Rational Design of N‐Doped Carbon‐Coated Cobalt Nanoparticles for Highly Efficient and Durable Photothermal CO₂ Conversion

Abstract Photothermal CO₂ hydrogenation to high‐value‐added chemicals and fuels is an appealing approach to alleviate energy and environmental concerns. However, it still relies on the development of earth‐abundant, efficient, and durable catalysts. Here, the design of N‐doped carbon‐coated Co nanoparticles (NPs), as a photothermal catalyst, synthesized through a two‐step pyrolysis of Co‐based ZIF‐67 precursor, is reported. Consequently, the catalyst exhibits remarkable activity and stability for photothermal CO₂ hydrogenation to CO with a 0.75 mol g_cat⁻¹ h⁻¹ CO production rate under the full spectrum of light illumination. The high activity and durability of these Co NPs are mainly attributed to the synergy of the attuned size of Co NPs, the thickness of carbon layers, and the N doping species. Impressively, the experimental characterizations and theoretical simulations show that such a simple N‐doped carbon coating strategy can effectively facilitate the desorption of generated CO and activation of reactants due to the strong photothermal effect. This work provides a simple and efficient route for the preparation of highly active and durable nonprecious metal catalysts for promising photothermal catalytic reactions.