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A special issue of Inorganics (ISSN 2304-6740). This special issue belongs to the section "Inorganic Solid-State Chemistry".

Deadline for manuscript submissions: closed (30 September 2017) | Viewed by 77130

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Prof. Dr. Torben R. Jensen

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Interdisciplinary Nanoscience Center and Department of Chemistry, Aarhus University, DK-8000 Aarhus C, Denmark
Interests: synthesis and characterization of inorganic materials; structural, chemical and physical properties; energy storage as hydrogen or electricity in novel types of batteries; multivalent solid state batteries
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Prof. Dr. Hai-Wen Li

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School of Advanced Energy, Sun Yat-Sen University, No.66, Gongchang Road, Guangming District, Shenzhen 518107, China
Interests: hydrogen storage; hydrogen energy; hydride; rechargeable battery materials
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Prof. Dr. Min Zhu

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School of Materials Science and Engineering, Key Laboratory of Advanced Energy Storage Materials of Guangdong Province, South China University of Technology, Guangzhou 510641, China
Interests: hydrogen storage; microstructure characterization; electrode materials for batteries; materials synthesis by plasma milling

Prof. Dr. Craig Buckley

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Physics and Astronomy, Curtin University, GPO Box U1987, Perth, WA 6845, Australia
Interests: hydrogen storage; energy storage materials; thermal energy storage materials; metal hydrides; thermodynamics
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Special Issue Information

Dear Colleagues,

Our extreme and growing energy consumption, based on fossil fuels, has significantly increased the levels of carbon dioxide, which may lead to global and irreversible climate changes. We have plenty of renewable energy, e.g., sun and wind, but the fluctuations over time and geography call for a range of new ideas, and possibly novel technologies. The most difficult challenge appears to be the development of efficient and reliable storage of renewable energy. Hydrogen has long been considered as a potential means of energy storage; however, storage of hydrogen is also challenging. Therefore, a wide range of hydrogen-containing materials, with energy-related functions, has been discovered over the past few decades. The chemistry of hydrogen is very diverse, and so also are the new hydrides that have been discovered, not only in terms of structure and composition, but also in terms of their properties. This has led to a wide range of new possible applications of metal hydrides that permeate beyond solid-state hydrogen storage. A variety of new hydrides, proposed as battery materials, has been discovered. These can exploit properties as fast ion conductors or as conversion-type electrodes with much higher potential energy capacities, as compared to materials currently used in commercial batteries. Solar heat storage is also an area of great potential with metal hydrides, in principle offering orders of magnitude better storage performance than phase change materials. Recently, hydrides with optical and superconducting properties have also been investigated. This Special Issue of Inorganics, entitled “Functional Materials Based on Metal Hydrides”, is dedicated to the full range of emerging electronic, photonic, and energy-related inorganic hydrogen-containing materials.

Prof. Dr. Torben R. Jensen
Associate Prof. Dr. Hai-Wen Li
Prof. Dr. Min Zhu
Prof. Dr. Craig Buckley
Guest Editors

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Keywords

Hydrides
Synthesis
Structural, chemical and physical properties
Functional energy materials
Hydrogen Storage
Ionic Conductivity
Battery Electrode
Metal hydride based batteries
Heat Storage
Optical Switch
Superconductivity

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Published Papers (14 papers)

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Editorial

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5 pages, 202 KiB

Open AccessEditorial

Functional Materials Based on Metal Hydrides

by Hai-Wen Li, Min Zhu, Craig Buckley and Torben R. Jensen

Inorganics 2018, 6(3), 91; https://doi.org/10.3390/inorganics6030091 - 4 Sep 2018

Cited by 14 | Viewed by 3818

Abstract

Storage of renewable energy remains a key obstacle for the implementation of a carbon free energy system. There is an urgent need to develop a variety of energy storage systems with varying performance, covering both long-term/large-scale and high gravimetric and volumetric densities for stationary and mobile applications. Novel materials with extraordinary properties have the potential to form the basis for technological paradigm shifts. Here, we present metal hydrides as a diverse class of materials with fascinating structures, compositions and properties. These materials can potentially form the basis for novel energy storage technologies as batteries and for hydrogen storage. Full article

