DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: 2D Nitrogen‐Doped Graphene Materials for Noble Gas Separation

Journal Article · · Small
ORCiD logo [1];  [2]; ORCiD logo [3];  [4];  [2]; ORCiD logo [5]; ORCiD logo [2]; ORCiD logo [5]; ORCiD logo [5];  [2]; ORCiD logo [6]; ORCiD logo [7]
  1. Regional Centre of Advanced Technologies and Materials Czech Advanced Technology and Research Institute (CATRIN) Palacký University Olomouc Šlechtitelů 27 Olomouc 783 71 Czech Republic
  2. Energy and Environmental Directorate, Pacific Northwest National Laboratory Richland WA 99352 USA
  3. IT4Innovations VŠB–Technical University of Ostrava 17. listopadu 2172/15 Ostrava‐Poruba 708 00 Czech Republic
  4. Hybrid Porous Materials Laboratory, Department of Chemistry Indian Institute of Technology Jammu Jammu and Kashmir 181221 India
  5. Regional Centre of Advanced Technologies and Materials Czech Advanced Technology and Research Institute (CATRIN) Palacký University Olomouc Šlechtitelů 27 Olomouc 783 71 Czech Republic, Nanotechnology Centre CEET VŠB‐Technical University of Ostrava 17. listopadu 2172/15 Ostrava‐Poruba 708 00 Czech Republic
  6. Regional Centre of Advanced Technologies and Materials Czech Advanced Technology and Research Institute (CATRIN) Palacký University Olomouc Šlechtitelů 27 Olomouc 783 71 Czech Republic, Hybrid Porous Materials Laboratory, Department of Chemistry Indian Institute of Technology Jammu Jammu and Kashmir 181221 India
  7. Regional Centre of Advanced Technologies and Materials Czech Advanced Technology and Research Institute (CATRIN) Palacký University Olomouc Šlechtitelů 27 Olomouc 783 71 Czech Republic, IT4Innovations VŠB–Technical University of Ostrava 17. listopadu 2172/15 Ostrava‐Poruba 708 00 Czech Republic

Abstract Noble gases, notably xenon, play a pivotal role in diverse high‐tech applications. However, manufacturing xenon is an inherently challenging task, due to its unique properties and trace abundance in the Earth's atmosphere. Consequently, there is a pressing need for the development of efficient methods for the separation of noble gases. Using mild fluorographene chemistry, nitrogen‐doped graphene (GNs) materials are synthesized with abundant aromatic regions and extensive nitrogen doping within the vacancies and holes of the aromatic lattice. Due to the organized interlayer “nanochannels”, nitrogen functional groups, and defects within the two‐dimensional (2D) structures, GNs exhibits effective selectivity for Xe over Kr at low pressure. This enhanced selectivity is attributed to the stronger binding affinity of Xe to GN compared to Kr. The adsorption is governed by London dispersion forces, as revealed by theoretical calculations using symmetry‐adapted perturbation theory (SAPT). Investigation of other GNs differing in nitrogen content, surface area, and pore sizes underscores the significance of nitrogen functional groups, defects, and interlayer nanochannels over the surface area in achieving superior selectivity. This work offers a new perspective on the design and fabrication of functionalized graphene derivatives, exhibiting superior noble gas storage and separation activity exploitable in gas production technologies.

Sponsoring Organization:
USDOE
Grant/Contract Number:
AC05-76RL01830
OSTI ID:
2476555
Journal Information:
Small, Journal Name: Small Journal Issue: 6 Vol. 21; ISSN 1613-6810
Publisher:
Wiley Blackwell (John Wiley & Sons)Copyright Statement
Country of Publication:
Germany
Language:
English

References (54)

