2022
DOI: 10.1039/d1cp05677h
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Exploring the materials space in the smallest particle size range: from heterogeneous catalysis to electrocatalysis and photocatalysis

Abstract: Ultrasmall clusters of subnanometer size can possess unique and even unexpected physical and chemical propensities which make them interesting in various fields of basic science and for potential applications, such...

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Cited by 22 publications
(9 citation statements)
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“…In the last few decades we have witnessed tremendous progress in synthetic methods designed for the exquisite control over the size, shape, structure, and elemental composition of nanoscale catalysts . The quest for developing effective size and shape control strategies resulted in a wide range of unique one-, two-, and three-dimensional architectures, and the list of well-defined structures in the size range exceeding 1 nm is rapidly growing. The situation is less optimistic toward the subnanometer structures, where inherently heterogeneous isomers of size-selective clusters coexist in samples prepared by even the most accurate deposition methods . Supported nanometer-scale catalysts have a relatively high degree of bonding disorder, hence embedding strong heterogeneities .…”
Section: Introductionmentioning
confidence: 99%
“…In the last few decades we have witnessed tremendous progress in synthetic methods designed for the exquisite control over the size, shape, structure, and elemental composition of nanoscale catalysts . The quest for developing effective size and shape control strategies resulted in a wide range of unique one-, two-, and three-dimensional architectures, and the list of well-defined structures in the size range exceeding 1 nm is rapidly growing. The situation is less optimistic toward the subnanometer structures, where inherently heterogeneous isomers of size-selective clusters coexist in samples prepared by even the most accurate deposition methods . Supported nanometer-scale catalysts have a relatively high degree of bonding disorder, hence embedding strong heterogeneities .…”
Section: Introductionmentioning
confidence: 99%
“…26 Supported single atoms and subnanometer clusters of transition metals have proven to be promising catalysts in various reactions, including CO 2 hydrogenation, the Fischer-Tropsch reaction and the hydrogenation/dehydrogenation of hydrocarbons. [27][28][29][30][31][32][33][34] Thanks to the small size of the cluster, usually less than 50 atoms, quantum effects occur. 35 By comparison with the bulk material, smaller clusters tend to have discrete electron levels and, as a result, they lose their metallic character and resemble isolated molecules, with their electronic (as well as geometric) structure altered by adding a single atom of the same or a different metal.…”
Section: Introductionmentioning
confidence: 99%
“…1,3,5−9 Cluster-support interactions also strongly influence cluster mobility, which, in turn, determines preferred binding sites, e.g., steps or defects, and their ability to aggregate into larger 2D islands or 3D nanoparticles under reaction conditions. 10−12 Although significant progress has been made in the preparation of atomically precise supported clusters and single atoms, 2,4,13,14 aggregation processes at elevated temperatures and/or pressures can lead to loss of active sites and a decrease in catalytic activity. 12,15 Hence, the use of ultrasmall clusters for catalysis applications requires detailed knowledge of the structure and thermal stability of the clusters on the surface since aggregation can largely negate any advantages of controlled size.…”
Section: Introductionmentioning
confidence: 99%
“…The use of ultrasmall supported clusters, down to single atoms, have gained considerable attention in heterogeneous catalysis as a way of optimizing activity and selectivity of catalytic reactions. In general, the atomic structure and electronic properties of ultrasmall clusters are highly sensitive to changes of 1–2 atoms and are not representative of the bulk material. In this nonscalable size regime, increased sensitivity to cluster structure and support effects can change the reaction energetics and thus alter the mechanism, activity, and selectivity. ,, Cluster-support interactions also strongly influence cluster mobility, which, in turn, determines preferred binding sites, e.g., steps or defects, and their ability to aggregate into larger 2D islands or 3D nanoparticles under reaction conditions. Although significant progress has been made in the preparation of atomically precise supported clusters and single atoms, ,,, aggregation processes at elevated temperatures and/or pressures can lead to loss of active sites and a decrease in catalytic activity. , Hence, the use of ultrasmall clusters for catalysis applications requires detailed knowledge of the structure and thermal stability of the clusters on the surface since aggregation can largely negate any advantages of controlled size.…”
Section: Introductionmentioning
confidence: 99%