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Hydrogen Storage in Metal Hydrides and Related Materials

A special issue of Materials (ISSN 1996-1944). This special issue belongs to the section "Energy Materials".

Deadline for manuscript submissions: closed (20 March 2023) | Viewed by 12473

Special Issue Editors

Centre of New Technologies, University of Warsaw, ul. Banacha 2c, 02-097 Warsaw, Poland
Interests: functional materials; hydrogen storage; ammonia borane; amidoboranes; batteries; solid state electrolytes; impedance spectroscopy
Centre of New Technologies, University of Warsaw, ul. Banacha 2c, 02-097 Warsaw, Poland
Interests: functional materials; hydrogen storage; borohydrides; weakly coordinating anions; ion metathesis; solid state electrolytes
Rudjer Boskovic Institute, Bijenicka c. 54, HR-10000 Zagreb, Croatia
Interests: hydrogen storage; vibrational spectroscopy; in-situ spectroscopic techniques; solid-state synthetic methods; mechanochemistry; hydrogen bonding; materials chemistry

Special Issue Information

Dear Colleagues,

Hydrogen storage is currently one of the most challenging issues impeding the broad introduction of a hydrogen economy. Solid-state hydrogen-rich materials are considered promising storing media for releasing and absorbing gaseous hydrogen due to the high gravimetric and volumetric capacities they are able to reach. However, the desired materials exhibiting large hydrogen content, favorable thermodynamics and fast kinetics have not been obtained, despite significant efforts.

The current special issue of Materials by MDPI focuses on metal-boron-nitrogen based hydrogen storage materials, which comprise various families of compounds and composites, including, amongst others, borohydrides, ammonia borane, amidoboranes and their derivatives. This selection of materials is justified by their very high hydrogen content and relatively low temperature of hydrogen desorption, which can be tuned by adjusting their cationic and anionic composition and doping. Attention will be directed to novel hydrogen-rich systems, their synthesis, characterization and possible applications. However, the Issue will not be limited to these topics, and related submissions are welcome.

We greatly encourage submissions of both young and experienced researchers in order to facilitate a fruitful exchange of ideas.

Dr. Karol J. Fijałkowski
Dr. Tomasz Jaroń
Dr. Nikola Biliskov
Guest Editors

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Materials is an international peer-reviewed open access semimonthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2600 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • hydrogen storage
  • complex hydrides
  • boron compounds
  • borohydrides
  • amidoboranes
  • ammonia borane derivatives
  • fuel cells
  • inorganic synthesis methods
  • mechanochemistry

Published Papers (8 papers)

