高等学校化学学报 ›› 2019, Vol. 40 ›› Issue (3): 431.doi: 10.7503/cjcu20180717
收稿日期:
2019-10-22
出版日期:
2019-01-24
发布日期:
2019-01-24
作者简介:
联系人简介: 王 存, 女, 讲师, 主要从事纳米材料及电化学生物传感器方面的研究. E-mail:
基金资助:
WANG Cun*(), MENG Li, HUI Junmin
Received:
2019-10-22
Online:
2019-01-24
Published:
2019-01-24
Contact:
WANG Cun
E-mail:wangcun5224@126.com
摘要:
以三聚氰胺为原料, 采用热聚合法合成了类石墨烯状二维片状氮化碳(g-C3N4)纳米材料; 通过电沉积和高电位氧化的方法制得氧化聚咪唑(PImox)/g-C3N4修饰电极(PImox/g-C3N4/GCE). 采用扫描电子显微镜(SEM)和X射线粉末衍射仪(XRD)对g-C3N4纳米材料进行了表征; 通过循环伏安法(CV)和差分脉冲伏安法(DPV)考察了尿酸(UA)、 黄嘌呤(XA)和次黄嘌呤(HX)在该电极上的电化学行为. 结果表明, UA, XA和HX的检测线性范围分别为2.0~216.0, 5.0~542.0和5.0~778.0 μmol/L; 检出限分别为0.17, 0.30和0.30 μmol/L. 将该修饰电极用于实际样品(血清和尿液)中UA, XA和HX的同时测定, 加标回收率为98.4%~105.2%.
中图分类号:
TrendMD:
王存, 孟丽, 惠俊敏. 聚咪唑/氮化碳新型纳米复合材料修饰电极对尿酸、 黄嘌呤和次黄嘌呤的同时检测. 高等学校化学学报, 2019, 40(3): 431.
WANG Cun,MENG Li,HUI Junmin. Simultaneous Determination of Uric Acid, Xanthine and Hypoxanthine Based on Polyimidazole/Carbon Nitride Novel Nanocomposite†. Chem. J. Chinese Universities, 2019, 40(3): 431.
Fig.3 Cyclic voltammograms(A) and electrochemical impedance analysis(B) at GCE(a), PIm/GCE(b),g-C3N4/GCE(c), PIm/g-C3N4/GCE(d) and PImox/g-C3N4/GCE(e)
Fig.4 CVs of g-C3N4/GCE(A), PIm/GCE(B), PImox/g-C3N4/GCE(C) in 5.0 mmol/L K3[Fe(CN)6]+ 5.0 mmol/L K4[Fe(CN)6] at different scan rates and plots of anodic peak current(Ip,a) vs. square root of scan rate of g-C3N4/GCE(A'), PIm/GCE(B') and PImox/g-C3N4/GCE(C')(A)—(C) Scan rate from inner to outer: 0.01, 0.05, 0.10, 0.15, 0.20, 0.25, 0.30, 0.35, 0.40 and 0.45 V/s.
Fig.7 DPV curves at PImox/g-C3N4/GCE in 0.1 mol/L PBS solution(pH=4.0)[(A)—(C)] and plots of Ip vs. concentration for UA(A'), XA(B') and HX(C')(A) 15 μmol/L XA, 15 μmol/L HX, concentrations of UA from inner to outer: 2, 6, 12, 20, 30, 42, 57, 74, 92, 112, 134, 159, 186, 216 μmol/L; (B) 50 μmol/L UA, 15 μmol/L HX, concentrations of XA from inner to outer: 5, 15, 25, 35, 47, 62, 122, 182, 272, 392, 542 μmol/L; (C) 50 μmol/L UA, 10 μmol/L XA, concentrations of HX from inner to outer: 5, 15, 30, 47, 67, 87, 117, 147, 197, 267, 357, 468, 598, 778 μmol/L.
