skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Low-temperature conversion of methane to methanol on CeOx/Cu2O catalysts: Water controlled activation of the C–H Bond

Journal Article · · Journal of the American Chemical Society
DOI:https://doi.org/10.1021/jacs.6b08668· OSTI ID:1333200
 [1];  [2];  [3];  [3];  [3]
  1. Taiyuan Univ. of Technology, Shanxi (China)
  2. Univ. Central de Venezuela (Venezuela)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States)
+ Show Author Affiliations

We are able to activate an inverse CeO2/Cu2O/Cu(111) catalyst with methane at room temperature producing C, CHx fragments and COx species and on the oxide surface. By adding water to the system leads to a drastic change in the selectivity of methane activation yielding only adsorbed CHx fragments. At a temperature of 450 K, in the presence of water, a CH4 → CH3OH catalytic transformation occurs with a high selectivity. OH groups formed by the dissociation of water saturate the catalyst surface, removing sites that could decompose CHx fragments, and generating centers on which methane can directly interact to yield methanol.

Research Organization:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC00112704
OSTI ID:
1333200
Alternate ID(s):
OSTI ID: 1345747
Report Number(s):
BNL-113196-2016-JA; BNL-113591-2017-JA; R&D Project: CO040; KC0302010
Journal Information:
Journal of the American Chemical Society, Vol. 138, Issue 42; ISSN 0002-7863
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 92 works
Citation information provided by
Web of Science

References (21)

Single Step Oxidation of Methane to Methanol–Towards Better Understanding journal January 2013
Single-site trinuclear copper oxygen clusters in mordenite for selective conversion of methane to methanol journal June 2015
Stability and reactivity of copper oxo-clusters in ZSM-5 zeolite for selective methane oxidation to methanol journal June 2016
Controlled Oxidation of Hydrocarbons by the Membrane-Bound Methane Monooxygenase: The Case for a Tricopper Cluster journal August 2008
Efficient Oxidation of Methane to Methanol by Dioxygen Mediated by Tricopper Clusters journal February 2013
Room temperature activation of methane over Zn modified H-ZSM-5 zeolites: Insight from solid-state NMR and theoretical calculations journal January 2012
Strategies for the Direct Catalytic Valorization of Methane Using Heterogeneous Catalysis: Challenges and Opportunities journal April 2016
Consequences of Metal–Oxide Interconversion for C–H Bond Activation during CH 4 Reactions on Pd Catalysts journal October 2013
Catalytic Oxidation of Methane into Methanol over Copper-Exchanged Zeolites with Oxygen at Low Temperature journal April 2016
Isothermal Cyclic Conversion of Methane into Methanol over Copper-Exchanged Zeolite at Low Temperature journal March 2016
CO Oxidation on Inverse CeO x /Cu(111) Catalysts: High Catalytic Activity and Ceria-Promoted Dissociation of O 2 journal March 2011
Nanopattering in CeO x /Cu(111): A New Type of Surface Reconstruction and Enhancement of Catalytic Activity journal March 2012
CeO 2 ↔ CuO x Interactions and the Controlled Assembly of CeO 2 (111) and CeO 2 (100) Nanoparticles on an Oxidized Cu(111) Substrate journal October 2011
Water-Gas Shift Reaction on a Highly Active Inverse CeO x /Cu(111) Catalyst: Unique Role of Ceria Nanoparticles journal October 2009
Inverse CeO 2 /CuO Catalyst As an Alternative to Classical Direct Configurations for Preferential Oxidation of CO in Hydrogen-Rich Stream journal January 2010
Dry Reforming of Methane on a Highly-Active Ni-CeO 2 Catalyst: Effects of Metal-Support Interactions on C−H Bond Breaking journal May 2016
Mechanistic Insights of Ethanol Steam Reforming over Ni–CeO x (111): The Importance of Hydroxyl Groups for Suppressing Coke Formation journal July 2015
Potassium-Induced Effect on the Structure and Chemical Activity of the Cu x O/Cu(1 1 1) ( x ≤ 2) Surface: A Combined Scanning Tunneling Microscopy and Density Functional Theory Study journal November 2015
Mechanistic Study of CO Titration on Cu x O/Cu(1 1 1) ( x ≤2) Surfaces journal June 2014
Nonoxidative Activation of Methane journal January 2003
Aqueous-Phase Methane Oxidation over Fe-MFI Zeolites; Promotion through Isomorphous Framework Substitution journal July 2013

Cited By (9)

The Direct Catalytic Oxidation of Methane to Methanol-A Critical Assessment journal November 2017
Hydroxylation of ZnO/Cu(1 1 1) inverse catalysts under ambient water vapor and the water–gas shift reaction journal August 2019
Thermal reduction of ceria nanostructures on rhodium(111) and re-oxidation by CO 2 journal January 2018
Partial oxidation of methane to methanol by isolated Pt catalyst supported on a CeO 2 nanoparticle journal February 2020
Mo 6 S 8 -based single-metal-atom catalysts for direct methane to methanol conversion journal July 2019
Misconceptions and challenges in methane-to-methanol over transition-metal-exchanged zeolites journal May 2019
Experimental and theoretical study of multinuclear indium–oxo clusters in CHA zeolite for CH 4 activation at room temperature journal January 2019
DME synthesis from methanol over hydrated γ-Al 2 O 3 (110) surface in slurry bed using continuum and atomistic models journal April 2017
Quasicatalytic and catalytic selective oxidation of methane to methanol over solid materials: a review on the roles of water journal October 2019

Similar Records

Tuning Selectivity in the Direct Conversion of Methane to Methanol: Bimetallic Synergistic Effects on the Cleavage of C–H and O–H Bonds over NiCu/CeO 2 Catalysts
Journal Article · Tue Jun 14 00:00:00 EDT 2022 · Journal of Physical Chemistry Letters · OSTI ID:1333200
+1 more
Selective Methane Oxidation to Methanol on ZnO/Cu2O/Cu(111) Catalysts: Multiple Site-Dependent Behaviors
Journal Article · Thu Nov 04 00:00:00 EDT 2021 · Journal of the American Chemical Society · OSTI ID:1333200
+7 more
Hydrogenation of CO2 to methanol on CeOx/Cu(111) and ZnO/Cu(111) catalysts: Role of the metal-oxide interface and importance of Ce3+ sites
Journal Article · Wed Jan 06 00:00:00 EST 2016 · Journal of Physical Chemistry. C · OSTI ID:1333200
+8 more

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY