以 Ce3+ 作为色源的颜色可控无机颜料,Inorganic Chemistry

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以 Ce3+ 作为色源的颜色可控无机颜料
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2023-09-13 , DOI: 10.1021/acs.inorgchem.3c01292
Kazuki Yamaguchi ₁ , Yusuke Shobu ₂ , Ryohei Oka ₃ , Toshiyuki Masui ₁

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采用常规固相反应方法合成Ba ₂ RE _{1– x} Ce _x TaO ₆ (RE = La, Gd, Y; 0 ≤ x ≤ 1)颜料，开发环保型微红无机颜料。主体为双钙钛矿型Ba ₂ RETaO ₆（RE：稀土元素），色源为Ce ³⁺。所有Ba ₂ RE _{1– x} Ce _x TaO ₆样品均以单相固溶体形式获得。Ba ₂ RETaO _{6 (RE = La、Ce、Gd 和 Y) 样品的 Rietveld 精化分析表明，RE}³⁺和 O之间的平均键长取决于 RE ³⁺的离子半径，RE– 越短O长度越长，Ce ³⁺周围的晶体场越强。^{Ce 3+}最大4f-5d吸收处的光子能量取决于RE ^{3+位点的加权平均离子半径(}r _{RE )(即Ce}³⁺离子周围的晶体场能)。响应于该现象，随着r _RE值的减小，样品颜色依次变为橙色、红色、粉色和紫色，并且色调角( h °)与其大致线性相关。_{为了验证这一趋势，我们演示了 Ba 2} La _0.5–_y Y _y Ce _0.5 TaO ₆的合成和表征，以获得更红的颜色。正如我们所预期的，在保持高C值的同时获得了更红的颜色。此外，y = 0.1 和 0.2 时的h ° 值与我们的估计非常一致。根据上述结果，通过控制Ce ^{3+周围晶体场的强度和/或Ce}³⁺的浓度，Ba ₂ RE _1–_x Ce _x TaO ₆体系的光吸收波长和吸收强度可以进行更改以调整颜色。

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Color Controllable Inorganic Pigments with Ce3+ as a Color Source

The Ba₂RE_1–xCe_xTaO₆ (RE = La, Gd, Y; 0 ≤ x ≤ 1) pigments were synthesized by a conventional solid-state reaction method to develop environmentally friendly reddish inorganic pigments. The host was the double-perovskite-type Ba₂RETaO₆ (RE: rare-earth elements), and the color source was Ce³⁺. All Ba₂RE_1–xCe_xTaO₆ samples were obtained in a single-phase form as solid solutions. Rietveld refinement analysis of the Ba₂RETaO₆ (RE = La, Ce, Gd, and Y) samples revealed that the average bond length between RE³⁺ and O depends on the ionic radius of RE³⁺, and the shorter the RE–O length, the stronger the crystal field surrounding Ce³⁺. A photon energy at the maximum 4f–5d absorption of Ce³⁺ depended on the weighted average ionic radius (r_RE) at the RE³⁺ site (i.e., the crystal field energy around the Ce³⁺ ions). In response to this phenomenon, the sample color was changed in order to orange, red, pink, and violet with a decrease in the r_RE value, and a hue angle (h°) was roughly linearly related to that. For validation of the tendency, we demonstrated the synthesis and characterization of Ba₂La_0.5–yY_yCe_0.5TaO₆ to obtain a more reddish color. As we exactly expected, a more reddish color was obtained while maintaining a high C value. Furthermore, the h° values for y = 0.1 and 0.2 were in good agreement with our estimation. In light of the above results, by controlling the intensity of the crystal field surrounding Ce³⁺ and/or the concentration of Ce³⁺, the optical absorption wavelength and absorption intensity of the Ba₂RE_1–xCe_xTaO₆ system can be changed to adjust the color.

更新日期：2023-09-13

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