Tip-activated single-atom catalysis: CO oxidation on Au adatom on oxidized rutile TiO2 surface

Yuuki Adachi; Ján Brndiar; Martin Konôpka; Robert Turanský; Qiang Zhu; Huan Fei Wen; Yasuhiro Sugawara; Lev Kantorovich; Ivan Štich; Yan Jun Li

doi:10.1126/sciadv.adi4799

Tip-activated single-atom catalysis: CO oxidation on Au adatom on oxidized rutile TiO2 surface

Yuuki Adachi, Ján Brndiar, Martin Konôpka, Robert Turanský, Qiang Zhu, Huan Fei Wen, Yasuhiro Sugawara, Lev Kantorovich, Ivan Štich, Yan Jun Li^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

2 Citations (Scopus)

Abstract

Single-atom catalysis of carbon monoxide oxidation on metal-oxide surfaces is crucial for greenhouse recycling, automotive catalysis, and beyond, but reports of the atomic-scale mechanism are still scarce. Here, using scanning probe microscopy, we show that charging single gold atoms on oxidized rutile titanium dioxide surface, both positively and negatively, considerably promotes adsorption of carbon monoxide. No carbon monoxide adsorption is observed on neutral gold atoms. Two different carbon monoxide adsorption geometries on gold atoms are identified. We demonstrate full control over the redox state of adsorbed gold single atoms, carbon monoxide adsorption geometry, and carbon monoxide adsorption/desorption by the atomic force microscopy tip. On charged gold atoms, we activate Eley-Rideal oxidation reaction between carbon monoxide and a neighboring oxygen adatom by the tip. Our results provide unprecedented insights into carbon monoxide adsorption and suggest that the gold dual activity for carbon monoxide oxidation after electron or hole attachment is also the key ingredient in photocatalysis under realistic conditions.

Original language	English
Article number	eadi4799
Journal	Science Advances
Volume	9
Issue number	39
DOIs	https://doi.org/10.1126/sciadv.adi4799
Publication status	Published - 2023

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@article{214bfffcdfe84d63b043cbdde310f5a4,

title = "Tip-activated single-atom catalysis: CO oxidation on Au adatom on oxidized rutile TiO2 surface",

abstract = "Single-atom catalysis of carbon monoxide oxidation on metal-oxide surfaces is crucial for greenhouse recycling, automotive catalysis, and beyond, but reports of the atomic-scale mechanism are still scarce. Here, using scanning probe microscopy, we show that charging single gold atoms on oxidized rutile titanium dioxide surface, both positively and negatively, considerably promotes adsorption of carbon monoxide. No carbon monoxide adsorption is observed on neutral gold atoms. Two different carbon monoxide adsorption geometries on gold atoms are identified. We demonstrate full control over the redox state of adsorbed gold single atoms, carbon monoxide adsorption geometry, and carbon monoxide adsorption/desorption by the atomic force microscopy tip. On charged gold atoms, we activate Eley-Rideal oxidation reaction between carbon monoxide and a neighboring oxygen adatom by the tip. Our results provide unprecedented insights into carbon monoxide adsorption and suggest that the gold dual activity for carbon monoxide oxidation after electron or hole attachment is also the key ingredient in photocatalysis under realistic conditions.",

author = "Yuuki Adachi and J{\'a}n Brndiar and Martin Kon{\^o}pka and Robert Turansk{\'y} and Qiang Zhu and Wen, {Huan Fei} and Yasuhiro Sugawara and Lev Kantorovich and Ivan {\v S}tich and {Jun Li}, Yan",

note = "Funding Information: Acknowledgments Funding:ThisworkwassupportedbyaGrant-in-AidforScientificResearchfromJapanSociety forthePromotionofScience(JSPS)fromtheMinistryofEducation,Culture,Sports,Science,and T echnology ofJapan(JP16H06327,JP16H06504,JP17H01061,andJP22H00282).Thisworkwas alsosupportedbytheInternationalJointResearchPromotionProgramofOsakaUniversity (16H06327,J171013014,J171013007,J181013004,J181013006,Ja1999001,Ja19990011,and A21J103560).ThisprojectwassupportedbytheNationalNaturalScienceFoundationofChina (NSFC)JSPS-NSFC(J191053055).W eacknowledgethesupportbyAPVV-18-0211,APVV-21-0272,VEGA-2/0070/21,andVEGA-2/0125/20projectsandH2020TREXGAno.952165project. W ealsoacknowledgeCenterforComputationalMaterialsScience,InstituteforMaterials Research,TohokuUniversityfortheuseofMASAMUNE-IMRsupercomputer.Author contributions:Conceptualization:Y .A., Y .J.L., Y .S., L.K.,andI.{\v S}.Methodology:Y .A., J.B.,M.K.,R.T ., Q.Z.,H.F .W ., Y .S., L.K.,I.{\v S}.,andY .J.L. Investigation:Y .A., J.B.,M.K.,R.T ., Q.Z.,H.F .W ., Y .S., L.K.,I.{\v S}.,and Y .J.L. Supervision:Y .J.L., Y .S., L.K.,andI.{\v S}.Writing—originaldraft:Y .A., Y .J.L., L.K.,andI.{\v S}.Writing —reviewand editing: Y .A., Y .J.L., L.K., and I.{\v S}. Competing interests: The authors declare that theyhav enocompetinginterests.Dataandmaterialsavailability:Alldataneededto evaluatetheconclusionsinthepaperarepresentinthepaperand/ortheSupplementary Materials. Publisher Copyright: {\textcopyright} 2023 The Authors.",

