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回收利用是稀土资源高效利用的可持续方案。氢化破碎技术因其高效环保特性被广泛采用，但氢破过程中产生的混合相会显著降低回收效率，这对工艺的优化提出了新的挑战。本文采用基于第一性原理计算结合机器学习方法，通过德拜模型系统地探究了氢化破碎过程中关键稀土氢化物（如NdH2、NdH3、Nd2H5）的热力学行为。研究结果表明，在600 kPa压强下，630 K左右的温度区间有望为氢化破碎工艺提供一个较为理想的操作条件，在此条件下，NdH2能够实现自发氢化，且能够有效抑制非稳定相的形成，有助于提高稀土回收效率。本研究还揭示了过高温度对NdH2热力学性质可能产生的不利影响，进一步强调了在特定温度区间操作的重要性。这些发现不仅为理解钕铁硼氢化过程的热力学机理提供了新的视角，而且为工业应用中氢化破碎工艺参数的优化提供了理论参考。Recycling is a sustainable strategy for the effcient utilization of rare earth resources. Hydrogenation milling has been widely adopted due to its high effciency and environmental benefits. However, the formation of non-stable phases during the hydrogenation process significantly reduces recovery effciency, presenting new challenges for process optimization. In this study, a combination of first-principles calculations and machine learning methods was employed to systematically investigate the thermodynamic behavior of key rare earth hydrides—such as NdH2, NdH3, and Nd2H5 during the hydrogenation milling process using the Debye model for lattice vibrations. The results show that a temperature range around 630 K under a pressure of 600 kPa may offer an ideal operational condition for the hydrogenation milling process. Under these conditions, NdH2 can undergo spontaneous hydrogenation, and the formation of unstable phases can be effectively suppressed, thereby improving rare earth recovery effciency. This study also reveals the potential adverse effects of excessively high temperatures on the stability and reactivity of NdH2, further emphasizing the importance of operating within a specific temperature range. These findings provide new insights into the thermodynamic mechanisms of the hydrogenation process in Nd2Fe14B permanent magnet material. Furthermore, they offer theoretical guidance for the optimization of industrial hydrogenation milling parameters.
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Keywords:
- Nd2Fe14B /
- hydrogenation recycling process /
- thermodynamic properties /
- Debye model
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