吸附电活性染料的活性炭电极电化学性能

doi:10.16085/j.issn.1000-6613.2021-1280

摘要/Abstract

摘要：

采用商用活性炭（AC）吸附二元混合染料亚甲基蓝（MB）和胭脂红（AR18），制备得到AC/(MB+AR18)电极材料。比较单一活性炭（AC）和吸附不同浓度的二元混合染料后的活性炭[AC/(MB+AR18)]的电化学性能。三电极体系的测试结果表明：在1mol/L H₂SO₄电解液中，当电流密度为1A/g时，吸附了浓度为400mg/L污染物的AC/(MB+AR18)比电容为182F/g，高于单一AC的比电容（109F/g）。随后选用性能最优的AC/(MB+AR18)-400作为电极材料，组装对称超级电容器器件，发现工作电压窗口从只用AC组装的对称超级电容器的1.1V提高到1.5V，电流密度为0.75A/g时，功率密度为843.84W/kg，能量密度可达32.23W·h/kg，远远高于AC组装的超级电容器(4.74W·h/kg)，说明MB和AR18不仅为AC提供额外的法拉第电容，同时有助于提高其工作电压窗口。

关键词: 活性炭, 吸附（作用）, 亚甲基蓝, 胭脂红, 电化学

Abstract:

Commercial activated carbon (AC) was used to adsorb binary mixed dyes of methylene blue (MB) and Carmine (AR18) to prepare AC/(MB+AR18) electrode materials. The electrochemical performance of activated carbon (AC) and that adsorbed different concentration binary mixed dyes [AC/(MB+AR18)] was compared. The test results of the three-electrode system showed that, in 1mol/L H₂SO₄ electrolyte and under the current density of 1A/g, the specific capacitance of AC/(MB+AR18) after adsorbing in a concentration of 400mg/L pollutants was 182F/g, higher than that of the single AC (109F/g). Subsequently, AC/(MB+AR18)-400 with the best performance was selected as the electrode material to assemble a symmetrical supercapacitor device. It is found that the operating voltage window of AC/(MB+AR18) was increased to 1.5V, compared to 1.1V for the symmetrical supercapacitors assembled with AC only. When the current density was 0.75A/g, the power density was 843.84W/kg, and the energy density reached 32.23W·h/kg, higher than that of the supercapacitor assembled by activated carbon (4.74W·h/kg), which suggested that MB and AR18 not only provided additional Faraday capacitance for AC, but also helped to increase its operating voltage window.

Key words: activated carbon, adsorption, methylene blue, carmine, electrochemistry

中图分类号:

TQ15

陈泳, 马妍楠, 徐成. 吸附电活性染料的活性炭电极电化学性能[J]. 化工进展, 2022, 41(5): 2537-2545.

CHEN Yong, MA Yannan, XU Cheng. Electrochemical performance of activated carbon electrode adsorbing electroactive dyes[J]. Chemical Industry and Engineering Progress, 2022, 41(5): 2537-2545.

图/表 10

图1 浓度对二元混合染料（MB+AR18）去除率的影响

表1 吸附30min时AC对MB和AR18的吸附容量

样品	不同浓度下的吸附容量/mg
样品	50mg/L	100mg/L	200mg/L	300mg/L	400mg/L
AC吸附MB	50	100	200	299.7	397.2
AC吸附AR18	50	98.8	134	160.5	190

图2 AC和AC/(MB+AR18)的扫描电镜图

图3 AC和AC/(MB+AR18)的傅里叶红外图谱

图4 AC/(MB+AR18)的XPS图谱

图5 AC和AC/(MB+AR18)的N2吸/脱附等温及孔径分布曲线

表2 AC和AC/(MB+AR18)的孔隙参数

样品	S_BET/m²·g^-1	V/m³·g^-1	D/nm
AC	1813.36	0.977	3.05
AC/（MB+AR18）-400	682.50	0.380	3.14

