Lanthanide metal-organic frameworks (Ln-MOFs) exhibit distinctive emission spectra and prolonged luminescent lifetimes, thereby offering a unique platform for the advancement of solid-state photoluminescence (PL) materials. However, the mismatch between the energy levels of metal ions and organic ligands leads to a weak PL emission. Herein, this study presents a pressure-treated strategy aimed at achieving efficient green PL in Tb₂(BDC)₃(H₂O)₄ MOF. Compared to the initial intensity, the PL intensity is enhanced eightfold below 3.1 GPa. Intriguingly, the PL intensity of pressure-treated sample is amplified by 2.5-fold compared to the initial state, and the green emission monochromaticity is maintained. Experiments and calculations reveal that the enhanced hydrogen bonds are retained to the ambient conditions after pressure treatment. They lock the conjugated configuration formed between the planes of carboxyl group and benzene ring, facilitating the intersystem crossing. The reduced distances between metal ions and organic ligands drive the ligand-to-metal energy transfer process. This finding provided significant insights into structure-property relationship of Tb₂(BDC)₃(H₂O)₄, offering a new platform for boosting emission enhancement in Ln-MOFs.

Keywords: Green‐light emission; Ligand‐to‐metal energy transfer; Metal‐organic frameworks; Pressure‐treated engineering.

© 2025 Wiley‐VCH GmbH.

镧系金属有机框架（Ln-MOFs）具有独特的发光光谱和延长的荧光寿命，从而为固态光致发光（PL）材料的发展提供了一个独特平台。然而，金属离子与有机配体能级之间的不匹配导致了较弱的PL发射。在此研究中，提出了一种压力处理策略，旨在实现Tb₂(BDC)₃(H₂O)₄ MOF高效绿色PL。与初始强度相比，在低于3.1 GPa的压力下PL强度提高了八倍。有趣的是，经过压力处理的样品的PL强度比初始状态增加了2.5倍，并且绿光发射单色性得以保持。实验和计算表明，增强的氢键在压力处理后保留到常温条件，它们锁定了羧基平面与苯环之间形成的共轭构型，促进了系间穿越。金属离子与有机配体之间的距离减小驱动了配体到金属的能量转移过程。这一发现为Tb₂(BDC)₃(H₂O)₄的结构-性能关系提供了重要见解，为提升Ln-MOFs发射增强提供了一个新的平台。

关键词： 绿色发光；配体到金属能量转移；金属有机框架；压力处理工程。

© 2025 Wiley‐VCH GmbH.