Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 143, Issue 32, Pages 12809-12816Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c06047
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Funding
- JSPS KAKENHI [JP20H04659, JP17H03037, JP15J09840]
- JST PRESTO [JPMJPR18T7]
- EPSRC [EP/H024107/1, EP/I033459/1, EP/J00135X/1, EP/J015156/1, EP/K021966/1, EP/K023004/1, EP/K038885/1, EP/L015668/1, EP/L023652/1]
- ERC [670467 SMART-POM]
- JSPS through a Research Fellowship for Young Scientists and Overseas Challenge Program for Young Researchers
- EPSRC [EP/I033459/1, EP/L015668/1, EP/J00135X/1, EP/K038885/1, EP/K021966/1, EP/H024107/1, EP/L023652/1, EP/K023004/1, EP/J015156/1] Funding Source: UKRI
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An efficient stepwise synthesis method was developed to discover new heteromultinuclear metal clusters using a robotic workflow, resulting in the discovery of novel nonanuclear tetrametallic oxo clusters with single-molecule magnet properties. These clusters showed higher energy barriers for magnetization reversal compared to the parent cluster, demonstrating the potential for unique properties in designed multistep reactions.
An efficient stepwise synthesis method for discovering new heteromultinuclear metal clusters using a robotic workflow is developed where numerous reaction conditions for constructing heteromultinuclear metal oxo clusters in polyoxometalates (POMs) were explored using a custom-built automated platform. As a result, new nonanuclear tetrametallic oxo clusters {FeMn4} Lu(2)A(2) in TBA(5)[(A-alpha-SiW9O34)(2)FeMn4O2{Lu-(acac)(2)}(2)A(2)] (IIA; A = Ag, Na, K; TBA = tetra-n-butylammonium; acac = acetylacetonate) were discovered by the installation of diamagnetic metal cations A(+) into a paramagnetic {FeMn4}Lu-2 unit in TBA(7)[(A-alpha-SiW9O34)(2)FeMn4O2{Lu(acac)(2)}(2)] (I). POMs IIA exhibited single-molecule magnet properties with the higher energy barriers for magnetization reversal (IIAg, 40.0 K; IINa, 40.3 K; IIK, 26.7 K) compared with that of the parent I (19.7 K). Importantly, these clusters with unique properties were constructed as designed by a step of the predictable sequential multistep reactions with the time-efficient platform.
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