Abstract

AbstractCatalytic hydrogenation of CO2 into CH4 is an effective method to convert waste CO2 and green hydrogen into clean fuel on a large scale. However, the viability of such process largely relies on the development of highly active heterogeneous catalysts. Here, a tailored methanation catalyst, Co nanoparticles immobilized into a highly porous N‐doped carbon matrix, is prepared by the carbonization of a cobalt‐based layered zeolitic imidazolate framework (ZIF−L) material under an argon atmosphere. This catalyst displays a specific activity of 22.3 molCH4/gcat.min at 350 °C, significantly outperforming a similar catalyst derived from the more conventional ZIF‐67 (11.7 molCH4/gcat.min). This is explained by the stabilization of small Co nanoparticles (∼20 nm) and by the presence of abundant medium‐strength basic sites related to the nitrogen doping in the catalyst prepared from ZIF−L. Notably, the new catalyst shows high stability; no deactivation is observed up to 60 hours on stream.

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