近日，西安交通大学丁书江团队研究了晶格压缩驱动的电子局域化和Ir-O耦合协同实现超低过电位Li-CO₂电池。2025年5月8日出版的《德国应用化学》杂志发表了这项成果。

开发高效的阴极催化剂在改善Li-CO₂电池中的CO₂还原反应（CO₂RR）和CO₂析出反应（CO₂ER）动力学方面起着至关重要的作用。然而，宽带隙绝缘体Li₂CO₃的化学稳定性严重阻碍了CO₂ER。为了应对这一挑战，研究组提出了一种晶格压缩策略，其中电子局域化加速了CO₂RR，从而增强了Ir-O耦合并诱导了低结晶度Li₂CO₃的形成，最终优化了CO₂ER工艺。这种方法使Li-CO₂电池能够实现0.33 V的超低过电位和约88.7%的极高能效。 

此外，即使在运行1100多个小时后，电池仍保持3.3V的稳定充电电位，这是迄今为止报告的最佳性能。通过原位和异位表征结合理论计算，研究组发现晶格压缩会导致配位环境的变化，从而增强电子局域化效应。这加速了Li⁺在催化剂表面附近的迁移，促进了其快速参与CO₂RR。随后，增强的Ir-O偶联调节了Li₂CO₃分子的对称性，降低了它们的结晶度，并最终促进了它们的有效分解。该研究通过晶面工程为高性能双向阴极催化剂的设计提供了新的见解。

附：英文原文

Title: Lattice Compression-Driven Electron Localization and Ir-O Coupling Synergistically Enable Ultra-Low Overpotential Li-CO2 Batteries

Author: Jiyuan Xiao, Limin Liu, Shuyang Ren, Menghang Sun, Bo Wen, Song Xue, Shuai Yang, Xiaofeng Liu, Ning Zhao, Xiaofei Hu, Shujiang Ding, Guorui Yang

Issue&Volume: 2025-05-08

Abstract: Developing efficient cathode catalysts plays a crucial role in improving the CO2 reduction reaction (CO2RR) and CO2 evolution reaction (CO2ER) kinetics in Li-CO2 batteries. However, the chemical stability of the wide-bandgap insulator Li2CO3 severely hinders the CO2ER. To address this challenge, this study proposes a lattice compression strategy in which electronic localization accelerates the CO2RR, thereby enhancing Ir-O coupling and inducing the formation of low-crystallinity Li2CO3, ultimately optimizing the CO2ER process. This approach enables the Li-CO2 battery to achieve an ultra-low overpotential of 0.33 V and an exceptionally high energy efficiency of ~88.7%. Moreover, even after over 1100 hours of operation, the battery maintains a stable charging potential of 3.3 V, representing the best performance reported to date. Through in situ and ex situ characterizations combined with theoretical calculations, we reveal that lattice compression leads to changes in the coordination environment, thereby enhancing electronic localization effects. This accelerates Li+ migration near the catalyst surface, facilitating its rapid participation in CO2RR. Subsequently, the strengthened Ir-O coupling modulates the symmetry of Li2CO3 molecules, reduces their crystallinity, and ultimately promotes their efficient decomposition. This study provides new insights into the design of high-performance bidirectional cathode catalysts through crystal facet engineering.

DOI: 10.1002/anie.202506635

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202506635