Recent Development in Nanoconfined Hydrides for Energy Storage
Abstract
:1. Introduction
2. Characterization Methods: Old, New, and Their Pitfalls
3. Bulk vs. Nanomaterials
3.1. Physical and Chemical Aspects of Nanoconfinement Effects
3.2. Nanocomposites
4. Types of Hosts Used as Hydride Matrix
4.1. Siloxanic Materials (MCM-41, SBA-15, SBA-48, etc.)
4.2. Carbonaceous Materials (C-Replica of Mesoporous Silica, C-NTs, C-Foam, C-Spheres, Graphene, Graphene Oxide GO, Reduced Graphene Oxide r-GO)
4.3. Metal-Organic Frameworks (MOFs) and Functionalized-MOFs
4.4. Main Group and TM (Transition Metal)-Oxides, Sulfides and Nitrides
4.5. Metal Component/Host
4.6. Gas Selective-Permeable Polymers
4.7. MXene
4.8. Catalytic Effects of Doping the Host and/or Substitution of the Hydride Species
4.9. (Nano)Catalyst Addition
5. Inclusion Methods of Hydride Materials into Appropriate Host—State-of-the-Art and Limitations
5.1. Direct Synthesis
5.2. Infiltration Methods
5.2.1. Melt Infiltration
5.2.2. Solvent Infiltration
5.2.3. Solvent-Assisted Ball-Milling
6. Metal Hydrides and Their Recent Nanoconfinement Studies
6.1. LiH
6.2. MgH2
6.3. AlH3
6.4. TM-Hydrides
7. Conclusions and Outlook
Funding
Institutional Review Board Statement
Informed Consent Statement
Data Availability Statement
Acknowledgments
Conflicts of Interest
References
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Silica Type | Hydrogen Storage Material | Nanoconfinement Method | Ref. |
---|---|---|---|
MSU-H | LiBH4 | solvent infiltration | [16] |
MCM-41 | NaBH4 | melt impregnation | [74] |
MCM-41, SBA-15 | LiBH4 | melt impregnation | [87] |
poly(acryalamide)-grafted mesoporous silica nanoparticles (PAM-MSN) | NH3BH3 (AB) | melt impregnation | [88] |
SBA-15 | Li2(BH4)(NH2). | melt impregnation | [89] |
silica aerogel | NH3BH3 (AB) | aerogel drying and AB gas antisolvent precipitation | [90] |
MCM-41, SBA-15 | LiBH4-LiNH2 | melt infiltration | [91] |
Carbon Type | Hydrogen Storage Material | Nanoconfinement Method | Ref. |
---|---|---|---|
MOFs incorporating activated carbon (AC) and aluminum doping | AlH3 | solution impregnation method | [40] |
Hollow carbon spheres (HCNs) | M(BH4)x (M = Li, Na, Mg, Ca) | solvent impregnation (best results, lower Td), melt infiltration | [42] |
Carbon aerogels with different porosities | Mg/MgH2 | direct solvent-based synthesis of MgH2 from MgBu2 | [53] |
Core-shell CoNi@C | MgH2 obtained by hydriding combustion synthesis (HCS) | high energy ball milling under Ar atmosphere | [65] |
Graphene | NaAlH4 | solvent infiltration (THF; bottom-up strategy (90% loading) | [69] |
Porous hollow carbon nanospheres | LiBH4-Mg(BH4)2 eutectic (LMBH) | melt-infiltration | [70] |
xNi-CMK-3; N-CMK-3 (x = 1 and 5 wt.%) | MgH2 | in situ generated from MgBu2 soln. in heptane | [92] |
Double-Layered Carbon Nanobowl | LiBH4 | melt infiltration | [93] |
Carbon shell (2–3 nm thick) | Mg/MgH2 | reactive gas evaporation | [94] |
TiO2-decorated amorphous carbon (AC) | MgH2 | ball milling | [95] |
High Surface Area Graphite (HSAG) | LiAlH4 | solvent infiltration/incipient wetness method | [96] |
Porous carbon, High Surface Area Graphite (HSAG-500) | Mg2CoH5 | bottom-up approach (Co2+ salt reduction, MgBu2 hydrogenation and solid-gas reaction Co + 2MgH2 + 0.5H2) | [97] |
Graphene | MgH2 | solvent-free, MgBu2 thermal decomposition | [98] |
Resorcinol-formaldehyde carbon aerogel (RFC) | 2LiBH4-LiAlH4 | two-step melt-infiltration | [99] |
Activated charcoal (AC) | LiBH4 | melt-infiltration | [100] |
NiCo2O4-anchored reduced graphene oxide (NiCo2O4@rGO) | LiAlH4 | low-temperature solution method coupled with annealing treatment; to yield NiCo2O4@rGO nanocomposites | [101] |
Nickel@nitrogen-doped carbon spheres (Ni@NCS) | MgH2 | hydriding combustion and subsequent high-energy ball milling | [102] |
Ultrathin, flexible Graphene (GR) | MgH2 | bottom-up self-assembly strategy (from MgBu2 in C6H12) | [103] |
Porous Hollow Carbon Nanospheres (PHCNSs) | LiBH4 | mortar grounded, then melt infiltration (300 °C, 30 min, 100 bar H2) | [104] |
Electrochemically synthesized reduced graphene oxide (erGO) | Mg-B | ball milling | [105] |
Fe3O4@C, Multifunctional porous scaffold of carbon wrapped ultrafine Fe3O4 | LiBH4 | melting infiltration (300 °C, 30 min, 100 bar H2) | [106] |
Activated carbon nanofibers (ACNF) impregnated with TiO2 | LiBH4 | mortar grinding (1:1, wt.), melt infiltration (310 °C at 5 °C/min rate under 60 bar H2, dwelling at 310 °C for 45 min, cooling to rt) | [108] |
Carbon nanotube (CNT) | xMgH2/AlH3 (x = 1–4) | ball milling (200 rpm, 1 h, under H2 atmosphere) for xMgH2/AlH3; ball milling in steel container (1 h, under H2 atmosphere) for MgH2/AlH3@CNTs | [109] |
Carbon nanoscaffolds (Graphite, CMK-3, Graphene, CNT) | MgH2 | solvent, melt infiltration | [110] |
N-doped CMK-3 carbon (NCMK-3) | LiAlH4 | solution infiltration of LiAlH4 freshly recrystallized from diethyl ether | [111] |
N-doped graphene hydrogels (resorcinol-formaldehyde) | LiBH4 | ball milling (300 min, 400 rpm), melt impregnation (30 min, 300 °C, 60 bar H2) | [112] |
N-Doped Graphene-Rich Aerogels Decorated with Ni and Co Nanoparticles | LiBH4 | pre-mixing (mortar, pestle; 30 min), then melt impregnation (30 min, 300 °C, 60 bar H2). | [113] |
Graphene sheets (G) | LiH (LiBH4, LiNH2BH3) | one-step solvothermal reaction of butyllithium supported by graphene in cyclohexane under a H2 pressure of 50 atm. | [114] |