year = "2023",

doi = "10.1126/sciadv.adi4799",

language = "English",

volume = "9",

journal = "Science Advances",

issn = "2375-2548",

publisher = "American Association for the Advancement of Science",

number = "39",

}

TY - JOUR

T1 - Tip-activated single-atom catalysis

T2 - CO oxidation on Au adatom on oxidized rutile TiO2 surface

AU - Adachi, Yuuki

AU - Brndiar, Ján

AU - Konôpka, Martin

AU - Turanský, Robert

AU - Zhu, Qiang

AU - Wen, Huan Fei

AU - Sugawara, Yasuhiro

AU - Kantorovich, Lev

AU - Štich, Ivan

AU - Jun Li, Yan

N1 - Funding Information: Acknowledgments Funding:ThisworkwassupportedbyaGrant-in-AidforScientificResearchfromJapanSociety forthePromotionofScience(JSPS)fromtheMinistryofEducation,Culture,Sports,Science,and T echnology ofJapan(JP16H06327,JP16H06504,JP17H01061,andJP22H00282).Thisworkwas alsosupportedbytheInternationalJointResearchPromotionProgramofOsakaUniversity (16H06327,J171013014,J171013007,J181013004,J181013006,Ja1999001,Ja19990011,and A21J103560).ThisprojectwassupportedbytheNationalNaturalScienceFoundationofChina (NSFC)JSPS-NSFC(J191053055).W eacknowledgethesupportbyAPVV-18-0211,APVV-21-0272,VEGA-2/0070/21,andVEGA-2/0125/20projectsandH2020TREXGAno.952165project. W ealsoacknowledgeCenterforComputationalMaterialsScience,InstituteforMaterials Research,TohokuUniversityfortheuseofMASAMUNE-IMRsupercomputer.Author contributions:Conceptualization:Y .A., Y .J.L., Y .S., L.K.,andI.Š.Methodology:Y .A., J.B.,M.K.,R.T ., Q.Z.,H.F .W ., Y .S., L.K.,I.Š.,andY .J.L. Investigation:Y .A., J.B.,M.K.,R.T ., Q.Z.,H.F .W ., Y .S., L.K.,I.Š.,and Y .J.L. Supervision:Y .J.L., Y .S., L.K.,andI.Š.Writing—originaldraft:Y .A., Y .J.L., L.K.,andI.Š.Writing —reviewand editing: Y .A., Y .J.L., L.K., and I.Š. Competing interests: The authors declare that theyhav enocompetinginterests.Dataandmaterialsavailability:Alldataneededto evaluatetheconclusionsinthepaperarepresentinthepaperand/ortheSupplementary Materials. Publisher Copyright: © 2023 The Authors.

PY - 2023

Y1 - 2023

N2 - Single-atom catalysis of carbon monoxide oxidation on metal-oxide surfaces is crucial for greenhouse recycling, automotive catalysis, and beyond, but reports of the atomic-scale mechanism are still scarce. Here, using scanning probe microscopy, we show that charging single gold atoms on oxidized rutile titanium dioxide surface, both positively and negatively, considerably promotes adsorption of carbon monoxide. No carbon monoxide adsorption is observed on neutral gold atoms. Two different carbon monoxide adsorption geometries on gold atoms are identified. We demonstrate full control over the redox state of adsorbed gold single atoms, carbon monoxide adsorption geometry, and carbon monoxide adsorption/desorption by the atomic force microscopy tip. On charged gold atoms, we activate Eley-Rideal oxidation reaction between carbon monoxide and a neighboring oxygen adatom by the tip. Our results provide unprecedented insights into carbon monoxide adsorption and suggest that the gold dual activity for carbon monoxide oxidation after electron or hole attachment is also the key ingredient in photocatalysis under realistic conditions.

AB - Single-atom catalysis of carbon monoxide oxidation on metal-oxide surfaces is crucial for greenhouse recycling, automotive catalysis, and beyond, but reports of the atomic-scale mechanism are still scarce. Here, using scanning probe microscopy, we show that charging single gold atoms on oxidized rutile titanium dioxide surface, both positively and negatively, considerably promotes adsorption of carbon monoxide. No carbon monoxide adsorption is observed on neutral gold atoms. Two different carbon monoxide adsorption geometries on gold atoms are identified. We demonstrate full control over the redox state of adsorbed gold single atoms, carbon monoxide adsorption geometry, and carbon monoxide adsorption/desorption by the atomic force microscopy tip. On charged gold atoms, we activate Eley-Rideal oxidation reaction between carbon monoxide and a neighboring oxygen adatom by the tip. Our results provide unprecedented insights into carbon monoxide adsorption and suggest that the gold dual activity for carbon monoxide oxidation after electron or hole attachment is also the key ingredient in photocatalysis under realistic conditions.

UR - http://www.scopus.com/inward/record.url?scp=85176002484&partnerID=8YFLogxK

U2 - 10.1126/sciadv.adi4799

DO - 10.1126/sciadv.adi4799

M3 - Article

AN - SCOPUS:85176002484

SN - 2375-2548

VL - 9

JO - Science Advances

JF - Science Advances

IS - 39

M1 - eadi4799

ER -

Tip-activated single-atom catalysis: CO oxidation on Au adatom on oxidized rutile TiO2 surface

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