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Alveoli‐Inspired Carbon Cathodes with Interconnected Porous Structure and Asymmetric Coordinated Vanadium Sites for Superior Li‐S Batteries
Angewandte Chemie International Edition ( IF 16.6 ) Pub Date : 2024-04-16 , DOI: 10.1002/anie.202404019
Rui Yan 1 , Zhenyang Zhao 1 , Ran Zhu 1 , Min Wu 1 , Xu Liu 1 , Mohsen Adeli 2 , Bo Yin 1 , Chong Cheng 3 , Shuang Li 1
Affiliation  

Accelerating sulfur conversion catalysis to alleviate the shuttle effect has become a novel paradigm for effective Li‐S batteries. Although nitrogen‐coordinated metal single‐atom (M‐N4) catalysts have been investigated, further optimizing its utilization rate and catalytic activities is urgently needed for practical applications. Inspired by the natural alveoli tissue with interconnected structure and well‐distributed enzyme catalytic sites on the wall for the simultaneously fast diffusion and in‐situ catalytic conversion of substrates, here, we proposed the controllable synthesis of bioinspired carbon cathode with interconnected porous structure and asymmetric coordinated V‐S1N3 sites for efficient and stable Li‐S batteries. The enzyme‐mimetic V‐S1N3 shows asymmetric electronic distribution and high tunability, therefore enhancing in‐situ polysulfide conversion activities. Experimental and theoretical results reveal that the high charge asymmetry degree and large atom radius of S in V‐S1N3 result in sloping adsorption for polysulfide, thereby exhibiting low thermodynamic energy barriers and long‐range stability (0.076% decay over 600 cycles).

中文翻译:

具有互连多孔结构和不对称配位钒位点的肺泡启发碳阴极,用于优质锂硫电池

加速硫转化催化以减轻穿梭效应已成为有效锂硫电池的新范例。尽管氮配位金属单原子(M-N4)催化剂已经得到研究,但实际应用中迫切需要进一步优化其利用率和催化活性。受具有互连结构的天然肺泡组织和壁上分布均匀的酶催化位点的启发,可同时快速扩散和底物的原位催化转化,在此,我们提出了具有互连多孔结构和不对称的仿生碳阴极的可控合成协调V-S1N3位点以实现高效稳定的Li-S电池。酶模拟物 V-S1N3 显示出不对称的电子分布和高可调性,因此增强了原位多硫化物转化活性。实验和理论结果表明,V-S1N3中S的高电荷不对称度和大原子半径导致多硫化物的倾斜吸附,从而表现出低热力学能垒和长程稳定性(600次循环衰减0.076%)。
更新日期:2024-04-16
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