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Article summary:
1. Metal ions doped into porous nitrogen-doped carbon (M–N–C) are a promising alternative to noble metals for energy-related transformations.
2. Cu–N–C SACs have shown potential in steering nitrate reduction towards ammonia, but the pre-formed M–Nx structure is not stable at highly reducing conditions.
3. This study reveals that the Cu–N4 structure undergoes successive transformations from Cu–N3 to near-free Cu0 single atoms and eventually to aggregated Cu0 nanoparticles, leading to an enhanced ammonia production rate with a Faradaic efficiency of 84.7%.
Article analysis:
This article presents a detailed study on the evolution of active sites during the electrochemical reduction of nitrate using operando X-ray absorption spectroscopy and Cu–N–C SAC as a model catalyst. The authors provide evidence that the as-synthesized Cu–N4 structure underwent successive transformations from Cu–N3 to near-free Cu0 single atoms and eventually to aggregated Cu0 nanoparticles with the applied potential moving from 0.00 to −1.00 V versus RHE, leading to an enhanced ammonia production rate with a Faradaic efficiency of 84.7%. The article is well written and provides sufficient evidence for its claims, however there are some points that could be further explored such as possible risks associated with this transformation or other possible catalysts that could be used for this reaction. Additionally, it would be beneficial if more information was provided on how these results compare to other studies in this field or how they can be applied in practical applications. All in all, this article is reliable and trustworthy due to its clear presentation of evidence and thorough discussion of results.