Nanoparticulate Pt on mesoporous SBA-15 doped with extremely low amount of W as a highly selective catalyst for glycerol hydrogenolysis to 1,3-propanediol
It has been documented that W-modified Pt catalysts with relatively high tungsten contents are effective for the catalytic transformation of biodiesel-derived glycerol to 1,3-propanediol (1,3-PDO). Herein, we report a new finding that Pt/W-SBA-15 catalysts with extremely low W/Si atomic ratios ( les...
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Published in | Green chemistry : an international journal and green chemistry resource : GC Vol. 19; no. 9; pp. 2174 - 2183 |
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Main Authors | , , , , , , , , , , |
Format | Journal Article |
Language | English |
Published |
2017
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Subjects | |
Online Access | Get full text |
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Summary: | It has been documented that W-modified Pt catalysts with relatively high tungsten contents are effective for the catalytic transformation of biodiesel-derived glycerol to 1,3-propanediol (1,3-PDO). Herein, we report a new finding that Pt/W-SBA-15 catalysts with extremely low W/Si atomic ratios ( less than or equal to 1/80) exhibit excellent catalytic performance in the hydrogenolysis of glycerol to 1,3-PDO. In particular, a Pt/W-SBA-15 catalyst with the W/Si ratio of as low as 1/640 (Pt/W-SBA-15(1/640)) gave rise to the highest 1,3-PDO selectivity of 70.8% at a high glycerol conversion of 86.8% and thus afforded the highest yield of 1,3-PDO of 61.5%. A combination of characterization techniques evidenced that tungsten was homogeneously incorporated into SBA-15 in the form of isolated tetragonal WO4 and only displayed Lewis acidity. The particle size of Pt evolved in a reverse volcanic curve with the W/Si ratio, with the smallest size being observed for Pt/W-SBA-15(1/640). Control experiments indicated strong synergy between Pt nanoparticles (NPs) and WO4 in the hydrogenolysis of glycerol. A probe reaction suggested that Broensted acid sites were generated in situ on the Pt/W-SBA-15 catalysts in a H2 atmosphere by the reaction between WO4 and spillover H atoms from the Pt NPs. It is plausible that the hydrided WO4 functioned as a highly selective active centre in the hydrogenolysis of glycerol to 1,3-PDO, whereas the Pt NPs played the role of a reservoir of spillover H atoms. Thus, a good match between the isolated WO4 and the small Pt NPs was responsible for the superior catalytic performance of Pt/W-SBA-15(1/640). |
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Bibliography: | ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 23 |
ISSN: | 1463-9262 1463-9270 |
DOI: | 10.1039/c7gc00317j |