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Construction of Boron- and Nitrogen-Enriched Nanoporous π-Conjugated Networks Towards Enhanced Hydrogen Activation
Abstract
Boron-enriched scaffolds have demonstrated unique features and promising performance in the field of catalysis towards the activation of small gas molecules. However, there is still a lack of facile approaches capable of achieving high B doping and abundant porous channels in the targeted catalysts. Here, in this paper, construction of boron- and nitrogen-enriched nanoporous π-conjugated networks (BN-NCNs) was achieved via a facile ionothermal polymerization procedure with hexaazatriphenylenehexacarbonitrile [HAT(CN)6] sodium borohydride as the starting materials. The as-produced BN-NCN scaffolds were featured by high heteroatoms doping (B up to 23 wt. % and N: up to 17 wt. %) and permanent porosity (surface area up to 759 m2 g-1 mainly contributed by micropores). With the unsaturated bonded B species acting as the active Lewis acid sites and defected N species acting as the active Lewis base sites, those BN-NCNs delivered attractive catalytic performance towards H2 activation/dissociation in both gaseous and liquid phase, acting as efficient metal-free heterogeneous frustrated Lewis pairs (FLPs) catalysts in hydrogenation procedures.
- Authors:
-
[1];
[1];
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
- University of Tennessee, Knoxville, TN (United States)
- Ames Laboratory, and Iowa State University, Ames, IA (United States)
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division; Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division; University of Tennessee, Knoxville, TN (United States)
- Publication Date:
- Research Org.:
- Ames Laboratory (AMES), Ames, IA (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE
- OSTI Identifier:
- 1987638
- Alternate Identifier(s):
- OSTI ID: 1983439; OSTI ID: 1992720
- Report Number(s):
- IS-J-11,073
Journal ID: ISSN 1433-7851
- Grant/Contract Number:
- AC02-07CH11358; AC02-06CH11357; AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Angewandte Chemie (International Edition)
- Additional Journal Information:
- Journal Name: Angewandte Chemie (International Edition); Journal Volume: 62; Journal Issue: 28; Journal ID: ISSN 1433-7851
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; B doping; frustrated Lewis pairs; hydrogen activation; hydrogenation; π-conjugated networks
Citation Formats
Li, Meijia, Qiu, Liqi, Popovs, Ilja, Yang, Weiwei, Ivanov, Alexander S., Kobayashi, Takeshi, Thapaliya, Bishnu P., Moitra, Debabrata, Yu, Xinbin, Wu, Zili, Yang, Zhenzhen, and Dai, Sheng. Construction of Boron- and Nitrogen-Enriched Nanoporous π-Conjugated Networks Towards Enhanced Hydrogen Activation. United States: N. p., 2023.
Web. doi:10.1002/anie.202302684.
Li, Meijia, Qiu, Liqi, Popovs, Ilja, Yang, Weiwei, Ivanov, Alexander S., Kobayashi, Takeshi, Thapaliya, Bishnu P., Moitra, Debabrata, Yu, Xinbin, Wu, Zili, Yang, Zhenzhen, & Dai, Sheng. Construction of Boron- and Nitrogen-Enriched Nanoporous π-Conjugated Networks Towards Enhanced Hydrogen Activation. United States. https://doi.org/10.1002/anie.202302684
Li, Meijia, Qiu, Liqi, Popovs, Ilja, Yang, Weiwei, Ivanov, Alexander S., Kobayashi, Takeshi, Thapaliya, Bishnu P., Moitra, Debabrata, Yu, Xinbin, Wu, Zili, Yang, Zhenzhen, and Dai, Sheng. Tue .
"Construction of Boron- and Nitrogen-Enriched Nanoporous π-Conjugated Networks Towards Enhanced Hydrogen Activation". United States. https://doi.org/10.1002/anie.202302684.
@article{osti_1987638,
title = {Construction of Boron- and Nitrogen-Enriched Nanoporous π-Conjugated Networks Towards Enhanced Hydrogen Activation},
author = {Li, Meijia and Qiu, Liqi and Popovs, Ilja and Yang, Weiwei and Ivanov, Alexander S. and Kobayashi, Takeshi and Thapaliya, Bishnu P. and Moitra, Debabrata and Yu, Xinbin and Wu, Zili and Yang, Zhenzhen and Dai, Sheng},
abstractNote = {Boron-enriched scaffolds have demonstrated unique features and promising performance in the field of catalysis towards the activation of small gas molecules. However, there is still a lack of facile approaches capable of achieving high B doping and abundant porous channels in the targeted catalysts. Here, in this paper, construction of boron- and nitrogen-enriched nanoporous π-conjugated networks (BN-NCNs) was achieved via a facile ionothermal polymerization procedure with hexaazatriphenylenehexacarbonitrile [HAT(CN)6] sodium borohydride as the starting materials. The as-produced BN-NCN scaffolds were featured by high heteroatoms doping (B up to 23 wt. % and N: up to 17 wt. %) and permanent porosity (surface area up to 759 m2 g-1 mainly contributed by micropores). With the unsaturated bonded B species acting as the active Lewis acid sites and defected N species acting as the active Lewis base sites, those BN-NCNs delivered attractive catalytic performance towards H2 activation/dissociation in both gaseous and liquid phase, acting as efficient metal-free heterogeneous frustrated Lewis pairs (FLPs) catalysts in hydrogenation procedures.},
doi = {10.1002/anie.202302684},
journal = {Angewandte Chemie (International Edition)},
number = 28,
volume = 62,
place = {United States},
year = {Tue May 09 00:00:00 EDT 2023},
month = {Tue May 09 00:00:00 EDT 2023}
}
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