无机材料学报 ›› 2021, Vol. 36 ›› Issue (12): 1330-1336.DOI: 10.15541/jim20210063
收稿日期:
2021-02-01
修回日期:
2021-03-30
出版日期:
2021-12-20
网络出版日期:
2021-04-05
通讯作者:
张 恒, 博士, 副教授. E-mail: zhangheng@qfnu.edu.cn
作者简介:
王婷婷(1979-), 女, 硕士. E-mail: wangting@qfnu.edu.cn
WANG Tingting(), SHI Shumei, LIU Chenyuan, ZHU Wancheng, ZHANG Heng(
)
Received:
2021-02-01
Revised:
2021-03-30
Published:
2021-12-20
Online:
2021-04-05
Contact:
ZHANG Heng, PhD, associate professor. E-mail: zhangheng@qfnu.edu.cn
About author:
WANG Tingting (1979-), female, Master. E-mail: wangting@qfnu.edu.cn
Supported by:
摘要:
层状硅酸镍因其独特的结构, 在电化学和催化等领域展现出良好的应用前景, 其合成与性能研究近年来受到广泛关注。本研究以氯化镍和正硅酸乙酯为原料, 采用水热法合成了硅酸镍微球, 并详细探究了镍硅比和碱源对产物组成、形貌及孔结构的影响。在优化条件下, 产物呈现由纳米片组装的、平均直径约为2.5 μm的微球形貌, 比表面积为119.6 m2·g-1, 孔容为0.673 cm3·g-1。Zeta电位分析表明, 该微球在pH=3~10范围内保持表面电负性。将硅酸镍微球用于处理碱性品红溶液, 吸附过程符合准二级动力学模型。在初始浓度为50 mg·L-1的条件下, 吸附容量可达120.7 mg·g-1, 脱除率达96.6%, 远优于改性粘土及近年来报道的多种材料。吸附量与平衡浓度的数据表明, 碱性品红在硅酸镍微球上的吸附符合Freundlich吸附模型, 1/n=0.1678, 表明该吸附为多层非均相吸附且吸附作用力强。
中图分类号:
王婷婷, 史书梅, 柳晨媛, 朱万诚, 张恒. 多级多孔硅酸镍微球的合成及其对碱性品红的高效吸附[J]. 无机材料学报, 2021, 36(12): 1330-1336.
WANG Tingting, SHI Shumei, LIU Chenyuan, ZHU Wancheng, ZHANG Heng. Synthesis of Hierarchical Porous Nickel Phyllosilicate Microspheres as Efficient Adsorbents for Removal of Basic Fuchsin[J]. Journal of Inorganic Materials, 2021, 36(12): 1330-1336.
Fig. 1 Effect of Ni/Si molar ratio on the phase composition of the products hydrothermally synthesized at 210 ℃ for 12 h with different Ni/Si molar ratios (a) 0.5 : 1; (b) 0.75 : 1; (c) 1 : 1; (d) 1.25 : 1; (e) 1.5 : 1
Fig. 3 N2 adsorption-desorption isotherms of the products hydrothermally synthesized at 210 ℃ for 12 h with different Ni/Si molar ratios (a) 0.5 : 1; (b) 0.75 : 1; (c) 1 : 1; (d) 1.25 : 1; (e) 1.5 : 1
Fig. 4 Pore size distribution derived from desorption (a) and adsorption (b) branch of the isotherm of the products hydrothermally synthesized with different Ni/Si molar ratios (a1, b1) 0.5 : 1; (a2, b2) 0.75 : 1; (a3, b3) 1 : 1; (a4, b4) 1.25 : 1; (a5, b5) 1.5 : 1
Fig. 5 Effect of alkali source on composition and morphology of the products (a1, b) Ammonia, 26.6 mmol; (a2, c) Sodium hydroxide, 26.6 mmol; (a3, d) Urea, 3.33 mmol; (a4, e) Urea, 6.66 mmol; (a5, f) Urea, 20.0 mmol
Fig. 7 Molecular structure of BF (a), Zeta potential of Ni3Si2O5(OH)4 microspheres (Ni/Si molar ratio of 1 : 1) (b), variation of the adsorption rate and capacity with adsorption time at different pH (Ni/Si molar ratio of 1 : 1) (c), and effect of Ni/Si molar ratio on the adsorption performance (d)
Ni/Si molar ratio | SBET /(m2·g-1) | Pore volume /(cm3·g-1) | Average pore diameter/nm |
---|---|---|---|
0.5 : 1 | 139.4 | 0.884 | 6.00 |
0.75 : 1 | 128.2 | 0.511 | 5.58 |
1 : 1 | 119.6 | 0.673 | 5.90 |
1.25 : 1 | 101.1 | 0.426 | 5.86 |
1.5 : 1 | 95.5 | 0.564 | 8.68 |
Table S1 Textural properties of the products
Ni/Si molar ratio | SBET /(m2·g-1) | Pore volume /(cm3·g-1) | Average pore diameter/nm |
---|---|---|---|
0.5 : 1 | 139.4 | 0.884 | 6.00 |
0.75 : 1 | 128.2 | 0.511 | 5.58 |
1 : 1 | 119.6 | 0.673 | 5.90 |
1.25 : 1 | 101.1 | 0.426 | 5.86 |
1.5 : 1 | 95.5 | 0.564 | 8.68 |
qe,exp /(mg·g-1) | Pseudo-first-order kinetic model | Pseudo-second-order kinetic model | ||||
