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Elements Of Chemical Reaction Engineering

Biorefinery roadmap based on catalytic production and upgrading 5-hydroxymethylfurfural

Selective organic transformations using metal-organic frameworks (MOFs) and MOF-based heterogeneous catalysts have been an intriguing but challenging research topic in both the chemistry and materials communities. Analogous to the reaction specificity achieved in enzyme pockets, MOFs are also powerful platforms for regulating the catalytic selectivity via engineering their catalytic microenvironments, such as metal node alternation, ligand functionalization, pore decoration, topology variation and others. In this review, we provide a comprehensive introduction and discussion about the role of MOFs played in regulating and even boosting the size-, shape-, chemo-, regio- and more appealing stereo-selectivity in organic transformations. We hope that it will be instructive for researchers in this field to rationally design, conveniently prepare and elaborately functionalize MOFs or MOF-based composites for the synthesis of high value-added organic chemicals with significantly improved selectivity.

Metal-organic frameworks as catalytic selectivity regulators for organic transformations.

Phosphotungstic acid-modified zeolite imidazolate framework (ZIF-67) as an acid-base bifunctional heterogeneous catalyst for biodiesel production from microalgal lipids

According to the need of sustainable development, solid catalysts are critical materials for green biodiesel production. In this study, a hydrothermal method was used to develop a reusable and highly active Fe-BTC and UiO-66 metal–organic framework encapsulated Zr-doped polyoxometalate nano-hybrid catalysts (ZrSiW/Fe-BTC and ZrSiW/UiO-66) for the acid-catalyzed esterification of oleic acid with methanol. The structural and compositional characterization of the synthesized catalysts were characterized using various techniques such as Fourier transform infrared spectrometry (FT-IR), X-ray diffraction (XRD), nitrogen adsorption–desorption, scanning electron microscopy (SEM), and thermogravimetric (TG) and temperature programmed desorption (NH3-TPD) analysis. The as-prepared ZrSiW/UiO-66 had excellent catalytic activity in the esterification of oleic acid with methanol, higher than that of ZrSiW/Fe-BTC catalyst, owing to the fact that ZrSiW/UiO-66 nano-hybrids have high acidity, large specific surface area and pore volumes, and relatively large average pore sizes. Furthermore, the reusability and stability of nano-hybrids were also evaluated, and it was found that the stability of ZrSiW/UiO-66 catalyst was better.

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Efficient biodiesel production from oleic acid using metal–organic framework encapsulated Zr-doped polyoxometalate nano-hybrids

Aldol condensation of 5-hydroxymethylfurfural (HMF) with acetone provides a route to upgrading of biomass intermediates into value-added compounds such as fuel precursors. This reaction gives C9 an...

Aldol Condensation of 5‑Hydroxymethylfurfuralto Fuel Precursor over Novel Aluminum Exchanged-DTP@ZIF‑8

ZIF-8 is a zeolitic imidazolate framework which is a subclass of metal organic framework (MOF). ZIF-8 is the emerging class of MOF with various applications. Dodecatungstophosphoric acid (DTP) encapsulated ZIF-8 was prepared first time using bottle around the ship strategy. This approach covers ZIF-8 synthesis along with DTP encapsulation in one pot synthesis. The synthesized catalyst shows highest catalytic activity for esterification reaction of benzoic anhydride with cinnamyl alcohol to form cinnamyl benzoate. Heterogeneous catalytic synthesis of cinnamyl benzoate with complete reaction kinetics is presented here for the first time. Cinnamyl benzoate is a famous perfumery and flavoring agent and GRAS listed food additive molecule. Catalyst preparation method is simple, rapid and can be done at room temperature using water as a solvent. DTP@ZIF-8 shows sodalite like structure and it was confirmed by applying several characterization techniques like SEM, TEM, XRD, BET, FTIR, TGA and ammonia-TPD. Duration of DTP@ZIF-8 crystal formation was studied and optimized up to 12 h. Catalyst is thermally stable up to 400 °C and showed reusability for 3 cycles. Reaction kinetics was studied with best fit of Eley-Rideal mechanism.

Synthesis of cinnamyl benzoate over novel heteropoly acid encapsulated ZIF-8

Innovative catalysis in Michael addition reactions for C-X bond formation

Selectivity Engineering in One Pot Synthesis of Raspberry Ketone: Crossed Aldol Condensation of p‐Hydroxybenzaldehyde and Acetone and Hydrogenation over Novel Ni/Zn‐La Mixed Oxide

Metal (M) exchanged dodecatungstophosphoric acid (DTP) encapsulated inside ZIF-8 framework were synthesized by an in situ method to produce a variety of active catalysts. Thus, M-DTP@ZIF-8 (M = Co, Zr, Al and Fe) were used for the formation of furfuryl acetate from the esterification of furfuryl alcohol and acetic acid. The highest activity of the catalyst was found for Fe-DTP@ZIF-8, which was also the catalyst with the highest number of acidic sites. DTP showed retention of the Keggin structure after exchanging protons with the metal ions, and upon encapsulation of ions the rhombic structure of ZIF-8 was also retained. Fe-DTP@ZIF-8, the most active catalyst, possessed a very high surface area (1114 m2 g−1) and the highest acidity (0.61 mmol g−1). Fresh and spent catalyst was characterized using NH3-TPD, powder XRD, DRIFTS, SEM, HRTEM and TGA. A kinetic model was developed based on the LHHW (Langmuir–Hinshelwood–Hougen–Watson) mechanism and activation energy was calculated for both the steps as 38.6 kJ mol−1 and 65.2 kJ mol−1, which proved that the esterification reaction was much faster than the self-etherification of furfuryl alcohol.

Novelty of iron-exchanged heteropolyacid encapsulated inside ZIF-8 as an active and superior catalyst in the esterification of furfuryl alcohol and acetic acid

Radhika S. Malkar

Papers

Aldol Condensation of 5‑Hydroxymethylfurfuralto Fuel Precursor over Novel Aluminum Exchanged-DTP@ZIF‑8

Synthesis of cinnamyl benzoate over novel heteropoly acid encapsulated ZIF-8

Innovative catalysis in Michael addition reactions for C-X bond formation

Selectivity Engineering in One Pot Synthesis of Raspberry Ketone: Crossed Aldol Condensation of p‐Hydroxybenzaldehyde and Acetone and Hydrogenation over Novel Ni/Zn‐La Mixed Oxide

Novelty of iron-exchanged heteropolyacid encapsulated inside ZIF-8 as an active and superior catalyst in the esterification of furfuryl alcohol and acetic acid