固体储氢材料的研究进展

doi:10.16085/j.issn.1000-6613.2022-1906

摘要/Abstract

摘要：

氢的廉价制取、安全储运以及高效应用是目前氢能研究领域的重点，而安全、高效的氢储运是实现氢能规模化应用的技术关键，因此高容量固态储氢材料的研发具有重要的学术意义和应用价值。固体材料储氢因储氢密度大、安全系数高而成为最有前景的储氢技术，得到了研究者们的广泛关注。本文针对目前国内外固体储氢材料研究现状，论述了几种固体储氢材料的研究进展，包括物理吸附类储氢材料、金属基储氢材料、配位氢化物和水合物储氢材料。重点评述了固态储氢材料中最具发展潜力的镁基储氢材料，并阐述了合金化、纳米化、添加催化剂以及复合轻金属配位氢化物等几种改性方法对镁基储氢材料储氢机理、微观结构、热力学性能、动力学性能的影响。制氢-储氢-用氢一体集成化设计应是固态储氢尤其是镁基储氢产业化应用发展道路，而镁基固态储运氢技术的发展，将可能实现氢气安全高效及大规模储运。

关键词: 固态储氢, 镁基储氢材料, 储氢性能, 镁基固态储氢系统

Abstract:

The low-cost production, safe storage and transportation, and efficient application of hydrogen are the focus of the current hydrogen energy researches. Among them, safe and efficient storage and transportation is the technical key to the large-scale application of hydrogen energy, so the research and development of high-capacity solid hydrogen storage materials have both academic significance and application value. Hydrogen storage by solid material has become the most promising hydrogen storage technology due to its large storage density and high safety factor, which has received widespread attention from researchers. In this paper, according to the current research status of solid hydrogen storage materials, the research progress of several solid hydrogen storage materials is discussed, including those based on physical adsorption, metal, coordinated hydride and hydrate. The most promising magnesium-based hydrogen storage materials are re-evaluated, and the effects of several modification methods such as alloying, nano-anodization, adding catalysts, and composite light metal coordination hydrides on the hydrogen storage mechanism, microstructure, thermodynamic properties and kinetic properties of magnesium-based hydrogen storage materials are elaborated. The integrated design considering production, storage and use of hydrogen should be the development trend for the industrialization of solid hydrogen storage.

Key words: solid stage hydrogen storage, Mg-based hydrogen storage materials, hydrogen storage properties, Mg-based solid state hydrogen storage system

中图分类号:

TK91

刘木子, 史柯柯, 赵强, 李晋平, 刘光. 固体储氢材料的研究进展[J]. 化工进展, 2023, 42(9): 4746-4769.

LIU Muzi, SHI Keke, ZHAO Qiang, LI Jinping, LIU Guang. Research progress of solid hydrogen storage materials[J]. Chemical Industry and Engineering Progress, 2023, 42(9): 4746-4769.

