CsOx Nanostructures on Au(111): Morphology- and Size-dependent Activity for the Water–Gas Shift Reaction

Shi, Rui; Ramírez, Pedro J.; Rosales, Rina; Mahapatra, Mausumi; Rui, Ning; Rodriguez, José A.

doi:10.1021/acs.jpcc.3c08190

This content will become publicly available on Wed Feb 19 00:00:00 EST 2025

Title: CsO_x Nanostructures on Au(111): Morphology- and Size-dependent Activity for the Water–Gas Shift Reaction

Abstract

Alkali oxides are typically used as promoters of heterogeneous catalysts for the water–gas shift (WGS; H₂O + CO → H₂ + CO₂) reaction. On Au(111), CsO_x exhibits diverse nanostructures at varying coverages, as revealed by scanning tunneling microscopy. Clusters of cesium oxide (Cs₂O₂) nucleate at elbow sites of the Au(111) herringbone when θ_Cs is less than 0.1 ML. Subsequently, these clusters transform into two-dimensional (2D) islands (Cs₂O, Cs₂O₂, CsO₂) as the cesium coverage increases (θ_Cs > 0.1 ML). Both types of CsO_x nanostructures enable the WGS process on Au(111). The highest activity was seen for the cesium oxide clusters which facilitated the partial dissociation of water and binding of CO. The CO_ads and OH_ads groups were not strongly bound and probably reacted to yield a short-lived HOCO intermediate that led to gaseous H₂ and CO₂. The 2D islands of CsO_x also enabled the WGS but their efficiency was reduced due to the formation of cesium hydroxide compounds (limiting mobility of OH groups) and the generation of CO₃ and C species (blocking of active centers). The fact that the performance of the CsO_x/Au(111) catalysts changed dramatically with variations in the chemical properties of the CsO_x nanostructures indicates that the alkali oxidemore »« less

Authors:

Shi, Rui ^[1]; Ramírez, Pedro J. ^[2]; Rosales, Rina ^[1]; Mahapatra, Mausumi ^[3];

^[4];

^[5]

Stony Brook Univ., NY (United States)
Universidad Central de Venezuela, Caracas (Venezuela); Zoneca-CENEX, R&D Laboratories, Monterrey (México)
Brookhaven National Laboratory (BNL), Upton, NY (United States); Loyola University Chicago, IL (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Stony Brook Univ., NY (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)

Publication Date:: Mon Feb 19 00:00:00 EST 2024

Research Org.:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

OSTI Identifier:: 2315623

Report Number(s):: BNL-225343-2024-JAAM
Journal ID: ISSN 1932-7447

Grant/Contract Number:: SC0012704

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Physical Chemistry. C

Additional Journal Information:: Journal Volume: 128; Journal Issue: 8; Journal ID: ISSN 1932-7447

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; Water-gas Shift; Hydrogen production; Cesium oxide; Gold

Citation Formats


                    Shi, Rui, Ramírez, Pedro J., Rosales, Rina, Mahapatra, Mausumi, Rui, Ning, and Rodriguez, José A. CsOx Nanostructures on Au(111): Morphology- and Size-dependent Activity for the Water–Gas Shift Reaction.  United States: N. p., 2024. 
Web.  doi:10.1021/acs.jpcc.3c08190.

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                    Shi, Rui, Ramírez, Pedro J., Rosales, Rina, Mahapatra, Mausumi, Rui, Ning, & Rodriguez, José A. CsOx Nanostructures on Au(111): Morphology- and Size-dependent Activity for the Water–Gas Shift Reaction.  United States.  https://doi.org/10.1021/acs.jpcc.3c08190

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                    Shi, Rui, Ramírez, Pedro J., Rosales, Rina, Mahapatra, Mausumi, Rui, Ning, and Rodriguez, José A. Mon .  
"CsOx Nanostructures on Au(111): Morphology- and Size-dependent Activity for the Water–Gas Shift Reaction".  United States.  https://doi.org/10.1021/acs.jpcc.3c08190.

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@article{osti_2315623,

  title        = {CsOx Nanostructures on Au(111): Morphology- and Size-dependent Activity for the Water–Gas Shift Reaction},

  author       = {Shi, Rui and Ramírez, Pedro J. and Rosales, Rina and Mahapatra, Mausumi and Rui, Ning and Rodriguez, José A.},

  abstractNote = {Alkali oxides are typically used as promoters of heterogeneous catalysts for the water–gas shift (WGS; H2O + CO → H2 + CO2) reaction. On Au(111), CsOx exhibits diverse nanostructures at varying coverages, as revealed by scanning tunneling microscopy. Clusters of cesium oxide (Cs2O2) nucleate at elbow sites of the Au(111) herringbone when θCs is less than 0.1 ML. Subsequently, these clusters transform into two-dimensional (2D) islands (Cs2O, Cs2O2, CsO2) as the cesium coverage increases (θCs > 0.1 ML). Both types of CsOx nanostructures enable the WGS process on Au(111). The highest activity was seen for the cesium oxide clusters which facilitated the partial dissociation of water and binding of CO. The COads and OHads groups were not strongly bound and probably reacted to yield a short-lived HOCO intermediate that led to gaseous H2 and CO2. The 2D islands of CsOx also enabled the WGS but their efficiency was reduced due to the formation of cesium hydroxide compounds (limiting mobility of OH groups) and the generation of CO3 and C species (blocking of active centers). The fact that the performance of the CsOx/Au(111) catalysts changed dramatically with variations in the chemical properties of the CsOx nanostructures indicates that the alkali oxide was an integral part of the active phase, playing a central role in the activation and conversion of the reactants. To attach the label of “promoter” to CsOx is a simplification that does not help in the design and optimization of catalysts for C1 chemistry. In conclusion, to achieve a rational design, one must consider the structural and chemical properties of the alkali oxide.},

  doi          = {10.1021/acs.jpcc.3c08190},

  journal      = {Journal of Physical Chemistry. C},

  number       = 8,

  volume       = 128,

  place        = {United States},

  year         = {Mon Feb 19 00:00:00 EST 2024},

  month        = {Mon Feb 19 00:00:00 EST 2024}

}

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Title: CsOx Nanostructures on Au(111): Morphology- and Size-dependent Activity for the Water–Gas Shift Reaction

Abstract

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A review of recent advances in water-gas shift catalysis for hydrogen production
journal, August 2020

Water Gas Shift Reaction on Cu and Au Nanoparticles Supported on CeO2(111) and ZnO(000): Intrinsic Activity and Importance of Support Interactions
journal, February 2007

Alkali-promoted alumina catalysts *1II. Water-gas shift reaction
journal, August 1982

Adsorption of oxygen on Au(111) by exposure to ozone
journal, August 1998

Low temperature CO oxidation on Au(111) and the role of adsorbed water
journal, June 2007

Cluster and periodic ab-initio calculations on K/TiO2(110)
journal, November 1998

Adsorption of carbon monoxide carbon dioxide on clean and cesium-covered copper(110)
journal, June 1989

In Situ and Theoretical Studies for the Dissociation of Water on an Active Ni/CeO ₂ Catalyst: Importance of Strong Metal-Support Interactions for the Cleavage of O-H Bonds
journal, February 2015

Water Activated by Atomic Oxygen on Au(111) to Oxidize CO at Low Temperatures
journal, May 2006

Empirical atomic sensitivity factors for quantitative analysis by electron spectroscopy for chemical analysis
journal, October 1981

Kinetics of low-temperature CO oxidation on Au(111)
journal, June 2016

Promotion of the water gas shift reaction by cesium surface doping of the model binary copper/zinc oxide catalyst
journal, February 1986