Experimental and computational study on roles of WOx promoting strong metal support promoter interaction in Pt catalysts during glycerol hydrogenolysis

Abstract 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 glyc...

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Autores principales:	Tinnakorn Saelee, Poonnapa Limsoonthakul, Phakaorn Aphichoksiri, Meena Rittiruam, Mongkol Lerdpongsiripaisarn, Takanori Miyake, Hiromi Yamashita, Kohsuke Mori, Yasutaka Kuwahara, Supareak Praserthdam, Piyasan Praserthdam
Formato:	article
Lenguaje:	EN
Publicado:	Nature Portfolio 2021
Materias:	Medicine R Science Q
Acceso en línea:	https://doaj.org/article/2ccde92897164eac837948f6b156c374
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spelling	oai:doaj.org-article:2ccde92897164eac837948f6b156c3742021-12-02T14:01:20ZExperimental and computational study on roles of WOx promoting strong metal support promoter interaction in Pt catalysts during glycerol hydrogenolysis10.1038/s41598-020-79764-32045-2322https://doaj.org/article/2ccde92897164eac837948f6b156c3742021-01-01T00:00:00Zhttps://doi.org/10.1038/s41598-020-79764-3https://doaj.org/toc/2045-2322Abstract 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.Tinnakorn SaeleePoonnapa LimsoonthakulPhakaorn AphichoksiriMeena RittiruamMongkol LerdpongsiripaisarnTakanori MiyakeHiromi YamashitaKohsuke MoriYasutaka KuwaharaSupareak PraserthdamPiyasan PraserthdamNature PortfolioarticleMedicineRScienceQENScientific Reports, Vol 11, Iss 1, Pp 1-12 (2021)
institution	DOAJ
collection	DOAJ
language	EN
topic	Medicine R Science Q
spellingShingle	Medicine R Science Q Tinnakorn Saelee Poonnapa Limsoonthakul Phakaorn Aphichoksiri Meena Rittiruam Mongkol Lerdpongsiripaisarn Takanori Miyake Hiromi Yamashita Kohsuke Mori Yasutaka Kuwahara Supareak Praserthdam Piyasan Praserthdam Experimental and computational study on roles of WOx promoting strong metal support promoter interaction in Pt catalysts during glycerol hydrogenolysis
description	Abstract 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.
format	article
author	Tinnakorn Saelee Poonnapa Limsoonthakul Phakaorn Aphichoksiri Meena Rittiruam Mongkol Lerdpongsiripaisarn Takanori Miyake Hiromi Yamashita Kohsuke Mori Yasutaka Kuwahara Supareak Praserthdam Piyasan Praserthdam
author_facet	Tinnakorn Saelee Poonnapa Limsoonthakul Phakaorn Aphichoksiri Meena Rittiruam Mongkol Lerdpongsiripaisarn Takanori Miyake Hiromi Yamashita Kohsuke Mori Yasutaka Kuwahara Supareak Praserthdam Piyasan Praserthdam
author_sort	Tinnakorn Saelee
title	Experimental and computational study on roles of WOx promoting strong metal support promoter interaction in Pt catalysts during glycerol hydrogenolysis
title_short	Experimental and computational study on roles of WOx promoting strong metal support promoter interaction in Pt catalysts during glycerol hydrogenolysis
title_full	Experimental and computational study on roles of WOx promoting strong metal support promoter interaction in Pt catalysts during glycerol hydrogenolysis
title_fullStr	Experimental and computational study on roles of WOx promoting strong metal support promoter interaction in Pt catalysts during glycerol hydrogenolysis
title_full_unstemmed	Experimental and computational study on roles of WOx promoting strong metal support promoter interaction in Pt catalysts during glycerol hydrogenolysis
title_sort	experimental and computational study on roles of wox promoting strong metal support promoter interaction in pt catalysts during glycerol hydrogenolysis
publisher	Nature Portfolio
publishDate	2021
url	https://doaj.org/article/2ccde92897164eac837948f6b156c374
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Experimental and computational study on roles of WOx promoting strong metal support promoter interaction in Pt catalysts during glycerol hydrogenolysis

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