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Mechanochemical synthesis and magnetic properties of the mixed-valent binary silver(I,II) fluorides, Ag$^I{}_2$Ag$^{II}$F$_4$ and Ag$^I$Ag$^{II}$F$_3$
ID
Belak Vivod, Matic
(
Avtor
),
ID
Jagličić, Zvonko
(
Avtor
),
ID
King, Graham
(
Avtor
),
ID
Hansen, Thomas C.
(
Avtor
),
ID
Lozinšek, Matic
(
Avtor
),
ID
Dragomir, Mirela
(
Avtor
)
PDF - Predstavitvena datoteka,
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(3,62 MB)
MD5: C6350165EA732B58BBFF6238239E078B
URL - Izvorni URL, za dostop obiščite
https://pubs.acs.org/doi/10.1021/jacs.4c11772
Galerija slik
Izvleček
Fluoridoargentates(II) represent a fascinating class of silver(II) compounds with structural and magnetic similarities to cuprate superconductors. However, their synthesis is challenging, leaving their properties largely underexplored and hindering the discovery of new phases. This study introduces mechanochemistry as a novel approach for the synthesis of fluoridoargentates(II), avoiding the use of anhydrous HF or elemental fluorine and employing readily available equipment. Notably, ball milling of commercially available precursors successfully produced the long-sought-after first two examples of binary mixed-valent silver(I,II) phases, Ag$^I$$_2$Ag$^{II}$F$_4$ (Ag$_3$F$_4$) and Ag$^I$Ag$^{II}$F$_3$ (Ag$_2$F$_3$). While the Ag$^I$$_2$Ag$^{II}$F$_4$ phase was obtained at room temperature, the Ag$^I$Ag$^{II}$F$_3$ phase is metastable and required milling under cryogenic conditions. Characterization by synchrotron powder X-ray and neutron diffraction revealed that Ag$^I$$_2$Ag$^{II}$F$_4$ crystallizes in the P2$_1$/c space group and is isostructural to β-K$_2$AgF$_4$. In this crystal structure, [Ag$^{II}$F$_2$F$_{4/2}$]$^{2−}$ distorted octahedral units with 4 + 2 coordination, extend parallel to a-crystallographic axis giving a quasi-one-dimensional canted antiferromagnetic character, as shown by magnetic susceptibility. The triclinic perovskite Ag$^I$Ag$^{II}$F$_3$ phase adopts the P$\overline{1}$ space group, is isostructural to AgCuF$_3$ and also shows features of a one-dimensional antiferromagnet. This mechanochemical approach, also successfully applied to synthesize β-K$_2$AgF$_4$, is expected to expand the field of silver(II) chemistry, accelerating the search for silver analogs to cuprate superconductors and potentially extending to other cations in unusual oxidation states.
Jezik:
Angleški jezik
Ključne besede:
fluoridoargentates(II)
,
organic reactions
,
anions
,
chemical structure
,
diffraction
,
magnetic properties
Vrsta gradiva:
Članek v reviji
Tipologija:
1.01 - Izvirni znanstveni članek
Organizacija:
FGG - Fakulteta za gradbeništvo in geodezijo
Status publikacije:
Objavljeno
Različica publikacije:
Objavljena publikacija
Leto izida:
2024
Št. strani:
Str. 30510–30517
Številčenje:
Vol. 146, iss. 44
PID:
20.500.12556/RUL-164686
UDK:
54
ISSN pri članku:
1520-5126
DOI:
10.1021/jacs.4c11772
COBISS.SI-ID:
213097987
Datum objave v RUL:
07.11.2024
Število ogledov:
123
Število prenosov:
37
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Objavi na:
Gradivo je del revije
Naslov:
Journal of the American Chemical Society
Skrajšan naslov:
J. Am. Chem. Soc.
Založnik:
American Chemical Society
ISSN:
1520-5126
COBISS.SI-ID:
512805913
Licence
Licenca:
CC BY 4.0, Creative Commons Priznanje avtorstva 4.0 Mednarodna
Povezava:
http://creativecommons.org/licenses/by/4.0/deed.sl
Opis:
To je standardna licenca Creative Commons, ki daje uporabnikom največ možnosti za nadaljnjo uporabo dela, pri čemer morajo navesti avtorja.
Sekundarni jezik
Jezik:
Slovenski jezik
Ključne besede:
organske reakcije
,
srebrove spojine
,
uklon
,
kemična sestava
,
anioni
,
magnetne lastnosti
,
kemijske reakcije
Projekti
Financer:
ARIS - Javna agencija za znanstvenoraziskovalno in inovacijsko dejavnost Republike Slovenije
Številka projekta:
J2-2496
Naslov:
Iskanje visoko temperaturne superprevodnosti in eksotičnega magnetizma v fluorido argentatih(II)
Financer:
ARIS - Javna agencija za znanstvenoraziskovalno in inovacijsko dejavnost Republike Slovenije
Številka projekta:
P2-0105
Naslov:
Multifunkcijski materiali in naprave: od kvantnega do makro nivoja
Financer:
ARIS - Javna agencija za znanstvenoraziskovalno in inovacijsko dejavnost Republike Slovenije
Številka projekta:
P2-0348
Naslov:
Nove slikovnoanalitske metode
Financer:
EC - European Commission
Program financ.:
H2020
Številka projekta:
101031415
Naslov:
Towards Quantum States of Matter via Chemistry under Extreme Conditions
Akronim:
QMatCh
Financer:
EC - European Commission
Program financ.:
H2020
Številka projekta:
950625
Naslov:
Challenging the Oxidation-State Limitations of the Periodic Table via High-Pressure Fluorine Chemistry
Akronim:
HiPeR-F
Financer:
Drugi - Drug financer ali več financerjev
Program financ.:
Jožef Stefan Institute Director’s Fund
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