Simultaneous Determination of Uric Acid, Xanthine and Hypoxanthine Based on Polyimidazole/Carbon Nitride Novel Nanocomposite†

doi:10.7503/cjcu20180717

Abstract

Abstract:

Two dimensional(2D) sheet-like structure of carbon nitride(g-C₃N₄) nanosheets containing winkles were synthesized, which were analogous to the crumpled graphene. At the same time, overoxidized polyimidazole(PImox)/g-C₃N₄ modified electrode(PImox/g-C₃N₄/GCE) was prepared by electrodeposition and oxidation at higher potentials. The composite materials were characterized by scanning electronmicroscopy(SEM) and X-ray diffractometry(XRD). The electrochemical behaviors of uric acid(UA), xanthine(XA) and hypoxanthine(HX) at the PImox/g-C₃N₄/GCE were investigated using cyclic voltammetry(CV) and differential pulse voltammetry(DPV). The calibration curves for UA, XA and HX were obtained over the ranges of 2.0—216.0, 5.0—542.0 and 5.0—778.0 μmol/L with the detection limits of 0.17, 0.30 and 0.30 μmol/L, respectively. PImox/g-C3N4/GCE has lower detection limits and wider linear range for simultaneous detection of UA, XA and HX. In addition, the modified electrode was applied to detect UA, XA and HX in real samples using standard addition method with satisfactory results. The recovery rates of the samples ranged between 98.4% and 105.2%.

Key words: Polyimidazole, Carbon nitride, Xanthine, Hypoxanthine, Uric acid

CLC Number:

O657

TrendMD:

WANG Cun,MENG Li,HUI Junmin. Simultaneous Determination of Uric Acid, Xanthine and Hypoxanthine Based on Polyimidazole/Carbon Nitride Novel Nanocomposite^†[J]. Chem. J. Chinese Universities, 2019, 40(3): 431.

Figures/Tables 10

Fig.1 SEM images of g-C3N4(A) and PImox/g-C3N4(B)

Fig.2 XRD pattern(A) and FTIR spectrum(B) of g-C3N4, EDX spectra of g-C3N4(C) and PImox/g-C3N4(D)

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.5 Differential pulse voltammetry at GCE(a), g-C3N4/GCE(b), PIm/GCE(c), PIm/g-C3N4/GCE(d) and PImox/g-C3N4/GCE(e)

Fig.6 Dependence of UA(a), XA(b) and HX(c) peak current(A) and peak potential(B) on pH values

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.

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	I_p,c=-5.82-0.137c	0.998	0.17
XA	5.0—62.0	I_p,c=-8.04-0.511c	0.987	0.30
	122.0—542.0	I_p,c=-42.8-0.0713c	0.981
HX	5.0—197.0	I_p,c=-12.9-0.149c	0.992	0.30
	267.0—778.0	I_p,c=-35.0-0.0446c	0.998

Table 2 Comparison of the response characteristics of different modified electrodes

Material	Linear range/(μmol·L^-1)			Detection limit/(μmol·L^-1)			Ref.
Material	UA	XA	HX	UA	XA	HX	Ref.
Poly(bromocresol purple)	0.5—120	0.1—100	0.2—80	0.2	0.06	0.12	[13]
Overoxidized dopamine polymer and	1.8—238	5.2—289	3.8—293	0.6	1.7	1.3	[23]
3,4,9,10-perylenetetracarboxylic acid
Poly(2-amino-1,3,4-thiadiazole)	5—45	5—45		0.19	0.59		[32]
Copper(Ⅱ)-polydopamine	60—1680			24.6			[37]
Functional single wall carbon nanotubes	0.1—100	0.2—100	0.8—100	0.08	0.146	0.562	[38]
Ru(DMSO)₄Cl₂ nano-aggregated	100—700	50—500	50—500	0.372	2.35	2.37	[39]
nafion membrane
Overoxidized polyimidazole/carbon nitride	2.0—216	5.0—542	5.0—778	0.17	0.30	0.30	This work

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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