Innovative microkinetic modelling-supported structure–activity analysis of Ni/ZSM-5 during vapor-phase hydrogenation of levulinic acid

Vu, Hue-Tong (author), Lavrič, Žan (author), Kostyniuk, Andrii (author), Dražić, Goran (author), Grilc, Miha (author), Likozar, Blaž (author), Zabukovec Logar, Nataša (author), Djinović, Petar (author), Novak Tušar, Nataša (author)

The study examines Ni/ZSM-5 catalysts in vapor phase hydrogenation of levulinic acid (LA) under continuous flow conditions (ambient pressure, 210–250 °C). Advanced characterization revealed the interplay between Al and Ni. This was further reinforced by new approach of microkinetic modeling, which demonstrates a pioneering work on mathematical description of pulse H2 sorption, TPD kinetics, DRIFT-supported determination of sorption energy barriers and (de)sorption kinetics. The Ni/ZSM-5 (3.7 wt.% Ni, Si/Al = 28) emerged as the optimal choice for obtaining γ-valerolactone (GVL) as the desired product. Al-rich catalysts with high acid site amounts and low metallic Ni active site concentrations favored esterification, reducing hydrogenation activity, and impeding further hydrogenation of GVL to pentanoic/valeric acid (PA). To enhance PA formation, Ni/ZSM-5 (4 wt.% Ni, Si/Al = 750) with a high Si/Al ratio, was identified as crucial. The combination of described experiments and modelling is demonstrated beneficial for insightful investigation of the structure–activity relationship of Ni/ZSM5 or any other mono/bi-functional catalysts.

• Language: English
• Keywords: property–activity relationship, Ni/ZSM-5, levulinic acid vapor-phase hydrogenation, microkinetic modeling, product distribution
• Work type: Article
• Typology: 1.01 - Original Scientific Article
• Organization: FKKT - Faculty of Chemistry and Chemical Technology
• Publication status: Published
• Publication version: Version of Record
• Year: 2024
• Number of pages: 14 str.
• Numbering: Vol. 495, art. 153456
• PID: 20.500.12556/RUL-159799
• UDC: 544.3/.4
• ISSN on article: 1873-3212
• DOI: 10.1016/j.cej.2024.153456
• COBISS.SI-ID: 202339587
• Publication date in RUL: 25.07.2024

VU, Hue-Tong, LAVRIČ, Žan, KOSTYNIUK, Andrii, DRAŽIĆ, Goran, GRILC, Miha, LIKOZAR, Blaž, ZABUKOVEC LOGAR, Nataša, DJINOVIĆ, Petar and NOVAK TUŠAR, Nataša, 2024, Innovative microkinetic modelling-supported structure–activity analysis of Ni/ZSM-5 during vapor-phase hydrogenation of levulinic acid. Chemical engineering journal [online]. 2024. Vol. 495, no. 153456. [Accessed 5 April 2025]. DOI 10.1016/j.cej.2024.153456. Retrieved from: https://repozitorij.uni-lj.si/IzpisGradiva.php?lang=eng&id=159799

Record is a part of a journal

• Title: Chemical engineering journal
• Publisher: Elsevier Science
• ISSN: 1873-3212
• COBISS.SI-ID: 23123973

Licences

• License: CC BY 4.0, Creative Commons Attribution 4.0 International
• Link: http://creativecommons.org/licenses/by/4.0/
• Description: This is the standard Creative Commons license that gives others maximum freedom to do what they want with the work as long as they credit the author.

Secondary language

• Language: Slovenian
• Keywords: kataliza, katalizatorji, mikrokinetično modeliranje, levulinska kislina