镁基固态储氢材料的研究进展

doi:10.19799/j.cnki.2095-4239.2023.0826

储能科学与技术 ›› 2024, Vol. 13 ›› Issue (3): 788-824.doi: 10.19799/j.cnki.2095-4239.2023.0826

镁基固态储氢材料的研究进展

梁宸曦¹(), 王振斌¹^,², 张明锦¹^,²(), 马存花¹^,²(), 梁宁³^,⁴

^1.青海师范大学化学化工学院，青海西宁 810016
^2.青海省人民政府-北京师范大学高原科学与可持续发展研究院，青海西宁 810008
^3.河南省地质矿产勘查开发局第三地质勘查院，河南郑州 451450
^4.河南省金属矿产深孔钻探工程技术研究中心，河南郑州 450003

收稿日期:2023-11-16 修回日期:2023-12-07 出版日期:2024-03-28 发布日期:2024-03-28
通讯作者: 张明锦,马存花 E-mail:1658548263@qq.com;zhangmingjin@qhnu.edu.cn;20211001@qhnu.edu.cn
作者简介:梁宸曦（2000—），男，硕士研究生，研究方向为镁基储氢材料，E-mail：1658548263@qq.com；

Research progress on magnesium-based solid hydrogen storage nanomaterials

Chenxi LIANG¹(), Zhenbin WANG¹^,², Mingjin ZHANG¹^,²(), Cunhua MA¹^,²(), Ning LIANG³^,⁴

^1.School of Chemistry and Chemical Engineering, Qinghai Normal University, Xining 810016, Qinghai, China
^2.Academy of Plateau Science and Sustainability, People's Government of Qinghai Province-Beijing Normal University, Xining, 810008, Qinghai, China
^3.The Third Geological Exploration Institute of Henan Bureau of Geology and Mineral Resources Exploration and Development, Zhengzhou 451450, Henan, China
^4.Henan Metal Mineral Deep Hole Drilling Engineering Technology Research Center, Zhengzhou 450003, Henan, China

Received:2023-11-16 Revised:2023-12-07 Online:2024-03-28 Published:2024-03-28
Contact: Mingjin ZHANG, Cunhua MA E-mail:1658548263@qq.com;zhangmingjin@qhnu.edu.cn;20211001@qhnu.edu.cn

摘要/Abstract

摘要：

氢能有望成为脱碳时代的“理想燃料”。高性能储氢材料的发现、开发和改性是未来发展固态储氢和氢能源利用的关键。而氢化镁（MgH₂）具有储氢能力强、自然储量丰富、环境友好等特点，在固态储氢材料领域备受关注。但是氢化镁较高的热力学稳定性、缓慢的动力学性能，以及循环过程中不可避免的团聚和粗化等问题在一定程度上限制了镁基固态储氢材料的大规模投产和实际应用。近年来，大量研究工作聚焦于镁基储氢材料的热/动力学改性，目前已经取得了大量的成果。本文通过回顾国内外相关文献，综述了改善镁基固态储氢材料储氢性能的最新研究进展，着重介绍了合金化、纳米化、引入催化剂等改性策略，阐述了不同策略具体的改性机理。最后对未来的发展方向进行了展望，旨在为高性能镁基储氢材料的研发提供借鉴与指导。

关键词: 固态储氢材料, 氢化镁, 合金化, 纳米化, 催化剂

Abstract:

Hydrogen energy is expected to become the "ideal fuel" in the era of decarbonization; therefore, the discovery, development, and modification of high-performance hydrogen storage materials are critical to the development of solid-state hydrogen storage and hydrogen energy use. Magnesium hydride (MgH₂) has attracted significant attention as a solid hydrogen storage material because of its strong hydrogen storage capacity, abundant natural reserves, and environmental friendly characteristics. However, the high thermodynamic stability, slow kinetic performance, and inevitable agglomeration and coiling during magnesium-hydride cycling limit the large-scale production and practical application of magnesium-based solid hydrogen storage materials. In recent years, several studies have focused on the thermal and kinetic modification of Mg-based hydrogen storage materials, leading to numerous achievements. This review discusses the latest research on magnesium-based solid hydrogen storage materials and summarizes modification strategies, such as alloying, nanification, and introduction of catalysts. Considering the current problems, future development directions are proposed to provide reference and guidance for the research and development of high-performance magnesium-based hydrogen storage materials.

Key words: solid hydrogen storage materials, magnesium hydride, alloying, nanification, catalysts

中图分类号:

TK 91

梁宸曦, 王振斌, 张明锦, 马存花, 梁宁. 镁基固态储氢材料的研究进展[J]. 储能科学与技术, 2024, 13(3): 788-824.

Chenxi LIANG, Zhenbin WANG, Mingjin ZHANG, Cunhua MA, Ning LIANG. Research progress on magnesium-based solid hydrogen storage nanomaterials[J]. Energy Storage Science and Technology, 2024, 13(3): 788-824.

