Tubular CoFeP@CN as a Mott–Schottky Catalyst with Multiple Adsorption Sites for Robust Lithium−Sulfur Batteries

Zhang Chaoqi; Du Ruifeng; Biendicho Jordi Jacas; Yi Mingjie; Xiao Ke; Yang Dawei; Zhang Ting; Wang Xiang; Arbiol Jordi; Llorca Jordi; Zhou Yingtang; Morante Joan Ramon; Cabot Andreu

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Tubular CoFeP@CN as a Mott–Schottky Catalyst with Multiple Adsorption Sites for Robust Lithium−Sulfur Batteries

机译：管状COFEP @ CN作为一种用于鲁棒锂 - 硫电池的多个吸附部位的Mott-Schottky催化剂

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The shuttle effect and the sluggish reaction kinetics of lithium polysulfide (LiPS) seriously compromise the performance of lithium-sulfur batteries (LSBs). To overcome these limitations and enable the fabrication of robust LSBs, here the use of a Mott-Schottky catalyst based on bimetallic phosphide CoFeP nanocrystals supported on carbon nitride tubular nanostructures as sulfur hosts is proposed. Theoretical calculations and experimental data confirm that CoFeP@CN composites are characterized by a suitable electronic structure and charge rearrangement that allows them to act as a Mott-Schottky catalyst to accelerate LiPS conversion. In addition, the tubular geometry of CoFeP@CN composites facilitates the diffusion of Li ions, accommodates volume change during the reaction, and offers abundant lithiophilic/sulfiphilic sites to effectively trap soluble LiPS. Therefore, S@CoFeP@CN electrodes deliver a superior rate performance of 630 mAh g(-1) at 5 C, and remarkable cycling stability with 90.44% capacity retention over 700 cycles. Coin cells with high sulfur loading, 4.1 mg cm(-2), and pouch cells with 0.1 Ah capacities are further produced to validate their superior cycling stability. In addition, it is demonstrated here that CoFeP@CN hosts greatly alleviate the often overlooked issues of low energy efficiency and serious self-discharging in LSBs.

机译：穿梭效果和多硫化锂（嘴唇）的缓慢反应动力学严重损害了锂 - 硫电池（LSB）的性能。为了克服这些限制并使鲁棒LSB的制造能够制造，这里提出了基于支撑在氮化物管状纳米结构上负载的双金属磷化物CoFep纳米晶体作为硫宿主的使用。理论计算和实验数据证实CoFep @ CN复合材料的特征在于合适的电子结构和电荷重新排列，其允许它们用作莫特 - 肖特基催化剂以加速嘴唇转换。此外，CoFep @ CN复合材料的管状几何形状有利于Li离子的扩散，适应反应过程中的体积变化，并提供丰富的锂硅基/硫纤维位点，以有效地捕获可溶性嘴唇。因此，S @ COFEP @ CN电极在5℃下提供630mAhg（-1）的优异速率性能，并具有90.44％的容量保持超过700次循环的显着循环稳定性。进一步制备具有高硫加载，4.1mg cm（-2）的硬币细胞，以及具有0.1αH容量的袋细胞以验证其优异的循环稳定性。此外，这里证明了Cofep @ CN主持人大大缓解了LSB中经常被忽视的低能量效率和严重的自放电问题。

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来源
《Advanced energy materials》 |2021年第24期|2100432.1-2100432.14|共14页
作者
Zhang Chaoqi; Du Ruifeng; Biendicho Jordi Jacas; Yi Mingjie; Xiao Ke; Yang Dawei; Zhang Ting; Wang Xiang; Arbiol Jordi; Llorca Jordi; Zhou Yingtang; Morante Joan Ramon; Cabot Andreu;
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作者单位

Catalonia Inst Energy Res IREC Barcelona 08930 Spain|Univ Barcelona Dept Elect & Biomed Engn Barcelona 08028 Spain;

Catalonia Inst Energy Res IREC Barcelona 08930 Spain|Univ Barcelona Dept Elect & Biomed Engn Barcelona 08028 Spain;

Catalonia Inst Energy Res IREC Barcelona 08930 Spain;

Harbin Inst Technol State Key Lab Adv Welding & Joining Shenzhen 518055 Peoples R China;

Catalonia Inst Energy Res IREC Barcelona 08930 Spain|Univ Barcelona Dept Elect & Biomed Engn Barcelona 08028 Spain;

Catalonia Inst Energy Res IREC Barcelona 08930 Spain|Univ Barcelona Dept Elect & Biomed Engn Barcelona 08028 Spain;

