European Journal of Inorganic Chemistry p. 2508 - 2516 (2011)
Update date:2022-08-11
Topics:
Michalowski, Tomasz
Malinowski, Przemyslaw J.
Derzsi, Mariana
Mazej, Zoran
Jaglicic, Zvonko
Leszczyanski, Piotr J.
Grochala, Wojciech
Dark brown AgI2AgII(SO3F) 4, known for over 30 years, is the first known example of four well-characterized mixed-valent (1+/2+) compounds of silver. It crystallizes in the monoclinic space group, P21/c, with a = 5.33670(19) A, b = 12.9486(4) A, c = 19.5976(7) A, β = 100.6407(13)°, V = 1330.95(8) A3, Z = 4 and dcalcd. = 3.59 gcm -3. Its chemical formula is best written as [AgI 2(SO3F)]+[AgII(SO3F) 3]-. AgII centres form 1D chains linked through OSO bridges that result in pronounced antiferromagnetic coupling with T N = 225 K and a superexchange coupling constant (J) of -7.5 meV per pair of coupled AgII cations. Ligand environments around Ag I and AgII differ substantially, which suggests a genuine mixed- (i.e., localized) and not intermediate-valent (i.e., delocalized) character of the title compound. Indeed, electronic absorption is not observed up to 7500 cm-1, so the intervalence charge-transfer transition across the electronic band gap must fall above 0.8 eV. The compound is stable up to a mere 75 °C, which marks the onset of its thermal decomposition to AgISO3F and the SO3F′· radical. AgI2AgII(SO3F)4 is, after AgSO4, the second-known 1D antiferromagnetic semiconducting oxa derivative of AgII. Dark brown monoclinic Ag3(SO 3F)4 shows 1D antiferromagnetism with an anomalously large superexchange coupling constant of -7.5 meV per pair of paramagnetic Ag II cations (for the spin density see the figure). One-dimensional [AgIISO3F]+ chains, linked through fluorosulfate anions into [AgII(SO3F)3] - sheets, constitute characteristic structural features responsible for magnetic behaviour.
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