Controlled site coverage of strong metal–support interaction (SMSI) on Pd NP catalysts

Breckner, Christian J.; Zhu, Kuixin; Wang, Mingrui; Zhang, Guanghui; Li, Christina W.; Miller, Jeffrey T.

doi:10.1039/d2cy01707e

Title: Controlled site coverage of strong metal–support interaction (SMSI) on Pd NP catalysts

Journal Article · Fri Nov 18 00:00:00 UTC 2022 · Catalysis Science and Technology

DOI: https://doi.org/10.1039/d2cy01707e · OSTI ID:2423320

^[1]; Zhu, Kuixin ^[1]; Wang, Mingrui ^[2];

^[2];

^[1];

^[1]

Purdue University, West Lafayette, IN (United States)
Dalian University of Technology, Liaoning (China)

Here, strong metal–support interaction catalysts have been shown to improve desired product selectivity at the cost of fractional rates due to active site coverage. The goal of this study was to determine if the active site coverage of metallic nanoparticles could be controlled to lower levels than have been previously reported in SMSI catalysts with the aim of improving the rate while maintaining high selectivity. 2Pd–XTi/SiO₂ (2 wt% Pd, X wt% Ti) strong metal–support interaction (SMSI) catalysts with Ti loadings between 0–1.0 wt% were synthesized to control Pd nanoparticle coverage. Calcination at 450 °C and reduction at 550 °C were sufficient for forming ~2 nm sized Pd particles in all catalysts. Increasing the Ti loading from 0.1 to 1.0 wt% increased the surface coverage from 40 to 85% at a fixed reduction temperature of 550 °C. The IR spectra of the SMSI catalysts were similar with a high fraction of linear bonded CO which was much higher than that of Pd nanoparticles of similar size. The SMSI overlayer could be removed by oxidation at 350 °C and re-reduction at 200 °C. EXAFS of the oxidized catalysts indicates that nearly full oxidation of the metallic nanoparticle was required to remove the SMSI overlayer. Oxidation temperatures from 30 to 300 °C partially oxidized the Pd nanoparticles and subsequent re-reduction at 200 °C partially decreases the SMSI coverage. The fractional surface coverage was determined by measuring the rate of propylene hydrogenation with and without the SMSI overlayer. Increasing the reduction temperature from 200 to 550 °C increased the SMSI coverage from 0 to 85% depending on the Ti loading and temperature. In conclusion, after reduction at 550 °C and oxidation at 350 °C, the range of coverages varied between ~10% with 0.1 wt% Ti after re-reduction at 300 °C and ~85% with 1 wt% Ti after reduction at 550 °C.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: National Natural Science Foundation of China; National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 2423320

Journal Information:: Catalysis Science and Technology, Journal Name: Catalysis Science and Technology Journal Issue: 1 Vol. 13; ISSN 2044-4753

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Title: Controlled site coverage of strong metal–support interaction (SMSI) on Pd NP catalysts

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