Graphene Nanosheet (G) | MgH2 | solid-state reaction (metathesis MgCl2, LiH), ball milling (30 h, 0.5 MPa H2, 500 rpm) | [115] |
Activated mesoporous carbon (MC-a) | Ca(BH4)2 | incipient wetness method (0.1 M Ca(BH4)2.MTBE methyl tert-butyl ether, anhydrous) | [116] |
Edge-Functionalized Graphene Nanoribbon (GNRs): unfunctionalized cGNR, nitrogen edge-doped N2-cGNR and N4-cGNR, and fluorenone GNR (f-cGNR) | Mg(/MgH2) | Rieke-like reaction (up to 98% Mg wt.%) | [117] |
Ultrafine Ni nanoparticles dispersed on porous hollow carbon nanospheres (PHCNSs) | MgH2 (Mg2Ni/Mg2NiH4) | ball-milling (50 bar H2, 24 h, planetary ball mill QM-3SP4, Nanjing, 500 rpm, ball-to-sample weight ratio of 120:1) | [118] |
Hydrogenated graphene (HG) | N/A | Li-reduction in graphene(G), then CH3OH hydrogenation | [119] |
Graphene decorated with Ni nanocrystals | LiBH4 | solvothermal reaction (50 bar H2 at 100 °C, 24 h, continuous stirring); nBuLi hydrogenation (to LiH) and C6H15NBH3 reaction (to LiBH4-C6H15N); Cp2Ni (for Ni) | [120] |
Defected graphene oxide (GO) or reduced graphene oxide (rGO) | Mg/MgH2 | in situ generation of Mg from a THF soln. of Cp2Mg | [121] |
Reduced graphene oxide (rGO)/Li foil | Mg/MgH2 | direct solvent-based synthesis of MgH2 from MgCp2 | [122] |
Carbon Matrix | LiBH4 | melt-impregnation | [123] |
1D Carbon Matrix (Fishbone Shaped): CNF, GNF | Mg/MgH2 | direct solvent-based synthesis of MgH2 from sonicated, solvent(THF)-impregnated MgCp2-CNF/GNF | [124] |
Nickel-Containing Porous Carbon Sheets (Ni-PCSs) | LiAlH4, NaAlH4, and Mg(AlH4)2 | pre-mixing in mortar (15 min.), high energy ball-milling (SPEX M8000 mixer/mill, 15 min.) w/ball-to-powder weight ratio 40:1. | [125] |
Reduced graphene oxide (rGO) | Mg(BH4)2 | in situ generation of rGO/Mg(BH4)2: rGO slurry with 1 M MgBu2 in heptane, added over BH3·S(CH3)2. | [126] |
MWCNT (w/TiO2 2 mol% relative to NaAlH4) | NaAlH4 | physical mixture; PEIS/MWCNT/NaAlH4; polyaniline (Pani) or sulfonated polyetherimide (PEIS) as polymer matrices | [127] |
Nitrogen-Doped Nanoporous Carbon Frameworks (N-doped NPC) | NaAlH4 | pre-mixing (mortar/pestle, 10 min), melt infiltration (Sievert apparatus, 190 bar H2, 45 min, 200 °C) | [128] |
Graphene oxide (GO) framework | NaAlH4 | incipient wetness impregnation | [129] |
Activated carbon (AC) | 2LiBH4-MgH2 | milling 2LiBH4:Mg in stainless-steel vial planetary ball mill; 20:1 ball-to-powder weight ratio (BPR), 10 h milling time, 580 rpm | [130] |
Ordered mesoporous carbon structures (CMK) | N/A (Ni NP) | Ni NPs inserting by wetting the CMK structures | [131] |
ultrafine Ni nanoparticles in a mesoporous carbon matrix (MC-Niinsitu) | Mg(BH4)2 | Mg(BH4)2 (45 wt.%) solution (THF, Et2O) slowly impregnated into the MC variant | [132] |
High surface area graphite (HSAG) | LiH | catalytic hydrogenation of lithium naphthalenide (for LiH), stirring at 400 rpm, 0.35 MPa H2, 40 °C, aged overnight. | [133] |
Fe-benzenetricarboxylate (Fe-BTC) | NaAlH4 | solution infiltration using tetrahydrofuran (THF) | [134] |
Activated carbon nanofibers (ACNF) | LiBH4-LiAlH4 | solution impregnation of LiAlH4 (Et2O) then melt infiltration of LiBH4 (310 °C, 110 bar H2, 45 min.) | [135] |
Carbon aerogel (CA) by resorcinol (R) and formaldehyde (F) process | N/A | triethylamine (as catalyst) | [136] |
3-D activated carbon (M-3D C) | MgH2 | solvent-reduction (NH2NH2) of a slurry MgBu2 (1 M, heptane) in M-3D C | [137] |
Reduced graphene oxide (rGO)/metal nanocrystal multilaminates | Mg/MgH2 | solution-based co-reduction method of MgCp2/GO with lithium naphthalenide solution (2 h stirring, then 20 min centrifuged @10,000 rpm) | [138] |
ZIF-67-Derived Co@Porous Carbon | NH3BH3 (AB, Ammonia Borane) | infiltration | [139] |
Carbon nanotube arrays (CMK-5) | AlH3 and NH3BH3 | pre-mixed (mortar, hand-milling); solvent (THF) infiltration into CMK-5. | [140] |
carbon nanomaterials MDC (based on calcined MOF-5) | NH3BH3 | solvent infiltration | [141] |
Ice templating sheets of graphene oxide (GO) or partially reduced graphene oxide (rGO) | NH3BH3 | solvent infiltration (AB infiltrated to a solvent suspension of GO) | [142] |
Bio-derived micro/mesoporous carbon with well-organized pores (TiO2/B co-catalysts) | NH3BH3 | solvent immersion (AB methanol solution into C-TiO2(B)), then vaporization | [143] |
Microporous carbon (ECMC, narrow PSD, obtained by CVD from ethylene-filled Zeolite EMC-2) | NH3BH3 | solvent infiltration (of AB methanol solution to ECMC) | [144] |
V2O3-supported cubic C-nanoboxes | MgH2 | ball milling (500 rpm, 24 h, BPR:120:1, 50 bar H2). | [146] |
MOF Type | Hydrogen Storage Material | Nanoconfinement Method | Ref. |
---|---|---|---|
Cu-BDC(DMF) (BDC = benzenedicarboxylate; DMF-dimethylformamide, used as removal/capping solvent) | AB (NH3BH3) | hand grinding (5 min, under Ar); AB: Cu-BDC(DMF) weight ration: 1:20, based on pore filling estimation | [39] |
MIL-101-NORIT-RB3 decorated (an activated carbon AC added in situ during synthesis of MOF) | AlH3 | solvent impregnation (THF, under Ar) | [40] |
Various MOFs (of type MOF-5, MIL, UiO, ZIF, IRMOF etc.) | Pg/PdH2 | Various: Liquid impregnation, Metal-Organic Chemical Vapour Deposition; Sol-Gel; Double Solvent Method | [68] |
HKUST-1, IRMOF-1, IRMOF-10, UiO-66, UiO-67, and MIL-53(Al), MIL-101, MOF-74(Mg) | AB (NH3BH3), NaAlH4, MHx (M = Li, Na, Mg, Ca, Al) | solvent- and melt infiltration | [86] |
