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  • 1
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    Regenerative adsorption and removal of H2S from hot fuel gas streams by rare earth oxides (2006)
    American Association for the Advancement of Science (AAAS)
    Details
    Publication Date: 2006-06-10
    Description: Sorbent materials that allow for high-temperature, regenerative desulfurization of fuel gas streams for the anode of a solid oxide fuel cell have been developed. Reversible adsorption of H2S on cerium and lanthanum oxide surfaces is demonstrated over many cycles at temperatures as high as 800 degrees C, on both fresh or presulfided sorbents, and at very high space velocities. The adsorption and desorption processes are very fast, and removal of H2S to sub-parts per million levels is achieved at very short (millisecond) contact times. Any type of sulfur-free gas, including water vapor, can be used to regenerate the sorbent surface. Preferably, the anode off-gas stream is used to sweep the desorbed H(2)S to a burner.〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Flytzani-Stephanopoulos, Maria -- Sakbodin, Mann -- Wang, Zheng -- New York, N.Y. -- Science. 2006 Jun 9;312(5779):1508-10.〈br /〉〈span class="detail_caption"〉Author address: 〈/span〉Department of Chemical and Biological Engineering, Tufts University, Medford, MA 02155, USA. maria.flytzani-stephanopoulos@tufts.edu〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/16763145" target="_blank"〉PubMed〈/a〉
    Print ISSN: 0036-8075
    Electronic ISSN: 1095-9203
    Topics: Biology , Chemistry and Pharmacology , Computer Science , Medicine , Natural Sciences in General , Physics
    Published by American Association for the Advancement of Science (AAAS)
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  • 2
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    Catalytically active Au-O(OH)x-species stabilized by alkali ions on zeolites and mesoporous oxides (2014)
    American Association for the Advancement of Science (AAAS)
    Details
    Publication Date: 2014-11-29
    Description: We report that the addition of alkali ions (sodium or potassium) to gold on KLTL-zeolite and mesoporous MCM-41 silica stabilizes mononuclear gold in Au-O(OH)x-(Na or K) ensembles. This single-site gold species is active for the low-temperature (〈200 degrees C) water-gas shift (WGS) reaction. Unexpectedly, gold is thus similar to platinum in creating -O linkages with more than eight alkali ions and establishing an active site on various supports. The intrinsic activity of the single-site gold species is the same on irreducible supports as on reducible ceria, iron oxide, and titania supports, apparently all sharing a common, similarly structured gold active site. This finding paves the way for using earth-abundant supports to disperse and stabilize precious metal atoms with alkali additives for the WGS and potentially other fuel-processing reactions.〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Yang, Ming -- Li, Sha -- Wang, Yuan -- Herron, Jeffrey A -- Xu, Ye -- Allard, Lawrence F -- Lee, Sungsik -- Huang, Jun -- Mavrikakis, Manos -- Flytzani-Stephanopoulos, Maria -- New York, N.Y. -- Science. 2014 Dec 19;346(6216):1498-501. doi: 10.1126/science.1260526. Epub 2014 Nov 27.〈br /〉〈span class="detail_caption"〉Author address: 〈/span〉Department of Chemical and Biological Engineering, Tufts University, MA 02155, USA. ; Department of Chemical and Biological Engineering, University of Wisconsin-Madison, WI 53706, USA. ; Department of Chemical Engineering, Louisiana State University, Baton Rouge, LA 70803, USA. ; Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA. ; X-ray Science Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439, USA. ; School of Chemical and Biomolecular Engineering, University of Sydney, NSW 2006, Australia. ; Department of Chemical and Biological Engineering, Tufts University, MA 02155, USA. maria.flytzani-stephanopoulos@tufts.edu.〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/25431492" target="_blank"〉PubMed〈/a〉
    Print ISSN: 0036-8075
    Electronic ISSN: 1095-9203
    Topics: Biology , Chemistry and Pharmacology , Computer Science , Medicine , Natural Sciences in General , Physics
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  • 3
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    Active nonmetallic Au and Pt species on ceria-based water-gas shift catalysts (2003)
    American Association for the Advancement of Science (AAAS)
    Details
    Publication Date: 2003-07-05
