通过压力处理工程在 Nonemission MOF-2 中增亮蓝色光致发光,Advanced Materials

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通过压力处理工程在 Nonemission MOF-2 中增亮蓝色光致发光
Advanced Materials ( IF 27.4 ) Pub Date : 2023-03-24 , DOI: 10.1002/adma.202211729
Ting Zhang ₁ , Xue Yong ₂ , Jingkun Yu ₃ , Yixuan Wang ₁ , Min Wu ₁ , Qing Yang ₁ , Xuyuan Hou ₁ , Zhaodong Liu ₁ , Kai Wang ₁ , Xinyi Yang ₁ , Siyu Lu ₃ , Bo Zou ₁

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与新材料的合成同样重要的是，操纵新的结构配置可以赋予现有材料全新的功能特性，这也是合成界的核心目标之一。在这方面，在非发射材料中触发光致发光 (PL) 的压力诱导发射 (PIE) 是一种新兴的刺激响应智能材料技术。然而，在 PIE 范例中，在环境条件下收获明亮的 PL 仍然难以实现。在此，在初始非发射 Zn(BDC)(DMF)(H ₂O) (MOF-2)，在压力下在 455 nm 处显示明亮的蓝色发射。有趣的是，亮蓝色 PL 具有高达 70.4% 的出色光致发光量子产率，在从 16.2 GPa 减压后，前所未有地保留在环境条件下。详细的结构分析与密度泛函理论计算相结合表明，氢键协同效应将连接转子的旋转势垒从最初的 0.91 eV mol ^{-1强大地提升至 3.87 eV mol}^-1通过压力处理。完全释放压力后，下行旋转自由度开启 MOF-2 的 PL。这是第一个将 PIE 收集到环境条件的案例。这些发现提供了一个新平台，用于创建基于最初无排放对应物的高性能 PL 材料的有前途的替代品。

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Brightening Blue Photoluminescence in Nonemission MOF-2 by Pressure Treatment Engineering

As equally essential as the synthesis of new materials, maneuvering new structure configurations can endow the brand-new functional properties to existing materials, which is also one of the core goals in the synthesis community. In this respect, pressure-induced emission (PIE) that triggers photoluminescence (PL) in nonemission materials is an emerging stimuli-responsive smart materials technology. In the PIE paradigms, harvesting bright PL at ambient conditions, however, has remained elusive. Herein, a remarkable PIE phenomenon is reported in initially nonemission Zn(BDC)(DMF)(H₂O) (MOF-2), which shows bright blue-emission at 455 nm under pressure. Intriguingly, the bright blue PL with an excellent photoluminescence quantum yield up to 70.4% is unprecedentedly retained to ambient conditions upon decompression from 16.2 GPa. The detailed structural analyses combined with density functional theory calculations reveal that hydrogen bonding cooperativity effect elevates powerfully the rotational barrier of the linker rotor to 3.87 eV mol⁻¹ from initial 0.91 eV mol⁻¹ through pressure treatment. The downgrade rotational freedom turns on PL of MOF-2 after releasing pressure completely. This is the first case of harvesting PIE to ambient conditions. These findings offer a new platform for the creation of promising alternatives to high-performance PL materials based on initially nonemission counterparts.

更新日期：2023-03-24

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