Abstract

MCM-41- and Al-MCM-41-supported nickel phosphide nanomaterials were synthesized at two different initial molar ratios of Ni/P: 10:2 and 10:3 and were tested as heterogeneous catalysts for the one-pot conversion of cellobiose to sorbitol. The catalysts were characterized by X-ray diffractometer (XRD), N2 adsorption-desorption, scanning electron microscope (SEM), transmission electron microscope (TEM), 27Al-magnetic angle spinning-nuclear magnetic resonance spectrometer (27Al MAS-NMR), temperature programmed desorption of ammonia (NH3-TPD), temperature-programmed reduction (H2-TPR), and inductively coupled plasma optical emission spectrophotometer (ICP-OES). The characterization indicated that nickel phosphide nanoparticles were successfully incorporated into both supports without destroying their hexagonal framework structures, that the catalysts contained some or all of the following Ni-containing phases: Ni0, Ni3P, and Ni12P5, and that the types and relative amounts of Ni-containing phases present in each catalyst were largely determined by the initial molar ratio of Ni/P as well as the type of support used. For cellobiose conversion at 150 °C for 3 h under 4 MPa of H2, all catalysts showed similarly high conversion of cellobiose (89.5–95.0%). Nevertheless, sorbitol yield was highly correlated to the relative amount of phases with higher content of phosphorus present in the catalysts, giving the following order of catalytic performance of the Ni-containing phases: Ni12P5 > Ni3P > Ni. Increasing the reaction temperature from 150 °C to 180 °C also led to an improvement in sorbitol yield (from 43.5% to 87.8%).

Highlights

  • The use of biomass as a renewable feedstock to produce fuels and chemicals has gained much attention due to the depletion of fossil fuels and global warming [1,2]

  • We report the synthesis and full characterization of supported nickel phosphide catalysts prepared with two different ratios of nickel to phosphorus where MCM-41 and Al-MCM-41 were used as supports in order to enhance the dispersion of nickel phosphide nanoparticles

  • The overall decrease in in catalyst performance be attributed to partial the partial leaching of amorphous nickel phosphides at catalyst performance can can be attributed to the leaching of amorphous nickel phosphides at high high temperature, which can occur following the transformation of crystalline nickel phosphides to temperature, which can occur following the transformation of crystalline nickel phosphides to their their amorphous

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Summary

Introduction

The use of biomass as a renewable feedstock to produce fuels and chemicals has gained much attention due to the depletion of fossil fuels and global warming [1,2]. Since glucose may be hydrolyzed from cellulose or cellobiose, many researches have investigated the two-step catalytic conversion of cellulose or cellobiose to sorbitol under hydrolytic hydrogenation [12,13,14,15,16]. It is of interest to develop nickel-based catalysts that contain both acidic and metallic functions in order to accomplish the one-pot hydrolytic hydrogenation for the conversion of cellulose/cellobiose to sorbitol. Due to the fact that different stoichiometric ratios of nickel to phosphorus can lead to the formation of different phases of nickel phosphides [23,24], it is of interest to investigate the bifunctional catalytic properties of different phases of nickel phosphide in the one-pot conversion of cellulose/cellobiose to sorbitol. The effect of different supports on the formation of nickel phosphide phases and on the catalytic performance was studied

Characterization of the Catalysts
27 AlTwo representative containing
The aluminum spectrum of
Catalytic Conversion of Cellobiose to Sorbitol
12 P5 phase
MPa mL
Catalytic Mechanism
Hydrolytic
Comparison of Catalytic Performance of Various Metal-Based Catalysts
Materials
Synthesis of Nickel Phosphide Nanoparticles Supported on MCM-41 and Al-MCM-41
Materials Characterization
Catalytic Cellobiose Conversion and Product Analysis
Conclusions
Full Text
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