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新能源	锂锂矿锂化合物金属锂镍镍矿镍铁精炼镍镍盐高冰镍 MHP 钴电解钴钴粉氯化钴四氧化三钴硫酸钴钴中间品氧化钴碳酸钴钴酸锂锰锰矿电解锰电池级硫酸锰锂电正负极三元前驱体磷酸铁正极材料石油焦针状焦包覆沥青人造石墨硅碳负极硅氧负极硅

分子转子动态自适应天线效应诱导的具有多色发光切换的智能镧系金属-有机框架

2025-06-05 16:36:35 来源：上海稀土协会责任编辑：潘利军

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镧系元素发射器因其半宽窄、光色纯、斯托克斯位移大、发光寿命长、吸光能力强等诸多优点而受到广泛关注。此外，4fn的屏蔽效果三价 Ln（III）离子的电子层导致电子激发到高能4f轨道几乎不受配体的影响。因此，镧系元素发射器可以显示明亮清晰的指纹发射线，而不是宽阔的发射峰。大多数有机配体的三重态寿命极短，并且它们与镧系元素离子的能级匹配不佳，阻碍了光亮镧系元素发射器的高效构建。迄今为止，镧系元素复合发射器的构建主要依赖于具有平面共轭和刚性结构的“静态”有机荧光团作为天线。尽管已经设计了多种刚性荧光基团作为天线，但固定的构型和刚性结构导致这些荧光基团的能级精确，很难被外界刺激轻易改变，从而无法有效构建自适应动态镧系元素络合发射器。2009 年，Tang 等人发现含有分子转子结构的有机荧光团的荧光随着分子聚集的增加而逐渐增强，并提出了聚集诱导发射（AIE）。具有分子转子和扭曲结构的 AIE 发光体（AIEgens）的光学行为和能级与其分子构型和转子的运动密切相关。显然，外部环境对AIEgens的轻微扰动很容易导致分子转子的运动程度或扭曲的快速变化，从而引起其能级的动态变化。2022年，Bu等人报道了一种柔性Zn-MOF（NKU-121），由构象适应性强的 AIEgen（3-TPPA，三（4-（吡啶-3-基）苯基）胺）和 Zn（II）离子组装而成。NKU-121 由 3-TPPA 配体构建，具有分子转子结构，在温度、压力和溶剂等外部刺激下实现全色范围动态荧光颜色调节。

以动态分子转子作为有机连接剂，通过交替连接具有出色光物理特性的镧系离子或镧系元素簇和指纹发射光谱作为二级建筑单元（SBU）来自组装镧系金属有机框架（Ln-MOFs），无疑将为构建新型人工智能变色材料开辟新蓝图。迄今为止，分子转子配体通常只像传统的平面刚性配体一样充当静态天线，以敏化镧系元素 MOF 结构内镧系离子的特征发光。2024 年，我们的团队使用 AIEgen 配体作为传统的静态天线构建了一系列镧系元素 MOF 发射器，并探索了这些镧系元素 MOF 发射器对 H 的智能传感性能2O2和 Al3+离子。显然，动态分子转子在受到外界刺激后分子构象的变化或扭曲程度会导致其能级发生显著变化，从而具有比静态配体更丰富的动态发光行为。结构内分子转子的扭曲程度和构象变化所引起的能级变化，可以实现对不同能级的镧系离子的自适应“天线效应”，从而有效地构建一个响应外部刺激的人工智能变色龙。此外，动态分子转子天线还可以调节共掺杂镧系元素离子之间的能量转移路径，轻松实现镧系元素 MOF 的多色或全色发射。此外，将动态分子转子配体引入晶体发光框架材料的孔隙中，有望有助于构建更敏感和更直观的新型光学传感器。这主要是因为多孔框架结构为分子转子配体的旋转提供了一定量的自由空间，使它们更容易受到靶分子或外部刺激引起的微扰动，并表现出明亮、高度可见和快速的发光变化。

