Bioinspired Fe3C@C as Highly Efficient Electrocatalyst for Nitrogen Reduction Reaction under Ambient Conditions
Bioinspired Fe3C@C as Highly Efficient Electrocatalyst for Nitrogen Reduction Reaction under Ambient Conditions
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仿生 Fe3C@C 作为常温条件下氮还原反应的高效电催化剂
DOI：
10.1021/acsami.9b14143
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发表时间：
2019-10-30
影响因子：
9.5
通讯作者：
Tan, Yongwen
中科院分区：
文献类型：
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作者：
Peng, Ming;Qiao, Yijin;Tan, Yongwen
开发高效的非贵金属电化学还原反应催化剂是实现常温人工固氮的关键。在此，我们报道了一种生物启发的Fe3C@C复合材料作为氮还原的有效电催化剂。基于叶片骨架的复合材料成功地复制了具有多通道的自然纹理结构。Fe 3 C @ C核壳结构作为真实的活性中心，对电催化氮气合成氨具有选择性，其法拉第效率为9.15%，产率为8.53 μ g/g（h mg（cat））或12.80 μ g/（h cm（2）），这优于最近报道的碳基和铁基材料，甚至与贵金属基催化剂相当。密度泛函理论计算结果表明，石墨烯包覆Fe 3C纳米粒子可以通过核壳相互作用促进电荷转移，有利于诱导N2吸附和活化的活性位点，从而促进氨合成。
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.