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Atom-by-atom assembly reveals structure-performance control in PdCu catalysts for CO 2 hydrogenation to methanol
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DOI：10.1039/D5SC06681F.png)
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Abstract
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The catalytic conversion of CO2 to methanol using bimetallic materials presents a promising pathway for sustainable chemical production. A major challenge is the lack of atomic-level control over the catalyst structure and composition; which hinders the understanding of each metal's role in activity and selectivity. Here; we present a solvent-free on-surface assembly of PdCu bimetallic particles; directly from atoms; on ZnO with precise control of the order and quantity of metal atoms added. This atomic-defined interface reveals when atoms are added simultaneously; the metal with stronger ZnO binding governs particle size; but when introduced sequentially the first metal determines particle size. The simultaneously deposited PdCu exhibits the highest reported methanol productivity for PdCu-systems; achieving 8.2 mol h-1 mol-1metal at 270 °C and 20 bar. In this catalyst; Cu enhances CO2 adsorption; suppresses Zn incorporation into the PdCu structure and modulates Pd binding strength to reaction intermediates. This enhances methanol selectivity while maintaining high Pd-driven CO2 conversion.
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