Graphene Activated Magnesium Diboride for Moderate Pressure and Temperature Hydrogenation to Magnesium Borohydride

Severa, Godwin; Wang, Lei; Kim, Stephen; Leick, Noemi; Kelly, Colleen; Sugai, Cody; Snider, Jonathan L.; Norman, Andrew G.; Dera, Przemyslaw; Kotsol, Isabella; Gennett, Thomas; Stavila, Vitalie; Jensen, Craig M.

doi:10.1021/acsaem.4c02302

Graphene Activated Magnesium Diboride for Moderate Pressure and Temperature Hydrogenation to Magnesium Borohydride

Journal Article · Tue Jan 07 04:00:00 EST 2025 · ACS Applied Energy Materials

DOI:https://doi.org/10.1021/acsaem.4c02302· OSTI ID:2522743

Severa, Godwin; Wang, Lei; Kim, Stephen; Leick, Noemi; Kelly, Colleen; Sugai, Cody; Snider, Jonathan L.; ; Dera, Przemyslaw; Kotsol, Isabella; Gennett, Thomas; Stavila, Vitalie; Jensen, Craig M.

The hydrogenation conditions of magnesium diboride (MgB2) to magnesium borohydride (Mg(BH4)2) can be significantly enhanced through the discovery of improved modifiers. This study demonstrates that the modification of MgB2 by mechanical milling with graphene nanoplatelets significantly reduces the hydrogenation conditions of MgB2 from 900 bar and 400 degrees C for pure MgB2 to 400 bar and 300 degrees C while achieving 77% conversion to Mg(BH4)2. The introduction of the graphene additives coupled with milling leads to a reduction of the temperature and pressure required for bulk hydrogenation by 100 degrees C and 500 bar, respectively, from that of pure MgB2. The identification of graphene additives that drastically improve the hydrogenation conditions of MgB2 represents an important step toward improving hydrogen uptake kinetics to Mg(BH4)2.

Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Hydrogen Fuel Cell Technologies Office (HFTO)

DOE Contract Number:: AC36-08GO28308

OSTI ID:: 2522743

Report Number(s):: NREL/JA-5900-91002; MainId:92780; UUID:5042a38d-ba70-4bbb-9a7e-9519aa121da5; MainAdminId:75534

Journal Information:: ACS Applied Energy Materials, Journal Name: ACS Applied Energy Materials Journal Issue: 2 Vol. 8

Country of Publication:: United States

Language:: English

References (42)

