Abstract
Single-atom metal catalysts offer a promising way to utilize precious noble metal elements more effectively, provided that they are catalytically active and sufficiently stable. Herein, we report a synthetic strategy for Pt single-atom catalysts with outstanding stability in several reactions under demanding conditions. The Pt atoms are firmly anchored in the internal surface of mesoporous Al2O3, likely stabilized by coordinatively unsaturated pentahedral Al3+ centres. The catalyst keeps its structural integrity and excellent performance for the selective hydrogenation of 1,3-butadiene after exposure to a reductive atmosphere at 200 °C for 24 h. Compared to commercial Pt nanoparticle catalyst on Al2O3 and control samples, this system exhibits significantly enhanced stability and performance for n-hexane hydro-reforming at 550 °C for 48 h, although agglomeration of Pt single-atoms into clusters is observed after reaction. In CO oxidation, the Pt single-atom identity was fully maintained after 60 cycles between 100 and 400 °C over a one-month period.
Highlights
Single-atom metal catalysts offer a promising way to utilize precious noble metal elements more effectively, provided that they are catalytically active and sufficiently stable
The reductive behaviour of Pt/m-Al2O3-O2 over H2 was determined from their temperature-programmed reduction (TPR) profiles (Supplementary Fig. 1)
Strong interactions between the metal atom and the support are conceived to be the key to preventing metal atom aggregation[6], while an overly strong interaction may lead to catalytically inactive species acting as spectators
Summary
Single-atom metal catalysts offer a promising way to utilize precious noble metal elements more effectively, provided that they are catalytically active and sufficiently stable. Despite the critical role of Pt in catalysis[2], it is rare, in short supply in recent years and has no adequate alternatives In this regard, single-atom catalysts (or atomically dispersed catalysts), in which all the metal atoms are exposed on the support available for catalytic reactions, could help to address the problem[3,4,5,6,7]. Many industrially important catalytic processes involving Pt catalysts, such as reforming of hydrocarbons in petroleum refineries, are operated at several hundred degrees under oxidative or reductive atmosphere[29,30] In this context, single-atom catalysts that are able to withstand harsh reaction conditions are highly desirable. The catalyst maintained the catalytic activity as well as structural integrity when scrutinized in a series of reactions under drastic conditions with long durations
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