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用于提升锂硫电池反应动力学和循环稳定性的金属Sn/N、B共掺杂碳基体的三相界面工程

Triphasic Interface Engineering with Metallic Sn/N, B Co-Doped Carbon Matrix for Boosting Reaction Kinetics and Cycling Stability in Lithium-Sulfur Batteries.

作者信息

Park Gwan Hyeon, Mangishetti Sandya Rani, Lim Won-Gwang, Ji Junhyuk, Jeong Yun Ho, Cho Jeongbin, Bae Hansol, Jo Changshin, Kim Won Bae

机构信息

Department of Chemical Engineering, Pohang University of Science and Technology (POSTECH), 77 Cheongam-ro, Nam-gu, Pohang-si, Gyeongsangbuk-do, 37673, Republic of Korea.

Department of Chemical and Biomolecular Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-Ro, Yuseong-Gu, Daejeon, 34141, Republic of Korea.

出版信息

Small. 2025 Jun 27:e2503534. doi: 10.1002/smll.202503534.

Abstract

Lithium-sulfur batteries undergo solid-liquid-solid phase transitions based on a dissolution-deposition reaction mechanism. To effectively suppress the shuttling of soluble polysulfides, catalysts should be incorporated into the cathode to enhance both the adsorption and conversion processes. The formation of a triphasic interface among the catalyst, conductive material, and electrolyte plays a key role in facilitating these reactions. In this study, a composite catalyst (Sn@NBGNs-CNTs), consisting of metallic tin microparticles anchored on nitrogen and boron co-doped graphene nanosheets and partially exfoliated carbon nanotubes, is synthesized as a sulfur host via a simple method. This structure effectively anchors polysulfides at the interface and provided abundant active sites to accelerate redox reaction kinetihcs. As a result, it facilitated charge transfer and polysulfide transport at the interface, leading to an increase in the nucleation-growth rate constants of LiS as determined using the critical deposition voltage from the potentiostatic intermittent titration technique. Consequently, the electrode exhibits excellent cycling stability, retaining 93% of its initial capacity after 350 cycles at 1 C with an extremely low-capacity decay rate of 0.003% per cycle.

摘要

锂硫电池基于溶解-沉积反应机理经历固-液-固相变。为了有效抑制可溶性多硫化物的穿梭,应将催化剂引入阴极以增强吸附和转化过程。催化剂、导电材料和电解质之间三相界面的形成在促进这些反应中起关键作用。在本研究中,通过一种简单方法合成了一种复合催化剂(Sn@NBGNs-CNTs),它由锚定在氮和硼共掺杂石墨烯纳米片上的金属锡微粒以及部分剥离的碳纳米管组成,用作硫宿主。这种结构有效地将多硫化物锚定在界面处,并提供了丰富的活性位点以加速氧化还原反应动力学。结果,它促进了界面处的电荷转移和多硫化物传输,导致使用恒电位间歇滴定技术的临界沉积电压测定的LiS成核生长速率常数增加。因此,该电极表现出优异的循环稳定性,在1 C下350次循环后保留其初始容量的93%,每循环的容量衰减率极低,为0.003%。

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