图6 三电极体系AC/(MB+AR18)的电化学性能测试

图7 MB和AR18氧化还原反应示意图

图8 SSC1和SSC2器件的电化学性能测试

参考文献 29

1	CHEN Chong, YU Dengfeng, ZHAO Gongyuan, et al. Three-dimensional scaffolding framework of porous carbon nanosheets derived from plant wastes for high-performance supercapacitors[J]. Nano Energy, 2016, 27: 377-389.
2	WANG Dewei, LIU Shijia, FANG Guoli, et al. From trash to treasure: direct transformation of onion husks into three-dimensional interconnected porous carbon frameworks for high-performance supercapacitors in organic electrolyte[J]. Electrochimica Acta, 2016, 216: 405-411.
3	HE Yafei, ZHUANG Xiaodong, LEI Chaojun, et al. Porous carbon nanosheets: synthetic strategies and electrochemical energy related applications[J]. Nano Today, 2019, 24: 103-119.
4	DU Weimin, ZHANG Zirui, DU Lange, et al. Designing synthesis of porous biomass carbon from wheat straw and the functionalizing application in flexible, all-solid-state supercapacitors[J]. Journal of Alloys and Compounds, 2019, 797: 1031-1040.
5	孔庆强，黄显虹，王振兵，等. 超级电容器用活性炭国产化关键化学与化工问题[J]. 化工进展，2021，40（9）：5088-5096.
	KONG Qingqiang, HUANG Xianhong, WANG Zhenbing, et al. Key chemistry and chemical engineering issues in the localization of active carbon for supercapacitor[J]. Chemical Industry and Engineering Progress, 2021,40（9）：5088-5096.
6	YAGLIKCI Savas, GOKCE Yavuz, YAGMUR Emine, et al. The performance of sulphur doped activated carbon supercapacitors prepared from waste tea[J]. Environmental Technology, 2020, 41(1): 36-48.
7	LIU Yeping, CHANG Zhexin, YAO Lu, et al. Nitrogen/sulfur dual-doped sponge-like porous carbon materials derived from pomelo peel synthesized at comparatively low temperatures for superior-performance supercapacitors[J]. Journal of Electroanalytical Chemistry, 2019, 847: 113111.
8	LI Yanhui, DU Qiuju, LIU Tonghao, et al. Comparative study of methylene blue dye adsorption onto activated carbon, graphene oxide, and carbon nanotubes[J]. Chemical Engineering Research and Design, 2013, 91(2): 361-368.
9	CHEN Xiaoyan, LI Heping, LIU Wanyi, et al. Effective removal of methyl orange and Rhodamine B from aqueous solution using furfural industrial processing waste: furfural residue as an eco-friendly biosorbent[J]. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 2019, 583: 123976.
10	YU Miao, LI Jian, WANG Lijuan. KOH-activated carbon aerogels derived from sodium carboxymethyl cellulose for high-performance supercapacitors and dye adsorption[J]. Chemical Engineering Journal, 2017, 310: 300-306.
11	CAHINO Arthur Marinho, LOUREIRO Rafaella Gouveia, DANTAS Joelda, et al. Characterization and evaluation of ZnO/CuO catalyst in the degradation of methylene blue using solar radiation[J]. Ceramics International, 2019, 45(11): 13628-13636.
12	BOND Alan M, MARKEN Frank, HILL Emma, et al. The electrochemical reduction of indigo dissolved in organic solvents and as a solid mechanically attached to a basal plane pyrolytic graphite electrode immersed in aqueous electrolyte solution[J]. Journal of the Chemical Society, Perkin Transactions 2, 1997, 22(9): 1735-1742.
13	WANG Shaobin, Choonwei NG, WANG Wentai, et al. Synergistic and competitive adsorption of organic dyes on multiwalled carbon nanotubes[J]. Chemical Engineering Journal, 2012, 197: 34-40.
14	PING Yunjie, LIU Zhe, LI Jingjing, et al. Boosting the performance of supercapacitors based hierarchically porous carbon from natural Juncus effuses by incorporation of MnO₂ [J]. Journal of Alloys and Compounds, 2019, 805: 822-830.
