能源化学(英文版)

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Development of a CO2 Tolerant Fischer-Tropsch Catalyst: from Laboratory to Commercial-Scale Demonstration in Alaska

Joep J H M Font Freide;Tim D Gamlin;J Richard Hensman;Barry Nay;Christopher Sharp

2004, 13 (1): 1-9.

摘要 ( 9031 )

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This article describes the development of BPs Fischer-Tropsch catalyst, used for the carbon monoxide conversion and hydrogen into liquid hydrocarbons. It covers the 18 year period from the early eighties, when laboratory scale preparations and micro-reactors were heavily used, right through to the present day with the commercial scale manufacture and proving of the finished catalyst in BPs new $86 million gas to liquids demonstration facility in Nikiski, Alaska. Extensive performance testing and scale- up experiments have been successfully carried out, all proof that a laboratory preparation can indeed be translated into a commercial manufacturing process. In addition, the resulting catalyst does not only meet the process design targets, but also exhibits enhanced stability and is tolerant to carbon dioxide. Above all, a commercial scale, _xed bed Fischer-Tropsch catalyst is now available and ready for licensing. Manufacturing procedures and quality control have all been successfully detailed and transferred to the commercial manufacturer.

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Recent Results on Fast Flow Gas-Phase Partial Oxidation of Lower Alkanes

Vladimir S. Arutyunov

2004, 13 (1): 10-22.

摘要 ( 7379 )

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Recent experimental results and kinetic modeling of fast flow gas-phase oxidation of methane and other lower alkanes to methanol and other oxygenates are discussed, alongside with prospects and possible areas for applications of the processes.

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Screening of MgO- and CeO2-Based Catalysts for Carbon Dioxide Oxidative Coupling of Methane to C2+ Hydrocarbons

Istadi;Nor Aishah Saidina Amin

2004, 13 (1): 23-35.

摘要 ( 9990 )

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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 (O22-) 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.

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Studies on Mo/HZSM-5 Complex catalyst for Methane Aromatization

Qun Dong;Xiaofei Zhao;Jian Wang;M Ichikawa

2004, 13 (1): 36-40.

摘要 ( 8875 )

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The influence of adding Fe, Cr, Co, and Ga into 3%Mo/HZSM-5 catalyst on methane aroma- tization, and the influence of additives ratio on methane conversion, selectivity to hydrocarbons and coke, as well as distribution of aromatics were investigated. The experimental results showed that the addition of Fe, Cr, Co and Ga promoted the dehydrogenation and dissociation of methane. The results of NH3-TPD indicated that the acidity of HZSM-5 was changed by adding Fe and Co components, consequently the catalytic properties of Mo/HZSM-5 were changed. It was also revealed that strong acid sites were the center of methane aromatization. The results of XRD characterization showed that the crystallinity of Mo on ZSM-5 zeolite was increased after adding Fe, Co additives.

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Preparation and Characterization of Modified-ZrO2 Catalysts for the Reaction of CO Hydrogenation

Qingjie Ge;A. Kiennemann;A. C. Roger;Wenzhao Li;Hengyong Xu

2004, 13 (1): 41-44.

摘要 ( 9734 )

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ZrO2 in different structures and CexZr4-xO8 solid solutions have been prepared by a sol-gel related method with propionic acid as the solvent. The results of their characterization and CO hydro- genation performance evaluation show that t-ZrO2 has better catalytic performance for CO hydrogenation to hydrocarbon than m-ZrO2. Cerium (III) acetate and zirconium (IV) acetylacetonate have been chosen as the most suitable starting materials for CexZr4-xO8 solid solution preparation. Ce-Zr reducibility prop- erties are increased by the incorporation of zirconium oxide in the ceria structure. Ce2Zr2O8 exhibits a higher activity, lower methane selectivity and higher iso-C4 selectivity than tetragonal ZrO2. This implies that the formation mechanism of C4 hydrocarbons, especially that for the iso-C4 fraction is different over Ce2Zr2O8 and t-ZrO2.

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Effect of Transition Metals on Catalytic Performance of Ru/Sepiolite Catalyst for Methanation of Carbon Dioxide

Laitao Luo;Songjun Li

2004, 13 (1): 45-48.

摘要 ( 8320 )

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The effects of Mo, Mn and Zr transitional metals on the catalytic performance of Ru/sepiolite for CO2 methanation were investigated. The results indicated that addition of the transitional metals affected the activity of the Ru/sepiolite remarkably, and the activities of the catalysts were closely asso- ciated with the electronic state of the ruthenium surface. The addition of Mo increased the active surface area, the Ru dispersity, the number of active sites, and the resistance to poisoning. According to the Transition State Theory, when Mo is added into the Ru/sepiolite catalyst, the decrease in surface energy is at a cost of an increment in steric hindrance. When T≤674 K, the energy factor was dominating, and resulted in a decreasing in the ratio of S(CH4)/S(CO). Otherwise, the steric factor dominated the reaction course.

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Methanol Steam Reforming Reactions on CuZn(Zr)AlO Catalyst

Yongfeng Li;Xinfa Dong;Weiming Lin

2004, 13 (1): 49-52.

摘要 ( 7322 )

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The catalytic performances of methanol steam reforming reactions on CuZn(Zr)AlO catalysts were studied. When the ZrO2 promoter was added to a CuZnAlO catalyst, its methanol conversion, H2 production and H2 selectivity improved greatly. By using the #COPZr-2 catalyst as an example, which exhibited the best catalytic performance, the optimized reaction conditions were established to be: 250oC, 0.1 MPa, H2O/MeOH=1.3, WHSV=3.56 h-1, and without carrier gas. A 150 h stability test of the #COPZr-2 catalyst showed that the catalyst had good stability, as the methanol conversion and H2 production could be kept at 88% and 83% respectively. Moreover, outlet H2 and CO contents were >63% and 0.20%--0.31%, respectively.

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Study on Pressure Swing Adsorption Removing C2+ Gas as Raw Material for Thermal Chlorination

Sulan Xia;Jiahua Zhu;Xiaobin Zeng;Zhaohua Feng;Xinyu Cheng

2004, 13 (1): 53-57.

摘要 ( 7214 )

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The experimental investigation demonstrates that a satisfactory result can be expected for pressure swing adsorption (PSA) purification of natural gas as raw material for thermal chlorination process. Using hh-4 molecular sieve as adsorbent for removing C2+ components, the suitable adsorption pressure is 0.4-0.45 MPa, desorption vacuum is 0.08-0.09 MPa and circulation time is 20-21 min.

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