Understanding electronic structure tunability by metal dopants for promoting MgB2 hydrogenation Lefcochilos-Fogelquist, H. M.; Wan, L. F.; Rowberg, A. J. E. Journal of Applied Physics, Vol. 135, Issue 2 https://doi.org/10.1063/5.0175546	journal	January 2024
Dehydriding and rehydriding processes of well-crystallized Mg(BH4)2 accompanying with formation of intermediate compounds Li, H. Acta Materialia, Vol. 56, Issue 6 https://doi.org/10.1016/j.actamat.2007.11.023	journal	April 2008
Phenomenological model of anisotropic peak broadening in powder diffraction Stephens, Peter W. Journal of Applied Crystallography, Vol. 32, Issue 2 https://doi.org/10.1107/S0021889898006001	journal	April 1999
Effects of ball milling and additives on dehydriding behaviors of well-crystallized Mg(BH4)2 Li, H. -W.; Kikuchi, K.; Nakamori, Y. Scripta Materialia, Vol. 57, Issue 8 https://doi.org/10.1016/j.scriptamat.2007.06.052	journal	October 2007
A dynamic calibration technique for temperature programmed desorption spectroscopy Hurst, K. E.; Heben, M. J.; Blackburn, J. L. Review of Scientific Instruments, Vol. 84, Issue 2 https://doi.org/10.1063/1.4770115	journal	February 2013
Hydrogenation via a low energy mechanochemical approach: the MgB ₂ case Pistidda, Claudio; Santhosh, Archa; Jerabek, Paul Journal of Physics: Energy, Vol. 3, Issue 4 https://doi.org/10.1088/2515-7655/abf81b	journal	August 2021
Reversibility and Improved Hydrogen Release of Magnesium Borohydride Newhouse, Rebecca J.; Stavila, Vitalie; Hwang, Son-Jong The Journal of Physical Chemistry C, Vol. 114, Issue 11 https://doi.org/10.1021/jp9116744	journal	February 2010
Direct hydrogenation of magnesium boride to magnesium borohydride: demonstration of >11 weight percent reversible hydrogenstorage Severa, Godwin; Rönnebro, Ewa; Jensen, Craig M. Chem. Commun., Vol. 46, Issue 3 https://doi.org/10.1039/B921205A	journal	January 2010
Reactive Vapor-Phase Additives toward Destabilizing γ-Mg(BH₄)₂ for Improved Hydrogen Release Strange, Nicholas A.; Leick, Noemi; Shulda, Sarah ACS Applied Energy Materials, Vol. 5, Issue 2 https://doi.org/10.1021/acsaem.1c03128	journal	January 2022
Lewis Base Complexes of Magnesium Borohydride: Enhanced Kinetics and Product Selectivity upon Hydrogen Release Chong, Marina; Autrey, Tom; Jensen, Craig Inorganics, Vol. 5, Issue 4 https://doi.org/10.3390/inorganics5040089	journal	December 2017
Hydrogen storage properties of Mg[BH4]2 Matsunaga, T.; Buchter, F.; Mauron, P. Journal of Alloys and Compounds, Vol. 459, Issue 1-2 https://doi.org/10.1016/j.jallcom.2007.05.054	journal	July 2008
Synthesis and properties of magnesium tetrahydroborate, Mg(BH4)2 Chłopek, Krzysztof; Frommen, Christoph; Léon, Aline Journal of Materials Chemistry, Vol. 17, Issue 33 https://doi.org/10.1039/b702723k	journal	January 2007
Selective Reversible Hydrogenation of Mg(B ₃ H ₈ ) ₂ /MgH ₂ to Mg(BH ₄ ) ₂ : Pathway to Reversible Borane-Based Hydrogen Storage? Chong, Marina; Matsuo, Motoaki; Orimo, Shin-ichi Inorganic Chemistry, Vol. 54, Issue 8 https://doi.org/10.1021/acs.inorgchem.5b00373	journal	March 2015
Facile synthesis and regeneration of Mg(BH ₄ ) ₂ by high energy reactive ball milling of MgB ₂ Gupta, Shalabh; Hlova, Ihor Z.; Kobayashi, Takeshi Chem. Commun., Vol. 49, Issue 8 https://doi.org/10.1039/C2CC36580D	journal	January 2013
Recent progress in magnesium borohydride Mg(BH4)2: Fundamentals and applications for energy storage Zavorotynska, Olena; El-Kharbachi, Abdelouahab; Deledda, Stefano International Journal of Hydrogen Energy, Vol. 41, Issue 32 https://doi.org/10.1016/j.ijhydene.2016.02.015	journal	August 2016
