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    Cation-Induced Strategy toward an Hourglass-Shaped Cu<sub>6</sub>I<sub>7</sub><sup>–</sup> Cluster and Its Color-Tunable Luminescence

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    We have designed and synthesized a series of two-dimensional materials featuring with a (3,6)-connected <b>kgd</b> layer, in which an unprecedented anionic Cu<sub>6</sub>I<sub>7</sub><sup>–</sup> cluster was first trapped through a cation-induced synthetic strategy. The emission colors of these cluster-based luminophores gradually shift from blue to yellow as the monovalent cations (Li<sup>+</sup>, Na<sup>+</sup>, NH<sub>4</sub><sup>+</sup>, K<sup>+</sup>, TEA<sup>+</sup>) located between the neighboring layers changed. SCXRD analyses discover that the variation of the emission may be attributed to the transformation of the hourglass-shaped Cu<sub>6</sub>I<sub>7</sub><sup>–</sup> cluster. The bright, tunable, and broad luminescent emissions make them promising candidates as phosphors for light-emitting diodes (LEDs). Particularly, compound <b>1-TEA</b> emitting intensive yellow light with high luminescence quantum efficiency (QY = 79.9%) shows extremely high thermal, pH, organic solvent, and mechanical photostabilities. By employing it as a yellow phosphor, we fabricate a series of white lighting materials with high color rendering index (CRI)
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