作为最经典的 AIEgens 之一，三苯胺（TPA）衍生物配体具有很高的对称性，已成为构建柔性发光MOF的首选。此外，具有螺旋桨构型的 TPA 衍生配体的扭曲程度和分子构象很容易被外部刺激改变。上述高度敏感的畸变角和分子构象变化也会导致能级的变化。在此，选择 4,4,4-三苯胺三羧酸盐（TPA-COOH）作为动态分子转子配体，构建智能Ln-MOFs，它可以适应温度变化并表现出发光转换行为。用于调节 Ln-MOF 能量转移（ET）途径的 TPA-COOH 天线和混合金属掺杂策略可以实现出色的多色发射、上转换发光、高阶多重智能防伪、商业钆盐纯度监测、对特定抗生素和氨基酸的智能光响应。具有分子转子接头和交错和反平行排列的层状 Ln-MOF 在强酸性和强碱性水溶液中表现出高稳定性。环境温度的变化会改变 TPA-COOH 的运动和扭曲程度，从而产生自适应天线效应，以选择性地匹配Tb（III）或 Eu（III）的能级欧盟x结核病（1−x）-MOF （MOFs）（x = 0.01–0.90）并实现循环温控发光切换行为和高阶多重防伪加密技术。此外，ET 通路欧盟x结核病（1−x）– MOF探索了 Tb（III）离子作为能量介质的机制，并通过精确控制结构中 Tb（III）和 Eu（III）离子的比例来研究。总值0.99欧盟0.01-MOFEu（III）离子含量极低时呈现亮红色发光，Eu（III）离子的特征发射峰强度总值x欧盟（1−x）-MOF （MOFs）与 1%–9% 的 Eu（III）离子含量呈线性关系（斜率≈ 2298.7），从而能够轻松鉴定不同制造商的钆盐中的 Eu（III）离子杂质。具有优异光物理特性的 Tb-MOF 和 Eu-MOF 对极低含量的特异性抗生素和氨基酸表现出高度敏感和视觉智能的光反应，并且通过试纸观察到由于上述智能光响应过程引起的发光转换。据我们所知，这项工作是首次利用 TPA-COOH 连接子的自适应天线效应来构建可以响应温度的 AI 变色龙。此外，详细研究了 TPA-COOH 配体和镧系元素离子之间的 ET 途径，推进了镧系元素发射器发光机制的研究和用于一体化应用的镧系元素MOF的构建。

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[ SQL ] SELECT * FROM `tb_cate` WHERE `pid` = 19 AND ( `id` < 3871 AND `id` NOT IN (25,3243,3244) ) ORDER BY `sortid` ASC [ RunTime:0.002443s ]
[ SQL ] SELECT * FROM `tb_cate` WHERE `pid` = 15 AND ( `id` < 3871 AND `id` NOT IN (25,3243,3244) ) ORDER BY `sortid` ASC [ RunTime:0.002439s ]
[ SQL ] SELECT * FROM `tb_cate` WHERE `pid` = 16 AND ( `id` < 3871 AND `id` NOT IN (25,3243,3244) ) ORDER BY `sortid` ASC [ RunTime:0.002502s ]
[ SQL ] SELECT * FROM `tb_cate` WHERE `pid` = 17 AND ( `id` < 3871 AND `id` NOT IN (25,3243,3244) ) ORDER BY `sortid` ASC [ RunTime:0.002436s ]
[ SQL ] SELECT * FROM `tb_cate` WHERE `pid` = 3 AND ( `id` < 3871 AND `id` NOT IN (25,3243,3244) ) ORDER BY `sortid` ASC [ RunTime:0.002448s ]
[ SQL ] SELECT * FROM `tb_advert` WHERE `id` = 48 LIMIT 1 [ RunTime:0.000429s ]
[ SQL ] SELECT * FROM `tb_advert` WHERE `id` = 49 LIMIT 1 [ RunTime:0.000402s ]
[ SQL ] SELECT * FROM `tb_advert` WHERE `id` = 50 LIMIT 1 [ RunTime:0.000390s ]
[ SQL ] SELECT * FROM `tb_para` WHERE `id` = 1 LIMIT 1 [ RunTime:0.000545s ]

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