图/表 8

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材料	T_des/℃	动力学	热力学		参考文献
材料	T_des/℃	动力学	E_a(abs/des)/kJ·mol^-1	ΔH(abs/des)/kJ·mol^-1	参考文献
MgH₂@BCNTs	220	Abs：5.79%/250℃/5min/80bar Des：5.70%/275℃/约1h/0.002MPa	—/97.94^KM	—/68.92	[70]
MgH₂-10% nano ZrMn₂	181.9	Abs：5.3%/100℃/10min/3MPa Des：6.7%/300℃/5min/—	22.1±2.7^AM/82.2±2.7^KM	—	[71]
MgH₂-Ni-N-C500	—	Abs：5.5%/275℃/15s/2MPa Des：5.4%/300℃/5min/0.01MPa	—/87.2±5.4^KM	—/ 48.4±2.1	[72]
MgH₂-9NiMoO₄	—	Abs：6.7%/300℃/60s/3MPa Des：6.7%/300℃/10min/100Pa	—/86.1^KM	—/ 73.4	[73]
MgH₂-5%VTi-5%CNTs	150	Abs：5.0%/200℃/30s/2MPa Des：6.0%/300℃/6min/Vacuum	10.1^AM/—	—	[74]
MgH₂-6%MnV₂O₆	183.8	Abs：3.09%/50℃/10min/3MPa Des：5.57%/250℃/10min/0.09atm	—/81.2±5.6^KM	—/ 67.0±0.7	[75]
MgH₂-0.1TiH₂	—	Abs：1.5%/25℃/4h /2MPa Des：6.0%/300℃/5min/100Pa	16.4^KM/—	—	[76]
MgH₂+fl-TiO₂@C	180.3	Abs：6.3%/150℃/40min/5MPa Des：6.0%/250℃/7min/1kPa	—/67.10^KM	—	[77]
MgH₂-10% N-Nb₂O₅	170	Abs：6.3%/120℃/1h/50atm Des：5.0%/250℃/3min/—	—/98±3^KM	—/76±1	[78]
MgH₂-10%Co@C	168	Abs：— Des：5.8%/300℃/25min/0~0.05MPa	—/84.5^KM	—	[79]
MgH₂-7mol%MnFe₂O₄	300	Abs：— Des：5.05%/300℃/1h/0.1MPa	—/64.55^KM	—	[80]
MgH₂-15%VNbO₅	234	Abs：5.5%/160℃/10min/2MPa Des：—	—/99±3^KM	—/70.65±0.43	[81]
60MgH₂/TiO₂	180	Abs：2.65%/200℃/11.9min/3MPa Des：2.43%/300℃/10min/0.001MPa	—/106.7^KM	—	[82]
MgH₂-10% FeOOH NDs@G	229.8	Abs：6.0%/200℃/10min/3.2MPa Des：6.7%/325℃/20min/—	58.2^AM/125.03^AM	—	[83]
MgH₂-4% Ni NFs	143	Abs：— Des：7.02%/325℃/11min/0.02atm	—/81.5^AM	—	[84]
MgH₂-2D TiO₂(B)	200	Abs：6.01%/100℃/~10s/6MPa Des：6.16%/250℃/10min/0.002MPa	—/75.3±1.0^KM	—/76.7	[85]
MgH₂-10% SrTiO₃	275	Abs：6.6%/320℃/1h/27atm Des：5.8%/320℃/60min/1atm	—/109^KM	—/76.8	[86]
MgH₂-TiH₂@Gr	204	Abs：约6.0%/300℃/约2.5min/15atm Des：6.77%/300℃/30min/1atm	—/88.89±3.86^KM	—/74.54	[87]
MgH₂-10% TiO₂@C	205	Abs：6.6%/140℃/10min/5MPa Des：6.5%/300℃/7min/	38±1^AM/106±6^KM	—/73.6±0.3	[52]
MgH₂/Ni@GS	约130	Abs：5.4%/250℃/10min/30atm Des：5.4%/250℃/10min/0.01atm	22.7^AM/64.7^AM	—/62.1	[88]
MgH₂-5% K₂Ti₆O₁₃	175	Abs：6.5%/200℃/0.5min/2.2MPa Des：6.7%/280℃/3min/—	—/105.67^KM	—	[89]
Mg-0.2mol%Nb₂O₅	—	Abs：7.0%/300℃/60s/0.84MPa Des：7.0%/300℃/90s/—	—/62	—	[78]
MgH₂-(Ni-V₂O₃)@C	190	Abs：6.00%/150℃/9min/60atm Des：6.02%/300℃/5min/0.001atm	42.1^AM/84.6^AM —/99.4±8.5^KM	—	[90]
MgH₂-7.5%(N-Nb₂O₅@Nb₂C)	178	Abs：5.0%/90℃/1.95min/3.5MPa Des：6.0%/275℃/7.1min/0.001MPa	37.7^AM/78.1^AM	—/78.9±2.3	[91]
MgH₂-7% TiNb₂O₇	177	Abs：6.0%/200℃/3min/5MPa Des：5.5%/250℃/10min/—	—/96±4^KM	—/74.4	[92]
MgH₂-Ni@Ti-MX	175	Abs：5.4%/125℃/25s/3MPa Des：5.2%/250℃/15min/0.002MPa	56±4^AM/73±3.5^KM	74.4/81.3	[93]
MgH₂-9% NbTiC	195	Abs：5.9%/150℃/2.5min/5MPa Des：5.8%/250℃/30min/—	—/ 80±3^KM	—	[94]

