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

Title: Graphene oxide/metal nanocrystal multilaminates as the atomic limit for safe and selective hydrogen storage

Abstract

© 2016, Nature Publishing Group. All rights reserved. Interest in hydrogen fuel is growing for automotive applications; however, safe, dense, solid-state hydrogen storage remains a formidable scientific challenge. Metal hydrides offer ample storage capacity and do not require cryogens or exceedingly high pressures for operation. However, hydrides have largely been abandoned because of oxidative instability and sluggish kinetics. We report a new, environmentally stable hydrogen storage material constructed of Mg nanocrystals encapsulated by atomically thin and gas-selective reduced graphene oxide (rGO) sheets. This material, protected from oxygen and moisture by the rGO layers, exhibits exceptionally dense hydrogen storage (6.5 wt% and 0.105 kg H 2 per litre in the total composite). As rGO is atomically thin, this approach minimizes inactive mass in the composite, while also providing a kinetic enhancement to hydrogen sorption performance. These multilaminates of rGO-Mg are able to deliver exceptionally dense hydrogen storage and provide a material platform for harnessing the attributes of sensitive nanomaterials in demanding environments.

Authors:
 [1];  [1];  [1];  [2];  [2];  [1]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1255552
Alternate Identifier(s):
OSTI ID: 1379103
Grant/Contract Number:  
AC02-05CH11231; EE0004946; AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
08 HYDROGEN

Citation Formats

Cho, Eun Seon, Ruminski, Anne M., Aloni, Shaul, Liu, Yi-Sheng, Guo, Jinghua, and Urban, Jeffrey J. Graphene oxide/metal nanocrystal multilaminates as the atomic limit for safe and selective hydrogen storage. United States: N. p., 2016. Web. doi:10.1038/ncomms10804.
Cho, Eun Seon, Ruminski, Anne M., Aloni, Shaul, Liu, Yi-Sheng, Guo, Jinghua, & Urban, Jeffrey J. Graphene oxide/metal nanocrystal multilaminates as the atomic limit for safe and selective hydrogen storage. United States. https://doi.org/10.1038/ncomms10804
Cho, Eun Seon, Ruminski, Anne M., Aloni, Shaul, Liu, Yi-Sheng, Guo, Jinghua, and Urban, Jeffrey J. Tue . "Graphene oxide/metal nanocrystal multilaminates as the atomic limit for safe and selective hydrogen storage". United States. https://doi.org/10.1038/ncomms10804. https://www.osti.gov/servlets/purl/1255552.
@article{osti_1255552,
title = {Graphene oxide/metal nanocrystal multilaminates as the atomic limit for safe and selective hydrogen storage},
author = {Cho, Eun Seon and Ruminski, Anne M. and Aloni, Shaul and Liu, Yi-Sheng and Guo, Jinghua and Urban, Jeffrey J.},
abstractNote = {© 2016, Nature Publishing Group. All rights reserved. Interest in hydrogen fuel is growing for automotive applications; however, safe, dense, solid-state hydrogen storage remains a formidable scientific challenge. Metal hydrides offer ample storage capacity and do not require cryogens or exceedingly high pressures for operation. However, hydrides have largely been abandoned because of oxidative instability and sluggish kinetics. We report a new, environmentally stable hydrogen storage material constructed of Mg nanocrystals encapsulated by atomically thin and gas-selective reduced graphene oxide (rGO) sheets. This material, protected from oxygen and moisture by the rGO layers, exhibits exceptionally dense hydrogen storage (6.5 wt% and 0.105 kg H 2 per litre in the total composite). As rGO is atomically thin, this approach minimizes inactive mass in the composite, while also providing a kinetic enhancement to hydrogen sorption performance. These multilaminates of rGO-Mg are able to deliver exceptionally dense hydrogen storage and provide a material platform for harnessing the attributes of sensitive nanomaterials in demanding environments.},
doi = {10.1038/ncomms10804},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = {Tue Feb 23 00:00:00 EST 2016},
month = {Tue Feb 23 00:00:00 EST 2016}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 190 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Precise and Ultrafast Molecular Sieving Through Graphene Oxide Membranes
journal, February 2014


