Abstract
Improving the low-temperature activity (below 100 °C) and noble-metal efficiency of automotive exhaust catalysts has been a continuous effort to eliminate cold-start emissions, yet great challenges remain. Here we report a strategy to activate the low-temperature performance of Pt catalysts on Cu-modified CeO2 supports based on redox-coupled atomic layer deposition. The interfacial reducibility and structure of composite catalysts have been precisely tuned by oxide doping and accurate control of Pt size. Cu-modified CeO2-supported Pt sub-nanoclusters demonstrate a remarkable performance with an onset of CO oxidation reactivity below room temperature, which is one order of magnitude more active than atomically-dispersed Pt catalysts. The Cu-O-Ce site with activated lattice oxygen anchors deposited Pt sub-nanoclusters, leading to a moderate CO adsorption strength at the interface that facilitates the low-temperature CO oxidation performance.
Highlights
Improving the low-temperature activity and noble-metal efficiency of automotive exhaust catalysts has been a continuous effort to eliminate cold-start emissions, yet great challenges remain
The atomically dispersed Pt catalysts were deposited on two supports via regular Pt atomic layer deposition (ALD) with the sequence of MeCpPtMe3-O2, which were denoted as Pt1/Ce and Pt1/CeCu
Cu dopants have been introduced to modulate the surface reducibility of CeO2 support, which led to the formation of Cu2+ ions in the CeO2 lattice and helped create active Cu–O–Ce sites for tuning the interfacial structures and anchoring the Pt catalysts
Summary
Improving the low-temperature activity (below 100 °C) and noble-metal efficiency of automotive exhaust catalysts has been a continuous effort to eliminate cold-start emissions, yet great challenges remain. We report a strategy to activate the low-temperature performance of Pt catalysts on Cu-modified CeO2 supports based on redox-coupled atomic layer deposition. Cu-modified CeO2-supported Pt sub-nanoclusters demonstrate a remarkable performance with an onset of CO oxidation reactivity below room temperature, which is one order of magnitude more active than atomically-dispersed Pt catalysts. The general consensus is that the generation catalyst must be active in the sub 100 °C range to reduce or eliminate cold-start emissions[3,4,5]. To further increase the utilization rate of the Pt component, supported single atoms and sub-nanocluster catalysts have been extensively investigated due to their higher atomic efficiency[19,20,21]
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