Oxidation at the sub-nanoscale: oxygen adsorption on graphene-supported size-selected Ag clusters

被引：8

作者：

Loi, Federico ^{[1
]}

Pozzo, Monica ^{[2
]}

Sbuelz, Luca ^{[1
]}

Bignardi, Luca ^{[1
]}

Lacovig, Paolo ^{[3
]}

Tosi, Ezequiel ^{[3
]}

Lizzit, Silvano ^{[3
]}

Kartouzian, Aras ^{[4
,5
]}

Heiz, Ueli ^{[4
,5
]}

Alfe, Dario ^{[2
,6
]}

Baraldi, Alessandro ^{[1
,3
]}

机构：

[1] Univ Trieste, Dept Phys, Via Valerio 2, I-34127 Trieste, Italy

[2] UCL, London Ctr Nanotechnol, Dept Earth Sci, Gower St, London WC1E 6BT, England

[3] Elettra Sincrotrone Trieste, AREA Sci Pk, I-34149 Trieste, Italy

[4] Tech Univ Munich, Chem Dept, Chair Phys Chem, Lichtenbergstr 4, D-85748 Garching, Germany

[5] Tech Univ Munich, Catalysis Res Ctr, Lichtenbergstr 4, D-85748 Garching, Germany

[6] Univ Napoli Federico II, Dipartimento Fis Ettore Pancini, I-80126 Naples, Italy

来源：

JOURNAL OF MATERIALS CHEMISTRY A | 2022年 / 10卷 / 27期

基金：

英国自然环境研究理事会;

关键词：

X-RAY PHOTOELECTRON; ELECTRONIC-PROPERTIES; SUBSURFACE OXYGEN; CRYSTAL-STRUCTURE; TIGHT-BINDING; CO OXIDATION; SILVER; NANOCLUSTERS; PHOTOEMISSION; GROWTH;

D O I：

10.1039/d2ta02539f

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

The evolution of the aggregation of condensed matter from single atoms to three-dimensional structures represents an important topic in nanoscience, since it contains essential information to achieve tailormade growth of nanostructured materials. Such an issue is particularly important in the case of the formation of nano-oxides, which have strong potentialities in heterogeneous catalysis reactions. Herein, we show that a Low-nucLearity graphene supported Ag duster (formed by 11 atoms) shows a local AgO4 configuration, spatial charge distribution and two oxidation states that are similar to those of buLk AgO. This result indicates that buLk oxide conformations can start to develop already for extremely small atomic aggregates (<1 nm), differently from metallic dusters. This local conformation shows the Lowest oxygen vacancy formation energy, which affords high efficiency in the ethylene epoxidation reaction with Ag and strongly supports the possibility of incorporating sub-nanometric dusters in important catalytic reactions.

引用

页码：14594 / 14603

页数：10

共 93 条

[1] Pristine and oxidised Ag-nanoparticles on free-standing graphene as explored by X-ray photoelectron and Auger spectroscopy [J].

Al-Hada, M. ;

Gregoratti, L. ;

Amati, M. ;

Neeb, M. .

SURFACE SCIENCE, 2020, 693

[2] Nanoparticle formation of deposited Agn-clusters on free-standing graphene [J].

Al-Hada, M. ;

Peters, S. ;

Gregoratti, L. ;

Amati, M. ;

Sezen, H. ;

Parisse, P. ;

Selve, S. ;

Niermann, T. ;

Berger, D. ;

Neeb, M. ;

Eberhardt, W. .

SURFACE SCIENCE, 2017, 665 :108-113

[3] Fine tuning of graphene-metal adhesion by surface alloying [J].

Alfe, D. ;

Pozzo, M. ;

Miniussi, E. ;

Guenther, S. ;

Lacovig, P. ;

Lizzit, S. ;

Larciprete, R. ;

Burgos, B. Santos ;

Mentes, T. O. ;

Locatelli, A. ;

Baraldi, A. .

SCIENTIFIC REPORTS, 2013, 3

[4] Electronic structures of silver oxides [J].

Allen, Jeremy P. ;

Scanlon, David O. ;

Watson, Graeme W. .

PHYSICAL REVIEW B, 2011, 84 (11)

[5] Electronic structure of mixed-valence silver oxide AgO from hybrid density-functional theory [J].

Allen, Jeremy P. ;

Scanlon, David O. ;

Watson, Graeme W. .

PHYSICAL REVIEW B, 2010, 81 (16)

[6] Structural properties of nanoclusters: Energetic, thermodynamic, and kinetic effects [J].

Baletto, F ;

Ferrando, R .

REVIEWS OF MODERN PHYSICS, 2005, 77 (01) :371-423

[7] Nanoclusters deposited on surfaces [J].

Binns, C .

SURFACE SCIENCE REPORTS, 2001, 44 (1-2) :1-49

[8] PROJECTOR AUGMENTED-WAVE METHOD [J].

BLOCHL, PE .

PHYSICAL REVIEW B, 1994, 50 (24) :17953-17979

[9] Formation of monodisperse (WO3)3 clusters on TiO2(110) [J].

Bondarchuk, Oleksandr ;

Huang, Xin ;

Kim, Jooho ;

Kay, Bruce D. ;

Wang, Lai-Sheng ;

White, J. M. ;

Dohnalek, Zdenek .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2006, 45 (29) :4786-4789

[10] Atomic oxygen species on silver:: Photoelectron spectroscopy and x-ray absorption studies -: art. no. 235422 [J].

Bukhtiyarov, VI ;

Hävecker, M ;

Kaichev, VV ;

Knop-Gericke, A ;

Mayer, RW ;

Schlögl, R .

PHYSICAL REVIEW B, 2003, 67 (23) :2354221-23542212

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