Moderate Active Hydrogen Generation over a Ni<sub>2</sub>P/CoP Heterostructure for One-Step Electrosynthesizing of Azobenzene with High Selectivity.
basic_science · Level V
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- Record sourced from PubMed, PMID 39762148.
- Also identified by DOI 10.1021/acs.nanolett.4c05315.
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Abstract
Through hydrogenation and N-N coupling, azobenzene can be produced via highly selective electrocatalytic nitrobenzene reduction, offering a mild, cost-effective, and sustainable industrial route. Inspired by the density functional theory calculations, the introduction of H* active Ni<sub>2</sub>P into CoP, which reduces the water dissociation energy barrier, optimizes H* adsorption, and moderates key intermediates' adsorption, is expected to assist its hydrogenation ability for one-step electrosynthesizing azobenzene. A self-supported NiCo@Ni<sub>2</sub>P/CoP nanorod array electrode was synthesized, featuring NiCo alloy nanoparticles within a Ni<sub>2</sub>P/CoP shell. By virtue of the thermodynamically optimal Ni<sub>2</sub>P/CoP heterostructure, along with overall fast electron transport in a core-shell integrated electrode, NiCo@Ni<sub>2</sub>P/CoP with abundant interfacial structure attains a great nitrobenzene conversion of 94.3%, especially prominent azobenzene selectivity of 97.2%, and Faradaic efficiency of 94.1% at -0.9 V (vs Hg/HgO). High-purity azobenzene crystals can also self-separate under refrigeration postelectrolysis. This work provides an energy-efficient and scalable pathway for the economical preparation of azobenzene in the electrocatalytic nitrobenzene hydrogenation.