Non defect-stabilized thermally stable single-atom catalyst

Abstract

Surface-supported isolated atoms in single-atom catalysts (SACs) are usually stabilized by diverse defects. The fabrication of high-metal-loading and thermally stable SACs remains a formidable challenge due to the difficulty of creating high densities of underpinning stable defects. Here we report that isolated Pt atoms can be stabilized through a strong covalent metal-support interaction (CMSI) that is not associated with support defects, yielding a high-loading and thermally stable SAC by trapping either the already deposited Pt atoms or the PtO2 units vaporized from nanoparticles during high-temperature calcination. Experimental and computational modeling studies reveal that iron oxide reducibility is crucial to anchor isolated Pt atoms. The resulting high concentrations of single atoms enable specific activities far exceeding those of conventional nanoparticle catalysts. This non defect-stabilization strategy can be extended to non-reducible supports by simply doping with iron oxide, thus paving a new way for constructing high-loading SACs for diverse industrially important catalytic reactions.

Dual‐function catalysis in propane dehydrogenation over Pt1–Ga2O3 catalyst: Insights from a microkinetic analysis

“…At the Pt–O′ site, the Pt 5 d and O′ 2 p orbitals are strongly hybridized in the region from −8 eV to the Fermi level (see Figure 1e), which may account for the high stability of Pt substitution in the Ga(o) vacancy 66 . The peaks of the Pt 5 d orbitals appear on both sides of the Fermi level, indicating both the occupied and unoccupied frontier 5 d orbitals of Pt can interact with adsorbed species.…”

Single vs double atom catalyst for N2 activation in nitrogen reduction reaction: A DFT perspective

“…The uniform dispersion of atomic catalyst with high density of active sites and stability is a major challenge in SAC research. The whole scientific research community have tried various kinds of methods both theoretically 10 and experimentally [11][12][13][14][15] to understand and solve this challenge.…”

Stable Discrete Pt1(0) in Crown Ether with Ultra‐High Hydrosilylation Activity

“…Single atoms may be stabilized on solid surface due to strong metal‐support interaction or ligand coordination . Supported on reducible metal oxides, single metal atoms have been found to be stable as oxidized ions, e. g. Pt(IV) . However, single atoms in reduced state tend to aggregate into nanoparticles in liquid media without strong ligand coordination .…”