Crystallization of RE2(OH)2CO3SO4.nH2O as a new family of layered hydroxides (RE = Gd−Lu lanthanides and Y), derivation of RE2O2SO4, photoluminescence and optical thermometry

Fan Li; Zhenqi Song; Zhiyuan Pan; Sihan Feng; Qi Zhu; Ji-Guang Li

doi:10.1016/j.jre.2023.07.008

Article Crystallization of RE2(OH)2CO3SO4.nH2O as a new family of layered hydroxides (RE = Gd−Lu lanthanides and Y), derivation of RE2O2SO4, photoluminescence and optical thermometry

Fan Li (Northeastern University) ; Zhenqi Song (Northeastern University) ; Zhiyuan Pan (Northeastern University) ; Sihan Feng (Northeastern University) ; Qi Zhu (Northeastern University) ; Ji-Guang Li (Research Center for Electronic and Optical Materials/Optical Materials Field/Polycrystalline Optical Material Group, National Institute for Materials Science)

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Fan Li, Zhenqi Song, Zhiyuan Pan, Sihan Feng, Qi Zhu, Ji-Guang Li. Crystallization of RE2(OH)2CO3SO4.nH2O as a new family of layered hydroxides (RE = Gd−Lu lanthanides and Y), derivation of RE2O2SO4, photoluminescence and optical thermometry. JOURNAL OF RARE EARTHS. 2023, 42 (8), 1496-1506. https://doi.org/10.1016/j.jre.2023.07.008

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Layered rare-earth hydroxides (LREHs) draw wide research interest because of their peculiar crystal structure, rich interlayer chemistry and abundant functionality of the RE element, but are limited to the two categories of RE2(OH)5A·nH2O (A: typical of Cl- or NO3-) and RE2(OH)4SO4·nH2O. On the other hand, RE2O2SO4 attracted attention for large-capacity oxygen storage, low-temperature magnetism and luminescence, whose preparation mostly involves toxic SOx gases and/or complicated procedures. This study produced RE2(OH)2CO3SO4·nH2O as a new family of LREHs (RE = Gd-Lu lanthanides and Y) via hydrothermal reaction, from which phase-pure RE2O2SO4 was derived via subsequent annealing at 800 °C in air without the involvement of SOx. The compounds were thoroughly characterized to reveal the intrinsic influence of lanthanide contraction (RE3+ radius) on crystal structure, thermal behavior (dehydroxylation/decarbonation/desulfurization), vibrational property and crystallite morphology. Analyzing the photoluminescence of Eu3+ and Sm3+ in the Gd2O2SO4 typical host found that the 617 nm (Eu3+, λex = 275 nm) and 608 nm (Sm3+, λex = 407 nm) main emissions can retain as high as ~79.6 and 85.5% of their room-temperature intensities at 423 K, with activation energies of ~0.19 and 0.21 eV for thermal quenching, respectively. Application also indicated that both the phosphors have the potential for optical temperature sensing via the fluorescence intensity ratio (FIR) technology, whose maximum relative sensitivity reached ~2.70% K−1 for Eu3+ and 1.73% K−1 for Sm3+ at 298 K.

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