Nb2O5@MOF (Zn-based MOF, ZIF-8 (Zn(2-methylimidazole)2)) | MgH2 | ball milling (400 rpm, 4 h, ball to powder ratio 40:1) yielding MgH2@7 wt.% Nb2O5@MOF | [147] |
MOF-5, MOF-177, HKUST-1, NOTT-100, Mg-IRMOF-74-I, NiIRMOF-74-I, Mg-IRMOF-74-II and Ni2(mdobdc) | Mg/MgH2; Ni/NiH2 | Hydrogen release/uptake in Ni-based MOFs | [148] |
Ni-MOF scaffold (Ni2(TMA), TMA-trimasic acid) | MgH2 | in-situ synthesis; infiltration of MgBu2 (1 M in heptane) in Ni-MOF porosity, hydrogenation (453 K, 4.8 MPa H2, 20 h) to yield MgH2@Ni-MOF | [149] |
UiO-66 (Zr6O4(BDC)6, BDC = 1,4-benzenedicarboxylate) | Ti(BH4)3 | gas adsorption of Ti(BH4)3 at dry-ice conditions (N2-carrier gas) into UiO-66 | [150] |
UiO-67bpy (Zr6O4(OH)4(bpydc)6 with bpydc2– = 2,2′-bipyridine-5,5′-dicarboxylate) | Mg(BH4)2 | solvent impregnation | [151] |
Various (High-throughput molecular simulations) | N/A | theoretical study (machine learning) | [152] |
IRMOF-1, IRMOF-10, UiO-66, UiO-67, and MIL-53(Al) | AB (NH3BH3) | solvent infiltration (CH3OH) | [153] |
MIL-53 | AB (NH3BH3) | incipient wetness impregnation method (CH3OH saturated solution) | [154] |
MIL-101-NH2 (Al) | Al/AlH3 | solvothermal treatment involving N,N-dimethylformamide (DMF) as solvent | [155] |
MOF-5 | M/MHx | post-confinement, in-situ confinement, double-solvent method (better efficiency) | [156] |
MOF = ZIF-8, ZIF-67, MOF-74 | Mg/MgH2 | in situ reduction in Mg2+-decorated MOFs by NpLi solution in THF | [157] |
Metal Oxide/Sulfide/Nitride | Hydrogen Storage Material | Nanoconfinement Method | Ref. |
---|---|---|---|
CoS nano-boxes (ZIF-67-derived) | MgH2 | infiltration MgBu2 (1 M in heptane; 1000 rpm, 48 h), followed by hydrogenation (453 K, 4.8 MPa H2, 24 h) | [80] |
Al-SBA-15, γ -Al2O3 | LiBH4-LiNH2 | melt infiltration | [91] |
Metal oxide nanoparticles (TiO2) anchored on amorphous carbon (SCNPs/AC) | MgH2 | in-situ pyrolysis assisted with quickly cooling | [95] |
NiCo2O4-anchored reduced graphene oxide (rGO) | LiAlH4 | low-temperature solution method coupled with annealing treatment; to yield NiCo2O4@rGO nanocomposites | [101] |
Fe3O4@C, Multifunctional porous scaffold of carbon wrapped ultrafine Fe3O4 | LiBH4 | melting infiltration (300 °C, 30 min, 100 bar H2) | [106] |
Nb2O5@MOF (Zn-based MOF, ZIF-8 (Zn(2-methylimidazole)2)) | MgH2 | ball milling (400 rpm, 4 h, ball to powder ratio BPR 40:1) yielding MgH2@7 wt.% Nb2O5@MOF | [147] |
Ni/CoMoO4 nanorods | MgH2 | ball milling (400 rpm, BPR: 60:1, 6 h); MgH2 is the host for NiCoO4/NiMoO4 nanorods to yield MgH2-10 wt.% Ni/CoMoO4 | [158] |
Al2O3 | γ-Mg(BH4)2 | Atomic Layer Deposition (ALD) | [159] |
B2O (Metal-Decorated Honeycomb Borophene Oxide) | Li/LiH; Na/NaH and K/KH. | Theoretical study: dispersion corrected density functional theory (DFT-D2) | [160] |
Al2O3 | LiBH4-LiI | melt infiltration (50 bar H2, 295 °C, 3 °C min−1, 30 min); 4LiBH4:LiI–manual grinding in mortar, added to Al2O3 (130% pore filling) | [161] |
(3D) boron nitride (BN) | AB (NH3BH3) | solvent impregnation of AB (6.92 M in THF) into mBN1000 and mBN1450 | [162] |
TiO2 (anatase) | MgH2 | crystal-facet-dependent catalysis ({001} and {101}) | [172] |
Metal as Host or Component | Hydrogen Storage Material | Nanoconfinement Method/Obs. | Ref. |
---|---|---|---|
Al | Al/AlH3@MIL-101-NORIT-RB3 decorated | solvent impregnation | [40] |
Pd | Pd@MOF | Various: Liquid impregnation, Metal-Organic Chemical Vapour Deposition; Sol-Gel; Double Solvent Method | [68] |
TiCx/Mg | Mg/MgH2 | reactive gas evaporation | [94] |
N-doped graphene | LiBH4 | ball milling | [112] |
Mg nanocrystals | Mg/MgH2@GO; Mg/MgH2@rGO | LiNp reduction in Cp2Mg/(r)GO slurry in THF. Various degrees of GO reduction (to rGO) to fine tune H2 storage properties by morphology modification of Mg confined in xGO/(1-x)rGO matrix. | [121] |
Mg | Mg/rGO | One-step growth of Mg particles; chemical reduction in Cp2Mg by Li-methyl-naphtalenide (LiNpMe) in THF, followed by addition of the reactive mixture over single layer GO (30 min sonication). Mg w/high-index {21̅1̅6} crystal surface exhibits increased hydrogen absorption up to 6.2 wt %. | [122] |
Mg | GO/Mg/MgH multilaminates | solution-based co-reduction method of MgCp2/GO with NpLi | [138] |
Mg@(rGO/Ni) | Mg/MgH2 | in situ reduction in (Cp2Mg and Cp2Ni)@GO,THF-sonicated slurry, with a THF sol. of LiN; 6.5 H2 wt.% of total composite; H2 uptake under 1 bar H2. | [163] |
Pd | Pd-Based Alloy Nanoparticles *RhPd-H NPs); PdH0.43 NPs (when np Pd used, control experiment) | one-pot solvothermal method-reduction of acetylacetonates Pd(acac)2 and Rh(acac)3 in mixed benzyl alcohol /acetaldehyde solvents with polyvinylpyrrolidone (PVP), at 180 °C in 30 min. RhPd confirmed by EDX. (111) diffraction peak outside that of either Rh/Pd, implying an expanded structure due to interstitial H atoms. | [164] |
Mg (as matrix) | Mg/MgH2 | (review) of solid-state processing: physical vapor deposition, powder blending and consolidation, and additive manufacturing. | [165] |
Raney Ni (3 nm pore size) as host | NaAlH4 to form NaAlH4/Raney Ni | wet impregnation | [166] |
Al/Ti (Ti-based doped porous Al scaffold) | NaAlH4/Al | melt-infiltrated | [167] |
Co | 2MgH2-Co (Mg2CoH5 and Mg6Co2H11) | compression to pellets (4.43 wt.% hydrogen storage) vs. powder (2.32 wt.% capacity) | [168] |
Mg | MgH2 and ETM hydrides (ScH2, YH3, TiH2, ZrH2, VH and NbH) | mechanochemistry under hydrogen gas; 5 mol% of Early Transition Metals (ETM = Sc, Y, Ti, Zr, V, and Nb) as hydrogenation catalysts | [169] |
