Carbon Overcoating of Supported Metal Catalysts for Improved Hydrothermal Stability

Commercial mesoporous oxides, such as silica, are not stable in liquid-phase reactions, particularly aqueous-phase reactions at elevated temperatures, which are corrosive to oxide supports. We have shown previously that the hydrothermal stability of silica is significantly improved by coating the surface with thin carbon layers. Herein, we show that controlled pyrolysis of sugars also provides a facile approach for coating supported metal catalysts, leading to improved dispersion of the active metal phase in the hydrothermally aged catalyst. The carbon overcoats are synthesized at mild temperatures, resulting in an open structure, as revealed by 13C NMR, which helps explain why the overcoats do not significantly block the active sites. We compare two approaches–depositing Pd on carbon-coated silica and depositing carbon overcoats on Pd/silica. The carbon overcoating approach leads to better performance after hydrothermal aging, as determined by using a probe reaction (CO oxidation) to quantify the number ...

[1]  Thomas J. Schwartz,et al.  Engineering catalyst microenvironments for metal-catalyzed hydrogenation of biologically derived platform chemicals. , 2014, Angewandte Chemie.

[2]  Abhaya K. Datye,et al.  Hydrothermally stable heterogeneous catalysts for conversion of biorenewables , 2014 .

[3]  P. Voyles,et al.  Pore Structure and Bifunctional Catalyst Activity of Overlayers Applied by Atomic Layer Deposition on Copper Nanoparticles , 2014 .

[4]  David H. K. Jackson,et al.  Stabilization of copper catalysts for liquid-phase reactions by atomic layer deposition. , 2013, Angewandte Chemie.

[5]  B. Shanks,et al.  Spectrally edited 2D 13C-13C NMR spectra without diagonal ridge for characterizing 13C-enriched low-temperature carbon materials. , 2013, Journal of magnetic resonance.

[6]  A. Datye,et al.  A facile approach for the synthesis of niobia/carbon composites having improved hydrothermal stability for aqueous-phase reactions , 2013 .

[7]  A. Datye,et al.  Improved hydrothermal stability of mesoporous oxides for reactions in the aqueous phase. , 2012, Angewandte Chemie.

[8]  Stephanie G. Wettstein,et al.  Bimetallic catalysts for upgrading of biomass to fuels and chemicals. , 2012, Chemical Society reviews.

[9]  J. Crittenden,et al.  Effects of Metal Precursors on the Stability and Observed Reactivity of Pt/γ‐Al2O3 Catalysts in Aqueous Phase Reactions , 2012 .

[10]  J. Crittenden,et al.  Stability of Pt/γ-Al2O3 Catalysts in Model Biomass Solutions , 2012, Topics in Catalysis.

[11]  G. Xiao,et al.  Coking- and Sintering-Resistant Palladium Catalysts Achieved Through Atomic Layer Deposition , 2012, Science.

[12]  A. Datye,et al.  Synthesis of Highly Ordered Hydrothermally Stable Mesoporous Niobia Catalysts by Atomic Layer Deposition , 2011 .

[13]  A. Datye,et al.  The Sintering of Supported Pd Automotive Catalysts , 2011 .

[14]  A. Datye,et al.  Improved hydrothermal stability of niobia-supported Pd catalysts , 2011 .

[15]  J. Crittenden,et al.  Structural Changes of γ-Al2O3-Supported Catalysts in Hot Liquid Water , 2011 .

[16]  Joseph J. Bozell,et al.  Connecting Biomass and Petroleum Processing with a Chemical Bridge , 2010, Science.

[17]  Jean-Paul Lange,et al.  Valeric biofuels: a platform of cellulosic transportation fuels. , 2010, Angewandte Chemie.

[18]  D. M. Alonso,et al.  γ-Valerolactone ring-opening and decarboxylation over SiO2/Al2O3 in the presence of water. , 2010, Langmuir : the ACS journal of surfaces and colloids.

[19]  J. Elam,et al.  Palladium Catalysts Synthesized by Atomic Layer Deposition for Methanol Decomposition , 2010 .

[20]  Dong Wang,et al.  Catalytic upgrading of levulinic acid to 5-nonanone , 2010 .

[21]  L. Fu,et al.  Synthesis of carbon coated nanoporous microcomposite and its rate capability for lithium ion battery , 2009 .

[22]  Young Ho Kim,et al.  Preparation and characterization of carbon covered TiO2 using sucrose for solar photodegradation , 2008 .

[23]  C. Liang,et al.  Mesoporous carbon materials: synthesis and modification. , 2008, Angewandte Chemie.

[24]  D. Schaubroeck,et al.  Ordered mesoporous materials at the beginning of the third millennium: new strategies to create hybrid and non-siliceous variants. , 2008, Physical chemistry chemical physics : PCCP.

[25]  G. Huber,et al.  Liquid-phase catalytic processing of biomass-derived oxygenated hydrocarbons to fuels and chemicals. , 2007, Angewandte Chemie.

[26]  Xijun Hu,et al.  Synthesis of SBA-15/carbon composite with an ink-bottle-like pore structure by a novel pulse CVD technique , 2007 .

[27]  S. Joo,et al.  Synthesis and characterization of mesoporous carbon for fuel cell applications , 2007 .

[28]  W. Daud,et al.  Carbon Modified Silica based Adsorbent for Potential Application , 2007 .

[29]  A. Corma,et al.  Chemical routes for the transformation of biomass into chemicals. , 2007, Chemical reviews.

[30]  A. Corma,et al.  Synthesis of transportation fuels from biomass: chemistry, catalysts, and engineering. , 2006, Chemical reviews.

[31]  W. Lin,et al.  Uniformly carbon-covered alumina and its surface characteristics. , 2005, Langmuir : the ACS journal of surfaces and colloids.

[32]  林莉,et al.  热解蔗糖／γ-氧化铝制备碳均匀覆盖的碳／氧化铝复合材料 , 2004 .

[33]  K. Klabunde,et al.  Carbon Dispersion and Morphology in Carbon-Coated Nanocrystalline MgO , 2003 .

[34]  Andrew Cool,et al.  A detailed study of thermal, hydrothermal, and mechanical stabilities of a wide range of surfactant assembled mesoporous silicas , 2002 .

[35]  K. Sing,et al.  Stabilization of MCM-41 by Pyrolytic Carbon Deposition , 2000 .

[36]  M. Inagaki,et al.  A new simple process for carbon coating of ceramic particles using poly(vinyl chloride) , 1998 .

[37]  Avelino Corma,et al.  From Microporous to Mesoporous Molecular Sieve Materials and Their Use in Catalysis. , 1997, Chemical reviews.

[38]  R. Prins,et al.  Carbon-covered alumina as a support for sulfide catalysts , 1988 .

[39]  J. Raistrick,et al.  The adsorption of nitrogen and water vapour by carbon-coated precipitated silica , 1986 .