Analyte | Linear range/(μmol·L-1) | Regression equation | Correlation coefficient | Detection limit/(μmol·L-1) |
---|---|---|---|---|
UA | 2.0—216.0 | Ip,c=-5.82-0.137c | 0.998 | 0.17 |
XA | 5.0—62.0 | Ip,c=-8.04-0.511c | 0.987 | 0.30 |
122.0—542.0 | Ip,c=-42.8-0.0713c | 0.981 | ||
HX | 5.0—197.0 | Ip,c=-12.9-0.149c | 0.992 | 0.30 |
267.0—778.0 | Ip,c=-35.0-0.0446c | 0.998 |
Table 1 Linear range, regression equation, correlation coefficient and detection limit for UA, XA and HX
Analyte | Linear range/(μmol·L-1) | Regression equation | Correlation coefficient | Detection limit/(μmol·L-1) |
---|---|---|---|---|
UA | 2.0—216.0 | Ip,c=-5.82-0.137c | 0.998 | 0.17 |
XA | 5.0—62.0 | Ip,c=-8.04-0.511c | 0.987 | 0.30 |
122.0—542.0 | Ip,c=-42.8-0.0713c | 0.981 | ||
HX | 5.0—197.0 | Ip,c=-12.9-0.149c | 0.992 | 0.30 |
267.0—778.0 | Ip,c=-35.0-0.0446c | 0.998 |
Material | Linear range/(μmol·L-1) | Detection limit/(μmol·L-1) | Ref. | ||||
---|---|---|---|---|---|---|---|
UA | XA | HX | UA | XA | HX | ||
Poly(bromocresol purple) | 0.5—120 | 0.1—100 | 0.2—80 | 0.2 | 0.06 | 0.12 | [ |
Overoxidized dopamine polymer and | 1.8—238 | 5.2—289 | 3.8—293 | 0.6 | 1.7 | 1.3 | [ |
3,4,9,10-perylenetetracarboxylic acid | |||||||
Poly(2-amino-1,3,4-thiadiazole) | 5—45 | 5—45 | | 0.19 | 0.59 | | [ |
Copper(Ⅱ)-polydopamine | 60—1680 | | | 24.6 | | | [ |
Functional single wall carbon nanotubes | 0.1—100 | 0.2—100 | 0.8—100 | 0.08 | 0.146 | 0.562 | [ |
Ru(DMSO)4Cl2 nano-aggregated | 100—700 | 50—500 | 50—500 | 0.372 | 2.35 | 2.37 | [ |
nafion membrane | |||||||
Overoxidized polyimidazole/carbon nitride | 2.0—216 | 5.0—542 | 5.0—778 | 0.17 | 0.30 | 0.30 | This work |
Table 2 Comparison of the response characteristics of different modified electrodes
Material | Linear range/(μmol·L-1) | Detection limit/(μmol·L-1) | Ref. | ||||
---|---|---|---|---|---|---|---|
UA | XA | HX | UA | XA | HX | ||
Poly(bromocresol purple) | 0.5—120 | 0.1—100 | 0.2—80 | 0.2 | 0.06 | 0.12 | [ |
Overoxidized dopamine polymer and | 1.8—238 | 5.2—289 | 3.8—293 | 0.6 | 1.7 | 1.3 | [ |
3,4,9,10-perylenetetracarboxylic acid | |||||||
Poly(2-amino-1,3,4-thiadiazole) | 5—45 | 5—45 | | 0.19 | 0.59 | | [ |
Copper(Ⅱ)-polydopamine | 60—1680 | | | 24.6 | | | [ |
Functional single wall carbon nanotubes | 0.1—100 | 0.2—100 | 0.8—100 | 0.08 | 0.146 | 0.562 | [ |
Ru(DMSO)4Cl2 nano-aggregated | 100—700 | 50—500 | 50—500 | 0.372 | 2.35 | 2.37 | [ |
nafion membrane | |||||||
Overoxidized polyimidazole/carbon nitride | 2.0—216 | 5.0—542 | 5.0—778 | 0.17 | 0.30 | 0.30 | This work |
Sample | Dilution factor | Analyte | Detected/(μmol·L-1) | Added/(μmol·L-1) | Found/(μmol·L-1) | Recovery(%) |
---|---|---|---|---|---|---|
Urine 1 | 50 | UA | 30.0 | 20.0 | 50.2 | 100.4 |
50 | XA | | 40.0 | 39.7 | 99.2 | |
50 | HX | | 30.0 | 31.1 | 103.7 | |
Urine 2 | 100 | UA | 25.0 | 80.0 | 105.5 | 100.5 |
100 | XA | | 100.0 | 98.6 | 98.6 | |
100 | HX | | 100.0 | 105.2 | 105.2 | |
Serum 1 | 150 | UA | | 90.0 | 89.2 | 99.1 |
150 | XA | | 50.0 | 49.3 | 98.6 | |
150 | HX | | 50.0 | 50.9 | 101.8 | |
Serum 2 | 200 | UA | | 150.0 | 147.6 | 98.4 |
200 | XA | | 400.0 | 398.7 | 99.7 | |
200 | HX | | 500.0 | 498.9 | 99.8 |
Table 3 Determination of UA, XA and HX in human serum and urine samples
Sample | Dilution factor | Analyte | Detected/(μmol·L-1) | Added/(μmol·L-1) | Found/(μmol·L-1) | Recovery(%) |
---|---|---|---|---|---|---|
Urine 1 | 50 | UA | 30.0 | 20.0 | 50.2 | 100.4 |
50 | XA | | 40.0 | 39.7 | 99.2 | |
50 | HX | | 30.0 | 31.1 | 103.7 | |
Urine 2 | 100 | UA | 25.0 | 80.0 | 105.5 | 100.5 |
100 | XA | | 100.0 | 98.6 | 98.6 | |
100 | HX | | 100.0 | 105.2 | 105.2 | |
Serum 1 | 150 | UA | | 90.0 | 89.2 | 99.1 |
150 | XA | | 50.0 | 49.3 | 98.6 | |
150 | HX | | 50.0 | 50.9 | 101.8 | |
Serum 2 | 200 | UA | | 150.0 | 147.6 | 98.4 |
200 | XA | | 400.0 | 398.7 | 99.7 | |
200 | HX | | 500.0 | 498.9 | 99.8 |
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