CSIC Catalan Inst Nanosci & Nanotechnol ICN2 Campus UAB Barcelona 08193 Spain|BIST Campus UAB Barcelona 08193 Spain;

Catalonia Inst Energy Res IREC Barcelona 08930 Spain|Univ Barcelona Dept Elect & Biomed Engn Barcelona 08028 Spain;

CSIC Catalan Inst Nanosci & Nanotechnol ICN2 Campus UAB Barcelona 08193 Spain|BIST Campus UAB Barcelona 08193 Spain|ICREA Pg Lluis Co 23 Barcelona 08010 Spain;

Univ Politecn Cataluna EEBE Inst Energy Technol Dept Chem Engn Barcelona 08019 Spain|Univ Politecn Cataluna EEBE Barcelona Res Ctr Multiscale Sci & Engn Barcelona 08019 Spain;

Zhejiang Ocean Univ Marine Sci & Technol Coll Natl Engn Res Ctr Marine Aquaculture Zhoushan 316004 Zhejiang Peoples R China;

Catalonia Inst Energy Res IREC Barcelona 08930 Spain|Univ Barcelona Dept Elect & Biomed Engn Barcelona 08028 Spain;

Catalonia Inst Energy Res IREC Barcelona 08930 Spain|ICREA Pg Lluis Co 23 Barcelona 08010 Spain;

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正文语种 eng
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关键词
carbon nitrides; lithium#8211; sulfur batteries; metal phosphides; Mott#8211; Schottky heterostructure; polysulfides; shuttle effect;

机译：碳氮化物;锂＆＃8211;硫磺电池;金属磷化物;MOTT＆＃8211;肖特基异质结构;多硫化物;梭效果;

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1. Tuning the electronic band structure of Mott-Schottky heterojunctions modified with surface sulfur vacancy achieves an oxygen electrode with high catalytic activity for lithium-oxygen batteries [J] . Liang Ranxi, Shu Chaozhu, Hu Anjun, Journal of Materials Chemistry, A. Materials for energy and sustainability . 2020,第22期

机译：调整用表面硫空位改性的Mott-Schottky异质结的电子带结构达到锂 - 氧电池具有高催化活性的氧电极
2. Sulfur film sandwiched between few-layered MoS2 electrocatalysts and conductive reduced graphene oxide as a robust cathode for advanced lithium-sulfur batteries [J] . Wei Yanju, Kong Zhenkai, Pan Yankai, Journal of Materials Chemistry, A. Materials for energy and sustainability . 2018,第14期

机译：硫膜夹在几层薄层的MOS2电催化剂和导电还原的石墨烯氧化物中，作为高级锂 - 硫电池的鲁棒阴极
3. Promoting sulfur adsorption using surface Cu sites in metal-organic frameworks for lithium sulfur batteries [J] . Baumann Avery E., Aversa Gabrielle E., Roy Anindya, Journal of Materials Chemistry, A. Materials for energy and sustainability . 2018,第11期

机译：使用表面Cu位点促进硫磺电池的金属有机框架中的硫吸附
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机译：一种新型硫/聚吡咯/多壁碳纳米管纳米复合型阴极，具有用于锂可充电电池的芯壳管状结构 - （PPT）
5. Nano-structured electrocatalysts for high performance lithium sulfur batteries [D] . Mosavati, Negar. 2016

机译：高性能锂硫电池的纳米结构电催化剂
6. Balancing surface adsorption and diffusion of lithium-polysulfides on nonconductive oxides for lithium–sulfur battery design [O] . Xinyong Tao, Jianguo Wang, Chong Liu, -1

机译：锂硫电池设计中非导电氧化物上多硫化锂的表面吸附和扩散的平衡
7. Lithium-Sulfur Batteries: Nitrogen-Doped Aligned Carbon Nanotube/Graphene Sandwiches: Facile Catalytic Growth on Bifunctional Natural Catalysts and Their Applications as Scaffolds for High-Rate Lithium-Sulfur Batteries (Adv. Mater. 35/2014) [O] . Cheng Tang, Qiang Zhang, Meng-Qiang Zhao, 2014

机译：锂 - 硫磺电池：氮气掺杂的碳纳米管/石墨烯三明治：双官能天然催化剂的催化生长及其作为高速锂 - 硫电池的支架（ADV。35/2014）

Tubular CoFeP@CN as a Mott–Schottky Catalyst with Multiple Adsorption Sites for Robust Lithium−Sulfur Batteries

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