Effects of Surface Features on Adsorption of SO2 on Graphite Oxide/Zr(OH)4 Composites

Zirconium hydroxide/graphene composites were synthesized from zirconium chloride and graphite oxide with the content of the graphene component between 5 and 50%. They were used as adsorbents of sulfur dioxide at ambient conditions. The initial and exhausted materials were characterized using adsorption of nitrogen, infrared spectroscopy, potentiometric titration, scanning electron microscopy and thermal analysis. The results indicated enhanced adsorption of SO2 on the composites, which is linked to the formation of new basic sites and porosity as a result of interactions between zirconium hydroxide units and the oxygen groups attached to the graphene layers. Both physical adsorption and reactive adsorption of SO2 via formation of sulfites play a role in the retention process. The graphene component catalyzes oxidation of SO2 and leads to the formation of sulfates.

[1]  Y. Gogotsi,et al.  Nitrogen modified carbide-derived carbons as adsorbents of hydrogen sulfide. , 2009, Journal of colloid and interface science.

[2]  David M. Cwiertny,et al.  Adsorption of sulfur dioxide on hematite and goethite particle surfaces. , 2007, Physical chemistry chemical physics : PCCP.

[3]  G. Peterson,et al.  Zirconium Hydroxide as a Reactive Substrate for the Removal of Sulfur Dioxide , 2009 .

[4]  Masaaki Yoshikawa,et al.  Removal of SOx and NOx over activated carbon fibers , 2000 .

[5]  Yu-Li Chen,et al.  Thermal, spectroscopic and X-ray diffractional analyses of zirconium hydroxides precipitated at low pH values , 2004 .

[6]  K. Kaneko,et al.  Effect of Pore Width on Micropore Filling Mechanism of SO2 in Carbon Micropores , 1998 .

[7]  H. Kanoh,et al.  Examination of synthesis conditions for graphite-derived nanoporous carbon–silica composites , 2006 .

[8]  Imre Dékány,et al.  Evolution of surface functional groups in a series of progressively oxidized graphite oxides , 2006 .

[9]  F. Carrasco-Marín,et al.  Activated carbons as adsorbents of sulfur dioxide in flowing air. Effect of their pore texture and surface basicity , 1993 .

[10]  G. L. Donnals,et al.  Adsorption of SO2 onto oxidized and heat-treated activated carbon fibers (ACFs) , 1997 .

[11]  S. Stankovich,et al.  Synthesis of graphene-based nanosheets via chemical reduction of exfoliated graphite oxide , 2007 .

[12]  F. Mondragón,et al.  Surface Complexes Formed during Simultaneous Catalytic Adsorption of NO and SO2 on Activated Carbons at Low Temperatures , 2007 .

[13]  W. S. Hummers,et al.  Preparation of Graphitic Oxide , 1958 .

[14]  J. A. Schwarz,et al.  SURFACE ACIDITY OF PILLARED TAENIOLITES IN TERMS OF THEIR PROTON AFFINITY DISTRIBUTIONS , 1995 .

[15]  M. Molina-Sabio,et al.  Adsorption of CO2 and SO2 on activated carbons with a wide range of micropore size distribution , 1995 .

[16]  J. Jagiello.  Stable Numerical Solution of the Adsorption Integral Equation Using Splines , 1994 .

[17]  M. Seredych,et al.  Mechanism of Ammonia Retention on Graphite Oxides: Role of Surface Chemistry and Structure† , 2007 .

[18]  M. Seredych,et al.  Adsorption of ammonia on graphite oxide/aluminium polycation and graphite oxide/zirconium-aluminium polyoxycation composites. , 2008, Journal of colloid and interface science.

[19]  J. Juan,et al.  The zirconium sulfate microcrystal structure in relation to their activity in the esterification. , 2007 .

[20]  Shin-Min Shih,et al.  Calcium hydroxide/fly ash sorbents for sulfur dioxide removal , 1992 .

[21]  Robert Schlögl,et al.  Enhancement of the catalytic activity of activated carbons in oxidation reactions by thermal treatment with ammonia or hydrogen cyanide and observation of a superoxide species as a possible intermediate , 1991 .

[22]  C. Petit,et al.  MOF–Graphite Oxide Composites: Combining the Uniqueness of Graphene Layers and Metal–Organic Frameworks , 2009 .

[23]  D. Cazorla-Amorós,et al.  Factors controling the SO2 removal by porous carbons: relevance of the SO2 oxidation step , 2000 .

[24]  Camille Petit,et al.  MOF–graphite oxide nanocomposites: surface characterization and evaluation as adsorbents of ammonia , 2009 .

