A novel magnetic nanoparticle supported basic ionic liquid was successfully prepared by covalently anchoring 1-(2′-piperidyl)ethyl-3-(3-propyltriethoxysilane)imidazolium chloride onto the surface of silica-coated Fe₃O₄ nanoparticles, and characterized by FT-IR, TEM, XRD, TGA, VSM and elemental analysis. The obtained supported ionic liquid was certified as a versatile and robust catalyst for the unsymmetrical Hantzsch reaction and Knoevenagel condensation under solvent-free conditions. Furthermore, the catalyst could be conveniently recovered by an external magnet and reused six times without significant loss of catalytic activity.

An efficient and eco-friendly procedure for the synthesis of 1-amidoalkyl-2-naphthol and tetrahydrobenzo[b]pyran derivatives has been developed through a one-pot three-component condensation of aldehydes with 2-naphthol and amides, or with malononitrile and dimedone in the presence of magnetic nanoparticle supported acidic ionic liquid (AIL@MNP) as a novel heterogeneous catalyst under solvent-free conditions. This new procedure offers several advantages such as short reaction time, excellent yields, operational simplicity and without any tedious work-up for catalyst recovery or product purification. Moreover, the catalyst could be simply separated by an external magnet and reused six times without significant loss of catalytic activity.

Radical transformations are powerful in organic synthesis for the construction of molecular scaffolds and introduction of functional groups. In radical difunctionalization reactions, the radicals in the first functionalized intermediates can be relocated through resonance, hydrogen atom or group transfer, and ring opening. The resulting radical intermediates can undertake the following paths for the second functionalization: (1) couple with other radical groups, (2) oxidize to cations and then react with nucleophiles, (3) reduce to anions and then react with electrophiles, (4) couple with metal-complexes. The rearrangements of radicals provide the opportunity for the synthesis of 1,3-, 1,4-, 1,5-, 1,6-, and 1,7-difunctionalization products. Multiple ways to initiate the radical reaction coupling with intermediate radical rearrangements make the radical reactions good for difunctionalization at the remote positions. These reactions offer the advantages of synthetic efficiency, operation simplicity, and product diversity.

A relay catalysis strategy was established by using a bifunctional catalyst which was prepared by immobilization of organic chains containing secondary amine and Cu(II) complex onto silica-coated nano-Fe₃O₄. The simply prepared nanoparticles acted as efficient, intramolecular relays and magnetically recyclable base-metal bifunctional catalysts for Knoevenagel condensation and 1,3-dipolar cycloaddition domino reactions to prepare 5-substituted 1H-tetrazoles with excellent yields.

S-doping emerged as a promising approach to further improve the catalytic performance of carbon-based materials for organic synthesis. Herein, a facile and gram-scale strategy was developed using zeolitic imidazole frameworks (ZIFs) as a precursor for the fabrication of the ZIF-derived N, S co-doped carbon-supported zinc single-atom catalyst (CNS@Zn₁-AA) via the pyrolysis of S-doped ZIF-8, which was modified by aniline, ammonia and thiourea and prepared by one-pot ball milling at room temperature. This catalyst, in which Zn is dispersed as the single atom, displays superior activity in N-alkylation via the hydrogen-borrowing strategy (120 °C, turnover frequency (TOF) up to 8.4 h⁻¹). S-doping significantly enhanced the catalytic activity of CNS@Zn₁-AA, as it increased the specific surface area and defects of this material and simultaneously increased the electron density of Zn sites in this catalyst. Furthermore, this catalyst had excellent stability and recyclability, and no obvious loss in activity after eight runs.