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Research

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12 pages, 2767 KiB  
Article
The Catalytic Effect of Vanadium on Sorption Properties of MgH2-Based Nanocomposites Obtained Using Low Milling Time
by Zorana Sekulić, Jasmina Grbović Novaković, Bojana Babić, Milica Prvulović, Igor Milanović, Nikola Novaković, Dragan Rajnović, Nenad Filipović and Vanja Asanović
Materials 2023, 16(15), 5480; https://0-doi-org.brum.beds.ac.uk/10.3390/ma16155480 - 05 Aug 2023
Viewed by 742
Abstract
The effects of catalysis using vanadium as an additive (2 and 5 wt.%) in a high-energy ball mill on composite desorption properties were examined. The influence of microstructure on the dehydration temperature and hydrogen desorption kinetics was monitored. Morphological and microstructural studies of [...] Read more.
The effects of catalysis using vanadium as an additive (2 and 5 wt.%) in a high-energy ball mill on composite desorption properties were examined. The influence of microstructure on the dehydration temperature and hydrogen desorption kinetics was monitored. Morphological and microstructural studies of the synthesized sample were performed by X-ray diffraction (XRD), laser particle size distribution (PSD), and scanning electron microscopy (SEM) methods, while differential scanning calorimetry (DSC) determined thermal properties. To further access amorph species in the milling blend, the absorption spectra were obtained by FTIR-ATR analysis (Fourier transform infrared spectroscopy attenuated total reflection). The results show lower apparent activation energy (Eapp) and H2 desorption temperature are obtained for milling bland with 5 wt.% added vanadium. The best explanation of hydrogen desorption reaction shows the Avrami-Erofeev model for parameter n = 4. Since the obtained value of apparent activation energy is close to the Mg-H bond-breaking energy, one can conclude that breaking this bond would be the rate-limiting step of the process. Full article
(This article belongs to the Special Issue Hydrogen Storage in Metal Hydrides and Related Materials)
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12 pages, 2900 KiB  
Article
The Preparation, Characterization, and Pressure-Influenced Dihydrogen Interactions of Tetramethylphosphonium Borohydride
by Tomasz Jaroń
Materials 2023, 16(15), 5334; https://0-doi-org.brum.beds.ac.uk/10.3390/ma16155334 - 29 Jul 2023
Viewed by 509
Abstract
Tetramethylphosphonium borohydride was synthesized via an ion metathesis reaction in a weakly-coordinating aprotic environment. [(CH3)4P]BH4, in contrast to related [(CH3)4N]+ compounds which tend to crystallize in a tetragonal system, adopts the distorted [...] Read more.
Tetramethylphosphonium borohydride was synthesized via an ion metathesis reaction in a weakly-coordinating aprotic environment. [(CH3)4P]BH4, in contrast to related [(CH3)4N]+ compounds which tend to crystallize in a tetragonal system, adopts the distorted wurtzite structure (P63mc), resembling some salts containing analogous ions of As and Sb. [(CH3)4P]BH4 decomposes thermally in several endo- and exothermic steps above ca. 240 °C. This renders it more stable than [(CH3)4N]BH4, with a lowered temperature of decomposition onset by ca. 20 °C and solely exothermic processes observed. Raman spectra measured at the 0–10 GPa range indicate that a polymorphic transition occurs within 0.53–1.86 GPa, which is further confirmed by the periodic DFT calculations. The latter suggests a phase transition around 0.8 GPa to a high-pressure phase of [(CH3)4N]BH4. The P63mc phase seems to be destabilized under high pressure by relatively closer dihydrogen interactions, including the C–H…H–C contacts. Full article
(This article belongs to the Special Issue Hydrogen Storage in Metal Hydrides and Related Materials)
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16 pages, 4868 KiB  
Article
The Effect of the Iridium Alloying and Hydrogen Sorption on the Physicochemical and Electrochemical Properties of Palladium
by Katarzyna Hubkowska, Małgorzata Pająk and Andrzej Czerwiński
Materials 2023, 16(13), 4556; https://0-doi-org.brum.beds.ac.uk/10.3390/ma16134556 - 24 Jun 2023
Cited by 1 | Viewed by 668
Abstract
Thin layers (up to 1 µm) of Pd-Ir alloys were electrodeposited from aqueous, galvanic baths of PdCl2 and IrCl3 mixtures. The morphology of the electrodeposits was examined by means of scanning electron microscopy. The composition of alloys was determined with the [...] Read more.
Thin layers (up to 1 µm) of Pd-Ir alloys were electrodeposited from aqueous, galvanic baths of PdCl2 and IrCl3 mixtures. The morphology of the electrodeposits was examined by means of scanning electron microscopy. The composition of alloys was determined with the use of energy-dispersive spectroscopy, atomic absorption spectrometry, X-ray photoelectron spectroscopy, and Auger electron spectroscopy. For the studies of the electrochemical properties of alloys, cyclic voltammetry, chronoamperometry, and chronopotentiometry were used. It was found that Pd-Ir alloy electrodes were surface-enriched with Pd. Pd-Ir alloys subjected to different electrochemical treatment involving hydrogen sorption changed their surface state. The continuous hydrogen sorption enhanced the Ir ions’ dissolution. The values of thermodynamic functions of hydrogen sorption in strong alkaline electrolytes were comparable with those in acidic electrolytes, whereas the kinetics of the process in alkaline medium was hindered. The miscibility gap in the Pd-Ir-H system vanished for the electrode containing ca. 93.7 at.% Pd. Full article
(This article belongs to the Special Issue Hydrogen Storage in Metal Hydrides and Related Materials)
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14 pages, 4598 KiB  
Article
In Situ Synthesis of NiFeLDH/A–CBp from Pyrolytic Carbon as High-Performance Oxygen Evolution Reaction Catalyst for Water Splitting and Zinc Hydrometallurgy
by Kai Che, Man Zhao, Yanzhi Sun and Junqing Pan
Materials 2023, 16(11), 3997; https://0-doi-org.brum.beds.ac.uk/10.3390/ma16113997 - 26 May 2023
Viewed by 1257
Abstract
Nickel–iron-layered double hydroxide (NiFeLDH) is one of the promising catalysts for the oxygen evolution reaction (OER) in alkaline electrolytes, but its conductivity limits its large-scale application. The focus of current work is to explore low-cost, conductive substrates for large-scale production and combine them [...] Read more.
