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II International Symposium on Carbon for Catalysis ABSTRACTS

II International Symposium on Carbon for Catalysis ABSTRACTS

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PP-I-19<br />

SOME REGULARITIES OF THE PREPARATION OF N-CONTAINING<br />

CATALYTIC FILAMENTOUS CARBON BY PYRIDINE DECOMPOSITION<br />

Ilinich G.N., Romanenko A.V., Salanov A.N., Titkov A.I., Likholobov V.A. 1<br />

Boreskov Institute of <strong>Catalysis</strong> SB RAS, Novosibirsk, Russia<br />

1 Institute of Hydrocarb<strong>on</strong>s Processing SB RAS, Omsk, Russia<br />

e-mail: ig@catalysis.nsk.su<br />

Nitrogen c<strong>on</strong>taining catalytic filamentous carb<strong>on</strong>s (N-CFCs) is a new type of carb<strong>on</strong><br />

materials. N-CFCs have great importance, primarily, as promising catalyst supports. The<br />

synthesis of these carb<strong>on</strong>s with the predetermined properties is complex process because of<br />

variety of reacti<strong>on</strong>s occurring in the gas phase, <strong>on</strong> the catalyst surface and <strong>on</strong> the newborn<br />

N-CFC filament itself. In this work we revealed some factors defining the yield, texture and<br />

chemical compositi<strong>on</strong> of the N-CFCs prepared by depositi<strong>on</strong> of gaseous mixtures of pyridine<br />

(C 5 H 5 N, Py) with H 2 or Ar over NiCu/Al 2 O 3 catalyst (Ni - 64 wt %, Cu – 4 wt %) at<br />

550-800 o C [1, 2].<br />

Table data show the Py decompositi<strong>on</strong> in the presence of H 2 at 750 o C provides the<br />

maximum N-CFC yield (sample № 4). In case of Py/Ar the yield of carb<strong>on</strong> decreases more<br />

than by an order (sample № 6).<br />

Reacti<strong>on</strong> c<strong>on</strong>diti<strong>on</strong>s 1)<br />

N-CFC<br />

№ Т, о С<br />

mixture 2)<br />

yield,<br />

Time, h<br />

compositi<strong>on</strong> 3) Oligomers<br />

g/g (Ni+Cu)<br />

1 550 Ру/Н 2 4,50 33 NC 104 H 13 -<br />

2 650 4,50 42 NC 56 H 6 -<br />

3 700 4,50 50 NC 46 H 5 -<br />

4 750 4,50 73 NC (32-38) H 3 +<br />

5 800 2,25 26 NC 33 H 0,7 ++<br />

6 750 Py/Ar 4,50 5 NC 18 H 1,4 -<br />

1) 0.05 g of the catalyst, atmospheric pressure and flow rate of mixture ~ 6 l/h; 2) [Py] = 10 %, mol; 3) elemental<br />

analysis data.<br />

We have c<strong>on</strong>cluded that the stage of Py hydrodenitrificati<strong>on</strong> (HDN) catalyzed by Ni<br />

precedes the N-CFC <strong>for</strong>mati<strong>on</strong> in Ру/H 2 mixture. The carb<strong>on</strong> fragments are <strong>for</strong>med by<br />

decompositi<strong>on</strong> of HDN products, supposedly of C 5 -hydrocarb<strong>on</strong>s. As a c<strong>on</strong>sequence, such<br />

carb<strong>on</strong>s have a lower c<strong>on</strong>tent of nitrogen in comparis<strong>on</strong> with N-CFC, prepared of Py/Ar<br />

mixtures. High catalyst activity in N-CFC <strong>for</strong>mati<strong>on</strong> is explained by lower binding energies in<br />

the molecules of C 5 -hydrocarb<strong>on</strong>s in comparis<strong>on</strong> with the <strong>on</strong>es in molecule of pyridine itself.<br />

156

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