Real-time dynamics and structures of supported subnanometer catalysts via multiscale simulations

Yifan Wang, Jake Kalscheur, Ya-Qiong Su, Emiel J. M. Hensen () and Dionisios G. Vlachos ()
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Yifan Wang: University of Delaware, Newark
Jake Kalscheur: University of Delaware, Newark
Ya-Qiong Su: Xi’an Jiaotong University
Emiel J. M. Hensen: Eindhoven University of Technology
Dionisios G. Vlachos: University of Delaware, Newark

Nature Communications, 2021, vol. 12, issue 1, 1-9

Abstract: Abstract Understanding the performance of subnanometer catalysts and how catalyst treatment and exposure to spectroscopic probe molecules change the structure requires accurate structure determination under working conditions. Experiments lack simultaneous temporal and spatial resolution and could alter the structure, and similar challenges hinder first-principles calculations from answering these questions. Here, we introduce a multiscale modeling framework to follow the evolution of subnanometer clusters at experimentally relevant time scales. We demonstrate its feasibility on Pd adsorbed on CeO2(111) at various catalyst loadings, temperatures, and exposures to CO. We show that sintering occurs in seconds even at room temperature and is mainly driven by free energy reduction. It leads to a kinetically (far from equilibrium) frozen ensemble of quasi-two-dimensional structures that CO chemisorption and infrared experiments probe. CO adsorption makes structures flatter and smaller. High temperatures drive very rapid sintering toward larger, stable/metastable equilibrium structures, where CO induces secondary structure changes only.

Date: 2021
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Persistent link: https://EconPapers.repec.org/RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-25752-8

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DOI: 10.1038/s41467-021-25752-8

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