Catalytic molten metals for the direct conversion of methane to hydrogen and separable carbon
Abstract
Metals that are active catalysts for methane (Ni, Pt, Pd), when dissolved in inactive low–melting temperature metals (In, Ga, Sn, Pb), produce stable molten metal alloy catalysts for pyrolysis of methane into hydrogen and carbon. All solid catalysts previously used for this reaction have been deactivated by carbon deposition. In the molten alloy system, the insoluble carbon floats to the surface where it can be skimmed off. A 27% Ni–73% Bi alloy achieved 95% methane conversion at 1065°C in a 1.1-meter bubble column and produced pure hydrogen without CO 2 or other by-products. Calculations show that the active metals in the molten alloys are atomically dispersed and negatively charged. There is a correlation between the amount of charge on the atoms and their catalytic activity.
- Authors:
-
- Department of Chemistry and Biochemistry, University of California, Santa Barbara, CA 93106-9510, USA.
- Department of Chemistry and Biochemistry, University of California, Santa Barbara, CA 93106-9510, USA., Department of Chemical Engineering, Indian Institute of Technology, Kanpur 208016, Uttar Pradesh, India.
- Department of Chemical Engineering, University of California, Santa Barbara, CA 93106-5080, USA.
- Publication Date:
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1436909
- Grant/Contract Number:
- FG03-89ER14048
- Resource Type:
- Published Article
- Journal Name:
- Science
- Additional Journal Information:
- Journal Name: Science Journal Volume: 358 Journal Issue: 6365; Journal ID: ISSN 0036-8075
- Publisher:
- American Association for the Advancement of Science (AAAS)
- Country of Publication:
- United States
- Language:
- English
Citation Formats
Upham, D. Chester, Agarwal, Vishal, Khechfe, Alexander, Snodgrass, Zachary R., Gordon, Michael J., Metiu, Horia, and McFarland, Eric W. Catalytic molten metals for the direct conversion of methane to hydrogen and separable carbon. United States: N. p., 2017.
Web. doi:10.1126/science.aao5023.
Upham, D. Chester, Agarwal, Vishal, Khechfe, Alexander, Snodgrass, Zachary R., Gordon, Michael J., Metiu, Horia, & McFarland, Eric W. Catalytic molten metals for the direct conversion of methane to hydrogen and separable carbon. United States. https://doi.org/10.1126/science.aao5023
Upham, D. Chester, Agarwal, Vishal, Khechfe, Alexander, Snodgrass, Zachary R., Gordon, Michael J., Metiu, Horia, and McFarland, Eric W. Thu .
"Catalytic molten metals for the direct conversion of methane to hydrogen and separable carbon". United States. https://doi.org/10.1126/science.aao5023.
@article{osti_1436909,
title = {Catalytic molten metals for the direct conversion of methane to hydrogen and separable carbon},
author = {Upham, D. Chester and Agarwal, Vishal and Khechfe, Alexander and Snodgrass, Zachary R. and Gordon, Michael J. and Metiu, Horia and McFarland, Eric W.},
abstractNote = {Metals that are active catalysts for methane (Ni, Pt, Pd), when dissolved in inactive low–melting temperature metals (In, Ga, Sn, Pb), produce stable molten metal alloy catalysts for pyrolysis of methane into hydrogen and carbon. All solid catalysts previously used for this reaction have been deactivated by carbon deposition. In the molten alloy system, the insoluble carbon floats to the surface where it can be skimmed off. A 27% Ni–73% Bi alloy achieved 95% methane conversion at 1065°C in a 1.1-meter bubble column and produced pure hydrogen without CO 2 or other by-products. Calculations show that the active metals in the molten alloys are atomically dispersed and negatively charged. There is a correlation between the amount of charge on the atoms and their catalytic activity.},
doi = {10.1126/science.aao5023},
journal = {Science},
number = 6365,
volume = 358,
place = {United States},
year = {2017},
month = {11}
}
https://doi.org/10.1126/science.aao5023
Web of Science
Works referenced in this record:
Decarbonisation of fossil energy via methane pyrolysis using two reactor concepts: Fluid wall flow reactor and molten metal capillary reactor
journal, September 2015
- Schultz, Ina; Agar, David W.