Size-Dependent Hydrogen Storage Properties of Mg Nanocrystals Prepared from Solution
journal, July 2011

  • Norberg, Nick S.; Arthur, Timothy S.; Fredrick, Sarah J.
  • Journal of the American Chemical Society, Vol. 133, Issue 28
  • DOI: 10.1021/ja201791y

Probing the Thermal Deoxygenation of Graphene Oxide Using High-Resolution In Situ X-ray-Based Spectroscopies
journal, August 2011

  • Ganguly, Abhijit; Sharma, Surbhi; Papakonstantinou, Pagona
  • The Journal of Physical Chemistry C, Vol. 115, Issue 34
  • DOI: 10.1021/jp203741y

High capacity hydrogenstorage materials: attributes for automotive applications and techniques for materials discovery
journal, January 2010

  • Yang, Jun; Sudik, Andrea; Wolverton, Christopher
  • Chem. Soc. Rev., Vol. 39, Issue 2
  • DOI: 10.1039/B802882F

Hydrogen in magnesium: new perspectives toward functional stores
journal, January 2010

  • Aguey-Zinsou, Kondo-François; Ares-Fernández, José-Ramón
  • Energy & Environmental Science, Vol. 3, Issue 5
  • DOI: 10.1039/b921645f

The impact of carbon materials on the hydrogen storage properties of light metal hydrides
journal, January 2011

  • Adelhelm, Philipp; de Jongh, Petra E.
  • J. Mater. Chem., Vol. 21, Issue 8
  • DOI: 10.1039/C0JM02593C

Mg-Based Nanocomposites with High Capacity and Fast Kinetics for Hydrogen Storage
journal, June 2006

  • Yao, Xiangdong; Wu, Chengzhang; Du, Aijun
  • The Journal of Physical Chemistry B, Vol. 110, Issue 24
  • DOI: 10.1021/jp057526w

Ultrathin, Molecular-Sieving Graphene Oxide Membranes for Selective Hydrogen Separation
journal, October 2013


Hydrogen vehicles: Fuel of the future?
journal, April 2010


Electric Field Effect in Atomically Thin Carbon Films
journal, October 2004


Hydrogen sorption properties of magnesium particles decorated with metallic nanoparticles as catalyst
journal, May 2009


Graphene: Status and Prospects
journal, June 2009


Metallic and Carbon Nanotube-Catalyzed Coupling of Hydrogenation in Magnesium
journal, December 2007

  • Yao, Xiangdong; Wu, Chengzhang; Du, Aijun
  • Journal of the American Chemical Society, Vol. 129, Issue 50
  • DOI: 10.1021/ja0751431

Visible-light-induced photocatalyst based on C-doped LaCoO3 synthesized by novel microorganism chelate method
journal, March 2009


Synergistic enhancement of hydrogen storage and air stability via Mg nanocrystal–polymer interfacial interactions
journal, January 2013

  • Ruminski, Anne M.; Bardhan, Rizia; Brand, Alyssa
  • Energy & Environmental Science, Vol. 6, Issue 11
  • DOI: 10.1039/c3ee41977k

A Simple Two-Step Template Approach for Preparing Carbon-Doped Mesoporous TiO 2 Hollow Microspheres
journal, July 2009

  • Wang, Haiqiang; Wu, Zhongbiao; Liu, Yue
  • The Journal of Physical Chemistry C, Vol. 113, Issue 30
  • DOI: 10.1021/jp9047693

Synthesis of nanocrystalline MgH2 powder by gas-phase condensation and in situ hydridation: TEM, XPS and XRD study
journal, May 2007


Preparation of Organometallic Compounds from Highly Reactive Metal Powders
journal, December 1989


Hydrogen-storage materials for mobile applications
journal, November 2001

  • Schlapbach, Louis; Züttel, Andreas
  • Nature, Vol. 414, Issue 6861
  • DOI: 10.1038/35104634

Nanotechnology in Mg-based materials for hydrogen storage
journal, July 2012


Selective Gas Transport Through Few-Layered Graphene and Graphene Oxide Membranes
journal, October 2013


Rate determining step in the absorption and desorption of hydrogen by magnesium
journal, June 2002


Air-stable magnesium nanocomposites provide rapid and high-capacity hydrogen storage without using heavy-metal catalysts
journal, March 2011

