Accurate Control Multiple Active Sites of Carbonaceous Anode for High Performance Sodium Storage: Insights into Capacitive Contribution Mechanism,Advanced Energy Materials

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Accurate Control Multiple Active Sites of Carbonaceous Anode for High Performance Sodium Storage: Insights into Capacitive Contribution Mechanism
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2020-01-10 , DOI: 10.1002/aenm.201903312
Yun Lu ₁ , Jianing Liang ₁ , Yezhou Hu ₁ , Yi Liu ₁ , Ke Chen ₁ , Shaofeng Deng ₁ , Deli Wang ₁

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Heteroatom doping is widely recognized as an appealing strategy to break the capacitance limitation of carbonaceous materials toward sodium storage. However, the concrete effects, especially for heteroatomic phase transformation, during the sodium storage reaction remain a confusing topic. Here, a novel hypercrosslinked polymerization approach is demonstrated to fabricate pyrrole/thiophene hypercrosslinked microporous copolymer and further give porous carbonaceous materials with accurately regulated N/S dual doping corresponding to starting feeding ratios. Significantly, the N doping contributes to the conductivity and surface wettability, while the S doping is bridged to build stable active sites, which can be electrochemically converted into mercaptan anions via faraday reaction and further enhancing reversible capacities. Meanwhile, the abundant S doping can also conduce to the expanded interlayer spacing to shorten the ions diffusion distance, thus optimizing the reaction kinetic. As a result, the N_0.2S_0.8‐micro‐dominant porous carbon delivers the highest reversible capacity of 521 mAh g⁻¹ at 100 mA g⁻¹ and excellent cyclic stability over 2000 cycles at 2000 mA g⁻¹ with a capacity decay of 0.0145 mAh g⁻¹ per cycle. This work is anticipated to provide an in‐depth understanding of capacitance contribution and illuminate the heteroatomic phase transformation during sodium storage reactions for doping carbonaceous anodes.

中文翻译：

碳酸钠阳极精确控制多个活性位点，用于高性能钠存储：对电容性贡献机理的见解

杂原子掺杂被公认为是打破碳质材料对钠存储的电容限制的有吸引力的策略。然而，钠存储反应期间的具体效果，特别是对于杂原子相变，仍然是一个令人困惑的话题。在此，证明了一种新颖的超交联聚合方法，该方法可制备吡咯/噻吩超交联的微孔共聚物，并进一步为多孔碳质材料提供与起始进料比相对应的N / S双掺杂精确调节。重要的是，N掺杂有助于导电性和表面润湿性，而S掺杂则被桥接以建立稳定的活性位点，可以通过法拉第反应将其电化学转化为硫醇阴离子并进一步增强可逆容量。与此同时，大量的S掺杂还可以扩大层间间距，缩短离子扩散距离，从而优化反应动力学。结果，N_0.2 š _0.8 -Micro显性多孔碳提供的521毫安克最高可逆容量^-1在100mA克^-1在2000毫安克和优异的循环稳定性超过2000个循环^-1与0.0145毫安g的容量衰减^-1每周期。预期这项工作将提供对电容贡献的深入了解，并阐明掺杂碳质阳极的钠存储反应期间的杂原子相变。

更新日期：2020-02-18

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