Constructing Intermediate Encapsulation on Ru/CeO 2 Nanocatalysts to Enhance Ammonia Synthesis
Source abstract
Abstract
ABSTRACT Engineering the metal‐support interfacial structure in supported heterogeneous catalysts opens wide opportunities to tailor catalytic performance, particularly by exploiting strong metal‐support interactions (SMSI) that modify active‐site electronic and geometric properties to tune adsorption energetics, activity and stability. However, designing SMSI that simultaneously meets the geometric requirement of sufficient active site exposure, and the electronic requirement remains challenging. Here, we achieved an intermediate encapsulation by forming crystallographically defined CeO x overlayers on Ru/CeO 2 via a Ru‐precursor‐mediated route. Using Ru 3 (CO) 12 as the precursors creates a locally reducing environment on CeO 2 {100}, inducing localized surface modification and formation of truncated‐pyramid‐shaped SMSI overlayers on Ru with a height of ∼2–3 atomic layers (Ru/CeO 2 ─CO). By contrast, catalysts prepared from Ru(NO)(NO 3 ) 3 (Ru/CeO 2 ─NO 3 ) show no SMSI encapsulation. Ru/CeO 2 ─CO exhibits significantly higher oxygen‐vacancy concentrations both overall and within the SMSI layer, which promotes electron transfer from the interface and overlayer to the Ru nanoparticles. The formation of electron‐rich Ru species, without blocking a significant number of active sites, facilitates nitrogen activation and enhances catalytic ammonia synthesis. This work presents a novel strategy to construct intermediate SMSI encapsulation and also provides mechanistic insight into precursor‐dependent activity at the nanoscale.
Source: crossref · Quality: baseline
Research context
OpenAlex topics: Ammonia Synthesis and Nitrogen Reduction · Electrocatalysts for Energy Conversion · Catalytic Processes in Materials Science
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
Affiliations
Center of Electron Microscopy and State Key Laboratory of Silicon and Advanced Semiconductor Materials School of Materials Science and Engineering Zhejiang University Hangzhou China
State Key Laboratory of Solidification Processing School of Materials Science and Engineering Northwestern Polytechnical University Xi'an China
Funding
National Key Research and Development Program of China · National Natural Science Foundation of China
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