Metal (boro-) hydrides for high energy density storage and relevant emerging technologies
L. J. Bannenberg, M. Heere, H. Benzidi, J. Montero, E. M. Dematteis, S. Suwarno, T. Jaroń, M. Winny, P. A. Orłowski, W. Wegner, A. Starobrat, K. J. Fijałkowski,… 展开作者
L. J. Bannenberg, M. Heere, H. Benzidi, J. Montero, E. M. Dematteis, S. Suwarno, T. Jaroń, M. Winny, P. A. Orłowski, W. Wegner, A. Starobrat, K. J. Fijałkowski, W. Grochala, Z. Qian, J. -P. Bonnet, I. Nuta, W. Lohstroh, C. Zlotea, O. Mounkachi, F. Cuevas, C. Chatillon, M. Latroche, M. Fichtner, M. Baricco, B. C. Hauback, A. El Kharbachi
The current energy transition imposes a rapid implementation of energy storage systems with high energy density and eminent regeneration and cycling efficiency. Metal hydrides are potential candidates for generalized energy storage, when coupled with fuel cell units and/or batteries. An overview of ongoing research is reported and discussed in this review work on the light of application as hydrogen and heat storage matrices, as well as thin films for hydrogen optical sensors. These include a selection of single-metal hydrides, Ti-V(Fe) based intermetallics, multi-principal element alloys (high-entropy alloys), and a series of novel synthetically accessible metal borohydrides. Metal hydride materials can be as well of important usefulness for MH-based electrodes with high capacity (e.g. MgH2 ~ 2000 mAh g-1) and solid-state electrolytes displaying high ionic conductivity suitable, respectively, for Li-ion and Li/Mg battery technologies. To boost further research and development directions some characterization techniques dedicated to the study of M-H interactions, their equilibrium reactions, and additional quantification of hydrogen concentration in thin film and bulk hydrides are presented at the end of this manuscript.
Despite high interest in compact and safe storage of hydrogen in the solid-state hydride form, the design of alloys that can reversibly and quickly store hydrogen at room temperature under pressures close to atmospheric pressure is a long-lasting challenge. In this study, first-principles calculations are combined with experiments to develop high-entropy alloys (HEAs) for room-temperature hydrogen storage. TixZr2-xCrMnFeNi (x = 0.4-1.6) alloys with the Laves phase structure and low hydrogen binding energies of -0.1 to -0.15 eV are designed and synthesized. The HEAs reversibly store hydrogen in…
Generally hydrogen will adopt the +1, 0 or -1 oxidation state in solids depending upon the chemical environment it occupy. Typically, there are some exceptional cases in which hydrogen exhibits both anionic and cationic behavior in the same structural frame works. In this study we briefly explore an amphoteric behavior of hydrogen present in ammine bimetallic borohydrides with the chemical formula M1M2 (BH4)3 (NH3)2 (M1= Na; M2 = Zn, Mg) using the state-of-the-art density functional calculations. In order to establish the amphoteric behavior of hydrogen in M1M2 (BH4)3 (NH3)2, we have made deta…
The study of superconductivity in compressed hydrides is of great interest due to measurements of high critical temperatures (Tc) in the vicinity of room temperature, beginning with the observations of LaH10 at 170-190 GPa. However, the pressures required for synthesis of these high Tc superconducting hydrides currently remain extremely high. Here we show the investigation of crystal structures and superconductivity in the La-B-H system under pressure with particle-swarm intelligence structure searches methods in combination with first-principles calculations. Structures with six stoichiometri…
In order to overcome the disadvantages of MgH2 towards its applications in on-board hydrogen storage, first principle calculations have been performed for Ti (2+, 3+, and 4+) substituted MgH2. Our calculated enthalpy of formation and H site energy implies that Ti substitution in Mg site reduces the stability of MgH2 which improve the hydrogen storage properties and Ti prefers to be in +4 oxidation state in MgH2. The bonding analyses through partial density of states, electron localization function and Bader charge of these systems confirm the existence of iono-covalent bonding. Electronic stru…
In this present investigation, we discussed the synthesis, microstructure, and hydrogen storage behavior intermetallic Laves phase in a hexanal TiVZrMnCoFe high entropy alloy. In this HEA, three elements are hydride-forming elements and the other three are non-hydride-forming elements (Fe, Mn, Co). The thermodynamic parameter like enthalpy of mixing was calculated using Meidmas model.The possibility of developing high entropy Laves phase-based hydrogen storage materials was advocated.
