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High-ammonia selective metal–organic framework–derived Co-doped Fe/Fe <sub>2</sub> O <sub>3</sub> catalysts for electrochemical nitrate reduction

Shuo Zhang, Miao Li, Jiacheng Li, Qinan Song, Xiang Liu

2022Proceedings of the National Academy of Sciences210 citationsDOIOpen Access PDF

Abstract

Significance Electrochemical reduction of nitrate pollution in water into value-added ammonium is essential for modern agriculture and industry and represents a potentially sustainable strategy to replace the traditional Haber–Bosch process. However, the nitrate reduction reaction (NO 3 − RR) process under ambient conditions often suffers from low selectivity. Here, we developed a strategy of tuning an electronic structure for preparing cobalt-doped Fe@Fe 2 O 3 electrocatalysts. Cobalt doping tunes the Fe d-band center, thereby modulating the adsorption energies of intermediates and suppressing hydrogen production. Therefore, the electrocatalysts exhibit superior NO 3 − RR activity with a high nitrate removal capacity (100.8 mg N g cat −1 h −1 ), NH 3 selectivity (99.0 ± 0.1%), and faradaic efficiency (85.2 ± 0.6%). This strategy provides an approach to design advanced materials for NO 3 − RR.

Topics & Concepts

CatalysisElectrochemistryCobaltInorganic chemistryNitrateAmmoniaFaraday efficiencyAdsorptionChemistryAmmonia productionSelectivityMaterials scienceElectrodeOrganic chemistryPhysical chemistryAmmonia Synthesis and Nitrogen ReductionAdvanced Photocatalysis TechniquesNanomaterials for catalytic reactions
High-ammonia selective metal–organic framework–derived Co-doped Fe/Fe <sub>2</sub> O <sub>3</sub> catalysts for electrochemical nitrate reduction | Litcius