Highly efficient NiCo alloy catalyst fabricated by MOFs-templated strategy for N-formylation reaction of amines with CO2 and phenylsilane

N-formylation of amines with carbon dioxide (CO2) and phenylsilane represents a sustainable and efficient pathway for synthesizing nitrogen-containing compounds, leveraging the growing interest in using CO2 as a feedstock in organic synthesis. Based on a bimetallic MOFs templating approach, this study synthesized an efficient NiCo alloy catalyst (termed as NiCo/CN-hmta) for the N-formylation reaction of phenylsilane, CO2, and N-methylbenzene amine. The catalytic performance results indicate that the NiCo/CN-hmta catalyst exhibits high catalytic activity in the N-formylation reaction process. Various characterizations and comparative experiments to explore the reasons for the enhancement in performance of NiCo/CN-hmta for N-formylation reaction. Additionally, there remain many speculative reaction pathways during the N-formylation reaction, and there is significant controversy regarding the order of interactions among phenylsilane, CO2, and N-methylbenzene amine. Therefore, this study aims to determine the reaction pathway of the MOFs-derived NiCo alloy catalyst in the N-formylation reaction through deuterated experiments, In-situ diffuse reflection infrared Fourier transform spectroscopy (in-situ DRIFTS) and 13C NMR tests to capture intermediates during the reaction process. We hope that our research can provide some insights for future applications of alloy catalysts in N-formylation reactions.