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An active and stable multifunctional catalyst with defective UiO-66 as a support for Pd over the continuous catalytic conversion of acetone and hydrogen
The one-pot synthesis of methyl isobutyl ketone (MIBK) and methyl isobutyl methanol (MIBC) from acetone and hydrogen is a typical cascade reaction comprised of aldol condensation-dehydration-hydrogenation. Pd loss and aggregation during long term operation are typical problems in industrial applicat...
Autores principales: | , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
The Royal Society of Chemistry
2020
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8690181/ https://www.ncbi.nlm.nih.gov/pubmed/35423013 http://dx.doi.org/10.1039/d0ra09217g |
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author | Hu, Yingjie Mei, Yuxin Lin, Baining Du, Xuhong Xu, Fan Xie, Huasheng Wang, Kang Zhou, Yonghua |
author_facet | Hu, Yingjie Mei, Yuxin Lin, Baining Du, Xuhong Xu, Fan Xie, Huasheng Wang, Kang Zhou, Yonghua |
author_sort | Hu, Yingjie |
collection | PubMed |
description | The one-pot synthesis of methyl isobutyl ketone (MIBK) and methyl isobutyl methanol (MIBC) from acetone and hydrogen is a typical cascade reaction comprised of aldol condensation-dehydration-hydrogenation. Pd loss and aggregation during long term operation are typical problems in industrial application. In this paper, an active and stable catalyst was achieved with defective UiO-66 as a support for Pd, which was synthesized with the ratio 15 : 1 of ZrOCl(2)·8H(2)O to ZrCl(4) as Zr-precursors. The resultant Pd catalyst remained active for at least 1000 h with a MIBK + MIBC selectivity of 84.87–93.09% and acetone conversion of 45.26–53.22% in a continuous trickle-bed reactor. Besides the increased Brønsted acid amount generated by the defect sites was favorable for the activity, the cavity confinement in the UiO-66 (R = 15 : 1) structure also efficiently prevented Pd loss and aggregation during the long term run. The contrast of the characterization of the fresh and used Pd/UiO-66 (R = 15 : 1) indicated that the deactivation of the catalyst was attributed to carbonaceous accumulation on the catalyst surface, which could be easily regenerated by calcination. This work supplied a new alternative for the design and utilization of industrial catalysts for MIBK and MIBC synthesis. |
format | Online Article Text |
id | pubmed-8690181 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2020 |
publisher | The Royal Society of Chemistry |
record_format | MEDLINE/PubMed |
spelling | pubmed-86901812022-04-13 An active and stable multifunctional catalyst with defective UiO-66 as a support for Pd over the continuous catalytic conversion of acetone and hydrogen Hu, Yingjie Mei, Yuxin Lin, Baining Du, Xuhong Xu, Fan Xie, Huasheng Wang, Kang Zhou, Yonghua RSC Adv Chemistry The one-pot synthesis of methyl isobutyl ketone (MIBK) and methyl isobutyl methanol (MIBC) from acetone and hydrogen is a typical cascade reaction comprised of aldol condensation-dehydration-hydrogenation. Pd loss and aggregation during long term operation are typical problems in industrial application. In this paper, an active and stable catalyst was achieved with defective UiO-66 as a support for Pd, which was synthesized with the ratio 15 : 1 of ZrOCl(2)·8H(2)O to ZrCl(4) as Zr-precursors. The resultant Pd catalyst remained active for at least 1000 h with a MIBK + MIBC selectivity of 84.87–93.09% and acetone conversion of 45.26–53.22% in a continuous trickle-bed reactor. Besides the increased Brønsted acid amount generated by the defect sites was favorable for the activity, the cavity confinement in the UiO-66 (R = 15 : 1) structure also efficiently prevented Pd loss and aggregation during the long term run. The contrast of the characterization of the fresh and used Pd/UiO-66 (R = 15 : 1) indicated that the deactivation of the catalyst was attributed to carbonaceous accumulation on the catalyst surface, which could be easily regenerated by calcination. This work supplied a new alternative for the design and utilization of industrial catalysts for MIBK and MIBC synthesis. The Royal Society of Chemistry 2020-12-21 /pmc/articles/PMC8690181/ /pubmed/35423013 http://dx.doi.org/10.1039/d0ra09217g Text en This journal is © The Royal Society of Chemistry https://creativecommons.org/licenses/by-nc/3.0/ |
spellingShingle | Chemistry Hu, Yingjie Mei, Yuxin Lin, Baining Du, Xuhong Xu, Fan Xie, Huasheng Wang, Kang Zhou, Yonghua An active and stable multifunctional catalyst with defective UiO-66 as a support for Pd over the continuous catalytic conversion of acetone and hydrogen |
title | An active and stable multifunctional catalyst with defective UiO-66 as a support for Pd over the continuous catalytic conversion of acetone and hydrogen |
title_full | An active and stable multifunctional catalyst with defective UiO-66 as a support for Pd over the continuous catalytic conversion of acetone and hydrogen |
title_fullStr | An active and stable multifunctional catalyst with defective UiO-66 as a support for Pd over the continuous catalytic conversion of acetone and hydrogen |
title_full_unstemmed | An active and stable multifunctional catalyst with defective UiO-66 as a support for Pd over the continuous catalytic conversion of acetone and hydrogen |
title_short | An active and stable multifunctional catalyst with defective UiO-66 as a support for Pd over the continuous catalytic conversion of acetone and hydrogen |
title_sort | active and stable multifunctional catalyst with defective uio-66 as a support for pd over the continuous catalytic conversion of acetone and hydrogen |
topic | Chemistry |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8690181/ https://www.ncbi.nlm.nih.gov/pubmed/35423013 http://dx.doi.org/10.1039/d0ra09217g |
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