Mg–Ti | Mg–Ti–H nanoparticle.(MgH2 andTiH2 crystalline phases) | gas-phase condensation of Mg and Ti vapors under He/H2 atmosphere | [170] |
Ni | AB/Ni matrix | NiCl2 reduction to Ni(0) on the surface of AB nanoparticles (1–7 nm) | [171] |
H2-Permeable Polymers | Hydrogen Storage Material | Nanoconfinement Details | Ref. |
---|---|---|---|
poly(acrylamide) (PAM)-grafted mesoporous silica nanoparticles (MSNs) | ammonia borane (AB) | solution infiltration (stirring of THF solution of AB and polymer for 2 h), to produce AB-PAM-COOH-MSNs and AB-PAM-COOHMSNs | [88] |
polyaniline (Pani) or sulfonated polyetherimide (PEIS) as polymer matrices | NaAlH4 | PEIS/NaAlH4 (70/30 wt.%): solution infiltration of NaAlH4 added over dispersed MWCNTs in NMP-solubilized PEIS (30 min, 40 °C). Pani/NaAlH4: dispersion of components (50 wt.%), w/2 mol.% TiO2 as catalyst | [127] |
mesoporous polystyrene | various metal hosts | post-confinement strategy | [156] |
Adaptive TPX™ Polymer Scaffold | Li-RHC (2LiH + MgB2 + 7.5(3TiCl3·AlCl3)) | ball milling of 2LiH + MgB2 + 7.5 (3TiCl3·AlCl3) and a solution of TPXTM in cyclohexane | [173] |
PTFE polytetrafluoroethylene; PMMA poly(methyl-methacrylate) | Pd or Pd70Au30 alloy | Pd@PTFe, Pd70Au30@PTFe, (Pd@PTFE@PMMA) acting as (tandem) sensors | [174] |
short-chain polyethylene oxide (PEO or PEG) | AB (NH3BH3) | slow interaction of AB and PEO powders (microscope slide, 10 months. rt) forms ammonia borane–polyethylene oxide cocrystal (5 PEO monomers per AB molecule) | [175] |
MXene Type | Hydrogen Storage Material | Nanoconfinement Method | Ref. |
---|---|---|---|
TiCX | Mg/MgH2 | reactive gas evaporation method | [94] |
Ti3C2Tx (T = surface termination: OH, O or F) | Ni@C spheres | in situ confinement strategy | [156] |
Ti3C2Tx (T = F) | N/A | hydrogen trapping (physisorption, chemisorption, and Kubas type particle interaction) | [176] |
Multilayer Ti3C2 (ML-Ti3C2) | MgH2 | ball milling MgH2 + ML − Ti3C2 | [177] |
Ti3C2 | LiAlH4 | ball milling LiBH4-Ti3C2 (1 wt.%, 3 wt.%, 5 wt.%, 10 wt.%, and 15 wt.%); (planetary ball mill Retsch PM 400, under Ar, 250 rpm, 10 h, BPR 250:1); doping strategy to LiAlH4, yielding LiAlH4 + 5 wt.% Ti3C2 | [178] |
Ti3C2 | 4MgH2-LiAlH4 | mechanical milling 4MgH2-LiAlH4 with additive Ti3C2 (10 wt.%) in planetary ball mill (24 h, 450 rpm, BPR 40:1, under Ar), forming 4MgH2-LiAlH4-Ti3C2 nanocomposites | [179] |
Ti3C2 | LiH + MgB2 | ball milling | [180] |
Nb4C3Tx | MgH2 | ball milling MgH2-5 wt.%Nb4C3Tx; chemical exfoliation of Nb4C3Tx | [181] |
Cr2C | N/A | First-principles studies (7.6 wt.% H2) | [182] |
Ti3C2 | NaAlH4 | NaAlH4-7 wt.% Ti3C2 | [183] |
(Ti0.5V0.5)3C2 | MgH2 | MgH2-10 wt.% (Ti0.5V0.5)3C2 | [184] |
Ti3C2 | LiBH4 | 40% Ti3C2 composite | [185] |
Ti3C2 | NaH/Al (Ti-doped NaAlH4) | NaH/Al–Ti3C2 | [186] |
Ti3C2 | Mg(BH4)2 | Mg(BH4)2-40 wt.% Ti3C2 composite | [187] |
C@TiO2/Ti3C2 | NaAlH4 | annealing Ti3C2 MXene under C2H2 atmosphere; 10 wt.% C@TiO2/Ti3C2 catalyzing NaAlH4 | [188] |
Ti3C2 | Mg(BH4)2 | ball-milling method; Mg(BH4)2–40Ti3C2 | [189] |
NbTiC solid-solution MXene | MgH2 | MgH2-9 wt.% NbTiC | [190] |
Ti3C2 | 2LiH + MgB2/2LiBH4 + MgH2 (RHC-system) | ball milling | [191] |
Ti3C2/TiO2(A)-C | MgH2 | ball milling; sandwich-like Ti3C2/TiO2(A)-C prepared by gas–solid method | [192] |
Ti3C2 | Mg/MgH2 | ball milling (50 bar H2, 24 h) producing MgH2-x wt.% Ti3C2 nanocomposites (x = 0, 1, 3, 5 and 7) | [193] |
Ti2N | N/A | first-principles calculations; 2.656–3.422 wt.% hydrogen storage capacity, ambient conditions | [194] |
Host Doping/Hydride Substitution | Hydrogen Storage Material | Nanoconfinement Method | Ref. |
---|---|---|---|
Alkali/Alkaline Earth Metals (AM) | hydrides of lightweight elements (HLEs) | development of AM amide-hydride composites | [19] |
Pd | Pd/PdHx@MOF | complex interaction Pd…H | [68] |
metal (Ni) or non-metal (N)-doping of carbon scaffold | MgH2 | xNi-CMK-3; N-CMK-3 (x = 1 and 5 wt.%) | [92] |
Ni@N-doped carbon spheres | MgH2 | hydriding combustion and subsequent high-energy ball milling | [102] |
Nitrogen-Doped Carbon Host | LiAlH4 | solution infiltration | [111] |
N-doped graphene in resorcinol-formaldehyde | LiBH4 | ball milling, melt impregnation | [112] |
N-Doped Graphene-Rich Aerogels Decorated with Nickel and Cobalt Nanoparticles | LiBH4 | melt impregnation | [113] |
Edge-Functionalized Graphene Nanoribbon N2-cGNR, N4-cGNR, and fluorenone GNR (f-cGNR) | Mg(/MgH2) | Rieke-like reaction (up to 98% Mg wt.%) | [117] |
Ni-Containing Porous Carbon Sheets | LiAlH4, NaAlH4, and Mg(AlH4)2 | high energy ball-milling | [125] |
Nitrogen-Doped Nanoporous Carbon Frameworks | NaAlH4 | melt infiltration | [128] |
Bipyridine-Functionalized MOF (UiO-67bpy) | Mg(BH4)2 | solution infiltration, stirring (DMS dimethyl sulfide solution of Mg(BH4)2, RT, 2 h) | [151] |
Li, Na, and K decorations on 2D honeycomb B2O | N/A | theoretical study: dispersion corrected density functional theory (DFT-D2) | [160] |
Al2O3 | LiBH4-LiI | partial anion substitution in the complex borohydride | [161] |
Ni, Cr and Mn/GO | Mg | in-situ reduction Cp2Mg, and each transition metal precursor (Cp2Ni) dissolved in THF (22.5 mL) added into GO solution, stirred for 30 min. Hydrogen absorption (125 °C, 15 bar H2)/desorption (300 °C, 0 bar) Ni-doped rGO–Mg | [163] |
Nitrogen doping | Nb | Suppression of nano-hydride growth on Nb(100) | [195] |
