MOF衍生的Fe2O3/MoSe2复合材料用于促进电催化固氮,Catalysis Science & Technology

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MOF衍生的Fe2O3/MoSe2复合材料用于促进电催化固氮
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2023-05-12 , DOI: 10.1039/d3cy00486d
Liming Huang _{1,

2} , Leiming Tao ₂ , Kui Pang _{2,

3} , Shuying He ₂ , GuanHua Zhu ₂ , LinHai Duan ₂ , Chenglin Wen ₂ , Changlin Yu ₂ , Hongbing Ji ₁

Affiliation

由于目前人工固氮催化剂活性低、选择性差，迫切需要开发高效、环保的电化学氨合成（EAS）电催化剂。电化学氨合成被认为是一种环境友好且可持续的人工固氮方法。在此，首先开发了组装在MoSe ₂ (Fe ₂ O ₃ /MoSe _{2 )上的Fe}₂ O _{3纳米颗粒，并被认为是一种具有高电活性的高效电催化固氮催化剂。}Fe ₂ O ₃ /MoSe ₂复合材料表现出优异的 NRR 活性和 NH₃在 -0.5 V 时的产率为 46.25 μg h^-1 mg^-1，在 -0.6 V 时的 FE 为 9.6%，相对于RHE。值得注意的是，Fe₂ O₃ /MoSe₂复合材料在回收测试中表现出出色的稳定性和耐久性。根据密度泛函理论（DFT）计算结果，发现界面电荷从Fe₂ O₃向MoSe_{2的传输可以显着增强Fe}₂ O₃ /MoSe₂的电化学氮还原反应（NRR）活性_{通过促进 Fe 2} O的导电性₃ /MoSe₂并降低速率决定 *N₂到 *N₂ H 形成步骤的自由能障碍。_{这项工作为NH 3}的绿色合成提供了一条有前途的途径。

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MOF-derived Fe2O3/MoSe2 composites for promoted electrocatalytic nitrogen fixation

Due to the low activity and poor selectivity of current artificial nitrogen fixation catalysts, there is an urgent need to develop efficient and environmentally friendly electrochemical ammonia synthesis (EAS) electrocatalysts. Electrochemical ammonia synthesis is considered an environmentally friendly and sustainable method for artificial nitrogen fixation. Herein, Fe₂O₃ nanoparticles assembled on MoSe₂ (Fe₂O₃/MoSe₂) were first developed and regarded as an efficient electrocatalytic nitrogen fixation catalyst with high electroactivity. The Fe₂O₃/MoSe₂ composites exhibited excellent NRR activity with an NH₃ yield of 46.25 μg h⁻¹ mg⁻¹ at −0.5 V and an FE of 9.6% at −0.6 V vs. RHE. Notably, the Fe₂O₃/MoSe₂ composites exhibited excellent stability and durability in recycling tests. According to the findings of density functional theory (DFT) calculations, it was discovered that the transmission of interfacial charges from Fe₂O₃ to MoSe₂ can considerably intensify the electrochemical nitrogen reduction reaction (NRR) activity of Fe₂O₃/MoSe₂ through facilitating the electrical conductivity of Fe₂O₃/MoSe₂ and lowering the free energy obstacle for the rate-determining *N₂ to *N₂H formation step. This work provides a promising avenue for the green synthesis of NH₃.

更新日期：2023-05-12

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