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Title: Methanation of Carbon Dioxide on Ni-Incorporated MCM-41 Catalysts: The Influence of Catalyst Pretreatment and Study of Steady-State Reaction

Abstract

The methanation of carbon dioxide was carried out over Ni-incorporated MCM-41 catalysts. The Ni-MCM-41 catalysts containing 1-3 wt% Ni were prepared by incorporating the Ni ions into the framework of siliceous MCM-41 with the procedure developed in our previous work. Pretreatment using pure H2 at different temperatures affected the reactivity. Pretreatment at 973 K for 0.5 h was the best among the conditions tested. At this temperature, the Ni was mostly reduced but remained highly dispersed. Significant selectivity to methane (85.1%) was obtained with 1 wt% Ni-MCM-41 at a reaction temperature as low as 573 K and gas hourly space velocity (GHSV) of 5760 l kg?1 h?1 under atmospheric pressure. Higher selectivity (96.0%) and space-time yield (91.4 g kg?1 h?1) were achieved with higher Ni loading catalysts (3 wt% Ni) at the same space velocity. This selectivity was maintained at higher temperature (673 K) with increased space-time yield (633 g kg?1 h?1). The X-ray absorption result demonstrates that the Ni particle size does not significantly change during reaction.

Authors:
; ; ; ; ;
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL) National Synchrotron Light Source
Sponsoring Org.:
Doe - Office Of Science
OSTI Identifier:
959706
Report Number(s):
BNL-82692-2009-JA
Journal ID: ISSN 0021-9517; JCTLA5; TRN: US201016%%850
DOE Contract Number:
DE-AC02-98CH10886
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Catalysis; Journal Volume: 49
Country of Publication:
United States
Language:
English
Subject:
03 NATURAL GAS; 10 SYNTHETIC FUELS; ABSORPTION; ATMOSPHERIC PRESSURE; CARBON DIOXIDE; CATALYSTS; METHANATION; METHANE; PARTICLE SIZE; SPACE-TIME; VELOCITY; national synchrotron light source

Citation Formats

Du,G., Lim, S., Yang, Y., Wang, C., Pfefferle, L., and Haller, G.. Methanation of Carbon Dioxide on Ni-Incorporated MCM-41 Catalysts: The Influence of Catalyst Pretreatment and Study of Steady-State Reaction. United States: N. p., 2007. Web. doi:10.1016/j.jcat.2007.03.029.
Du,G., Lim, S., Yang, Y., Wang, C., Pfefferle, L., & Haller, G.. Methanation of Carbon Dioxide on Ni-Incorporated MCM-41 Catalysts: The Influence of Catalyst Pretreatment and Study of Steady-State Reaction. United States. doi:10.1016/j.jcat.2007.03.029.
Du,G., Lim, S., Yang, Y., Wang, C., Pfefferle, L., and Haller, G.. Mon . "Methanation of Carbon Dioxide on Ni-Incorporated MCM-41 Catalysts: The Influence of Catalyst Pretreatment and Study of Steady-State Reaction". United States. doi:10.1016/j.jcat.2007.03.029.
@article{osti_959706,
title = {Methanation of Carbon Dioxide on Ni-Incorporated MCM-41 Catalysts: The Influence of Catalyst Pretreatment and Study of Steady-State Reaction},
author = {Du,G. and Lim, S. and Yang, Y. and Wang, C. and Pfefferle, L. and Haller, G.},
abstractNote = {The methanation of carbon dioxide was carried out over Ni-incorporated MCM-41 catalysts. The Ni-MCM-41 catalysts containing 1-3 wt% Ni were prepared by incorporating the Ni ions into the framework of siliceous MCM-41 with the procedure developed in our previous work. Pretreatment using pure H2 at different temperatures affected the reactivity. Pretreatment at 973 K for 0.5 h was the best among the conditions tested. At this temperature, the Ni was mostly reduced but remained highly dispersed. Significant selectivity to methane (85.1%) was obtained with 1 wt% Ni-MCM-41 at a reaction temperature as low as 573 K and gas hourly space velocity (GHSV) of 5760 l kg?1 h?1 under atmospheric pressure. Higher selectivity (96.0%) and space-time yield (91.4 g kg?1 h?1) were achieved with higher Ni loading catalysts (3 wt% Ni) at the same space velocity. This selectivity was maintained at higher temperature (673 K) with increased space-time yield (633 g kg?1 h?1). The X-ray absorption result demonstrates that the Ni particle size does not significantly change during reaction.},
doi = {10.1016/j.jcat.2007.03.029},
journal = {Journal of Catalysis},
number = ,
volume = 49,
place = {United States},
year = {Mon Jan 01 00:00:00 EST 2007},
month = {Mon Jan 01 00:00:00 EST 2007}
}