Pd | Mg NPs; Pd@Mg NPs | Rieke method–co-reduction/precipitation of a Pd2+:Mg2+ = 1:9 wt. ration (chloride source) in THF, using LiNp as reductant to form Pd@Mg NPs | [196] |
Pd/Halloysite Nanotubes (HNTs) | AB (NH3BH3) | AB encapsulation and thin layer coating of the scaffold Pd/HNTs by solvent infiltration and solvent evaporation (THF) to yield AB@Pd/HNTs. Strong electrostatic adsorption (SEA) of ([Pd(NH3)4]2+) is onto the external surface of HNTs, precursor reduction (H2, 250 °C) to form (Pd/HNTs). | [197] |
Hydrogen Storage Class | Hydrogen Storage Material | (Nano)Catalyst Utilized | Ref. |
---|---|---|---|
Li-based | LiBH4 | TiO2 (activated carbon nanofibers); N-Doped Graphene-Rich Aerogels Decorated with Ni and Co NPs; Nano-synergy catalyst; Ti3C2 | [108,113,120,185] |
LiAlH4 | Nickel-Containing Porous Carbon Sheets | [125] | |
Na-based | NaAlH4 | Ti; Nickel-Containing Porous Carbon Sheets; Raney Ni; Al; 2D titanium carbide; Ti-based 2D MXene; Two-dimensional C@TiO2/Ti3C2 | [82,125,166,167,183,186,188] |
Mg-based | Mg NPs, films | Pd; Ti | [196,211,212] |
MgH2 | VTiCr; catalysts (review); nanocatalysts; anatase TiO2; core-shell CoNi@C; TiMn2; Carbon scaffold modified by metal (Ni) or non-metal (N); nickel@nitrogen-doped carbon spheres; ultrafine Ni nanoparticles dispersed on porous hollow carbon nanospheres; Nb2O5 NPs @MOF; Ni/CoMoO4 nanorods; Co; (Ti0.5V0.5)3C2; ultrafine NbTi nanocrystals, from NbTiC solid-solution MXene; sandwich-like Ti3C2/TiO2(A)-C; FeCo nanosheets; flake Ni nano-catalyst composite; Transition metal (Co, Ni) nanoparticles wrapped with carbon; TiH2 thin layer; MgCCo1.5Ni1.5; MgCNi3; supported Co–Ni Nanocatalysts | [34,43,57,60,65,77,92,102,118,147,158,168,184,190,192,201,202,204,205,208,209,210] | |
MgB2 | LiH + TiH2 | [198] | |
Mg(BH4)2 | ultrafine Ni NPs; Ti3C2; various additives | [132,187,189,207] | |
Mg(AlH4)2 | Ni-Containing Porous Carbon Sheets | [125] | |
Al-based | α-AlH3 | TiF3; Li3N | [203,206] |
RCH | 2LiH + MgB2 | Ti3C2 | [191] |
2LiBH4 − MgH2 | ZrCl4 | [134,191] | |
AB | NH3BH3 | ZIF-67-Derived Co@Porous Carbon; TiO2(B) NPs; Pd/Halloysite Nanotubes; | [139,143,197] |
Misc. | Pd | Pd@MOF | [68,200] |
B2O | Li, Na, and K-Decorated | [160] | |
Various hydrides | Alkali/Alkaline Earth Metals; Highly Dispersed Supported Transition Metal; metallic NPs supported on carbon substrates; Heterostructures | [19,20,131,199] | |
Carbon aerogel | N-Doped Graphene-Rich Aerogels Decorated with Ni and Co NPs; ZrCl4; NEt3 | [113,134,136] | |
Ti2N MXene | Pristine (DFT) | [194] |
Additive Used | Other H-Storing Source | H-Storing Composite | wt.% H2 | Obs. | Ref. |
---|---|---|---|---|---|
G(graphene) | (LiBH4 and LiNH2BH3 after B2H6 and BH3NH3 reaction) | LiH@G (LiH nanospheres, 2 nm thick | 6.8 wt.% (50 wt.% LiH in LiH@G); 12.8 wt.% (69.1 wt.% LiBH4@G) | LiH@G Tonset = 445 °C, Td ≈ 500 °C (6.8 wt.%). LiNH2BH3@G Tonset = 53 °C, 15 °C lower than for bulk LiNH2BH3; Td ≈ 79 °C. LiBH4@G Tonset = 346 °C (124 °C lower than that for bulk), 12.8 wt.%. Li2B12H12 apparent in XRD after 4 cycles (LiBH4@G). | [114] |
TiCl4.2THF | HSAG | LiH@HSAG | 1.9 wt.% (340 °C, one step) | Hydrogenation of LiNp(THF) under 0.35 MPa H2, 400 rpm, 40 °C, 12 h (cat.:TiCl4.2THF) | [133] |
N/A (TiH2) | MgB2 | LiH/MgB2 | not investigated | different “top” and “bottom” fractions present in vial. At 700 bar H2, 280 °C, 24 h, borohydride formation. | [198] |
Activator: hν (light) to Au NPs | N/A (Au) | Au/LiH | 11.1 wt.% (as-synthesized); 8.2 wt.% (heat desorption); 3.4 wt.% (light desorption) | plasmonic heating effect of Au NPs (100 °C), under Xe lamp radiation | [214] |
LiNH2 | (Li3N) | LiNH2 + 2LiH | 10.5 wt.% | Li3N + 2H2 = Li2NH + LiH + H2 = LiNH2 + 2LiH. 2LiNH2 = Li2NH + NH3 | [215] |
- | - | LiH | 12.6 wt.% | LiH = Li + 1/2 H2Tm = 689 °C; Td = 720 °C | [216] |
Si | - | LiH | 5 wt.% | Li:Si = 2.35:1; Td = 490 °C | [216] |
Co(OH)2 | - | Li@SiO2@Co(OH)2 | N/A | αLiOH + 2αLi+ + 2αe- = α Li2O + αLiH (0 < α < 1); High Li+ storage in anode | [217] |
Additive/Host Used | Other H-Storing Source | H-Storing Nanocomposite | wt.% H2 | Obs. | Ref. |
---|---|---|---|---|---|
4 carbon aerogels, 15 < Davg < 26 nm, surface area 800 < SBET < 2100 m2/g, and total pore volume, 1.3 < Vtot < 2.5 cm3/g | Mg/MgH2 | MgH2@C (MgH2 loading: 17–20 vol%, 24–40 wt.%) | 3.06 (Mg_CX1); degrades to 1.9 (Mg_CX1, 4th cycle, stable); | Mg(C4H9)2(s) + 2H2(g) ! MgH2(s) + 2C4H10(g) 5 cycles des./abs. at 355 °C, 15 h (vacuup/des., 50 bar H2/abs.) Mg_CX1, Mg_CX2 – 0.046 wt.%H2/min (best result in this study). Highlights the importance of conducting des/abs cycles (different results obtained for “conditions 1 and 2”). | [53] |
Mg-B | Mg-B/MgH2/ MgB12H12/Mg(BH4)2 | Mg-B (MgB0.75) | N/A (abs., 280 °C, 700 bar H2, MgB0.75), N/A (abs., 380 °C, 700 bar H2, MgB2), | nanoscale Mg–B material (MgB0.75) made by surfactant ball milling MgB2 in a mixture of heptane, oleic acid, and oleylamine | [55] |
core-shell CoNi@C | CoNi: 2 coupled H-pumps: Mg2Co/Mg2CoH5 and Mg2Ni/Mg2NiH4, | MgH2-8 wt.% CoNi@C | 5.83 (275 °C, 1800 s); 6.17 (300 °C, 1800 s); 6 (150 °C, 200 s) | 173 °C dehydrogenation onset for MgH2-8 wt.% CoNi@C. Excellent thermal conductivity of the nanocomposite due to C-shell. Ea, des = 78.5 kJ mol−1. | [65] |
