Shu Shi, Zi-Da Ma, Yu-Xia Li, Shi-Chao Qi and Lin-Bing Sun*,
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引用次数: 0
摘要
开发高性能吸附剂对于吸附分离至关重要。传统的吸附剂由于其固定的表面特性,在兼顾选择性吸附和高效解吸方面存在局限性。在这项工作中,我们通过瓶中船方法在 Y 沸石中原位合成了螺吡喃(SP),从而构建了基于可见光响应的吸附剂,用于可控 CO 吸附。这避免了绝大多数通过紫外线调节吸附容量的系统所存在的缺点。SP 分子可以在 Y 沸石中发生可逆的异构化,在黑暗中呈现美蓝(MC)态,而在可见光刺激下则恢复到 SP 态。研究结果表明,MC 向 SP 的异构化可使 CO 吸附能力提高 34%。密度泛函理论模拟显示,由于 MC 与 CO 的结合能更高,因此 MC 比 SP 更容易捕获 CO 分子。我们进一步证明,异构化诱导的可调吸附容量可在循环过程中保持而不会降解。
Spiropyran-Incorporated Y Zeolite: A Visible-Light-Responsive System for Controllable CO adsorption
The development of high-performance adsorbents is vital for adsorptive separation. Conventional adsorbents have limitations in combining selective adsorption and efficient desorption due to their fixed surface properties. In this work, we have constructed spiropyran (SP)-based visible-light-responsive adsorbents for controllable CO adsorption by synthesizing SP in situ in Y zeolite via the ship-in-the-bottle method. This avoids the drawbacks associated with the vast majority of systems that modulate adsorption capacity by UV light. SP molecules can undergo reversible isomerization within the Y zeolite, which exhibit the merocyanine (MC) state in the dark and revert to the SP form upon visible light stimulation. The results show that the isomerization of MC to SP leads to a tunable CO adsorption capacity of up to 34%. Simulations performed by density functional theory reveal that MC is more likely to trap CO molecules than SP due to its higher binding energy with CO. We further demonstrate that the isomerization-induced tunable adsorption capacity can be maintained during cycles without degradation.