Boron Doping‐Induced Ultrahigh Ce <sup>3+</sup> Ratio in Amorphous CeO <sub>2</sub> /GO Catalyst for Low‐Concentration CO <sub>2</sub> Photoreduction
Yanhong Li, Qian Yin, Binbin Jia, Huiqing Wang, Hongfei Gu, Qi Hu, Haosen Yang, Tianqi Guo, Pengfei Hu, Lidong Li, Li‐Min Liu, Lin Guo
Abstract
Abstract Direct utilization of diluted CO 2 enables sustainable CO 2 conversion into valuable products, with reduced CeO 2 emerging as an attractive candidate due to its exceptional redox flexibility. The catalytic efficacy of CeO 2 is intimately tied to the electronic structure of 4 f , yet the persistent challenge lies in maintaining a high and stable concentration of Ce 3+ . In this study, we propose a symmetry‐breaking‐induced amorphization strategy to achieve an exceptionally high Ce 3+ ratio by B doping, which facilitates the reduction of Ce 4+ to Ce 3+ in amorphous CeO 2 . First‐principles calculations and infrared spectroscopy reveal that B doping with three excess electrons induces the formation of planar triangular B–O₃ units by disrupting the original high‐symmetry structure of CeO 2 , facilitating the spontaneous transition to the amorphous phase. Electronic structure analysis confirms that even a modest 7.5% B doping can significantly elevate the Ce 3+ ratio to 85.7%. The resulting amorphous B‐doped CeO 2 /GO shows a remarkable CO 2 ‐to‐CO conversion rate of 249.33 µmol g −1 h −1 (under 15% CO 2 ) and 103.4 µmol g −1 h −1 (under 1% CO 2 ), with 100% selectivity in both cases. This performance highlights how amorphization stabilizes defect states, making amorphous CeO 2 /GO with high Ce 3+ an effective material for CO 2 photoreduction and addressing key challenges in CO 2 capture and utilization.