Mixed-Valence Intermetallic Compounds for Urea Electrosynthesis.
basic_science · Level V
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- Record sourced from PubMed, PMID 41084159.
- Also identified by DOI 10.1021/acsnano.5c14949.
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Abstract
Efficient urea electrosynthesis relies on precisely controlling the kinetics of two parallel reduction reactions, i.e., carbon dioxide (CO<sub>2</sub>) reduction and nitrate (NO<sub>3</sub><sup>-</sup>) reduction. However, a major challenge lies in constructing stable and different active sites at the atomic scale, which are essential for synchronizing the reaction kinetics of these two reactions and facilitating C-N coupling. Herein, we introduce a mixed-valence intermetallic compound (Mv-IMC) Cu<sub>2</sub>Sb, featuring Cu<sup>+</sup>-Cu<sup>2+</sup> dual-sites as modular building blocks to regulate and synchronize CO<sub>2</sub> and NO<sub>3</sub><sup>-</sup> reduction kinetics. Mechanistic studies reveal that the constructed dual-sites stabilize *CO and *NO intermediates, lower the energy barrier of C-N coupling, and significantly enhance the urea synthesis efficiency. The Cu<sub>2</sub>Sb catalyst achieves a urea yield of 22.9 mmol h<sup>-1</sup> g<sub>cat</sub><sup>-1</sup> with a Faradaic efficiency of 64.9% at -0.4 V, maintaining stability over 200 h, surpassing most previously reported catalysts. This work pioneers the precise construction of multivalent active sites in Mv-IMCs, establishing a paradigm for designing high-performance electrocatalysts tailored to value-added organic synthesis.