沥青基多孔炭材料的制备及在超级电容器中的应用进展

doi:10.16085/j.issn.1000-6613.2022-1030

化工进展 ›› 2023, Vol. 42 ›› Issue (4): 1895-1906.DOI: 10.16085/j.issn.1000-6613.2022-1030

沥青基多孔炭材料的制备及在超级电容器中的应用进展

蔡江涛¹^,²(), 候刘华¹, 兰雨金¹, 张晨陈¹, 刘国阳¹, 朱由余¹, 张建兰¹^,², 赵世永¹^,², 张亚婷¹^,²()

^1.西安科技大学化学与化工学院，陕西西安 710054
^2.自然资源部煤炭资源勘查与综合利用重点实验室，陕西西安 710021

收稿日期:2022-06-02 修回日期:2022-07-06 出版日期:2023-04-25 发布日期:2023-05-08
通讯作者: 张亚婷
作者简介:蔡江涛（1973—），女，副教授，硕士生导师，研究方向为功能炭材料及其复合材料的制备与应用。E-mail：caijt@xust.edu.cn。
基金资助:
国家自然科学基金(52102051);陕西省科技厅项目(2022GY-168);榆林市科技计划(CXY-2022-155);西安科技大学重点专项(2040422042)

Preparation of pitch-based porous carbon materials and application in supercapacitors

CAI Jiangtao¹^,²(), HOU Liuhua¹, LAN Yujin¹, ZHANG Chenchen¹, LIU Guoyang¹, ZHU Youyu¹, ZHANG Jianlan¹^,², ZHAO Shiyong¹^,², ZHANG Yating¹^,²()

^1.College of Chemistry & Chemical Engineering, Xi’an University of Science & Technology, Xi’an 710054, Shaanxi, China
^2.Key Laboratory of Coal Resources Exploration & Comprehensive Utilization, Ministry of Natural Resource, Xi’an 710021, Shaanxi, China

Received:2022-06-02 Revised:2022-07-06 Online:2023-04-25 Published:2023-05-08
Contact: ZHANG Yating

摘要/Abstract

摘要：

沥青是由富含稠环芳烃的系列碳氢化合物及其非金属衍生物组成的复杂混合物，具有较高的碳含量。开发沥青作为炭材料前体，用于制备超级电容器炭电极材料，既拓展了沥青的应用市场及提升其附加值，更是响应国家对于新型能源利用的需求。本文首先对超级电容器的储能机理进行了阐述，探讨了影响超级电容器用炭材料电化学性能的结构因素及规律，概述了沥青的组成、结构模型、来源及其应用。然后综述了沥青基多孔炭用作超级电容器电极材料的研究进展，并对活化法、模板法及熔盐法等方法制备沥青基多孔炭的特点与进展进行了分析，着重对沥青基多孔炭材料的改性研究进行了总结。最后指出了沥青基多孔炭材料作为超级电容器电极材料的发展优势及不足，建议对沥青原料进行预处理联合炭化后脱除金属杂原子，以获得稳定长循环寿命的电容炭；加强对沥青中四组分炭化成炭规律的研究，以提高沥青基超容炭材料的成炭率；KOH活化法与其他活化方法相结合，以期在获得高性能活性炭基础上减少对设备的损耗与环境的影响。

关键词: 沥青, 多孔炭, 超级电容器, 电极材料

Abstract:

Pitch is a complex mixture of a series of hydrocarbons rich in thick rings aromatic hydrocarbons and their non-metallic derivatives with high carbon content. The development of pitch as a carbon material precursor for the preparation of supercapacitor carbon electrode material not only expands the application market of pitch and enhances its added value, but also responds to the national demand for new energy utilization. In this paper, the energy storage mechanism of supercapacitors was firstly described, and the structural factors and laws affecting the electrochemical properties of carbon materials for supercapacitors were discussed. The composition, structural model, sources and applications of pitch were outlined. Then, the research progress of pitch-based porous carbon for supercapacitor electrode materials was reviewed, and the characteristics and progress of pitch-based porous carbon preparation by activation method, template method and molten salt method were analyzed. A summary of the research on the modification of pitch-based porous carbon materials was highlighted. Finally, the advantages and disadvantages of pitch-based porous carbon materials as electrode materials for supercapacitors were pointed out. It is suggested that the asphalt raw materials should be pretreated and carbonized to remove metal heteroatoms from the obtained carbon materials to obtain capacitor carbon with stable and long cycle life. The research on the carbonization law of four components in asphalt should be strengthened, so as to improve the carbonization rate of pitch-based supercapacitive carbon materials. The KOH activation method should be combined with other activation methods in order to reduce the loss of equipment and the impact on the environment on the basis of obtaining high-performance activated carbon.

Key words: pitch, porous carbon, supercapacitor, electrode materials

中图分类号:

TQ127.1

蔡江涛, 候刘华, 兰雨金, 张晨陈, 刘国阳, 朱由余, 张建兰, 赵世永, 张亚婷. 沥青基多孔炭材料的制备及在超级电容器中的应用进展[J]. 化工进展, 2023, 42(4): 1895-1906.

CAI Jiangtao, HOU Liuhua, LAN Yujin, ZHANG Chenchen, LIU Guoyang, ZHU Youyu, ZHANG Jianlan, ZHAO Shiyong, ZHANG Yating. Preparation of pitch-based porous carbon materials and application in supercapacitors[J]. Chemical Industry and Engineering Progress, 2023, 42(4): 1895-1906.

