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化学进展 2020, Vol. 32 Issue (5): 665-686 DOI: 10.7536/PC190829 前一篇   

• 综述 •

金属硼氢化物基固态储氢体系

顾婷婷1,2, 顾坚1,2,**(), 张喻3, 任华1,2   

  1. 1.南京大学现代工程与应用科学学院 南京 210093
    2.南京大学材料工程技术研究院 南通 226019
    3.湖北汽车工业学院材料科学与工程学院 十堰 442002
  • 收稿日期:2019-08-29 修回日期:2019-12-12 出版日期:2020-05-15 发布日期:2020-02-20
  • 通讯作者: 顾坚
  • 基金资助:
    国家自然科学基金项目(51701092); 江苏省自然科学基金项目(BK20160419); 南通市科技计划(JC2018111)
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Metal Borohydride-Based System for Solid-State Hydrogen Storage

Tingting Gu1,2, Jian Gu1,2,**(), Yu Zhang3, Hua Ren1,2   

  1. 1.College of Engineering and Applied Sciences, Nanjing University, Nanjing 210093, China
    2.Institute of Materials Engineering, Nanjing University, Nantong 226019, China
    3.College of Materials and Engineering, Hubei University of Automotive Technology, Shiyan 442002, China
  • Received:2019-08-29 Revised:2019-12-12 Online:2020-05-15 Published:2020-02-20
  • Contact: Jian Gu
  • About author:
    ** e-mail:
  • Supported by:
    National Natural Science Foundation of China(51701092); Natural Science Foundation of Jiangsu Province(BK20160419); Science and Technology Plan of Nantong City(JC2018111)

氢气储存仍是制约氢经济推行的关键问题,开发一种高效、安全的储氢技术仍面临着巨大挑战。近年来,利用固态氢化物的化学吸附储氢技术由于可靠、结构紧密和高储氢容量的特点,被视为最有潜力的储氢手段之一。在众多固态氢化物储氢材料中,金属硼氢化物由于其极高的重量和体积储氢密度而备受关注。然而,金属硼氢化物热力学稳定,动力学缓慢,导致其吸/放氢温度高、速率慢、可逆性及循环稳定性差。本文从替代、复合、掺杂、纳米结构限域及相应的反应机理等角度总结了金属硼氢化物储氢材料的最新改性研究和应用,并提出了其中存在的问题和相应对策,同时指出了未来的研究方向。

关键词： 储氢材料, 热力学, 动力学, 金属硼氢化物, 性能调控

Hydrogen storage is the key technological problem for a viable hydrogen economy and so far, finding an efficient and safe method of storing hydrogen remains an indomitable challenge. Chemical sorption via solid-state hydrides, offering reliable, compact and high capacity features, is considered one of the most promising avenues for hydrogen storage. Among the diverse hydrides, metal borohydrides are excellent candidates on account of their high gravimetric and volumetric density. However, these hydrides generally suffer from high temperatures of de/rehydrogenation, slow sorption rate, limited reversiblity and poor cyclability due to the intrinsic thermodynamic stability and/or sluggish kinetics. In this review, we summarize recent researches and applications on the aspect of optimizing performance through substitution, composite, doping, and nanostructure, cognizing the relevant reaction mechanism for the metal borohydride-based system. The challenges and countermeasures are illustrated, and the direction to further enhancing the hydrogen storage properties of the system is also pointed out.