(This article belongs to the Special Issue Functional Materials Based on Metal Hydrides)

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11 pages, 2620 KiB

Open AccessArticle

Interface Enthalpy-Entropy Competition in Nanoscale Metal Hydrides

by Nicola Patelli, Marco Calizzi and Luca Pasquini

Inorganics 2018, 6(1), 13; https://doi.org/10.3390/inorganics6010013 - 12 Jan 2018

Cited by 8 | Viewed by 4426

Abstract

We analyzed the effect of the interfacial free energy on the thermodynamics of hydrogen sorption in nano-scaled materials. When the enthalpy and entropy terms are the same for all interfaces, as in an isotropic bi-phasic system, one obtains a compensation temperature, which does not depend on the system size nor on the relative phase abundance. The situation is different and more complex in a system with three or more phases, where the interfaces have different enthalpy and entropy. We also consider the possible effect of elastic strains on the stability of the hydride phase and on hysteresis. We compare a simple model with experimental data obtained on two different systems: (1) bi-phasic nanocomposites where ultrafine TiH₂ crystallite are dispersed within a Mg nanoparticle and (2) Mg nanodots encapsulated by different phases. Full article

(This article belongs to the Special Issue Functional Materials Based on Metal Hydrides)

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1752 KiB

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Improvement in the Electrochemical Lithium Storage Performance of MgH₂

by Shuo Yang, Hui Wang, Liuzhang Ouyang, Jiangwen Liu and Min Zhu

Inorganics 2018, 6(1), 2; https://doi.org/10.3390/inorganics6010002 - 26 Dec 2017

Cited by 17 | Viewed by 3600

Abstract

Magnesium hydride (MgH₂) exhibits great potential for hydrogen and lithium storage. In this work, MgH₂-based composites with expanded graphite (EG) and TiO₂ were prepared by a plasma-assisted milling process to improve the electrochemical performance of MgH₂. The resulting MgH₂–TiO₂–EG composites showed a remarkable increase in the initial discharge capacity and cycling capacity compared with a pure MgH₂ electrode and MgH₂–EG composite electrodes with different preparation processes. A stable discharge capacity of 305.5 mAh·g⁻¹ could be achieved after 100 cycles for the 20 h-milled MgH₂–TiO₂–EG-20 h composite electrode and the reversibility of the conversion reaction of MgH₂ could be greatly enhanced. This improvement in cyclic performance is attributed mainly to the composite microstructure by the specific plasma-assisted milling process, and the additives TiO₂ and graphite that could effectively ease the volume change during the de-/lithiation process as well as inhibit the particle agglomeration. Full article

(This article belongs to the Special Issue Functional Materials Based on Metal Hydrides)

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809 KiB

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Lewis Base Complexes of Magnesium Borohydride: Enhanced Kinetics and Product Selectivity upon Hydrogen Release

by Marina Chong, Tom Autrey and Craig M. Jensen

Inorganics 2017, 5(4), 89; https://doi.org/10.3390/inorganics5040089 - 6 Dec 2017

Cited by 24 | Viewed by 4676

Abstract

Tetrahydofuran (THF) complexed to magnesium borohydride has been found to have a positive effect on both the reactivity and selectivity, enabling release of H₂ at <200 °C and forms Mg(B₁₀H₁₀) with high selectivity. Full article

(This article belongs to the Special Issue Functional Materials Based on Metal Hydrides)

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1755 KiB

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Microstructure and Hydrogen Storage Properties of Ti₁V_0.9Cr_1.1 Alloy with Addition of x wt % Zr (x = 0, 2, 4, 8, and 12)

by Salma Sleiman and Jacques Huot

Inorganics 2017, 5(4), 86; https://doi.org/10.3390/inorganics5040086 - 3 Dec 2017

