期刊
ACS APPLIED MATERIALS & INTERFACES
卷 11, 期 43, 页码 40062-40068出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.9b14143
关键词
Fe3C@C; electrochemical nitrogen reduction; biotemplating; charge transfer; ammonia electrosynthesis
资金
- Natural Science Foundation of China [51771072, 51901076]
- Youth 1000 Talent Program of China
- Natural Science Foundation of Hunan Province [2019JJ50051]
- Fundamental Research Funds for the Central Universities
- State Key Laboratory of Powder Metallurgy, Central South University [621011813]
Developing highly efficient non-precious-metal catalysts for electrochemical reduction reaction is vital for artificial nitrogen fixation under ambient conditions. Herein, we report a bioinspired Fe3C@C composite as an efficient electrocatalyst for nitrogen reduction. The composite based on a leaf skeleton successfully replicates the natural vein structure with multichannels. The Fe3C@C core-shell structure as the real active center contributes to selective electrocatalytic synthesis of ammonia from nitrogen with Faraday efficiency of 9.15% and production rate of 8.53 mu g/(h mg(cat)) or 12.80 mu g/(h cm(2)) at a low potential of -0.2 V versus reversible hydrogen electrode (vs RHE), which is better than that of recently reported carbon- and iron-based materials, even comparable with that of noble-metal-based catalyst. Experiments with density functional theory calculations reveal that graphene-encapsulated Fe3C nanoparticles can improve charge transfer due to core-shell interaction, beneficial for inducing active sites for N-2 adsorption and activation and thereby facilitate ammonia synthesis.
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