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Title: MCM-41 support for ultrasmall γ-Fe 2O 3 nanoparticles for H 2S removal

Abstract

In this paper, MCM-41 is proposed to build mesostructured Fe 2O 3-based sorbents as an alternative to other silica or alumina supports for mid-temperature H 2S 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-Fe 2O 3@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.

Authors:
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
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States); Univ. of Cagliari, Monserrato (Italy)
Sponsoring Org.:
USDOE Office of Science (SC); Consorzio AUSI (Italy); Univ. of Cagliari (Italy)
OSTI Identifier:
1425090
Report Number(s):
BNL-203302-2018-JAAM
Journal ID: ISSN 2050-7488; TRN: US1802041
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 5; Journal Issue: 41; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Cara, C., Rombi, E., Musinu, A., Mameli, V., Ardu, A., Sanna Angotzi, M., Atzori, L., Niznansky, D., Xin, H. L., and Cannas, C. MCM-41 support for ultrasmall γ-Fe2O3 nanoparticles for H2S removal. United States: N. p., 2017. Web. doi:10.1039/C7TA03652C.
Cara, C., Rombi, E., Musinu, A., Mameli, V., Ardu, A., Sanna Angotzi, M., Atzori, L., Niznansky, D., Xin, H. L., & Cannas, C. MCM-41 support for ultrasmall γ-Fe2O3 nanoparticles for H2S removal. United States. doi:10.1039/C7TA03652C.
Cara, C., Rombi, E., Musinu, A., Mameli, V., Ardu, A., Sanna Angotzi, M., Atzori, L., Niznansky, D., Xin, H. L., and Cannas, C. Sat . "MCM-41 support for ultrasmall γ-Fe2O3 nanoparticles for H2S removal". United States. doi:10.1039/C7TA03652C. https://www.osti.gov/servlets/purl/1425090.
@article{osti_1425090,
title = {MCM-41 support for ultrasmall γ-Fe2O3 nanoparticles for H2S removal},
author = {Cara, C. and Rombi, E. and Musinu, A. and Mameli, V. and Ardu, A. and Sanna Angotzi, M. and Atzori, L. and Niznansky, D. and Xin, H. L. and Cannas, C.},
abstractNote = {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.},
doi = {10.1039/C7TA03652C},
journal = {Journal of Materials Chemistry. A},
number = 41,
volume = 5,
place = {United States},
year = {2017},
month = {7}
}

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