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储氢类型	气态储氢	液态储氢	固态储氢
储氢原理	通过压缩、吸附等方式将氢气储存于钢瓶中	将氢气冷却到20 K，进行液化储存	使用固体材料，通过物理或化学吸附实现吸氢
储氢密度 (质量分数)	1%~5%(含气瓶)	5.5%(含储罐)	1.4%~20%
优点	1. 吸放氢速度快 2. 能在零下几十度环境下工作	1. 液态氢密度高 2. 储氢量大	1. 储氢量大 2. 不易爆炸，安全性好 3. 储存、运输方便 4. 多数材料可循环使用

缺点	1. 易泄漏，危险系数高 2. 储氢量低	1. 液化过程氢的热值损耗20%~30% 2. 需要苛刻的绝热条件	1. 储氢量与吸放氢温度不能兼顾 2. 多数材料使用前需要进行循环活化

合金	脱氢焓ΔH/(kJ/mol)	储氢量(质量分数)/%	文献
MgAl	62.7	4.44	[55]
Mg₂Fe	87.0	5.5	[56]
Mg₂Si	36.4	5.0	[57]
Mg_0.95In_0.05	68.1	5.3	[58]
Mg₃La	81.0	2.89	[59]

合金	脱氢活化能E_a/(kJ/mol)	初始脱氢温度T/℃	脱氢焓ΔH/(kJ/mol)	脱氢量/%(质量分数)	文献
Gd₅Mg₈₀Ni₁₅	75.07	280	75.1	4.87	[66]
Mg₉₀Ce₃Ni₇	72.2	100	80.0	3.5	[67]
Mg₉₈Ni_1.67La_0.33	107.26	175	—	5.59	[68]
Mg₉₀Ce₅Sm₅	106	300	81.2	4.95	[69]
Mg₉₆Y₂Zn₂	166.504	389	—	6.2	[70]
Mg₈₀Ni₁₀La₆₄	70.30	278.4	—	4.7	[71]
Mg₂₂Y₃Ni₉C	66.13	235.1	64.29	2.8	[72]
AlMg₂TiZn	148	310	76	1.4	[73]

材料	制备方法	尺寸/nm	脱氢量 /%(质量分数)	脱氢E_a/(kJ/mol)	技术难点	文献
MgH₂	高能球磨	—	7	—	球磨时间过长，效率较低	[84]
MgH₂	介质阻挡放电等离子体辅助球磨	2~6	6.5	—	设备要求过高	[87]
MgH₂-MgC_0.5Co₃	氢化燃烧合成法	—	4.38	126.7±1.4	制备过程存在危险性	[89]
胶体MgH₂	化学还原法	5	7.6	—	材料的规模和形貌难以调控	[96]
Mg纳米线	气相沉积法	30~170	7.6	—	制备过程复杂	[99]
MgH₂@Ni-MOF	纳米限域	3	1.45	41.5±3.7	材料储氢性能较差	[109]

材料	初始脱氢T/℃	脱氢E_a/ (kJ/mol)	脱氢量/%(质量分数)	文献
MgH₂-BiVO₄	265	84.33	1.1	[134]
MgH₂-TiNb₂O₇	178	100.4±0.1	7.0	[135]
MgH₂-MnV₂O₆	182.1	67±0.7	5.57	[136]
MgH₂-NiTiO₃	235	74±4	7.1	[137]
MgH₂-TiVO_3.5	197	62.4	5.0	[138]
MgH₂-NiV₂O₆	227	75.32±4.2	5.3	[139]
MgH₂-LiNbO₃	228	79.2±0.5	5.45	[140]
MgH₂-NaNbO₃	251	73	6.5	[141]

镁基固态储氢材料的研究进展

Research progress on magnesium-based solid hydrogen storage nanomaterials

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材料	初始脱氢T/℃	脱氢E_a/ (kJ/mol)	脱氢量/%(质量分数)	文献
Mg-NiF₂	362	139.21	3.85	[143]
MgH₂-K₂NiF₆	260	111.0	4.9	[144]
MgH₂-TiS₂	204	50.8	5.9	[146]
MgH₂-FeNi₂S₄ Mg/ZIF-67 MgH₂-Ni-MOF MgH₂-Nb₂O₅@MOF	267 275 292 181.9	65.5 161.73 107.8 75.57±4.16	1.92 3.7 5.7 6.2	[147] [154] [155] [157]

材料	脱氢E_a/(kJ/mol)	初始脱氢T/℃	脱氢ΔH/(kJ/mol)	脱氢量/%(质量分数)	文献
MgH₂-Co/Pd@BCNTs MgH₂-Ni₃ZnC_0.7/CNT MgH₂+Fe–Ni@3DG MgH₂- CoNi@C	76.66 84.22 83.8 78.5	198.9 110 — 173	— 75.17 72.2 —	6.35 5.36 5.13 5.83	[164] [165] [167] [175]
MgH₂-ML-Ti₃C₂	99	142	—	6.45	[176]
MgH₂-NbTiC	80	195	—	5.8	[177]
MgH₂-PrF₃/Ti₃C₂	78.11	180	—	7.0	[178]
MgH₂-V₂C	87.6	190	73.6	6.4	[179]

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