Self‐Adjusting Metal–Organic Framework for Efficient Capture of Trace Xenon and Krypton journal January 2022
Graphene Fluoride: A Stable Stoichiometric Graphene Derivative and its Chemical Conversion to Graphene journal November 2010
User-friendly graphical user interface software for ideal adsorbed solution theory calculations journal November 2017
Separation of noble gases through nano porous material membranes journal December 2020
Tunable nano-wrinked channels of reduced graphene oxide membranes for molecular sieving gas separation journal January 2024
Effect of functional groups on separating carbon dioxide from CO2/N2 gas mixtures using edge functionalized graphene nanoribbons journal January 2015
Xenon Gas Separation and Storage Using Metal-Organic Frameworks journal March 2018
Microporous Metal-Organic Framework Materials for Gas Separation journal February 2020
Graphene and graphene oxide membranes for gas separation applications journal May 2017
Two-dimensional materials for gas separation membranes journal March 2023
Effects of natural zeolites on field-scale geologic noble gas transport journal September 2020
Aluminum-based microporous metal–organic framework for noble gas separation journal February 2023
Tunable sieving of small gas molecules using horizontal graphene oxide membrane journal September 2020
The effect of doping on adsorption of Xe and Kr on graphyne and graphdiyne journal March 2020
Efficient Xe/Kr separation on two Metal-Organic frameworks with distinct pore shapes journal November 2021
Breaking trade-off effect of Xe/Kr separation on microporous and heteroatoms-rich carbon adsorbents journal March 2023
Computation-informed optimization of Ni(PyC)2 functionalization for noble gas separations journal September 2022
Two-Dimensional-Material Membranes: Manipulating the Transport Pathway for Molecular Separation journal January 2021
Hybrid Two-Dimensional Porous Materials journal October 2023
Facile Preparation of Graphene Oxide Membranes for Gas Separation journal April 2016
Graphene-Based Metal–Organic Framework Hybrids for Applications in Catalysis, Environmental, and Energy Technologies journal November 2022
Metal–Organic Frameworks Possessing Suitable Pores for Xe/Kr Separation journal March 2024
Impact of Edge Groups on the Hydration and Aggregation Properties of Graphene Oxide journal February 2018
Tunable Sub-nanopores of Graphene Flake Interlayers with Conductive Molecular Linkers for Supercapacitors journal June 2016
Electron–Hole Symmetry Breaking in Charge Transport in Nitrogen-Doped Graphene journal April 2017
Local Plasmon Engineering in Doped Graphene journal February 2018
Tunable Synthesis of Nitrogen Doped Graphene from Fluorographene under Mild Conditions journal February 2020
Atomic-Scale Charge Distribution Mapping of Single Substitutional p- and n-Type Dopants in Graphene journal February 2020
Potential of Metal–Organic Frameworks for Separation of Xenon and Krypton journal December 2014
Metal–Organic Frameworks for Separations journal September 2011
Carbon Dioxide Capture in Metal–Organic Frameworks journal September 2011
Functionalization of Graphene: Covalent and Non-Covalent Approaches, Derivatives and Applications journal September 2012
A Two-Column Method for the Separation of Kr and Xe from Process Off-Gases journal July 2014
Programmed Polarizability Engineering in a Cyclen-Based Cubic Zr(IV) Metal–Organic Framework to Boost Xe/Kr Separation journal January 2023
Electrostatic Doping of Graphene through Ultrathin Hexagonal Boron Nitride Films journal November 2011
Porous Graphene as the Ultimate Membrane for Gas Separation journal December 2009
Halogenated Graphenes: Rapidly Growing Family of Graphene Derivatives journal July 2013
Improvements in noble gas separation methodology: A nude cryogenic trap journal December 2001
Metal–organic framework with optimally selective xenon adsorption and separation journal June 2016
Proton and molecular permeation through the basal plane of monolayer graphene oxide journal November 2023
ZIF-Derived Nitrogen-Doped Porous Carbons for Xe Adsorption and Separation journal February 2016
Hybrid porous solids past, present, future journal January 2008
Graphene and graphene oxide: advanced membranes for gas separation and water purification journal January 2015
Modulating the electronic and magnetic properties of graphene journal January 2017
Two-dimensional nanosheet-based gas separation membranes journal January 2018
Selective separation of Xe/Kr and adsorption of water in a microporous hydrogen-bonded organic framework journal January 2019
Two-dimensional material membranes for critical separations journal January 2020
Nitrogen doped graphene with diamond-like bonds achieves unprecedented energy density at high power in a symmetric sustainable supercapacitor journal January 2022
Emerging graphene derivatives as active 2D coordination platforms for single-atom catalysts journal January 2022
Recent advances in the applications of graphene materials for the oil and gas industry journal January 2023
Selective gas adsorption and separation in metal–organic frameworks journal January 2009
Systematic Design of Pore Size and Functionality in Isoreticular MOFs and Their Application in Methane Storage journal January 2002
The Chemistry and Applications of Metal-Organic Frameworks journal August 2013
ОТРИМАННЯ КРИПТОНУ І КСЕНОНУ ВИСОКОЇ ЧИСТОТИ journal January 2024