Lithium-Ion Battery Materials as Tunable, “Redox Non-Innocent” Catalyst Supports
Abstract
The development of general strategies for the electronic tuning of a catalyst’s active site is an ongoing challenge in heterogeneous catalysis. To this end, herein, we describe the application of Li-ion battery cathode and anode materials as redox non-innocent catalyst supports that can be continuously modulated as a function of lithium intercalation. A zero-valent nickel complex was oxidatively grafted onto the surface of lithium manganese oxide (LixMn2O4) to yield isolated Ni2+ occupying the vacant interstitial octahedral site in the Li diffusion channel on the surface and subsurface of the spinel structure (Ni/LixMn2O4). Additionally, the activity of Ni/LixMn2O4 for olefin hydrogenation, as a representative probe reaction, was found to increase monotonically as a function of support reductive lithiation. Simulation of Ni/LixMn2O4 reveals the dramatic impact of surface redox states on the viability of the homolytic oxidative addition mechanism for H2 activation. Catalyst control through support lithiation was extended to an organotantalum complex on LixTiO2, demonstrating the generality of this phenomenon.
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- Argonne National Lab. (ANL), Lemont, IL (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Argonne National Lab. (ANL), Lemont, IL (United States). Center for Nanoscale Materials
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1871874
- Alternate Identifier(s):
- OSTI ID: 1879424
- Report Number(s):
- BNL-223195-2022-JAAM
Journal ID: ISSN 2155-5435
- Grant/Contract Number:
- AC05-00OR22725; SC0012704; AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Catalysis
- Additional Journal Information:
- Journal Volume: 12; Journal Issue: 12; Journal ID: ISSN 2155-5435
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalyst design; tunable catalysis; hydrogenation; surface organometallic chemistry; nickel; catalysts; materials; oxides; redox reactions; transition metals; 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY
Citation Formats
Chapovetsky, Alon, Kennedy, Robert M., Witzke, Ryan, Wegener, Evan C., Dogan, Fulya, Patel, Prajay, Ferrandon, Magali, Niklas, Jens, Poluektov, Oleg G., Rui, Ning, Senanayake, Sanjaya D., Rodriguez, José A., Zaluzec, Nestor J., Yu, Lei, Wen, Jianguo, Johnson, Christopher, Jenks, Cynthia J., Kropf, A. Jeremy, Liu, Cong, Delferro, Massimiliano, and Kaphan, David M. Lithium-Ion Battery Materials as Tunable, “Redox Non-Innocent” Catalyst Supports. United States: N. p., 2022.
Web. doi:10.1021/acscatal.2c00935.
Chapovetsky, Alon, Kennedy, Robert M., Witzke, Ryan, Wegener, Evan C., Dogan, Fulya, Patel, Prajay, Ferrandon, Magali, Niklas, Jens, Poluektov, Oleg G., Rui, Ning, Senanayake, Sanjaya D., Rodriguez, José A., Zaluzec, Nestor J., Yu, Lei, Wen, Jianguo, Johnson, Christopher, Jenks, Cynthia J., Kropf, A. Jeremy, Liu, Cong, Delferro, Massimiliano, & Kaphan, David M. Lithium-Ion Battery Materials as Tunable, “Redox Non-Innocent” Catalyst Supports. United States. https://doi.org/10.1021/acscatal.2c00935
Chapovetsky, Alon, Kennedy, Robert M., Witzke, Ryan, Wegener, Evan C., Dogan, Fulya, Patel, Prajay, Ferrandon, Magali, Niklas, Jens, Poluektov, Oleg G., Rui, Ning, Senanayake, Sanjaya D., Rodriguez, José A., Zaluzec, Nestor J., Yu, Lei, Wen, Jianguo, Johnson, Christopher, Jenks, Cynthia J., Kropf, A. Jeremy, Liu, Cong, Delferro, Massimiliano, and Kaphan, David M. Thu .
"Lithium-Ion Battery Materials as Tunable, “Redox Non-Innocent” Catalyst Supports". United States. https://doi.org/10.1021/acscatal.2c00935. https://www.osti.gov/servlets/purl/1871874.
@article{osti_1871874,
title = {Lithium-Ion Battery Materials as Tunable, “Redox Non-Innocent” Catalyst Supports},
author = {Chapovetsky, Alon and Kennedy, Robert M. and Witzke, Ryan and Wegener, Evan C. and Dogan, Fulya and Patel, Prajay and Ferrandon, Magali and Niklas, Jens and Poluektov, Oleg G. and Rui, Ning and Senanayake, Sanjaya D. and Rodriguez, José A. and Zaluzec, Nestor J. and Yu, Lei and Wen, Jianguo and Johnson, Christopher and Jenks, Cynthia J. and Kropf, A. Jeremy and Liu, Cong and Delferro, Massimiliano and Kaphan, David M.},
abstractNote = {The development of general strategies for the electronic tuning of a catalyst’s active site is an ongoing challenge in heterogeneous catalysis. To this end, herein, we describe the application of Li-ion battery cathode and anode materials as redox non-innocent catalyst supports that can be continuously modulated as a function of lithium intercalation. A zero-valent nickel complex was oxidatively grafted onto the surface of lithium manganese oxide (LixMn2O4) to yield isolated Ni2+ occupying the vacant interstitial octahedral site in the Li diffusion channel on the surface and subsurface of the spinel structure (Ni/LixMn2O4). Additionally, the activity of Ni/LixMn2O4 for olefin hydrogenation, as a representative probe reaction, was found to increase monotonically as a function of support reductive lithiation. Simulation of Ni/LixMn2O4 reveals the dramatic impact of surface redox states on the viability of the homolytic oxidative addition mechanism for H2 activation. Catalyst control through support lithiation was extended to an organotantalum complex on LixTiO2, demonstrating the generality of this phenomenon.},
doi = {10.1021/acscatal.2c00935},
journal = {ACS Catalysis},
number = 12,
volume = 12,
place = {United States},
year = {2022},
month = {6}
}
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