---|---|---|---|---|---|---|
qe,calc1/(mg·g-1) | k1/min-1 | R2 | qe,calc2/(mg·g-1) | k2/(mg·g-1·min-1) | R2 | |
120.7 | 55.2 | 0.0483 | 0.8526 | 118.5 | 0.0051 | 0.9979 |
Table S2 Adsorption kinetic model parameters for the adsorption of BF on the Ni3Si2O5(OH)4 microspheres
qe,exp /(mg·g-1) | Pseudo-first-order kinetic model | Pseudo-second-order kinetic model | ||||
---|---|---|---|---|---|---|
qe,calc1/(mg·g-1) | k1/min-1 | R2 | qe,calc2/(mg·g-1) | k2/(mg·g-1·min-1) | R2 | |
120.7 | 55.2 | 0.0483 | 0.8526 | 118.5 | 0.0051 | 0.9979 |
Adsorbents | Initial concentration of BF solution/(mg·L-1) | Adsorption equilibrium time/min | Maximum adsorption capacity /(mg·g-1) | Ref. |
---|---|---|---|---|
Alkali-activated diatomite | 15 | 30 | 4.85 | [1] |
(Acrylamide-co-sodium methacrylate )-graft-chitosan gel | 125 | 180 | 6.1 | [2] |
β-cyclodextrin-carboxymethyl cellulose-graphene oxide composite | 100 | 150 | 6.5 | [3] |
Hydroxy-aluminum pillared bentonite | 100 | 10-15 | 6.6 | [4] |
Iron-manganese oxide coated kaolinite | 40 | 50 | 8.16 | [5] |
Copper vinylphosphonate | 30 | 150 | 19.29 | [6] |
Fe-ZSM-5 | 20 | 240 | 25.8 | [7] |
β-cyclodextrin-styrene-based polymer | 50 | 180 | 29.6 | [8] |
CoFe2O4-HA-ECH | 33.8 | 30 | 31.3 | [9] |
Magnetic chitosan/graphene oxide | 50 | 70 | 32.8 | [10] |
Activated carbon/ferrospinel composite | 100 | 60 | 49.9 | [11] |
Al-MCM-41 | 60 | 240 | 54 | [12] |
Ba(B2Si2O8) microspheres | 30 | 240 | 58.0 | [13] |
NiFe2O4/polythiophene nanocomposite | 50 | 30 | 76 | [14] |
Ni3Si2O5(OH)4 | 50 | 180 | 120.7 | This work |
Table S3 Comparison of the adsorption capacities for BF on various adsorbents
Adsorbents | Initial concentration of BF solution/(mg·L-1) | Adsorption equilibrium time/min | Maximum adsorption capacity /(mg·g-1) | Ref. |
---|---|---|---|---|
Alkali-activated diatomite | 15 | 30 | 4.85 | [1] |
(Acrylamide-co-sodium methacrylate )-graft-chitosan gel | 125 | 180 | 6.1 | [2] |
β-cyclodextrin-carboxymethyl cellulose-graphene oxide composite | 100 | 150 | 6.5 | [3] |
Hydroxy-aluminum pillared bentonite | 100 | 10-15 | 6.6 | [4] |
Iron-manganese oxide coated kaolinite | 40 | 50 | 8.16 | [5] |
Copper vinylphosphonate | 30 | 150 | 19.29 | [6] |
Fe-ZSM-5 | 20 | 240 | 25.8 | [7] |
β-cyclodextrin-styrene-based polymer | 50 | 180 | 29.6 | [8] |
CoFe2O4-HA-ECH | 33.8 | 30 | 31.3 | [9] |
Magnetic chitosan/graphene oxide | 50 | 70 | 32.8 | [10] |
Activated carbon/ferrospinel composite | 100 | 60 | 49.9 | [11] |
Al-MCM-41 | 60 | 240 | 54 | [12] |
Ba(B2Si2O8) microspheres | 30 | 240 | 58.0 | [13] |
NiFe2O4/polythiophene nanocomposite | 50 | 30 | 76 | [14] |
Ni3Si2O5(OH)4 | 50 | 180 | 120.7 | This work |
Langmuir isotherm model | Freundlich isotherm model | ||||
---|---|---|---|---|---|
qm/(mg·g-1) | b/(L·mg-1) | R2 | kf | 1/n | R2 |
176.7 | 4.7474 | 0.7920 | 104.9 | 0.1678 | 0.9919 |
Table S4 Corresponding fitting parameters originated from the non-linear regression by using Langmuir and Freundlich isotherm models
Langmuir isotherm model | Freundlich isotherm model | ||||
---|---|---|---|---|---|
qm/(mg·g-1) | b/(L·mg-1) | R2 | kf | 1/n | R2 |
176.7 | 4.7474 | 0.7920 | 104.9 | 0.1678 | 0.9919 |
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