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Sustainable conversion of alkaline nitrate to ammonia at activities greater than 2 A cm−2
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Journal Article
Sustainable conversion of alkaline nitrate to ammonia at activities greater than 2 A cm−2
2024
Overview
Nitrate (NO
3
‒
) pollution poses significant threats to water quality and global nitrogen cycles. Alkaline electrocatalytic NO
3
‒
reduction reaction (NO
3
RR) emerges as an attractive route for enabling NO
3
‒
removal and sustainable ammonia (NH
3
) synthesis. However, it suffers from insufficient proton (H
+
) supply in high pH conditions, restricting NO
3
‒
-to-NH
3
activity. Herein, we propose a halogen-mediated H
+
feeding strategy to enhance the alkaline NO
3
RR performance. Our platform achieves near-100% NH
3
Faradaic efficiency (pH = 14) with a current density of 2 A cm
–2
and enables an over 99% NO
3
–
-to-NH
3
conversion efficiency. We also convert NO
3
‒
to high-purity NH
4
Cl with near-unity efficiency, suggesting a practical approach to valorizing pollutants into valuable ammonia products. Theoretical simulations and in situ experiments reveal that Cl-coordination endows a shifted
d
-band center of Pd atoms to construct local H
+
-abundant environments, through arousing dangling O-H water dissociation and fast *H desorption, for *NO intermediate hydrogenation and finally effective NO
3
‒
-to-NH
3
conversion.
Alkaline nitrate electroreduction to ammonia is restricted by insufficient H
+
supply. Here, the authors propose a halogen-mediated H
+
feeding strategy, by triggering dangling O-H water dissociation and fast *H desorption for *NO intermediate hydrogenation, to enhance the formation of ammonia.
Publisher
Nature Publishing Group UK,Nature Publishing Group,Nature Portfolio
Subject
