期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 160, 期 -, 页码 35-43出版社
ELSEVIER SCIENCE BV
DOI: 10.1016/j.apcatb.2014.05.004
关键词
Formic acid; Hydrogen production; Doping; Potassium formate; Palladium
资金
- Science Foundation Ireland [06/CP/E007]
- Chinese Scholarship Council
- INSPIRE programme - Irish Government's Programme
- Science Foundation Ireland (SFI) [06/CP/E007] Funding Source: Science Foundation Ireland (SFI)
Doping a 1 wt.% Pd/C catalyst with alkali metal carbonates has a very significant promotional effect on its activity in hydrogen production from the decomposition of formic acid vapour (2 vol.%, 1 bar), potassium and caesium carbonates giving the largest effects. The K carbonate species present on the fresh catalysts react with formic acid to form formate ions, these being dissolved in a formic acid/water solution condensed in the pores of the support. The steady-state activities of the samples containing formate ions were 1-2 orders of magnitude greater than those of the unpromoted Pd/C and CO content was lower than 30 ppm. The activation energies for the reaction increased with doping from 66 to 88-99 kJ mo1-1, relatively independent of the cation of the dopant. Similar but lesser effects were found with unsupported Pd nanocrystals doped with K carbonate. The rate-determining step for the promoted samples appears to be the decomposition of formate ions on the Pd surface. (C) 2014 Elsevier B.V. All rights reserved.
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