    Description: Traditional analysis of reactions catalyzed by supported metals involves the structure of the metallic particles. However, we report here that for the class of nanostructured gold- or platinum-cerium oxide catalysts, which are active for the water-gas shift reaction, metal nanoparticles do not participate in the reaction. Nonmetallic gold or platinum species strongly associated with surface cerium-oxygen groups are responsible for the activity.〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Fu, Qi -- Saltsburg, Howard -- Flytzani-Stephanopoulos, Maria -- New York, N.Y. -- Science. 2003 Aug 15;301(5635):935-8. Epub 2003 Jul 3.〈br /〉〈span class="detail_caption"〉Author address: 〈/span〉Department of Chemical and Biological Engineering, Tufts University, Medford, MA 02155, USA.〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/12843399" target="_blank"〉PubMed〈/a〉
    Print ISSN: 0036-8075
    Electronic ISSN: 1095-9203
    Topics: Biology , Chemistry and Pharmacology , Computer Science , Medicine , Natural Sciences in General , Physics
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  • 4
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    Alkali-stabilized Pt-OHx species catalyze low-temperature water-gas shift reactions (2010)
    American Association for the Advancement of Science (AAAS)
    Details
    Publication Date: 2010-10-12
    Description: We report that alkali ions (sodium or potassium) added in small amounts activate platinum adsorbed on alumina or silica for the low-temperature water-gas shift (WGS) reaction (H(2)O + CO --〉 H(2) + CO(2)) used for producing H(2). The alkali ion-associated surface OH groups are activated by CO at low temperatures (~100 degrees C) in the presence of atomically dispersed platinum. Both experimental evidence and density functional theory calculations suggest that a partially oxidized Pt-alkali-O(x)(OH)(y) species is the active site for the low-temperature Pt-catalyzed WGS reaction. These findings are useful for the design of highly active and stable WGS catalysts that contain only trace amounts of a precious metal without the need for a reducible oxide support such as ceria.〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Zhai, Yanping -- Pierre, Danny -- Si, Rui -- Deng, Weiling -- Ferrin, Peter -- Nilekar, Anand U -- Peng, Guowen -- Herron, Jeffrey A -- Bell, David C -- Saltsburg, Howard -- Mavrikakis, Manos -- Flytzani-Stephanopoulos, Maria -- New York, N.Y. -- Science. 2010 Sep 24;329(5999):1633-6. doi: 10.1126/science.1192449.〈br /〉〈span class="detail_caption"〉Author address: 〈/span〉Department of Chemical and Biological Engineering, Tufts University, Medford, MA 02155, USA.〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/20929844" target="_blank"〉PubMed〈/a〉
    Print ISSN: 0036-8075
    Electronic ISSN: 1095-9203
    Topics: Biology , Chemistry and Pharmacology , Computer Science , Medicine , Natural Sciences in General , Physics
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  • 5
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    Isolated metal atom geometries as a strategy for selective heterogeneous hydrogenations (2012)
    American Association for the Advancement of Science (AAAS)
    Details
    Publication Date: 2012-03-10
    Description: Facile dissociation of reactants and weak binding of intermediates are key requirements for efficient and selective catalysis. However, these two variables are intimately linked in a way that does not generally allow the optimization of both properties simultaneously. By using desorption measurements in combination with high-resolution scanning tunneling microscopy, we show that individual, isolated Pd atoms in a Cu surface substantially lower the energy barrier to both hydrogen uptake on and subsequent desorption from the Cu metal surface. This facile hydrogen dissociation at Pd atom sites and weak binding to Cu allow for very selective hydrogenation of styrene and acetylene as compared with pure Cu or Pd metal alone.〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Kyriakou, Georgios -- Boucher, Matthew B -- Jewell, April D -- Lewis, Emily A -- Lawton, Timothy J -- Baber, Ashleigh E -- Tierney, Heather L -- Flytzani-Stephanopoulos, Maria -- Sykes, E Charles H -- New York, N.Y. -- Science. 2012 Mar 9;335(6073):1209-12. doi: 10.1126/science.1215864.〈br /〉〈span class="detail_caption"〉Author address: 〈/span〉Department of Chemistry, Tufts University, 62 Talbot Avenue, Medford, MA 02155, USA.〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/22403387" target="_blank"〉PubMed〈/a〉
    Print ISSN: 0036-8075
    Electronic ISSN: 1095-9203
    Topics: Biology , Chemistry and Pharmacology , Computer Science , Medicine , Natural Sciences in General , Physics
