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Tailored synthesis of transition-metallosilicates for the conversion of biomass-derived dihydroxyacetone to alkyl lactates – an aerosol-assisted sol-gel approach

Malik, Ali-Shan;Van der Verren, Margot;Debecker, Damien;Aprile, Carmela
(2023) PREPA13 - 13th International Symposium on “Scientific Bases for the Preparation of Heterogeneous Catalysts” — Location: Louvain-la-Neuve, Belgium (2023.July.9AD)

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Authors
  • Malik, Ali-Shan
    Author
  • Van der Verren, MargotUCLouvain
    Author
  • Debecker, Damienorcid-logoUCLouvain
    Author
  • Aprile, CarmelaUNamur
    Author
Abstract
Efficient and cost-effective approaches to produce value-added bio-based chemicals from sustainable biomass are highly required in both industry and academia. Biomass-derived feedstock such as sugars are usually highly oxygenated and possesses low levels of vapor pressure and thermal stability making it incompatible to employ in conventional gas-solid approaches of upgrading [2]. Therefore, low-temperature, liquid-phase catalysis seems preferable since it could bring improved process efficiency, sustainability and requires comparatively less energy. This could be realized by the development of new high surface area (HSA), inorganic materials with mesopores allowing easy access to well-defined, isolated active sites displaying enhanced activity, stability and recyclability in liquid media [3]. Moreover, such solid catalysts bring additional benefits such as facile separation from the product stream and reuse in several cycles thus providing a valid alternative to conventional non-catalyzed route or processes employing homogeneous catalysts [4]. Herein, a variety of eco-friendly silica-based catalysts loaded with well dispersed Hf atoms over highly mesoporous SiO2 network were synthesized and extensively explored for the efficient conversion of dihydroxyacetone (DHA) to ethyl lactate (EtL). High surface area (HSA) mesoporous Hf/SiO2 were synthesized via aerosol-assisted sol-gel (ASG) process (Fig.1). This process allows inserting successfully isolated Hf as single sites into the SiO2 matrix as evidenced by XPS (Fig.2). It was previously demonstrated that ASG process successfully produces metallosilicates with spherical morphology, high homogeneity and tunable texture exhibiting superior catalytic performance. These results were also achieved in this case as well-evidenced by employing different characterization techniques as TEM and BET. Moreover, we carefully tuned the texture of Hf/SiO2 with the addition of triethanolamine by adjusting the pH of the solution before the aerosol process. This approach strongly influenced the BET specific surface area, pore size distribution and degree of Hf insertion into the SiO2 matrix. In terms of catalytic reaction, DHA conversion is usually triggered by the presence of Brønsted/Lewis acid sites which initiate the dehydration of DHA to pyruvic aldehyde which – by rearrangement on Lewis sites – is subsequently transformed to ethyl lactates as shown in scheme 1. Complete conversion of DHA was observed with the best Hf/SiO2 catalyst under optimized process conditions with > 50% yield of EtL.
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Malik, A.-S., Van der Verren, M., Debecker, D., & Aprile, C. (2023). Tailored synthesis of transition-metallosilicates for the conversion of biomass-derived dihydroxyacetone to alkyl lactates – an aerosol-assisted sol-gel approach. PREPA13 - 13th International Symposium on “Scientific Bases for the Preparation of Heterogeneous Catalysts”, Louvain-la-Neuve, Belgium. https://hdl.handle.net/2078.5/25891