A comprehensive first principles investigation of A$_2$BH$_6$ type (A= Li,Na, and K; B= Al, and Si) double perovskite hydrides for high capacity hydrogen storage
Climate change motivates the search for non-carbon-emitting energy generation and storage solutions. Metal hydrides show promising characteristics for this purpose. They can be further stabilized by tailoring the negative pressure of microstructural and structural defects. Using systematic ab initio and atomistic simulations, we demonstrate that an enhancement in the formation of hydrides at the negatively pressurized crack tip region is feasible by increasing the mechanical tensile load on the specimen. The theoretical predictions have been used to reassess and interpret atom probe tomography…
A Hybrid Machine Learning Framework for Predicting Hydrogen Storage Capacities in Metal Hydrides: Unsupervised Feature Learning with Deep Neural Networks
Machine learning to explore high-entropy alloys with desired enthalpy for room-temperature hydrogen storage: Prediction of density functional theory and experimental data
Physical properties of transition metal hydride superconductors Mg2TmH6 (Tm = Rh, Pd, Ir, Pt) by first-principles calculations
Mawlana Bhashani Science and Technology University（毛拉纳·巴沙尼科技大学）；University of Rajshahi（拉杰沙希大学）；Rajshahi University of Engineering and Technology（拉杰沙希工程与技术大学）
Chemical transformation of MgH2/V2O5 composite to Mg-V-O rock salt and its influence on the electrochemical Li conversion and hydrogen storage characteristics of MgH2
University of Aveiro（阿威罗大学）；LASI - Intelligent Systems Associate Laboratory（智能系统联合实验室）；International Iberian Nanotechnology Laboratory (INL)（伊比利亚纳米技术国际实验室）
Covalent functionalization is a way to tune the electrochemical properties of hexagonal boron nitride (h-BN) monolayers. The wide band gap insulator h-BN may become metallic conductor upon functionalization with strong oxidants, such as fluorosulfonyl radicals ($\cdot$OSO$_2$F), as known since 1978 [N. Bartlett et al., J. Chem. Soc. Chem. Comm. {\bf 5}, 200 (1978)], with electrical conductivity of 1.5 S/cm [C. Shen et al., J. Solid State Chem. {\bf 147}, 74 (1999)] that greatly surpasses commercial cathode material Li$_{x}$CoO$_{2}$ while retaining excellent ionic conductivity. Functionalized …
A generative machine learning model for designing metal hydrides applied to hydrogen storage
Mathematics and Statistics, Louisiana Tech University（数学与统计学系，拉法叶技术大学）；Louisiana Tech University（拉法叶技术大学）；Institute for Micromanufacturing, Louisiana Tech University（微制造研究所，拉法叶技术大学）；National Energy Technology Laboratory, United States Department of Energy, Pittsburgh, PA 15236（美国能源部国家能源技术实验室，匹兹堡，PA 15236）
The electride Sr$_3$CrN$_3$ has a one-dimensional channel of electron density, which is a rare feature that offers great potential for fast ion conduction. Using density functional theory, we find that Sr$_3$CrN$_3$ is an excellent hydride conductor within this channel, with a diffusion barrier as low as 0.30 eV and an estimated diffusion coefficient of $5.37\times 10^{-8}$ cm$^2$/s. This diffusion barrier is lower than those reported for the best hydride conductors to date. We also show the most-stable amount of hydride in the host material under standard conditions and the corresponding chan…
The interaction of hydrogen and metals continues to be industrially relevant and is a critical part of creating and supporting a safety case for nuclear reactor operation. In the present work, we explore hydrogen storage and hydride formation in a zirconium alloy. We characterise the structure and interfaces of fine scale hydrides using scanning transmission electron microscopy (STEM) including energy dispersive spectroscopy (EDS/EDX), electron energy loss spectroscopy (EELS), and high-resolution STEM. Chemical characterisation is supported further with atom probe tomography (APT). Samples wer…
