Selective Electrosynthesis of a Nylon-6 Precursor via Facet-Promoted NO*-to-NHO* Conversion.
basic_science · Level V
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- Record sourced from PubMed, PMID 41729731.
- Also identified by DOI 10.1021/acs.nanolett.5c06489.
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Abstract
The electrosynthesis of cyclohexanone oxime (CHO) from NO is significant but suffers from low Faradaic efficiency (FE) due to the severe competitive NO*-NO* coupling at high NO concentrations. Here, a facet-regulation strategy is proposed to accelerate the NO hydrogenation process and inhibit NO*-NO* coupling. As a result, the Ag nanocubes with {100} surfaces exhibit an 86.5% FE, a 4.45 mmol h<sup>-1</sup> cm<sup>-2</sup> yield rate, and a 358 mA cm<sup>-2</sup> CHO partial current density, outperforming Ag nanohexahedrons with exposed {111} surfaces. Experimental and theoretical research has shown that stronger NO and H<sub>2</sub>O adsorption and lower thermodynamic and kinetic barriers of hydrogenation of NO* to NHO* over the {100} surface promote hydrogenation of NO* to NHO*, the key step that determines the CHO or NO*-NO* coupling products. Thus, NO*-NO* coupling is restrained, and a high CHO FE is achieved on Ag with a {100} surface.