Nickel–iron-layered double hydroxide (NiFeLDH) is one of the promising catalysts for the oxygen evolution reaction (OER) in alkaline electrolytes, but its conductivity limits its large-scale application. The focus of current work is to explore low-cost, conductive substrates for large-scale production and combine them with NiFeLDH to improve its conductivity. In this work, purified and activated pyrolytic carbon black (CBp) is combined with NiFeLDH to form an NiFeLDH/A–CBp catalyst for OER. CBp not only improves the conductivity of the catalyst but also greatly reduces the size of NiFeLDH nanosheets to increase the activated surface area. In addition, ascorbic acid (AA) is introduced to enhance the coupling between NiFeLDH and A–CBp, which can be evidenced by the increase of Fe-O-Ni peak intensity in FTIR measurement. Thus, a lower overvoltage of 227 mV and larger active surface area of 43.26 mF·cm−2 are achieved in 1 M KOH solution for NiFeLDH/A–CBp. In addition, NiFeLDH/A–CBp shows good catalytic performance and stability as the anode catalyst for water splitting and Zn electrowinning in alkaline electrolytes. In Zn electrowinning with NiFeLDH/A–CBp, the low cell voltage of 2.08 V at 1000 A·m−2 results in lower energy consumption of 1.78 kW h/KgZn, which is nearly half of the 3.40 kW h/KgZn of industrial electrowinning. This work demonstrates the new application of high-value-added CBp in hydrogen production from electrolytic water and zinc hydrometallurgy to realize the recycling of waste carbon resources and reduce the consumption of fossil resources. Full article
(This article belongs to the Special Issue Hydrogen Storage in Metal Hydrides and Related Materials)
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9 pages, 2330 KiB  
Article
Synthesis Method of Unsolvated Organic Derivatives of Metal Borohydrides
by Wojciech Wegner and Karol J. Fijalkowski
Materials 2022, 15(23), 8653; https://0-doi-org.brum.beds.ac.uk/10.3390/ma15238653 - 05 Dec 2022
Cited by 2 | Viewed by 985
Abstract
A new, scalable, wet-chemistry single-pot method of synthesising pure unsolvated organic derivatives of metal borohydrides is presented. The metathetic reaction in a weakly coordinating solvent is exemplified by the synthesis of [(n-C4H9)4N][Y(BH4)4] and [...] Read more.
A new, scalable, wet-chemistry single-pot method of synthesising pure unsolvated organic derivatives of metal borohydrides is presented. The metathetic reaction in a weakly coordinating solvent is exemplified by the synthesis of [(n-C4H9)4N][Y(BH4)4] and [Ph4P][Y(BH4)4] systems. For the latter compound, the crystal structure was solved and described. Organic borohydride salts obtained by the new method can find various applications, e.g., can be used as precursors in synthesis of hydrogen-rich mixed-metal borohydrides—promising materials for solid-state chemical storage of hydrogen. Full article
(This article belongs to the Special Issue Hydrogen Storage in Metal Hydrides and Related Materials)
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9 pages, 3868 KiB  
Article
Hydrogen Generation by Hydrolysis of MgH2-LiH Composite
by Xiaojuan Wu, Huaqing Xue, Yong Peng, Jifeng Deng, Zewei Xie, Jie Zheng, Xingguo Li and Shuan Li
Materials 2022, 15(4), 1593; https://0-doi-org.brum.beds.ac.uk/10.3390/ma15041593 - 21 Feb 2022
Cited by 14 | Viewed by 2303
Abstract
As a most promising material for hydrogen generation by hydrolysis, magnesium hydride (MgH2) is also trapped by its yielded byproduct Mg(OH)2 whose dense passivated layers prevent the further contact of intimal MgH2 with water. In this work, LiH, as [...] Read more.
As a most promising material for hydrogen generation by hydrolysis, magnesium hydride (MgH2) is also trapped by its yielded byproduct Mg(OH)2 whose dense passivated layers prevent the further contact of intimal MgH2 with water. In this work, LiH, as a destroyer, has been added to promote the hydrogen properties of MgH2. The results demonstrate that even 3 wt % LiH was added into MgH2-G, the hydrogen generation yield can increase about 72% compared to the hydrogen generation yield of MgH2-G. The possible mechanism is that Mg2+ from the hydrolysis of MgH2 preferentially bound with OH ions from the hydrolysis of LiH to form Mg(OH)2 precipitation, which is dispersed in water rather than coated on the surface of MgH2. Moreover, adding MgCl2 into hydrolysis solution, using ball milling technology, and increasing the hydrolysis temperature can make the hydrolysis rate higher and reaction process more complete. It is noted that a too high weight ratio of LiH with too high of a hydrolysis temperature will make the reaction too violent to be safe in the experiment. We determinate the best experimental condition is that the LiH ratio added into MgH2 is 3 wt %, the hydrolysis temperature is 60 °C, and the concentration of MgCl2 hydrating solution is 1 M. MgH2-LiH composite hydrogen generation technology can meet the needs of various types of hydrogen supply and has broad application prospects. Full article
(This article belongs to the Special Issue Hydrogen Storage in Metal Hydrides and Related Materials)
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12 pages, 1366 KiB  
Article
Synthesis, Polymorphism and Thermal Decomposition Process of (n-C4H9)4NRE(BH4)4 for RE = Ho, Tm and Yb
by Wojciech Wegner and Tomasz Jaroń
Materials 2021, 14(6), 1329; https://0-doi-org.brum.beds.ac.uk/10.3390/ma14061329 - 10 Mar 2021
Cited by 4 | Viewed by 1814
Abstract
In total, three novel organic derivatives of lanthanide borohydrides, n-But4NRE(BH4)4 (TBAREB), RE = Ho, Tm, Yb, have been prepared utilizing mechanochemical synthesis and purified via solvent extraction. Studies by single crystal and powder X-ray [...] Read more.
In total, three novel organic derivatives of lanthanide borohydrides, n-But4NRE(BH4)4 (TBAREB), RE = Ho, Tm, Yb, have been prepared utilizing mechanochemical synthesis and purified via solvent extraction. Studies by single crystal and powder X-ray diffraction (SC-XRD and PXRD) revealed that they crystalize in two polymorphic forms, α- and β-TBAREB, adopting monoclinic (P21/c) and orthorhombic (Pnna) unit cells, previously found in TBAYB and TBAScB, respectively. Thermal decomposition of these compounds has been investigated using thermogravimetric analysis and differential scanning calorimetry (TGA/DSC) measurements, along with the analysis of the gaseous products with mass spectrometry (MS) and with analysis of the solid decomposition products with PXRD. TBAHoB and TBAYbB melt around 75 °C, which renders them new ionic liquids with relatively low melting points among borohydrides. Full article
(This article belongs to the Special Issue Hydrogen Storage in Metal Hydrides and Related Materials)
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Review

