化工学报 ›› 2022, Vol. 73 ›› Issue (7): 3057-3067.DOI: 10.11949/0438-1157.20220329
朱江伟1(),马鹏飞1(),杜晓1,杨言言2,郝晓刚1(),罗善霞3
收稿日期:
2022-03-03
修回日期:
2022-05-19
出版日期:
2022-07-05
发布日期:
2022-08-01
通讯作者:
马鹏飞,郝晓刚
作者简介:
朱江伟(1997—),男,硕士研究生,基金资助:
Jiangwei ZHU1(),Pengfei MA1(),Xiao DU1,Yanyan YANG2,Xiaogang HAO1(),Shanxia LUO3
Received:
2022-03-03
Revised:
2022-05-19
Online:
2022-07-05
Published:
2022-08-01
Contact:
Pengfei MA,Xiaogang HAO
摘要:
磷是一种不可再生资源。为解决现有磷污染以及磷资源流失等问题,通过油浴与热化学还原相结合的方法,成功制备出一种NiFe-LDH/rGO电活性杂化膜材料。使用电化学方法,在氧化还原电位的控制下,Ni、Fe(Ⅱ/Ⅲ)双金属发生核外电子的跃迁,高价态的Ni、Fe(Ⅲ)与
中图分类号:
朱江伟, 马鹏飞, 杜晓, 杨言言, 郝晓刚, 罗善霞. 基于可变价NiFe-LDH/rGO对磷酸根离子的特异性电控分离[J]. 化工学报, 2022, 73(7): 3057-3067.
Jiangwei ZHU, Pengfei MA, Xiao DU, Yanyan YANG, Xiaogang HAO, Shanxia LUO. Specific electronically controlled separation of phosphate anions based on variable valence NiFe-LDH/rGO[J]. CIESC Journal, 2022, 73(7): 3057-3067.
图1 (a)~(c) 不同放大倍数下LDH的SEM图; (d) LDH/GO杂化材料的SEM图; (e)、(f)不同放大倍数下LDH/rGO杂化材料的SEM图
Fig.1 (a)—(c) SEM images of LDH at different magnification; (d) SEM image of LDH/GO hybrid matrials;(e), (f) SEM images of LDH/rGO hybrid matrials at different magnification
图3 (a) 0.1 mol·L-1 Na3PO4溶液中NiFe-LDH/rGO杂化膜在50 mV·s-1扫速下的CV曲线; (b) 0.1 mol·L-1 Na3PO4溶液中NiFe-LDH/rGO杂化膜阳极和阴极峰值电流随扫速平方根的变化规律
Fig.3 (a) CV curves of NiFe-LDH/rGO hybrid films in 0.1 mol·L-1 Na3PO4 solution at 50 mV·s-1; (b) The variation of anode and cathode peak current of the NiFe-LDH /rGO hybrid film with the square root of scanning speed in 0.1 mol·L-1 Na3PO4 solution
I/mA | |||||
---|---|---|---|---|---|
Ni(阳极) | Ni(阴极) | Fe(阳极) | Fe(阴极) | ||
10 | 3.162 | 0.167 | -0.232 | -0.038 | -0.188 |
20 | 4.472 | 0.291 | -0.362 | -0.021 | -0.241 |
30 | 5.477 | 0.390 | -0.481 | 0.002 | -0.294 |
40 | 6.324 | 0.500 | -0.590 | 0.020 | -0.342 |
50 | 7.071 | 0.589 | -0.693 | 0.047 | -0.389 |
表1 0.1 mol·L-1 Na3PO4溶液中不同扫速对应的阴、阳极峰值电流
Table 1 Cathodic and anodic peak currents corresponding to different scanning rates in 0.1 mol·L-1 Na3PO4 solution
I/mA | |||||
---|---|---|---|---|---|
Ni(阳极) | Ni(阴极) | Fe(阳极) | Fe(阴极) | ||
10 | 3.162 | 0.167 | -0.232 | -0.038 | -0.188 |
20 | 4.472 | 0.291 | -0.362 | -0.021 | -0.241 |
30 | 5.477 | 0.390 | -0.481 | 0.002 | -0.294 |
40 | 6.324 | 0.500 | -0.590 | 0.020 | -0.342 |
50 | 7.071 | 0.589 | -0.693 | 0.047 | -0.389 |
图4 0.1 mol·L-1 Na3PO4溶液中NiFe-LDH/rGO杂化膜在初始(上)、氧化(中)与还原(下)状态时的XPS谱图
Fig.4 XPS spectra of NiFe-LDH/rGO hybrid film in 0.1 mol·L-1 Na3PO4 solution at initial (top), oxidation (middle) and reduction (bottom) states
图5 不同初始浓度下NiFe-LDH/rGO杂化膜对PO43-的吸附容量
Fig.5 The adsorption capacity of NiFe-LDH/rGO hybrid films for phosphate anionsat different initial concentrations
C0/(mg·L-1) | qe(exp)/( mg·g-1) | Pseudo-first-order | Pseudo-second-order | ||||
