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Breaking New Ground: MBene Route toward Selective Vinyl Double Bond Hydrogenation in Nitroarenes
Abstract
Doping, or incremental substitution of one element for another, is an effective way to tailor a compound’s structure as well as its physical and chemical properties. Herein, we replaced up to 30% of Ni with Co in members of the family of layered LiNiB compounds, stabilizing the high-temperature polymorph of LiNiB while the room-temperature polymorph does not form. By studying this layered boride with in situ high-temperature powder diffraction, we obtained a distorted variant of LiNi0.7Co0.3B featuring a perfect interlayer placement of [Ni0.7Co0.3B] layers on top of each other–a structural motif not seen before in other borides. Because of the Co doping, LiNi0.7Co0.3B can undergo a nearly complete topochemical Li deintercalation under ambient conditions, resulting in a metastable boride with the formula Li0.04Ni0.7Co0.3B. Heating of Li0.04Ni0.7Co0.3B in anaerobic conditions led to yet another metastable boride, Li0.01Ni0.7Co0.3B, with a CoB-type crystal structure that cannot be obtained by simple annealing of Ni, Co, and B. No significant alterations of magnetic properties were detected upon Co-doping in the temperature-independent paramagnet LiNi0.7Co0.3B or its Li-deintercalated counterparts. Finally, Li0.01Ni0.7Co0.3B stands out as an exceptional catalyst for the selective hydrogenation of the vinyl C=C bond in 3-nitrostyrene, even in the presence of other competing functional groups.more »
- Authors:
-
[3];
[3];
[1]
- Iowa State Univ., Ames, IA (United States)
- Iowa State Univ., Ames, IA (United States); Univ. of Alberta, Edmonton, AB (Canada)
- Iowa State Univ., Ames, IA (United States); Ames Laboratory (AMES), Ames, IA (United States)
- Ames Lab., and Iowa State Univ., Ames, IA (United States)
- Publication Date:
- Research Org.:
- Ames Laboratory (AMES), Ames, IA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)
- OSTI Identifier:
- 2305643
- Report Number(s):
- IS-J-11,214
Journal ID: ISSN 0002-7863
- Grant/Contract Number:
- AC02-07CH11358; AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 145; Journal Issue: 50; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalysts; chemical structure; diffraction; hydrogenation; layers
Citation Formats
Bhaskar, Gourab, Behera, Ranjan K., Gvozdetskyi, Volodymyr, Carnahan, Scott L., Ribeiro, Raquel A., Oftedahl, Paul, Ward, Charles, Canfield, Paul C., Rossini, Aaron J., Huang, Wenyu, and Zaikina, Julia V. Breaking New Ground: MBene Route toward Selective Vinyl Double Bond Hydrogenation in Nitroarenes. United States: N. p., 2023.
Web. doi:10.1021/jacs.3c08642.
Bhaskar, Gourab, Behera, Ranjan K., Gvozdetskyi, Volodymyr, Carnahan, Scott L., Ribeiro, Raquel A., Oftedahl, Paul, Ward, Charles, Canfield, Paul C., Rossini, Aaron J., Huang, Wenyu, & Zaikina, Julia V. Breaking New Ground: MBene Route toward Selective Vinyl Double Bond Hydrogenation in Nitroarenes. United States. https://doi.org/10.1021/jacs.3c08642
Bhaskar, Gourab, Behera, Ranjan K., Gvozdetskyi, Volodymyr, Carnahan, Scott L., Ribeiro, Raquel A., Oftedahl, Paul, Ward, Charles, Canfield, Paul C., Rossini, Aaron J., Huang, Wenyu, and Zaikina, Julia V. Thu .
"Breaking New Ground: MBene Route toward Selective Vinyl Double Bond Hydrogenation in Nitroarenes". United States. https://doi.org/10.1021/jacs.3c08642.
@article{osti_2305643,
title = {Breaking New Ground: MBene Route toward Selective Vinyl Double Bond Hydrogenation in Nitroarenes},
author = {Bhaskar, Gourab and Behera, Ranjan K. and Gvozdetskyi, Volodymyr and Carnahan, Scott L. and Ribeiro, Raquel A. and Oftedahl, Paul and Ward, Charles and Canfield, Paul C. and Rossini, Aaron J. and Huang, Wenyu and Zaikina, Julia V.},
abstractNote = {Doping, or incremental substitution of one element for another, is an effective way to tailor a compound’s structure as well as its physical and chemical properties. Herein, we replaced up to 30% of Ni with Co in members of the family of layered LiNiB compounds, stabilizing the high-temperature polymorph of LiNiB while the room-temperature polymorph does not form. By studying this layered boride with in situ high-temperature powder diffraction, we obtained a distorted variant of LiNi0.7Co0.3B featuring a perfect interlayer placement of [Ni0.7Co0.3B] layers on top of each other–a structural motif not seen before in other borides. Because of the Co doping, LiNi0.7Co0.3B can undergo a nearly complete topochemical Li deintercalation under ambient conditions, resulting in a metastable boride with the formula Li0.04Ni0.7Co0.3B. Heating of Li0.04Ni0.7Co0.3B in anaerobic conditions led to yet another metastable boride, Li0.01Ni0.7Co0.3B, with a CoB-type crystal structure that cannot be obtained by simple annealing of Ni, Co, and B. No significant alterations of magnetic properties were detected upon Co-doping in the temperature-independent paramagnet LiNi0.7Co0.3B or its Li-deintercalated counterparts. Finally, Li0.01Ni0.7Co0.3B stands out as an exceptional catalyst for the selective hydrogenation of the vinyl C=C bond in 3-nitrostyrene, even in the presence of other competing functional groups. Finally, this research showcases an innovative approach to heterogeneous catalyst design by meticulously synthesizing metastable compounds.},
doi = {10.1021/jacs.3c08642},
journal = {Journal of the American Chemical Society},
number = 50,
volume = 145,
place = {United States},
year = {Thu Dec 07 00:00:00 EST 2023},
month = {Thu Dec 07 00:00:00 EST 2023}
}
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