Boron-Modulated Electronic-Configuration Tuning of Cobalt for Enhanced Nitric Oxide Fixation to Ammonia

Nano Lett. 2023 Aug 9;23(15):7120-7128. doi: 10.1021/acs.nanolett.3c01994. Epub 2023 Jul 25.

Abstract

Electrocatalytic nitric oxide reduction (eNORR) to ammonia (NH3) provides an environmental route to alleviate NO pollution and yield great-value chemicals. The evolution of eNORR has been primarily hindered, however, by the poor reaction kinetics and low solubility of the NO in aqueous electrolytes. Herein, we have rationally designed a cobalt-based composite with a heterostructure as a highly efficient eNORR catalyst. In addition, by integrating boron to modulate the electronic structure, the catalyst CoB/Co@C delivered a significant NH3 yield of 315.4 μmol h-1 cm-2 for eNORR and an outstanding power density of 3.68 mW cm-2 in a Zn-NO battery. The excellent electrochemical performance of CoB/Co@C is attributed to the enrichment of NO by cobalt and boron dual-site adsorption and fast charge-transfer kinetics. It is demonstrated that the boron is pivotal in the enhancement of NO, the suppression of hydrogen evolution, and Co oxidation to boost eNORR performance.

Keywords: NO enrichment; NO reduction reaction; ammonia production; boron modulation.