Research output: Contribution to journal › Article › peer-review
Ruthenium Clusters on Carbon Nanofibers for Formic Acid Decomposition : Effect of Doping the Support with Nitrogen. / Zacharska, Monika; Podyacheva, Olga Yu; Kibis, Lidiya S. et al.
In: ChemCatChem, Vol. 7, No. 18, 01.09.2015, p. 2910-2917.Research output: Contribution to journal › Article › peer-review
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TY - JOUR
T1 - Ruthenium Clusters on Carbon Nanofibers for Formic Acid Decomposition
T2 - Effect of Doping the Support with Nitrogen
AU - Zacharska, Monika
AU - Podyacheva, Olga Yu
AU - Kibis, Lidiya S.
AU - Boronin, Andrey I.
AU - Senkovskiy, Boris V.
AU - Gerasimov, Evgeny Yu
AU - Taran, Oxana P.
AU - Ayusheev, Artemiy B.
AU - Parmon, Valentin N.
AU - Leahy, J. J.
AU - Bulushev, Dmitri A.
PY - 2015/9/1
Y1 - 2015/9/1
N2 - The catalytic properties of 1wt % Ru catalysts with the same mean Ru cluster size of 1.4-1.5nm supported on herringbone-type carbon nanofibers with different N contents were compared for H2 production from formic acid decomposition. The Ru catalyst on the support with 6.8wt % N gave a 1.5-2times higher activity for the dehydrogenation reaction (CO2, H2) than the catalyst on the undoped support. The activity in the dehydration reaction (CO, H2O) was the same. As a result, the selectivity to H2 increased significantly from 83 to 92 % with N-doping, and the activation energies for both reactions were close (55-58kJ mol-1). The improvement could be explained by the presence of Ru clusters stabilized by pyridinic N located on the open edges of the external surface of the carbon nanofibers. This N may activate formic acid by the formation of an adduct (>NH+HCOO-) followed by its dehydrogenation on the adjacent Ru clusters. Nanoparticles on nanofibers: Ru catalysts on N-doped carbon nanofibers show a higher selectivity for hydrogen production from formic acid decomposition compared to undoped samples. This is attributed to the activation of formic acid on the pyridinic sites of the support followed by dehydrogenation on adjacent Ru clusters.
AB - The catalytic properties of 1wt % Ru catalysts with the same mean Ru cluster size of 1.4-1.5nm supported on herringbone-type carbon nanofibers with different N contents were compared for H2 production from formic acid decomposition. The Ru catalyst on the support with 6.8wt % N gave a 1.5-2times higher activity for the dehydrogenation reaction (CO2, H2) than the catalyst on the undoped support. The activity in the dehydration reaction (CO, H2O) was the same. As a result, the selectivity to H2 increased significantly from 83 to 92 % with N-doping, and the activation energies for both reactions were close (55-58kJ mol-1). The improvement could be explained by the presence of Ru clusters stabilized by pyridinic N located on the open edges of the external surface of the carbon nanofibers. This N may activate formic acid by the formation of an adduct (>NH+HCOO-) followed by its dehydrogenation on the adjacent Ru clusters. Nanoparticles on nanofibers: Ru catalysts on N-doped carbon nanofibers show a higher selectivity for hydrogen production from formic acid decomposition compared to undoped samples. This is attributed to the activation of formic acid on the pyridinic sites of the support followed by dehydrogenation on adjacent Ru clusters.
KW - dehydrogenation
KW - doping
KW - hydrogen
KW - ruthenium
KW - supported catalysts
UR - http://www.scopus.com/inward/record.url?scp=84941317327&partnerID=8YFLogxK
U2 - 10.1002/cctc.201500216
DO - 10.1002/cctc.201500216
M3 - Article
AN - SCOPUS:84941317327
VL - 7
SP - 2910
EP - 2917
JO - ChemCatChem
JF - ChemCatChem
SN - 1867-3880
IS - 18
ER -
ID: 25400796