A Review of the MSCA ITN ECOSTORE—Novel Complex Metal Hydrides for Efficient and Compact Storage of Renewable Energy as Hydrogen and Electricity
Abstract
:Table of Content | |
1. Introduction……… | 3 |
2. Promising Metal Hydrides for Battery Application……… | 4 |
2.1. Metal Hydrides for Li-ion and Post Li Batteries……… | 4 |
2.1.1. Metal Hydrides as Negative Electrode Material with Liquid Electrolyte……… | 5 |
2.1.2. Promising Complex Metal Hydrides as Solid-State Electrolytes……… | 8 |
Lithium Borohydride……… | 9 |
Lithium Nitride and Lithium Hydride……… | 9 |
Binary Phases of Hydrides with Lithium Halides ……… | 11 |
LiBH4-Li2NH: Li5(BH4)3NH—thorough characterization of a cluster complex hydride ……… | 11 |
Argyrodite Structure Materials ……… | 12 |
2.1.3. Application of Metal Hydrides in Solid-State Cells……… | 13 |
Solid-State Half-Cell ……… | 13 |
A Full Solid-State Li-ion Cell ……… | 15 |
2.1.4. Conclusions……… | 15 |
2.2. Na-Based Closo-Borates for Na Batteries……… | 16 |
2.2.1. Na-Based Closo-Borates Solid Electrolyte……… | 16 |
The Na2B12H12 Polymorphism ……… | 16 |
Nax+2y(CB11H12)x(B12H12)y Solid Electrolyte ……… | 17 |
2.2.2. Conclusions……… | 20 |
3. Advances in Hydrogen Storage Materials……… | 20 |
3.1. Pure Metal Hydrides (Mg, Pd, Ti)……… | 21 |
3.2. Amide and Imide Based Systems for H2 Storage……… | 22 |
3.2.1. Insights into Alkali-Based Amides and Imides Including Boron……… | 23 |
LiBH4-LiNH2 ……… | 23 |
LiNH2-Li2NH ……… | 25 |
3.2.2. Insights into the Structure and Reaction Mechanism of Metal Amide—Metal Hydride Composite Systems……… | 25 |
Ammonolysis of Alkali and Alkaline-Earth Metal Amides ……… | 26 |
K-Mg-N-H System ……… | 26 |
KNH2-KH System ……… | 27 |
Rb-Mg-N-H and Rb-N-H Systems ……… | 27 |
3.2.3. Conclusions……… | 27 |
3.3. Eutectic Metal Borohydride Systems……… | 28 |
3.3.1. Experimental Study and Assessment of Eutectic Borohydride Systems……… | 29 |
LiBH4-NaBH4 ……… | 29 |
LiBH4-KBH4 ……… | 30 |
NaBH4-KBH4 ……… | 30 |
LiBH4-NaBH4-KBH4 ……… | 30 |
Other Systems ……… | 31 |
3.3.2. Thermodynamic Properties of Eutectic Borohydride Systems……… | 31 |
3.3.3. Hydrogen Sorage Properties of Eutectic Metal Borohydride Systems……… | 33 |
3.3.4. Conclusions ……… | 33 |
3.4. Kinetic Tailoring of 2LiBH4 + MgH2/2LiH + MgB2 with Cost Effective 3TiCl3·AlCl3……… | 34 |
3.5. Role of Nanoconfinement in Enhancing the Properties of Hydrogen Storage Materials……… | 39 |
3.5.1. Nanoconfinement Approaches……… | 40 |
3.5.2. Confined Borohydrides……… | 41 |
3.5.3. Conclusions……… | 43 |
3.6. Rare Earth Borohydrides……… | 43 |
3.6.1. Synthesis of Rare Earth Borohydrides (REB)……… | 44 |
Solvent Free Synthesis of REB ……… | 44 |
Solvent-Based Synthesis of REB ……… | 44 |
3.6.2. Crystal Structures of Monometalic REB……… | 45 |
3.6.3. Crystal Structures of Bimetallic REB ……… | 46 |
3.6.4. Reactive Hydride Composites with REB……… | 49 |
3.6.5. Conclusions……… | 51 |
4. Final Conclusion and Outlook……… | 51 |
References……… | 53 |
1. Introduction
2. Promising Metal Hydrides for Battery Application
2.1. Metal Hydrides for Li-ion and Post Li Batteries
2.1.1. Metal Hydrides as Negative Electrode Material with Liquid Electrolyte
2.1.2. Promising Complex Metal Hydrides as Solid-State Electrolytes
