Open AccessHigh-ammonia selective metal–organic framework–derived Co-doped Fe/Fe 2 O 3 catalysts for electrochemical nitrate reduction
Author(s) -
Shuo Zhang,
Miao Li,
Jiacheng Li,
Qinan Song,
Xiang Liu
Publication year - 2022
Publication title -
proceedings of the national academy of sciences of the united states of america
Language(s) - English
Resource type - Journals
eISSN - 1091-6490
pISSN - 0027-8424
DOI - 10.1073/pnas.2115504119
Subject(s) - catalysis , electrochemistry , cobalt , inorganic chemistry , nitrate , ammonia , faraday efficiency , chemistry , adsorption , ammonia production , hydrogen , electrode , organic chemistry
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 (NO3 − 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@Fe2 O3 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 NO3 − RR activity with a high nitrate removal capacity (100.8 mg N gcat −1 h−1 ), NH3 selectivity (99.0 ± 0.1%), and faradaic efficiency (85.2 ± 0.6%). This strategy provides an approach to design advanced materials for NO3 − RR.