Research output: Contribution to journal › Article › peer-review
Boosting hydrogen production from formic acid over Pd catalysts by deposition of N-Containing precursors on the carbon support. / Golub, Fedor S.; Beloshapkin, Sergey; Gusel'Nikov, Artem V. et al.
In: Energies, Vol. 12, No. 20, 3885, 14.10.2019.Research output: Contribution to journal › Article › peer-review
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TY - JOUR
T1 - Boosting hydrogen production from formic acid over Pd catalysts by deposition of N-Containing precursors on the carbon support
AU - Golub, Fedor S.
AU - Beloshapkin, Sergey
AU - Gusel'Nikov, Artem V.
AU - Bolotov, Vasily A.
AU - Parmon, Valentin N.
AU - Bulushev, Dmitri A.
PY - 2019/10/14
Y1 - 2019/10/14
N2 - Formic acid is a promising liquid organic hydrogen carrier (LOHC) since it has relatively high hydrogen content (4.4 wt%), low inflammability, low toxicity and can be obtained from biomass or from CO2. The aim of the present research was the creation of efficient 1 wt% Pd catalysts supported on mesoporous graphitic carbon (Sibunit) for the hydrogen production from gas-phase formic acid. For this purpose, the carbon support was modified by pyrolysis of deposited precursors containing pyridinic nitrogen such as melamine (Mel), 2,20-bipyridine (Bpy) or 1,10-phenanthroline (Phen) at 673 K. The following activity trend of the catalysts Pd/Mel/C > Pd/C ~ Pd/Bpy/C > Pd/Phen/C was obtained. The activity of the Pd/Mel/C catalyst was by a factor of 4 higher than the activity of the Pd/C catalyst at about 373 K and the apparent activation energy was significantly lower than those for the other catalysts (32 vs. 42-46 kJ/mol). The high activity of the melamine-based samples was explained by a high dispersion of Pd nanoparticles (~2 nm, HRTEM) and their strong electron-deficient character (XPS) provided by interaction of Pd with pyridinic nitrogen species of the support. The presented results can be used for the development of supported Pd catalysts for hydrogen production from different liquid organic hydrogen carriers.
AB - Formic acid is a promising liquid organic hydrogen carrier (LOHC) since it has relatively high hydrogen content (4.4 wt%), low inflammability, low toxicity and can be obtained from biomass or from CO2. The aim of the present research was the creation of efficient 1 wt% Pd catalysts supported on mesoporous graphitic carbon (Sibunit) for the hydrogen production from gas-phase formic acid. For this purpose, the carbon support was modified by pyrolysis of deposited precursors containing pyridinic nitrogen such as melamine (Mel), 2,20-bipyridine (Bpy) or 1,10-phenanthroline (Phen) at 673 K. The following activity trend of the catalysts Pd/Mel/C > Pd/C ~ Pd/Bpy/C > Pd/Phen/C was obtained. The activity of the Pd/Mel/C catalyst was by a factor of 4 higher than the activity of the Pd/C catalyst at about 373 K and the apparent activation energy was significantly lower than those for the other catalysts (32 vs. 42-46 kJ/mol). The high activity of the melamine-based samples was explained by a high dispersion of Pd nanoparticles (~2 nm, HRTEM) and their strong electron-deficient character (XPS) provided by interaction of Pd with pyridinic nitrogen species of the support. The presented results can be used for the development of supported Pd catalysts for hydrogen production from different liquid organic hydrogen carriers.
KW - Bipyridine
KW - Formic acid decomposition
KW - G-C3N4
KW - Hydrogen production
KW - Melamine
KW - N-doped carbon
KW - Pd/C
KW - Phenanthroline
KW - g-C3N4
KW - bipyridine
KW - NANOFIBERS
KW - formic acid decomposition
KW - DOPED CARBON
KW - CO2
KW - melamine
KW - NITRIDE
KW - hydrogen production
KW - phenanthroline
KW - HIGH-SURFACE-AREA
KW - TEMPERATURE
KW - SITES
KW - EFFICIENCY
UR - http://www.scopus.com/inward/record.url?scp=85074969213&partnerID=8YFLogxK
U2 - 10.3390/en12203885
DO - 10.3390/en12203885
M3 - Article
AN - SCOPUS:85074969213
VL - 12
JO - Energies
JF - Energies
SN - 1996-1073
IS - 20
M1 - 3885
ER -
ID: 22319533