Journal
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
Volume 9, Issue 16, Pages 5705-5715Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.1c00880
Keywords
gold additive; promoter; glycerol; 1,3-PDO; Pt-W catalyst
Categories
Funding
- National Key R&D Program of China [2018YFB1501602]
- National Natural Science Foundation of China [21690080, 21690084, 21673228, 21721004, 21878289]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDB17020100, XDA21060203]
- Dalian National Laboratory for the Clean Energy (DNL) Cooperation Fund, the CAS [DNL 180303]
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The study introduces a new catalyst for the selective hydrogenolysis of glycerol to 1,3-propanediol. The catalyst was found to increase the 1,3-PDO selectivity by generating Bronsted acid sites at the interface between Pt and WOx.
The selective hydrogenolysis of glycerol to 1,3-propanediol (1,3-PDO) is an important yet challenging reaction because it requires the selective cleavage of the sterically hindered secondary C-O bond of glycerol. In this work, we have developed a new catalyst, 0.1Au-2Pt/7.5W/Al, which affords both high glycerol conversion (77.5%) and 1,3-PDO selectivity (54.8%), which are significantly higher than the Au-free counterpart. HAADF-STEM reveals that the structure of 0.1Au-2Pt/7.5W/Al is characterized with similar to 2 nm Pt NPs decorated with Au-WOx at the periphery, where the Au additive exists most likely as single atoms. Chemisorption and XPS show that the electron transfer from W to Au can help to weaken the strong metal support interaction (SMSI) between Pt and WOx, and thus greatly enlarges the exposed Pt surface and increases the H-spillover capacity. The 2-butanol dehydration in H-2 reveals that the H-spillover capacity is proportional to the number of Bronsted acid sites, which, in conjunction with the only water desorption in H-2-TPD results, strongly suggests that the active sites for breaking the secondary C-O bond of glycerol should be Bronsted acid sites generated by the H-spillover at the interface between Pt and WOx, and the modification by the Au additive increases the number of interfacial sites, and thus enhances the 1,3-PDO yield.
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