Atomically dispersed Pd as an effective modifier of Cu‐based catalysts for enhanced CO 2 hydrogenation to methanol

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Abstract Catalytic CO 2 hydrogenation to methanol is pivotal for sustainable carbon closed‐loops. Copper‐based catalysts are widely used for this reaction, but are inherently limited by sluggish hydrogen dissociation kinetics. Although Pd can overcome the sluggish low‐temperature H 2 activation of traditional Cu catalysts, its introduction typically triggers side reactions that diminish methanol selectivity. Herein, we resolve this trade‐off by precisely tailoring Pd dispersion in covalent triazine framework (CTF)‐supported Cu catalysts ( x Pd/CZC). We demonstrate that atomically dispersed Pd boosts hydrogen dissociation while retaining high methanol selectivity, whereas aggregated Pd promotes undesired pathways. The optimal 2.5Pd/CZC achieves a methanol space–time yield of 1217 mg MeOH g Cu+Pd −1 h −1 with 80% selectivity at 240°C and 5 MPa, outperforming the pristine Cu catalyst 1.86‐fold. Mechanistic studies reveal atomic Pd balances H 2 dissociation and H* binding affinity, effectively suppressing side reactions. This work provides valuable insights for the rational design of high‐performance catalysts via atomic‐scale promoter engineering.

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