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Energy-efficient electrochemical ammonia production from dilute nitrate solution

Abstract:
Highly efficient electrochemical nitrate reduction could become a key process for sustainable ammonia production overcoming many limitations of the Haber–Bosch process. Current state-of-the-art electrocatalysts have severe drawbacks regarding yield, selectivity and energy efficiency when dealing with dilute nitrate solutions. Herein, we report a layered double hydroxide (LDH)/Cu foam hybrid electrocatalyst that offers a potential solution to this challenge. The [Ni0.75Fe0.25(OH)2](CO3)0.125 (Ni3Fe–CO3 LDH) exhibits an appropriate kinetic energy barrier for the Volmer step generating hydrogen radicals as well as suppressing H–H bond formation by inhibition of the Heyrovsky step. The electrochemically generated hydrogen radicals transfer to a Cu surface enabling NO3− reduction to NH3. The Ni3Fe–CO3 LDH/Cu foam hybrid electrode exhibits an 8.5-fold higher NH3 yield compared to a pristine Cu surface, while exhibiting an NH3 selectivity of 95.8% at 98.5% NO3− conversion. The best half-cell energy efficiency (36.6%) was recorded while achieving 96.8% faradaic efficiency at −0.2 V in 5 mM NO3−(aq).
Publication status:
Published
Peer review status:
Peer reviewed

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Publisher copy:
10.1039/D2EE03461A

Authors

More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Chemistry
Sub department:
Chemistry Research Laboratory
Role:
Author
More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Chemistry
Sub department:
Chemistry Research Laboratory
Role:
Author
More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Chemistry
Sub department:
Chemistry Research Laboratory
Role:
Author


Publisher:
Royal Society of Chemistry
Journal:
Energy & Environmental Science More from this journal
Volume:
16
Issue:
2
Pages:
663-672
Publication date:
2023-01-24
Acceptance date:
2023-01-09
DOI:
EISSN:
1754-5706
ISSN:
1754-5692


Language:
English
Keywords:
Pubs id:
1328590
Local pid:
pubs:1328590
Deposit date:
2023-03-07
ARK identifier:

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