[25]  K. Kaneko,et al.  Dipole Oriented States of SO2 Confined in a Slit-Shaped Graphitic Subnanospace from Calorimetry , 1995 .

[26]  C. Petit,et al.  Graphite Oxide/Polyoxometalate Nanocomposites as Adsorbents of Ammonia , 2009 .

[27]  R. Semiat,et al.  Adsorption of sulfur dioxide by active carbon treated by nitric acid: I. Effect of the treatment on adsorption of SO2 and extractability of the acid formed , 1997 .

[28]  R. Siriwardane,et al.  In Situ Fourier Transform Infrared Characterization of Sulfur Species Resulting from the Reaction of Water Vapor and Oxygen with Zinc Sulfide , 1997 .

[29]  I. Dukhno,et al.  Mechanism of reductive oxygen adsorption on active carbons with various surface chemistry , 2004 .

[30]  S. Musić,et al.  The effect of mechanical treatment of zirconium(IV) hydroxide on its thermal behaviour , 1995 .

[31]  I. Dékány,et al.  DRIFT study of deuterium-exchanged graphite oxide , 2005 .

[32]  J. Sohn,et al.  Preparation of new solid superacid catalyst, zirconium sulfate supported on γ-alumina and activity for acid catalysis , 2003 .

[33]  J. A. Schwarz,et al.  Carbon surface characterization in terms of its acidity constant distribution , 1994 .

[34]  A. Goodman,et al.  Heterogeneous Uptake of Sulfur Dioxide On Aluminum and Magnesium Oxide Particles , 2001 .

[35]  T. Bandosz,et al.  Adsorption/Reduction of NO2 on Graphite Oxide/Iron Composites , 2009 .

[36]  Cheol-Woong Yang,et al.  Evidence of graphitic AB stacking order of graphite oxides. , 2008, Journal of the American Chemical Society.

[37]  Jacek Klinowski,et al.  Structure of Graphite Oxide Revisited , 1998 .

[38]  T. Bandosz,et al.  Adsorption of SO2 on sewage sludge-derived materials. , 2001, Environmental science & technology.

[39]  C. Petit,et al.  On the reactive adsorption of ammonia on activated carbons modified by impregnation with inorganic compounds. , 2009, Journal of colloid and interface science.

[40]  M. Seredych,et al.  Desulfurization of air at high and low H2S concentrations , 2009 .

[41]  A. Lua,et al.  Adsorption of sulfur dioxide onto activated carbons prepared from oil-palm shells impregnated with potassium hydroxide , 2000 .

[42]  John A. N. Lee.  Influence of tension during oxidative stabilization on SO2 adsorption characteristics of polyacrylonitrile (PAN) based activated carbon fibres , 1997 .

[43]  Turkan Kopac,et al.  Adsorption equilibrium and breakthrough analysis for sulfur dioxide adsorption on silica gel , 2002 .

[44]  T. Bandosz,et al.  Adsorption of SO2 on activated carbons: The effect of nitrogen functionality and pore sizes , 2002 .

[45]  K. Ooi,et al.  Selective adsorption of phosphate from seawater and wastewater by amorphous zirconium hydroxide. , 2006, Journal of colloid and interface science.

[46]  J. D. Lopez-Gonzalez,et al.  Study of oxygen-containing groups in a series of graphite oxides: Physical and chemical characterization , 1995 .

[47]  Alexandra Buchsteiner,et al.  Water dynamics in graphite oxide investigated with neutron scattering. , 2006, The journal of physical chemistry. B.

[48]  P. Davini.  SO2 and NOx adsorption properties of activated carbons obtained from a pitch containing iron derivatives , 2001 .

[49]  Camille Petit,et al.  Revisiting the chemistry of graphite oxides and its effect on ammonia adsorption , 2009 .

[50]  J. Órfão,et al.  Adsorption of SO2 using vanadium and vanadium–copper supported on activated carbon , 2003 .

[51]  M. Seredych,et al.  Combined role of water and surface chemistry in reactive adsorption of ammonia on graphite oxides. , 2010, Langmuir : the ACS journal of surfaces and colloids.

[52]  K. Morishige,et al.  Iron oxide pillared graphite. , 2005, Langmuir : the ACS journal of surfaces and colloids.

[53]  M. Grutzeck,et al.  The Adsorption of SO2 by Zeolites Synthesized from Fly Ash , 1999 .

[54]  M. Zaki,et al.  Fourier-transform laser Raman spectroscopy of adsorbed pyridine and nature of acid sites on calcined phosphate/Zr(OH)4 , 1998 .

[55]  J. DeBarr,et al.  The mechanism of SO2 removal by carbon , 1997 .

[56]  E. Bottani,et al.  SO2 physisorption on exfoliated graphite , 2003 .