Boosting supercapacitor and capacitive deionization performance of hierarchically porous carbon by polar surface and structural engineering†,Journal of Materials Chemistry A

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Boosting supercapacitor and capacitive deionization performance of hierarchically porous carbon by polar surface and structural engineering†
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2019-12-14 , DOI: 10.1039/c9ta12170f
Silu Huo _{1,

2,

3,

4,

5} , Yubo Zhao _{1,

2,

3,

4,

5} , Mingzhu Zong _{1,

2,

3,

4,

5} , Bolong Liang _{1,

2,

3,

4,

5} , Xueli Zhang _{1,

2,

3,

4,

5} , Izhar Ullah Khan _{1,

2,

3,

4,

5} , Xue Song _{1,

2,

3,

4,

5} , Kexun Li _{1,

2,

3,

4,

5}

Affiliation

Heteroatom doped hierarchically porous carbon materials are considered as promising candidates for high performance capacitive deionization and supercapacitor applications. However, the development of carbons simultaneously having both a reasonable polar surface and a hierarchically porous structure via a flexible synthetic strategy is critical but still a great challenge. Herein, a facile and effective strategy is presented for the preparation of N and P dual-doped hierarchically porous carbon networks by one-pot carbonization of a rationally designed precursor that was built using a metal–organic gel with a zinc ion metallic cluster and nitrogen/phosphorus chelate ligands. Due to the abundant exposed polar surface groups and the highly developed interconnected macro-/meso-/microporous structure, the optimal sample delivers a high specific capacitance of 373 F g⁻¹ at a current density of 1 A g⁻¹ and retains 270 F g⁻¹ at 100 A g⁻¹ with a capacitive retention of 72.3%. Furthermore, the symmetric supercapacitors assembled in aqueous and PVA/KOH solid electrolytes exhibit excellent energy outputs of 38.5 and 7.5 W h kg⁻¹, respectively. For capacitive deionization, the sample displays a superior salt adsorption capacity of 7.7, 10.3 and 18.1 mg g⁻¹ in NaCl solution with an initial concentration of 250 mg L⁻¹ at applied voltages of 1, 1.2 and 1.4 V, respectively. Additionally, kinetics studies and density functional theory simulations reveal that N/P dual-doping not only reliably introduces pseudocapacitance, but also greatly enhances the chemisorption of Na and Cl, resulting in a remarkable electrochemical performance. This work provides a new insight into the relationship between polar surface/structural engineering and the capacitive performance of the designed materials.

中文翻译：

通过极性表面和结构工程提高多层多孔碳的超级电容器和电容去离子性能†

杂原子掺杂的分级多孔碳材料被认为是高性能电容去离子和超级电容器应用的有希望的候选者。然而，碳的发展同时既具有合理的极性表面和分层多孔结构通过灵活的综合策略至关重要，但仍然是巨大的挑战。本文提出了一种简便有效的策略，该方法是通过对一合理设计的前驱体进行一锅式碳化来制备N和P双掺杂的分级多孔碳网络，该前驱体是使用具有锌离子金属簇和氮的金属有机凝胶构建的/磷螯合物。由于大量暴露的极性表面基团和高度发达的相互连接的大/中/微孔结构，最佳样品在1 A g ^-1的电流密度下可提供373 F g ^-1的高比电容并保持270 F g ^-1在100 A时g ^-1电容保持率为72.3％。此外，组装在水性和PVA / KOH固体电解质中的对称超级电容器分别显示出38.5和7.5 W h kg ^-1的优异能量输出。对于电容性去离子，样品在初始浓度为250 mg L ^-1的NaCl溶液中显示出7.7、10.3和18.1 mg g ^-1的优异盐吸附能力分别施加1、1.2和1.4 V的电压。此外，动力学研究和密度泛函理论模拟表明，N / P双掺杂不仅可靠地引入了假电容，而且还大大增强了Na和Cl的化学吸附，从而产生了出色的电化学性能。这项工作为极性表面/结构工程与设计材料的电容性能之间的关系提供了新的见解。

更新日期：2020-01-10

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