Cargando…

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...

Descripción completa

Detalles Bibliográficos
Autores principales: Hu, Yingjie, Mei, Yuxin, Lin, Baining, Du, Xuhong, Xu, Fan, Xie, Huasheng, Wang, Kang, Zhou, Yonghua
Formato: Online Artículo Texto
Lenguaje:English
Publicado: The Royal Society of Chemistry 2020
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
_version_ 1784618615986716672
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
work_keys_str_mv AT huyingjie anactiveandstablemultifunctionalcatalystwithdefectiveuio66asasupportforpdoverthecontinuouscatalyticconversionofacetoneandhydrogen
AT meiyuxin anactiveandstablemultifunctionalcatalystwithdefectiveuio66asasupportforpdoverthecontinuouscatalyticconversionofacetoneandhydrogen
AT linbaining anactiveandstablemultifunctionalcatalystwithdefectiveuio66asasupportforpdoverthecontinuouscatalyticconversionofacetoneandhydrogen
AT duxuhong anactiveandstablemultifunctionalcatalystwithdefectiveuio66asasupportforpdoverthecontinuouscatalyticconversionofacetoneandhydrogen
AT xufan anactiveandstablemultifunctionalcatalystwithdefectiveuio66asasupportforpdoverthecontinuouscatalyticconversionofacetoneandhydrogen
AT xiehuasheng anactiveandstablemultifunctionalcatalystwithdefectiveuio66asasupportforpdoverthecontinuouscatalyticconversionofacetoneandhydrogen
AT wangkang anactiveandstablemultifunctionalcatalystwithdefectiveuio66asasupportforpdoverthecontinuouscatalyticconversionofacetoneandhydrogen
AT zhouyonghua anactiveandstablemultifunctionalcatalystwithdefectiveuio66asasupportforpdoverthecontinuouscatalyticconversionofacetoneandhydrogen
AT huyingjie activeandstablemultifunctionalcatalystwithdefectiveuio66asasupportforpdoverthecontinuouscatalyticconversionofacetoneandhydrogen
AT meiyuxin activeandstablemultifunctionalcatalystwithdefectiveuio66asasupportforpdoverthecontinuouscatalyticconversionofacetoneandhydrogen
AT linbaining activeandstablemultifunctionalcatalystwithdefectiveuio66asasupportforpdoverthecontinuouscatalyticconversionofacetoneandhydrogen
AT duxuhong activeandstablemultifunctionalcatalystwithdefectiveuio66asasupportforpdoverthecontinuouscatalyticconversionofacetoneandhydrogen
AT xufan activeandstablemultifunctionalcatalystwithdefectiveuio66asasupportforpdoverthecontinuouscatalyticconversionofacetoneandhydrogen
AT xiehuasheng activeandstablemultifunctionalcatalystwithdefectiveuio66asasupportforpdoverthecontinuouscatalyticconversionofacetoneandhydrogen
AT wangkang activeandstablemultifunctionalcatalystwithdefectiveuio66asasupportforpdoverthecontinuouscatalyticconversionofacetoneandhydrogen
AT zhouyonghua activeandstablemultifunctionalcatalystwithdefectiveuio66asasupportforpdoverthecontinuouscatalyticconversionofacetoneandhydrogen