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Journal ArticleDOI

CATALYTIC CONVERSION OF METHANE TO MORE USEFUL CHEMICALS AND FUELS: A CHALLENGE FOR THE 21st CENTURY

25 Dec 2000-Catalysis Today (Elsevier)-Vol. 63, Iss: 2, pp 165-174
TL;DR: The potential for the production of ethylene or liquid hydrocarbon fuels has not been fully realized as mentioned in this paper, and a number of strategies are being explored at levels that range from fundamental science to engineering technology.
About: This article is published in Catalysis Today.The article was published on 2000-12-25. It has received 1063 citations till now. The article focuses on the topics: Methane reformer & Steam reforming.
Citations
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Journal ArticleDOI
11 Oct 2011
TL;DR: This book discusses the history and present uses of Methanol, the discovery and properties of Hydrogen, and the production and Uses ofhydrogen from Fossil Fuels, as well as the challenges and opportunities facing the industry.

1,633 citations

Journal ArticleDOI
TL;DR: This Review focuses on the analysis of new approaches and results in the field of solution combustion synthesis (SCS) obtained during recent years, emphasizing the chemical mechanisms that are responsible for rapid self-sustained combustion reactions.
Abstract: Solution combustion is an exciting phenomenon, which involves propagation of self-sustained exothermic reactions along an aqueous or sol–gel media. This process allows for the synthesis of a variety of nanoscale materials, including oxides, metals, alloys, and sulfides. This Review focuses on the analysis of new approaches and results in the field of solution combustion synthesis (SCS) obtained during recent years. Thermodynamics and kinetics of reactive solutions used in different chemical routes are considered, and the role of process parameters is discussed, emphasizing the chemical mechanisms that are responsible for rapid self-sustained combustion reactions. The basic principles for controlling the composition, structure, and nanostructure of SCS products, and routes to regulate the size and morphology of the nanoscale materials are also reviewed. Recently developed systems that lead to the formation of novel materials and unique structures (e.g., thin films and two-dimensional crystals) with unusual...

841 citations

Journal ArticleDOI
TL;DR: This Review describes how transfer of oxygen atoms, bond activation, and coupling of fragments can be mediated by atomic or cluster metal ions, and improves the understanding of the intrinsic operation of a practical catalyst at a strictly molecular level.
Abstract: Gas-phase experiments with state-of-the-art techniques of mass spectrometry provide detailed insights into numerous elementary processes. The focus of this Review is on elementary reactions of ions that achieve complete catalytic cycles under thermal conditions. The examples chosen cover aspects of catalysis pertinent to areas as diverse as atmospheric chemistry and surface chemistry. We describe how transfer of oxygen atoms, bond activation, and coupling of fragments can be mediated by atomic or cluster metal ions. In some cases truly unexpected analogies of the idealized gas-phase ion catalysis can be drawn with related chemical transformations in solution or the solid state, and so improve our understanding of the intrinsic operation of a practical catalyst at a strictly molecular level.

747 citations

Journal ArticleDOI
TL;DR: In this paper, the major routes for the production of lower olefins from synthesis gas with an emphasis on a direct or single step process, the so-called Fischer-Tropsch to olefin process, is described.
Abstract: C2 to C4 olefins are traditionally produced from steam cracking of naphtha. The necessity for alternative production routes for these major commodity chemicals via non-oil-based processes has driven research in past times during the oil crises. Currently, there is a renewed interest in producing lower olefins from alternative feedstocks such as coal, natural gas, or biomass, in view of high oil prices, environmental regulations, and strategies to gain independence from oil imports. This review describes the major routes for the production of lower olefins from synthesis gas with an emphasis on a direct or single step process, the so-called FTO or Fischer–Tropsch to olefins process. The different catalysts for FTO are outlined and compared, and the key issues and requirements for future developments are highlighted. Iron-based catalysts are prevailing for FTO, and reproducible lower olefin selectivities of 50 wt % of hydrocarbons produced have been realized at CO conversions higher than 70% for 60 to 1000 ...

738 citations

Journal ArticleDOI
TL;DR: The article discusses oxidation catalysis by substitutional cation doping of binary oxides by assuming that the 'as-prepared' catalyst is a doped oxide that, under reducing reaction conditions, is converted to very small metallic dopant clusters supported on the host oxide.
Abstract: The article discusses oxidation catalysis by substitutional cation doping of binary oxides. Substitutional cation doping is not the only possibility. One can imagine that replacing some anions with other anions may also be beneficial. There is evidence that the presence of small amounts of halogen in the feed or on the oxide surface improves its catalytic activity. It is very likely that doped oxide catalysts have been used before the concept was formulated explicitly. Most oxide catalysts have low levels of impurities that may be substitutional dopants. If they segregate at the surface, they can affect the catalytic activity without our knowledge even though their net concentration is very low. It is also possible that the 'as-prepared' catalyst is a doped oxide that, under reducing reaction conditions, is converted to very small metallic dopant clusters supported on the host oxide. The physical and chemical properties of such clusters are different from those of a bulk metal, and it is difficult to distinguish them from a doped oxide.