Usually the ions of a particular element in solids are in positive or negative oxidation states, depending upon the chemical environment. It is highly unusual for an atom having both positive as well as negative oxidation states simultaneously within the same structural framework in a particular compound. Our structural and chemical bonding analyses show that the hydrogen ions in the transition metal ammine borohydrides (TMABHs) with the chemical formula M(BH4)2(NH3)2 (M = Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu and Zn) have both positive and negative oxidation states. Our detailed analyses confirm …
In order to identify potential hydrogen storage materials, worldwide attention has been focused on hydrides with high gravimetric and volumetric capacity. Hydrogen is a unique element that possess positive, negative or neutral oxidation state in solids depending upon the chemical environment. If one can find hydrogen storage materials where hydrogen is present in both negative and positive oxidation state within the same structural framework then one can accommodate hydrogen with high volume density. So, it is fundamentally as well as technologically important to identify compounds in which hy…
Ambient and Pressure Dependent Superconductivity with Hydrogen Storage Potential in Quaternary Hydride LiMgZr2H12: A Comprehensive First-principles Insights
Department of Physics, University of Rajshahi（拉杰沙希大学物理系）
A unified descriptor framework for hydrogen storage capacity and equilibrium pressure in interstitial hydrides
Advanced Institute for Materials Research (WPI-AIMR), Tohoku University（东北大学先进材料研究所）；Unprecedented-scale Data Analytics Center, Tohoku University（东北大学超大规模数据分析中心）；Frontier Research Institute for Interdisciplinary Sciences (FRIS), Tohoku University（东北大学前沿交叉科学研究所）；Department of Materials Engineering, The University of Tokyo（东京大学材料工程系）；Institute for Materials Research, Tohoku University（东北大学物质材料研究机构）；Institute of Fluid Science, Tohoku University（东北大学流体科学研究所）
First principles based DFT calculations performed to insight structural and electronic properties of Boron doped Magnesium atom decorated graphene sheet for application of hydrogen storage. The four H2 molecules stably binds magnesium atom with Boron doped graphene sheet. The average binding energy extracted in the range-0.566 to -0.687 eV/H2.Partial density of states of complex system shows s and d orbitals of H2 molecule and Mg atom at -0.1eV overlaps of main peaks indicates strong hybridizing and binding of s and d orbitals of H2 and Mg atom respectively. The gravimetric capacity of studied…
The recent progress in the field of hydrogen storage in carbon and boron nitride nanostructures has been summarized. Carbon and boron nitride nanostructures are considered advantageous in this prospect due to their lightweight and high surface area. Demerits of pristine structures to hold hydrogen molecules for mobile applications have been highlighted by many researchers. In such cases, weak van der Waals interaction comes into account, hence, the hydrogen molecules are weakly bonded with the host materials and hence weak adsorption energy and low hydrogen molecules uptake. So, to tune the ad…
Machine learning via artificial neural networks coupled with density functional theory and experiments for thermodynamic optimization of high-entropy alloys for hydrogen storage at room temperature
WPI, International Institute for Carbon-Neutral Energy Research (WPI-I2CNER), Kyushu University（九州大学）；Department of Automotive Science, Graduate School of Integrated Frontier Sciences, Kyushu University（九州大学）；Institute for Materials Science, University of Stuttgart（斯图加特大学）
Hydrogen-based fuels demand high-density storage that can operate under ambient temperatures. Pd and its alloys are the most investigated metal hydrides for hydrogen fuel cell applications. This study presented an alternative Pd alloy for hydrogen storage that can store and release hydrogen at room temperature. The surface of the most studied Pd (110) was modified with Au and Rh so that the hydrogen adsorption energy was 0.49 eV and the release temperature was 365 K. Both values are quite near to the optimum values for the adsorption energy and release temperature of a hydrogen fuel cell in re…
