Study on Shaped Activated Carbon from Catechol Rectification Residue

doi:10.12422/j.issn.1006-396X.2023.03.010

Abstract

Abstract:

The preparation of activated carbon from residue of a distillation reactor is an efficient and economical strategy for the utilization of hazardous waste resources.However,the prepared activated carbon is generally powdered,which is difficult to meet the requirements of industrial application.In this work,the activated carbon microspheres were prepared based on the rectification residue activated carbon from the powders,using deionized water as the solvent and polyacrylic acid (PAA),sodium alginate (SA) and Ca²⁺ as the additives.The effects of SA,Ca²⁺ and PAA amount on the structure and mechanical strength of the activated carbon microspheres were investigated.X?ray diffraction,Fourier transform infrared spectroscopy and Raman spectroscopy were used to investigate the shaping mechanism of activated carbon microspheres.The activated carbon microspheres were applied in the tetracycline adsorption,and the maximum adsorption capacity of tetracycline was up to 257.8 mg/g.At the same time,after 9 months of water stability test,the activated carbon microspheres still had good adsorption performance and mechanical strength. This shaping strategy adopted green and economical raw materials,which could effectively solve the problems of powder shaping and poor performance of microspheres,and provide the effective solution for the industrial application of high?performance materials.

Key words: Catechol rectification residue, Activated carbon microspheres, Stability, Adsorption, Tetracycline

摘要：

采用精馏釜残制备活性炭是一种高效、经济的危废资源化利用策略，但是制得的活性炭一般呈粉末状，难以满足工业化应用要求。以自制的苯二酚精馏釜残粉末活性炭为原料，采用去离子水为溶剂，聚丙烯酸(PAA)、海藻酸钠(SA)和Ca²⁺为添加剂，制备了活性炭微球。通过调控SA、Ca²⁺、PAA的添加质量，考察其对活性炭微球的结构与机械强度的影响；采用X射线衍射、傅里叶变换红外光谱、拉曼光谱等表征手段，探讨活性炭微球的成型机理。以吸附四环素为工业化目的进行研究的结果表明，活性炭微球最高吸附量为257.8 mg/g；同时，经历9个月的水稳定测试，活性炭微球依然具有良好的吸附性能和机械强度。该成型策略采用绿色化、经济性原料，有效解决了粉末成型难与活性炭微球性能差的问题，为高性能材料工业化应用提供了有效的解决方案。

关键词: 苯二酚精馏釜残, 活性炭微球, 稳定性, 吸附, 四环素

CLC Number:

TQ127.1

Xiang Wang, Jinhui Gu, Qing Liu, Zhaoyang Fei, Xian Chen, Mifen Cui, Xu Qiao. Study on Shaped Activated Carbon from Catechol Rectification Residue[J]. Journal of Petrochemical Universities, 2023, 36(3): 66-73.

王翔, 顾金辉, 刘清, 费兆阳, 陈献, 崔咪芬, 乔旭. 苯二酚精馏釜残成型活性炭的研究[J]. 石油化工高等学校学报, 2023, 36(3): 66-73.

Figures/Tables 14

Fig.1 Schematic of the preparation of activated carbon microspheres

Table 1 Influence of m（SA）/m（RAC） on the properties of activated carbon microspheres

m（SA）/ m（RAC）	比表面积/ (m² $⋅$ g^-1)	总孔容/ (cm³ $⋅$ g^-1)	机械强度/N
空白	1 800	0.91	0
0∶1.0	-	-	-
0.1∶1.0	1 180	0.52	6.70
0.2∶1.0	1 719	0.85	6.20
0.4∶1.0	1 703	0.81	6.50

Table 1 Influence of m（SA）/m（RAC） on the properties of activated carbon microspheres

m（SA）/ m（RAC）	比表面积/ (m² $⋅$ g^-1)	总孔容/ (cm³ $⋅$ g^-1)	机械强度/N
空白	1 800	0.91	0
0∶1.0	-	-	-
0.1∶1.0	1 180	0.52	6.70
0.2∶1.0	1 719	0.85	6.20
0.4∶1.0	1 703	0.81	6.50

Table 2 Influence of m（Ca2+）/m（RAC） on the properties of activated carbon microspheres

m（Ca²⁺）/ m（RAC）	比表面积/ (m² $⋅$ g^-1)	总孔容/ (cm³ $⋅$ g^-1)	机械强度/N
空白	1 800	0.91	0
0∶1.0	-	-	-
0.1∶1.0	1 743	0.89	1.70
0.2∶1.0	1 719	0.85	6.20
0.5∶1.0	1 673	0.79	6.30

Table 2 Influence of m（Ca2+）/m（RAC） on the properties of activated carbon microspheres

m（Ca²⁺）/ m（RAC）	比表面积/ (m² $⋅$ g^-1)	总孔容/ (cm³ $⋅$ g^-1)	机械强度/N
空白	1 800	0.91	0
0∶1.0	-	-	-
0.1∶1.0	1 743	0.89	1.70
0.2∶1.0	1 719	0.85	6.20
0.5∶1.0	1 673	0.79	6.30

Table 3 Influence of m（PAA）/m（RAC） on the properties of activated carbon microspheres

m（PAA）/ m（RAC）	比表面积/ (m² $⋅$ g^-1)	总孔容/ (cm³ $⋅$ g^-1)	机械强度/N
空白	1 800	0.91	0
0∶1.0	1 780	0.88	0.50
0.2∶1.0	1 743	0.86	1.70
0.5∶1.0	1 719	0.85	6.20
1.0∶1.0	1 373	0.59	7.50

Table 3 Influence of m（PAA）/m（RAC） on the properties of activated carbon microspheres

m（PAA）/ m（RAC）	比表面积/ (m² $⋅$ g^-1)	总孔容/ (cm³ $⋅$ g^-1)	机械强度/N
空白	1 800	0.91	0
0∶1.0	1 780	0.88	0.50
0.2∶1.0	1 743	0.86	1.70
0.5∶1.0	1 719	0.85	6.20
1.0∶1.0	1 373	0.59	7.50

Fig.2 XRD patterns of MLRAC, RAC and RAC@SA0.2/(CaCl2)0.2/PAA0.5 samples

Fig.3 SEM and EDS?mapping of RAC and RAC@SA0.2/(CaCl2)0.2/PAA0.5

Fig.4 FT?IR spectra of MLRAC,RAC and RAC@SA0.2/(CaCl2)0.2/PAA0.5

Fig.5 Raman spectra of RAC,RAC@SA0.2/(CaCl2)0.2/PAA0 and RAC@SA0.2/(CaCl2)0.2/PAA0.5

Fig.6 N2 adsorption?desorption curves and pore size distribution curves of RAC and RAC@SA0.2/(CaCl2)0.2/PAA0.5

Fig.7 Shaping mechanism of RAC@SA0.2/(CaCl2)0.2/PAA0.5

Fig.8 The adsorption capacity of TC on activated carbon microspheres with different m（SA）/m（RAC），m（Ca2+）/m（RAC）and m（PAA）/m（RAC）

Fig.9 generation rate of RAC@SA0.2/(CaCl2)0.2/PAA0.5 in recycle test

Fig.10 Water stability test for RAC@SA0.2/(CaCl2)0.2/PAA0.5

Fig.11 TC adsorption capacity and mechanical strength of RAC@SA0.2/(CaCl2)0.2/PAA0.5 after 9 months in aqueous solutions at different pH values

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