TY - JOUR
T1 - Hydrodeoxygenation of guaiacol over carbon-supported molybdenum nitride catalysts
T2 - Effects of nitriding methods and support properties
AU - Ghampson, I. Tyrone
AU - Sepúlveda, Catherine
AU - Garcia, Rafael
AU - Radovic, Ljubisa R.
AU - Fierro, J. L.García
AU - Desisto, William J.
AU - Escalona, Nestor
N1 - Funding Information:
The authors acknowledge the financial support of DOE Epscor Grant # DE-FG02-07ER46373 and the financial support from CONICYT Chile , projects PFB-27, PIA-ACT-130 and FONDECYT No. 1100512 grants. I. Tyrone Ghampson is indebted to NSF Career Award 0547103 for sponsoring a trip to the University of Concepción. The authors also gratefully acknowledge valuable discussions on N 2 sorption with Rachel Pollock, and the technical assistance of Nick Hill and Manuel Veliz.
PY - 2012
Y1 - 2012
N2 - Molybdenum nitride catalysts supported on activated carbon materials with different textural and chemical properties were synthesized by nitriding supported Mo oxide precursors with gaseous NH 3 or N 2/H 2 mixtures using a temperature-programmed reaction. The supports and catalysts were characterized by N 2 physisorption, XRD, chemical analysis, TPD, FT-IR and XPS. Guaiacol (2-methoxyphenol) hydrodeoxygenation (HDO) activities at 5 MPa and 300 °C were evaluated in a batch autoclave reactor. Molybdenum nitrides prepared using a N 2/H 2 mixture resulted in more highly dispersed catalysts, and consequently more active catalysts, relative to those prepared using ammonolysis. The HDO activity was also related to pore size distribution and the concentration of oxygen-containing surface groups of the different carbon supports. Increased mesoporosity is argued to have facilitated the access to active sites while increased surface acidity enhanced their catalytic activity through modification of their electronic properties. The highest activity was thus attributed to the highest dispersion of the unsaturated catalyst species and the highest support mesoporosity. Surprisingly, addition of Co did not improve the HDO activity.
AB - Molybdenum nitride catalysts supported on activated carbon materials with different textural and chemical properties were synthesized by nitriding supported Mo oxide precursors with gaseous NH 3 or N 2/H 2 mixtures using a temperature-programmed reaction. The supports and catalysts were characterized by N 2 physisorption, XRD, chemical analysis, TPD, FT-IR and XPS. Guaiacol (2-methoxyphenol) hydrodeoxygenation (HDO) activities at 5 MPa and 300 °C were evaluated in a batch autoclave reactor. Molybdenum nitrides prepared using a N 2/H 2 mixture resulted in more highly dispersed catalysts, and consequently more active catalysts, relative to those prepared using ammonolysis. The HDO activity was also related to pore size distribution and the concentration of oxygen-containing surface groups of the different carbon supports. Increased mesoporosity is argued to have facilitated the access to active sites while increased surface acidity enhanced their catalytic activity through modification of their electronic properties. The highest activity was thus attributed to the highest dispersion of the unsaturated catalyst species and the highest support mesoporosity. Surprisingly, addition of Co did not improve the HDO activity.
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U2 - 10.1016/j.apcata.2012.06.047
DO - 10.1016/j.apcata.2012.06.047
M3 - Article
AN - SCOPUS:84865114104
SN - 0926-860X
VL - 439-440
SP - 111
EP - 124
JO - Applied Catalysis A: General
JF - Applied Catalysis A: General
ER -