Cited by 13 | Viewed by 4834

Abstract

The effect of adding Zr on microstructure and hydrogen storage properties of BCC Ti₁V_0.9Cr_1.1 synthesized by arc melting was studied. The microstructures of samples with Zr were multiphase with a main BCC phase and secondary Laves phases C15 and C14. The abundance of secondary phases increased with increasing amount of zirconium. We found that addition of Zr greatly enhanced the first hydrogenation kinetics. The addition of 4 wt % of Zr produced fast kinetics and high hydrogen storage capacity. Addition of higher amount of Zr had for effect of decreasing the hydrogen capacity. The reduction in hydrogen capacity might be due to the increased secondary phase abundance. The effect of air exposure was also studied. It was found that, for the sample with 12 wt % of Zr, exposure to the air resulted in appearance of an incubation time in the first hydrogenation and a slight reduction of hydrogen capacity. Full article

(This article belongs to the Special Issue Functional Materials Based on Metal Hydrides)

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13146 KiB

Open AccessArticle

Investigation of the Reversible Lithiation of an Oxide Free Aluminum Anode by a LiBH4 Solid State Electrolyte

by Jason A. Weeks, Spencer C. Tinkey, Patrick A. Ward, Robert Lascola, Ragaiy Zidan and Joseph A. Teprovich

Inorganics 2017, 5(4), 83; https://doi.org/10.3390/inorganics5040083 - 23 Nov 2017

Cited by 9 | Viewed by 4970

Abstract

In this study, we analyze and compare the physical and electrochemical properties of an all solid-state cell utilizing LiBH4 as the electrolyte and aluminum as the active anode material. The system was characterized by galvanostatic lithiation/delithiation, cyclic voltammetry (CV), X-ray diffraction (XRD), energy dispersive X-ray spectroscopy (EDS), Raman spectroscopy, electrochemical impedance spectroscopy (EIS), and scanning electron microscopy (SEM). Constant current cycling demonstrated that the aluminum anode can be reversibly lithiated over multiple cycles utilizing a solid-state electrolyte. An initial capacity of 895 mAh/g was observed and is close to the theoretical capacity of aluminum. Cyclic voltammetry of the cell was consistent with the constant current cycling data and showed that the reversible lithiation/delithiation of aluminum occurs at 0.32 V and 0.38 V (vs. Li⁺/Li) respectively. XRD of the aluminum anode in the initial and lithiated state clearly showed the formation of a LiAl (1:1) alloy. SEM-EDS was utilized to examine the morphological changes that occur within the electrode during cycling. This work is the first example of reversible lithiation of aluminum in a solid-state cell and further emphasizes the robust nature of the LiBH4 electrolyte. This demonstrates the possibility of utilizing other high capacity anode materials with a LiBH4 based solid electrolyte in all-solid-state batteries. Full article

(This article belongs to the Special Issue Functional Materials Based on Metal Hydrides)

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2606 KiB

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Dehydrogenation of Surface-Oxidized Mixtures of 2LiBH₄ + Al/Additives (TiF₃ or CeO₂)

by Juan Luis Carrillo-Bucio, Juan Rogelio Tena-García and Karina Suárez-Alcántara

Inorganics 2017, 5(4), 82; https://doi.org/10.3390/inorganics5040082 - 21 Nov 2017

Cited by 8 | Viewed by 3632

Abstract

Research for suitable hydrogen storage materials is an important ongoing subject. LiBH₄–Al mixtures could be attractive; however, several issues must be solved. Here, the dehydrogenation reactions of surface-oxidized 2LiBH₄ + Al mixtures plus an additive (TiF₃ or CeO₂) at two different pressures are presented. The mixtures were produced by mechanical milling and handled under welding-grade argon. The dehydrogenation reactions were studied by means of temperature programmed desorption (TPD) at 400 °C and at 3 or 5 bar initial hydrogen pressure. The milled and dehydrogenated materials were characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), and Fourier transformed infrared spectroscopy (FT-IR) The additives and the surface oxidation, promoted by the impurities in the welding-grade argon, induced a reduction in the dehydrogenation temperature and an increase in the reaction kinetics, as compared to pure (reported) LiBH₄. The dehydrogenation reactions were observed to take place in two main steps, with onsets at 100 °C and 200–300 °C. The maximum released hydrogen was 9.3 wt % in the 2LiBH₄ + Al/TiF₃ material, and 7.9 wt % in the 2LiBH₄ + Al/CeO₂ material. Formation of CeB₆ after dehydrogenation of 2LiBH₄ + Al/CeO₂ was confirmed. Full article