TiMn2 | Mg/MgH2 | MgH2/10 wt.% TiMn2 | 5.1 (reversible, 225 °C, 100 s, 10 barH2/abs; 400 s, 0.2 bar H2/des.) | cold pressing technique; potential for PEM fuel cell applications. Ea,des = 82.9 kJ mol−1; Ea,abs = 19.3 kJ mol−1. 414 cycles within 600 h continuously without degradations (hydrogen flow at an average rate of 150 mL/min) | [77] |
Ni | Ni4B3 intermediate confirmed by XRNES | Ni-doped-2LiBH4–MgH2 in graphene | 0.47 (0.48 theoretical) | ball milling 2LiBH4-MgH2-Ni/C (x = 0, 5, 10, 15). Heterogeneous nucleation of MgNi3B2. X-ray absorption near-edge structure (XRNES) used to probe intermediate Ni4B3 3LiBH4 + 4Ni = 3LiH + Ni4B3 + 4.5H2 | [78] |
CoS nano-boxes scaffold | Mg/MgH2; MgS-catalytic effect | MgH2@CoS-NBs | 3.17 (300 °C); 3.37 (400 °C) | hydriding and dehydriding enthalpies (−65.6 ± 1.1 and 68.1 ± 1.4 kJ mol−1 H2. hydriding and dehydriding (57.4 ± 2.2 and 120.8 ± 3.2 kJ mol−1 H2) | [80] |
Ni- or N-doped C scaffold: xNi-CMK-3 (x = 1 and 5 wt.%) and N-CMK-3 | Ni | MgH2@xNi-CMK-3; MgH2@ N-CMK-3 | 7.5 (MgH2@5Ni-CMK-3); 6.5 (MgH2@1Ni-CMK-3 and MgH2@N-CMK-3) at 200 °C, 2 h | Hydrogenation is faster at 300 °C, MgH2@5Ni-CMK-3, MgH2@1Ni-CMK-3 and MgH2@N-CMK-3 absorb 6 wt.% H2 in 10 min (6.5 wt.%, 2 h). Enhanced kinetics, Ea: MgH2@CMK-3 (125.3 ± 2.1 kJ mol−1); MgH2@N-CMK-3 (116.2 ± 1.8 kJ mol−1), MgH2@1Ni-CMK-3 (109.2 ± 1.3 kJ mol−1), MgH2@5Ni-CMK-3 (107.6 ± 1.2 kJ mol−1) | [92] |
Mg-TiCX@C | TiCx | Mg-TiCX@C | 4.5 (des., 60 min, 300 °C); 5.5 (abs., 25 min, 250 °C) | TiCX-decorated Mg nanoparticles (NPs) in 2–3 nm carbon shells through a reactive gas evaporation method. Mg88(TiC0.6)12@C best results. Stable after 10 hydrogenation/dehydrogenation cycles at 250/300 °C. | [94] |
Monodispersed single-crystal-like TiO2 with amorphous carbon | - | Mg@C-TiO2 | 6.5 (des. 275 °C, 10 min.); 6.5 (abs., 200 °C, 5 min) | reductions in hydrogen desorption temperature (163.5 °C) and Ea (69.2 kJ mol−1). The sample can be fully rehydrogenated with a reversible capacity of 6.5 wt.% at 200 °C within 5 min. | [95] |
Graphene nanosheet (GN) | - | MgH2@GN-40wt.% | 4.5 (reversible, 6 cycles, 300 °C) | Ea = 80.8 kJ mol−1 (des., 0.01 atm H2) MgH2 size tunable by adjusting MgBu2/G wt. ratio before hydrogenation | [98] |
nickel@nitrogen-doped carbon spheres | Ni/Mg2NiH4 | MgH2–Ni@NCS | 4.3 (des.), 5.7 (abs.) in 8 min, 350 °C; 4.2 (abs., 60 min, 100 °C) | high-energy ball milling process; negligible degradation after 10 cycles. In situ formed Mg2NiH4 induced dehydrogenation of MgH2 and prevented Mg agglomeration. | [102] |
AlH3@CNT | AlH3 | MgH2/AlH3@CNT | 8.20 (des., 1 h, 200 °C); 5.61 (abs., 0.16 h, 250 °C) | CNTs: high specific surface area (550 m2 g−1), small diameter (6–8 nm), afford 60–80 nm crystal size nanocomposite MgH2/AlH3@CNT nanoparticles, releases H2 at ~71 °C. | [109] |
Graphene Nanosheet GNS | - | MgH2 –10 wt.% GNS | 5.1 (des., 20 min, 325 °C); 5.2 (abs., 10 min, 250 °C) | well-dispersed MgH2 nanoparticles (~3 nm); confinement effect of graphene | [115] |
ultrafine Ni nanoparticles dispersed on porous hollow carbon nanospheres | Mg2Ni/Mg2NiH4 | Ni loading up to 90 wt.% in composite catalyst; MgH2-5 wt.% (90 wt.%Ni-10 wt.%CNS) | 6.4 (reversible). 6.2 (des. 30 min, 250 °C; abs., 250 s, 150 °C) | Des. onset (190 °C) and des. peak (242 °C). Reversible capacity of 6.4 wt.% achieves after 50 cycles at a moderate cyclic regime. | [118] |
Graphene oxide (GO), reduced graphene oxide (rGO) | - | MgH2@GO, MgH2@rGO (rGO50, rGO100, and rGO200) | 6.25 (200 °C, 15 bar H2, MgH2@GO) | role of graphene defects; rGO is detrimental, as Ea is lower on defected GO. MgH2@rGO: disturbed diffusion pathway of hydrogen atoms caused by the coalesced morphology | [121] |
Reduced graphene oxide (rGO) | Mg/MgH2 | Mg/rGO | 6.2 (des., 2 h, Mg{21̅1̅6}) 5.1 (des, 2 h, (random)Mg/rGO) | preferential orientation of Mg/rGA nanocomposites was investigated: Mg growth on {0001} and {21̅1̅6} planes of rGO Mg (21̅1̅6) stabilizes hydrogen absorption thermodynamics | [122] |
1D Carbon Matrix, fishbone shaped (CNF) | - | Ultrathin Mg Nanosheet @ 1D-C | 6 (abs., 1 h, no catalyst, 200–250 °C); 6 (des, 1.5 h, 200–325 °C) | 90% of the total capacity is absorbed within 1 h at all temperatures and desorbed within 1.5 h | [124] |
AC activated carbon | LiBH4 | 2LiBH4-MgH2 @AC (LB-MH-AC) | 5.7 (theoretical); 2.56–4.55 (350 °C, abs. under 30–40 bar H2) | melt infiltration of hydride in AC (400 °C, 40–50 bar H2, 10 h) improvement of thermal conductivity of materials and temperature control system could alleviate wt.% decrease | [130] |
ZrCl4- doped carbon aerogel scaffold (CAS) | 2LiBH4–MgH2 | 2LiBH4–MgH2@ ZrCl4-CAS x wt.% (x = 50, 67, 75) | 5.4 (5.7, theoretical, x = 50); 3.4 (3.8 th., x = 67); 2.5 (2.9 th., x = 75) at 301–337 °C | melt infiltration technique. Up to 97 and 93% of theoretical H2 capacity released and reproduced, respectively. 2LiBH4 + MgH2 = 2LiH + MgB2 + 4H2 (350–500 °C) | [134] |
3-D activated carbon with TM dispersion (Co, Fe, and Ni) | TM/(TM)Hx | MgH2@3D-AC (MHCH) | 6.63 (abs., 5 min, 180 °C, for Ni-MHCH-5); 6.55 (des., 75 min, 180 °C) | TEA ((HOCH2CH2)3N)/NH2NH2 reduction in nBu2Mg-infiltrated 3D-C. MgH2 embedded in 3D-AC with periodic synchronization of transition metals (MHCH). Excellent long-term cycling stability over ~435 h for MHCH-5. Ni more efficient than Co or Fe. | [137] |
nano-TiO2@C | Mg/MgH2 | MgH2-10 wt.% TiO2@C | 6.5 (7 min, 300 °C, des.); 6.6 (10 min, 140 °C, abs.) | 10 wt.% nanocrystalline TiO2@C weakens the Mg-H bond, thus lowering desorption temperature | [146] |
