高效铁、镍基催化剂在电催化氮循环中的应用研究
Research on the Applications of High Efficiency Iron and Nickel-Based Catalysts in Electrocatalytic Nitrogen Cycle
摘要: 氨具有较高能量密度和易液化的特点，是一种优良的储氢载体，而且储存与运输技术比较成熟，具有非常广阔的产业应用前景，同时氨作为农业与工业生产中的基础原料具有不可替代的作用。然而，目前大规模合成氨仍采用高温与高压的Haber-Bosch工艺，该工艺过程的能耗约占全球总能耗的1.4%，且排放的二氧化碳占据全球温室气体总排放量的1%左右。常温常压下电催化氮气与水合成氨是一种极具潜力的替代技术。但目前电催化氮还原合成氨与直接氨燃料电池技术面临着催化剂活性低、动力学速率缓慢以及法拉第效率低等关键问题。因此，探索高活性与高选择性的新型催化剂用于电催化氮还原与直接氨燃料电池中势在必行。铁基和镍基材料具有出色的本征活性与特有的表面电子结构，作为电催化剂已经引起了广泛的研究兴趣。本论文从Fe基与Ni基电催化剂的设计合成与改性出发，在电催化氮还原与直接氨燃料电池两个方面开展系列工作，利用密度泛函理论计算揭示了Fe基与Ni基催化剂带来的电催化优势。
Abstract: Ammonia is an excellent hydrogen storage carrier because of its unique characteristics, such as high energy density, easy liquefaction, and relatively mature technologies of storage and transpor-tation, which exhibits very broad industrial application prospects. At the same time, ammonia plays an irreplaceable role in agricultural and industrial production as the basic raw material. However, the Haber-Bosch process at high temperature and high pressure is still used for large-scale ammo-nia synthesis at present, which accounts for about 1.4% of the global total energy consumption and emits nearly 1% of the global total greenhouse gas emissions. Electrocatalytic nitrogen reduction reaction has been regarded as the most potential strategy to replace the Haber-Bosch process due to its green environmental protection, zero carbon emissions, and abundant raw materials. Never-theless, the technologies of electrocatalytic nitrogen reduction reaction and direct ammonia fuel cells face the key problems of low catalyst activity, slow kinetic rate, and poor Faradaic efficiency. Therefore, it is imperative to explore new catalysts with high activity and selectivity for electrocat-alytic nitrogen reduction and direct ammonia fuel cells. Iron and nickel based materials have at-tracted extensive interest as electrocatalysts due to their excellent intrinsic activities and unique surface electronic structures. This paper focuses on the design, synthesis, and modification of Fe-based and Ni-based electrocatalysts, and conducts a series of works in the fields of electrocata-lytic nitrogen reduction and direct ammonia fuel cells. Density functional theory calculations are utilized to reveal the electrocatalytic advantages brought by Fe-based and Ni-based catalysts.
文章引用：蒋玉卓, 钱涛, 樊冬娌. 高效铁、镍基催化剂在电催化氮循环中的应用研究[J]. 分析化学进展, 2023, 13(4): 500-512. https://doi.org/10.12677/AAC.2023.134053

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