Mechanochemistry-Induced Strong Metal-Support Interactions Construction toward Enhanced Hydrogenation

Meijia Li, Tianyu Zhang, Shi Ze Yang, Yifan Sun, Junyan Zhang, Felipe Polo-Garzon, Kevin M. Siniard, Xinbin Yu, Zili Wu, Darren M. Driscoll, Alexander S. Ivanov, Hao Chen, Zhenzhen Yang, Sheng Dai

Research output: Contribution to journalArticlepeer-review

7 Scopus citations

Abstract

The construction of strong metal-support interactions (SMSIs) represented an attractive approach to producing supported noble metal nanocatalysts possessing enhanced stability by overlayer encapsulation. The development of facile approaches capable of achieving efficient, controllable, and extensive SMSI overlayer formation, particularly under neat and ambient conditions, is a long-standing challenge. In this work, a mechanochemistry-driven pathway was deployed for efficient and controllable SMSI construction under neat and ambient conditions to customize the capsulation degree and overlayer structures toward enhanced catalysis. The reducibility of the additives and the high interaction efficiency provided by the mechanochemical treatment could afford abundant active intermediates (e.g., Ti3+ species and oxygen defects) within a short time to induce and tune the overlayer encapsulation. This facile approach could be extensively deployed to TiO2-derived nanocatalysts with diverse phases, diverse reducible metal oxides-involved systems, and different supported noble metal nanoparticles. Enhanced hydrogenation activity was achieved by the as-afforded nanocatalysts upon SMSI construction and further tuned by the encapsulation degree.

Original languageEnglish
Pages (from-to)6114-6125
Number of pages12
JournalACS Catalysis
Volume13
Issue number9
DOIs
StatePublished - May 5 2023

Funding

The research was supported financially by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science Program. The authors acknowledge the use of facilities within the Eyring Materials Center at Arizona State University, supported in part by NNCI-ECCS-1542160. This research used resources from the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science user facility operated for the DOE Office of Science by the Argonne National Laboratory under Contract No. DE-AC02-06CH11357. The DRIFTS and gas phase hydrogenation test were conducted as part of a user project at the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory.

FundersFunder number
U.S. Department of Energy
Office of Science
Basic Energy SciencesNNCI-ECCS-1542160
Argonne National LaboratoryDE-AC02-06CH11357
Oak Ridge National Laboratory

    Keywords

    • encapsulation
    • hydrogenation
    • mechanochemistry
    • strong metal−support interaction
    • supported noble metal catalyst

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