Zhou Jingwen, Xu Zhihang, Cui Kai, Yin Jian-An, Chen Hsiao-Chien, Wang Yunhao, Liu Fu, Wang Tianshuai, Hao Fengkun, Xiong Yuecheng, Wang Cheng, Ma Yangbo, Lu Pengyi, Yin Jinwen, Guo Liang, Meng Xiang, Ye Chenliang, Ming Chen Hao, Zhu Ye, Lu Jian, Fan Zhanxi
Department of Chemistry, City University of Hong Kong, Kowloon, Hong Kong, SAR 999077, China.
Hong Kong Branch of National Precious Metals Material Engineering Research Center (NPMM), City University of Hong Kong, Kowloon, Hong Kong SAR, 999077, China.
Angew Chem Int Ed Engl. 2025 Jan 27;64(5):e202416947. doi: 10.1002/anie.202416947. Epub 2024 Nov 6.
Lithium-carbon dioxide (Li-CO) and Li-air batteries hold great potential in achieving carbon neutral given their ultrahigh theoretical energy density and eco-friendly features. However, these Li-gas batteries still suffer from low discharging-charging rate and poor cycling life due to sluggish decomposition kinetics of discharge products especially LiCO. Here we report the theory-guided design and preparation of unconventional phase metal heteronanostructures as cathode catalysts for high-performance Li-CO/air batteries. The assembled Li-CO cells with unconventional phase 4H/face-centered cubic (fcc) ruthenium-nickel heteronanostructures deliver a narrow discharge-charge gap of 0.65 V, excellent rate capability and long-term cycling stability over 200 cycles at 250 mA g. The constructed Li-air batteries can steadily run for above 150 cycles in ambient air. Electrochemical mechanism studies reveal that 4H/fcc Ru-Ni with high-electroactivity facets can boost redox reaction kinetics and tune discharge reactions towards LiCO path, alleviating electrolyte/catalyst failures induced by the aggressive singlet oxygen from solo decomposition of LiCO.
锂-二氧化碳（Li-CO₂）和锂-空气电池因其超高的理论能量密度和环保特性，在实现碳中和方面具有巨大潜力。然而，由于放电产物尤其是Li₂CO₃的分解动力学缓慢，这些锂-气体电池仍存在充放电速率低和循环寿命差的问题。在此，我们报告了作为高性能Li-CO₂/空气电池阴极催化剂的非常规相金属异质纳米结构的理论指导设计与制备。具有非常规相4H/面心立方（fcc）钌-镍异质纳米结构的组装Li-CO₂电池在250 mA g⁻¹下具有0.65 V的窄充放电间隙、优异的倍率性能和超过200次循环的长期循环稳定性。构建的锂-空气电池在 ambient air中可稳定运行超过150次循环。电化学机理研究表明，具有高电活性面的4H/fcc Ru-Ni可以促进氧化还原反应动力学，并将放电反应调节为Li₂CO₃路径，减轻由Li₂CO₃单独分解产生的活性单线态氧引起的电解质/催化剂失效。