15	DENG Lingjuan, ZHOU Caihua, MA Zhanying, et al. Methylene blue functionalized graphene as binder-free electrode for high-performance solid state supercapacitors[J]. Journal of Colloid and Interface Science, 2020, 561: 416-425.
16	PENG Chao, YAN Xingbin, WANG Rutao, et al. Promising activated carbons derived from waste tea-leaves and their application in high performance supercapacitors electrodes [J]. Electrochimica Acta, 2013, 87: 401-408.
17	LIANG Ji, JIAO Yan, JARONIEC Mietek, et al. Sulfur and nitrogen dual-doped mesoporous graphene electrocatalyst for oxygen reduction with synergistically enhanced performance [J]. Angewandte Chemie, 2012, 124(46):11664-11668.
18	WANG Changshui, LIU Tingzhi. Nori-based N, O, S, Cl co-doped carbon materials by chemical activation of ZnCl₂ for supercapacitor[J]. Journal of Alloys and Compounds, 2017, 696: 42-50.
19	LEE Jung-Soo, KIM Sun-I, YOON Jong-Chul, et al. Chemical vapor deposition of mesoporous graphene nanoballs for supercapacitor[J]. ACS Nano, 2013, 7(7): 6047-6055.
20	彭超. 生物质活性炭的制备及电化学电容性能研究[D]. 兰州: 兰州理工大学, 2013.
	PENG Chao. The preparation and study on performance of electrochemical capacitive based on activated carbon derived from biomass[D]. Lanzhou: Lanzhou University of Technology, 2013.
21	GAO Haiwen, WANG Xiaohong, WANG Ganghu, et al. An urchin-like MgCo₂O₄@ PPy core-shell composite grown on Ni foam for a high performance all-solid-state asymmetric supercapacitor[J]. Nanoscale, 2018, 10(21): 10190-10202.
22	YANG Yuan, LI Shuo, HUANG Wei, et al. Effective synthetic strategy for Zn_0.76Co_0.24S encapsulated in stabilized N-doped carbon nanoarchitecture towards ultra-long-life hybrid supercapacitors[J]. Journal of Materials Chemistry A, 2019, 7(24): 14670-14680.
23	WANG Yuan, CHANG Zheng, QIAN Meng, et al. Enhanced specific capacitance by a new dual redox-active electrolyte in activated carbon-based supercapacitors [J]. Carbon, 2019, 143: 300-308.
24	TANG Xiaohui, Yuhui LUI, CHEN Bolin, et al. Functionalized carbon nanotube based hybrid electrochemical capacitors using neutral bromide redox-active electrolyte for enhancing energy density[J]. Journal of Power Sources, 2017, 352: 118-126.
25	WAN Liu, CHEN Dequan, LIU Jiaxing, et al. Facile preparation of porous carbons derived from orange peel via basic copper carbonate activation for supercapacitors[J]. Journal of Alloys and Compounds, 2020, 823: 153747.
26	LI Pan, FENG Cuining, LI Hongping, et al. Facile fabrication of carbon materials with hierarchical porous structure for high-performance supercapacitors[J]. Journal of Alloys and Compounds, 2021, 851: 156922.
27	SU Xiaoli, CHEN Jingran, ZHENG Guangping, et al. Three-dimensional porous activated carbon derived from loofah sponge biomass for supercapacitor applications[J]. Applied Surface Science, 2018, 436: 327-336.
28	ZHOU Hua, ZHOU Yanmei, WU Shumeng, et al. Synthesis of N/S co-doped porous carbon microspheres based on amino acid protic salt for supercapacitor[J]. Journal of Alloys and Compounds, 2020, 829: 154549.
29	POURJAVADI Ali, ABDOLMALEKI Hamed, DOROUDIAN Mohadeseh, et al. Novel synthesis route for preparation of porous nitrogen-doped carbons from lignocellulosic wastes for high performance supercapacitors[J]. Journal of Alloys and Compounds, 2020, 827: 154116.

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