IF: 17.6！国仪量子高压储氢吸附仪助力高水平固态储氢材料研究

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JMA:纳米Ni颗粒改善MgH₂放氢动力学催化机理

Catalytic mechanisms of nickel nanoparticles for the improved dehydriding kinetics of magnesium hydride.Journal of magnesium and alloys（2023）

——燕山大学沈同德老师课题组

研究中使用国仪量子H-Sorb X600系列产品

摘要

固态储氢具有安全性高、可以常温储氢以及体积储氢密度高等优点，是最具商业化发展前景的储氢方式之一。在双碳政策的大背景下，固态储氢作为氢能源产业链关键的中游环节而受到了广泛关注及研究。

近日，燕山大学沈同德老师课题组合成了介孔碳（Ni@C）负载Ni纳米颗粒（Ni-NPs）的催化剂，有效改善了MgH2储氢材料的脱氢动力学。Ni@C的使用使脱氢活化能从176.9降低到79.3 kJ mol−1，脱氢峰温度从375.5降低到235 ℃。添加Ni等催化剂可以改善MgH2的脱氢动力学，但鉴于Ni、Mg2Ni、Mg2NiH0.3和Mg2NiH4等不同物质的催化作用不同，他们进一步研究表明复合材料MgH2-Ni@C中MgH2的分解最初是由Ni-NPs触发的，这是限速步骤。随后，生成的Mg与Ni-NPs快速反应生成Mg2Ni，进一步促进了残余MgH2的脱氢。在接下来的脱氢循环中，Mg2NiH4可以快速分解为Mg2Ni，并不断促进MgH2的分解。该研究不仅阐明了Ni催化剂的机理，而且有助于设计和组装具有改善MgH2脱氢动力学的催化剂。

Fig. 8. Schematic description for 

the hydriding/dehydriding of MgH2–Ni@C.[1]

材料吸放H2性能分析

为了表征MgH2-Ni@C材料的吸/放氢性能，在0.01 MPa的氢气压力下，进行了不同温度（300、320和340 ℃）下MgH2-Ni@C材料的等温解吸动力学曲线测试。为了对比，在300 °C下也进行了未加任何催化剂的MgH2材料的等温动力学曲线测试。氢的解吸动力学曲线如下左图所示。MgH2在300 ℃下脱氢缓慢，30 min内脱氢量仅为3.1 wt.%。相比之下，MgH2-Ni@C在300 ℃下脱氢量为5.4 wt.%，7.5 min内脱氢量为5.4 wt.%。75 ℃下氢气压力为2 MPa时的吸氢动力学曲线如下右图所示。MgH2-Ni@C在200 min内可吸收4.6 wt.%的氢，而MgH2在同一时间内只能吸收1.7 wt.%的氢。显然，Ni@C的引入显著改善了MgH2的放氢及吸氢性能。

Fig. 3d Isothermal dehydrogenation curves of MgH2–Ni@C at 300 °C, 320 °C, 340 °C and as-milled MgH2 at 300 °C under a hydrogen pressure of 0.01 MPa; Fig. S4 Isothermal hydrogenation curves of MgH2-Ni@C and as-milled MgH2 at 75 ℃ under a hydrogen pressure of 2 MPa. [1]

此外，MgH2-Ni@C和MgH2的吸氢和放氢PCT曲线分别如下图a和图b所示。平台压力Peq与试验温度T的关系可以用范霍夫方程拟合，吸氢和放氢的范霍夫图分别如下图c和图d所示。MgH2-Ni@C的拟合加氢△H值为-78.7±0.2 kJ mol−1，与MgH2的-76±0.3 kJ mol−1接近。MgH2-Ni@C的脱氢焓△H为76.2±0.2 kJ mol−1，与MgH2的脱氢焓(76.48±0.1 kJ mol−1)接近。这些△H值表明，引入Ni@C不会显著改变MgH2吸氢和放氢时的热力学性质。

Fig. S5 Thermodynamic properties of MgH2-Ni@C and as-milled MgH2. PCT curves for the hydrogen absorption/desorption of MgH2-Ni@C (a) and as-milled MgH2 (b). Van’t Hoff plots for hydrogen absorption/desorption (c-d). [1]

高压储氢吸附仪可以实现材料在不同温度及不同的高压环境下对氢气的吸放氢行为检测，可有效表征材料吸脱附氢气的温度和压力、吸脱附量以及吸脱附速率等储氢材料吸放氢热/动力学关键性能。

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