Xiao Kang, Xiao Bo-Hao, Li Jian-Xi, Cao Shunsheng, Liu Zhao-Qing
School of Chemistry and Chemical Engineering, Ministry of Education, Guangzhou University, Guangzhou 510006.
Key Laboratory for Clean Energy and Materials, Ministry of Education, Guangzhou University, Guangzhou 510006.
Proc Natl Acad Sci U S A. 2024 Sep 10;121(37):e2409201121. doi: 10.1073/pnas.2409201121. Epub 2024 Sep 6.
Transition metal oxides ion diffusion channels have been developed for ammonium-ion batteries (AIBs). However, the influence of microstructural features of diffusion channels on the storage and diffusion behavior of NH is not fully unveiled. In this study, by using MnCoO spinel as a model electrode, the asymmetric ion diffusion channels of MnCoO have been regulated through bond length optimization strategy and investigate the effect of channel size on the diffusion process of NH. In addition, the reducing channel size significantly decreases NH adsorption energy, thereby accelerating hydrogen bond formation/fracture kinetics and NH reversible diffusion within 3D asymmetric channels. The optimized MnCoO with oxygen vacancies/carbon nanotubes composite exhibits impressive specific capacity (219.2 mAh g at 0.1 A g) and long-cycle stability. The full cell with 3,4,9,10-perylenetetracarboxylic diimide anode demonstrates a remarkable energy density of 52.3 Wh kg and maintains 91.9% capacity after 500 cycles. This finding provides a unique approach for the development of cathode materials in AIBs.
过渡金属氧化物离子扩散通道已被开发用于铵离子电池（AIBs）。然而，扩散通道的微观结构特征对NH储存和扩散行为的影响尚未完全揭示。在本研究中，通过使用锰钴尖晶石作为模型电极，通过键长优化策略调控了锰钴氧化物的不对称离子扩散通道，并研究了通道尺寸对NH扩散过程的影响。此外，减小通道尺寸显著降低了NH吸附能，从而加速了三维不对称通道内氢键形成/断裂动力学以及NH的可逆扩散。具有氧空位/碳纳米管复合材料的优化锰钴氧化物表现出令人印象深刻的比容量（在0.1 A g下为219.2 mAh g）和长循环稳定性。具有3,4,9,10-苝四羧酸二亚胺阳极的全电池表现出52.3 Wh kg的显著能量密度，并且在500次循环后保持91.9%的容量。这一发现为AIBs中阴极材料的开发提供了一种独特的方法。
