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Title: In-situ and theoretical studies for the dissociation of water on an active Ni/CeO₂ catalyst: Importance of strong metal-support interactions for the cleavage of O-H bonds

Journal Article · · Angewandte Chemie (International Edition)
 [1];  [2];  [1];  [2];  [3];  [4];  [5];  [6];  [3];  [7]
  1. Inst. de Catalisis y Petroleoquimica, CSIC, Madrid (Spain); CIC Energigune, Minana, Alava (Spain)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States); Stony Brook Univ., NY (United States)
  3. Charles Univ., Praha (Czech Republic)
  4. Univ. Central de Venezuela, Caracas (Venezuela)
  5. Brookhaven National Lab. (BNL), Upton, NY (United States)
  6. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  7. Inst. de Catalisis y Petroleoquimica, CSIC, Madrid (Spain)
+ Show Author Affiliations

Water dissociation is crucial in many catalytic reactions on oxide-supported transition-metal catalysts. Here, supported by experimental and density-functional theory results, we elucidate the effect of the support on O-H bond cleavage activity for nickel/ceria systems. Ambient-pressure O1s photoemission spectra at low Ni loadings on CeO₂(111) reveal a substantially larger amount of OH groups as compared to the bare support. Our computed activation energy barriers for water dissociation show an enhanced reactivity of Ni adatoms on CeO₂(111) compared with pyramidal Ni₄ particles with one Ni atom not in contact with the support, and extended Ni(111) surfaces. At the origin of this support effect is the ability of ceria to stabilize oxidized Ni²⁺ species by accommodating electrons in localized f-states. The fast dissociation of water on Ni/CeO₂ has a dramatic effect on the activity and stability of this system as a catalyst for the water-gas shift and ethanol steam reforming reactions.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC00112704
OSTI ID:
1183857
Report Number(s):
BNL-107982-2015-JA; R&D Project: CO-040; KC0302010
Journal Information:
Angewandte Chemie (International Edition), Vol. 54, Issue 13; ISSN 1433-7851
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 181 works
Citation information provided by
Web of Science

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Cited By (22)

Anode-Engineered Protonic Ceramic Fuel Cell with Excellent Performance and Fuel Compatibility journal August 2016
Well‐Dispersed Nickel‐ and Zinc‐Tailored Electronic Structure of a Transition Metal Oxide for Highly Active Alkaline Hydrogen Evolution Reaction journal February 2019
Photochemical Synthesis of Radiate Titanium Oxide Microrods Arrays Supporting Platinum Nanoparticles for Photoassisted Electrooxidation of Methanol journal August 2018
How Do Structurally Distinct Au/α‐Fe 2 O 3 Interfaces Determine Surface OH/H 2 O reactivity, Intermediate Evolution, and Product Formation in Low‐temperature Water‐gas Shift Reaction? journal May 2019
Advantageous Interfacial Effects of AgPd/g‐C 3 N 4 for Photocatalytic Hydrogen Evolution: Electronic Structure and H 2 O Dissociation journal March 2019
Integrating Catalysis of Methane Decomposition and Electrocatalytic Hydrogen Evolution with Ni/CeO 2 for Improved Hydrogen Production Efficiency journal February 2019
Highly efficient steam reforming of ethanol (SRE) over CeO x grown on the nano Ni x Mg y O matrix: H 2 production under a high GHSV condition journal March 2019
Activating cobalt(II) oxide nanorods for efficient electrocatalysis by strain engineering journal November 2017
Ceria-based model catalysts: fundamental studies on the importance of the metal–ceria interface in CO oxidation, the water–gas shift, CO 2 hydrogenation, and methane and alcohol reforming journal January 2017
Ru/ceria-catalyzed direct formylation of amines and CO to produce formamides journal January 2017
The adsorption of Cu on the CeO 2 (110) surface journal January 2017
DFT insights into oxygen vacancy formation and CH 4 activation over CeO 2 surfaces modified by transition metals (Fe, Co and Ni) journal January 2018
CO 2 and water activation on ceria nanocluster modified TiO 2 rutile (110) journal January 2018
Alkaline earth metal oxide nanocluster modification of rutile TiO 2 (110) promotes water activation and CO 2 chemisorption journal January 2018
Insights into interface engineering in steam reforming reactions for hydrogen production journal January 2019
An organic ligand promoting the electrocatalytic activity of cobalt oxide for the hydrogen evolution reaction journal January 2019
Exotic electronic structures of Sm x Ce 3−x O y (x = 0-3; y = 2-4) clusters and the effect of high neutral density of low-lying states on photodetachment transition intensities journal August 2018
In situ growing of CoO nanoparticles on g-C 3 N 4 composites with highly improved photocatalytic activity for hydrogen evolution journal July 2019
Hydrogen Production by Ethanol Steam Reforming (ESR) over CeO2 Supported Transition Metal (Fe, Co, Ni, Cu) Catalysts: Insight into the Structure-Activity Relationship journal March 2016
CO2 and Water Activation on Ceria Nanocluster Modified TiO2 Rutile (110) preprint February 2018
Alkaline Earth Metal Oxide Nanocluster Modification of Rutile TiO2 (110) Promotes Water Activation and CO2 Chemisorption preprint February 2018
CO2 and Water Activation on Ceria Nanocluster Modified TiO2 Rutile (110) preprint February 2018

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