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Hydrogenolysis of glycerol over TiO₂-supported Pt-WO_x catalysts: Effects of the TiO₂ crystal phase and WO_x loading.

ABSTRACT: The selective hydrogenolysis of glycerol to 1,3-propanediol (1,3-PDO) with high added value is attraction but challenging. Pt-WO_x-based catalysts have been extensively studied in the selective hydrogenolysis of glycerol. The catalyst support and the physicochemical state of WO_x play important roles on this reaction. In this paper, Pt-WO_x catalysts supported on TiO₂ with different crystal forms were prepared and studied for their catalytic performance in hydrogenolysis of glycerol. It was observed that the catalytic performance of anatase-type (A-type) TiO₂-supported catalyst (Pt/W/A-Ti) is much better than that of the rutile-type (R-type) TiO₂ catalyst (Pt/W/R-Ti) due to its higher stability. Furthermore, the influence of W loading amount and state were thoroughly investigated for the Pt/W/A-Ti catalysts, and Pt/W/A-TiO₂ with 5 wt% loading of WO_x achieved the best catalytic performance (100% conversion of glycerol and 41% yield of 1,3-PDO under the optimal reaction conditions), owing to the suitable WO_x domains and high dispersion of W species, as evidenced by XRD patterns and TEM images. Mechanism study by in-situ DRIFTS experiments indicated that glycerol was first converted to 3-hydroxypropanal and then converted to 1,3-PDO through subsequent reactions.

SUBMITTER: Wang Y

PROVIDER: S-EPMC9532750 | biostudies-literature | 2022

REPOSITORIES: biostudies-literature

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Hydrogenolysis of glycerol over TiO2-supported Pt-WOx catalysts: Effects of the TiO2 crystal phase and WOx loading.

Wang Yaju Y Zhou Zhiming Z Wang Chao C Zhao Leihong L Xia Qineng Q

Frontiers in chemistry 20220921

The selective hydrogenolysis of glycerol to 1,3-propanediol (1,3-PDO) with high added value is attraction but challenging. Pt-WOx-based catalysts have been extensively studied in the selective hydrogenolysis of glycerol. The catalyst support and the physicochemical state of WOx play important roles on this reaction. In this paper, Pt-WOx catalysts supported on TiO2 with different crystal forms were prepared and studied for their catalytic performance i ...[more]

PMID: 36212063

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Project description:Biodiesel is of high interest due to increased demand for energy with the concern regarding more sustainable production processes. However, an inevitable by-product is glycerol. Hence, the conversion of this by-product to higher-value chemicals, especially 1,3-propanediol (1,3-PDO) via glycerol hydrogenolysis reaction, is one of the most effective pathways towards a profitable process. In general, this process is catalyzed by a highly active Pt-based catalyst supported on γ-Al2O3. However, its low 1,3-PDO selectivity and stability due to surface deactivation of such catalysts remained. This led to the surface modification by WOx to improve both the selectivity by means of the increased Brønsted acidity and the stability in terms of Pt leaching-resistance. Hence, we applied experimental and density functional theory (DFT)-based techniques to study the fundamentals of how WOx modified the catalytic performance in the Pt/γ-Al2O3 catalyst and provided design guidelines. The effects of WOx promoter on improved activity were due to the shifting of the total density of states towards the antibonding region evident by the total density of states (TDOS) profile. On the improved 1,3-PDO selectivity, the main reason was the increasing number of Brønsted acid sites due to the added WOx promoter. Interestingly, the stability improvement was due to the strong metal-support interaction (SMSI) that occurred in the catalyst, like typical high leaching-resistant catalysts. Also, the observed strong metal-support-promoter interaction (SMSPI) is an additional effect preventing leaching. The SMSPI stemmed from additional bonding between the WOx species and the Pt active site, which significantly strengthened Pt adsorption to support and a high electron transfer from both Pt and Al2O3 to WOx promoter. This suggested that the promising promoter for our reaction performed in the liquid phase would improve the stability if SMSI occurred, where the special case of the WOx promoter would even highly improve the stability through SMSPI. Nevertheless, various promoters that can promote SMSPI need investigations.

Dataset Information

Hydrogenolysis of glycerol over TiO₂-supported Pt-WO_x catalysts: Effects of the TiO₂ crystal phase and WO_x loading.

Publications

Hydrogenolysis of glycerol over TiO<sub>2</sub>-supported Pt-WO<sub>x</sub> catalysts: Effects of the TiO<sub>2</sub> crystal phase and WO<sub>x</sub> loading.

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