- International Journal of Hydrogen Energy, Vol. 40, Issue 35
Generalized Gradient Approximation Made Simple
journal, October 1996
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
Development of methane decarbonisation based on liquid metal technology for CO2-free production of hydrogen
journal, May 2016
- Abánades, Alberto; Rathnam, Renu Kumar; Geißler, Tobias
- International Journal of Hydrogen Energy, Vol. 41, Issue 19
Experimental investigation and thermo-chemical modeling of methane pyrolysis in a liquid metal bubble column reactor with a packed bed
journal, November 2015
- Geißler, T.; Plevan, M.; Abánades, A.
- International Journal of Hydrogen Energy, Vol. 40, Issue 41
A molecular dynamics method for simulations in the canonical ensemble
journal, June 1984
- Nosé, Shūichi
- Molecular Physics, Vol. 52, Issue 2
Technological challenges for industrial development of hydrogen production based on methane cracking
journal, October 2012
- Abánades, A.; Rubbia, C.; Salmieri, D.
- Energy, Vol. 46, Issue 1
An experimental proof for negative oxidation states of platinum: ESCA-measurements on barium platinides
journal, January 2006
- Karpov, Andrey; Konuma, Mitsuharu; Jansen, Martin
- Chemical Communications, Issue 8
Computer "Experiments" on Classical Fluids. I. Thermodynamical Properties of Lennard-Jones Molecules
journal, July 1967
- Verlet, Loup
- Physical Review, Vol. 159, Issue 1
Initial Experimental and Theoretical Investigation of Solar Molten Media Methane Cracking for Hydrogen Production
journal, January 2014
- Paxman, D.; Trottier, S.; Nikoo, M.
- Energy Procedia, Vol. 49
Projector augmented-wave method
journal, December 1994
- Blöchl, P. E.
- Physical Review B, Vol. 50, Issue 24, p. 17953-17979
Oxygen Vacancy Formation on α-MoO 3 Slabs and Ribbons
journal, August 2016
- Agarwal, Vishal; Metiu, Horia
- The Journal of Physical Chemistry C, Vol. 120, Issue 34
Catalytic activity of carbons for methane decomposition reaction
journal, May 2005
- Muradov, Nazim; Smith, Franklyn; T-Raissi, Ali
- Catalysis Today, Vol. 102-103
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996
- Kresse, G.; Furthmüller, J.
- Computational Materials Science, Vol. 6, Issue 1, p. 15-50
Thermo-catalytic decomposition of methane: The effect of reaction parameters on process design and the utilization possibilities of the produced carbon
journal, October 2016
- Keipi, Tiina; Tolvanen, Katariina E. S.; Tolvanen, Henrik
- Energy Conversion and Management, Vol. 126
Bismuth Toxicity, Often Mild, Can Result in Severe Poisonings
journal, January 2001
- DiPalma, Joseph R.
- Emergency Medicine News, Vol. 23, Issue 3
Catalysis of methane decomposition over elemental carbon
journal, July 2001
- Muradov, N.
- Catalysis Communications, Vol. 2, Issue 3-4
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996
- Kresse, G.; Furthmüller, J.
- Physical Review B, Vol. 54, Issue 16, p. 11169-11186
Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium
journal, May 1994
- Kresse, G.; Hafner, J.
- Physical Review B, Vol. 49, Issue 20, p. 14251-14269
Techno-Economic Analysis of Methane Pyrolysis in Molten Metals: Decarbonizing Natural Gas
journal, March 2017
- Parkinson, Brett; Matthews, Joshua W.; McConnaughy, Thomas B.