Nanoscale Mg–B via Surfactant Ball Milling of MgB ₂ : Morphology, Composition, and Improved Hydrogen Storage Properties Liu, Y. -S.; Ray, K. G.; Jørgensen, M. The Journal of Physical Chemistry C, Vol. 124, Issue 39 https://doi.org/10.1021/acs.jpcc.0c05142	journal	September 2020
A Density Functional Study of α-Mg(BH ₄ ) ₂ Setten, Michiel J. van; Wijs, Gilles A. de; Fichtner, Maximilian Chemistry of Materials, Vol. 20, Issue 15 https://doi.org/10.1021/cm800358k	journal	August 2008
Nanostructure-induced hydrogenation of layered compound MgB2 Li, Hai-Wen; Matsunaga, Tomoya; Yan, Yigang Journal of Alloys and Compounds, Vol. 505, Issue 2 https://doi.org/10.1016/j.jallcom.2010.06.101	journal	September 2010
Effect of several metal chlorides on the thermal decomposition behaviour of α-Mg(BH4)2 Bardají, Elisa Gil; Hanada, Nobuko; Zabara, Oleg International Journal of Hydrogen Energy, Vol. 36, Issue 19 https://doi.org/10.1016/j.ijhydene.2011.07.008	journal	September 2011
Elucidating the mechanism of MgB ₂ initial hydrogenation via a combined experimental–theoretical study Ray, Keith G.; Klebanoff, Leonard E.; Lee, Jonathan R. I. Physical Chemistry Chemical Physics, Vol. 19, Issue 34 https://doi.org/10.1039/C7CP03709K	journal	January 2017
High Pressure Single Crystal Diffraction at PX^2 Zhang, Dongzhou; Dera, Przemyslaw K.; Eng, Peter J. Journal of Visualized Experiments, Issue 119 https://doi.org/10.3791/54660-v	journal	January 2017
A hydride composite featuring mutual destabilisation and reversible boron exchange: Ca(BH ₄ ) ₂ –Mg ₂ NiH ₄ Bergemann, N.; Pistidda, C.; Milanese, C. Journal of Materials Chemistry A, Vol. 6, Issue 37 https://doi.org/10.1039/C8TA04748K	journal	January 2018
Methylamine Magnesium Borohydrides as Electrolytes for All-Solid-State Magnesium Batteries Amdisen, Mads B.; Grinderslev, Jakob B.; Skov, Lasse N. Chemistry of Materials, Vol. 35, Issue 3 https://doi.org/10.1021/acs.chemmater.2c03641	journal	January 2023
Kinetic Enhancement of Direct Hydrogenation of MgB ₂ to Mg(BH ₄ ) ₂ upon Mechanical Milling with THF, MgH ₂ , and/or Mg Sugai, Cody; Kim, Stephen; Severa, Godwin ChemPhysChem, Vol. 20, Issue 10 https://doi.org/10.1002/cphc.201801187	journal	March 2019
Synthesis of amorphous Mg(BH4)2 from MgB2 and H2 at room temperature Pistidda, Claudio; Garroni, Sebastiano; Dolci, Francesco Journal of Alloys and Compounds, Vol. 508, Issue 1 https://doi.org/10.1016/j.jallcom.2010.07.226	journal	October 2010
Understanding Hydrogenation Chemistry at MgB ₂ Reactive Edges from Ab Initio Molecular Dynamics Ray, Keith G.; Klebanoff, Leonard E.; Stavila, Vitalie ACS Applied Materials & Interfaces, Vol. 14, Issue 18 https://doi.org/10.1021/acsami.1c23524	journal	March 2022
Hydrogen Storage in Partially Exfoliated Magnesium Diboride Multilayers Gunda, Harini; Ray, Keith G.; Klebanoff, Leonard E. Small, Vol. 19, Issue 6 https://doi.org/10.1002/smll.202205487	journal	December 2022
The influence of LiH and TiH2 on hydrogen storage in MgB2 II. XPS study of surface and near-surface phenomena Snider, J. L.; Mattox, T. M.; Liu, Y. -S. International Journal of Hydrogen Energy, Vol. 47, Issue 1 https://doi.org/10.1016/j.ijhydene.2021.09.163	journal	January 2022
Controllable decomposition of Ca(BH ₄ ) ₂ for reversible hydrogen storage Yan, Y.; Rentsch, D.; Remhof, A. Physical Chemistry Chemical Physics, Vol. 19, Issue 11 https://doi.org/10.1039/C7CP00448F	journal	January 2017
Thermal Decomposition of Magnesium Borohydride: New Insights from Synchrotron X-ray Scattering Strange, Nicholas A.; Leick, Noemi; Bell, Robert T. Chemistry of Materials, Vol. 34, Issue 24 https://doi.org/10.1021/acs.chemmater.2c02925	journal	December 2022
