Abstract
Alloyed materials are promising candidates to improve catalytic processes. Ni-Cu nanoparticles are used for various reactions, including processes with biomass-derived components. However, dynamical restructuring effects alter the catalytic properties and can deactivate the sample. To understand these structural modifications, a multimodal investigation of NiCu3/C was performed to determine compositional and morphological changes during a redox cycle to simulate reduction and oxidation of the catalyst during reaction. We exploit a novel correlative, multimodal approach that combines in situ X-ray absorption spectroscopy (XAS) and in situ scanning transmission electron microscopy and electron energy-loss spectroscopy (STEM-EELS) to describe changes that occur in the sample in realistic conditions. In the fresh sample, there are two morphologies present: core-shell and hollow. Segregation of Cu was observed in both types of particles after synthesis, with Cu being more oxidized in the hollow structures. Upon reduction for 2 h under H2 at 400 °C, the Cu was reduced, although segregation of Cu and Ni was still observed. Subsequent exposure to O2 at 400 °C led to a strong reoxidation of Cu with the formation of hollow particles with compositional heterogeneities. The oxidation of metals and segregation phenomena can be related to known catalytic properties of NiCu3/C particles, especially regarding the hydrodeoxygenation of 5-hydroxymethylfurfural to 2,5-dimethylfuran.
Original language | English |
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Pages (from-to) | 1991-2002 |
Number of pages | 12 |
Journal | Journal of Physical Chemistry C |
Volume | 126 |
Issue number | 4 |
DOIs | |
State | Published - Feb 3 2022 |
Externally published | Yes |
Funding
This work was supported as part of the Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award no. DE-SC0012573. This research used the 4-BM (XFM) beamline of the National Synchrotron Light Source, a U.S. DOE Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory (BNL) under Contract No. DE-SC0012704. Experiments were also carried out at the Singh Center for Nanotechnology at the University of Pennsylvania, supported by the National Science Foundation (NSF) National Nanotechnology Coordinated Infrastructure Program grant NNCI-1542153. Additional support to the Nanoscale Characterization Facility at the Singh Center has been provided by the Laboratory for Research on the Structure of Matter (MRSEC) supported by the National Science Foundation (DMR-1720530).
Funders | Funder number |
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Laboratory for Research on the Structure of Matter | |
National Science Foundation | NNCI-1542153 |
U.S. Department of Energy | |
Office of Science | |
Basic Energy Sciences | DE-SC0012573 |
Brookhaven National Laboratory | DE-SC0012704 |
Materials Research Science and Engineering Center, Harvard University | DMR-1720530 |
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Dive into the research topics of 'Dynamical Change of Valence States and Structure in NiCu3Nanoparticles during Redox Cycling'. Together they form a unique fingerprint.Datasets
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Replication Data for: Dynamical Change of Valence States and Structure in NiCu 3 Nanoparticles during Redox Cycling
Foucher, A. (Creator), Marcella, N. (Creator), Lee, J. D. (Creator), Tappero, R. (Creator), Murray, C. B. (Creator), Frenkel, A. I. (Creator) & Stach, E. A. (Creator), Harvard Dataverse, Apr 8 2022
DOI: 10.7910/DVN/MYCEOK
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