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Understanding electronic structure tunability by metal dopants for promoting MgB2 hydrogenation

Journal Article · · Journal of Applied Physics
DOI:https://doi.org/10.1063/5.0175546· OSTI ID:2370166
 [1];  [2];  [2];  [2];  [2];  [3];  [3];  [3];  [2]
  1. Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States). Laboratory for Energy Applications for the Future (LEAF); Yale Univ., New Haven, CT (United States)
  2. Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States). Laboratory for Energy Applications for the Future (LEAF)
  3. Sandia National Lab. (SNL-CA), Livermore, CA (United States)
+ Show Author Affiliations
Hydrogen is a promising energy carrier, but its onboard application is limited by the need for compact, low-pressure storage solutions. Solid-state complex metal hydride systems, such as MgB2/Mg(BH4)2, offer high storage capacities but suffer from sluggish kinetics and poor reversibility. One avenue for improving reactivity is to introduce metal dopants to alter electronic and atomic properties, but the role of these chemical additives remains poorly understood, particularly for the hydrogenation reaction. In this work, we used density functional theory calculations on model MgB2 systems to rationalize the potential role of metal dopants in destabilizing B–B bonding within the MgB2 lattice. We carried out detailed electronic structure analyses for 28 different metal dopant adatoms to identify properties that contribute to a dopant’s efficacy. Based on the simulation results, we propose that an intermediate ionic and covalent character of the bonds between adatoms and B atoms is desirable for facilitating charge redistribution, disrupting the B–B bond network, and promoting H2 dissociation and H atom chemisorption on MgB2.
Research Organization:
Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Sponsoring Organization:
USDOE National Nuclear Security Administration (NNSA); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Hydrogen Fuel Cell Technologies Office (HFTO)
Grant/Contract Number:
AC52-07NA27344; NA0003525
OSTI ID:
2370166
Report Number(s):
LLNL--JRNL-829306; 1045063
Journal Information:
Journal of Applied Physics, Journal Name: Journal of Applied Physics Journal Issue: 2 Vol. 135; ISSN 0021-8979
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English

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Figures / Tables (12)

FIG. 1(p. 5)figure FIG. 1
FIG. 2(p. 6)figure FIG. 2
FIG. 3(p. 8)figure FIG. 3
FIG. 4(p. 9)figure FIG. 4
FIG. 5(p. 11)figure FIG. 5
FIG. S1(p. 14)figure FIG. S1
FIG. S2(p. 15)figure FIG. S2
FIG. S3(p. 16)figure FIG. S3
FIG. S4(p. 17)figure FIG. S4
FIG. S5(p. 18)figure FIG. S5
FIG. S6(p. 19)figure FIG. S6
FIG. S7(p. 20)figure FIG. S7

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08 HYDROGEN
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