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Progress in Chemistry 2020, Vol. 32 Issue (5): 665-686 DOI: 10.7536/PC190829 Previous Articles   

• Review •

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: Revised: Online: Published:
  • 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)
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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
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
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
Fig. 1 Schematic illustration of desorption process and two main approaches to tailor the thermodynamic stability of M(BH4) n
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
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]
Fig. 2 Adsorption van't Hoff plot of the composite 2LiBH4: MgH2: 5 wt% Ni[138]
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]
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
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]
Fig. 5 Schematic illustration(a) and equipment(b) of the fabrication procedure for Mg(BH4)2·6NH3 nanoparticles[195]
Fig. 6 A schematic diagram of the nanorodpreparation process[238]
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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