Highly Efficient Ni–Co Alloy Catalyst Fabricated by a Multivariate CoNiMgZn‐MOF Template for the Cascade Reaction of Nitroarenes With Alcohols

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A porous carbon/MgO composite–supported CoNi alloy catalyst (denoted as CoNi @Zn /MC) was synthesized via a multivariate metal–organic framework (MTV‐MOF) pyrolysis strategy. The catalyst, derived from Zn‐doped CoNiMgZn‐MOF precursors, demonstrated exceptional performance in the tandem hydrogenation–alkylation of nitroarenes with diverse alcohols. Comparative studies revealed that CoNi @Zn /MC achieved 100% selectivity for N ‐phenylbenzylamine, significantly outperforming the Zn‐free CoNi/MC counterpart (80.2% selectivity). The incorporation of Zn 2+ ions in the MOF precursors enhanced the reduction efficiency and dispersion of Co/Ni species during pyrolysis, as evidenced by HAADF‐STEM and XRD analyses. Notably, CoNi @Zn /MC exhibited robust magnetic recyclability, maintaining full catalytic activity over seven consecutive cycles. This work provides a generalized template strategy for designing high‐efficiency alloy catalysts for tandem reactions.