  • Jeon, Ki-Joon; Moon, Hoi Ri; Ruminski, Anne M.
  • Nature Materials, Vol. 10, Issue 4
  • DOI: 10.1038/nmat2978

Raman spectroscopy as a versatile tool for studying the properties of graphene
journal, April 2013


An ultrafast nickel–iron battery from strongly coupled inorganic nanoparticle/nanocarbon hybrid materials
journal, January 2012

  • Wang, Hailiang; Liang, Yongye; Gong, Ming
  • Nature Communications, Vol. 3, Issue 1
  • DOI: 10.1038/ncomms1921

Raman Spectrum of Graphene and Graphene Layers
journal, October 2006


Catalytic Effects of Subsurface Carbon in the Chemisorption of Hydrogen on a Mg(0001) Surface:  an Ab-initio Study
journal, February 2006

  • Du, A. J.; Smith, Sean C.; Yao, X. D.
  • The Journal of Physical Chemistry B, Vol. 110, Issue 4
  • DOI: 10.1021/jp055972d

Tailoring the hydrogen storage properties of Li4BN3H10 by confinement into highly ordered nanoporous carbon
journal, January 2013

  • Liu, Xiangfeng; Peaslee, David; Majzoub, E. H.
  • Journal of Materials Chemistry A, Vol. 1, Issue 12
  • DOI: 10.1039/c3ta00174a

One-Pot Synthesis of Platinum Nanoparticles Embedded on Reduced Graphene Oxide for Oxygen Reduction in Methanol Fuel Cells
journal, January 2011

  • Ha, Hyung-Wook; Kim, In Young; Hwang, Seong-Ju
  • Electrochemical and Solid-State Letters, Vol. 14, Issue 7
  • DOI: 10.1149/1.3584092

Hydrogen-storage materials for mobile applications
book, October 2010


Raman spectroscopy as a versatile tool for studying the properties of graphene.
text, January 2013

  • Ferrari, Andrea; Basko, Denis M.
  • Apollo - University of Cambridge Repository
  • DOI: 10.17863/cam.26732

Precise and ultrafast molecular sieving through graphene oxide membranes
text, January 2014


Electric Field Effect in Atomically Thin Carbon Films
text, January 2004


Graphene Oxide: A New Platform for High-Performance Gas- and Liquid-Separation Membranes
journal, July 2014

  • Smith, Zachary P.; Freeman, Benny D.
  • Angewandte Chemie International Edition, Vol. 53, Issue 39
  • DOI: 10.1002/anie.201404407

Metallic and Carbon Nanotube-Catalyzed Coupling of Hydrogenation in Magnesium
journal, December 2007

  • Yao, Xiangdong; Wu, Chengzhang; Du, Aijun
  • Journal of the American Chemical Society, Vol. 129, Issue 50
  • DOI: 10.1021/ja0751431

Size-Dependent Hydrogen Storage Properties of Mg Nanocrystals Prepared from Solution
journal, July 2011

  • Norberg, Nick S.; Arthur, Timothy S.; Fredrick, Sarah J.
  • Journal of the American Chemical Society, Vol. 133, Issue 28
  • DOI: 10.1021/ja201791y

Catalytic Effects of Subsurface Carbon in the Chemisorption of Hydrogen on a Mg(0001) Surface:  an Ab-initio Study
journal, February 2006

  • Du, A. J.; Smith, Sean C.; Yao, X. D.
  • The Journal of Physical Chemistry B, Vol. 110, Issue 4
  • DOI: 10.1021/jp055972d

Mg-Based Nanocomposites with High Capacity and Fast Kinetics for Hydrogen Storage
journal, June 2006

  • Yao, Xiangdong; Wu, Chengzhang; Du, Aijun
  • The Journal of Physical Chemistry B, Vol. 110, Issue 24
  • DOI: 10.1021/jp057526w

Hydrogen-storage materials for mobile applications
journal, November 2001

  • Schlapbach, Louis; Züttel, Andreas
  • Nature, Vol. 414, Issue 6861
  • DOI: 10.1038/35104634

Raman spectroscopy as a versatile tool for studying the properties of graphene
journal, April 2013