Lithium Borohydride
Lithium Nitride and Lithium Hydride
Binary Phases of Hydrides with Lithium Halides
LiBH4-Li2NH: Li5(BH4)3NH—thorough characterization of a cluster complex hydride
Argyrodite Structure Materials
2.1.3. Application of Metal Hydrides in Solid-State Cells
Solid-State Half-Cell
A Full Solid-State Li-ion Cell
2.1.4. Conclusions
2.2. Na-Based Closo-Borates for Na Batteries
2.2.1. Na-Based Closo-Borates Solid Electrolyte
The Na2B12H12 Polymorphism
Nax+2y(CB11H12)x(B12H12)y Solid Electrolyte
2.2.2. Conclusions
3. Advances in Hydrogen Storage Materials
3.1. Pure Metal Hydrides (Mg, Pd, Ti)
3.2. Amide and Imide Based Systems for H2 Storage
3.2.1. Insights into Alkali-Based Amides and Imides Including Boron
LiBH4-LiNH2
LiNH2-Li2NH
3.2.2. Insights into the Structure and Reaction Mechanism of Metal Amide—Metal Hydride Composite Systems
Ammonolysis of Alkali and Alkaline-Earth Metal Amides
K-Mg-N-H System
KNH2-KH System
Rb-Mg-N-H and Rb-N-H Systems
3.2.3. Conclusions
3.3. Eutectic Metal Borohydride Systems
3.3.1. Experimental Study and Assessment of Eutectic Borohydride Systems
LiBH4-NaBH4
LiBH4-KBH4
NaBH4-KBH4
LiBH4-NaBH4-KBH4
Other Systems
3.3.2. Thermodynamic Properties of Eutectic Borohydride Systems
3.3.3. Hydrogen Sorage Properties of Eutectic Metal Borohydride Systems
3.3.4. Conclusions
3.4. Kinetic Tailoring of 2LiBH4 + MgH2/2LiH + MgB2 with Cost Effective 3TiCl3·AlCl3
→ 0.072LiCl(s) + 0.024Mg(s) + 0.006AlB2(s) + 0.018TiB2(s) + 0.036H2(g)
ΔG1bar, 25 °C = –10.9 kJ mol−1
ΔG1bar, 25 °C = –7.6 kJ mol−1
3.5. Role of Nanoconfinement in Enhancing the Properties of Hydrogen Storage Materials
3.5.1. Nanoconfinement Approaches
3.5.2. Confined Borohydrides
3.5.3. Conclusions
3.6. Rare Earth Borohydrides
3.6.1. Synthesis of Rare Earth Borohydrides (REB)
Solvent Free Synthesis of REB
Solvent-Based Synthesis of REB
3.6.2. Crystal Structures of Monometalic REB
3.6.3. Crystal Structures of Bimetallic REB
3.6.4. Reactive Hydride Composites with REB
3.6.5. Conclusions
4. Final Conclusions and Outlook
Author Contributions
Funding
Acknowledgments
Conflicts of Interest
References
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Cell Configuration | Maximum Capacity, mAh g−1 | Reversible Capacity at C-Rate | Reported Cycle Number | Retention Capacity, mAh g−1 at the Last Cycle | Reference |
---|---|---|---|---|---|
0.7MgH2 − 0.3TiH2│LiBH4│Li | 1950 | 90% at C/50 | 35 | 900 (51%) | [114] |
MgH2│LiBH4│Li | 1750 | 94% at C/20 | 50 | 924 (45%) | [105] |
TiH2│LiBH4│Li | 1052 | 86% at 2.5C | 50 | 878 (82%) | [108] |
25Al2O3 − 75MgH2│80Li2S − 20P2S5│Li | 3300 | 50% at | 9 | 580 (17.6%) | [106] |
Systems | Constituents | Eutectic Mixture | Reference | ||||
---|---|---|---|---|---|---|---|
Tmp1 | Tmp2 | Tmp3 | Tmp | Tdec | ρg | ||
0.62LiBH4-0.38NaBH4 | 280 | 510 | - | 225 | 300 | 14.5 | [237,246,247] |
0.71LiBH4-0.29NaBH4 | 280 | 510 | - | 219 | n.a. | 15.2 | [247] |
0.725LiBH4-0.275KBH4 | 280 | 605 | - | 105 | 420 | 13.2 | [238,245] |
0.68NaBH4-0.32KBH4 | 510 | 605 | - | 460 | 465 | 9.4 | [248] |
0.66LiBH4-0.11NaBH4-0.23KBH4 | 280 | 510 | 605 | 102 | n.a. | 13.0 | [249] |
