Magnetic Boron Nitride Nanosheets Decorated with Cobalt Nanoparticles as Catalyst for the Synthesis of 3,4-Dihydropyrimidin-2(1H)-ones/thiones

Abstract

Atomically thin two-dimensional boron nitride nanosheets have spawned futuristic advancements in the arena of nanocatalysis research through their intriguing capability to act as exceptional support matrixes. Motivated by their phenomenal attributes, we have fabricated a magnetic boron nitride nanosheet-based cobalt catalytic system wherein boron nitride nanosheets are initially integrated with magnetic Fe 3 O 4 nanoparticles (NPs), and the resulting nanostructure is further surface-engineered with cobalt NPs to yield an h-BN/Fe 3 O 4 /Co hybrid. For gaining an insight into their structural and morphological features, reliable spectroscopic and microscopic characterization techniques including TEM, SEM, XRD, FT-IR, VSM, ED-XRF, XPS, BET, TGA, and AAS were employed. The developed nanohybrid material was then utilized to provide ready access to a library of highly bioactive 3,4-dihydropyrimidin-2(1H)-ones/thiones under ambient conditions. A plausible mechanistic route for furnishing 3,4dihydropyrimidin-2(1H)-ones catalyzed by h-BN/Fe 3 O 4 /Co has also been delineated. Ambient reaction conditions, solvent-free conditions, high product yield, and excellent thermal and mechanical stability of the catalyst along with facile magnetic retrievability and efficient recyclability are some of the phenomenal characteristics of this methodology. The present protocol besides exhibiting a wider functional group tolerance and a high turnover number was devoid of any additive, thus making it superior to literature precedents reported to date. In consideration of the striking catalytic activity of the h-BN/Fe 3 O 4 /Co nanomaterial, it can be anticipated that the present catalyst can not only possess a stupendous potential to expedite substantial manufacturing of other industrially demanding organic motifs but may also unlock insights for designing next-generation 2D catalytic materials.

A comprehensive review on synthesis of dihydropyrimidione via Biginelli reaction catalyzed by reusable magnetic nanocatalyst (from 2020–till date)

“…Given h‐BN/Fe 3 O 4 /Co nanomaterial's remarkable catalytic activity, it is assumed that the current catalyst will not only have an immense potential to expedite significant production of numerous industrially demanding organic motifs but may also provide perspectives for developing next‐generation 2D catalytic components. [ 148 ]…”

“…Benzaldehyde, acetoacetate, and urea h-BN/Fe 3 O 4 /Co hybrid Solvent-free, 90 C, 40 min 98 [148] 23.…”

“…Given h-BN/Fe 3 O 4 /Co nanomaterial's remarkable catalytic activity, it is assumed that the current catalyst will not only have an immense potential to expedite significant production of numerous industrially demanding organic motifs but may also provide perspectives for developing next-generation 2D catalytic components. [148] To create a new heterogeneous catalyst, in 2022, Najjar and colleagues developed MNPs of Fe 3 O 4 that were coated with silicate that had been transformed with graphene quantum dots of copper (GQD/Cu). This catalyst was successfully employed in the Biginelli and Hantzsch multicomponent processes.…”

Insights into the catalytic potential of a rationally designed magnetic boron nitride nanosheet supported nickel catalyst for the efficient synthesis of 1,4-dihydropyridines

“…To date, several synthetic approaches for the synthesis of polyhydroquinolines have been reported but due to considerable shortcomings manifested by these protocols, such as prolonged reaction times, acidic or basic conditions, tedious experimental procedures, use of expensive metal salts, etc., [23][24][25][26][27][28][29][30][31][32] we focused our research towards the development of an alternative milder strategy via designing a magnetically incorporated h-BN nanosheet based catalytic system that surpasses the aforesaid issues remarkably. Impressed by the immense benefits governed by surface engineered h-BN nanocomposites and our on-going laboratory work, [33][34][35][36][37][38][39][40][41] we herein demonstrate the fabrication of a novel h-BN@Fe 3 O 4 @APTES@TPC@Ni catalyst and its utility in the multicomponent coupling of aldehydes, dimedone, ethyl acetoacetate and ammonium acetate to access the respective 1,4-dihydropyridines of biological importance. Such recyclable heterogeneous supported nanocatalysts have been grabbing the attention of the scientific community for years to deliver diverse heterocyclic organic products at the industrial scale.…”

Preparation and characterization of theh-BN/Fe3O4/APTES-AMF/CuIInanocomposite as a new and efficient catalyst for the one-pot three-component synthesis of 2-amino-4-aryl(or heteroaryl)-7,7-dimethyl-5-oxo-5,6,7,8-tetrahydro-4H-chromene-3-carbonitriles

“…[58][59][60][61][62][63][64][65] Thus, the development of a more proficient route towards the synthesis of heterocyclic 2-amino-4-aryl(or heteroaryl)-7,7-dimethyl-5-oxo-5,6,7,8-tetrahydro-4Hchromene-3-carbonitriles need to be adopted in order to surpass the aforementioned limitations. Inspired by our continuing research innovations towards the development of hybrid organic-inorganic nanomaterials, [66][67][68][69] we herein executed an idea of synthesizing novel magnetically retrievable hexagonal boron nitride nanosheets supported copper catalytic system (h-BN/Fe 3 O 4 /APTES-AMF/Cu II ) through an operationally-facile covalent approach, wherein copper was chosen as a metallic entity to facilitate the reaction due to its low cost, non-toxicity, earth-abundance and high catalytic activity. Moreover, the high boiling point of copper makes it a stupendous candidate to catalyze high-temperature reactions.…”