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35 pages, 6080 KiB  
Review
Hydrogen Storage Performance of Mg/MgH2 and Its Improvement Measures: Research Progress and Trends
by Xinglin Yang, Wenxuan Li, Jiaqi Zhang and Quanhui Hou
Materials 2023, 16(4), 1587; https://0-doi-org.brum.beds.ac.uk/10.3390/ma16041587 - 14 Feb 2023
Cited by 9 | Viewed by 2974
Abstract
Due to its high hydrogen storage efficiency and safety, Mg/MgH2 stands out from many solid hydrogen storage materials and is considered as one of the most promising solid hydrogen storage materials. However, thermodynamic/kinetic deficiencies of the performance of Mg/MgH2 limit its [...] Read more.
Due to its high hydrogen storage efficiency and safety, Mg/MgH2 stands out from many solid hydrogen storage materials and is considered as one of the most promising solid hydrogen storage materials. However, thermodynamic/kinetic deficiencies of the performance of Mg/MgH2 limit its practical applications for which a series of improvements have been carried out by scholars. This paper summarizes, analyzes and organizes the current research status of the hydrogen storage performance of Mg/MgH2 and its improvement measures, discusses in detail the hot studies on improving the hydrogen storage performance of Mg/MgH2 (improvement measures, such as alloying treatment, nano-treatment and catalyst doping), and focuses on the discussion and in-depth analysis of the catalytic effects and mechanisms of various metal-based catalysts on the kinetic and cyclic performance of Mg/MgH2. Finally, the challenges and opportunities faced by Mg/MgH2 are discussed, and strategies to improve its hydrogen storage performance are proposed to provide ideas and help for the next research in Mg/MgH2 and the whole field of hydrogen storage. Full article
(This article belongs to the Special Issue Hydrogen Storage in Metal Hydrides and Related Materials)
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