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Intermetallic PdZn nanoparticles catalyze the continuous-flow hydrogenation of alkynols to cis-enols
Designing highly active and stable lead-free palladium-based catalysts without introducing surfactants and stabilizers is vital for large-scale and high-efficiency manufacturing of cis-enols via continuous-flow semi-hydrogenation of alkynols. Herein, we report an intermetallic PdZn/ZnO catalyst, des...
Autores principales: | , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2021
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9814770/ https://www.ncbi.nlm.nih.gov/pubmed/36697793 http://dx.doi.org/10.1038/s42004-021-00612-0 |
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author | Chen, Xiao Shi, Chuang Wang, Xing-Bao Li, Wen-Ying Liang, Changhai |
author_facet | Chen, Xiao Shi, Chuang Wang, Xing-Bao Li, Wen-Ying Liang, Changhai |
author_sort | Chen, Xiao |
collection | PubMed |
description | Designing highly active and stable lead-free palladium-based catalysts without introducing surfactants and stabilizers is vital for large-scale and high-efficiency manufacturing of cis-enols via continuous-flow semi-hydrogenation of alkynols. Herein, we report an intermetallic PdZn/ZnO catalyst, designed by using the coupling strategy of strong electrostatic adsorption and reactive metal-support interaction, which can be used as a credible alternative to the commercial PdAg/Al(2)O(3) and Lindlar catalysts. Intermetallic PdZn nanoparticles with electron-poor active sites on a Pd/ZnO catalyst significantly boost the thermodynamic selectivity with respect to the mechanistic selectivity and therefore enhance the selectivity towards cis-enols. Based on in situ diffuse reflectance infrared Fourier-transform spectra as well as simulations, we identify that the preferential adsorption of alkynol over enol on PdZn nanoparticles suppresses the over-hydrogenation of enols. These results suggest the application of fine surface engineering technology in oxide-supported metal (particles) could tune the ensemble and ligand effects of metallic active sites and achieve directional hydrogenation in fine chemical synthesis. |
format | Online Article Text |
id | pubmed-9814770 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2021 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
spelling | pubmed-98147702023-01-10 Intermetallic PdZn nanoparticles catalyze the continuous-flow hydrogenation of alkynols to cis-enols Chen, Xiao Shi, Chuang Wang, Xing-Bao Li, Wen-Ying Liang, Changhai Commun Chem Article Designing highly active and stable lead-free palladium-based catalysts without introducing surfactants and stabilizers is vital for large-scale and high-efficiency manufacturing of cis-enols via continuous-flow semi-hydrogenation of alkynols. Herein, we report an intermetallic PdZn/ZnO catalyst, designed by using the coupling strategy of strong electrostatic adsorption and reactive metal-support interaction, which can be used as a credible alternative to the commercial PdAg/Al(2)O(3) and Lindlar catalysts. Intermetallic PdZn nanoparticles with electron-poor active sites on a Pd/ZnO catalyst significantly boost the thermodynamic selectivity with respect to the mechanistic selectivity and therefore enhance the selectivity towards cis-enols. Based on in situ diffuse reflectance infrared Fourier-transform spectra as well as simulations, we identify that the preferential adsorption of alkynol over enol on PdZn nanoparticles suppresses the over-hydrogenation of enols. These results suggest the application of fine surface engineering technology in oxide-supported metal (particles) could tune the ensemble and ligand effects of metallic active sites and achieve directional hydrogenation in fine chemical synthesis. Nature Publishing Group UK 2021-12-13 /pmc/articles/PMC9814770/ /pubmed/36697793 http://dx.doi.org/10.1038/s42004-021-00612-0 Text en © The Author(s) 2021 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) . |
spellingShingle | Article Chen, Xiao Shi, Chuang Wang, Xing-Bao Li, Wen-Ying Liang, Changhai Intermetallic PdZn nanoparticles catalyze the continuous-flow hydrogenation of alkynols to cis-enols |
title | Intermetallic PdZn nanoparticles catalyze the continuous-flow hydrogenation of alkynols to cis-enols |
title_full | Intermetallic PdZn nanoparticles catalyze the continuous-flow hydrogenation of alkynols to cis-enols |
title_fullStr | Intermetallic PdZn nanoparticles catalyze the continuous-flow hydrogenation of alkynols to cis-enols |
title_full_unstemmed | Intermetallic PdZn nanoparticles catalyze the continuous-flow hydrogenation of alkynols to cis-enols |
title_short | Intermetallic PdZn nanoparticles catalyze the continuous-flow hydrogenation of alkynols to cis-enols |
title_sort | intermetallic pdzn nanoparticles catalyze the continuous-flow hydrogenation of alkynols to cis-enols |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9814770/ https://www.ncbi.nlm.nih.gov/pubmed/36697793 http://dx.doi.org/10.1038/s42004-021-00612-0 |
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