Metallofullerenes present an ideal research object for developing new carbon structures with improved properties under high pressure. In this study, high pressure investigation is realized on metallofullerene derivatives (Gd@C₈₂(morpholine)₇) by applying in situ synchrotron XRD, Raman, and IR spectroscopy, combined with high pressure density functional theory (DFT) calculations. The regulations of multi-configuration morpholine ligands avoid the direct collapse of the carbon cages commonly happened to fullerenes, making the fine structure transformation possible for the first time, including ligand configuration exchange, anisotropic shrinkage of cage, new constructed bonds, and even the encaged metal’s movement with increasing pressure. The charge-transfer principle as the beneath driving force of structural transition is found. These findings demonstrate that multi-configuration ligand maps an innovative strategy for phase transition control of metallofullerenes under high pressure, thus providing deep insight, step by step, into the phase transition mechanism of these hybrid molecular systems on molecular level.

金属富勒烯是开发具有改善的高压性能的新型碳结构的理想研究对象。在这项研究中，对金属富勒烯衍生物（Gd @ C ₈₂（吗啉）₇）进行了高压研究。），方法是应用原位同步加速器XRD，拉曼光谱和红外光谱，并结合高压密度泛函理论（DFT）计算。多构型吗啉配体的规定避免了富勒烯常见的碳笼的直接塌陷，使首次精细结构转变成为可能，包括配体构型交换，笼的各向异性收缩，新构建的键，甚至是包封的金属的运动随着压力的增加。发现电荷转移原理是结构转变的根本驱动力。这些发现表明，多构型配体为高压下金属富勒烯的相变控制提供了创新的策略，从而逐步提供了深刻的见解，