Revealing Sintering Kinetics of MoS2-Supported Metal Nanocatalysts in Atmospheric Gas Environments via Operando Transmission Electron Microscopy

Song, Boao; Yang, Timothy T.; Yuan, Yifei; Sharifi-Asl, Soroosh; Cheng, Meng; Saidi, Wissam A.; Liu, Yuzi; Shahbazian-Yassar, Reza

doi:10.1021/acsnano.9b08757

Revealing Sintering Kinetics of MoS₂-Supported Metal Nanocatalysts in Atmospheric Gas Environments via Operando Transmission Electron Microscopy

Journal Article · Mon Apr 13 00:00:00 EDT 2020 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.9b08757· OSTI ID:1632853

^[1]; ^[2]; ^[3]; ^[1]; Cheng, Meng ^[1]; ^[2]; ^[4]; ^[1]

Univ. of Illinois, Chicago, IL (United States)
Univ. of Pittsburgh, PA (United States)
Department of Mechanical and Industrial Engineering, University of Illinois at Chicago, Chicago, Illinois 60607, United States
Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials

The decoration of two-dimensional (2D) substrates with nanoparticles (NPs) serve as heterostructures for various catalysis applications. Deep understanding of catalyst degradation mechanisms during service conditions is crucial to improve the catalyst durability. In this work, we studied the sintering behavior of Pt and bimetallic Au-core Pt-shell (Au@Pt core–shell) NPs on MoS₂ supports at high temperatures under vacuum, nitrogen (N₂), hydrogen (H₂), and air environments by in situ gas-cell transmission electron microscopy (TEM). The key observations are summarized as effect of environment: while particle migration and coalescence (PMC) was the main mechanism that led to Pt and Au@Pt NPs degradation under vacuum, N₂, and H₂ environments, the degradation of MoS₂ substrate was prominent under exposure to air at high temperatures. Pt NPs were less stable in H₂ environment when compared with the Pt NPs under vacuum or N₂, due to Pt–H interactions that weakened the adhesion of Pt on MoS₂. Effect of NP composition: under H₂, the stability of Au@Pt NPs was higher in comparison to Pt NPs. This is because H₂ promotes the alloying of Pt–Au, thus reducing the number of Pt at the surface (reducing H₂ interactions) and increasing Pt atoms in contact with MoS₂. Effect of NP size: The alloying effect promoted by H₂ was more pronounced in small size Au@Pt NPs resulting in their higher sintering resistance in comparison to large size Au@Pt NPs and similar size Pt NPs. The present work provides key insights into the parameters affecting the catalyst degradation mechanisms on 2D supports.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1632853

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 4 Vol. 14; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Revealing Sintering Kinetics of MoS2-Supported Metal Nanocatalysts in Atmospheric Gas Environments via Operando Transmission Electron Microscopy

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Revealing Sintering Kinetics of MoS₂-Supported Metal Nanocatalysts in Atmospheric Gas Environments via Operando Transmission Electron Microscopy