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"Objectives of this research are mainly to study impacts of acidity strength (by varying amount of precipitant and loading Al-Si) and the effect of nickel particle size (by varying calcinations temperature) on decomposition reaction performances. In this research, high-nickel-loaded catalyst is prepared with two methods. Ni-Cu/Al catalysts were prepared with co-precipitation method. While the Ni-Cu/Al-Si catalyst were prepared by combined co-precipitation and sol-gel method. The direct cracking of methane was performed in 8mm quartz fixed bed reactor at atmospheric pressure and 500-700°C. The main results showed that the Al content of catalyst increases with the increasing amount of precipitant. The activity of catalyst increases with the increasing of catalyst?s acidity to the best possible point, and then increasing of acidity will reduce the activity of catalyst. Ni-Cu/4Al and Ni-Cu/11Al deactivated in a very short time hence produced fewer amount of nanocarbon, while Ni-Cu/15Al was active in a very long period. The most effective catalyst is Ni-Cu/22Al, which produced the biggest amount of nanocarbon (4.15 g C/g catalyst). Ni catalyst diameter has significant effect on reaction performances mainly methane conversion and product yield. A small Ni crystal size gave a high methane conversion, a fast deactivation and a low carbon yield. Large Ni particle diameter yielded a slow decomposition and low methane conversion. The highest methane conversion was produced by catalyst diameter of 4 nm and maximum yield of carbon of 4.08 g C/ g catalyst was achieved by 15.5 nm diameter of Ni catalyst."

"Objectives of this research are mainly to study impacts of acidity strength (by varying amount of precipitant and loading Al-Si) and the effect of nickel particle size (by varying calcinations temperature) on decomposition reaction performances. In this research, high-nickel-loaded catalyst is prepared with two methods. Ni-Cu/Al catalysts were prepared with co-precipitation method. While the Ni-Cu/Al-Si catalyst were prepared by combined co-precipitation and sol-gel method. The direct cracking of methane was performed in 8mm quartz fixed bed reactor at atmospheric pressure and 500-700°C. The main results showed that the Al content of catalyst increases with the increasing amount of precipitant. The activity of catalyst increases with the increasing of catalyst?s acidity to the best possible point, and then increasing of acidity will reduce the activity of catalyst. Ni-Cu/4Al and Ni-Cu/11Al deactivated in a very short time hence produced fewer amount of nanocarbon, while Ni-Cu/15Al was active in a very long period. The most effective catalyst is Ni-Cu/22Al, which produced the biggest amount of nanocarbon (4.15 g C/g catalyst). Ni catalyst diameter has significant effect on reaction performances mainly methane conversion and product yield. A small Ni crystal size gave a high methane conversion, a fast deactivation and a low carbon yield. Large Ni particle diameter yielded a slow decomposition and low methane conversion. The highest methane conversion was produced by catalyst diameter of 4 nm and maximum yield of carbon of 4.08 g C/ g catalyst was achieved by 15.5 nm diameter of Ni catalyst."

