dc.contributor.author |
Alberto, Roger |
|
dc.contributor.author |
Iannuzzi, Marcella |
|
dc.contributor.author |
Gurdal, Yeliz |
|
dc.contributor.author |
Probst, Benjamin |
|
dc.date.accessioned |
2023-03-13T07:15:38Z |
|
dc.date.available |
2023-03-13T07:15:38Z |
|
dc.date.issued |
2019-11 |
|
dc.identifier.citation |
Alberto, R., Iannuzzi, M., Gurdal, Y., & Probst, B. (2019). [Coᴵᴵ(BPyPy₂COH)(OH₂)₂]²⁺: A Catalytic Pourbaix Diagram and AIMD Simulations on Four Key Intermediates. CHIMIA, 73(11), 906. https://doi.org/10.2533/chimia.2019.906 |
tr_TR |
dc.identifier.issn |
0009-4293 |
|
dc.identifier.uri |
http://openacccess.atu.edu.tr:8080/xmlui/handle/123456789/4151 |
|
dc.identifier.uri |
http://dx.doi.org/10.2533/chimia.2019.906 |
|
dc.description |
WOS indeksli yayınlar koleksiyonu. / WOS indexed publications collection. |
tr_TR |
dc.description.abstract |
Proton reduction by [Co-II(BPyPy2COH)(OH2)(2)](2+)(BPyPy2COH = [2,2'-bipyridin]-6-yl-di[pyridin-2-yllmethanol) proceeds through two distinct, pH-dependent pathways involving proton-coupled electron transfer (PCET), reduction and protonation steps. In this account we give an overview of the key mechanistic aspects in aqueous solution from pH 3 to 10, based on electrochemical data, time-resolved spectroscopy and ab initio molecular dynamics simulations of the key catalytic intermediates. In the acidic pH branch, a PCET to give a Co-III hydride is followed by a reduction and a protonation step, to close the catalytic cycle. At elevated pH, a reduction to Co-I is observed, followed by a PCET to a Co-II hydride, and the catalytic cycle is closed by a slow protonation step. In our simulation, both Co-I and Co-II-H feature a strong interaction with the surrounding solvent via hydrogen bonding, which is expected to foster the following catalytic step. |
tr_TR |
dc.language.iso |
en |
tr_TR |
dc.publisher |
CHIMIA / SWISS CHEMICAL SOCIETY |
tr_TR |
dc.relation.ispartofseries |
2019;Volume: 73 Issue: 11 |
|
dc.subject |
Ab initio Molecular dynamics |
tr_TR |
dc.subject |
Cobalt polypyridyl |
tr_TR |
dc.subject |
Density functional theory |
tr_TR |
dc.subject |
Pourbaix diagram |
tr_TR |
dc.subject |
Proton coupled electron transfer |
tr_TR |
dc.title |
[Co-II(BPyPy2COH)(OH2)(2)](2+) A Catalytic Pourbaix Diagram and AIMD Simulations on Four Key Intermediates |
tr_TR |
dc.type |
Article |
tr_TR |