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Ni12 tetracubane cores with slow relaxation of magnetization and efficient charge utilization for photocatalytic hydrogen evolution.

ABSTRACT: We report two Ni12 multicubane topologies enclosed in the polyanions [Ni12(OH)9(WO4)3(PO4)(B-α-PW9O34)3]21-{Ni12W30} and [Ni12(OH)9(HPO4)3(PO4)(B-α-PW9O34)(A-α-PW9O34)2]21-{Ni12W27} that magnetically behave as Ni12 units clearly distinguishing them from typical Ni4 cubanes as shown by magnetic studies together with high field and frequency electron paramagnetic resonance (HFEPR). Beyond the unprecedented static properties, {Ni12W30} shows the unusual coexistence of slow relaxation of the magnetization and a diamagnetic ground state (S = 0), providing the unique opportunity of studying the essentially elusive magnetic relaxation behavior in excited states. The cubane-topology dependent activity of {Ni12W30} and {Ni12W27} as homogeneous HER photocatalysts unveils the structural key features significant for the design of photocatalysts with efficient charge utilization exemplified by high quantum yields (QY) of 10.42% and 8.36% for {Ni12W30} and {Ni12W27}, respectively.

SUBMITTER: Tanuhadi E 

PROVIDER: S-EPMC9686624 | biostudies-literature | 2022 Nov

REPOSITORIES: biostudies-literature

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Ni<sub>12</sub> tetracubane cores with slow relaxation of magnetization and efficient charge utilization for photocatalytic hydrogen evolution.

Tanuhadi Elias E   Cano Joan J   Batool Samar S   Cherevan Alexey A   Eder Dominik D   Rompel Annette A  

Journal of materials chemistry. C 20221018 45

We report two Ni<sub>12</sub> multicubane topologies enclosed in the polyanions [Ni<sub>12</sub>(OH)<sub>9</sub>(WO<sub>4</sub>)<sub>3</sub>(PO<sub>4</sub>)(B-α-PW<sub>9</sub>O<sub>34</sub>)<sub>3</sub>]<sup>21-</sup>{Ni<sub>12</sub>W<sub>30</sub>} and [Ni<sub>12</sub>(OH)<sub>9</sub>(HPO<sub>4</sub>)<sub>3</sub>(PO<sub>4</sub>)(B-α-PW<sub>9</sub>O<sub>34</sub>)(A-α-PW<sub>9</sub>O<sub>34</sub>)<sub>2</sub>]<sup>21-</sup>{Ni<sub>12</sub>W<sub>27</sub>} that magnetically behave as Ni<sub>12</sub>  ...[more]

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