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

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

doi:10.1002/anie.202302684

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

Journal Article · Tue May 09 00:00:00 EDT 2023 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.202302684· OSTI ID:1987638

^[1]; Qiu, Liqi ^[2]; Popovs, Ilja ^[1]; Yang, Weiwei ^[1]; Ivanov, Alexander S. ^[1]; Kobayashi, Takeshi ^[3]; Thapaliya, Bishnu P. ^[1]; Moitra, Debabrata ^[2]; Yu, Xinbin ^[1]; Wu, Zili ^[4]; ^[1]; Dai, Sheng ^[5]

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)

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.

View Accepted Manuscript (DOE)

Research Organization:: Ames Laboratory (AMES), Ames, IA (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: AC02-06CH11357; AC02-07CH11358; AC05-00OR22725

OSTI ID:: 1987638

Alternate ID(s):: OSTI ID: 1983439
OSTI ID: 1992720

Report Number(s):: IS-J-11,073

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 28 Vol. 62; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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

Journal Article · Thu May 25 20:00:00 EDT 2023 · Angewandte Chemie · OSTI ID:1983539

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
B doping
frustrated Lewis pairs
hydrogen activation
hydrogenation
π-conjugated networks

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

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