SnTUD-1: a solid acid catalyst for three component coupling reactions at room temperature

Pachamuthu, Muthusamy Poomalai; Shanthi, K.; Luque, Rafael; Ramanathan, Anand

doi:10.1039/c3gc40792f

Cited by 76 publications

(71 citation statements)

References 48 publications

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“…Noteworthy, distinction between Sn(IV) and lower valency tin species is not possible by XPS [105]. Overall, the XPS results together with the above characterization studies indicate that different amounts of tin were incorporated into the frameworks of the dealuminated materials deAl-betan.…”

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confidence: 69%

One-pot conversion of furfural to useful bio-products in the presence of a Sn,Al-containing zeolite beta catalyst prepared via post-synthesis routes

Antunes

Lima

Neves

et al. 2015

Journal of Catalysis

137

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Aiming at the valorisation of furfural (Fur) via sustainable routes based on process intensification and heterogeneous catalysis, the one-pot conversion of this renewable platform chemical to useful bio-products, namely furfuryl alkyl ethers (FEs), levulinate esters (LEs), levulinic acid (LA), angelica lactones (AnLs) and -valerolactone (GVL), was investigated using a single heterogeneous catalyst, in 2-butanol, at 120 ºC. Various chemical 2 reactions are involved in this process, which requires catalysts with active sites for acid and reduction chemistry. For this purpose, it was explored for the first time the catalytic potentialities of modified versions of zeolite beta containing Al and Sn sites prepared from commercially available nanocrystaline zeolite beta via post-synthesis partial dealumination followed by solid-state ion-exchange. The post-synthesis conditions influenced considerably the catalytic performances of these types of materials. The best-performing catalyst was (Sn) SSIE -beta1 with Si/(Al+Sn)=19 (Sn/Al=27.6), which led to total yield of bio-products of 83% at 86% Fur conversion, and exhibited steady catalytic performance for six consecutive runs. A systematic catalytic study using the prepared catalysts with different bio-products as substrates, together with the molecular level and microstructural characterisation of the materials, helped understand the effects of different material properties on the specific reaction pathways in the overall system. These studies led to mechanistic insights into the reaction network of Fur to the bio-products in alcohol media, upon which a kinetic model was developed for the first time. The superior performance of (Sn) SSIE -beta1 in various steps was related to the dealumination degree, dispersion and amount of Sn-sites, and acid properties.

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confidence: 69%

One-pot conversion of furfural to useful bio-products in the presence of a Sn,Al-containing zeolite beta catalyst prepared via post-synthesis routes

Antunes

Lima

Neves

et al. 2015

Journal of Catalysis

137

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“…in tetrahedral oxygen coordination and as observed in the spectrum of Mn 3 O 4 [3,18]. In addition, a low intensity band [2,3,19,20]. The observations from diffuse reflectance UV-Vis spectra clearly demonstrate that the majority of Mn species are in tetrahedral coordination Mn 3?…”

Section: Resultsmentioning

confidence: 73%

“…7) reveal characteristic [2,19,20]. In sharp contrast, calcined Mn-FDU-5 samples displayed a weak and board hyperfine splitting signal centered around 3300G with similar magnitude of g (&2.0) due to electrostatic and dipolar interaction of Mn 2?…”

Section: Resultsmentioning

confidence: 76%

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Unique characteristics of MnOx-incorporated mesoporous silicate, Mn-FDU-5, prepared via evaporation induced self assembly

et al. 2015

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Mn containing 3D mesostructured FDU-5 (Ia3d) silicates with varying Si/Mn ratios were synthesized for the first time via evaporation induced self assembly (EISA) technique under acidic conditions at room temperature, employing Pl23 triblock copolymer as a structure directing agent. This method facilitates complete incorporation of higher amounts of Mn in the framework and extraframework locations of FDU-5 even under highly acidic synthesis conditions. The Mn-FDU-5 samples possessed surface areas of 300-500 m 2 /g, pore volumes of 0.42-0.55 cm 3 /g and narrow pore size distributions of 4.1-4.9 nm. Homogeneous dispersion of Mn species and aggregated Mn oxide clusters were evidenced from FIB-SEM micrographs. Complementary analytical techniques such as diffuse reflectance UV-Vis, FTIR, TPR and EPR analyses provide insights into the nature of the different types of Mn species (Mn 2? , Mn 3? and Mn 3 O 4 nanoparticles) that co-exist in FDU-5. The Mn-FDU-5 material is shown to be active for the epoxidation of trans-stilbene (TS, *60 % conversion) to trans-stilbene epoxide (*64 % selectivity) with TBHP as oxidant. Although the activity of Mn-FDU-5 (*45 % TS conversion) is similar to those observed with MCM-41 and MCM-48 supports containing similar amounts of Mn (1 wt%), higher epoxide selectivity (*64 %) was observed with Mn-FDU-5. The mixed oxidation states of Mn (Mn 2? , Mn 3? ) along with the extraframework Mn 3 O 4 are found to be beneficial in catalyzing TS epoxidation.

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“…We have shown recently that inexpensive Sn [28] and Fe [29] containing TUD-1 type materials yielded excellent activities in one-pot three-component Mannich-type reactions of ketones with aldehydes and amines at room temperature and synthesis of pyrazolylbiscoumarin. In addition these catalysts are cheap and can be prepared in an environmentally friendly method [30].…”

Section: Introductionmentioning

confidence: 99%

Lewis acidic mesoporous Fe-TUD-1 as catalysts for synthesis of Hantzsch 1,4-dihydropyridine derivatives

2015

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SnTUD-1: a solid acid catalyst for three component coupling reactions at room temperature

Cited by 76 publications

References 48 publications

One-pot conversion of furfural to useful bio-products in the presence of a Sn,Al-containing zeolite beta catalyst prepared via post-synthesis routes

One-pot conversion of furfural to useful bio-products in the presence of a Sn,Al-containing zeolite beta catalyst prepared via post-synthesis routes

Unique characteristics of MnOx-incorporated mesoporous silicate, Mn-FDU-5, prepared via evaporation induced self assembly

Lewis acidic mesoporous Fe-TUD-1 as catalysts for synthesis of Hantzsch 1,4-dihydropyridine derivatives

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