Skip to main content
OSTI.GOVU.S. Department of Energy Office of Scientific and Technical Information
U.S. Department of Energy
Office of Scientific and Technical Information
 

Mechanisms of adsorbing hydrogen gas on metal decorated graphene

Journal Article · · Physical Review Materials
 [1];  [2];  [3];  [4]
  1. University College London (United Kingdom)
  2. Università di Napoli Federico II (Italy)
  3. University of Cambridge (United Kingdom)
  4. University College London (United Kingdom); Università di Napoli Federico II (Italy)
+ Show Author Affiliations
Hydrogen is a key player in global strategies to reduce greenhouse gas emissions. In order to make hydrogen a widely used fuel, we require more efficient methods of storing it than the current standard of pressurized cylinders. An alternative method is to adsorb H2 in a material and avoid the use of high pressures. Among many potential materials, layered materials such as graphene present a practical advantage as they are lightweight. However, graphene and other 2D materials typically bind H2 too weakly to store it at the typical operating conditions of a hydrogen fuel cell, meaning that high pressure would still be required. Modifying the material, for example by decorating graphene with adatoms, can strengthen the adsorption energy of H2 molecules, but the underlying mechanisms are still not well understood. In this work, we systematically screen alkali and alkaline-earth metal decorated graphene sheets for the static thermodynamic adsorption of hydrogen gas from first principles and focus on the mechanisms of binding. We show that there are three mechanisms of adsorption on metal decorated graphene and each leads to distinctly different hydrogen adsorption structures. The three mechanisms can be described as weak van der Waals physisorption, metal adatom facilitated polarization, and Kubas adsorption. Among these mechanisms, we find that Kubas adsorption is easily perturbed by an external electric field, providing a way to tune H2 adsorption. In conclusion, this work is foundational and builds our understanding of H2 adsorption under idealized conditions.
Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF)
Sponsoring Organization:
EPSRC Tier-2 capital grant; Leverhulme Grant; USDOE Office of Science (SC); United Kingdom Car Parrinello (UKCP) consortium
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
2424022
Journal Information:
Physical Review Materials, Journal Name: Physical Review Materials Journal Issue: 3 Vol. 7; ISSN 2475-9953
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

References (62)

