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Title: A study on methanol steam reforming to CO{sub 2} and H{sub 2} over the La{sub 2}CuO{sub 4} nanofiber catalyst

Abstract

The La{sub 2}CuO{sub 4} crystal nanofibers were prepared by using single-walled carbon nanotubes as templates under mild hydrothermal conditions. The steam reforming of methanol (SRM) to CO{sub 2} and H{sub 2} over such nanofiber catalysts was studied. At the low temperature of 150 deg. C and steam/methanol=1.3, methanol was completely (100%, 13.8 g/h g catalyst) converted to hydrogen and CO{sub 2} without the generation of CO. Within the 60 h catalyst lifespan test, methanol conversion was maintained at 98.6% (13.6 g/h g catalyst) and with 100% CO{sub 2} selectivity. In the meantime, for distinguishing the advantage of nanoscale catalyst, the La{sub 2}CuO{sub 4} bulk powder was prepared and tested for the SRM reaction for comparison. Compared with the La{sub 2}CuO{sub 4} nanofiber, the bulk powder La{sub 2}CuO{sub 4} showed worse catalytic activity for the SRM reaction. The 100% conversion of methanol was achieved at the temperature of 400 deg. C, with the products being H{sub 2} and CO{sub 2} together with CO. The catalytic activity in terms of methanol conversion dropped to 88.7% (12.2 g/h g catalyst) in 60 h. The reduction temperature for nanofiber La{sub 2}CuO{sub 4} was much lower than that for the La{sub 2}CuO{sub 4} bulk powder.more » The nanofibers were of higher specific surface area (105.0 m{sup 2}/g), metal copper area and copper dispersion. The in situ FTIR and EPR experiments were employed to study the catalysts and catalytic process. In the nanofiber catalyst, there were oxygen vacancies. H{sub 2}-reduction resulted in the generation of trapped electrons [e] on the vacancy sites. Over the nanofiber catalyst, the intermediate H{sub 2}CO/HCO was stable and was reformed to CO{sub 2} and H{sub 2} by steam rather than being decomposed directly to CO and H{sub 2}. Over the bulk counterpart, apart from the direct decomposition of H{sub 2}CO/HCO to CO and H{sub 2}, the intermediate H{sub 2}COO might go through two decomposition ways: H{sub 2}COO=CO+H{sub 2}O and H{sub 2}COO=CO{sub 2}+H{sub 2}. - Graphical abstract: The steam reforming of methanol (SRM) to CO{sub 2} and H{sub 2} over La{sub 2}CuO{sub 4} nanofiber catalyst was studied. At the temperature as low as 150 deg. C, methanol was completely (100%) converted to hydrogen and CO{sub 2} without the generation of CO. Within the 60 h catalyst lifespan test, methanol conversion was maintained at 98.6% and with 100% CO{sub 2} selectivity.« less

Authors:
;  [1]
  1. Department of Chemical and Biomolecular Engineering, National University of Singapore, 4 Engineering Drive 4, Singapore 117576, Republic of Singapore (Singapore)
Publication Date:
OSTI Identifier:
21043853
Resource Type:
Journal Article
Journal Name:
Journal of Solid State Chemistry
Additional Journal Information:
Journal Volume: 181; Journal Issue: 1; Other Information: DOI: 10.1016/j.jssc.2007.10.029; PII: S0022-4596(07)00443-4; Copyright (c) 2007 Elsevier Science B.V., Amsterdam, The Netherlands, All rights reserved; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0022-4596
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; CALIBRATION STANDARDS; CARBON DIOXIDE; CARBON MONOXIDE; CATALYSIS; CATALYSTS; CRYSTALS; CUPRATES; ELECTRON SPIN RESONANCE; FOURIER TRANSFORMATION; HYDROGEN; INFRARED SPECTRA; LANTHANUM COMPOUNDS; METHANOL; NANOTUBES; SPECIFIC SURFACE AREA; TEMPERATURE RANGE 0065-0273 K; TRAPPED ELECTRONS; VACANCIES; WATER

