Herein, we report the green synthesis of copper–zirconium bimetallic nanoparticles (Cu–Zr BNPs) from aqueous solutions using Azadirachta indica leaf extract as a reducing and stabilizing agent. The CuO, ZrO 2 NP, and Cu–Zr BNP samples were characterized by X-ray diffraction and Fourier transform infrared (FTIR) spectroscopy, and the morphologies of the samples were analyzed by high-resolution transmission electron microscopy (HR-TEM) with selected area electron diffraction analysis (SAED). The synthesized Cu–Zr BNPs have been employed as efficient catalysts for the selective N -methylation of aromatic and aliphatic amines with dimethyl carbonate. The effect of process conditions on the percentage conversion of benzylamine with dimethyl carbonate as a model reaction has been investigated. The Cu–Zr bimetallic nanoparticle catalytic system in a 1:2 molar ratio was able to convert amines into the corresponding N -methylated amines with a selectivity up to 91% at 180 °C in 4 h. The analysis of catalytic reusability confirmed that the reported heterogeneous catalyst can be used for five consecutive cycles without much loss in activity. Thus, the current protocol can be considered as a simpler, reproducible, and environmentally benign approach for N -methylation of amines.

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A novel 2-D flakes like Al-BPED ((N 1 ,N 2 -bis [pyridine-2-yl]methyl)ethane-1,-2-diamine) metal-organic framework (MOF) have been explored for its catalytic potential in the N-alkylation of amines with dialkyl carbonates. The Al-BPED MOF catalyst has been synthesized by hydrothermal route. The X-ray diffraction, Fourier Transform Infrared Spectroscope (FTIR), and High Resolution Transmission Electron Microscopy (HRTEM) images were used to analyze the morphology of the synthesized Al-BPED MOF samples. With the use of Al-BPED MOF, the primary and secondary aromatic amines were selectively and efficiently methylated with dimethyl carbonate. The effect of process conditions has been investigated toward N-methylation, N-ethylation, and N-benzylation of aromatic amines. Under the optimal conditions with 10 mol % of the MOF catalyst, a maximum aniline conversion of 88% and a selectivity >90% toward N-alkylation was achieved. The kinetic studies revealed the N-alkylation reaction in presence of Al-BPED MOF followed pseudo-first order rate kinetics.