Rational design of novel two-dimensional (2D) electrode materials with high capacity is crucial for the further development of Li-ion and Na-ion batteries. Herein, based on first-principles calculations, we systemically investigate Li and Na storage behaviors in the recently discovered 2D topological nodal-loop metal - the honeycomb borophene oxide (h-B2O). We show that h-B2O is an almost ideal anode material. It has good conductivity before and after Li/Na adsorption, fast ion diffusion with diffusion barrier less than 0.5 eV, low open-circuit voltage (less than 1 V), and small lattice change…
Magnesium hydride owns the largest share of publications on solid materials for hydrogen storage. The Magnesium group of international experts contributing to IEA Task 32 Hydrogen Based Energy Storage recently published two review papers presenting the activities of the group focused on magnesium hydride based materials and on Mg based compounds for hydrogen and energy storage. This review article not only overviews the latest activities on both fundamental aspects of Mg-based hydrides and their applications, but also presents a historic overview on the topic and outlines projected future deve…
Hydrogen uptake and hydride formation in Al$_x$CoCrFeNi high-entropy alloys: First-principles, universal-potential, and experimental study
Ruhr-Universität Bochum（波鸿鲁尔大学）；Max-Planck-Institut for Sustainable Materials（马克斯·普朗克可持续材料研究所）；University of Stuttgart（斯图加特大学）；Deutsches Elektronen-Synchrotron DESY（德国电子同步辐射中心）；Goethe University Frankfurt（法兰克福歌德大学）；Federal Institute for Materials Research and Testing (BAM)（联邦材料研究与测试研究所）
Synthesis and Characterization of TiFe0.7-xMn0.3Vx (x=0.05, and 0.1) and Ti1-yTayFe0.7Mn0.3 (y=0.2, and 0.4) Nanostructured Metal Hydrides for Low Temperature Applications
The integrity of irradiated zirconium based nuclear fuel cladding is related to the precipitation of hydrides which is closely connected with the solubility of hydrogen. A review on the development of measurement technologies is given and the resulting terminal solid solubilities are reflected with respect to the established model of hydrogen solubility in zirconium alloys. The results often allow for a different interpretation than the established model. An alternative qualitative approach is proposed in which the fixed TSSp for the precipitation of zirconium hydrides is replaced by a kinetic…
Lightweight 2D materials due to its large surface area are being studied for its hydrogen storage applications. The characteristics of hydrogen adsorption on the electric field-induced h-BN bilayer were investigated. The overall storage capacity of the bilayer is 6.7 wt% from our theoretical calculation with E ads of 0.308 eV/H$_2$. The desorption temperature for H$_2$ molecules from the h-BN bilayer system in the absence of an external electric field is 243 K. With the introduction of an external electric field, the E$_{\rm ads}$ lies in the range 0.311-0.918 eV/H$_2$ with a desorption temper…
Metal hydrides are critical materials in numerous technologies including hydrogen storage, gas separation, and electrocatalysis. Here, using Pd-H as a model metal hydride, we perform electrochemical insertion studies of hydrogen via liquid and solid state electrolytes at 1 atm ambient pressure, and achieve H:Pd ratios near unity, the theoretical solubility limit. We show that the compositions achieved result from a dynamic balance between the rate of hydrogen insertion and evolution from the Pd lattice, the combined kinetics of which are sufficiently rapid that operando experiments are necessa…
Discovery of high-temperature superconductivity in hydrogen-rich compounds has fuelled the enthusiasm for finding materials with more promising superconducting properties among hydrides. However, the ultrahigh pressure needed to synthesize and maintain high-temperature hydrogen-rich superconductors hinders the experimental investigation of these materials. For practical applications, it is also highly desired to find more hydrogen-rich materials that superconduct at high temperatures but under relatively lower pressures. Based on first-principles density functional theory, we calculate the ele…