材料	T_des/℃	动力学	热力学		参考文献
材料	T_des/℃	动力学	E_a(abs/des)/kJ·mol^-1	ΔH(abs/des)/kJ·mol^-1	参考文献
MgH₂@BCNTs	220	Abs：5.79%/250℃/5min/80bar Des：5.70%/275℃/约1h/0.002MPa	—/97.94^KM	—/68.92	[70]
MgH₂-10% nano ZrMn₂	181.9	Abs：5.3%/100℃/10min/3MPa Des：6.7%/300℃/5min/—	22.1±2.7^AM/82.2±2.7^KM	—	[71]
MgH₂-Ni-N-C500	—	Abs：5.5%/275℃/15s/2MPa Des：5.4%/300℃/5min/0.01MPa	—/87.2±5.4^KM	—/ 48.4±2.1	[72]
MgH₂-9NiMoO₄	—	Abs：6.7%/300℃/60s/3MPa Des：6.7%/300℃/10min/100Pa	—/86.1^KM	—/ 73.4	[73]
MgH₂-5%VTi-5%CNTs	150	Abs：5.0%/200℃/30s/2MPa Des：6.0%/300℃/6min/Vacuum	10.1^AM/—	—	[74]
MgH₂-6%MnV₂O₆	183.8	Abs：3.09%/50℃/10min/3MPa Des：5.57%/250℃/10min/0.09atm	—/81.2±5.6^KM	—/ 67.0±0.7	[75]
MgH₂-0.1TiH₂	—	Abs：1.5%/25℃/4h /2MPa Des：6.0%/300℃/5min/100Pa	16.4^KM/—	—	[76]
MgH₂+fl-TiO₂@C	180.3	Abs：6.3%/150℃/40min/5MPa Des：6.0%/250℃/7min/1kPa	—/67.10^KM	—	[77]
MgH₂-10% N-Nb₂O₅	170	Abs：6.3%/120℃/1h/50atm Des：5.0%/250℃/3min/—	—/98±3^KM	—/76±1	[78]
MgH₂-10%Co@C	168	Abs：— Des：5.8%/300℃/25min/0~0.05MPa	—/84.5^KM	—	[79]
MgH₂-7mol%MnFe₂O₄	300	Abs：— Des：5.05%/300℃/1h/0.1MPa	—/64.55^KM	—	[80]
MgH₂-15%VNbO₅	234	Abs：5.5%/160℃/10min/2MPa Des：—	—/99±3^KM	—/70.65±0.43	[81]
60MgH₂/TiO₂	180	Abs：2.65%/200℃/11.9min/3MPa Des：2.43%/300℃/10min/0.001MPa	—/106.7^KM	—	[82]
MgH₂-10% FeOOH NDs@G	229.8	Abs：6.0%/200℃/10min/3.2MPa Des：6.7%/325℃/20min/—	58.2^AM/125.03^AM	—	[83]
MgH₂-4% Ni NFs	143	Abs：— Des：7.02%/325℃/11min/0.02atm	—/81.5^AM	—	[84]
MgH₂-2D TiO₂(B)	200	Abs：6.01%/100℃/~10s/6MPa Des：6.16%/250℃/10min/0.002MPa	—/75.3±1.0^KM	—/76.7	[85]
MgH₂-10% SrTiO₃	275	Abs：6.6%/320℃/1h/27atm Des：5.8%/320℃/60min/1atm	—/109^KM	—/76.8	[86]
MgH₂-TiH₂@Gr	204	Abs：约6.0%/300℃/约2.5min/15atm Des：6.77%/300℃/30min/1atm	—/88.89±3.86^KM	—/74.54	[87]
MgH₂-10% TiO₂@C	205	Abs：6.6%/140℃/10min/5MPa Des：6.5%/300℃/7min/	38±1^AM/106±6^KM	—/73.6±0.3	[52]
MgH₂/Ni@GS	约130	Abs：5.4%/250℃/10min/30atm Des：5.4%/250℃/10min/0.01atm	22.7^AM/64.7^AM	—/62.1	[88]
MgH₂-5% K₂Ti₆O₁₃	175	Abs：6.5%/200℃/0.5min/2.2MPa Des：6.7%/280℃/3min/—	—/105.67^KM	—	[89]
Mg-0.2mol%Nb₂O₅	—	Abs：7.0%/300℃/60s/0.84MPa Des：7.0%/300℃/90s/—	—/62	—	[78]
MgH₂-(Ni-V₂O₃)@C	190	Abs：6.00%/150℃/9min/60atm Des：6.02%/300℃/5min/0.001atm	42.1^AM/84.6^AM —/99.4±8.5^KM	—	[90]
MgH₂-7.5%(N-Nb₂O₅@Nb₂C)	178	Abs：5.0%/90℃/1.95min/3.5MPa Des：6.0%/275℃/7.1min/0.001MPa	37.7^AM/78.1^AM	—/78.9±2.3	[91]
MgH₂-7% TiNb₂O₇	177	Abs：6.0%/200℃/3min/5MPa Des：5.5%/250℃/10min/—	—/96±4^KM	—/74.4	[92]
MgH₂-Ni@Ti-MX	175	Abs：5.4%/125℃/25s/3MPa Des：5.2%/250℃/15min/0.002MPa	56±4^AM/73±3.5^KM	74.4/81.3	[93]
MgH₂-9% NbTiC	195	Abs：5.9%/150℃/2.5min/5MPa Des：5.8%/250℃/30min/—	—/ 80±3^KM	—	[94]