Process intensification of alkynol semihydrogenation in a tube reactor coated with a Pd/ZnO catalyst

Abstract

Semihydrogenation of 2-methyl-3-butyn-2-ol (MBY) was studied in a 5 m tube reactor wall-coated with a 5 wt % Pd/ZnO catalyst. The system allowed for the excellent selectivity towards the intermediate alkene of 97.8 ± 0.2% at an ambient H 2 pressure and a MBY conversion below 90%. The maximum alkene yield reached 94.6% under solvent-free conditions and 96.0% in a 30 vol % MBY aqueous solution. The reactor stability was studied for 80 h on stream with a deactivation rate of only 0.07% per hour. Such a low deactivation rate provides a continuous operation of one month with only a two-fold decrease in catalyst activity and a metal leaching below 1 parts per billion (ppb). The excellent turn-over numbers (TON) of above 10 5 illustrates a very efficient utilisation of the noble metal inside catalyst-coated tube reactors. When compared to batch operation at 70 °C, the reaction rate in flow reactor can be increased by eight times at a higher reaction temperature, keeping the same product decomposition of about 1% in both cases.

Publication DOI: https://doi.org/10.3390/catal7120358
Divisions: College of Engineering & Physical Sciences
College of Engineering & Physical Sciences > School of Infrastructure and Sustainable Engineering > Chemical Engineering & Applied Chemistry
College of Engineering & Physical Sciences > Energy and Bioproducts Research Institute (EBRI)
Funding Information: The continuous flow hydrogenation allows for a significant process intensification by increasing  The continuous flow hydrogenation allows for a significant process intensification by increasing the process temperature by 90 ◦°C above that used in a conventional batch reactor with a minimum  the process temperature by 90 C above that used in a conventional batch reactor with a minimum substrate decomposition that does not exceed 1 mol% at the highest temperature studied. Under such  substrate decomposition that does not exceed 1 mol% at the highest temperature studied. Under such conditions, the reaction rates increases by eight times without compromising the product selectivity,  conditions, the reaction rates increases by eight times without compromising the product selectivity, allowing us to reduce the residence time from hours required in batch to seconds in flow.  allowing us to reduce the residence time from hours required in batch to seconds in flow. Acknowledgments: The authors are grateful to Jonathan Strong for the ICP analysis, Guannan Hu for the XRD  study of the Pd/ZnO catalyst. We also acknowledge the support of the European Research Council Proof of  concept grant (project MiCARF 693739) and InnovateUK grant (900041) for funding this research.   concept grant (project MiCARF 693739) and InnovateUK grant (900041) for funding this research. Author Contributions: N.C. and E.R. conceived and designed the experiments; Y.B. prepared the catalyst‐coated  Author Contributions: N.C. and E.R. conceived and designed the experiments; Y.B. prepared the catalyst-coated tubes and performed the experiments; N.C. and Y.B. analysed the data; All the authors contributed to writing tthhee ppaappeerr..
Additional Information: This is an open access article distributed under the Creative Commons Attribution License which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited (CC BY 4.0).
Uncontrolled Keywords: Acetylene,Ethylene,Flow chemistry,Hydrogenation,Lindlar,Palladium,Process intensification,Selectivity,Catalysis,Physical and Theoretical Chemistry
Publication ISSN: 2073-4344
Last Modified: 20 Feb 2026 10:58
Date Deposited: 12 Jul 2019 15:11
Full Text Link:
Related URLs: https://www.sco ... ons/85036593975 (Scopus URL)
PURE Output Type: Article
Published Date: 2017-11-25
Accepted Date: 2017-11-20
Authors: Cherkasov, Nikolay
Bai, Yang (ORCID Profile 0000-0002-8050-5716)
Rebrov, Evgeny

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