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Title: MCM-41 support for ultrasmall γ-Fe2O3 nanoparticles for H2S removal

Journal Article · · Journal of Materials Chemistry. A
DOI:https://doi.org/10.1039/C7TA03652C· OSTI ID:1425090
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [1]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [4]; ORCiD logo [5]; ORCiD logo [1]
  1. Univ. of Cagliari, Monserrato (Italy). Dept. of Chemical and Geological Sciences; Consorzio AUSI, Iglesias (Italy); National Interuniversity Consortium of Materials Science and Technology (INSTM), Cagliari (Italy)
  2. Univ. of Cagliari, Monserrato (Italy). Dept. of Chemical and Geological Sciences
  3. Univ. of Cagliari, Monserrato (Italy). Dept. of Chemical and Geological Sciences; National Interuniversity Consortium of Materials Science and Technology (INSTM), Cagliari (Italy)
  4. Charles Univ., Prague (Czech Republic). Dept. of Inorganic Chemistry; Inst. of Inorganic Chemistry of the Czech Academy Of Sciences, Husinec Rez (Czech Republic)
  5. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials

In this paper, MCM-41 is proposed to build mesostructured Fe2O3-based sorbents as an alternative to other silica or alumina supports for mid-temperature H2S removal. MCM-41 was synthesized as micrometric (MCM41_M) and nanometric (MCM41_N) particles and impregnated through an efficient two-solvent (hexane–water) procedure to obtain the corresponding γ-Fe2O3@MCM-41 composites. The active phase is homogeneously dispersed within the 2 nm channels in the form of ultrasmall maghemite nanoparticles assuring a high active phase reactivity. The final micrometric (Fe_MCM41_M) and nanometric (Fe_MCM41_N) composites were tested as sorbents for hydrogen sulphide removal at 300 °C and the results were compared with a reference sorbent (commercial unsupported ZnO) and an analogous silica-based sorbent (Fe_SBA15). MCM-41 based sorbents, having the highest surface areas, showed superior performances that were retained after the first sulphidation cycle. Specifically, the micrometric sorbent (Fe_MCM41_M) showed a higher SRC value than the nanometric one (Fe_MCM41_N), due to the low stability of the nanosized particles over time caused by their high reactivity. Finally and furthermore, the low regeneration temperature (300–350 °C), besides the high removal capacity, renders MCM41-based systems an alternative class of regenerable sorbents for thermally efficient cleaning up processes in Integrated Gasification Combined Cycles (IGCC) systems.

Research Organization:
Brookhaven National Lab. (BNL), Upton, NY (United States); Univ. of Cagliari, Monserrato (Italy)
Sponsoring Organization:
USDOE Office of Science (SC); Consorzio AUSI (Italy); Univ. of Cagliari (Italy)
Grant/Contract Number:
SC0012704
OSTI ID:
1425090
Report Number(s):
BNL-203302-2018-JAAM; TRN: US1802041
Journal Information:
Journal of Materials Chemistry. A, Vol. 5, Issue 41; ISSN 2050-7488
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 50 works
Citation information provided by
Web of Science

References (53)