668 citations

References
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Journal ArticleDOI
TL;DR: The history and trends of FT synthesis can be divided into several lines which are elaborated individually: • The changing environment of demand and supply of fossil energies and the more stringently upcoming aspects of pollution control, of cleanliness of the automotive fuels and of energy saving.
Abstract: Due to the large volume of existing literature on Fischer–Tropsch (FT) synthesis, the diversity of the subject and the actually reoriented interest, it seemed indicated to write a historical sketch about the process, putting also emphasis on present trends and future options. The matter is complicated and may be regarded from different positions. Thus history and trends have been divided into several lines which are elaborated individually: • The changing environment of demand and supply of fossil energies and the more stringently upcoming aspects of pollution control, of cleanliness of the automotive fuels and of energy saving. • The development of FT-reactors and processes, an area of highest present industrial activity and progress. • Preparation and performance of catalysts with particular concern about cobalt as the base metal. • FT intermediates and elemental reactions, difficult subjects as the FT multistep conversion features on the catalyst surface in the adsorbed state and kinetic principles as selective inhibition and spatial constraints seem to rule the regime. • Kinetic modelling of FT synthesis which has made great progress recently, particularly on the basis of newly provided detailed experimental data. Of course, presenting history and trends of FT synthesis on a few pages means generalising from many individual investigations and developments and also selection of only a few citations. So I want to apologise for all the contributions to science and technology around FT synthesis which I have missed to include into the article.

1,250 citations

Journal ArticleDOI
24 Apr 1998-Science
TL;DR: Mechanistic studies show that platinum(II) is the most active oxidation state of platinum for reaction with methane, and are consistent with reaction proceeding through carbon-hydrogen bond activation of methane to generate a platinum-methyl intermediate that is oxidized to generate the methyl ester product.
Abstract: Platinum catalysts are reported for the direct, low-temperature, oxidative conversion of methane to a methanol derivative at greater than 70 percent one-pass yield based on methane. The catalysts are platinum complexes derived from the bidiazine ligand family that are stable, active, and selective for the oxidation of a carbon-hydrogen bond of methane to produce methyl esters. Mechanistic studies show that platinum(II) is the most active oxidation state of platinum for reaction with methane, and are consistent with reaction proceeding through carbon-hydrogen bond activation of methane to generate a platinum-methyl intermediate that is oxidized to generate the methyl ester product.

1,144 citations

Journal ArticleDOI
TL;DR: In this paper, a modified ZSM-5 zeolite catalysts with a fixed bed continuous-flow reactor and with a temperature programmed reactor were used for the de-hydrogenation and aromatization of methane.
Abstract: The dehydrogenation and aromatization of methane on modified ZSM-5 zeolite catalysts has been studied under non-oxidizing conditions with a fixed bed continuous-flow reactor and with a temperature programmed reactor. The results show that benzene is the only hydrocarbon product of the catalytic conversion of methane at high temperature (973 K). The catalytic activity of ZSM-5 is greatly improved by incorporating a metal cation (Mo or Zn). H2 and ethene have been directly detected in the products with a mass spectrometer during TPAR. A carbenium ion mechanism for the activation of methane is suggested.

738 citations

Journal ArticleDOI
TL;DR: In this article, a fiinfbandige Werk besteht inhaltlich aus zwei Teilen, von denen der erste, in den Banden 1, 2 and 3 the allgemeinen Prinzipien und Methoden sowie die Reaktionstechnik behandelt, der zweite, die Bande 4 and 5, hat die katalytischen Prozesse zum Gegenstand.
Abstract: esse der Qualitat des neuen Handbuches fiir die umfassende Darstellung alléin der heterogénen Katalyse in all ihren Facetten mehr als 200, auf den jeweils von ihnen behandelten Teilgebieten international anerkannte Wissenschaftler, von den Herausgebern herangezogen werden. War das Handbuch der Katalyse noch iiberwiegend in deutscher Sprache abgefaBt, so bedient sich das Handbuch der Heterogénen Katalyse ausschieBlich der englischen Sprache. Dies ist Ausdruck der immer aktiveren Beteiligung von Wissenschaftlern aus nahezu alien Landern der Welt an der Entwicklung der heterogénen Katalyse. DaB sich die Herausgeber der Miihe unterzogen haben, eine notwendigerweise so groBe Anzahl von Fachleuten an dem Handbuch zu beteiligen und dieses nunmehr vorliegt, ist angesichts der noch immer zunehmenden Bedeutung der heterogénen Katalyse sehr verdienstvoll und auBerordentlich zu begriiBen. Das fiinfbandige Werk besteht inhaltlich aus zwei Teilen, von denen der erste, in den Banden 1, 2 und 3 die allgemeinen Prinzipien und Methoden sowie die Reaktionstechnik behandelt. Der zweite Teil, die Bande 4 und 5, hat die katalytischen Prozesse zum Gegenstand. Die Einfiihrung zum Gesamtwerk beginnt mit einer Erlauterung der Grundbegriffe der heterogénen Katalyse gefolgt von kurzen Darstellungen der Entwicklung der Katalyse als Wissenschaftszweig sowie der Entwicklung der industriellen Katalyse. Neben der Einfiihrung enthàlt der 1. Band nur das Kapitel 2, das ausschlieBlich der Herstellung von Katalysatoren gewidmet ist. In einem kurzen Abschnitt werden Anforderungen und Prinzipien abgeleitet, die bei der Entwicklung industrieller Katalysatoren zu beachten sind. Die folgenden Unterkapitel beschreiben die Katalysatorherstellung iiberwiegend im LaboratoriumsmaBstab. Breiten Raum nehmen dabei die wissenschaftlichen Grundlagen der Herstellungsprozesse wie Fallung, Tràgerfixierung, Sol-Gel-Umwandlung

706 citations


"CATALYTIC CONVERSION OF METHANE TO ..." refers background in this paper

  • ...At the time of this writing, crude oil is selling for ca. $25 per barrel, which makes the production of high grade fuels from methane more attractive....

    [...]

Journal ArticleDOI
TL;DR: In this paper, the authors characterized the phase composition of the NiO/Al 2 O 3 phase of a 25 wt% NiO+Al 2O 3 catalyst for complete oxidation of methane feed to CO 2 and H 2 O. The authors showed that the previously calcined catalyst bed consists of three different regions.

703 citations