Highly destabilized Mg-Ti-Ni-H system investigated by density functional theory and hydrogenography

Broedersz, Chase P.; Gremaud, Robin; Dam, B.; Griessen, R.; Løvvik, Ole Martin

doi:10.1103/physrevb.77.024204

Cited by 41 publications

(22 citation statements)

References 40 publications

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“…This is probably related to the formation of stable Ti-Ni alloy nanograins. [31] A composition with optimal stability and good gravimetric capacity is, for example, Mg 0.69 Ni 0.26 Ti 0.05 , whose Van 't Hoff plot is shown in Figure 3d. The central results of our investigation are that i) p-c isotherms and the enthalpy of hydride formation can be measured optically and simultaneously on a large number of samples under exactly the same external parameters of pressure and temperatures.…”

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confidence: 97%

Hydrogenography: An Optical Combinatorial Method To Find New Light‐Weight Hydrogen‐Storage Materials

et al. 2007

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The standard approach for the search of new hydrogen-storage materials is to synthesize bulk samples and to use volumetric [1,2] or gravimetric [3] techniques to follow their hydrogenation reaction and to record pressure-concentration isotherms (p-c isotherms). The equilibrium pressure of the metal-to-hydride transition is determined from the plateau of the p-c isotherm. The enthalpy of hydride formation is extracted from the temperature dependence of the equilibrium pressure, by means of the Van 't Hoff relation [4] lnwhere DH is the enthalpy of formation in kJ (mol H 2 ) -1 , DS 0 is the entropy of formation in JK -1 (mol H 2 ) -1 at standard pressure, R the gas constant, the absolute temperature, p 0 = 1.013 × 10 5 Pa the standard pressure, and p eq the H 2 equilibrium plateau pressure of the p-c isotherm. The great disadvantage of this approach is that a bulk sample is needed for each investigated chemical composition. Thin films provide an interesting alternative to bulk, as their nanostructure is controlled by the deposition conditions. Because of the small amount of material and large surfaces present, diffusion and local heating issues are minimized, the kinetics are fast, and the measurement time is reduced drastically. [5] Moreover, a large number of different chemical compositions can be deposited on a single substrate in a combinatorial way. The fact that hydrogen absorption in a metal leads to large optical changes [6,7] is the basis of a new combinatorial method that we call hydrogenography. With a straightforward optical setup, hydrogenography makes it possible to monitor hydrogen ab-and desorption simultaneously on thousands of samples under exactly the same experimental conditions. [8][9][10] We show here that hydrogenography is much more than a monitoring technique, as it also provides a high-throughput method to measure quantitatively the key thermodynamic properties (enthalpy and entropy) of hydride formation. We describe the essential ingredients of hydrogenography with the Mg-Ti-H system and demonstrate its combinatorial power with the Mg-Ti-Ni-H system. We show in particular that there is a relatively narrow range of compositions in the ternary Mg-Ti-Ni phase diagram with a remarkable combination of favorable properties for light-weight hydrogen storage. Pure MgH 2 would in principle be an attractive system for hydrogen storage as it can contain as much as 7.6 wt % of hydrogen. However, its large negative enthalpy of formation (-74 kJ (mol H 2 ) -1

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confidence: 97%

Hydrogenography: An Optical Combinatorial Method To Find New Light‐Weight Hydrogen‐Storage Materials

et al. 2007

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“…326 Hydrogenography has also been utilized as a switchable mirror technology, taking advantage of the change in transmissivity that results from hydrogenation, as well as other applications. [327][328][329][330] Hydrogenography has been applied for compositional mapping of a number of Mg based systems such as Mg-Ni, 309,331 Mg-Ni-Ti, 332 Mg-Al, 333 and Mg-Al-Ti. 334 A notable result from this body of work was the discovery 316 of the alloy Mg 69 Ni 26 Ti 5 , Fig.…”

Section: Thin Film Combinatorial Workmentioning

confidence: 99%

Applications of high throughput (combinatorial) methodologies to electronic, magnetic, optical, and energy-related materials