图/表 9

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种类	常见分子结构模型	已工业化用途
石油沥青		燃料、交通运输（道路、铁路、航空等）、建筑业、工业（采掘业、制造业）、农业、水利工程、民用等
煤焦沥青		生产橡胶、塑料、合成纤维、染料、医药、耐高温材料等的重要原料
天然沥青		高级公路的改性调和沥青、钻井助剂、高软化点特种沥青

种类	常见分子结构模型	已工业化用途
石油沥青		燃料、交通运输（道路、铁路、航空等）、建筑业、工业（采掘业、制造业）、农业、水利工程、民用等
煤焦沥青		生产橡胶、塑料、合成纤维、染料、医药、耐高温材料等的重要原料
天然沥青		高级公路的改性调和沥青、钻井助剂、高软化点特种沥青

材料	制备方法	比表面积/m²·g^-1	孔容积/cm³·g^-1	电极体系	电流密度/A·g^-1	比电容/F·g^-1	循环次数	电容保持率/%	参考文献
PCM	水蒸气活化	1638	0.153	两电极	1	252	10000	97.3	[39]
α-CLR-8h-900-4h	CO₂活化	2179.3	2.61	三电极	0.1	151	—	—	[40]
HPC₇₅	KOH活化	3473	1.714	三电极	1	339	10000	92.8	[3]
WPC-850	Na₂CO₃活化	1912	0.94	三电极	0.05	232	5000	97.5	[41]
EBC₈₀₀	K₂CO₃活化	854	0.48	三电极	0.106^①	340	50000	98.1	[42]
HPC_1∶2∶3	SiO₂模板	1952.6	1.15	三电极	1	341	10000	—	[43]
HPCNC-700-a	MgO模板	1777	0.94	三电极	1	380	—	—	[20]
C₇	ZnO模板	1537	—	两电极	5^②	200.5	8000	95	[44]
PC_18-800	Mg(OH)₂模板	3145	1.68	三电极	0.05	272	10000	96.69	[45]
HPC_4/4	三聚氰胺软模板	2038	—	三电极	0.05	221	5000	95.3	[46]
IPC_-2-0.2-8	MCC模板	3305	1.66	三电极	1	308	20000	101.7	[47]
HPCs	NaCl-KCl	2227	1.43	两电极	0.05	265	10000	91.1	[48]
HPCs-5-800	ZnCl₂-NaCl	2984	2.2	三电极	1	327	10000	94	[49]

材料	制备方法	比表面积/m²·g^-1	孔容积/cm³·g^-1	电极体系	电流密度/A·g^-1	比电容/F·g^-1	循环次数	电容保持率/%	参考文献
PCM	水蒸气活化	1638	0.153	两电极	1	252	10000	97.3	[39]
α-CLR-8h-900-4h	CO₂活化	2179.3	2.61	三电极	0.1	151	—	—	[40]
HPC₇₅	KOH活化	3473	1.714	三电极	1	339	10000	92.8	[3]
WPC-850	Na₂CO₃活化	1912	0.94	三电极	0.05	232	5000	97.5	[41]
EBC₈₀₀	K₂CO₃活化	854	0.48	三电极	0.106^①	340	50000	98.1	[42]
HPC_1∶2∶3	SiO₂模板	1952.6	1.15	三电极	1	341	10000	—	[43]
HPCNC-700-a	MgO模板	1777	0.94	三电极	1	380	—	—	[20]
C₇	ZnO模板	1537	—	两电极	5^②	200.5	8000	95	[44]
PC_18-800	Mg(OH)₂模板	3145	1.68	三电极	0.05	272	10000	96.69	[45]
HPC_4/4	三聚氰胺软模板	2038	—	三电极	0.05	221	5000	95.3	[46]
IPC_-2-0.2-8	MCC模板	3305	1.66	三电极	1	308	20000	101.7	[47]
HPCs	NaCl-KCl	2227	1.43	两电极	0.05	265	10000	91.1	[48]
HPCs-5-800	ZnCl₂-NaCl	2984	2.2	三电极	1	327	10000	94	[49]

材料	掺杂元素及含量	比表面积/m²·g^-1	电极体系	电流密度/A·g^-1	比电容/F·g^-1	循环次数	电容保持率/%	参考文献
N-CNS	N, 7.06%^①	1181	三电极	0.1	210	5000	91.2	[50]
NFPC_0.4-0.4Y-700	N, 8.22%^②	1474	三电极	1	349	2000	92	[65]
NPC	N, 4.48%^②	495.9	三电极	2	232.2	5000	89.8	[66]
N, P-PGC	N, 5.34%^① P, 2.7%^①	1606.6	两电极	0.5	219	10000	95.6	[51]
PAC-4-600	O, 15.9%^①	2245	三电极	0.5	427	10000	95	[68]
PC-CTP	O, 3.13%^②	2087	三电极	0.5	318.1	—	—	[30]
BNC-900	B, 1.703%^②	1103	三电极	0.1	349	—	—	[70]
HPC-4	S, 1.03%^②	3318	三电极	1	327	5000	96.5	[72]

沥青基多孔炭材料的制备及在超级电容器中的应用进展

Preparation of pitch-based porous carbon materials and application in supercapacitors

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材料	比表面积/m²·g^-1	电解液及浓度	电极体系	电流密度/A·g^-1	比电容/F·g^-1	循环次数	电容保持率/%	参考文献
HPC/MnO₂	2079	6mol/L KOH	三电极	1	480	5000	79.1	[72]
MnO₂@PCN	836	1mol/L Na₂SO₄	三电极	0.5	377	5000	88.3	[73]
ACPPy-2	966	1mol/L Na₂SO₄	三电极	1	82.3	1000	82	[74]
PPMn-CNF	620	6mol/L KOH	两电极	1^①	188	—	—	[77]
MPC/G_10-2-24	2164	6mol/L KOH	三电极	0.05	278	10000	93	[78]
PO-GO-16	2196	6mol/L KOH	三电极	0.1	296	—	—	[27]

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