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Angewandte Chemie International Edition, 2021-09, Vol.60 (38), p.20711-20716
International ed. in English, 2021
Volltextzugriff (PDF)

Details

Autor(en) / Beteiligte
Titel
Schottky Barrier‐Induced Surface Electric Field Boosts Universal Reduction of NOx− in Water to Ammonia
Ist Teil von
  • Angewandte Chemie International Edition, 2021-09, Vol.60 (38), p.20711-20716
Auflage
International ed. in English
Ort / Verlag
Weinheim: Wiley Subscription Services, Inc
Erscheinungsjahr
2021
Quelle
Alma/SFX Local Collection
Beschreibungen/Notizen
  • NOx− reduction acts a pivotal part in sustaining globally balanced nitrogen cycle and restoring ecological environment, ammonia (NH3) is an excellent energy carrier and the most valuable product among all the products of NOx− reduction reaction, the selectivity of which is far from satisfaction due to the intrinsic complexity of multiple‐electron NOx−‐to‐NH3 process. Here, we utilize the Schottky barrier‐induced surface electric field, by the construction of high density of electron‐deficient Ni nanoparticles inside nitrogen‐rich carbons, to facilitate the enrichment and fixation of all NOx− anions on the electrode surface, including NO3− and NO2−, and thus ensure the final selectivity to NH3. Both theoretical and experimental results demonstrate that NOx− anions were continuously captured by the electrode with largely enhanced surface electric field, providing excellent Faradaic efficiency of 99 % from both electrocatalytic NO3− and NO2− reduction. Remarkably, the NH3 yield rate could reach the maximum of 25.1 mg h−1 cm−2 in electrocatalytic NO2− reduction reaction, outperforming the maximum in the literature by a factor of 6.3 in neutral solution. With the universality of our electrocatalyst, all sorts of available electrolytes containing NOx− pollutants, including seawater or wastewater, could be directly used for ammonia production in potential through sustainable electrochemical technology. The tunable surface electric field induced by Schottky barrier boosts the reduction of NOx− in water for ammonia production. The tunable amounts of Ni nanoparticles inside a nitrogen‐rich carbon support could gradually enhance the surface electric field for enriching and fixation of NOx− anions, achieving a high Faradaic efficiency of 99 % for ammonia production from both electrocatalytic NO3− and NO2− reduction.

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