---|---|---|---|---|---|---|---|
k1/min-1 | qe(cal)/( mg·g-1) | R2 | k2/min-1 | qe(cal)/(mg·g-1) | R2 | ||
101.58 | 76.35 | 0.011 | 60.138 | 0.948 | 1.55×10-4 | 90.090 | 0.997 |
192.72 | 121.74 | 0.017 | 105.047 | 0.866 | 8.87×10-5 | 149.477 | 0.986 |
301.93 | 200.18 | 0.018 | 174.493 | 0.971 | 4.38×10-5 | 236.967 | 0.996 |
512.36 | 269.68 | 0.012 | 265.219 | 0.966 | 4.57×10-5 | 282.486 | 0.996 |
表2 不同浓度下NiFe-LDH/rGO杂化膜对PO43-的动力学模型参数和相关因子
Table 2 Kinetic model parameters and related factors of phosphate anions induced by NiFe-LDH/rGO hybrid film at different concentrations
C0/(mg·L-1) | qe(exp)/( mg·g-1) | Pseudo-first-order | Pseudo-second-order | ||||
---|---|---|---|---|---|---|---|
k1/min-1 | qe(cal)/( mg·g-1) | R2 | k2/min-1 | qe(cal)/(mg·g-1) | R2 | ||
101.58 | 76.35 | 0.011 | 60.138 | 0.948 | 1.55×10-4 | 90.090 | 0.997 |
192.72 | 121.74 | 0.017 | 105.047 | 0.866 | 8.87×10-5 | 149.477 | 0.986 |
301.93 | 200.18 | 0.018 | 174.493 | 0.971 | 4.38×10-5 | 236.967 | 0.996 |
512.36 | 269.68 | 0.012 | 265.219 | 0.966 | 4.57×10-5 | 282.486 | 0.996 |
图6 ESIX (rGO)、 IX (NiFe-LDH/rGO)、 ESIX (NiFe-LDH)和ESIX (NiFe-LDH/rGO)对磷酸盐阴离子的吸附容量曲线
Fig.6 Phosphate anions uptake capacity curves of ESIX (rGO), IX (NiFe-LDH/rGO), ESIX (NiFe-LDH) and ESIX (NiFe-LDH/rGO)
图7 (a)NiFe-LDH/rGO杂化膜在初始浓度均为300 mg·L-1下对PO43-、 SO42-、 NO3-和Cl-的竞争性吸附; (b) 0.30 mol·L-1 NaNO3, 0.30 mol·L-1 NaCl, 0.15 mol·L-1 Na2SO4和0.10 mol·L-1 Na3PO4电解液中NiFe-LDH/rGO复合膜的CV曲线
Fig.7 (a) Competitive adsorption of PO43-, SO42-, NO3-, and Cl- for NiFe-LDH/rGO hybrid films at an initial concentration of 300 mg·L-1; (b) CV curves of NiFe-LDH/rGO hybrid film in 0.30 mol·L-1 NaNO3, 0.30 mol·L-1 NaCl, 0.15 mol·L-1 Na2SO4, and 0.10 mol·L-1 Na3PO4 electrolytic solutions
Anion | Adsorption capacity/(mg·g-1) | Separation coefficient (KD) | Relative separation factor (α) |
---|---|---|---|
178.012 | 0.865 | 1 | |
70.871 | 0.274 | 3.163 | |
50.336 | 0.185 | 4.678 | |
Cl- | 45.248 | 0.156 | 5.551 |
表3 NiFe-LDH/rGO杂化膜在初始浓度均为300 mg·L-1下对PO43-、SO42-、NO3-和Cl-的分离系数和相对分离因子
Table 3 Separation coefficients and relative separation factors of PO43-, SO42-, NO3-, and Cl- of the NiFe-LDH/rGO hybrid film at the initial concentration of 300 mg·L-1
Anion | Adsorption capacity/(mg·g-1) | Separation coefficient (KD) | Relative separation factor (α) |
---|---|---|---|
178.012 | 0.865 | 1 | |
70.871 | 0.274 | 3.163 | |
50.336 | 0.185 | 4.678 | |
Cl- | 45.248 | 0.156 | 5.551 |
图8 NiFe-LDH/rGO杂化膜在300 mg·L-1的磷酸钠 (吸附) 和硝酸钠 (脱附) 溶液中对PO43-的吸脱附容量(a)和再生效率(b)
Fig.8 The adsorption and desorption capacity (a) and regeneration rate (b) of NiFe-LDH /rGO hybrid film for phosphate ions in 300 mg·L-1 sodium phosphate and sodium nitrate solutions, respectively
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