MOF模板法合成氮掺杂碳材料用于增强电化学钠离子储存和去除

引用本文: 王卓, 白雪, 张可新, 王鸿志, 董家宝, 高源, 赵斌. MOF模板法合成氮掺杂碳材料用于增强电化学钠离子储存和去除[J]. 物理化学学报, 2025, 41(3): 240500. doi: 10.3866/PKU.WHXB202405002 shu

Citation: Zhuo Wang, Xue Bai, Kexin Zhang, Hongzhi Wang, Jiabao Dong, Yuan Gao, Bin Zhao. MOF-Templated Synthesis of Nitrogen-Doped Carbon for Enhanced Electrochemical Sodium Ion Storage and Removal[J]. Acta Physico-Chimica Sinica, 2025, 41(3): 240500. doi: 10.3866/PKU.WHXB202405002 shu

MOF模板法合成氮掺杂碳材料用于增强电化学钠离子储存和去除

上海理工大学材料与化学学院, 上海 200093

通讯作者: Bin Zhao, Email: zhaobin@usst.edu.cn

基金项目:
国家自然科学基金 22209114

上海市教育委员会和上海市教育发展基金会晨光计划 21CGA56

上海市自然科学基金 21ZR1445700

上海市青年科技英才扬帆计划 21YF1430800

摘要: 电极材料在电容去离子技术中起到决定性作用，影响着盐离子的去除和电荷储存能力。本文通过碳化MOF-5和三聚氰胺的混合物，成功制备了氮掺杂的分级多孔碳，其中三聚氰胺起着氮源和造孔剂的双重作用。通过优化碳化温度，得到的MOF-5衍生纳米多孔碳(NPC-800)，其不但保持着MOF-5原始的立方体形貌、还具有大的比表面积、高氮含量和良好的润湿性。NPC-800电极在0.2 A·g^-1电流密度下具有91.8 mAh·g^-1的高比容量。在5 A·g^-1的电流密度下循环50000次，容量保持率为100%，展现出超长的循环稳定性。在500 mg·L^-1的NaCl溶液，施加恒压1.2 V，NPC-800电极具有高的脱盐容量24.17 mg·g^-1，快的脱盐速度2.8 mg·g^-1·min^-1和较稳定的再生循环能力。因此，以金属有机框架为模板合成氮掺杂的碳材料，能够有效增强钠离子的电化学储存和去除能力，有望成为电容去离子电极材料的最佳选择。

关键词:

English

MOF-Templated Synthesis of Nitrogen-Doped Carbon for Enhanced Electrochemical Sodium Ion Storage and Removal

School of Materials and Chemistry, University of Shanghai for Science and Technology, Shanghai 200093, China

Corresponding author: Bin Zhao, zhaobin@usst.edu.cn

Received Date: 01 May 2024
Accepted Date: 31 May 2024
Revised Date: 24 May 2024
Available Online: 15 March 2025
Fund Project:
the National Natural Science Foundation of China

the Chenguang Program of Shanghai Education Development Foundation and Shanghai Municipal Education

the Natural Science Foundation of Shanghai

the Shanghai Sailing Program

Abstract: Water scarcity has become a prominent global challenge in the twenty-first century, prompting the rapid advancement of desalination technology. Capacitive deionization (CDI) stands out as a cost-effective solution for sustainable water purification. The electrode material plays a pivotal role in capacitive deionization, impacting the salt ion removal and charge storage capacity. Carbon-based materials, characterized by high surface area and electrical conductivity, are ideal materials for capacitive deionization. However, their effectiveness in salt ion removal is hindered by unclear pore structures and poor wettability, limiting salt ion transport and storage. In this study, nitrogen-doped hierarchical porous carbon is successfully synthesized through the carbonization of MOF-5 and melamine mixtures, wherein melamine serves as both a nitrogen source and porogenic agent. Through optimization of carbonization temperature, the resulting MOF-5-derived nanoporous carbon (referred to as NPC-800) retains the cubic morphology of MOF-5, possesses a large surface area (754.34 m²∙g^-1), high nitrogen content (10.13%), and favorable wettability. Electrochemical analysis reveals that the NPC-800 electrode demonstrates specific capacities of 91.8, 76.1, 66.3, 51.0, 28.0, and 15.2 mAh∙g^-1 at current densities of 0.2, 0.5, 1.0, 2.0, 4.0, and 6.0 A∙g^-1, respectively, outperforming NPC-700 (26.3, 19.7, 13.1, 6.90, 2.30, and 1.30 mAh∙g^-1) and NPC-900 (46.0, 37.8, 30.4, 21.3, 11.7, and 7.50 mAh∙g^-1). The superior electrochemical performance of NPC-800 can be attributed to its maximal specific surface area, abundant pore structure, and optimal wettability, facilitating increased active sites for salt ion adsorption and diffusion. Moreover, NPC-800 exhibits low intrinsic resistance, rapid ion transfer kinetics, and exceptional cycling stability (50000 cycles) with 100% capacity retention at 5 A∙g^-1. Further investigation into the CDI performance of NPC electrodes under different applied voltages (0.8, 1.0, and 1.2 V) and initial NaCl solution concentrations (100, 300, and 500 mg∙L^-1) demonstrates the superior adsorption capacity of the NPC-800 electrode compared to the other two electrodes. Specifically, at 1.2 V in a 500 mg∙L^-1 salt solution, NPC-800 exhibits a faster salt adsorption rate (2.8 mg∙g^-1∙min^-1) and higher salt adsorption capacity (24.17 mg∙g^-1) compared to NPC-700 and NPC-900. Consequently, the melamine-assisted synthesis of N-doped porous carbon material holds promise as an optimal choice for capacitive deionization.

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

MOF模板法合成氮掺杂碳材料用于增强电化学钠离子储存和去除

通讯作者: Bin Zhao, Email: zhaobin@usst.edu.cn

English

MOF-Templated Synthesis of Nitrogen-Doped Carbon for Enhanced Electrochemical Sodium Ion Storage and Removal

Corresponding author: Bin Zhao, zhaobin@usst.edu.cn

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

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CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

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CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

MOF模板法合成氮掺杂碳材料用于增强电化学钠离子储存和去除

通讯作者: Bin Zhao, Email: zhaobin@usst.edu.cn

English

MOF-Templated Synthesis of Nitrogen-Doped Carbon for Enhanced Electrochemical Sodium Ion Storage and Removal

Corresponding author: Bin Zhao, zhaobin@usst.edu.cn

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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