Physisorption of gases, with special reference to the evaluation of surface area and pore size distribution (IUPAC Technical Report) journal October 2015
Study of the Adsorption Properties of MCM-41 Molecular Sieves Prepared at Different Synthesis Times journal March 2005
A high-performance adsorbent for hydrogen sulfide removal journal May 2014
Chemical mapping at atomic resolution using energy-dispersive x-ray spectroscopy journal January 2012
Effect of the adsorbate kinetic diameter on the accuracy of the Dubinin–Radushkevich equation for modeling adsorption of organic vapors on activated carbon journal November 2012
The mechanism of coal gas desulfurization by iron oxide sorbents journal February 2015
Hierarchical Formation Mechanism of CoFe 2 O 4 Mesoporous Assemblies journal June 2015
Dialkylamide as Both Capping Agent and Surfactant in a Direct Solvothermal Synthesis of Magnetite and Titania Nanoparticles journal March 2015
The Iron Oxides book July 2003
A new family of mesoporous molecular sieves prepared with liquid crystal templates journal December 1992
Magnetic nanoparticle-based therapeutic agents for thermo-chemotherapy treatment of cancer journal January 2014
Hydrogen Sulfide Adsorption on MOFs and MOF/Graphite Oxide Composites journal October 2010
Pyrophoric oxidation of iron sulphide journal March 1988
Oxidation of H 2 S by Iron Oxides in Unsaturated Conditions journal May 2003
Isoreticular rare earth fcu -MOFs for the selective removal of H 2 S from CO 2 containing gases journal September 2017
Evaluation of a novel mixed pyrite/pyrrhotite catalyst for coal liquefaction journal June 1993
Surfactant-assisted route to fabricate CoFe2O4 individual nanoparticles and spherical assemblies journal March 2010
Catalysts from MCM-41: framework modification, pore size engineering, and organic–inorganic hybrid materials journal March 2002
One-step room temperature synthesis of very small γ-Fe2O3 nanoparticles journal September 2013
The dry oxidation of tetragonal FeS 1- x mackinawite journal October 2001
CO oxidation and preferential oxidation of CO in the presence of hydrogen over SBA-15-templated CuO-Co3O4 catalysts journal November 2012
Simultaneous Adsorption of H 2 S and CO 2 on Triamine-Grafted Pore-Expanded Mesoporous MCM-41 Silica journal March 2011
Mechanism of H 2 S Oxidation by Ferric Oxide and Hydroxide Surfaces journal June 1998
Synthesis, characterization and catalytic performance for phenol hydroxylation of Fe-MCM41 with high iron content journal August 2008
SBA-15 Mesoporous Silica as Catalytic Support for Hydrodesulfurization Catalysts—Review journal September 2013
Preparation of high thermal stability MCM-41 in the low surfactant/silicon molar ratio synthesis systems journal March 2001
Facile Synthesis of Monodispersed Mesoporous Silica Nanoparticles with Ultralarge Pores and Their Application in Gene Delivery journal April 2011
The variable property grain model applied to the zinc oxide-hydrogen sulfide reaction journal January 1981
Modifications induced by pretreatments on Au/SBA-15 and their influence on the catalytic activity for low temperature CO oxidation journal January 2009
Nanostructured ZnO/sepiolite monolithic sorbents for H 2 S removal journal January 2015
Adsorption of hydrogen sulfide on ZSM 5 zeolites journal March 1992
Solid-State NMR Study of MCM-41-type Mesoporous Silica Nanoparticles journal March 2005
Magnetic properties of nanoscale crystalline maghemite obtained by a new synthetic route journal September 2012
A Multiunit Catalyst with Synergistic Stability and Reactivity: A Polyoxometalate–Metal Organic Framework for Aerobic Decontamination journal October 2011
Metal–organic frameworks to satisfy gas upgrading demands: fine-tuning the soc -MOF platform for the operative removal of H 2 S journal January 2017
High efficient fluorescent stable colloidal sealed dye-doped mesostructured silica nanoparticles journal May 2016
Low temperature H2S dry-desulfurization with zinc oxide journal February 2010
Manual of methods and procedures for catalyst characterization (Technical Report) journal January 1995
MeO x /SBA-15 (Me = Zn, Fe): highly efficient nanosorbents for mid-temperature H 2 S removal journal January 2014
Sulfur removal from coal-derived syngas: thermodynamic considerations and review
  • Dolan, Michael D.; Ilyushechkin, Alex Y.; McLennan, Keith G.
  • Asia-Pacific Journal of Chemical Engineering, Vol. 7, Issue 1 https://doi.org/10.1002/apj.528
journal December 2010
Novel mesoporous silica supported ZnO adsorbents for the desulphurization of biogas at low temperatures journal April 2012
A study on sulphidation and regeneration of Z-Sorb III sorbent for H2S removal from simulated ELCOGAS IGCC syngas journal June 2005
Effective removal of hydrogen sulfide using 4A molecular sieve zeolite synthesized from attapulgite journal March 2017
Review of Mid- to High-Temperature Sulfur Sorbents for Desulfurization of Biomass- and Coal-derived Syngas journal November 2009
Evaluation of Zinc Oxide Sorbents in a Pilot-Scale Transport Reactor:  Sulfidation Kinetics and Reactor Modeling journal March 2004
Synthesis and Characterization of γ-Fe 2 O 3 for H 2 S Removal at Low Temperature journal August 2015
Evaluation of candidate solids for high-temperature desulfurization of low-Btu gases journal July 1976
ZnO/SBA-15 composites for mid-temperature removal of H2S: Synthesis, performance and regeneration studies journal December 2012
Characterization of active sites, determination of mechanisms of H2S, COS and CS2 sorption and regeneration of ZnO low-temperature sorbents: past, current and perspectives journal January 2011
XRD, TEM and 29Si MAS NMR study of sol-gel ZnO-SiO2 nanocomposites journal January 1999
Triblock Copolymer Syntheses of Mesoporous Silica with Periodic 50 to 300 Angstrom Pores journal January 1998
Thermal and hydrothermal stability of framework-substituted MCM-41 mesoporous materials journal December 1997
Spherical Nanoporous Assemblies of Iso-Oriented Cobalt Ferrite Nanoparticles: Synthesis, Microstructure, and Magnetic Properties journal October 2008

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