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Schottky Barrier‐Induced Surface Electric Field Boosts Universal Reduction of NO x − in Water to Ammonia
Author(s) -
Gao Peng,
Xue ZhongHua,
Zhang ShiNan,
Xu Dong,
Zhai GuangYao,
Li QiYuan,
Chen JieSheng,
Li XinHao
Publication year - 2021
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.202107858
Subject(s) - electrochemistry , ammonia , selectivity , faraday efficiency , electrode , electric field , electrolyte , reversible hydrogen electrode , chemistry , electrocatalyst , inorganic chemistry , nitrogen , materials science , analytical chemistry (journal) , working electrode , catalysis , physics , environmental chemistry , biochemistry , organic chemistry , quantum mechanics
NO x − reduction acts a pivotal part in sustaining globally balanced nitrogen cycle and restoring ecological environment, ammonia (NH 3 ) is an excellent energy carrier and the most valuable product among all the products of NO x − reduction reaction, the selectivity of which is far from satisfaction due to the intrinsic complexity of multiple‐electron NO x − ‐to‐NH 3 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 NO x − anions on the electrode surface, including NO 3 − and NO 2 − , and thus ensure the final selectivity to NH 3 . Both theoretical and experimental results demonstrate that NO x − anions were continuously captured by the electrode with largely enhanced surface electric field, providing excellent Faradaic efficiency of 99 % from both electrocatalytic NO 3 − and NO 2 − reduction. Remarkably, the NH 3 yield rate could reach the maximum of 25.1 mg h −1 cm −2 in electrocatalytic NO 2 − 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 NO x − pollutants, including seawater or wastewater, could be directly used for ammonia production in potential through sustainable electrochemical technology.