焦耳热制备高熵合金催化剂及其在锌空气电池中的应用

IrO₂和RuO₂等贵金属氧化物具有较高的氧析出催化活性，但其成本昂贵，而且动力学缓慢，在实际应用中会降低电池的稳定性。近年来，高熵合金催化剂以其独特的性质备受瞩目，高熵合金中不同原子之间形成的鸡尾酒效应、结构和晶格畸变效应以及动力学延迟扩散效应等，赋予了该材料优异的催化活性，因此高熵合金有望成为新型高效的氧析出反应催化剂。另一方面，锌-空气电池具有高能量密度、低成本和高安全性能的优点，有望成为下一代新能源电池应用于可穿戴电子器件和大规模储能。然而，锌-空气电池的催化剂仍面临着效率低和稳定性差等问题，因此，开发具有高活性和高稳定性的氧析出催化剂用于锌-空气电池十分关键。

本论文采用高效快速的焦耳热方法来制备高熵合金催化剂，大幅度简化了催化剂的制备工艺，缩短了制备时间。基于焦耳热快速升温与冷却特性，本论文成功设计并制备出了一种均匀的包覆型高熵合金氧析出催化剂，并进一步研究了其在可充电锌-空气电池和柔性电池中的应用。以氧化石墨烯和金属化合物为前驱体，通过焦耳热方法快速制备了还原氧化石墨烯（rGO）包覆的Fe₈Ni₈CoMnCu高熵合金催化剂材料。高熵合金催化剂均匀分散在大比表面积的rGO表面，可以充分暴露活性位点，提高了催化活性。此外，高结晶度的rGO包覆层可以有效提高催化剂的晶体结构稳定性，从而提高了催化剂的催化稳定性。基于该催化剂的可充电锌-空气在电流密度为10 mA·cm^-2条件下实现了高达800 mAh·g_Zn^-1的比容量，并且可稳定循环250小时。为了进一步探究使用焦耳热方法在二维过渡金属硫化物制备包覆型高熵合金的可行性，本论文以二硫化钼作为载体，通过焦耳热方法成功地合成了Fe₈Ni₈CoMnCu_0.5/MoS₂催化剂材料。以Fe₈Ni₈CoMnCu_0.5/MoS₂作为空气阴极装配成可充电锌-空气电池，在电流密度为10 mA·cm^-2的充放电下可稳定循环超过250小时，同时也展示了其在可穿戴柔性电子器件中的应用。

Noble metal oxides such as IrO₂ and RuO₂ have high oxygen evolution catalytic activity, but their high cost and slow kinetics reduce the stability of batteries in practical applications. In recent years, high-entropy alloy catalysts have attracted much attention for their unique properties. The cocktail effect, structural and lattice distortion effects, and kinetic delayed diffusion effects formed between different atoms in high-entropy alloys endow the material with excellent catalytic activity. Therefore, high-entropy alloys are expected to become a new efficient catalyst for the oxygen evolution reaction. On the other hand, zinc-air batteries have the advantages of high energy density, low cost, and high safety performance, which are expected to be applied in next-generation new energy batteries for wearable electronic devices and large-scale energy storage. However, the catalysts for zinc-air batteries still face problems such as low efficiency and poor stability. Therefore, it is crucial to develop oxygen evolution catalysts with high activity and stability for zinc-air batteries.

This paper adopts efficient and rapid Joule heating to prepare high-entropy alloy catalysts, which significantly simplifies the preparation process of the catalyst and shortens the preparation time. Based on the rapid heating and cooling characteristics of Joule heating, a uniformly dispersed encapsulated high-entropy alloy oxygen evolution catalyst is successfully designed and prepared, and further research is conducted on its application in rechargeable zinc-air batteries and flexible batteries. Using graphene oxide and metal compounds as precursors, the reduced graphene oxide (rGO) encapsulated Fe₈Ni₈CoMnCu high-entropy alloy catalyst material is prepared by rapid Joule heating. The high-entropy alloy is uniformly dispersed on the large specific surface area of rGO, which can fully expose the active sites, thereby improving the catalytic activity. Additionally, the high crystallinity of the rGO encapsulation layer can effectively improve the stability of the catalyst's crystal structure, enhancing the catalyst's catalytic stability. Based on this catalyst, the rechargeable zinc-air battery achieves a specific capacity of up to 800 mAh·g_Zn^-1 at a current density of 10 mA·cm^-2 and can stably cycle for 250 h. To further investigate the feasibility in the preparation of encapsulated high entropy alloys by two-dimensional transition metal sulfides, we also successfully synthesized Fe₈Ni₈CoMnCu_0.5/MoS₂ catalyst, with molybdenum disulfide as the support using the Joule heating. The rechargeable zinc-air battery assembled with Fe₈Ni₈CoMnCu_0.5/MoS₂ as the air cathode demonstrated stable cycling for over 250 h at a current density of 10 mA cm^-2, highlighting its significance in portable flexible battery devices.

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