现代纺织技术

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碳化纳米纤维限域高熵硫化物的合成及其析氧性能

  

  • 网络出版日期:2025-03-20

Carbonized nanofibers' confined synthesis of high entropy sulfides for oxygen evolution reaction

  • Online:2025-03-20

摘要: 为应对传统化石能源过度消耗引发的环境问题,开发高活性、高稳定性的析氧反应(OER)催化材料具有重要意义。采用静电纺丝技术制备碳化纳米纤维作为载体,通过浸渍法将5种过渡金属盐(铁、钴、镍、铬和锰)与硫脲前驱体负载于碳化纳米纤维表面,并利用焦耳热快速升降温特性,在碳化纳米纤维上原位合成多元金属高熵硫化物纳米颗粒。通过调控高熵硫化物合成温度,研究合成温度对材料电催化性能的影响。结果表明:在1600 ℃的合成温度下制备的高熵硫化物材料(HES-1600)表现出优异的碱性OER催化活性,其在50 mA/cm2的电流密度下的过电位仅为320 mV,Tafel斜率为171 mV/dec,电荷转移电阻低至4.8 Ω,性能显著优于其他对比样品。此外,经过80 h的稳定性测试,该材料的电流密度仅下降了10.6%,展现出卓越的稳定性。本研究为提升析氧反应电催化性能提供了一种高效制备方法,同时为能源转换和环境保护领域的技术创新提供了新思路。

关键词: 静电纺丝, 浸渍法, 高熵硫化物, 析氧反应, 纳米纤维

Abstract: "The advancement of renewable energy sources is regarded as an effective approach to address the environmental challenges and energy crises arising from excessive consumption of traditional fossil fuels. Hydrogen energy, distinguished by its exceptional combustion heat value and green sustainability, stands out among various renewable energy options. Hydrogen production by electrolysis of water represents a highly efficient and direct method capable of rapidly generating high-purity hydrogen to meet the escalating energy demands. However, the core challenge in electrolysis of water is to develop catalysts with high activity and high stability to reduce the cell voltage during the electrolysis process and thus improve energy efficiency. Traditional metallic alloys and their compound materials, constrained by limited elemental diversity and the absence of versatile means to modulate their chemical compositions and electronic structures, exhibit confined potential for improving catalytic performance. High-entropy materials, as a class of innovative multicomponent materials, have profoundly impacted traditional alloy design paradigms. High-entropy alloys (HEAs) exhibit unprecedented stability and performance advantages due to their unique characteristics, including the high-entropy effect, lattice distortion effect, sluggish diffusion effect, and ""cocktail effect"". Among these, the high-entropy effect facilitates the formation of stable solid solutions by enhancing the mixing entropy, thereby overcoming the immiscibility between elements. High-entropy sulfides (HES), emerging as novel multicomponent materials, demonstrate remarkable compositional tunability. By adjusting the metal composition, the adsorption free energy between the catalyst and reaction intermediates can be precisely controlled, optimizing catalytic performance. Furthermore, benefiting from the high-entropy effect, high-entropy sulfides exhibit superior electrocatalytic stability. In this study, HES nanoparticles supported on carbonized nanofibers were successfully prepared by electrospinning, impregnation and Joule pyrolysis, showing excellent catalytic performance of oxygen evolution reaction (OER) in alkaline media. The HES with M9S8 and MnS2 composite configurations was obtained by introducing sulfur sources and a variety of metal ions and pyrolysis at different temperatures in Joule pyrolysis. The catalyst prepared at 1,600 °C requires only overpotential of 320 mV to achieve a current density of 50 mA/cm², with a Tafel slope as low as 171 mV/dec. Moreover, its performance remained essentially unchanged after 10 h stability test. The introduction of sulfur led to the formation of a more complex M9S8 crystal structure, promoting synergistic catalysis between metals and sulfur, and significantly enhancing OER activity. This preparation method provides a new strategy for developing efficient and stable high-entropy sulfide catalysts for the oxygen evolution reaction."

Key words: electrospinning, impregnation, high entropy sulfides, oxygen evolution reaction, nanofibers

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