Green

Takeuchi

Hattrick‐Simpers

2013

Journal of Applied Physics

227

189

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High throughput (combinatorial) materials science methodology is a relatively new research paradigm that offers the promise of rapid and efficient materials screening, optimization, and discovery. The paradigm started in the pharmaceutical industry but was rapidly adopted to accelerate materials research in a wide variety of areas. High throughput experiments are characterized by synthesis of a "library" sample that contains the materials variation of interest (typically composition), and rapid and localized measurement schemes that result in massive data sets. Because the data are collected at the same time on the same "library" sample, they can be highly uniform with respect to fixed processing parameters. This article critically reviews the literature pertaining to applications of combinatorial materials science for electronic, magnetic, optical, and energy-related materials. It is expected that high throughput methodologies will facilitate commercialization of novel materials for these critically important applications. Despite the overwhelming evidence presented in this paper that high throughput studies can effectively inform commercial practice, in our perception, it remains an underutilized research and development tool. Part of this perception may be due to the inaccessibility of proprietary industrial research and development practices, but clearly the initial cost and availability of high throughput laboratory equipment plays a role. Combinatorial materials science has traditionally been focused on materials discovery, screening, and optimization to combat the extremely high cost and long development times for new materials and their introduction into commerce. Going forward, combinatorial materials science will also be driven by other needs such as materials substitution and experimental verification of materials properties predicted by modeling and simulation, which have recently received much attention with the advent of the Materials Genome Initiative. Thus, the challenge for combinatorial methodology will be the effective coupling of synthesis, characterization and theory, and the ability to rapidly manage large amounts of data in a variety of formats. V C 2013 AIP Publishing LLC. [http://dx

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“…10,11,12,13,14,15,16,17 These DFT calculations require a priori knowledge of the hydride crystal structures, and hence are most directly applicable for those materials that have already been structurally well characterized. In contrast, DFT becomes more difficult for new materials, whose crystal structures are unknown.…”

Section: Introductionmentioning

confidence: 99%

First-principles prediction of phase stability and crystal structures in Li-Zn and Na-Zn mixed-metal borohydrides

Aidhy

Wolverton

2011

Phys. Rev. B

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We use a combination of first principles density functional theory (DFT) calculations and the recently developed Prototype Electrostatic Ground State (PEGS) method to predict low energy crystal structures and study phase stability of Li-Zn and Na-Zn mixed-metal borohydride compounds, i.e., NaZn(BH 4 ) 3 , NaZn 2 (BH 4 ) 5 , LiZn(BH 4 ) 3 and LiZn 2 (BH 4 ) 5 .We find the following: (i) DFT+PEGS successfully predicts low-energy structures in these mixed-metal borohydride systems. (ii) DFT calculations show negative mixing energies in both the Li-Zn and Na-Zn borohydride systems, consistent with the observation of mixed-metal ordering in these systems. (iii) Our DFT calculations of the recently reported experimental crystal structures of NaZn 2 (BH 4 ) 5 and NaZn(BH 4 ) 3 show that the former has a negative mixing energy, while the latter has a positive mixing energy, (iv) Using the PEGS approach, we predict a new crystal structure of NaZn(BH 4 ) 3 with negative mixing energy and find that the experimental structure of NaZn 2 (BH 4 ) 5 and the PEGS obtained structure of NaZn(BH 4 ) 3 lie on the ground state convex hull. (v) In the Li-Zn borohydride system, we have used the PEGS+DFT approach to predict a stable crystal structure of new, previously unobserved stoichiometry, LiZn(BH 4 ) 3 . As a consequence of this predicted low-energy compound,

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Highly destabilized Mg-Ti-Ni-H system investigated by density functional theory and hydrogenography

Cited by 41 publications

References 40 publications

Hydrogenography: An Optical Combinatorial Method To Find New Light‐Weight Hydrogen‐Storage Materials

Hydrogenography: An Optical Combinatorial Method To Find New Light‐Weight Hydrogen‐Storage Materials

Applications of high throughput (combinatorial) methodologies to electronic, magnetic, optical, and energy-related materials

First-principles prediction of phase stability and crystal structures in Li-Zn and Na-Zn mixed-metal borohydrides

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