Citation Formats

Gao Lizhen, Gebiao, Sun, and Kawi, Sibudjing. A study on methanol steam reforming to CO{sub 2} and H{sub 2} over the La{sub 2}CuO{sub 4} nanofiber catalyst. United States: N. p., 2008. Web.
Gao Lizhen, Gebiao, Sun, & Kawi, Sibudjing. A study on methanol steam reforming to CO{sub 2} and H{sub 2} over the La{sub 2}CuO{sub 4} nanofiber catalyst. United States.
Gao Lizhen, Gebiao, Sun, and Kawi, Sibudjing. 2008. "A study on methanol steam reforming to CO{sub 2} and H{sub 2} over the La{sub 2}CuO{sub 4} nanofiber catalyst". United States.
@article{osti_21043853,
title = {A study on methanol steam reforming to CO{sub 2} and H{sub 2} over the La{sub 2}CuO{sub 4} nanofiber catalyst},
author = {Gao Lizhen and Gebiao, Sun and Kawi, Sibudjing},
abstractNote = {The La{sub 2}CuO{sub 4} crystal nanofibers were prepared by using single-walled carbon nanotubes as templates under mild hydrothermal conditions. The steam reforming of methanol (SRM) to CO{sub 2} and H{sub 2} over such nanofiber catalysts was studied. At the low temperature of 150 deg. C and steam/methanol=1.3, methanol was completely (100%, 13.8 g/h g catalyst) converted to hydrogen and CO{sub 2} without the generation of CO. Within the 60 h catalyst lifespan test, methanol conversion was maintained at 98.6% (13.6 g/h g catalyst) and with 100% CO{sub 2} selectivity. In the meantime, for distinguishing the advantage of nanoscale catalyst, the La{sub 2}CuO{sub 4} bulk powder was prepared and tested for the SRM reaction for comparison. Compared with the La{sub 2}CuO{sub 4} nanofiber, the bulk powder La{sub 2}CuO{sub 4} showed worse catalytic activity for the SRM reaction. The 100% conversion of methanol was achieved at the temperature of 400 deg. C, with the products being H{sub 2} and CO{sub 2} together with CO. The catalytic activity in terms of methanol conversion dropped to 88.7% (12.2 g/h g catalyst) in 60 h. The reduction temperature for nanofiber La{sub 2}CuO{sub 4} was much lower than that for the La{sub 2}CuO{sub 4} bulk powder. The nanofibers were of higher specific surface area (105.0 m{sup 2}/g), metal copper area and copper dispersion. The in situ FTIR and EPR experiments were employed to study the catalysts and catalytic process. In the nanofiber catalyst, there were oxygen vacancies. H{sub 2}-reduction resulted in the generation of trapped electrons [e] on the vacancy sites. Over the nanofiber catalyst, the intermediate H{sub 2}CO/HCO was stable and was reformed to CO{sub 2} and H{sub 2} by steam rather than being decomposed directly to CO and H{sub 2}. Over the bulk counterpart, apart from the direct decomposition of H{sub 2}CO/HCO to CO and H{sub 2}, the intermediate H{sub 2}COO might go through two decomposition ways: H{sub 2}COO=CO+H{sub 2}O and H{sub 2}COO=CO{sub 2}+H{sub 2}. - Graphical abstract: The steam reforming of methanol (SRM) to CO{sub 2} and H{sub 2} over La{sub 2}CuO{sub 4} nanofiber catalyst was studied. At the temperature as low as 150 deg. C, methanol was completely (100%) converted to hydrogen and CO{sub 2} without the generation of CO. Within the 60 h catalyst lifespan test, methanol conversion was maintained at 98.6% and with 100% CO{sub 2} selectivity.},
doi = {},
url = {https://www.osti.gov/biblio/21043853}, journal = {Journal of Solid State Chemistry},
issn = {0022-4596},
number = 1,
volume = 181,
place = {United States},
year = {Tue Jan 15 00:00:00 EST 2008},
month = {Tue Jan 15 00:00:00 EST 2008}
}