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  • 6
    Electronic Resource
    Electronic Resource
    Morphology and etching processes on macroscopic metal catalysts
    Amsterdam : Elsevier
    Progress in Surface Science 9 (1979), S. 83-111 
    Details
    ISSN: 0079-6816
    Source: Elsevier Journal Backfiles on ScienceDirect 1907 - 2002
    Topics: Physics
    Type of Medium: Electronic Resource
    URL: http://linkinghub.elsevier.com/retrieve/pii/0079-6816(79)90001-7
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  • 7
    Electronic Resource
    Electronic Resource
    Mixed-oxide sorbents for high-temperature removal of hydrogen sulfide (1986)
    s.l. : American Chemical Society
    Industrial and engineering chemistry 25 (1986), S. 429-437 
    Details
    Source: ACS Legacy Archives
    Topics: Chemistry and Pharmacology , Process Engineering, Biotechnology, Nutrition Technology
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1021/i200033a014
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  • 8
    Electronic Resource
    Electronic Resource
    High-temperature sulfidation-regeneration of copper(II) oxide-alumina sorbents (1989)
    s.l. : American Chemical Society
    Industrial & engineering chemistry research 28 (1989), S. 931-940 
    Details
    ISSN: 1520-5045
    Source: ACS Legacy Archives
    Topics: Chemistry and Pharmacology , Process Engineering, Biotechnology, Nutrition Technology
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1021/ie00091a008
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  • 9
    Electronic Resource
    Electronic Resource
    Vapor etching of GaAs and AlGaAs by CH3I (1992)
    Woodbury, NY : American Institute of Physics (AIP)
    Applied Physics Letters 60 (1992), S. 1459-1461 
    Details
    ISSN: 1077-3118
    Source: AIP Digital Archive
    Topics: Physics
    Notes: With the objective of developing an improved process for in situ etching of GaAs-based materials in organometallic vapor phase epitaxy reactors, GaAs wafers and AlxGa1−xAs epilayers have been etched with CH3I vapor in a horizontal reactor operated at atmospheric pressure with H2 or He carrier gas. For a H2 flow rate of 2.1 s lpm, etching temperatures from 400 to 625 °C, and CH3I mol fractions (yCH3I)from 0.0012 to 0.015, the measured GaAs etch rate r (in A(ring) min−1) is given by r = k0 y0.83CH3I exp[ − 45(kcal mol−1)/RT] with k0=3.2×1016 A(ring) min−1. The value of k0 depends on the type of carrier gas, flow rate, total pressure, and reactor geometry. The etch rate appears to be controlled mainly by the decomposition of CH3I to CH3 and I, for which the activation energy has been reported to be 43.5 kcal mol−1. The etch rate of AlxGa1−xAs epilayers with x up to 0.7, which was measured at 480 °C with yCH3I= 0.015, does not depend on Al content. The surface morphology of etched GaAs wafers improves with decreasing temperature. Specular surfaces are maintained at temperatures below 500 °C for etch depths up to 5000 A(ring).
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.107270
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  • 10
    Electronic Resource
    Electronic Resource
    Alkali-alumina sorbents for high-temperature removal of SO2 (1987)
    Hoboken, NJ : Wiley-Blackwell
    AIChE Journal 33 (1987), S. 258-266 
    Details
    ISSN: 0001-1541
    Keywords: Chemistry ; Chemical Engineering
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology , Process Engineering, Biotechnology, Nutrition Technology
    Notes: The high-temperature removal of SO2 by sorbents consisting of sodium and lithium salts supported on α-Al2O3 has been investigated with emphasis on the chemistry of regeneration. The sulfated sorbents were regenerated by reduction with CO at 700-800°C in a thermogravimetric analyzer and a packed-bed microreactor. Sulfur removal from the sorbent and distribution of gaseous products were measured at different alkali loadings, temperatures, and CO concentrations. The results are interpreted in terms of a network of reactions wherein alumina is important as a catalyst and as a reactant. During regeneration sulfate is converted to aluminate and sulfide, the fraction of aluminate defining the extent of regeneration. The rate and extent of sulfur removal increase with the ratio of alumina to alkali and are higher in the presence of lithium. The product gas consists of SO2, COS, and elemental sulfur, the latter compound constituting up to 35% of the sulfur removed.
    Additional Material: 14 Ill.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1002/aic.690330212
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