(This article belongs to the Special Issue Functional Materials Based on Metal Hydrides)

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3177 KiB

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Thermodynamic Properties and Reversible Hydrogenation of LiBH₄–Mg₂FeH₆ Composite Materials

by Guanqiao Li, Motoaki Matsuo, Shigeyuki Takagi, Anna-Lisa Chaudhary, Toyoto Sato, Martin Dornheim and Shin-ichi Orimo

Inorganics 2017, 5(4), 81; https://doi.org/10.3390/inorganics5040081 - 16 Nov 2017

Cited by 4 | Viewed by 4295

Abstract

In previous studies, complex hydrides LiBH₄ and Mg₂FeH₆ have been reported to undergo simultaneous dehydrogenation when ball-milled as composite materials (1 − x)LiBH₄ + xMg₂FeH₆. The simultaneous hydrogen release led to a decrease of the dehydrogenation temperature by as much as 150 K when compared to that of LiBH₄. It also led to the modified dehydrogenation properties of Mg₂FeH₆. The simultaneous dehydrogenation behavior between stoichiometric ratios of LiBH₄ and Mg₂FeH₆ is not yet understood. Therefore, in the present work, we used the molar ratio x = 0.25, 0.5, and 0.75, and studied the isothermal dehydrogenation processes via pressure–composition–isothermal (PCT) measurements. The results indicated that the same stoichiometric reaction occurred in all of these composite materials, and x = 0.5 was the molar ratio between LiBH₄ and Mg₂FeH₆ in the reaction. Due to the optimal composition ratio, the composite material exhibited enhanced rehydrogenation and reversibility properties: the temperature and pressure of 673 K and 20 MPa of H₂, respectively, for the full rehydrogenation of x = 0.5 composite, were much lower than those required for the partial rehydrogenation of LiBH₄. Moreover, the x = 0.5 composite could be reversibly hydrogenated for more than four cycles without degradation of its H₂ capacity. Full article

(This article belongs to the Special Issue Functional Materials Based on Metal Hydrides)

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4139 KiB

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Unique Hydrogen Desorption Properties of LiAlH₄/h-BN Composites

by Yuki Nakagawa, Shigehito Isobe, Takao Ohki and Naoyuki Hashimoto

Inorganics 2017, 5(4), 71; https://doi.org/10.3390/inorganics5040071 - 25 Oct 2017

Cited by 6 | Viewed by 4879

Abstract

Hexagonal boron nitride (h-BN) is known as an effective additive to improve the hydrogen de/absorption properties of hydrogen storage materials consisting of light elements. Herein, we report the unique hydrogen desorption properties of LiAlH₄/h-BN composites, which were prepared by ball-milling. The desorption profiles of the composite indicated the decrease of melting temperature of LiAlH₄, the delay of desorption kinetics in the first step, and the enhancement of the kinetics in the second step, compared with milled LiAlH₄. Li₃AlH₆ was also formed in the composite after desorption in the first step, suggesting h-BN would have a catalytic effect on the desorption kinetics of Li₃AlH₆. Finally, the role of h-BN on the desorption process of LiAlH₄ was discussed by comparison with the desorption properties of LiAlH₄/X (X = graphite, LiCl and LiI) composites, suggesting the enhancement of Li ion mobility in the LiAlH₄/h-BN composite. Full article

(This article belongs to the Special Issue Functional Materials Based on Metal Hydrides)