0.55LiBH4-0.45Mg(BH4)2 | 280 | 280 | - | 180 | 250 | 16.1 | [244,250,251] |
0.68LiBH4-0.32Ca(BH4)2 | 280 | 370 | - | 200 | 350 | 14.5 | [236,252] |
0.45NaBH4-0.55Mg(BH4)2 | 510 | 280 | - | 205 | 360 | 13.4 | [252,253] |
Composition | ΔHmEXP | ΔHmASS | ΩASS | Reference |
---|---|---|---|---|
LiBH4 | 7.200 | [202] | ||
NaBH4 | 16.900 | [275] | ||
KBH4 | 19.200 | [249] | ||
0.70LiBH4 0.30NaBH4 | 6.990 | 6.520 | −19.604 * | [249] |
0.725LiBH4 0.275KBH4 | 11.025 | 9.828 | −13.016 | [249] |
0.682NaBH4 0.318KBH4 | 17.028 | 15.331 | 1.056 | [249] |
M2 | M1 | M1M2(BH4)n M1M2(BH4)nClz | Structure | Structural Prototype | Investigated Application, Reference |
---|---|---|---|---|---|
La | Li | c-LiLa(BH4)3Cl | Spinel | Li ion conductivity, [63,391] | |
c-LiLa(BH4)3Br | Spinel | Li ion conductivity, [411] | |||
c-LiLa(BH4)3I | Spinel | Li ion conductivity, [411] | |||
Na | o-NaLa(BH4)4 | Pbcn | New | Hydrogen storage, [412] | |
K | m-K3La(BH4)6 | P21/n | rt-Na3AlF6 | Hydrogen storage, [412] | |
Ce | Li | c-LiCe(BH4)3Cl | Spinel | Li ion conductivity, [394,413] | |
Na | o-NaCe(BH4)4 | Pbcn | Own | Hydrogen storage, [401] | |
K | m-K3Ce(BH4)6 | P21/n | rt-Na3AlF6 | Hydrogen storage, [414] | |
Rb | m-Rb3Ce(BH4)6 | P21/n | rt-Na3AlF6 | not specified, [415] | |
Pr | Li | c-LiPr(BH4)3Cl | Spinel | not specified, [391] | |
Na | o-NaPr(BH4)4 | Pbcn | Own | Hydrogen storage, [401] | |
Nd | Li | c-LiNd(BH4)3Cl | Spinel | not specified, [391] | |
Sm | Li | c-LiSm(BH4)4Cl | Spinel | not specified, [391] | |
K | o-KSm(BH4)3 | P21cn | CdTiO3 | Hydrogen storage, [416] | |
Rb | o-RbSm(BH4)3 | Pbn21 | CdTiO3 | Hydrogen storage, [416] | |
Cs | o-CsSm(BH4)3 | P22121 | NaNbO3 | Hydrogen storage, [416] | |
Eu | Rb | o-RbEu(BH4)3 | Pbn21/Pna21 | CdTiO3 | not specified, [415] |
Cs | t-CsEu(BH4)3 | P4/mbm | NaNbO3 | Luminescence, [415] | |
Gd | Li | c-LiGd(BH4)3Cl | Spinel | Li ion conductivity, [63,391] | |
K | m-KGd(BH4)4 | P21/c | LiMnF4 | Magneto-calorimetry, [417] | |
m-K2Gd(BH4)5 | P21/m | Own | Magneto-calorimetry, [417] | ||
m-K3Gd(BH4)6 | P21/n | rt-Na3AlF6 | Magneto-calorimetry, [417] | ||
c-Cs3Gd(BH4)6 | (NH4)3AlF6 | Magneto-calorimetry, [415] | |||
Ho | K | o-KHo(BH4)4 | Cmcm | ht-CrVO4 | not reported, [403] |
Y | Li | t-LiY(BH4)4 | CuAlCl4 | Li ion conductivity, [418,419] | |
Na | o-NaY(BH4)4 | C2221 | ht-CrVO4 | Na ion conductivity, [418,419] | |
m-NaY(BH4)2Cl2 | P2/c | MgWO4 | not specified, [420] | ||
K | o-KY(BH4)4 | Cmcm | ht-CrVO4 | not specified, [421] | |
m-KY(BH4)4 | C2/c | rt-LaNbO4 | not specified, [422] | ||
Rb | o-RbY(BH4)4 | Pnma | BaSO4 | not specified, [422] | |
m-RbY(BH4)4 | P21/c | AgMnO4 (deformed BaSO4) | not specified, [423] | ||
c-Rb3Y(BH4)6 | (NH4)3AlF6 | not specified, [415,422] | |||
Cs | c-CsY(BH4)4 | I41/a | CaWO4-scheelite | not specified, [423] | |
c-Cs3Y(BH4)6 | (NH4)3AlF6 | not specified, [415,422] | |||
Er | Na | o-NaEr(BH4)4 | Cmcm | ht-CrVO4 | Hydrogen storage, [401] |
K | o-KEr(BH4)4 | Cmcm | ht-CrVO4 | not specified, [424] | |
Yb | Li | c-LiYb(BH4)3Cl | CuAlCl4 | not specified, [392] | |
Na | o-NaYb(BH4)4 | Cmcm | ht-CrVO4 | not specified, [425] | |
K | o-KYb(BH4)4 | Cmcm | ht-CrVO4 | not specified, [425] | |
c-KYb(BH4) |