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Unique hollow Ni–Fe@MoS2 nanocubes with boosted electrocatalytic activity for N2 reduction to NH3
Journal of Materials Chemistry A ( IF 11.9 ) Pub Date : 2020/03/24 , DOI: 10.1039/c9ta13336d
Libin Zeng 1, 2, 3, 4, 5 , Xinyong Li 1, 2, 3, 4, 5 , Shuai Chen 1, 2, 3, 4, 5 , Jiali Wen 1, 2, 3, 4, 5 , Wei Huang 1, 2, 3, 4, 5 , Aicheng Chen 1, 2, 3, 4, 5
Affiliation  

Nanostructure tailoring is considered as an efficient strategy to design high-performance electrocatalysts for improving electrocatalytic properties by exposing more active sites and promoting rapid electron transfer. Unfortunately, nanomaterials with a well-constructed morphology for the nitrogen reduction reaction (NRR) under ambient conditions are insufficient, and the yield rate and faradaic efficiency are still not high. Herein, NiFe–MoS2 nanocubes (NiFe@MoS2 NCs) are successfully synthesized derived from the corresponding Prussian blue analog self-templating strategy. Owing to its four-pointed star face-dependent hollow structure and trimetallic synergistic interactions, it largely exposes abundant active sites, making it present superb electrocatalytic performance for N2 conversion to NH3. In a 0.1 M Na2SO4 electrolyte, these as-prepared Ni–Fe@MoS2 NCs exhibit a significant NH3 yield of 128.17 μg h−1 mgcat.−1 and a satisfactory faradaic efficiency of 11.34% at −0.3 V vs. reversible hydrogen electrode (RHE) operation at 40 °C. The stability of the catalyst was determined by performing 15 hour continuous N2 reduction with a constant current density. The possible NRR catalytic paths, mechanism and electron transfer paths are elucidated in detail by in situ electrochemical-Fourier transform infrared spectroscopy combined with density functional theory calculations. This work offers new inspirations to the development of various cost-effective electrocatalysts for N2 fixation.

中文翻译:

独特的空心Ni–Fe @ MoS2纳米立方体,具有增强的电催化活性,可将N2还原为NH3

纳米结构修整被认为是设计高性能电催化剂的有效策略,可通过暴露更多的活性位并促进快速的电子转移来改善电催化性能。不幸的是,在环境条件下具有良好结构的氮还原反应(NRR)形态的纳米材料是不够的,并且产率和法拉第效率仍然不高。在这里,从相应的普鲁士蓝模拟自模板化策略成功地合成了NiFe–MoS 2纳米立方体(NiFe @ MoS 2 NCs)。由于它具有四点星形面相关的空心结构和三金属协同作用,它在很大程度上暴露了丰富的活性位,使其对N具有极好的电催化性能。2转化为NH 3。在0.1 M Na 2 SO 4电解质中,这些制备的Ni-Fe @ MoS 2 NCs的NH 3产率很高,为128.17μgh -1 mg cat。-1和-0.3 V在40°C下相对于可逆氢电极(RHE)的令人满意的法拉第效率为11.34%。通过以恒定的电流密度进行15小时的连续N 2还原来确定催化剂的稳定性。通过原位详细阐明了可能的NRR催化途径,机理和电子转移途径电化学-傅立叶变换红外光谱结合密度泛函理论计算。这项工作为开发各种具有成本效益的N 2固定电催化剂提供了新的启示。
更新日期:2020-04-15
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