- Chemical Engineering & Technology, Vol. 40, Issue 6
THE ACTIVATION ENERGY FOR THE PYROLYSIS OF METHANE 1
journal, March 1963
- Palmer, Howard B.; Hirt, Thomas J.
- The Journal of Physical Chemistry, Vol. 67, Issue 3
Hydrogen production via methane pyrolysis in a liquid metal bubble column reactor with a packed bed
journal, September 2016
- Geißler, T.; Abánades, A.; Heinzel, A.
- Chemical Engineering Journal, Vol. 299
Nonoxidative Activation of Methane
journal, January 2003
- Choudhary, Tushar V.; Aksoylu, Erhan; Wayne Goodman, D.
- Catalysis Reviews, Vol. 45, Issue 1
A fast and robust algorithm for Bader decomposition of charge density
journal, June 2006
- Henkelman, Graeme; Arnaldsson, Andri; Jónsson, Hannes
- Computational Materials Science, Vol. 36, Issue 3
How to produce hydrogen from fossil fuels without CO2 emission
journal, March 1993
- Muradov, N.
- International Journal of Hydrogen Energy, Vol. 18, Issue 3
Hydrogen production by methane decomposition: A review
journal, February 2010
- Abbas, Hazzim F.; Wan Daud, W. M. A.
- International Journal of Hydrogen Energy, Vol. 35, Issue 3, p. 1160-1190
Canonical dynamics: Equilibrium phase-space distributions
journal, March 1985
- Hoover, William G.
- Physical Review A, Vol. 31, Issue 3
Sankey-Diagram-based insights into the hydrogen economy of today
journal, May 2016
- Bakenne, Adetokunboh; Nuttall, William; Kazantzis, Nikolaos
- International Journal of Hydrogen Energy, Vol. 41, Issue 19
Ab initiomolecular dynamics for liquid metals
journal, January 1993
- Kresse, G.; Hafner, J.
- Physical Review B, Vol. 47, Issue 1, p. 558-561
Pyrolysis of methane and the role of surface area
journal, February 1989
- Van Der Zwet, G. P.; Hendriks, P. A. J. M.; Van Santen, R. A.
- Catalysis Today, Vol. 4, Issue 3-4
Thermal cracking of methane in a liquid metal bubble column reactor: Experiments and kinetic analysis
journal, July 2015
- Plevan, M.; Geißler, T.; Abánades, A.
- International Journal of Hydrogen Energy, Vol. 40, Issue 25
Hydrogen Production by Direct Contact Pyrolysis of Natural Gas
journal, May 2003
- Serban, Manuela; Lewis, Michele A.; Marshall, Christopher L.
- Energy & Fuels, Vol. 17, Issue 3
A unified formulation of the constant temperature molecular dynamics methods
journal, July 1984
- Nosé, Shuichi
- The Journal of Chemical Physics, Vol. 81, Issue 1
A comparative overview of hydrogen production processes
journal, January 2017
- Nikolaidis, Pavlos; Poullikkas, Andreas
- Renewable and Sustainable Energy Reviews, Vol. 67
Experimental analysis of direct thermal methane cracking
journal, October 2011
- Abánades, A.; Ruiz, E.; Ferruelo, E. M.
- International Journal of Hydrogen Energy, Vol. 36, Issue 20
Hydrogen generation by direct decomposition of hydrocarbons over molten magnesium
journal, March 2008
- Wang, K.; Li, W. S.; Zhou, X. P.
- Journal of Molecular Catalysis A: Chemical, Vol. 283, Issue 1-2
A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu
journal, April 2010
- Grimme, Stefan; Antony, Jens; Ehrlich, Stephan
- The Journal of Chemical Physics, Vol. 132, Issue 15
Cs2Pt: A Platinide(-II) Exhibiting Complete Charge Separation
journal, October 2003
- Karpov, Andrey; Nuss, Jürgen; Wedig, Ulrich
- Angewandte Chemie International Edition, Vol. 42, Issue 39