Following recent investigation in the ternary system Sr–Al–Pt led to the discovery of SrAl5Pt3 which crystallizes in the orthorhombic YNi5Si3 type (Pnma) structure. Interestingly, only two more aluminum representatives, CeAl5Pt3 and EuAl5Pt3, have been reported to adopt this structure type. Therefore, we decided to investigate the existence range of compounds adopting the YNi5Si3 type structure. Besides the already known Sr, Ce and Eu members, the series could be extended to Ca, Y and La–Nd as well as Sm–Er. All compounds were synthesized from the elements and characterized by powder X-ray diffraction. While for CaAl5Pt3 and LaAl5Pt3 also the respective M2Al16Pt9 members were observed, the other compounds could be obtained either as X-ray pure materials or with small amounts of Al3Pt2 as a side phase. The structure of ErAl5Pt3 could be refined from single crystal data, verifying that also the small rare-earth elements adopt the YNi5Si3 type structure. Selected members of the series were furthermore characterized by magnetization and susceptibility measurements. Since YAl5Pt3 could be obtained as a phase pure material and exhibits no paramagnetic behaviour it was investigated by 27Al MAS NMR investigations. Also, XPS measurements were conducted on this compound to gain an insight into the charge distribution. Finally, quantum-chemical calculations supported the NMR measurements and gave an insight into the chemical bonding and the charge distribution.
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