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Peer-reviewedCC BYJournal of the American Chemical Society

Room-Temperature Adsorption on Magnetite Induces Spontaneous Fragmentation of Early Transition-Metal Size-Selected Nanoclusters.

  • Gabriele Coltrioli1
  • Deborah Perco1
  • Luca Sementa2
  • Marco Bianchi3
  • Andrea Berti1
  • Mikhail Bandurist1
  • Paolo Lacovig3
  • Silvano Lizzit3
  • Aras Kartouzian3
  • Ueli Heiz4
  • Alessandro Fortunelli5
  • Alessandro Baraldi1,3
5 affiliations
  1. 1Department of Physics, University of Trieste, Via Valerio 2, 34127Trieste, Italy.
  2. 2Istituto per i Processi Chimico-Fisici, Consiglio Nazionale delle Ricerche, Via Giovanni Moruzzi 1, Pisa56124, Italy.
  3. 3Elettra - Sincrotrone Trieste, S.S. 14 Km 163.5, AREA Science Park, 34149Basovizza-Trieste, Italy.
  4. 4Chemistry Department & Catalysis Research Center, Technical University of Munich, Lichtenbergstrasse 4, GarchingD-85748, Germany.
  5. 5Istituto di Chimica dei Composti Organometallici, Consiglio Nazionale delle Ricerche (CNR-ICCOM), Via Giovanni Moruzzi 1, 56124Pisa, Italy.
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Abstract

The stability of supported metal nanoclusters, namely, their ability to preserve structure, composition, and catalytic activity over time, is a fundamental prerequisite for catalyst durability, resistance to deactivation, and long-term performance under operating conditions. Despite their often-exceptional intrinsic activity, nanoclusters are particularly susceptible to structural evolution driven by strong metal-support interactions. Here, we demonstrate that size-selected early transition-metal nanoclusters (W, Mo, and Ta) soft-landed on reconstructed Fe3O4(001) undergo spontaneous breakdown already at room temperature, in the absence of thermal activation or reactive gas environments. Combining high-energy resolution photoelectron spectroscopy and scanning tunneling microscopy with density functional theory, we show that strong metal-oxygen bonding, together with reconstruction-induced surface defects of the oxide support, provides the driving force required to overcome metal-metal cohesion within the clusters, leading to their dissociation. Upon further oxidation, an enhanced degree of atomization is produced, particularly for larger clusters, yielding highly dispersed metal species. The propensity for fragmentation, i.e., the partial or total breaking of metal-metal bonds in the cluster, follows the trend Ta > W > Mo, which correlates closely with metal oxophilicity, adsorption energies, and intrinsic metal-metal bond strengths. These findings establish adsorption-induced fragmentation of metal nanoclusters as an intrinsic manifestation of metal-support interactions for early transition metals on reducible oxides. More broadly, they reveal a spontaneous room temperature pathway to cluster destabilization and identify an innovative strategy for the controlled generation of high densities of single metal atoms from well-defined nanocluster precursors.

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Cite

BibTeXRIS
BibTeX
@article{coltrioli2026roomtemperature,
  title = {{Room-Temperature Adsorption on Magnetite Induces Spontaneous Fragmentation of Early Transition-Metal Size-Selected Nanoclusters.}},
  author = {Gabriele Coltrioli and Deborah Perco and Luca Sementa and Marco Bianchi and Andrea Berti and Mikhail Bandurist and Paolo Lacovig and Silvano Lizzit and Aras Kartouzian and Ueli Heiz and Alessandro Fortunelli and Alessandro Baraldi},
  journal = {Journal of the American Chemical Society},
  year = {2026},
  month = sep,
  doi = {10.1021/jacs.6c15419},
  url = {https://europepmc.org/article/MED/42937882},
  note = {CC BY},
}
RIS
TY  - JOUR
TI  - Room-Temperature Adsorption on Magnetite Induces Spontaneous Fragmentation of Early Transition-Metal Size-Selected Nanoclusters.
AU  - Gabriele Coltrioli
AU  - Deborah Perco
AU  - Luca Sementa
AU  - Marco Bianchi
AU  - Andrea Berti
AU  - Mikhail Bandurist
AU  - Paolo Lacovig
AU  - Silvano Lizzit
AU  - Aras Kartouzian
AU  - Ueli Heiz
AU  - Alessandro Fortunelli
AU  - Alessandro Baraldi
PY  - 2026
DA  - 2026/09/01
JO  - Journal of the American Chemical Society
DO  - 10.1021/jacs.6c15419
UR  - https://europepmc.org/article/MED/42937882
AB  - The stability of supported metal nanoclusters, namely, their ability to preserve structure, composition, and catalytic activity over time, is a fundamental prerequisite for catalyst durability, resistance to deactivation, and long-term performance under operating conditions. Despite their often-exceptional intrinsic activity, nanoclusters are particularly susceptible to structural evolution driven by strong metal-support interactions. Here, we demonstrate that size-selected early transition-metal nanoclusters (W, Mo, and Ta) soft-landed on reconstructed Fe3O4(001) undergo spontaneous breakdown already at room temperature, in the absence of thermal activation or reactive gas environments. Combining high-energy resolution photoelectron spectroscopy and scanning tunneling microscopy with density functional theory, we show that strong metal-oxygen bonding, together with reconstruction-induced surface defects of the oxide support, provides the driving force required to overcome metal-metal cohesion within the clusters, leading to their dissociation. Upon further oxidation, an enhanced degree of atomization is produced, particularly for larger clusters, yielding highly dispersed metal species. The propensity for fragmentation, i.e., the partial or total breaking of metal-metal bonds in the cluster, follows the trend Ta > W > Mo, which correlates closely with metal oxophilicity, adsorption energies, and intrinsic metal-metal bond strengths. These findings establish adsorption-induced fragmentation of metal nanoclusters as an intrinsic manifestation of metal-support interactions for early transition metals on reducible oxides. More broadly, they reveal a spontaneous room temperature pathway to cluster destabilization and identify an innovative strategy for the controlled generation of high densities of single metal atoms from well-defined nanocluster precursors.
SN  - 0002-7863
SN  - 1520-5126
ER  -