"Dekomposisi katalitik metana adalah salah satu alternatif untuk memproduksi hidrogen dan nanokarbon bermutu tinggi secara simultan. Nanokarbon banyak diaplikasikan dalam penyimpanan hidrogen, support katalis, alat penyimpan memory, penyimpanan emisi, dan industri polimer, sedangkan hidrogen dapat digunakan sebagai umpan pada sel bahan bakar (fuel cell) yang ramah lingkungan karena apabila dibakar tidak menghasilkan polutan. Masalah yang biasanya timbul dalam reaksi dekomposisi katalitik metana ini adalah terjadinya deaktivasi katalis akibat deposit karbon dan terjadinya pressure drop di dalam reaktor. Penelitian ini bertujuan menguji kinerja reaktor dengan katalis terstruktur untuk mengatasi pressure drop di dalam reaktor. Katalis Ni-Cu-Al dipreparasi dengan menggunakan metode sol-gel dengan perbandingan atomik 2:1:1. Katalis ini dilapisi pada kawat stainless steel yang telah dibentuk dengan metode dip coating. Reaksi dilakukan dengan mengalirkan metana ke dalam reaktor pada temperatur 650°C dan 700°C serta tekanan atmosferik. Produk gas dianalisis dengan menggunakan gas chromatography yang terpasang secara online dengan aliran keluar reaktor. Penggunaan katalis terstruktur pada dua temperatur berbeda ini dapat menghasilkan konversi metana hingga 87.55 % dan 94.87%. Produk dari reaksi dekomposisi katalitik metana berupa hidrogen memiliki kemurnian hingga 87.53% dan 95.14%. Karbon yang dihasilkan memiliki yield 28.45 dan 32.85 gr karbon/gr katalis untuk waktu reaksi 8.4 jam. Untuk reaksi selama 33 jam menghasilkan 201 gr karbon/gr katalis. Karakterisasi dengan menggunakan TEM menunjukkan karbon yang dihasilkan berbentuk nanotube dengan diameter 50-100. Pada reaktor dengan katalis terstruktur ini tidak terjadi pressure drop yang dapat mengakibatkan berakhirnya reaksi. Reaksi berakhir karena katalis sudah terdeaktivasi akibat tertutupnya permukaan katalis oleh deposit karbon. Lifetime katalis dapat mencapai 33 jam dan masih dapat berlanjut.

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Methane decomposition is an alternative way to produce high quality carbon nanotubes (CNTs) and hydrogen simultaneously. CNTs can been used for various applications such as hydrogen storage, electronic device, composite materials, field emission source, and catalyst support. Hydrogen can be used as the future clean energy resource such as for fuel cells, which doesn't emit pollutants when combusted. The problem often found in methane catalytic decomposition is the presence of pressure drop. This problem is expected to be solved by designing a structured catalyst reactor.

In this experiment, Ni-Cu-Al catalyst is prepared by sol-gel method. Stainless steel wiremesh is coated with catalyst by dip coating method and put into a quartz tube reactor. The experiment was done at 650°C and 700°C with atmospheric pressure. Methane is fed into the reactor and decomposed by the catalyst. An online chromatograph is used to detect the gas products. The morphology of CNTs is characterized by TEM. The use of structured catalyst in these two different temperature gives conversion of methane up to 87.55 % and 94.87%. Hydrogen as the product has a purity of 87.53% dan 95.14% .

The carbon yields are 28.45 and 32.85 gr carbon / gr catalyst for 8.4 hours of reaction. For 33 hours of reaction, the yield becomes 201 gr carbon/ gr catalyst. TEM characterization shows that the diameter of CNTs are between 50-100 nm for both cases. Pressure drop isn't found in this structured catalyst reactor which could end the reaction. The reaction ends when the catalyst is deactivated due to carbon deposit on the catalyst. The lifetime of the catalyst can reach 33 hours and can still continue."

"Produksi karbon nanotube yang memiliki nilai komersil sekaligus hidrogen sebagai bahan bakar ramah lingkungan dapat dilakukan melalui reaksi dekomposisi katalitik metana. Untuk memproduksinya pada skala komersil dibutuhkan studi kinetika untuk memperoleh parameter kinetika reaksi yang berguna untuk keperluan perancangan reaktor. Pada penelitian ini, dilakukan preparasi katalis Ni/Cu/Al yang dilapiskan pada substrat katalis gauze. Percobaan pendahuluan dilakukan untuk memperoleh daerah kinetika yang tidak dipengaruhi oleh fenomena perpindahan massa dan panas, dengan memvariasikan laju alir pada rentang 15-23 ml/menit pada suhu 650oC. Uji kinetika reaksi pada tekanan 1 atm dan variasi suhu 650-750oC dilakukan untuk memperoleh data kinetika. Data kinetika lalu diuji dengan model kinetika mikro yang diturunkan dari mekanisme reaksi permukaan katalis. Model kinetika yang paling sesuai menunjukkan tahap penentu laju reaksi dekomposisi metana. Hasil penelitian uji kinetika menunjukkan bahwa tahap penentu laju reaksi dekomposisi metana adalah tahap reaksi permukaan dimana terjadi pelepasan 1 molekul H dari molekul metana yang teradsorpsi pada inti aktif katalis. Energi aktivasi yang diperoleh sebesar 19,3 kJ/mol. Deaktivasi katalis terjadi pada reaksi sehingga diperlukan suatu faktor koreksi terhadap persamaan laju reaksi.

