Unravelling the origin of reaction-driven aggregation and fragmentation of atomically dispersed Pt catalyst on ceria support

Wang, Haodong; Choi, Hyuk; Shimogawa, Ryuichi; Li, Yuanyuan; Zhang, Lihua; Kim, Hyun You; Frenkel, Anatoly I.

doi:10.1039/d4nr01396d

Title: Unravelling the origin of reaction-driven aggregation and fragmentation of atomically dispersed Pt catalyst on ceria support

Journal Article · 14 May 2024 · Nanoscale

DOI: https://doi.org/10.1039/d4nr01396d · OSTI ID:2372682

Wang, Haodong ^[1]; Choi, Hyuk ^[2]; Shimogawa, Ryuichi ^[3]; Li, Yuanyuan ^[4]; Zhang, Lihua ^[5];

^[2];

^[6]

Stony Brook Univ., NY (United States)
Chungnam National Univ., Daejeon (Korea, Republic of)
Stony Brook Univ., NY (United States); Mitsubishi Chemical Corporation, Yokohama (Japan). Science and Innovation Center
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Stony Brook Univ., NY (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)

Metal–support interaction plays a crucial role in governing the stability and activity of atomically dispersed platinum catalysts on ceria support. The migration and aggregation of platinum atoms during the catalytic reaction leads to the redistribution of active sites. In this study, by utilizing a multimodal characterization scheme, we observed the aggregation of platinum atoms at high temperatures under reverse water gas shift reaction conditions and the subsequent fragmentation of platinum clusters, forming “single atoms” upon cooling. Theoretical simulations of both effects uncovered the roles of carbon monoxide binding on perimeter Pt sites in the clusters and hydrogen coverage in the aggregation and fragmentation mechanisms. Finally, this study highlights the complex effects of adsorbate and supports interactions with metal sites in Pt/ceria catalysts that govern their structural transformations under in situ conditions.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: SC0012704; SC0022199

OSTI ID:: 2372682

Report Number(s):: BNL-225696-2024-JAAM

Journal Information:: Nanoscale, Journal Name: Nanoscale Journal Issue: 31 Vol. 16; ISSN 2040-3364

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

References (24)