The influence of LiH and TiH2 on hydrogen storage in MgB2 I: Promotion of bulk hydrogenation at reduced temperature Snider, J. L.; Liu, Y. -S.; Sawvel, A. M. International Journal of Hydrogen Energy, Vol. 47, Issue 1 https://doi.org/10.1016/j.ijhydene.2021.09.169	journal	January 2022
Challenges to developing materials for the transport and storage of hydrogen Allendorf, Mark D.; Stavila, Vitalie; Snider, Jonathan L. Nature Chemistry, Vol. 14, Issue 11 https://doi.org/10.1038/s41557-022-01056-2	journal	October 2022
Magnesium borohydride Mg(BH4)2 for energy applications: A review Li, Xiao; Yan, Yigang; Jensen, Torben R. Journal of Materials Science & Technology, Vol. 161 https://doi.org/10.1016/j.jmst.2023.03.040	journal	October 2023
Development of group II borohydrides as hydrogen storage materials Rönnebro, Ewa Current Opinion in Solid State and Materials Science, Vol. 15, Issue 2 https://doi.org/10.1016/j.cossms.2010.10.003	journal	April 2011
Interfacial Insight from Operando XAS/TEM for Magnesium Metal Deposition with Borohydride Electrolytes Arthur, Timothy S.; Glans, Per-Anders; Singh, Nikhilendra Chemistry of Materials, Vol. 29, Issue 17 https://doi.org/10.1021/acs.chemmater.7b01189	journal	August 2017
Complex Hydrides for Hydrogen Storage Orimo, Shin-ichi; Nakamori, Yuko; Eliseo, Jennifer R. Chemical Reviews, Vol. 107, Issue 10 https://doi.org/10.1021/cr0501846	journal	October 2007
Inducing One‐Step Dehydrogenation of Magnesium Borohydride via Confinement in Robust Dodecahedral Nitrogen‐Doped Porous Carbon Scaffold Jia, Yuxiao; Han, Bo; Wang, Jianchuan Advanced Materials https://doi.org/10.1002/adma.202406152	journal	July 2024
Complex hydrides for energy storage Milanese, C.; Jensen, T. R.; Hauback, B. C. International Journal of Hydrogen Energy, Vol. 44, Issue 15 https://doi.org/10.1016/j.ijhydene.2018.11.208	journal	March 2019
Differential Scanning Calorimetry Measurements of Magnesium Borohydride Mg(BH₄)₂ Yan, Yigang; Li, Hai-Wen; Nakamori, Yuko MATERIALS TRANSACTIONS, Vol. 49, Issue 11 https://doi.org/10.2320/matertrans.MEP2008224	journal	January 2008
Hydrogen storage properties of γ–Mg(BH4)2 modified by MoO3 and TiO2 Saldan, I.; Frommen, C.; Llamas-Jansa, I. International Journal of Hydrogen Energy, Vol. 40, Issue 36 https://doi.org/10.1016/j.ijhydene.2015.07.082	journal	September 2015
Reversible dehydrogenation of magnesium borohydride to magnesium triborane in the solid state under moderate conditions Chong, Marina; Karkamkar, Abhi; Autrey, Tom Chem. Commun., Vol. 47, Issue 4 https://doi.org/10.1039/C0CC03461D	journal	January 2011
DIOPTAS : a program for reduction of two-dimensional X-ray diffraction data and data exploration Prescher, Clemens; Prakapenka, Vitali B. High Pressure Research, Vol. 35, Issue 3 https://doi.org/10.1080/08957959.2015.1059835	journal	May 2015

Similar Records

Direct Hydrogenation Magnesium Boride to Magnesium Borohydride: Demonstration of >11 Weight Percent Reversible Hydrogen Storage

Journal Article · Mon Nov 15 23:00:00 EST 2010 · Chemical Communications, 46(3):421-423 · OSTI ID:972526

Melting of Magnesium Borohydride under High Hydrogen Pressure: Thermodynamic Stability and Effects of Nanoconfinement

Journal Article · Tue Jul 14 00:00:00 EDT 2020 · Chemistry of Materials · OSTI ID:1673309

Melting of Magnesium Borohydride under High Hydrogen Pressure: Thermodynamic Stability and Effects of Nanoconfinement

Journal Article · Thu Jun 04 00:00:00 EDT 2020 · Chemistry of Materials · OSTI ID:1665874

Related Subjects

MATERIALS SCIENCE
complex hydrides
doping
graphene additives
hydrogen storage
magnesium boride
magnesium borohydride
structural defects

Graphene Activated Magnesium Diboride for Moderate Pressure and Temperature Hydrogenation to Magnesium Borohydride

Citation Formats

References (42)

Similar Records

Related Subjects