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Production of carbon nanotubes which has high commercial values together with hydrogen as green energy can be done by catalytic decomposition of methane. Producing hydrogen and carbon nanotubes into commercial scale needs a kinetic study in order to get the kinetic reaction parameters which is useful for design of reactor. In this research, preparation of gauze wire as substrat of Ni/Cu/Al catalyst was done by coating the Ni/Cu/Al catalysts to the wire.

Initial experiment has been done to obtain the kinetics area which is not controlled by mass and heat transfer, by making variation of the flowrate in the range of 15-23 ml/minutes at the temperatur of 650oC. Kinetics evaluation was done at the pressure of 1 atm and the temperatur range of 650-750oC to obtain kinetics data. This data next will be evaluated by the model of micro kinetics that has been formulated by reaction mechanism of the surface of catalysts. The best kinetic model that fits with the data means that the reaction is the rate limiting step of methane decomposition.

The result of kinetic study shows that the rate limiting step is the surface reaction when a molecule of hydrogen released from the methane which is adsorbed in active site of catalysts. The activation energy obtained is 19,3 kJ/mol. Catalysts deactivation occurs in this reaction, so that it is necessary to make a correction of the rate laws."

"Peningkatan kualitas nanotube karbon dapat dilakukan dengan menggunakan katalis berpenyangga. MgO secara luas telah digunakan sebagai penyangga katalis Fe untuk menghasilkan nanotube karbon berkualitas baik. Disisi lain, penelitian Ni berpenyangga MgO belum banyak digunakan padahal Ni merupakan logam yang paling aktif dalam reaksi dekomposisi metana. Untuk itu penelitian dilakukan untuk mengkaji perbandingan kedua katalis tersebut dalam sintesis nanotube karbon. Reaktor yang digunakan untuk reaksi dekomposisi katalitik metana adalah reaktor terstruktur Gauze, sedangkan metode yang digunakan dalam preparasi katalis adalah sol gel dan teknik pelapisan dip coating. Kinerja katalis ditentukan dari konversi metana, kemurnian hidrogen, yield dan karakterisasi nanotube karbon menggunakan SEM. Dari hasil penelitian, diperoleh perbandingan nanotube karbon yang dihasilkan yaitu katalis terstruktur Ni/MgO memberikan konversi metana rata-rata 23.5%, kemunian hidrogen rata-rata 23.9%, yield 9.76 g karbon/g katalis dan karakterisasi nanotube karbon dengan morfologi yang baik. Katalis ini juga mampu bertahan untuk reaksi selama 4.17 jam dengan konversi minimal 16.04%. Katalis terstruktur Fe/MgO memberikan konversi metana rata-rata 10.7%, kemunian hidrogen rata-rata 15.5%, yield 3.45 g karbon/g katalis dan karakterisasi nanotube karbon dengan morfologi yang kurang baik akibat terjadinya aglomerasi partikel Fe. Katalis ini hanya mampu bertahan untuk reaksi selama 2.83 jam dengan konversi minimal sebesar 7.27%.

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Improvement of Carbon Nanotube (CNT) quality can be obtained by using supported catalyst. MgO has been generally used as support for Fe catalyst to produce CNT with good quality. On the other hand, there is only few research regarding the usage of MgO supported Ni catalyst despite its nature as the most reactive catalyst for catalytic methane decomposition. For that reason, this research has done to compare the two catalysts. Reactor structured Gauze is used for catalytic methane decomposition, sol gel method is used for catalyst preparation and dip coating is used for catalyst coating on substrat. Performance of the two catalysts are determined from methane conversion, hydrogen purity, yield and CNT characterization by SEM. Structured catalyst Ni/MgO gives the average conversion of 23.5%, average hydrogen purity of 23.9%, yield of 9.76 g C/g catalyst and good morfology of CNT. This catalyst can endured for 4.17 hours with the minimum conversion of 16.04%. In comparison, structured Fe/MgO catalyst gives the average conversion of 10.7%, average hydrogen purity of 15.5% and yield of 3.45 g carbon/g catalyst. Moreover, the resulting CNT morfology is not very good due to agglomeration of Fe particles. This catalyst can only endured for 2.83 hours with the minimum conversion of 7.27%."

