Flash-Thermal Shock Synthesis of Single Atoms in Ambient Air.

Single-atom catalysts feature interesting catalytic activity toward applications that rely on surface reactions such as electrochemical energy storage, catalysis, and gas sensors. However, conventional synthetic approaches for such catalysts require extended periods of high-temperature annealing in vacuum systems, limiting their throughput and increasing their production cost. Herein, we report an ultrafast flash-thermal shock (FTS)-induced annealing technique (temperature > 2850 °C, <10 ms duration, and ramping/cooling rates of ∼105 K/s) that operates in an ambient-air environment to prepare single-atom-stabilized N-doped graphene. Melamine is utilized as an N-doping source to provide thermodynamically favorable metal-nitrogen bonding sites, resulting in a uniform and high-density atomic distribution of single metal atoms. To demonstrate the practical utility of the single-atom-stabilized N-doped graphene produced by the FTS method, we showcased their chemiresistive gas sensing capabilities and electrocatalytic activities. Overall, the air-ambient, ultrafast, and versatile (e.g., Co, Ni, Pt, and Co-Ni dual metal) FTS method provides a general route for high-throughput, large area, and vacuum-free manufacturing of single-atom catalysts.

Ultrafast Ambient-Air Exsolution on Metal Oxide via Momentary Photothermal Effect.

The process of exsolution for the synthesis of strongly anchored metal nanoparticles (NPs) on host oxide lattices has been proposed as a promising strategy for designing robust catalyst-support composite systems. However, because conventional exsolution processes occur in harsh reducing environments at high temperatures for long periods of time, the choice of support materials and dopant metals are limited to those with inherently high thermal and chemical stability. Herein, we report the exsolution of a series of noble metal catalysts (Pt, Rh, and Ir) from metal oxide nanofibers (WO3 NFs) supports in an entirely ambient environment induced by intense pulsed light (IPL)-derived momentary photothermal treatment (>1000 °C). Since the exsolution process spans an extremely short period of time (<20 ms), unwanted structural artifacts such as decreased surface area and phase transition of the support materials are effectively suppressed. At the same time, exsolved NPs (<5 nm) with uniform size distributions could successfully be formed. To prove the practical utility of exsolved catalytic NPs functionalized on WO3 NFs, the chemiresistive gas sensing characteristics of exsolved Pt-decorated WO3 NFs were analyzed, exhibiting high durability (>200 cyclic exposures), enhanced response (Rair/Rgas > 800 @ 1 ppm/350 °C), and selectivity toward H2S target gas. Altogether, we successfully demonstrated that ultrafast exsolution within a few milliseconds could be induced in ambient conditions using the IPL-derived momentary photothermal treatment and contributed to expanding the practical viability of the exsolution-based synthetic approaches for the production of highly stable catalyst systems.