氨水水热改性煤基多孔炭超级电容器性能  

Supercapacitor performance of ammonia hydrothermal modified coal based porous carbon

作　　者：袁超 叶彦 杨春燕 田国亮 李婉晴 秦志宏[3] 杨小芹[3] YUAN Chao;YE Yan;YANG Chunyan;TIAN Guoliang;LI Wanqing;QIN Zhihong;YANG Xiaoqin(Shanxi Provincial Key Laboratory of Intelligent Evaluation and Efficient Utilization of Coking Coal,Taiyuan 030024,China;Coking Coal Clean Utilization Laboratory,Shanxi Coking Coal Group Co.,Ltd.,Taiyuan 030023,China;School of Chemical Engineering and Technology,China University of Mining and Technology,Xuzhou 221116,China)

机构地区：[1]炼焦煤智慧评价与高效利用山西省重点实验室,山西太原030024 [2]山西焦煤集团有限责任公司炼焦煤清洁利用实验室分公司,山西太原030023 [3]中国矿业大学化工学院,江苏徐州221116

出　　处：《洁净煤技术》2025年第1期105-114,共10页Clean Coal Technology

基　　金：国家自然科学基金资助项目(21706276)。

摘　　要：煤炭由于其高碳含量、缩合芳香结构及显著的经济性,作为生产电容炭的前驱体具有独特优势。通过对山西炼焦煤进行溶剂萃取得到煤基重质组(HC)作为碳源,KOH为活化剂制备多孔炭材料(AHC),再用氨水对其进行特定条件的水热改性,得到了一种具有高倍率性能和高循环稳定性的氮掺杂多孔炭。通过SEM、FTIR、XPS、Raman及N2吸附等表征分析,研究了不同氨水添加量下多孔炭的微观形貌、孔结构、表面化学性质等对其电化学性能的影响。结果发现:改性后多孔炭表面形貌和孔结构都有所改善,当氨水添加量为8 mL时,所得改性多孔炭AHC−N8呈现明显的蠕虫状纳米裂隙孔结构,中孔占比增大,且表面氮原子数分数由水热改性前的0.66%增至2.83%。该多孔炭电极材料在1 A/g电流密度下比电容达351.3 F/g,倍率性能达82%,与未改性AHC的63.5%相比得到了极大的提升。10 A/g下10000次循环充放电后比电容保持率也由未改性AHC的91.4%增至95.6%。AHC−N8的高比表面积、适宜的微/介孔分布以及表面较多的吡啶氮和吡咯氮掺杂对其突出的电化学性能起到了主要的作用。Coal has unique advantages as a precursor for producing porous carbon electrode materials for supercapacitors due to its high carbon content,condensed aromatic structure,and significant economic benefits.By solvent extraction of coking coal from Shanxi,coal based heavy component(HC)was obtained as carbonaceous precursor,and KOH was used as an activator to prepare porous carbon materials(AHC).Then,ammonia water was used for hydrothermal modification at certain conditions to obtain a nitrogen-doped porous carbon with high rate performance and high cycling stability.The influence of different amounts of ammonia water addition on the microstructure,pore structure,surface chemical properties,and electrochemical performance of porous carbons was studied through characterization analyses such as SEM,FTIR,XPS,Raman,and N2 adsorption.The results showed that the surface morphology and pore structure of the modified porous carbons were improved.When the ammonia addition was 8 mL,the resulting modified porous carbon AHC−N8 exhibited a distinct wormlike nano crack pore nitrogen content from 0.66%(without modification)to 2.83%.The porous carbon electrode material has a structure,with an increased proportion of mesopores and a surface specific capacitance of 351.3 F/g and a rate performance of 82%at a current density of 1 A/g,which is greatly improved compared to AHC(63.5%).After 10000 cycles of charging and discharging at 10 A/g,the specific capacitance retention rate increased from 91.4%to 95.6%.The high specific surface area,suitable micro/mesoporous distribution,and high surface doping of pyridine nitrogen and pyrrole nitrogen contribute to the outstanding electrochemical performance of AHC−N8.

关 键 词：超级电容器 煤基多孔炭 氨水改性 氮掺杂 电化学性能 

分 类 号：TQ536.9[化学工程—煤化学工程]