Nano-sized Ag rather than single-atom Ag determines CO oxidation activity and stability Wang, Fei; Li, Zhao; Wang, Honghong Nano Research, Vol. 15, Issue 1 https://doi.org/10.1007/s12274-021-3501-1	journal	July 2021
Identification of relevant active sites and a mechanism study for reverse water gas shift reaction over Pt/CeO 2 catalysts Chen, Xiaodong; Su, Xiong; Liang, Binglian Journal of Energy Chemistry, Vol. 25, Issue 6 https://doi.org/10.1016/j.jechem.2016.11.011	journal	November 2016
Tuning the Placement of Pt “Single Atoms” on a Mixed CeO₂–TiO₂ Support Wang, Haodong; Rui, Ning; Senanayake, Sanjaya D. The Journal of Physical Chemistry C, Vol. 126, Issue 38 https://doi.org/10.1021/acs.jpcc.2c05198	journal	September 2022
Aliovalent Doping of CeO₂ Improves the Stability of Atomically Dispersed Pt Wang, Haodong; Kottwitz, Matthew; Rui, Ning ACS Applied Materials & Interfaces, Vol. 13, Issue 44 https://doi.org/10.1021/acsami.1c18330	journal	October 2021
Elucidation of the Active Sites in Single-Atom Pd ₁ /CeO ₂ Catalysts for Low-Temperature CO Oxidation Jiang, Dong; Wan, Gang; García-Vargas, Carlos E. ACS Catalysis, Vol. 10, Issue 19 https://doi.org/10.1021/acscatal.0c02480	journal	August 2020
Continuous CO₂ Capture and Selective Hydrogenation to CO over Na-Promoted Pt Nanoparticles on Al₂O₃ Li, Lingcong; Miyazaki, Shinta; Yasumura, Shunsaku ACS Catalysis, Vol. 12, Issue 4 https://doi.org/10.1021/acscatal.1c05339	journal	February 2022
Reduction of Nitric Oxide with Hydrogen on Catalysts of Singly Dispersed Bimetallic Sites Pt ₁ Co _m and Pd ₁ Co _n Nguyen, Luan; Zhang, Shiran; Wang, Lei ACS Catalysis, Vol. 6, Issue 2 https://doi.org/10.1021/acscatal.5b00842	journal	January 2016
Utilizing Quantitative in Situ FTIR Spectroscopy To Identify Well-Coordinated Pt Atoms as the Active Site for CO Oxidation on Al ₂ O ₃ -Supported Pt Catalysts Kale, Matthew J.; Christopher, Phillip ACS Catalysis, Vol. 6, Issue 8 https://doi.org/10.1021/acscatal.6b01128	journal	July 2016
Catalysis on Singly Dispersed Rh Atoms Anchored on an Inert Support Zhang, Shiran; Tang, Yan; Nguyen, Luan ACS Catalysis, Vol. 8, Issue 1 https://doi.org/10.1021/acscatal.7b01788	journal	December 2017
In Situ Elucidation of the Active State of Co–CeO _x Catalysts in the Dry Reforming of Methane: The Important Role of the Reducible Oxide Support and Interactions with Cobalt Zhang, Feng; Liu, Zongyuan; Zhang, Shuhao ACS Catalysis, Vol. 8, Issue 4 https://doi.org/10.1021/acscatal.7b03640	journal	March 2018
Nanoceria-Supported Single-Atom Platinum Catalysts for Direct Methane Conversion Xie, Pengfei; Pu, Tiancheng; Nie, Anmin ACS Catalysis, Vol. 8, Issue 5 https://doi.org/10.1021/acscatal.8b00004	journal	April 2018
Local Structure and Electronic State of Atomically Dispersed Pt Supported on Nanosized CeO ₂ Kottwitz, Matthew; Li, Yuanyuan; Palomino, Robert M. ACS Catalysis, Vol. 9, Issue 9 https://doi.org/10.1021/acscatal.9b02083	journal	August 2019
Low-Temperature Catalytic NO Reduction with CO by Subnanometric Pt Clusters Fernández, Estefanía; Liu, Lichen; Boronat, Mercedes ACS Catalysis, Vol. 9, Issue 12 https://doi.org/10.1021/acscatal.9b03207	journal	October 2019
Dynamic Evolution of Palladium Single Atoms on Anatase Titania Support Determines the Reverse Water–Gas Shift Activity Chen, Linxiao; Allec, Sarah I.; Nguyen, Manh-Thuong Journal of the American Chemical Society, Vol. 145, Issue 19 https://doi.org/10.1021/jacs.3c02326	journal	May 2023
Catalyst Architecture for Stable Single Atom Dispersion Enables Site-Specific Spectroscopic and Reactivity Measurements of CO Adsorbed to Pt Atoms, Oxidized Pt Clusters, and Metallic Pt Clusters on TiO ₂ DeRita, Leo; Dai, Sheng; Lopez-Zepeda, Kimberly Journal of the American Chemical Society, Vol. 139, Issue 40 https://doi.org/10.1021/jacs.7b07093	journal	September 2017
Single-atom catalysis of CO oxidation using Pt1/FeOx Qiao, Botao; Wang, Aiqin; Yang, Xiaofeng Nature Chemistry, Vol. 3, Issue 8 https://doi.org/10.1038/nchem.1095	journal	July 2011
Dynamic structure of active sites in ceria-supported Pt catalysts for the water gas shift reaction Li, Yuanyuan; Kottwitz, Matthew; Vincent, Joshua L. Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-21132-4	journal	February 2021
Interrogating site dependent kinetics over SiO2-supported Pt nanoparticles Kim, Taek-Seung; O’Connor, Christopher R.; Reece, Christian Nature Communications, Vol. 15, Issue 1 https://doi.org/10.1038/s41467-024-46496-1	journal	March 2024
Functional CeOx nanoglues for robust atomically dispersed catalysts Li, Xu; Pereira-Hernández, Xavier Isidro; Chen, Yizhen Nature, Vol. 611, Issue 7935 https://doi.org/10.1038/s41586-022-05251-6	journal	October 2022
Migration and aggregation of Pt atoms on metal oxide-supported ceria nanodomes control reverse water gas shift reaction activity Wang, Haodong; Shimogawa, Ryuichi; Zhang, Lihua Communications Chemistry, Vol. 6, Issue 1 https://doi.org/10.1038/s42004-023-01064-4	journal	December 2023
Promotion of Pt/CeO ₂ catalyst by hydrogen treatment for low-temperature CO oxidation Jan, Asif; Shin, Jisu; Ahn, Junsung RSC Advances, Vol. 9, Issue 46 https://doi.org/10.1039/C9RA05965B	journal	January 2019
The importance of being together Stephens, I. E. L.; Elias, J. S.; Shao-Horn, Y. Science, Vol. 350, Issue 6257 https://doi.org/10.1126/science.aad3716	journal	October 2015
Thermally stable single-atom platinum-on-ceria catalysts via atom trapping Jones, J.; Xiong, H.; DeLaRiva, A. T. Science, Vol. 353, Issue 6295 https://doi.org/10.1126/science.aaf8800	journal	July 2016
Activation of surface lattice oxygen in single-atom Pt/CeO ₂ for low-temperature CO oxidation Nie, Lei; Mei, Donghai; Xiong, Haifeng Science, Vol. 358, Issue 6369 https://doi.org/10.1126/science.aao2109	journal	December 2017