Jin Ou, Shang Yuanyuan, Huang Xiaohui, Mu Xiaoke, Szabó Dorothée Vinga, Le Thi Thu, Wagner Stefan, Kübel Christian, Pistidda Claudio, Pundt Astrid
Institute of Applied Materials, Karlsruhe Institute of Technology, 76131 Karlsruhe, Germany.
Institute of Nanotechnology, Karlsruhe Institute of Technology, 76344 Eggenstein-Leopoldshafen, Germany.
Nanomaterials (Basel). 2022 May 31;12(11):1893. doi: 10.3390/nano12111893.
The hampered kinetics of reactive hydride composites (RHCs) in hydrogen storage and release, which limits their use for extensive applications in hydrogen storage S1and energy conversion, can be improved using additives. However, the mechanism of the kinetic restriction and the additive effect on promoting the kinetics have remained unclear. These uncertainties are addressed by utilizing versatile transmission electron microscopy (TEM) on the LiBH-MgH composite under the influence of the 3TiCl·AlCl additives. The formation of the MgB phase, as the rate-limiting step, is emphatically studied. According to the observations, the heterogeneous nucleation of MgB relies on different nucleation centers (Mg or TiB and AlB). The varied nucleation and growth of MgB are related to the in-plane strain energy density at the interface, resulting from the atomic misfit between MgB and its nucleation centers. This leads to distinct MgB morphologies (bars and platelets) and different performances in the dehydrogenation kinetics of LiBH-MgH. It was found that the formation of numerous MgB platelets is regarded as the origin of the kinetic improvement. Therefore, to promote dehydrogenation kinetics in comparable RHC systems for hydrogen storage, it is suggested to select additives delivering a small atomic misfit.
储氢和释氢过程中反应性氢化物复合材料(RHCs)的动力学受阻,这限制了它们在储氢和能量转换方面的广泛应用,而使用添加剂可以改善这种情况。然而,动力学限制的机制以及添加剂对促进动力学的影响仍不清楚。通过在3TiCl·AlCl添加剂影响下对LiBH-MgH复合材料进行多功能透射电子显微镜(TEM)研究,解决了这些不确定性。重点研究了作为限速步骤的MgB相的形成。根据观察结果,MgB的异质形核依赖于不同的形核中心(Mg或TiB和AlB)。MgB不同的形核和生长与界面处的面内应变能密度有关,这是由MgB与其形核中心之间的原子失配引起的。这导致了不同的MgB形态(棒状和片状)以及LiBH-MgH脱氢动力学的不同表现。研究发现,大量MgB片状物的形成被认为是动力学改善的根源。因此,为了在类似的用于储氢的RHC系统中促进脱氢动力学,建议选择原子失配小的添加剂。