Abstract
Zr-doped mesoporous silicas with different textural parameters have been synthesized in the presence of structure-modifying agents, and then characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), N2 adsorption-desorption at −196 °C, NH3 thermoprogrammed desorption (NH3–TPD), CO2 thermoprogrammed desorption (CO2–TPD), and X-ray photoelectron spectroscopy (XPS). These porous materials were evaluated in the furfural hydrogenation through the Meerwein-Ponndorf-Verley (MPV) reaction. The catalytic results indicate that the catalyst synthesized under hydrothermal conditions and adding a pore expander agent is more active and selective to furfuryl alcohol. However, the Zr-doped porous silica catalysts that were synthesized at room temperature, which possess narrow pore sizes, tend to form i-propyl furfuryl and difurfuryl ethers, coming from etherification between furfuryl alcohol (FOL) and isopropanol molecules (used as H-donor) by a SN2 mechanism.
Highlights
The depletion of fossil fuels has generated a need to look for alternative renewable resources to satisfy the world energetic demand
To FUR conversion, catalysts prepared at room temperature display the same selectivity pattern, since the furfuryl alcohol (FOL) yield is negligible, while the i-propyl furfuryl ether (i-PFE) yield is in the range 43–51% and the difurfuryl ether (DFE) yield is between 17–22%
Zr-doped porous silicas have been synthesized by the sol-gel method
Summary
The depletion of fossil fuels has generated a need to look for alternative renewable resources to satisfy the world energetic demand. IItniotnhsi.s sInentshe,isit sheanssper, eivtiohuasslypbreevnioruesployrtbeeden thraetpthoretemdictehlaletstohfePm-1i2c3e,llueseodf aPs-t1e2m3,pulasteed, inastetreamctpedlatwe,ithinatedrjaaccteendt mwitchellaedsjacternotomitceemllepseraatturoreo,m leatedminpgetroattuhree,tylepaicdainl gpatroaltlheel mtyepsioccahl apnanraelsleol fmtheesoScBhAan-1n5elsstroufcthuereS, BinAte-1rc5osntnruectuedreb, eintwteerecnontnhecmted bybmetwicreoecnhtahnenmelsb,ywmhicrhofcahcainlintaetlesd, wthheicdhifffaucsiiloitnataeldonthgethdeifpfuosrioounsasltornugcttuhree p[6o1r]o.uIsnstthreucctausreeo[f61th].eIn the case of the Zr-doped silicas synthesized under hydrothermal conditions, the interaction between adjacent micelles diminishes The XPS data suggests that Zr alkoxides suffer a faster hydrolysis rate than Si alkoxides, in such a way that a high proportion of Zr is incorporated into the inner regions of silica, decreasing the amount of surface Zr species These data are in agreement with those previously reported in the literature, where the study of a Zr-doped mesoporous MCM-41 silica by XPS, after different times of Ar+ sputtering, allowed the observance of an enrichment of Zr from the outer to inner regions of this mesoporous material [63].
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