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1904 KiB

Open AccessArticle

Hydrogen Storage Stability of Nanoconfined MgH₂ upon Cycling

by Priscilla Huen, Mark Paskevicius, Bo Richter, Dorthe B. Ravnsbæk and Torben R. Jensen

Inorganics 2017, 5(3), 57; https://doi.org/10.3390/inorganics5030057 - 23 Aug 2017

Cited by 23 | Viewed by 5297

Abstract

It is of utmost importance to optimise and stabilise hydrogen storage capacity during multiple cycles of hydrogen release and uptake to realise a hydrogen-based energy system. Here, the direct solvent-based synthesis of magnesium hydride, MgH₂, from dibutyl magnesium, MgBu₂, in four different carbon aerogels with different porosities, i.e., pore sizes, 15 < D_avg < 26 nm, surface area 800 < S_BET < 2100 m²/g, and total pore volume, 1.3 < V_tot < 2.5 cm³/g, is investigated. Three independent infiltrations of MgBu₂, each with three individual hydrogenations, are conducted for each scaffold. The volumetric and gravimetric loading of MgH₂ is in the range 17 to 20 vol % and 24 to 40 wt %, which is only slightly larger as compared to the first infiltration assigned to the large difference in molar volume of MgH₂ and MgBu₂. Despite the rigorous infiltration and sample preparation techniques, particular issues are highlighted relating to the presence of unwanted gaseous by-products, Mg/MgH₂ containment within the scaffold, and the purity of the carbon aerogel scaffold. The results presented provide a research path for future researchers to improve the nanoconfinement process for hydrogen storage applications. Full article

(This article belongs to the Special Issue Functional Materials Based on Metal Hydrides)

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3708 KiB

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Synthesis of LiAlH₄ Nanoparticles Leading to a Single Hydrogen Release Step upon Ti Coating

by Lei Wang and Kondo-Francois Aguey-Zinsou

Inorganics 2017, 5(2), 38; https://doi.org/10.3390/inorganics5020038 - 7 Jun 2017

Cited by 22 | Viewed by 8755

Abstract

Lithium aluminum hydride (LiAlH₄) is an interesting high capacity hydrogen storage material with fast hydrogen release kinetics when mechanically activated with additives. Herein, we report on a novel approach to produce nanoscale LiAlH₄ via a bottom-up synthesis. Upon further coating of these nanoparticles with Ti, the composite nanomaterial was found to decompose at 120 °C in one single and extremely sharp exothermic event with instant hydrogen release. This finding implies a significant thermodynamic alteration of the hydrogen properties of LiAlH₄ induced by the synergetic effects of the Ti catalytic coating and nanosizing effects. Ultimately, the decomposition path of LiAlH₄ was changed to LiAlH₄ → Al + LiH + 3/2H₂. Full article

(This article belongs to the Special Issue Functional Materials Based on Metal Hydrides)

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2214 KiB

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Hydrogen Sorption in Erbium Borohydride Composite Mixtures with LiBH₄ and/or LiH

by Michael Heere, Seyed Hosein Payandeh GharibDoust, Matteo Brighi, Christoph Frommen, Magnus H. Sørby, Radovan Černý, Torben R. Jensen and Bjørn C. Hauback

Inorganics 2017, 5(2), 31; https://doi.org/10.3390/inorganics5020031 - 26 Apr 2017

Cited by 23 | Viewed by 6526

Abstract

Rare earth (RE) metal borohydrides have recently been receiving attention as possible hydrogen storage materials and solid-state Li-ion conductors. In this paper, the decomposition and reabsorption of Er(BH₄)₃ in composite mixtures with LiBH₄ and/or LiH were investigated. The composite of 3LiBH₄ + Er(BH₄)₃ + 3LiH has a theoretical hydrogen storage capacity of 9 wt %, nevertheless, only 6 wt % hydrogen are accessible due to the formation of thermally stable LiH. Hydrogen sorption measurements in a Sieverts-type apparatus revealed that during three desorption-absorption cycles of 3LiBH₄ + Er(BH₄)₃ + 3LiH, the composite desorbed 4.2, 3.7 and 3.5 wt % H for the first, second and third cycle, respectively, and thus showed good rehydrogenation behavior. In situ synchrotron radiation powder X-ray diffraction (SR-PXD) after ball milling of Er(BH₄)₃ + 6LiH resulted in the formation of LiBH₄, revealing that metathesis reactions occurred during milling in these systems. Impedance spectroscopy of absorbed Er(BH₄)₃ + 6LiH showed an exceptional high hysteresis of 40–60 K for the transition between the high and low temperature phases of LiBH₄, indicating that the high temperature phase of LiBH₄ is stabilized in the composite. Full article