Contents

1 Introduction

2 Metal Borohydrides

2.1 Substitution

2.2 Composite

2.3 Doping

2.4 Nanostructure

3 Conclusion and prospect

Key words: hydrogen storage materials, thermodynamics, kinetics, metal borohydrides, performance adjustment
()
表1 DOE为车载氢气车辆设定的技术指标[16]
Table 1 The technical targets set by the DOE for on-board hydrogen based vehicles[16]
Parameter Unit 2017 Ultimate
System gravimetric capacity wt% H2 5.5 7.5
System volumetric capacity g H2/L 40 70
H2 transfer T(to FC) ℃ -40/85 -40/95~105
Operating P(min/max) MPa 0.5/1.2 0.5/1.2
System kinetics(5 kg) min 3.3 2.5
Cycle life cycles 1500 1500
表2 几种代表性硼氢化物的储氢性能
Table 2 Hydrogen storage properties for several representative borohydrides
M(BH4) n Hydrogen Density(mass%) Desorption Temperature Emission Gas ref
LiBH4 18.5 390 H2 56
NaBH4 10.8 400 H2 57
Be(BH4)2 20.8 40
sublimation		 B2H6+H2 58, 59
Mg(BH4)2 14.9 230 H2 60
Ca(BH4)2 11.6 300 H2 61, 62
Al(BH4)3 16.9 61 B2H6+H2 63, 64
Mn(BH4)2 9.5 130 H2+B2H6 65
图1 M(BH4) n 热力学性能调控方法示意图
Fig. 1 Schematic illustration of desorption process and two main approaches to tailor the thermodynamic stability of M(BH4) n
表3 代表性双阳离子硼氢化物的合成方法及其纯度
Table 3 The synthesis method and purity of the representative mixed-cation borohydrides
MM'(BH4) n H2 content(wt%) Synthesis method Byproduct Purity(%) ref
LiK(BH4)2 10.6 LiBH4: KBH4(d) NA 77.5R 80
LiZr(BH4)5 11.7 ZrCl4: LiBH4(d) LiCl 50.4C 84
Li2Zr(BH4)6 12.5 ZrCl4: LiBH4(d) LiCl 53.4C 84
LiMn(BH4)3 11.3 MnCl2: LiBH4(d) LiCl 55.6C 85
LiSc(BH4)4 14.5 ScCl3: LiBH4(d) LiCl 46.6C 86
Na2Mn(BH4)2 6.1 MnCl2: NaBH4(d) NaCl 42.0C 87
LiZn2(BH4)5 9.5 ZnCl2: LiBH4(d) LiCl 55.6C 88
NaZn2(BH4)5 8.8 ZnCl2: NaBH4(d) NaCl 49.4C 88
NaZn(BH4)3 9.0 ZnCl2: NaBH4(d) NaCl 53.2C 88
Li-Mg-B-H 15.8 MgCl2: LiBH4(w+f) NA - 89
Li-Ca-B-H 13.1 CaCl2: LiBH4(w+h) LiCl 51.9C 90
LiMg(BH4)3 15.8 LiBH4: Mg(BH4)2(d) NA - 91
LiCa(BH4)3 13.1 LiBH4: Ca(BH4)2(d) NA - 92
LiY(BH4)4 10.3 LiBH4: Y(BH4)3(d@200 ℃+q) NA 87R 93
NaY(BH4)4 9.4 NaBH4: Y(BH4)3(d@180 ℃+q) NA 69R 93
图式1 混合金属硼氢化物( M y 3 [M2(BH4) z ], z=x+y)的合成示意图以含Zn混合金属硼氢化物合成为例,M1=Li, M2=Zn, M3=Li、Na、K、[Cat]=[Ph4P] or [nBu4N], [An]=[Al{OC(CF3)3}4]或[B{3,5-(CF3)2C6H3}4][94]
Scheme 1 Illustration of the synthesis of mixed-metal borohydrides, M y 3 [M2(BH4) z ], z=x+y. For zinc compounds prepared this way: M1=Li, M2=Zn, M3=Li, Na, K, [Cat]=[Ph4P] or [nBu4N], [An]=[Al{OC(CF3)3}4] or [B{3,5-(CF3)2C6H3}4][94]
图2 2LiBH4: MgH2: 5 wt% Ni体系的吸氢van't Hoff曲线[138]
Fig. 2 Adsorption van't Hoff plot of the composite 2LiBH4: MgH2: 5 wt% Ni[138]
图3 2LiBH4 + nano-MgH2和2LiBH4 + 商用 MgH2体系在360 ℃下的放氢(空心点)和吸氢(实心点)压力-组分-等温(PCI)曲线[140]
Fig. 3 Desorption(open marks) and absorption(filled marks) pressure-composition isotherm(PCI) curves of 2LiBH4 + nano-MgH2 composite and 2LiBH4 + commercial MgH2 composite at 360 ℃[140]
表4 共晶熔融复合体系的热解行为
Table 4 Summary of the pyrolysis behavior for the eutectic melting composites
System Event temperature( ℃) Behavior ref
0.65LiBH4-0.35NaBH4 94 o-LiBH4→h-LiBH4 164
220 Melting
>300 H2 release
0.725LiBH4-0.275KBH4 113 o-LiBH4→h-LiBH4 165
105 Melting
>400 H2 release
0.55LiBH4-0.45Mg(BH4)2 112 o-LiBH4→h-LiBH4 166
180 H2 release
250 H2 release(frothing)
0.68LiBH4-0.32Ca(BH4)2 110 o-LiBH4→h-LiBH4 83
250 Frothing/expansion
>320 H2 release(Bubbling)
0.4NaBH4-0.6Mg(BH4)2 205 Melting 167
>240 H2 release
0.5LiBH4-0.5Mn(BH4)2 110 o-LiBH4→h-LiBH4 168
150 Melting
>160 H2& B2H6 release
0.45LiBH4-0.1NaBH4-0.45KBH4 103 Melting 169
>400 H2 release
图4 Ca(BH4)2 + 2LiBH4 + 2MgH2, Ca(BH4)2、Ca(BH4)2 + MgH2以及2LiBH4 + MgH2体系的TPD (a)和体积放氢(b)曲线[174]
Fig. 4 TPD(a) and volumetric dehydrogenation(b) curves of the ball-milled Ca(BH4)2 + 2LiBH4 + 2MgH2,Ca(BH4)2, Ca(BH4)2 + MgH2 and 2LiBH4 + MgH2 systems[174]
图5 Mg(BH4)2·6NH3纳米颗粒的合成示意图(a)和合成设备(b)[195]
Fig. 5 Schematic illustration(a) and equipment(b) of the fabrication procedure for Mg(BH4)2·6NH3 nanoparticles[195]
图6 纳米棒制备方法示意图[238]
Fig. 6 A schematic diagram of the nanorodpreparation process[238]
图7 (a)多孔CapB2H7/0.1TiO2体系的合成过程;(b)从室温加热到550 ℃的TG-MS曲线:纯Ca(BH4)2(1),Ca(BH4)2+0.1Ti(OEt)4球磨混合物(2)和多孔CaB2H7/0.1TiO2体系(3)[275]
Fig. 7 (a) Schematic illustration of the synthetic procedure of the porous CaB2H7/0.1TiO2 system;(b) TG(lines + symbols)-MS(lines) curves of the pure Ca(BH4)2(1), the as-milled Ca(BH4)2+0.1Ti(OEt)4 mixture(2) and porous CaB2H7/0.1TiO2 system(3) upon heating from RT to 550 ℃[275]
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摘要

金属硼氢化物基固态储氢体系