Construction of Boron- and Nitrogen-Enriched Nanoporous π-Conjugated Networks Towards Enhanced Hydrogen Activation

Meijia Li; Liqi Qiu; Ilja Popovs; Weiwei Yang; Alexander S. Ivanov; Takeshi Kobayashi; Bishnu P. Thapaliya; Debabrata Moitra; Xinbin Yu; Zili Wu; Zhenzhen Yang; Sheng Dai

doi:10.1002/anie.202302684

Construction of Boron- and Nitrogen-Enriched Nanoporous π-Conjugated Networks Towards Enhanced Hydrogen Activation

Meijia Li, Liqi Qiu, Ilja Popovs, Weiwei Yang, Alexander S. Ivanov, Takeshi Kobayashi, Bishnu P. Thapaliya, Debabrata Moitra, Xinbin Yu, Zili Wu, Zhenzhen Yang, Sheng Dai

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4 Scopus citations

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. Herein, 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.

Original language	English
Article number	e202302684
Journal	Angewandte Chemie - International Edition
Volume	62
Issue number	28
DOIs	https://doi.org/10.1002/anie.202302684
State	Published - Jul 10 2023

Funding

The research was supported financially by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science Program. A part of this work (solid‐state NMR) was supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences, Materials Science and Engineering Division. The research was performed at the Ames National Laboratory, which is operated for the U.S. DOE by Iowa State University under Contract No. DE‐AC02‐07CH11358. Use of the Advanced Photon Source at Argonne National Laboratory was supported by the U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE‐AC02‐06CH11357. DRIFTS was conducted as part of a user project at the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory. In situ The research was supported financially by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science Program. A part of this work (solid-state NMR) was supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences, Materials Science and Engineering Division. The research was performed at the Ames National Laboratory, which is operated for the U.S. DOE by Iowa State University under Contract No. DE-AC02-07CH11358. Use of the Advanced Photon Source at Argonne National Laboratory was supported by the U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. In situ DRIFTS was conducted as part of a user project at the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory.

Funders	Funder number
Ames National Laboratory
U.S. Department of Energy	DE‐AC02‐06CH11357
Office of Science
Basic Energy Sciences
Oak Ridge National Laboratory
Iowa State University	DE‐AC02‐07CH11358
Division of Materials Sciences and Engineering

Keywords

B Doping
Frustrated Lewis Pairs
Hydrogen Activation
Hydrogenation
π-Conjugated Networks

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10.1002/anie.202302684

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title = "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. Herein, 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.",

keywords = "B Doping, Frustrated Lewis Pairs, Hydrogen Activation, Hydrogenation, π-Conjugated Networks",

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AU - Li, Meijia

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AU - Popovs, Ilja

AU - Yang, Weiwei

AU - Ivanov, Alexander S.

AU - Kobayashi, Takeshi

AU - Thapaliya, Bishnu P.

AU - Moitra, Debabrata

AU - Yu, Xinbin

AU - Wu, Zili

AU - Yang, Zhenzhen

AU - Dai, Sheng

PY - 2023/7/10

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AB - 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. Herein, 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.

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Construction of Boron- and Nitrogen-Enriched Nanoporous π-Conjugated Networks Towards Enhanced Hydrogen Activation

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