(This article belongs to the Special Issue Functional Materials Based on Metal Hydrides)

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Review

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12 pages, 2261 KiB

Open AccessReview

A Recycling Hydrogen Supply System of NaBH₄ Based on a Facile Regeneration Process: A Review

by Liuzhang Ouyang, Hao Zhong, Hai-Wen Li and Min Zhu

Inorganics 2018, 6(1), 10; https://doi.org/10.3390/inorganics6010010 - 6 Jan 2018

Cited by 51 | Viewed by 8480

Abstract

NaBH₄ hydrolysis can generate pure hydrogen on demand at room temperature, but suffers from the difficult regeneration for practical application. In this work, we overview the state-of-the-art progress on the regeneration of NaBH₄ from anhydrous or hydrated NaBO₂ that is a byproduct of NaBH₄ hydrolysis. The anhydrous NaBO₂ can be regenerated effectively by MgH₂, whereas the production of MgH₂ from Mg requires high temperature to overcome the sluggish hydrogenation kinetics. Compared to that of anhydrous NaBO₂, using the direct hydrolysis byproduct of hydrated NaBO₂ as the starting material for regeneration exhibits significant advantages, i.e., omission of the high-temperature drying process to produce anhydrous NaBO₂ and the water included can react with chemicals like Mg or Mg₂Si to provide hydrogen. It is worth emphasizing that NaBH₄ could be regenerated by an energy efficient method and a large-scale regeneration system may become possible in the near future. Full article

(This article belongs to the Special Issue Functional Materials Based on Metal Hydrides)

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Tetrahydroborates: Development and Potential as Hydrogen Storage Medium

by Julián Puszkiel, Sebastiano Garroni, Chiara Milanese, Fabiana Gennari, Thomas Klassen, Martin Dornheim and Claudio Pistidda

Inorganics 2017, 5(4), 74; https://doi.org/10.3390/inorganics5040074 - 31 Oct 2017

Cited by 60 | Viewed by 7139

Abstract

The use of fossil fuels as an energy supply becomes increasingly problematic from the point of view of both environmental emissions and energy sustainability. As an alternative, hydrogen is widely regarded as a key element for a potential energy solution. However, different from fossil fuels such as oil, gas, and coal, the production of hydrogen requires energy. Alternative and intermittent renewable sources such as solar power, wind power, etc., present multiple advantages for the production of hydrogen. On one hand, the renewable sources contribute to a remarkable reduction of pollutants released to the air. On the other hand, they significantly enhance the sustainability of energy supply. In addition, the storage of energy in form of hydrogen has a huge potential to balance an effective and synergetic utilization of the renewable energy sources. In this regard, hydrogen storage technology presents a key roadblock towards the practical application of hydrogen as “energy carrier”. Among the methods available to store hydrogen, solid-state storage is the most attractive alternative both from the safety and the volumetric energy density points of view. Because of their appealing hydrogen content, complex hydrides and complex hydride-based systems have attracted considerable attention as potential energy vectors for mobile and stationary applications. In this review, the progresses made over the last century on the development in the synthesis and research on the decomposition reactions of homoleptic tetrahydroborates is summarized. Furthermore, theoretical and experimental investigations on the thermodynamic and kinetic tuning of tetrahydroborates for hydrogen storage purposes are herein reviewed. Full article

(This article belongs to the Special Issue Functional Materials Based on Metal Hydrides)

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