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Strong oxidation induced quinone-rich dopamine polymerization onto porous carbons as ultrahigh-capacity organic cathode for sodium-ion batteries
Energy Storage Materials ( IF 18.9 ) Pub Date : 2021-09-03 , DOI: 10.1016/j.ensm.2021.08.043
Chao Huangfu 1 , Zheng Liu 1 , Xiaolong Lu 1 , Qun Liu 1 , Tong Wei 1 , Zhuangjun Fan 1
Affiliation  

Organic cathodes have emerged as promising candidate for sodium ions batteries (SIBs) because of their high theoretical capacity, molecular diversity, and sustainability. However, the inferior rate performance and poor cycle life still restrict their large-scale applications. Herein, a facile strategy for the synthesis of ultrathin quinone-rich polydopamine (PDA) coating which is tightly adhered on 3D porous carbon surface (PC-PDA-APS) is prepared through a superfast (∼1.5 h) heterogeneous nucleation process. Ammonium persulfate (APS) used as initiating agent can not only restrain the self-nucleation of dopamine, but also promote the transformation from bi-hydroxyl to bi-carbonyl with an ultra-high conversion rate up to 81%. Having benefited from the synergistic effect of inter-connective 3D carbon skeleton, ultrathin PDA coating, and ultrahigh quinone content, the PC-PDA-APS exhibits significantly high specific capacity (322 mA h g−1 at 0.1 A g−1), and excellent rate performance (102 mA h g−1 at 10 A g−1). More specially, the combination of DFT calculations and in-situ FTIR spectroscopy verifies the synergistic Na+ storage mechanisms of reversible enol reaction of C=O groups with Na+ and imine groups (R=N-R') with Na+. This research fundamentally provides a structural engineering method for remarkably improving the performance of sodium-organic cathode.



中文翻译:

强氧化诱导富醌多巴胺聚合到多孔碳上作为钠离子电池的超高容量有机阴极

有机正极因其高理论容量、分子多样性和可持续性而成为钠离子电池 (SIB) 的有希望的候选者。然而,较差的倍率性能和较差的循环寿命仍然限制了它们的大规模应用。在此,通过超快(~1.5 小时)非均相成核过程制备了一种用于合成紧密粘附在 3D 多孔碳表面(PC-PDA-APS)上的超薄富含醌的聚多巴胺(PDA)涂层的简便策略。过硫酸铵(APS)作为引发剂,不仅能抑制多巴胺的自成核,还能促进双羟基向双羰基的转化,转化率高达81%。受益于相互连接的3D碳骨架、超薄PDA涂层的协同作用,-1 at 0.1 A g -1)和优异的倍率性能(102 mA hg -1 at 10 A g -1)。更具体地说,结合 DFT 计算和原位FTIR 光谱验证了C=O 基团与 Na +和亚胺基团 (R=N-R') 与 Na +的可逆烯醇反应的协同 Na +存储机制。该研究从根本上为显着提高钠有机正极性能提供了一种结构工程方法。

更新日期:2021-09-09
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