AbstractThe mysterious 21 μm emission feature seen in only 12 C-rich proto-planetary nebulae (PPNe) remains unidentified since its discovery in 1989. Over a dozen materials have been suggested as the carrier candidates while none of them has received general acceptance. We investigate the inorganic carrier candidates by applying the observational constraints of the feature strength and associated features. It is found that: (1) three candidates, TiC clusters, fullerenes with Ti impurity atoms, and SiS₂, are not abundant enough to account for the emission power of the 21 μm band, (2) five candidates, doped-SiC, SiO₂-mantled SiC dust, carbon and silicon mixtures, Fe₂O₃, and Fe₃O₄, all show associated features which are either not detected in the 21 μm sources or detected but with a much lower strength, and (3) FeO, which satisfies the abundance constraints, does not display any associated features which are not seen in the 21 μm sources. Moreover, FeO is more likely to survive in the C-rich environment than Fe₂O₃and Fe₃O₄. Thus FeO seems to be the most plausible one among the inorganic carrier candidates.