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Synergistic Modulation of Defect and Pyridinic Nitrogen in ZIF-Derived Carbon for Highly Dispersed Cobalt Confinement and High-Efficiency DMC Synthesis
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DOI：10.1039/D6NJ01662F.png)
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Abstract
En 中文
The quest for high-performance; chlorine-free catalysts in methanol oxidative carbonylation to dimethyl carbonate (DMC) is persistently hindered by the difficulty in simultaneously achieving high metal dispersion and robust stability against sintering. Herein; we report a rational design of cobalt/nitrogen-carbon (Co/NC) catalysts via pyrolysis of bimetallic ZIF-8/ZIF-67 precursors; where the Zn/Co ratio serves as a precise knob to tailor the carbon support. We uncover a critical synergistic effect between structural defect density and pyridinic nitrogen content: the evaporation of Zn generates abundant defects; together with the in situ formed pyridinic-N; which constructs a dual-anchoring site. This synergy imposes a strong constraint during pyrolysis; effectively suppressing the migration and coalescence of Co species; thereby yielding highly dispersed Co nanoparticles with an average size of 9.7 nm. The optimized CoNC-3 catalyst; possessing the highest defect density and pyridinic-N content; exhibits exceptional catalytic performance with a DMC space-time yield of 4.2 g g-1 cat. h-1 and selectivity of 98.5%; significantly outperforming counterparts lacking this synergistic regulation. This work elucidates a key structural-activity relationship and establishes a generalizable strategy for designing advanced non-precious metal catalysts through the coordinated engineering of defects and heteroatoms in carbon matrices.
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