Research output: Contribution to journal › Article › peer-review
Factors Influencing the Performance of Pd/C Catalysts in the Green Production of Hydrogen from Formic Acid. / Zacharska, Monika; Bulusheva, Lyubov G.; Lisitsyn, Alexander S. et al.
In: ChemSusChem, Vol. 10, No. 4, 22.02.2017, p. 720-730.Research output: Contribution to journal › Article › peer-review
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TY - JOUR
T1 - Factors Influencing the Performance of Pd/C Catalysts in the Green Production of Hydrogen from Formic Acid
AU - Zacharska, Monika
AU - Bulusheva, Lyubov G.
AU - Lisitsyn, Alexander S.
AU - Beloshapkin, Sergey
AU - Guo, Yina
AU - Chuvilin, Andrey L.
AU - Shlyakhova, Elena V.
AU - Podyacheva, Olga Y.
AU - Leahy, James J.
AU - Okotrub, Alexander V.
AU - Bulushev, Dmitri A.
N1 - Publisher Copyright: © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
PY - 2017/2/22
Y1 - 2017/2/22
N2 - Formic acid derived from biomass is known to be used for hydrogen production over Pd catalysts. The effects of preparation variables, structure of the carbon support, surface functional composition on the state of Pd, and catalytic properties of the samples in the vapor-phase decomposition of formic acid were studied. In all catalysts derived from Pd acetate, metal particles visible by conventional TEM had similar sizes, but the adsorption capacity towards CO responded strongly to N-doping of the carbon surface. Moreover, a decrease in the CO/Pd values was accompanied by a significant increase in the reaction rate. Taking account of X-ray photoelectron spectroscopy (XPS) and atomic resolution high-angle annular dark-field scanning transmission electron microscopy (HAADF/STEM) data, the trends observed were assigned to a larger fraction of single electron-deficient Pd atoms in the N-doped samples, which do not adsorb CO but interact with formic acid to produce hydrogen. This was confirmed by extended DFT studies. The obtained results are valuable for the development of Pd catalysts on carbon supports for different processes.
AB - Formic acid derived from biomass is known to be used for hydrogen production over Pd catalysts. The effects of preparation variables, structure of the carbon support, surface functional composition on the state of Pd, and catalytic properties of the samples in the vapor-phase decomposition of formic acid were studied. In all catalysts derived from Pd acetate, metal particles visible by conventional TEM had similar sizes, but the adsorption capacity towards CO responded strongly to N-doping of the carbon surface. Moreover, a decrease in the CO/Pd values was accompanied by a significant increase in the reaction rate. Taking account of X-ray photoelectron spectroscopy (XPS) and atomic resolution high-angle annular dark-field scanning transmission electron microscopy (HAADF/STEM) data, the trends observed were assigned to a larger fraction of single electron-deficient Pd atoms in the N-doped samples, which do not adsorb CO but interact with formic acid to produce hydrogen. This was confirmed by extended DFT studies. The obtained results are valuable for the development of Pd catalysts on carbon supports for different processes.
KW - biomass
KW - carbon
KW - doping
KW - hydrogen
KW - palladium
KW - Carbon Monoxide
KW - Carbon/chemistry
KW - Biomass
KW - Hydrogen/chemistry
KW - Green Chemistry Technology/methods
KW - Palladium/chemistry
KW - Adsorption
KW - Catalysis
KW - Formates/chemistry
KW - PALLADIUM
KW - ROOM-TEMPERATURE
KW - SELECTIVE OXIDATION
KW - NANOFIBERS
KW - MONOXIDE OXIDATION
KW - DECOMPOSITION
KW - NITROGEN-DOPED CARBON
KW - NANOPARTICLES
KW - DEHYDROGENATION
KW - CLUSTERS
UR - http://www.scopus.com/inward/record.url?scp=85012041456&partnerID=8YFLogxK
U2 - 10.1002/cssc.201601637
DO - 10.1002/cssc.201601637
M3 - Article
C2 - 27996206
AN - SCOPUS:85012041456
VL - 10
SP - 720
EP - 730
JO - ChemSusChem
JF - ChemSusChem
SN - 1864-5631
IS - 4
ER -
ID: 9047674