Defect-Regulated Frustrated-Lewis-Pair Behavior of Boron Nitride in Ambient Pressure Hydrogen Activation

Chen, Hao; Xiong, Chuanye; Moon, Jisue; Ivanov, Alexander S.; Lin, Wenwen; Wang, Tao; Fu, Jie; Jiang, De-en; Wu, Zili; Yang, Zhenzhen; Dai, Sheng

doi:10.1021/jacs.2c00343

Defect-Regulated Frustrated-Lewis-Pair Behavior of Boron Nitride in Ambient Pressure Hydrogen Activation

Journal Article · Thu May 19 00:00:00 EDT 2022 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.2c00343· OSTI ID:1874637

^[1]; Xiong, Chuanye ^[2]; Moon, Jisue ^[3]; ^[4]; Lin, Wenwen ^[5]; ^[3]; ^[5]; ^[2]; ^[3]; ^[3]; ^[6]

University of Tennessee, Knoxville, TN (United States); Hunan University, Changsha (China)
University of California, Riverside, CA (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
Zhejiang University, Hangzhou (China)
University of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

We report the construction of heterogeneous frustrated Lewis pairs (FLPs) with performance comparable to or surpassing the homogeneous counterparts in H₂ activation is a long-standing challenge. Herein, sterically hindered Lewis acid (“B” center) and Lewis base (“N” center) sites were anchored within the rigid lattice of highly crystalline hexagonal boron nitride (h-BN) scaffolds. The active sites were created via precision defect regulation during the molten-salt-involved (NaNH₂ and NaBH₄) h-BN construction procedure. The as-afforded h-BN scaffolds achieved highly efficient H₂/D₂ activation and dissociation under ambient pressure via FLP-like behavior, and attractive catalytic efficiency in hydrogenation reactions surpassing the current heterogeneous analogues.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

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

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1874637

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 24 Vol. 144; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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