehydroaromatization methane W-supported ZSM-5 partial ion exchange H+ ion Li ion catalyst activity catalyst stability catalyst acidity oxygen presence improved performance

Characterization and Activity of Cr, Cu and Ga Modified ZSM-5 for Direct Conversion of Methane to Liquid Hydrocarbons

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Journal of Natural Gas Chemistry 2003年第2期12卷 123-134页

作者： nor aishah saidina amin Didi Dwi Anggoro Faculty of Chemical and Natural Resources Engineering Universiti Teknologi Malaysia 81130 Skudai Johor MalaysiaFaculty of Chemical and Natural Resources Engineering Universiti Teknologi Malaysia 81130 Skudai Johor Malaysia 2 Department of Chemical Engineering University of Diponegoro 23589 Semarang Indonesia

Direct conversion of methane using a metal-loaded ZSM-5 zeolite prepared viaacidic ion exchange was investigated to elucidate the roles of metal and acidity in the formation ofliquid hydrocarbons. ZSM-5 (SiO_2/Al_2O_3=30) was loaded with different metals (Cr, Cu and Ga)according to the acidic ion-exchange method to produce metal-loaded ZSM-5 zeolite catalysts. XRD,NMR, FT-IR and N_2 adsorption analyses indicated that Cr and Ga species managed to occupy thealuminum positions in the ZSM-5 framework. In addition, Cr species were deposited in the pores ofthe structure. However, Cu oxides were deposited on the surface and in the mesopores of the ZSM-5zeolite. An acidity study using TPD-NH_3, FT-IR, and IR-pyridine analyses revealed that the totalnumber of acid sites and the strengths of the Broensted and Lewis acid sites were significantlydifferent after the acidic ion exchange treatment. Cu loaded HZSM-5 is a potential catalyst fordirect conversion of methane to liquid hydrocarbons. The successful production of gasoline via thedirect conversion of methane depends on the amount of aluminum in the zeolite framework and thestrength of the Broensted acid sites.

关键词： characterization activity modified ZSM-5 methane direct conversion liquid hydrocarbons

Ethylene Conversion to Higher Hydrocarbon over Copper Loaded BZSM-5 in the Presence of Oxygen

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Journal of Natural Gas Chemistry 2006年第4期15卷 259-265页

作者： Ramli Mat nor aishah saidina amin Zainab Ramli W.Azelee W.Abu Bakar Dept.of Chemical Engineering Faculty of Chemical & Natural Resources EngineeringUniversiti Teknologi MalaysiaSkudai81310 Johor BahruMalaysia Dept.of Chemistry Universiti Teknologi MalaysiaSkudai81310 Johor BahruMalaysia

The successful production of higher hydrocarbons from methane depends on the stability or the oxidation rate of the intermediate products. The performances of the BZSM-5 and the modified BZSM-5 catalysts were tested for ethylene conversion into higher hydrocarbons. The catalytic experiments were carried out in a fixed-bed micro reactor at atmospheric pressure. The catalysts were characterized using XRD, NH3-TPD, and IR for their structure and acidity. The result suggests that BZSM-5 is a weak acid. The introduction of copper into BZSM-5 improved the acidity of BZSM-5. The conversion of ethylene toward higher hydrocarbons is dependent on the acidity of the catalyst. Only weaker acid site is required to convert ethylene to higher hydrocarbons. The loading of Cu on BZSM-5 improved the selectivity for higher hydrocarbons especially at low percentage. The reactivity of ethylene is dependent on the amount of acidity as well as the presence of metal on the catalyst surface. Cul%BZSM-5 is capable of converting ethylene to higher hydrocarbons. The balances between the metal and acid sites influence the performance of ethylene conversion and higher hydrocarbon selectivity. Higher loading of Cu leads to the formation of COx.

关键词： ethylene conversion BZSM-5 zeolite acidity higher hydrocarbon

Reforming of Greenhouse Gas into Syngas over Ni-Ce/Al2O3 in a Dielectric Barrier Plasma Reactor

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Reforming of Greenhouse Gas into Syngas over Ni-Ce/Al2O3 in ...

Preface for the Special Column of the INRET 2006

2012年等离子体催化与能源材料应用国际研讨会

作者： Maryam khoshtinat Nikoo nor aishah saidina amin Department of Catalyst and Process R&D of Bandar Imam Petrochemical Complex (BIPC)Mahshahr Iran Chemical Reaction Engineering Group(CREG) Faculty of Chemical and Natural Resources Engineering Universiti Teknologi MalaysiaUTM 81310 Skudai JohorMalaysia

＜正＞The activation of CO2 and CH4 was conducted at atmospheric pressure and lowtemperature in a DBD plasma reactor for syngas production. The influences of CO2/CH4 ratios, reactant flow rate, gap spacing, and input power, frequency onreactant conversions and products distribution as well as energy efficiency werestudied. According to the results, H2/CO ratio, the selectivity of H2 and CO

关键词： Methane conversion carbon dioxide DBD non-thermal plasma catalytic-plasma.

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Journal of Natural Gas Chemistry 2006年第4期15卷 I0003-I0003页

作者： nor aishah saidina amin Professor Dr.Research Management Centre/Faculty of Chemical and Natural Resources Engineering Universiti Teknologi Malaysia 81310 UTM Skudai JohorMalaysia

I would like to take this opportunity to thank the editorial board of Journal of Natural Gas Chemistry for allowing me to write a preface for this special column. The articles appearing in this section are specially selected from the First International Conference on Natural Resources Engineering and Technology 2006 （INRET 2006）. In line with the theme of JNGC, the selected articles are focused on natural gas or low hydrocarbon conversions to important chemicals, fuels and materials. The conference was held on July 24-25, 2006 in Marriott Putrajaya, Malaysia. It was organized by the Chemical and Biotechnology （ChemBio） Focus Group, under the Research Management Centre, Universiti Teknologi Malaysia.

关键词： Preface for the Special Column of the INRET 2006

Dealuminated ZSM-5 Zeolite Catalyst for Ethylene Oligomerization to Liquid Fuels

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Journal of Energy Chemistry 2002年第Z1期 79-86页

作者： nor aishah saidina amin,Didi Dwi Anggoro1. Faculty of Chemical and Natural Resources Engineering, Universiti Teknologi Malaysia, 81310 Skudai, Johor, Malaysia2. Department of Chemical Engineering, University of Diponegoro, Semarang 50232, Indonesia[Manusc

Ethylene oligomerization using ZSM-5 zeolite was investigated to study the role of Bronsted acid sites in the formation of higher hydrocarbons. The oligomerization of olefins, dependent on the acidity of ZSM-5 zeolite, is an important step in the conversion of natural gas to liquid fuels. The framework Si/Al ratio reflects the number of potential acid sites and the acid strength of the ZSM-5 catalyst. ZSM-5 with the mole ratio SiO2/Al2O3 equal to 30 was dealuminated for different periods of time according to the acidic ion-exchange method to produce ZSM-5 with various Si/Al ratios. The FT-IR analysis revealed that the integrated framework aluminum band, non-framework aluminum band, and silanol groups areas of the ZSM-5 zeolites decreased after being dealuminated. The performance of the dealuminated zeolite was tested for ethylene oligomerization. The results demonstrated that the dealumination of ZSM-5 led to higher ethylene conversion, but the gasoline selectivity was reduced compared to the performance

关键词： ethylene liquid fuels oligomerization dealumination ZSM-5