A1 Vertaisarvioitu alkuperäisartikkeli tieteellisessä lehdessä
New bi-functional catalysts for a novel continuous production of propylene oxide with in-situ generated hydrogen peroxide
Tekijät: Schmidt, Christoph; Alvear, Matias; Sandri, Francesco; Mandon, Seo; Ojala, Satu; Laitinen, Tiina; Lastusaari, Mika; Angervo, Ilari; Salmi, Tapio
Kustantaja: Elsevier
Julkaisuvuosi: 2026
Lehti: Journal of Catalysis
Artikkelin numero: 116637
Vuosikerta: 454
ISSN: 0021-9517
eISSN: 1090-2694
DOI: https://doi.org/10.1016/j.jcat.2025.116637
Julkaisun avoimuus kirjaamishetkellä: Avoimesti saatavilla
Julkaisukanavan avoimuus : Osittain avoin julkaisukanava
Verkko-osoite: https://www.sciencedirect.com/science/article/pii/S0021951725007031?via%3Dihubhttps://www.sciencedirect.com/science/article/pii/S0021951725007031?via%3Dihub
Rinnakkaistallenteen osoite: https://research.utu.fi/converis/portal/detail/Publication/508908749
Rinnakkaistallenteen lisenssi: CC BY
Rinnakkaistallennetun julkaisun versio: Kustantajan versio
Combined direct synthesis of hydrogen peroxide (DSHP) and epoxidation of propene to propylene oxide with hydrogen peroxide (HPPO) was carried out first time in a continuous laboratory-scale trickle bed reactor operating under mild conditions of 8 bar and 10°C. The reaction was performed with bimetallic gold–palladium catalysts supported on titanium silicalite 1 (TS-1). Three series of catalysts were synthesized from two different lots of TS-1 and different calcination heating rates. The catalysts were extensively examined using XRD, SEMEDS, TEM-SAED, STEM-EDS, ICP-OES, XPS, UV–vis DRS, nitrogen-physisorption and ammonia-TPD. The metal-modification of TS-1 containing anatase impurities was shown first time, where the preferential deposition site for the bimetallic nanoparticles was on the minor anatase phase, found in different amounts in commercial TS-1 materials. In the first catalyst series, a higher anatase content was found, which led to a decrease of the AuPd nanoparticle size compared to the second and third series. Increasing the heating rate in calcination resulted in an additional reduction of the AuPd nanoparticle size. The propylene oxide selectivity was 55.7 % using catalysts of the third series, while the propylene oxide production rate was
0.17 mol⋅kgcat-1 ⋅h−1 with 19.2 % propene conversion. The use of a palladium-poor alloy was found to be crucial for this reaction system to limit the hydrogenation of hydrogen peroxide and propene. The catalyst activity was investigated in the separate processes of DSHP and epoxidation to get a deeper insight into the reaction mechanism. In the switch experiments, DSHP followed by the combined reaction of DSHP and HPPO, the competing side reactions, hydrogenation of propene and hydrogen peroxide were confirmed. In another experiment, the dismutation of hydrogen peroxide was disproved.
Ladattava julkaisu This is an electronic reprint of the original article. |
Julkaisussa olevat rahoitustiedot:
This work is part of the activities of Johan Gadolin Process Chemistry Centre (PCC) at Åbo Akademi. The research has been financed by Academy of Finland, through the Academy Professor grants 319002 and 320115 (T.S. and C.S.), the Scholarship of the Rector of Åbo Akademi and Neste and Fortum Foundation (C.S.). Part of the work was carried out with the support of the Centre for Material Analysis, University of Oulu, Finland.