Atomically Dispersed Cu Sites on Dual-Mesoporous N-Doped Carbon for Efficient Ammonia Electrosynthesis from Nitrate.
ChemSusChem
; 15(11): e202200231, 2022 Jun 08.
Article
en En
| MEDLINE
| ID: mdl-35384362
ABSTRACT
The industrial Haber-Bosch process for ammonia synthesis is extremely important in modern society. However, it is energy intensive and leads to severe pollution, which has motivated eco-friendly NH3 synthesis research. Electroreduction of contaminant nitrate ions back to NH3 is an effective complement but is still limited by low NH3 yields and nitrate-to-NH3 selectivities. In this study, the electrochemical nitrate reduction reaction (NTRR) is carried out over a single-atom Cu catalyst. Atomically dispersed Cu sites anchored on dual-mesoporous N-doped carbon framework display excellent NTRR performance with NH3 production rate of 13.8â
mol NH 3 gcat -1 h-1 and NO3 - -to-NH3 faradaic efficiency (FE) of 95.5 % at -1.0â
V. Cu-N-C catalyst can sustain continuous 120â
h NTRR test in the simulated NH3 synthesis scenarios with large current density (about 200â
mA cm-2 ) and amplified volume of NO3 - solution (9â
times). Theoretical calculations reveal that atomically dispersed Cu1 -N4 sites reduce the energy barrier of potential-determining step in NTRR and promote the decomposition of primary intermediate in NO3 - -to-N2 process. These findings provide a guideline for the rational design of highly active, selective and durable electrocatalysts for the NTRR.
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Colección:
01-internacional
Base de datos:
MEDLINE
Idioma:
En
Revista:
ChemSusChem
Asunto de la revista:
QUIMICA
/
TOXICOLOGIA
Año:
2022
Tipo del documento:
Article