How to Design Hydrogen Storage Materials? Fundamentals, Synthesis, and Storage Tanks journal June 2019
The Hydrogen Issue journal December 2010
Review of operating condition, design parameters and material properties for proton exchange membrane fuel cells journal August 2020
Improved grid-based algorithm for Bader charge allocation journal January 2007
Pseudopotentials for H to Kr optimized for gradient-corrected exchange-correlation functionals journal May 2005
First principles calculations of H-storage in sorption materials journal May 2012
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set journal July 1996
Metal–dihydrogen and σ-bond coordination: the consummate extension of the Dewar–Chatt–Duncanson model for metal–olefin π bonding journal October 2001
A first-principles study of calcium-decorated, boron-doped graphene for high capacity hydrogen storage journal April 2011
A fast and robust algorithm for Bader decomposition of charge density journal June 2006
Quickstep: Fast and accurate density functional calculations using a mixed Gaussian and plane waves approach journal April 2005
Ab initio study of Kubas-type dihydrogen fixation onto d-orbital states of Ca adatoms journal September 2011
Tunable H2 binding on alkaline and alkaline earth metals decorated graphene substrates from first-principles calculations journal April 2017
Hydrogen storage on uncharged and positively charged Mg-decorated graphene journal February 2019
First-principles study of high-capacity hydrogen storage on graphene with Li atoms journal February 2012
Benchmarking Calculated Lattice Parameters and Energies of Molecular Crystals Using van der Waals Density Functionals journal July 2014
Improved Description of the Structure of Molecular and Layered Crystals: Ab Initio DFT Calculations with van der Waals Corrections journal November 2010
Effects of van der Waals Interactions in the Adsorption of Isooctane and Ethanol on Fe(100) Surfaces journal July 2014
Atomic Scale Identification of Coexisting Graphene Structures on Ni(111) journal January 2014
Optimum Conditions for Adsorptive Storage journal February 2006
Scaling laws for van der Waals interactions in nanostructured materials journal August 2013
Exceptional hydrogen storage achieved by screening nearly half a million metal-organic frameworks journal April 2019
An assessment of strategies for the development of solid-state adsorbents for vehicular hydrogen storage journal January 2018
Metals on graphene: correlation between adatom adsorption behavior and growth morphology journal January 2012
Improved tangent estimate in the nudged elastic band method for finding minimum energy paths and saddle points journal December 2000
A climbing image nudged elastic band method for finding saddle points and minimum energy paths journal December 2000
Theoretical evaluation of hydrogen storage capacity in pure carbon nanostructures journal July 2003
Gaussian basis sets for accurate calculations on molecular systems in gas and condensed phases journal September 2007
A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu journal April 2010
Metal-dispersed porous graphene for hydrogen storage journal February 2011
Assessing weak hydrogen binding on Ca + centers: An accurate many-body study with large basis sets journal October 2011
Perspective: Advances and challenges in treating van der Waals dispersion forces in density functional theory journal September 2012
The role of van der Waals forces in water adsorption on metals journal January 2013
Long-range correlation energy calculated from coupled atomic response functions journal May 2014
A van der Waals density functional theory comparison of metal decorated graphene systems for hydrogen adsorption journal June 2014
How strongly do hydrogen and water molecules stick to carbon nanomaterials? journal March 2017
Extension of the D3 dispersion coefficient model journal July 2017
First principles study of graphene on metals with the SCAN and SCAN+rVV10 functionals journal April 2019
The ORCA quantum chemistry program package journal June 2020
CP2K: An electronic structure and molecular dynamics software package - Quickstep: Efficient and accurate electronic structure calculations journal May 2020
Progress on first-principles-based materials design for hydrogen storage journal November 2012
A grid-based Bader analysis algorithm without lattice bias journal January 2009
Adsorbate-substrate and adsorbate-adsorbate interactions of Na and K adlayers on Al(111) journal December 1992
Ab initiomolecular dynamics for liquid metals journal January 1993
Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium journal May 1994
Periodic boundary conditions in ab initio calculations journal February 1995
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal October 1996
Separable dual-space Gaussian pseudopotentials journal July 1996
Hydrogen storage of calcium atoms adsorbed on graphene: First-principles plane wave calculations journal January 2009
Accuracy of density functional theory methods for weakly bonded systems: The case of dihydrogen binding on metal centers journal August 2010
Quantum Monte Carlo calculations of dihydrogen binding energetics on Ca cations: An assessment of errors in density functionals for weakly bonded systems journal August 2010
First-principles study of the stability of calcium-decorated carbon nanostructures journal October 2010
Graphene on Ni(111): Strong interaction and weak adsorption journal November 2011
van der Waals effects at molecule-metal interfaces journal September 2014
Spatially resolving density-dependent screening around a single charged atom in graphene journal May 2017
Inaccuracy of Density Functional Theory Calculations for Dihydrogen Binding Energetics onto Ca Cation Centers journal November 2009
Comment on “Inaccuracy of Density Functional Theory Calculations for Dihydrogen Binding Energetics onto Ca Cation Centers” journal April 2010
Accurate and Efficient Method for Many-Body van der Waals Interactions journal June 2012
Generalized Gradient Approximation Made Simple journal October 1996
Hydrogen Storage in Graphene-Based Materials: Efforts Towards Enhanced Hydrogen Absorption journal January 2013
Effect of Temperature on the Performance Factors and Durability of Proton Exchange Membrane of Hydrogen Fuel Cell: A Narrative Review journal August 2020
sumo: Command-line tools for plotting and analysis of periodic ab initio calculations journal August 2018

Similar Records

Unraveling H2 chemisorption and physisorption on metal decorated graphene using quantum Monte Carlo
Journal Article · Mon Nov 27 19:00:00 EST 2023 · Journal of Chemical Physics · OSTI ID:2582110
H{sub 2} adsorption in Li-decorated porous graphene
Journal Article · Wed Jun 24 00:00:00 EDT 2015 · AIP Conference Proceedings · OSTI ID:22490322
Metal-silicane: Stability and properties
Journal Article · Thu Aug 28 00:00:00 EDT 2014 · Journal of Applied Physics · OSTI ID:22314323

Related Subjects

36 MATERIALS SCIENCE
Adsorption
Chemical bonding
Electronic structure
Graphene
Hydrogen storage materials
Materials Science
Physisorption