期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 61, 期 25, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202203114
关键词
Calixarene; Cerium; Host-Guest Complexes; Palladium; Palladium-Oxo Clusters
资金
- German Research Council (DFG) [KO-2288/29-1, KO-2288/26-1, NA 686/15-1, NA 686/8-2]
- Jacobs University
- National Science Center (NCN, Poland) [2018/29/B/ST5/02627]
- Projekt DEAL
We report the discovery of the first two cationic palladium(II)-oxo clusters (POCs) containing f-metal ions, and investigate their physicochemical characterization. The molecular structure of these novel POCs consists of an octahedral {Pd6O12} core capped by eight M-IV ions, forming a cationic, cubic assembly {Pd6O12M8IV}. We also found that these POCs can form host-guest inclusion complexes with 4-sulfocalix[n]arenes, and can be used as pre-catalysts for electrocatalytic CO2 reduction and HCOOH oxidation.
We report on the discovery of the first two examples of cationic palladium(II)-oxo clusters (POCs) containing f-metal ions, [(Pd6O12M8)-O-II{(CH3)(2)AsO2}(16)(H2O)(8)](4+) (M=Ce-IV, Th-IV), and their physicochemical characterization in the solid state, in solution and in the gas phase. The molecular structure of the two novel POCs comprises an octahedral {Pd6O12}(12-) core that is capped by eight M-IV ions, resulting in a cationic, cubic assembly {Pd6O12M8IV}(20+), which is coordinated by a total of 16 terminal dimethylarsinate and eight water ligands, resulting in the mixed Pd-II-Ce-IV/Th-IV oxo-clusters [(Pd6O12M8)-O-II{(CH3)(2)AsO2}(16)(H2O)(8)](4+) (M=Ce, Pd6Ce8; Th, Pd6Th8). We have also studied the formation of host-guest inclusion complexes of Pd6Ce8 and Pd6Th8 with anionic 4-sulfocalix[n]arenes (n=4, 6, 8), resulting in the first examples of discrete, enthalpically-driven supramolecular assemblies between large metal-oxo clusters and calixarene-based macrocycles. The POCs were also found to be useful as pre-catalysts for electrocatalytic CO2-reduction and HCOOH-oxidation.
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