Electric Field Effect in Atomically Thin Carbon Films
journal, October 2004


Graphene: Status and Prospects
journal, June 2009


Ultrathin, Molecular-Sieving Graphene Oxide Membranes for Selective Hydrogen Separation
journal, October 2013


Preparation of Organometallic Compounds from Highly Reactive Metal Powders
journal, December 1989


Works referencing / citing this record:

Hierarchically Controlled Inside-Out Doping of Mg Nanocomposites for Moderate Temperature Hydrogen Storage
journal, October 2017

  • Cho, Eun Seon; Ruminski, Anne M.; Liu, Yi-Sheng
  • Advanced Functional Materials, Vol. 27, Issue 47
  • DOI: 10.1002/adfm.201704316

Local Structure and Chemistry of C-Doped ZnO@C Core-Shell Nanostructures with Room-Temperature Ferromagnetism
journal, December 2017

  • Ngo, Duc-The; Cuong, Le Thanh; Cuong, Nguyen Huu
  • Advanced Functional Materials, Vol. 28, Issue 8
  • DOI: 10.1002/adfm.201704567

Metal Hydride Nanoparticles with Ultrahigh Structural Stability and Hydrogen Storage Activity Derived from Microencapsulated Nanoconfinement
journal, April 2017

  • Zhang, Jiguang; Zhu, Yunfeng; Lin, Huaijun
  • Advanced Materials, Vol. 29, Issue 24
  • DOI: 10.1002/adma.201700760

Runaway Carbon Dioxide Conversion Leads to Enhanced Uptake in a Nanohybrid Form of Porous Magnesium Borohydride
journal, September 2019

  • Jeong, Sohee; Milner, Phillip J.; Wan, Liwen F.
  • Advanced Materials, Vol. 31, Issue 44
  • DOI: 10.1002/adma.201904252

Graphene-Based Nanocomposites for Energy Storage
journal, June 2016

  • Ji, Liwen; Meduri, Praveen; Agubra, Victor
  • Advanced Energy Materials, Vol. 6, Issue 16
  • DOI: 10.1002/aenm.201502159

Molecular Bridges Stabilize Graphene Oxide Membranes in Water
journal, January 2020

  • Zhang, Mengchen; Mao, Yangyang; Liu, Guozhen
  • Angewandte Chemie International Edition, Vol. 59, Issue 4
  • DOI: 10.1002/anie.201913010

Study of Ion Permeation through the Graphene Oxide/Polyether Sulfone Membranes
journal, January 2020


In‐Situ/Operando X‐ray Characterization of Metal Hydrides
journal, March 2019


Superior Hydrogen Absorption–Desorption Cycle Durability of Ball‐Milled 82MgH 2 ‐3PrH 2 ‐15Al Composite
journal, October 2019


Functionalized graphene materials for hydrogen storage
journal, November 2019


Magnesium–Graphene Composite Coated on SS Mesh as Cathode Material for Rechargeable Magnesium ion Battery
journal, May 2019

  • Malyala, Latha; Thatipamula, Sahithi; Jetti, Vatsala Rani
  • Transactions of the Indian Institute of Metals, Vol. 72, Issue 9
  • DOI: 10.1007/s12666-019-01718-9

Combining photocatalytic hydrogen generation and capsule storage in graphene based sandwich structures
journal, July 2017

  • Yang, Li; Li, Xiyu; Zhang, Guozhen
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms16049

Self-Printing on Graphitic Nanosheets with Metal Borohydride Nanodots for Hydrogen Storage
journal, August 2016

  • Li, Yongtao; Ding, Xiaoli; Zhang, Qingan
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep31144

Hydrogen-induced magnesium–zirconium interfacial coupling: enabling fast hydrogen sorption at lower temperatures
journal, January 2017

  • Ding, Xiaoli; Li, Yongtao; Fang, Fang
  • Journal of Materials Chemistry A, Vol. 5, Issue 10
  • DOI: 10.1039/c7ta00460e

Two- and three-dimensional graphene-based hybrid composites for advanced energy storage and conversion devices
journal, January 2018

