Ruthenium Clusters on Carbon Nanofibers for Formic Acid Decomposition: Effect of Doping the Support with Nitrogen
Full article
| Общее |
Language:
Английский,
Genre:
Full article,
Status:
Published,
Source type:
Original
|
| Journal |
ChemCatChem
ISSN: 1867-3880
, E-ISSN: 1867-3899
|
| Output data |
Year: 2015,
Volume: 7,
Number: 18,
Pages: 2910-2917
Pages count
: 8
DOI:
10.1002/cctc.201500216
|
| Tags |
dehydrogenation, doping, hydrogen, ruthenium, supported catalysts |
| Authors |
Zacharska Monika
1,2
,
Podyacheva Olga Yu.
3,4
,
Kibis Lidiya S.
3,4
,
Boronin Andrey I.
3,4
,
Senkovskii Boris V.
5,6
,
Gerasimov Evgeny Yu.
3
,
Taran Oxana P.
3
,
Ayusheev Artemiy B.
3
,
Parmon Valentin N.
3,4
,
Leahy J. J.
1,2
,
Bulushev Dmitri A.
1,3,4
|
| Affiliations |
| 1 |
Chemical & Environmental Sciences Department University of Limerick (Ireland)
|
| 2 |
Materials & Surface Science Institute University of Limerick (Ireland)
|
| 3 |
Boreskov Institute of Catalysis SB RAS Novosibirsk 630090 (Russia)
|
| 4 |
Novosibirsk State University Novosibirsk 630090 (Russia)
|
| 5 |
Dresden University of Technology 01062 Dresden (Germany)
|
| 6 |
St. Petersburg State University 198504 St. Petersburg (Russia)
|
|
Funding (4)
|
1
|
Science Foundation Ireland
|
06/CP/E007
|
|
2
|
European Commission
|
|
|
3
|
The Ministry of Education and Science of the Russian Federation
|
|
|
4
|
Higher Education Authority
|
|
The catalytic properties of 1 wt % Ru catalysts with the same mean Ru cluster size of 1.4–1.5 nm 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 6.8 wt % N gave a 1.5–2 times 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 (55–58 kJ 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.