摘要
Electrocatalytic reduction of nitrate(NO_(3)^(−))and nitride(NO_(2)^(−))to ammonia(NH3)is of wide interest as a promising alternative to the energy-intensive Haber-Bosch route for mitigating the vast energy consumption and the accompanied carbon dioxide emission,as well as benefiting for the relevant sewage treatment.However,exploring an efficient and low-cost catalyst with high atomic utilization that can effectively facilitate the slow multi-electron transfer process remains a grand challenge.Herein,we present an efficient hydrogenation of NO_(3)^(−)/NO_(2)^(−)species to NH3 in both alkaline and neutral environments over the Fe_(2)(MoO_(4))_(3)derived hybrid electrocatalyst with the metallic Fe site on FeMoO_(4)(Fe/FeMoO_(4)).The Mo ingredient can play a synergistically positive role in further promoting the NH_(3) production on Fe.As a result,Fe/FeMoO_(4)behaves well in the electrochemical NH_(3) generation from NO_(2)^(−)with a maximum NH_(3) Faradaic efficiency(FE)of 96.53%and 87.68%in alkaline and neutral electrolyte,corresponding to the NH_(3) yield rate of 640.68 and 302.56 mg·h^(−1)·mg_(cat.)^(−1),respectively,which outperforms the Fe and Mo counterpart and other similar catalyst,showing the robust catalytic capacity of each active site.
基金
supported in part by the National Natural Science Foundation of China(Nos.51925102 and 52273277)
H.-X.Z.acknowledges funding from the National Natural Science Foundation of China Outstanding Youth Science Foundation of China(Overseas).