Nb2O5@MOF | Nb2O5@MOF | 7 wt.% Nb2O5@ MOF doped MgH2 | 6.2 (6.3 min, 250 °C; 2.6 min, 275 °C) | Desorption onset: 181.9 °C. Ea = 75.57 ± 4.16 kJ mol−1 Absorption: 4.9 wt.% (6 min, 175 °C); 6.5 wt.% (6 min, 150 °C); Ea = 51.38 ± 1.09 kJ mol−1 Capacity loss: 0.5 wt.% after 30 cycles | [147] |
Ni-MOF (7.58 nm, 0.46 cm3g−1) | Mg2Ni/Mg2NiH4 | MgH2@Ni-MOF | 4.03 abs-3.94 des (325 °C); 4.02 abs-3.91 des (350 °C); 3.95 abs = 3.87 des (375 °C). The Ni-MOF contribution (physisorption): 0.91 (325 °C); 0.85 (350 °C), 0.97 (375 °C), 0.88 (300 °C). | The abs/des plateau pressure: 4.63 atm/3.45 atm (325 °C). thermodynamics (−65.7 ± 2.1 and 69.7 ± 2.7 kJ mol–1 H2 for ab-/desorption, respectively) and kinetics (41.5 ± 3.7 and 144.7 ± 7.8 kJ mol−1 H2 for ab-/desorption, respectively) of Mg/MgH2 in the MgH2@Ni-MOF composite. The Ni-MOF scaffold acts as “aggregation blocker”. shortened H diffusion distance results in the ultrafast H diffusion rate in the nanosized Mg/MgH2. (C4H9)2Mg + 2H2 → MgH2 + 2C4H10 (g) 2(C4H9)2Mg + Ni(Ni-MOF) + 4H2 → Mg2NiH4 + 4C4H10 (g) Mg2NiH4 = Mg2Ni + 2H2 (g) | [149] |
(Ni/Co)MoO4 nanorods | Mo/Mg2Ni/Mg2NiH4 | MgH2-10 wt.% NiMoO4 MgH2-10 wt.% CoMoO4 | 7.41 (319.4 °C, MgH2) 6.51 (243.3 °C, MgH2-10 wt.% NiMoO4) 6.49 (277.6 °C, MgH2-10 wt.% Co-MoO4) from TPD up to 400 °C, 3°/min. 6 (des., MgH2-NiMoO4, 10min, 300 °C) 5.5 (abs., MgH2-NiMoO4, 10 min, 300 °C, 31.6 atm H2) | Ni/CoMoO4 were doped into MgH2 ball milling method at 400 rpm with a ball-to-powder ratio of 60:1 for 6 h. superior promoting effect of NiMoO4 over CoMoO4; NiMoO4 reacts with MgH2 during the first dehydrogenation to in situ form Mg2Ni and Mo0, Mg2Ni/Mg2NiH4′ mutual transformation upon hydrogen release/uptake is the well-known ‘hydrogen pump’. Mo0 played for the hydrogen storage in MgH2: (i) it accelerates the hydrogen de/absorption of MgH2 through weakening the Mg–H bonding; (ii) it facilitates the mutual ‘Mg2Ni/Mg2NiH4′. No tdn effect: ΔHabs./ΔHdes of −71.14/78.25 close to that of pure MgH2: −72.42/74.08 kJ mol−1 | [158] |
Co | Mg2CoH5 and Mg6Co2H11 | 2MgH2-Co | 4.43 (pellet); 2.32 (powder) | high pressure compacting in pellet doubles H2 storage | [168] |
ScH2, YH3, TiH2, ZrH2, VH and NbH | Mg/MgH2 | 0.95 MgH2–0.05 (TM)Hx | ≥5 wt.% | (TM)Hx crystallite size of ∼10 nm, obtained by mechanochemistry (RMB, reactive ball milling) MgH2 + TM (Sc, Y, Ti, Zr, V, Nb) under H2 pressure. Early Transition Metals (ETM) chosen by the known stability of their respective hydrides under normal conditions. | [169] |
BiphasicMgH2/TiH2 within Mg–Ti–H NP | Mg/MgH2 | Mg–x at.%Ti–H NPs Mg-14Ti-H and Mg-63Ti-H (26–10 nm) | 4 (x = 7); 2.2 (x = 35); 0.8 (x = 63) abs, full at 150 °C. | Equilibrium data for H2 ab-/de-sorption by Mg/MgH2 at low 100–150 °C range. Fast H2 release from MgH2 at 100–150 °C (no Pd catalyst). The free energy change at the TiH2/Mg interface induces MgH2 destabilization. Hydrogen uptake (100 s) and release (1000 s, 0.1…0.2 wt.%/min) for Mg–x at.%Ti–H NPs. | [170] |
TiO2 (anatase) | TiO2/Mg | MgH2-TiO2 | 2.70 (abs, 500 s, 100 °C.); 4.5 (abs, 100 °C. 120 min); 5.3 (abs., 44 s, 200 °C) for MgH2-5 wt.% TF70: | Influence of TiO2 facets {001} and {101}: MgH2-TiO2{001} superior properties. Ea,des = 76.1± 1.6 kJ mol−1 for MgH2-TF70 | [172] |
Multilayer Ti3C2 (ML-Ti3C2) | Ti3C2 | MgH2 + x wt.% ML-Ti3C2, x = 4, 6, 8, 10 | 6.45 (des.; 240 °C, 10 min.) 1.95–3.63 (des.; 140 °C, in 10–60 min). 6.47 (abs. 150 °C); 4.20 (abs., 75 °C) | Ti3C2 was introduced into MgH2 by ball milling. ML-Ti3C2 prepared in-house, by chemical exfoliation. | [177] |
Ti3C2 | Mg/MgH2 | MgH2-x wt.% Ti3C2 (x = 0, 1, 3, 5 and 7) | 6.2 (x = 5; 1 min, 300 °C, des.); 6.1 (x = 5; 30 s, 150 °C) | MgH2-5 wt.% Ti3C2 shows excellent dehydrogenation/hydrogenation kinetics (chargind/discharging in <1 min) | [193] |
Pd | Pd/PdHx; Mg-Mg6Pd | Mg@Pd: γ-MgH2, PdH0.706 | 3 (abs, 50 °C, 2 h) | Mg NPs (40–70 nm). Ea,des = 93.8 kJ/mol at 216.8 °C; Ea,des = 44.3 kJ/mol at 50 °C. ΔHdes = 72.7 kJ/mol; ΔHabs = −71.5 kJ/mol. Pd-Mg alloy important role. | [196] |
FeCo nanosheets | FeCo (50nm) | FeCo-catalyzed MgH2 | 6 (des., 9.5 min, 300 °C), 6.7 (abs, 1 min, 300 °C); 3.5 (abs, 10 min, 150 °C) | Ea,des = 65.3 ± 4.7 kJ mol−1 (60 kJ mol−1 reduction from pristine MgH2) Ea,abs = 53.4 ± 1.0 kJ mol−1 | [201] |
flake Ni nano-catalyst composite | Mg2Ni/Mg2NiH4 | MgH2 + 5 wt.% Ni | 6.7 (des., 3 min, 300 °C). 4.6 (125 °C, 20 min, 29.6 atm H2) | Ea, des = 71 kJ mol−1; Ea,abs = 28.03 kJ mol−1. | [202] |
TM (Co, Ni) nanoparticles wrapped with carbon | Mg2Ni/Mg2NiH4 | MgH2-6%Ni/C | 6.1 des. at 250 °C; 5.0 (abs., 100 °C, 20 s) | dehydrogenation temperature 275.7 °C. Absorption/desorption stability with respect to both capacity (up to 6.5 wt.%) and kinetics (within 8 min at 275 °C for dehydrogenation and within 10 s at 200 °C for rehydrogenation | [204] |
TiH2 | - | MgH2-TiH2 | 6.45 (DFT) | MgH2/TiH2 interface is thermodynamically stable, and promotes the generation and diffusion of hydrogen. | [205] |
MgCCo1.5Ni1.5 | Mg2NiH4, MgC0.5Co3 and C catalysts (from MgCCo1.5Ni1.5) | Mg/MgH2-MgCCo1.5Ni1.5 | 6.1–6 (abs, 5 min, 350 °C, 1st cycle-10th cycle); 5.9-5.8 (des, 1st cycle-10th cycle) | ball-milling and hydriding combustion method. Desorbs H2 at 216 °C (onset). Ea,des = 39.6 kJ mol−1 | [208] |
MgCNi3 | MgCNi3 | MgH2-MgCNi3 | 4.42 (abs, 150 °C, 1200s) | Mg-MgCNi3 composite shows excellent cyclic stability with a 98% retention rate. | [209] |