  • Azadmanjiri, Jalal; Srivastava, Vijay K.; Kumar, Parshant
  • Journal of Materials Chemistry A, Vol. 6, Issue 3
  • DOI: 10.1039/c7ta08748a

Solid-phase hydrogen in a magnesium–carbon composite for efficient hydrogenation of carbon disulfide
journal, January 2018

  • Chen, Haipeng; Han, Zongying; Feng, Xun
  • Journal of Materials Chemistry A, Vol. 6, Issue 7
  • DOI: 10.1039/c7ta09289j

Facile synthesis of tin-doped mayenite electride composite as a non-noble metal durable electrocatalyst for oxygen reduction reaction (ORR)
journal, January 2018

  • Khan, Karim; Khan Tareen, Ayesha; Li, Jia
  • Dalton Transactions, Vol. 47, Issue 38
  • DOI: 10.1039/c8dt02548g

High loading nanoconfinement of V-decorated Mg with 1 nm carbon shells: hydrogen storage properties and catalytic mechanism
journal, January 2019

  • Chen, Ming; Hu, Miaomiao; Xie, Xiubo
  • Nanoscale, Vol. 11, Issue 20
  • DOI: 10.1039/c8nr09909j

Efficient hydrogen generation from water using nanocomposite flakes based on graphene and magnesium
journal, January 2018

  • Bartali, R.; Speranza, G.; Aguey-Zinsou, K. F.
  • Sustainable Energy & Fuels, Vol. 2, Issue 11
  • DOI: 10.1039/c8se00370j

Magnesium oxide clusters as promising candidates for hydrogen storage
journal, January 2019

  • Mojica-Sánchez, Juan Pablo; Zarate-López, Tania Isabel; Flores-Álvarez, José Manuel
  • Physical Chemistry Chemical Physics, Vol. 21, Issue 41
  • DOI: 10.1039/c9cp05075b

Molecular simulations of phenol and ibuprofen removal from water using multilayered graphene oxide membranes
journal, September 2019


Production and processing of graphene and related materials
journal, January 2020


Catalysis and Downsizing in Mg-Based Hydrogen Storage Materials
journal, February 2018


Differential Cytotoxicity of Different Sizes of Graphene Oxide Nanoparticles in Leydig (TM3) and Sertoli (TM4) Cells
journal, January 2019

  • Gurunathan, Sangiliyandi; Kang, Min-Hee; Jeyaraj, Muniyandi
  • Nanomaterials, Vol. 9, Issue 2
  • DOI: 10.3390/nano9020139

Production and processing of graphene and related materials
text, January 2020

  • Backes, C.; Abdelkader, Am; Alonso, C.
  • Apollo - University of Cambridge Repository
  • DOI: 10.17863/cam.63418

Molecular Bridges Stabilize Graphene Oxide Membranes in Water
journal, December 2019

  • Zhang, Mengchen; Mao, Yangyang; Liu, Guozhen
  • Angewandte Chemie, Vol. 132, Issue 4
  • DOI: 10.1002/ange.201913010

Production and processing of graphene and related materials
text, January 2020


Ultra-fast self-assembly and stabilization of reactive nanoparticles in reduced graphene oxide films
journal, August 2016

  • Chen, Yanan; Egan, Garth C.; Wan, Jiayu
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms12332

Combining photocatalytic hydrogen generation and capsule storage in graphene based sandwich structures
journal, July 2017

  • Yang, Li; Li, Xiyu; Zhang, Guozhen
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms16049

Characterization of nitrogen doped graphene bilayers synthesized by fast, low temperature microwave plasma-enhanced chemical vapour deposition
journal, September 2019


Self-Printing on Graphitic Nanosheets with Metal Borohydride Nanodots for Hydrogen Storage
journal, August 2016

  • Li, Yongtao; Ding, Xiaoli; Zhang, Qingan
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep31144

Production and processing of graphene and related materials
journal, January 2020


Differential Cytotoxicity of Different Sizes of Graphene Oxide Nanoparticles in Leydig (TM3) and Sertoli (TM4) Cells
journal, January 2019

  • Gurunathan, Sangiliyandi; Kang, Min-Hee; Jeyaraj, Muniyandi
  • Nanomaterials, Vol. 9, Issue 2
  • DOI: 10.3390/nano9020139