NbSe2 Meets C2N: A 2D-2D Heterostructure Catalysts as Multifunctional Polysulfide Mediator in Ultra-Long-Life Lithium–Sulfur Batteries,Advanced Energy Materials

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NbSe2 Meets C2N: A 2D-2D Heterostructure Catalysts as Multifunctional Polysulfide Mediator in Ultra-Long-Life Lithium–Sulfur Batteries
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2021-08-12 , DOI: 10.1002/aenm.202101250
Dawei Yang _{1,

2} , Zhifu Liang _{1,

3} , Chaoqi Zhang _{1,

2} , Jordi Jacas Biendicho ₁ , Marc Botifoll ₃ , Maria Chiara Spadaro ₃ , Qiulin Chen ₄ , Mengyao Li _{1,

2} , Alberto Ramon _{1,

2} , Ahmad Ostovari Moghaddam ₅ , Jordi Llorca ₆ , Jiaao Wang ₇ , Joan Ramon Morante _{1,

2} , Jordi Arbiol _{3,

8} , Shu‐Lei Chou ₉ , Andreu Cabot _{1,

8}

Affiliation

Catalonia Institute for Energy Research – IREC Sant Adrià de Besòs Barcelona 08930 Spain
Department of Electronic and Biomedical Engineering Universitat de Barcelona Barcelona 08028 Spain
Catalan Institute of Nanoscience and Nanotechnology (ICN2) CSIC and BIST Campus UAB Bellaterra Barcelona 08193 Spain
State Key Laboratory for Physical Chemistry of Solid Surfaces Fujian Key Laboratory of Materials Genome College of Materials Xiamen University Xiamen 361005 China
South Ural State University 76, Lenin Ave. Chelyabinsk 454080 Russia
Institute of Energy Technologies Department of Chemical Engineering and Barcelona Research Center in Multiscale Science and Engineering Universitat Politècnica de Catalunya EEBE Barcelona 08019 Spain
Department of Chemistry and the Oden Institute for Computational Engineering and Sciences The University of Texas at Austin Austin TX 78712 USA
ICREA Pg. Lluís Companys 23 Barcelona 08010 Spain
Institute for Superconducting and Electronic Materials University of Wollongong Innovation Campus North Wollongong New South Wales 2500 Australia

The shuttle effect and sluggish conversion kinetics of lithium polysulfides (LiPS) hamper the practical application of lithium–sulfur batteries (LSBs). Toward overcoming these limitations, herein an in situ grown C₂N@NbSe₂ heterostructure is presented with remarkable specific surface area, as a Li–S catalyst and LiPS absorber. Density functional theory (DFT) calculations and experimental results comprehensively demonstrate that C₂N@NbSe₂ is characterized by a suitable electronic structure and charge rearrangement that strongly accelerates the LiPS electrocatalytic conversion. In addition, heterostructured C₂N@NbSe₂ strongly interacts with LiPS species, confining them at the cathode. As a result, LSBs cathodes based on C₂N@NbSe₂/S exhibit a high initial capacity of 1545 mAh g⁻¹ at 0.1 C. Even more excitingly, C₂N@NbSe₂/S cathodes are characterized by impressive cycling stability with only 0.012% capacity decay per cycle after 2000 cycles at 3 C. Even at a sulfur loading of 5.6 mg cm⁻², a high areal capacity of 5.65 mAh cm⁻² is delivered. These results demonstrate that C₂N@NbSe₂ heterostructures can act as multifunctional polysulfide mediators to chemically adsorb LiPS, accelerate Li-ion diffusion, chemically catalyze LiPS conversion, and lower the energy barrier for Li₂S precipitation/decomposition, realizing the “adsorption-diffusion-conversion” of polysulfides.

中文翻译：

NbSe2 与 C2N 相遇：一种二维-二维异质结构催化剂作为超长寿命锂硫电池中的多功能多硫化物介体

多硫化锂（LiPS）的穿梭效应和缓慢的转化动力学阻碍了锂硫电池（LSB）的实际应用。为了克服这些限制，本文提出了一种具有显着比表面积的原位生长的 C ₂ N@NbSe ₂异质结构，作为 Li-S 催化剂和 LiPS 吸收剂。密度泛函理论 (DFT) 计算和实验结果综合表明，C ₂ N@NbSe ₂具有合适的电子结构和电荷重排，可强烈加速 LiPS 电催化转化。此外，异质结构的 C ₂ N@NbSe ₂与 LiPS 物质强烈相互作用，将它们限制在阴极。因此，基于 C ₂ N@NbSe ₂ /S 的LSBs 正极在 0.1 C 下表现出 1545 mAh g ^-1的高初始容量。更令人兴奋的是，C ₂ N@NbSe ₂ /S 正极具有令人印象深刻的循环稳定性在 3 C 下进行 2000 次循环后，每个循环只有 0.012% 的容量衰减。即使在 5.6 mg cm ^-2的硫负载下，也提供了 5.65 mAh cm ^-2的高面积容量。这些结果表明 C ₂ N@NbSe ₂异质结构可以作为多功能多硫化物介体化学吸附LiPS，加速锂离子扩散，化学催化LiPS转化，降低Li ₂ S沉淀/分解的能垒，实现多硫化物的“吸附-扩散-转化”。

更新日期：2021-09-23

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