Proton Transfer in Molten Lithium Carbonate: Mechanism and Kinetics by Density Functional Theory Calculations

Abstract Using static and dynamic density functional theory (DFT) methods with a cluster model of [(Li2CO3)8H]+, the mechanism and kinetics of proton transfer in lithium molten carbonate (MC) were investigated. The migration of proton prefers an inter-carbonate pathway with an energy barrier of 8.0 ...

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Autores principales:	Xueling Lei, Kevin Huang, Changyong Qin
Formato:	article
Lenguaje:	EN
Publicado:	Nature Portfolio 2017
Materias:	Medicine R Science Q
Acceso en línea:	https://doaj.org/article/8fc11196e4fb4cf2a60162ea717e1db2
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spelling	oai:doaj.org-article:8fc11196e4fb4cf2a60162ea717e1db22021-12-02T16:06:25ZProton Transfer in Molten Lithium Carbonate: Mechanism and Kinetics by Density Functional Theory Calculations10.1038/s41598-017-07726-32045-2322https://doaj.org/article/8fc11196e4fb4cf2a60162ea717e1db22017-08-01T00:00:00Zhttps://doi.org/10.1038/s41598-017-07726-3https://doaj.org/toc/2045-2322Abstract Using static and dynamic density functional theory (DFT) methods with a cluster model of [(Li2CO3)8H]+, the mechanism and kinetics of proton transfer in lithium molten carbonate (MC) were investigated. The migration of proton prefers an inter-carbonate pathway with an energy barrier of 8.0 kcal/mol at the B3LYP/6-31 G(d,p) level, which is in good agreement with the value of 7.6 kcal/mol and 7.5 kcal/mol from experiment and FPMD simulation, respectively. At transition state (TS), a linkage of O–H–O involving O 2p and H 1 s orbitals is formed between two carbonate ions. The calculated trajectory of H indicates that proton has a good mobility in MC, oxygen can rotate around carbon to facilitate the proton migration, while the movement of carbon is very limited. Small variations on geometry and atomic charge were detected on the carbonate ions, implying that the proton migration is a synergetic process and the whole carbonate structure is actively involved. Overall, the calculated results indicate that MC exhibits a low energy barrier for proton conduction in IT-SOFCs.Xueling LeiKevin HuangChangyong QinNature PortfolioarticleMedicineRScienceQENScientific Reports, Vol 7, Iss 1, Pp 1-9 (2017)
institution	DOAJ
collection	DOAJ
language	EN
topic	Medicine R Science Q
spellingShingle	Medicine R Science Q Xueling Lei Kevin Huang Changyong Qin Proton Transfer in Molten Lithium Carbonate: Mechanism and Kinetics by Density Functional Theory Calculations
description	Abstract Using static and dynamic density functional theory (DFT) methods with a cluster model of [(Li2CO3)8H]+, the mechanism and kinetics of proton transfer in lithium molten carbonate (MC) were investigated. The migration of proton prefers an inter-carbonate pathway with an energy barrier of 8.0 kcal/mol at the B3LYP/6-31 G(d,p) level, which is in good agreement with the value of 7.6 kcal/mol and 7.5 kcal/mol from experiment and FPMD simulation, respectively. At transition state (TS), a linkage of O–H–O involving O 2p and H 1 s orbitals is formed between two carbonate ions. The calculated trajectory of H indicates that proton has a good mobility in MC, oxygen can rotate around carbon to facilitate the proton migration, while the movement of carbon is very limited. Small variations on geometry and atomic charge were detected on the carbonate ions, implying that the proton migration is a synergetic process and the whole carbonate structure is actively involved. Overall, the calculated results indicate that MC exhibits a low energy barrier for proton conduction in IT-SOFCs.
format	article
author	Xueling Lei Kevin Huang Changyong Qin
author_facet	Xueling Lei Kevin Huang Changyong Qin
author_sort	Xueling Lei
title	Proton Transfer in Molten Lithium Carbonate: Mechanism and Kinetics by Density Functional Theory Calculations
title_short	Proton Transfer in Molten Lithium Carbonate: Mechanism and Kinetics by Density Functional Theory Calculations
title_full	Proton Transfer in Molten Lithium Carbonate: Mechanism and Kinetics by Density Functional Theory Calculations
title_fullStr	Proton Transfer in Molten Lithium Carbonate: Mechanism and Kinetics by Density Functional Theory Calculations
title_full_unstemmed	Proton Transfer in Molten Lithium Carbonate: Mechanism and Kinetics by Density Functional Theory Calculations
title_sort	proton transfer in molten lithium carbonate: mechanism and kinetics by density functional theory calculations
publisher	Nature Portfolio
publishDate	2017
url	https://doaj.org/article/8fc11196e4fb4cf2a60162ea717e1db2
work_keys_str_mv	AT xuelinglei protontransferinmoltenlithiumcarbonatemechanismandkineticsbydensityfunctionaltheorycalculations AT kevinhuang protontransferinmoltenlithiumcarbonatemechanismandkineticsbydensityfunctionaltheorycalculations AT changyongqin protontransferinmoltenlithiumcarbonatemechanismandkineticsbydensityfunctionaltheorycalculations
_version_	1718385038011138048

Proton Transfer in Molten Lithium Carbonate: Mechanism and Kinetics by Density Functional Theory Calculations

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