In situ identification of the metallic state of Ag nanoclusters in oxidative dispersion
Open Access
- 3 March 2021
- journal article
- research article
- Published by Springer Science and Business Media LLC in Nature Communications
- Vol. 12 (1), 1-9
- https://doi.org/10.1038/s41467-021-21552-2
Abstract
Oxidative dispersion has been widely used in regeneration of sintered metal catalysts and fabrication of single atom catalysts, which is attributed to an oxidation-induced dispersion mechanism. However, the interplay of gas-metal-support interaction in the dispersion processes, especially the gas-metal interaction has not been well illustrated. Here, we show dynamic dispersion of silver nanostructures on silicon nitride surface under reducing/oxidizing conditions and during carbon monoxide oxidation reaction. Utilizing environmental scanning (transmission) electron microscopy and near-ambient pressure photoelectron spectroscopy/photoemission electron microscopy, we unravel a new adsorption-induced dispersion mechanism in such a typical oxidative dispersion process. The strong gas-metal interaction achieved by chemisorption of oxygen on nearly-metallic silver nanoclusters is the internal driving force for dispersion. In situ observations show that the dispersed nearly-metallic silver nanoclusters are oxidized upon cooling in oxygen atmosphere, which could mislead to the understanding of oxidation-induced dispersion. We further understand the oxidative dispersion mechanism from the view of dynamic equilibrium taking temperature and gas pressure into account, which should be applied to many other metals such as gold, copper, palladium, etc. and other reaction conditions.Funding Information
- National Science Foundation of China | National Natural Science Foundation of China-Yunnan Joint Fund (21688102, 21825203, 21872145, and 21773287)
This publication has 55 references indexed in Scilit:
- Atmosphere-dependent stability and mobility of catalytic Pt single atoms and clusters on γ-Al2O3Nanoscale, 2019
- Tuning the Structure of Platinum Particles on Ceria In Situ for Enhancing the Catalytic Performance of Exhaust Gas CatalystsAngewandte Chemie, 2017
- Reversible Transformation of Pt Nanoparticles into Single Atoms inside High-Silica Chabazite ZeoliteJournal of the American Chemical Society, 2016
- Metal Redispersion Strategies for Recycling of Supported Metal Catalysts: A PerspectiveACS Catalysis, 2015
- Heterogeneous Catalyst Deactivation and Regeneration: A ReviewCatalysts, 2015
- Sintering of Catalytic Nanoparticles: Particle Migration or Ostwald Ripening?Accounts of Chemical Research, 2013
- Redispersion of Gold Supported on OxidesACS Catalysis, 2012
- Deactivation and Regeneration of Spent Three-Way Automotive Exhaust Gas Catalysts (TWC)Topics in Catalysis, 2004
- The Effect of Size-Dependent Nanoparticle Energetics on Catalyst SinteringScience, 2002
- Self-regeneration of a Pd-perovskite catalyst for automotive emissions controlNature, 2002