"ABSTRAKProduksi nanotube karbon jenis Single Walled Nanotube Carbon (SWNT) danFew Walled Nanotube Carbon (FWNT) masih sulit untuk dilakukan. Salah satupenyebab utama adalah pemilihan katalis yang kurang tepat. Penelitian inimenggunakan katalis Fe/Mo/MgO untuk menghasilkan SWNT atau FWNT(diameter luar nanotube karbon kurang dari 10 nm). Katalis Fe/Mo/MgOdipreparasi dengan metode sol gel/spray coating. Nanokarbon akan dihasilkanmelalui reaksi dekomposisi katalitik metana pada suhu 850oC dengan katalisFe/Mo/MgO. Hasil penelitian menunjukkan konversi metana tertinggi mencapai97,64% dan yield karbon sebesar 1,48 gc/gkat. Nanokarbon kemudiandikarakterisasi dengan Transmission Electron Microscope (TEM). Nanokarbonyang dihasilkan pada penelitian ini terdiri atas nanotube karbon jenis FWNT(range diameter luar 4,5 nm ? 10 nm). Selain itu, MWNT (Multi Walled NanotubeCarbon, range diameter luar 10 nm ? 89,5 nm), carbon nanofiber, coil nanotube,dan bamboo-shaped carbon juga telah dihasilkan. Jenis nanokarbon yangdihasilkan bukan hanya jenis nanotube karbon disebabkan oleh waktu reaksi yangterlalu panjang serta diameter partikel katalis 20 nm hingga 100 nm yangterdeteksi dari hasil X-Ray Diffraction (XRD) dan Field Emmision ScanningElectron Microscope (FE SEM). Untuk memperbaiki hasil ini, running padapenelitian ini dilakukan sekali lagi dengan waktu reaksi 30 menit dengan waktureduksi 30 menit di suhu 850oC dan suhu kalsinasi 550oC di udara. Hasilnanokarbon yang diperoleh memiliki range diameter luar yang lebih kecil danberkisar antara 8,5 nm hingga 66,85 nm yang terukur pada FE SEM. Namun, jenisnanokarbon belum diketahui berupa FWNT atau MWNT atau nanokarbonlainnya.

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AbstractProduction of Single Walled Nanotubes Carbon (SWNT) dan Few WalledNanotubes Carbon (FWNT) is really hard to do recently. It occured due toinappropriate catalyst selection. Fe/Mo/MgO catalyst, used in literature, was usedto make nanotubes carbon. Fe/Mo/MgO catalyst was prepared by sol gel/spraycoating method and it would be reacted with methane in 850oC (methanedecomposition catalytic reaction). The research result shows that the highestmethane conversion reached 97,64% and carbon yield is 1,48 gc/gkat.Transmission Electron Microscope (TEM) indicated that the synthesized productwas FWNT (carbon nanotubes with outer diameter between 4,5 nm ? 10 nm),MWNT (Multi Walled Nanotubes Carbon, outer diameter between 10 nm ? 89,5nm), coil nanotube, carbon nanofiber, dan bamboo-shaped carbon. It is happeneddue to longer time reaction and catalyst diameters have range between 20 nm ?100 nm which detected by XRD and SEM characterization. Then, methanedecomposition catalytic reaction to get nanotube carbon was done once again inshorter times (30 minutes), longer time of reduction (40 minutes), and lowercalcination temperature (550oC) in air. FE SEM indicated that range of outerdiameter nanocarbon between 8,5 nm ? 66,85 nm but its types can not bedetermined by FE SEM."