Co–Ni Nanocatalysts | Mg/MgH2 | 0.95MgH2–0.5(CoNi(OH)x); Ni@G-doped MgH2; CoNi@G-doped MgH2 | 6.5 (des, Ni@G-doped MgH2, 45 min, 260 °C; or 25 min, 280 °C) | ball milling MgH2 and Co-Ni, 5 bar H2, 2 h, 400 rpm, 20:1 BPR. Co-subst. of Ni changes shape of catalyst (sphere-to-plate) and decreases catalytic efficiency. | [210] |
Mg-Ti-H nanoparticles | Mg/MgH2 | Mg-x Ti-H NPs (x = 14…63 at.%) | 4.2 (22 at.%Ti, at 100…150 °C) | gas phase condensation of mixed Mg-Ti vapors under H2. Ea,abs. 43…52 kJ/mol, the rate constant (150 °C) increases from 2.7×10−2 s−1 to 9.2×10−2 s−1 with increasing [Ti]. Hydrogen desorption: sequence of surface-limited (Ea = 32 kJ/mol) and contracting-volume kinetics, except at the highest Ti content where nucleation and growth is observed. kdes (at 150 °C) increases from 0.5–10−3 s−1 to 1.2×10−3 s−1 with [Ti]. The activation energy for H2 recombination is remarkably small (~32 kJ/mol) | [211] |
light activation, Au(HAuCl4) | - | Mg@Au, hν | 5.2 (350 °C, 3h, Mgbulk); 4.9 (350 °C, 3 h, MgH2-Au 5 wt.%) | Rehydrogenation at 12 h illumination, 14.8 atm H2. No H2 release at 100 °C, limited at 200 °C (0.7 wt.%) and at 300 °C (1wt.%) for Mg@Au 5 wt.%. | [214] |
- | - | ultrafine MgH2 | 6.7 (reversible; abs: 360 min, 30 °C; or 60 min, 85 °C, 30 bar H2); vol capacity: 65.6 gH2/L | novel metathesis process of liquid–solid phase driven by ultrasonication (2 h) was proposed from THF. Pressed into pellet under 200 MPa.Stable and rapid hydrogen cycling behavior in 50 cycles at 150 °C. Equilibrium pressure: 0.0304 (120 °C), 0.151 (160 °C), 1.014 (215 °C), 30-20-10 times higher than that of pristine MgH2. | [222] |
Mg(B3H8)2 | Mg(B3H8)2 | Mg(B3H8)2-MgH2 | 2.16 (93.6…138 °C) | Synergistic role in Mg(B3H8)2-MgH2 composite. No H2 release below 150° for the pristine components. | [224] |
Additive Used | Other H-Storing Source | H-Storing Composite | wt.% H2 | Obs. | Ref. |
---|---|---|---|---|---|
Al-doping (925 ppm), AC | AC@MOF (activated carbon@MOF) | Al@AC-MIL-101 | 0.55 (MIL-101)…1.74 (Al@AC-MIL-101) | Al/α-AlH3 hydrogenation release/uptake cycles ran at 298 K, and pressure < 100 bar H2 | [40] |
HSAG (high surface area graphite) | - | AlH3@HSAG | 0.25 (14.4 wt.%AlH3 by ICP-OES data, and only 15% of Al behaves reversibly) | H2 uptake commences at 60…270 °C (mean 150 °C, peak 165 °C) and 60 bar H2 pressure | [44] |
CTF-bipyridine (CTF-bipy) AlH3@CTF- | - | AlH3@CTF-bipyridine; AlH3@CTF-biph—no reversibility (bipyridyl group was compulsory) | 0.65, 0.58, 0.57 (2nd, 3rd, 4th cycles) | H2 desorption between 95…154 °C rapidly (completes at 250 °C) from AlH3@CTF-bipyridine composite. Reversible at 700 bar H2 and 60 °C (incomplete, 24 h). | [51] |
CNT | MgH2 | MgH2/AlH3@CNT | 8.2 (1 h, 200 °C, dehydrogenation); 5.61 (0.16 h, 250 °C) | CNT prevent aggregation and enhance MgH2-ALH3 interaction | [109] |
TiF3 | - | α-AlH3/LiCl-TiF3 (3:1:0.1 molar ratio) | 9.92 (80–160 °C, 750 s) | α-AlH3 obtained by milling of LiH and AlCl3. | [203] |
Li3N | Li3N | Li3N@AlH3 | 8.24 (100 °C); 6.18 (90 °C) and 5.75 (80 °C) | 10 wt.% doping of AlH3 with Li3N leads to ~8.0 wt.% H2 release at 100 °C. Nanoscale dispersion of the two hexagonal phases (AlH3, Li3N) by ball milling. Ea = 100.4 kL mol−1 (0.9 AlH3-0.1 Li3N) | [206] |
- | - | AlH3 | 10.0 (140 °C, 3600 s) | neat AlH3 (commercial) | [227] |
Al(OH)3 | - | core-shell α-AlH3@Al(OH)3 | 10.0 (140 °C, 1000 s) | α-AlH3@Al(OH)3 nanocomposite can be stored in air (7 days) | [227] |
Additive Used | Other H-Storing Souce | H-Storing Composite | wt.% H2 | Obs. | Ref. |
---|---|---|---|---|---|
porous carbon (HSAG) | Co | Mg2CoH5@HSAG Co + MgH2@HSAG | N/A | bottom-up approach affords PSD 2–50 nm (max. at 15 nm); wt.% H2 capacity decrease due to Mg oxidation. 2MgH2 + Co + ½ H2 → Mg2CoH5 MgH2 NPs: 5nm. Co@Mg NPs: 7 nm. Desorption temperature increases with cycle number (1..7) in a 5 wt.% Mg2CoH5@HSAG nanocomposite from ~590 to ~610 K. Possible disproportionation: Mg2CoH5 → MgH2 + Mg6Co2H11 | [97] |
ScH2, YH3, TiH2, ZrH2, VH and NbH | MgH2 | 0.95 MgH2–0.05 (TM)Hx | ≥5 wt.% | (TM)Hx crystallite size of ~10 nm, obtained by mechanochemistry (RMB, reactive ball milling) MgH2 + TM (Sc, Y, Ti, Zr, V, Nb) under H2 pressure. Early Transition Metals (ETM) chosen by the known stability of their respective hydrides under normal conditions. | [169] |
MOF | Ir, Rh | TM-H@MOF (TM = Pd, Ir, Rh) | 0.18H/Pd (cubes); 0.27H/Pd (octahedrons) | ΔHabs of the TM NPs change from endothermic to exothermic with decreasing particle size. Pd@HKUST-1 [copper(II) 1,3,5-benzenetricarboxylate (Cu3(BTC)2] abs. 0.87H/Pd compared to Pd(bulk, cubes, 0.5 H/Pd) | [200,234] |
Mg nanofilm | Mg | Pd NPs@Mg film | N/A | DHfilm ≈ 8 × 10−18 m2 s−1 | [212] |
- | - | TaHx (0 < x < 0.7) | <0.389 wt.% | higher H-sensing activity than Pd-alloy (10−2…10+4 Pa H2) | [216] |
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Comanescu, C. Recent Development in Nanoconfined Hydrides for Energy Storage. Int. J. Mol. Sci. 2022, 23, 7111. https://doi.org/10.3390/ijms23137111
Comanescu C. Recent Development in Nanoconfined Hydrides for Energy Storage. International Journal of Molecular Sciences. 2022; 23(13):7111. https://doi.org/10.3390/ijms23137111
Chicago/Turabian StyleComanescu, Cezar. 2022. "Recent Development in Nanoconfined Hydrides for Energy Storage" International Journal of Molecular Sciences 23, no. 13: 7111. https://doi.org/10.3390/ijms23137111