title: Ambient Carbon Dioxide Capture Using Boron-Rich Porous Boron Nitride: A Theoretical Study.
abstract: The development of highly efficient sorbent materials for CO2capture under ambient conditions is of great importance for reducing the impact of CO2on the environment and climate change. In this account, strong CO2adsorption on a boron antisite (BN) in boron-rich porous boron nitrides (p-BN) was developed and studied. The results indicated that the material achieved larger adsorption energies of 2.09 eV (201.66 kJ/mol, PBE-D). The electronic structure calculations suggested that the introduction of BNin p-BN induced defect electronic states in the energy gap region, which strongly impacted the adsorption properties of the material. The bonding between the BNdefect and the CO2molecule was clarified, and it was found that the electron donation first occurred from CO2to the BNdouble-acceptor state then, followed by electron back-donation from BNto CO2accompanied by the formation of a BN-C bond. The thermodynamic properties indicated that the adsorption of CO2on the BNdefect to form anionic CO2δ-species was spontaneous at temperatures below 350 K. Both the large adsorption energies and the thermodynamic properties ensured that p-BN with a BNdefect could effectively capture CO2under ambient conditions. Finally, to evaluate the energetic stability, the defect formation energies were estimated. The formation energy of the BNdefects was found to strongly depend on the chemical environment, and the selection of different reactants (B or N sources) would achieve the goal of reducing the formation energy. These findings provided a useful guidance for the design and fabrication of a porous BN sorbent for CO2capture.
authors.affiliation: Key Lab for Micro- and Nano-Scale Boron Nitride Materials in Hebei Province, School of Materials Science and Engineering, Hebei University of Technology , Tianjin 300130, China.
authors.forename: Lanlan
authors.identifier: http://orcid.org/0000-0002-9759-3230
authors.initials: L
authors.lastname: Li
authors.affiliation: Key Lab for Micro- and Nano-Scale Boron Nitride Materials in Hebei Province, School of Materials Science and Engineering, Hebei University of Technology , Tianjin 300130, China.
authors.forename: Yan
authors.initials: Y
authors.lastname: Liu
authors.affiliation: Key Lab for Micro- and Nano-Scale Boron Nitride Materials in Hebei Province, School of Materials Science and Engineering, Hebei University of Technology , Tianjin 300130, China.
authors.forename: Xiaojing
authors.initials: X
authors.lastname: Yang
authors.affiliation: Key Lab for Micro- and Nano-Scale Boron Nitride Materials in Hebei Province, School of Materials Science and Engineering, Hebei University of Technology , Tianjin 300130, China.
authors.forename: Xiaofei
authors.identifier: http://orcid.org/0000-0002-8366-1052
authors.initials: X
authors.lastname: Yu
authors.affiliation: Key Lab for Micro- and Nano-Scale Boron Nitride Materials in Hebei Province, School of Materials Science and Engineering, Hebei University of Technology , Tianjin 300130, China.
authors.forename: Yi
authors.initials: Y
authors.lastname: Fang
authors.affiliation: Key Lab for Micro- and Nano-Scale Boron Nitride Materials in Hebei Province, School of Materials Science and Engineering, Hebei University of Technology , Tianjin 300130, China.
authors.forename: Qiaoling
authors.initials: Q
authors.lastname: Li
authors.affiliation: Key Lab for Micro- and Nano-Scale Boron Nitride Materials in Hebei Province, School of Materials Science and Engineering, Hebei University of Technology , Tianjin 300130, China.
authors.forename: Peng
authors.initials: P
authors.lastname: Jin
authors.affiliation: Key Lab for Micro- and Nano-Scale Boron Nitride Materials in Hebei Province, School of Materials Science and Engineering, Hebei University of Technology , Tianjin 300130, China.
authors.forename: Chengchun
authors.initials: C
authors.lastname: Tang
keywords: Porous boron nitrides; adsorption; boron antisite defect; carbon dioxide capture; density functional calculations