Eine Plattform für die Wissenschaft: Bauingenieurwesen, Architektur und Urbanistik
Eine Plattform für die Wissenschaft: Bauingenieurwesen, Architektur und Urbanistik
First-Principles Study of the Degradation of Perfluorooctanesulfonate and Perfluorobutanesulfonate on a Magnéli Phase Ti4O7 Anode
https://orcid.org/0000-0001-8863-9404
The anodic degradation of perfluorooctanesulfonate (PFOS) and perfluorobutanesulfonate (PFBS) on a Magnéli phase titanium suboxide (Ti4O7) surface was investigated via density functional theory simulations. The adsorption energy on the Ti4O7 cluster surface decreases in the following order: OH• > C4F9SO3 – (PFBS–) ∼ C8F17SO3 – (PFOS–) > H2O. This suggests that OH• formed from water oxidation strongly adsorbs on the Ti4O7 cluster surface. C8F17SO3 – and C4F9SO3 – adsorbed on a model of an OH•-bound Ti4O7 cluster [Ti4O7(OH)] were examined computationally in response to different anodic potentials that were simulated by varying the number of added background charges. This indicates a gradual loss of one electron from C8F17SO3 – and C4F9SO3 – as the background charges increase on Ti4O7(OH). This is accompanied by elongation and eventual breakage of the C–S bond in PFOS and PFBS. The conversion from C8F17SO3 – to C8F17SO3 • by direct electron transfer involves the largest barrier energy (1.21 eV) in the process of PFOS degradation, while the breakage of the C–S bond in C4F9SO3 • is the rate-limiting step of PFBS– degradation (1.49 eV). The first-principles computation here in combination with experimental measurements elucidated the elementary steps involved in the degradation of perfluoroalkyl acids (PFAAs) on a Ti4O7 anode and its dependence on the molecular structures of PFAAs.
First-principles computations elucidated the elementary steps involved in the degradation of perfluoroalkyl acids on a Ti4O7 anode.
First-Principles Study of the Degradation of Perfluorooctanesulfonate and Perfluorobutanesulfonate on a Magnéli Phase Ti4O7 Anode
https://orcid.org/0000-0001-8863-9404
The anodic degradation of perfluorooctanesulfonate (PFOS) and perfluorobutanesulfonate (PFBS) on a Magnéli phase titanium suboxide (Ti4O7) surface was investigated via density functional theory simulations. The adsorption energy on the Ti4O7 cluster surface decreases in the following order: OH• > C4F9SO3 – (PFBS–) ∼ C8F17SO3 – (PFOS–) > H2O. This suggests that OH• formed from water oxidation strongly adsorbs on the Ti4O7 cluster surface. C8F17SO3 – and C4F9SO3 – adsorbed on a model of an OH•-bound Ti4O7 cluster [Ti4O7(OH)] were examined computationally in response to different anodic potentials that were simulated by varying the number of added background charges. This indicates a gradual loss of one electron from C8F17SO3 – and C4F9SO3 – as the background charges increase on Ti4O7(OH). This is accompanied by elongation and eventual breakage of the C–S bond in PFOS and PFBS. The conversion from C8F17SO3 – to C8F17SO3 • by direct electron transfer involves the largest barrier energy (1.21 eV) in the process of PFOS degradation, while the breakage of the C–S bond in C4F9SO3 • is the rate-limiting step of PFBS– degradation (1.49 eV). The first-principles computation here in combination with experimental measurements elucidated the elementary steps involved in the degradation of perfluoroalkyl acids (PFAAs) on a Ti4O7 anode and its dependence on the molecular structures of PFAAs.
First-principles computations elucidated the elementary steps involved in the degradation of perfluoroalkyl acids on a Ti4O7 anode.
First-Principles Study of the Degradation of Perfluorooctanesulfonate and Perfluorobutanesulfonate on a Magnéli Phase Ti4O7 Anode
https://orcid.org/0000-0001-8863-9404
The anodic degradation of perfluorooctanesulfonate (PFOS) and perfluorobutanesulfonate (PFBS) on a Magnéli phase titanium suboxide (Ti4O7) surface was investigated via density functional theory simulations. The adsorption energy on the Ti4O7 cluster surface decreases in the following order: OH• > C4F9SO3 – (PFBS–) ∼ C8F17SO3 – (PFOS–) > H2O. This suggests that OH• formed from water oxidation strongly adsorbs on the Ti4O7 cluster surface. C8F17SO3 – and C4F9SO3 – adsorbed on a model of an OH•-bound Ti4O7 cluster [Ti4O7(OH)] were examined computationally in response to different anodic potentials that were simulated by varying the number of added background charges. This indicates a gradual loss of one electron from C8F17SO3 – and C4F9SO3 – as the background charges increase on Ti4O7(OH). This is accompanied by elongation and eventual breakage of the C–S bond in PFOS and PFBS. The conversion from C8F17SO3 – to C8F17SO3 • by direct electron transfer involves the largest barrier energy (1.21 eV) in the process of PFOS degradation, while the breakage of the C–S bond in C4F9SO3 • is the rate-limiting step of PFBS– degradation (1.49 eV). The first-principles computation here in combination with experimental measurements elucidated the elementary steps involved in the degradation of perfluoroalkyl acids (PFAAs) on a Ti4O7 anode and its dependence on the molecular structures of PFAAs.
First-principles computations elucidated the elementary steps involved in the degradation of perfluoroalkyl acids on a Ti4O7 anode.
First-Principles Study of the Degradation of Perfluorooctanesulfonate and Perfluorobutanesulfonate on a Magnéli Phase Ti4O7 Anode
Li, Lei (Autor:in) / Wang, Yaye (Autor:in) / Huang, Qingguo (Autor:in)
ACS ES&T Water ; 1 ; 1737-1744
13.08.2021
Aufsatz (Zeitschrift)
Elektronische Ressource
Englisch
PFBS , Ti4O7 , PFOS , DFT , degradation
| American Chemical Society | 2024
Ecotoxicological Evaluation of Perfluorooctanesulfonate (PFOS)
| Springer Verlag | 2006
Development of a new material : Monolithic Ti4o7 ebonex ceramic
UB Braunschweig | 2001
Magneli-phase titanium black ceramic, preparation method thereof and inert electrode
| Europäisches Patentamt | 2022