In fact, clay minerals, especially 2:1 layer-chain palygorskite (Pal) and sepiolite, were developed to be used as inorganic host for sequestering organic molecules to preserve their properties for long time. However, the abundant natural dyes derived from the plants and animals lack the stable hues toward the heating, light and chemicals presenting the poor thermostability and chemical durability. In fact, natural dyes and pigments have been used to decorate prehistoric murals since the dawn of man. Natural dyes and pigments play an important role in our colorful world, which are an integral part of all creatures on the Earth. Based on the synergistic effects between organic and inorganic compositions of hybrid pigments, incorporation of hybrid pigments enhanced the mechanical properties of chitosan composite film with the desired color, and thus the as-prepared hybrid pigments could be served as promising colorant and reinforced materials for coloring and reinforcing of polymeric packing materials. Incorporation of palygorskite and CoNi LDHs obviously enhanced the thermal stability of the organic dyes. What's more, the samples loaded with the sensing dye of methyl orange exhibited intelligent behavior at different pH values (2.5–5.5). The results indicated that the colors of hybrid pigments were determined with the colors of the involved cationic dyes, anionic dyes and CoNi LDHs, which could be accurately designed by adjusting the colors and contents of cationic and anionic dyes. The colors, compositions, and morphologies of hybrid pigments were analyzed by combining with different characterization techniques. In this study, the novel and multicolor organic/inorganic hybrid pigments with the controlled colors were facilely fabricated by wet-method adsorption of cationic dyes using palygorskite followed by one-step loading and intercalation of CoNi layered double hydroxides (CoNi LDHs) with anionic dyes. Maya blue or Maya blue-like pigments are famous for their vivid colors and good environmental stability, but their colors are dependent on the natural or synthetic organic dyes, thus the color system is not complete due to the limited types of organic dyes.
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