Abstract
Our DFT results demonstrate that hydrogen evolution from water catalyzed by a nickel pyradinedithiolate (dcpdt) molecular hydrogen evolution catalyst [Ni II (dcpdt) 2 ] 2− proceeds via the formation of a square-planar nickel(ii) hydride intermediate which is given by unprecedented structural transformation of a doubly reduced triply protonated species [Ni II (dcpdtH 2 )(dcpdtH)] − , afforded as a result of two consecutive ligand-based reductions of [Ni II (dcpdt)(dcpdtH)] − through proton-coupled electron transfer (PCET) pathways.
| Original language | English |
|---|---|
| Pages (from-to) | 635-640 |
| Number of pages | 6 |
| Journal | Dalton Transactions |
| Volume | 48 |
| Issue number | 2 |
| DOIs | |
| Publication status | Published - Jan 1 2019 |
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All Science Journal Classification (ASJC) codes
- Inorganic Chemistry
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Consecutive ligand-based PCET processes affording a doubly reduced nickel pyrazinedithiolate which transforms into a metal hydride required to evolve H 2 . / Koshiba, Keita; Yamauchi, Kosei; Sakai, Ken.
In: Dalton Transactions, Vol. 48, No. 2, 01.01.2019, p. 635-640.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Consecutive ligand-based PCET processes affording a doubly reduced nickel pyrazinedithiolate which transforms into a metal hydride required to evolve H 2
AU - Koshiba, Keita
AU - Yamauchi, Kosei
AU - Sakai, Ken
PY - 2019/1/1
Y1 - 2019/1/1
N2 - Our DFT results demonstrate that hydrogen evolution from water catalyzed by a nickel pyradinedithiolate (dcpdt) molecular hydrogen evolution catalyst [Ni II (dcpdt) 2 ] 2− proceeds via the formation of a square-planar nickel(ii) hydride intermediate which is given by unprecedented structural transformation of a doubly reduced triply protonated species [Ni II (dcpdtH 2 )(dcpdtH)] − , afforded as a result of two consecutive ligand-based reductions of [Ni II (dcpdt)(dcpdtH)] − through proton-coupled electron transfer (PCET) pathways.
AB - Our DFT results demonstrate that hydrogen evolution from water catalyzed by a nickel pyradinedithiolate (dcpdt) molecular hydrogen evolution catalyst [Ni II (dcpdt) 2 ] 2− proceeds via the formation of a square-planar nickel(ii) hydride intermediate which is given by unprecedented structural transformation of a doubly reduced triply protonated species [Ni II (dcpdtH 2 )(dcpdtH)] − , afforded as a result of two consecutive ligand-based reductions of [Ni II (dcpdt)(dcpdtH)] − through proton-coupled electron transfer (PCET) pathways.
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U2 - 10.1039/c8dt04497j
DO - 10.1039/c8dt04497j
M3 - Article
VL - 48
SP - 635
EP - 640
JO - Dalton Transactions
JF - Dalton Transactions
SN - 1477-9226
IS - 2
ER -