Tuning the acid/metal balance of carbon nanofiber-supported nickel catalysts for hydrolytic hydrogenation of cellulose.
Carbon nanofibers (CNFs) are a class of graphitic support materials with considerable potential for catalytic conversion of biomass. Earlier, we demonstrated the hydrolytic hydrogenation of cellulose over reshaped nickel particles attached at the tip of CNFs. The aim of this follow-up study was to find a relationship between the acid/metal balance of the Ni/CNFs and their performance in the catalytic conversion of cellulose. After oxidation and incipient wetness impregnation with Ni, the Ni/CNFs were characterized by various analytical methods. To prepare a selective Ni/CNF catalyst, the influences of the nature of oxidation agent, Ni activation, and Ni loading were investigated. Under the applied reaction conditions, the best result, that is, 76 % yield in hexitols with 69 % sorbitol selectivity at 93 % conversion of cellulose, was obtained on a 7.5 wt % Ni/CNF catalyst prepared by chemical vapor deposition of CH(4) on a Ni/γ-Al(2)O(3) catalyst, followed by oxidation in HNO(3) (twice for 1 h at 383 K), incipient wetness impregnation, and reduction at 773 K under H(2). This preparation method leads to a properly balanced Ni/CNF catalyst in terms of Ni dispersion and hydrogenation capacity on the one hand, and the number of acidic surface-oxygen groups responsible for the acid-catalyzed hydrolysis on the other.
Centre for Surface Chemistry and Catalysis, Katholieke Universiteit Leuven, Kasteelpark Arenberg 23, 3001 Heverlee, Belgium.
Stijn
S
Van de Vyver
Jan
J
Geboers
Wouter
W
Schutyser
Michiel
M
Dusselier
Pierre
P
Eloy
Emmie
E
Dornez
Jin Won
JW
Seo
Christophe M
CM
Courtin
Eric M
EM
Gaigneaux
Pierre A
PA
Jacobs
Bert F
BF
Sels
D002244:Carbon / Q000737:chemistry*; D002384:Catalysis; D002482:Cellulose / Q000737:chemistry*; D006863:Hydrogen-Ion Concentration; D006865:Hydrogenation; D006868:Hydrolysis; D057139:Nanofibers / Q000737:chemistry*; D009532:Nickel / Q000737:chemistry*; D010084:Oxidation-Reduction; D013696:Temperature; D014835:Volatilization
D002244:Carbon; D009532:Nickel; D002482:Cellulose