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Title: Low-Temperature Methane Partial Oxidation to Syngas with Modular Nanocrystal Catalysts [Targeting Low-Temperature Methane Partial Oxidation to Syngas with Modular Nanocrystal Catalysts]

Journal Article · · ACS Applied Nano Materials

Here, the low-temperature conversion of methane into value-added products is an appealing goal due to the abundance of methane in the form of natural gas. Industrially, methane is used to produce synthesis gas (syngas), a precursor mixture used heavily in the production of ammonia, methanol, and synthetic fuels. In practice, this mixture is produced via the energy-intensive methane steam reforming reaction at temperatures between 750 and 1450 °C. The exothermic methane partial oxidation reaction stands as an alternative for syngas formation at lower temperatures, especially for gas to liquid fuels applications, yet awaits large-scale implementation due to dangerous operating conditions and temperatures. Using colloidally synthesized Ru catalysts, we identify two unifying rules that govern the low-temperature production of synthesis gas: depletion of oxygen within the catalyst bed and facile RuO2 → Ru reduction kinetics, which is a strong function of supporting material and Ru nanostructure. Using these design rules, we demonstrate the enhanced low-temperature activity of a bifunctional Ru/Pd catalyst which produces synthesis gas at ~400 °C, with nearly complete CH4 conversion and CO selectivity at 670 °C.

Research Organization:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
DGE-1656518
OSTI ID:
1471402
Journal Information:
ACS Applied Nano Materials, Vol. 1, Issue 9; ISSN 2574-0970
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 15 works
Citation information provided by
Web of Science

References (53)

The main catalytic challenges in GTL (gas-to-liquids) processes journal January 2011
Low temperature catalytic partial oxidation of methane for gas-to-liquids applications journal September 2005
Gas to liquids technologies for natural gas reserves valorization: The Eni experience journal April 2009
Methane activation: the past and future journal January 2014
Partial oxidation of methane to H2 and CO over Rh/SiO2 and Ru/SiO2 catalysts journal September 2004
Partial Oxidation of Methane to Syngas Over γ-Al 2 O 3 -Supported Rh Nanoparticles: Kinetic and Mechanistic Origins of Size Effect on Selectivity and Activity journal August 2014
Preparation and characterization of Ni based catalysts for the catalytic partial oxidation of methane: Effect of support basicity on H2/CO ratio and carbon deposition journal November 2010
Methane partial oxidation on NiCu-based catalysts journal July 2009
Partial oxidation of methane over ruthenium catalysts journal January 1993
Reaction Pathways and Site Requirements for the Activation and Chemical Conversion of Methane on Ru−Based Catalysts journal June 2004
XPS and FTIR Study of Ru/Al 2 O 3 and Ru/TiO 2 Catalysts:  Reduction Characteristics and Interaction with a Methane−Oxygen Mixture journal June 1999
The relevance of Ru nanoparticles morphology and oxidation state to the partial oxidation of methane journal November 2003
Partial oxidation of methane over supported ruthenium catalysts journal May 2007
Catalytic partial oxidation of methane to synthesis gas over a ruthenium catalyst: the role of the oxidation state journal January 2007
Partial oxidation of methane to synthesis gas via the direct reaction scheme over Ru/TiO2 catalyst journal January 1996
Comparison of Partial Oxidation and Steam-CO2Mixed Reformingof CH4to Syngas on MgO-Supported Metals journal March 1996
Visualizing a Catalyst at Work during the Ignition of the Catalytic Partial Oxidation of Methane journal January 2009
Partial oxidation of methane to synthesis gas over Pt nanoparticles supported on nanocrystalline CeO 2 catalyst journal January 2016
Systematic Structure–Property Relationship Studies in Palladium-Catalyzed Methane Complete Combustion journal October 2017
Novel embedded Pd@CeO 2 catalysts: a way to active and stable catalysts journal January 2010
Simple method to synthesize high surface area magnesium oxide and its use as a heterogeneous base catalyst journal November 2012
Efficient Removal of Organic Ligands from Supported Nanocrystals by Fast Thermal Annealing Enables Catalytic Studies on Well-Defined Active Phases journal May 2015
Irena : tool suite for modeling and analysis of small-angle scattering journal February 2009
QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials journal September 2009
Assessing the reliability of calculated catalytic ammonia synthesis rates journal July 2014
Inhomogeneous Electron Gas journal November 1964
Self-Consistent Equations Including Exchange and Correlation Effects journal November 1965
Pseudopotentials for high-throughput DFT calculations journal January 2014
Reversible work transition state theory: application to dissociative adsorption of hydrogen journal February 1995
Quantum and thermal effects in H 2 dissociative adsorption: Evaluation of free energy barriers in multidimensional quantum systems journal February 1994
A climbing image nudged elastic band method for finding saddle points and minimum energy paths journal December 2000
Improved tangent estimate in the nudged elastic band method for finding minimum energy paths and saddle points journal December 2000
CatMAP: A Software Package for Descriptor-Based Microkinetic Mapping of Catalytic Trends journal February 2015
A Theoretical Investigation into the Role of Surface Defects for Oxygen Evolution on RuO 2 journal August 2017
Assembling gas-phase reaction mechanisms for high temperature inorganic systems based on quantum chemistry calculations and reaction rate theories journal February 2005
Ceria-based fluorite-like oxide solid solutions as catalysts of methane selective oxidation into syngas by the lattice oxygen: synthesis, characterization and performance journal September 2004
Dynamics and Thermodynamics of Pd–PdO Phase Transitions: Effects of Pd Cluster Size and Kinetic Implications for Catalytic Methane Combustion journal January 2016
Metastable Pd ↔ PdO Structures During High Temperature Methane Oxidation journal March 2017
Fundamentals and Catalytic Applications of CeO 2 -Based Materials journal April 2016
The rate controlling step in the oxidative coupling of methane over a lithium-promoted magnesium oxide catalyst journal January 1988
Isotopic and kinetic assessment of the mechanism of reactions of CH4 with CO2 or H2O to form synthesis gas and carbon on nickel catalysts journal June 2004
Predicting CH 4 Dissociation Kinetics on Metals: Trends, Sticking Coefficients, H Tunneling, and Kinetic Isotope Effect journal October 2013
Steam Reforming and Graphite Formation on Ni Catalysts journal July 2002
A Theory of the Catalytic Surface journal May 1925
Identification of the "Active Sites" of a Surface-Catalyzed Reaction journal September 1996
Highly Site-Specific H 2 Adsorption on Vicinal Si ( 001 ) Surfaces journal December 1998
Role of Steps in N 2 Activation on Ru(0001) journal August 1999
Methane activation on Ni(111): Effects of poisons and step defects journal October 2005
Uniform Pt/Pd Bimetallic Nanocrystals Demonstrate Platinum Effect on Palladium Methane Combustion Activity and Stability journal May 2017
Oscillatory behaviour of catalytic properties, structure and temperature during the catalytic partial oxidation of methane on Pd/Al2O3 journal January 2010
Oscillatory Behavior during the Catalytic Partial Oxidation of Methane: Following Dynamic Structural Changes of Palladium Using the QEXAFS Technique journal December 2011
Consequences of Metal–Oxide Interconversion for C–H Bond Activation during CH 4 Reactions on Pd Catalysts journal October 2013
Elementary Steps, the Role of Chemisorbed Oxygen, and the Effects of Cluster Size in Catalytic CH 4 –O 2 Reactions on Palladium journal August 2011

Cited By (1)

Chromium-Ruthenium Oxides Supported on Gamma-Alumina as an Alternative Catalyst for Partial Combustion of Methane journal April 2019