Research Article

Received: 31 January 2009, Revised: 26 March 2009, Accepted: 28 March 2009, Published online in Wiley Interscience: 7 July 2009

(www.interscience.wiley.com) DOI 10.1002/bio.1140

Copyright © 2009 John Wiley & Sons, Ltd. Luminescence 2010; 25: 36–42

36

John Wiley & Sons, Ltd.

New luminol chemiluminescence reaction using diperiodatoargentate as oxidate for the determination of amikacin sulfateNew luminol chemiluminescence reaction

Chunyan Yang, Zhujun Zhang* and Jinli Wang

ABSTRACT: A new chemiluminescence (CL) reaction between luminol and diperiodatoargentate {K2 [Ag (H2IO6) (OH) 2]} wasobserved in alkaline medium. The CL intensity could be greatly enhanced by amikacin sulfate. Therefore a new CL method forthe determination of amikacin sulfate was built by combining with flow injection technology. A possible mechanism of theCL reaction was proposed via the investigation of the CL kinetic characteristics, the CL spectrum and the UV absorptionspectra of some related substance. The concentration range of linear response was 5.1 ×××× 10−−−−8 to 5.1 ×××× 10−−−−6 mol L−−−−1 with a detec-tion limit of 1.9 ×××× 10−−−−8 mol L−−−−1 (3σσσσ). The proposed method had good reproducibility with a relative standard deviation of2.8% (n = 7) for 5.1 ×××× 10−−−−7 mol L−−−−1 of amikacin sulfate. It was successfully applied to determine amikacin sulfate in serum.Copyright © 2009 John Wiley & Sons, Ltd.

Keywords: chemiluminescence; amikacin sulfate; luminol; diperiodatoargentate

Introduction

Amikacin sulfate (AKS) (Fig. 1) is a semisynthetic, water-soluble,broad-spectrum aminoglycoside antibiotic. It was developed toresolve drug resistance to gentamicin, kanamycin and tobramy-cin because the amikacin molecule has fewer points susceptibleto enzymatic attack than the other aminoglycosides. However,like other aminoglycosides, amikacin has a comparatively narrowsafety margin. It may cause both ototoxicity and nephrotoxicityin patients, especially during long-term therapy. Its therapeuticplasma concentration is in the range of 1.0–2.0 × 10−5 mol L−1.[1]

Monitoring of amikacin levels in plasma is required for therapeu-tic and toxic control, so a simple, sensitive and specific methodfor trace analysis in plasma is essential.

Some methods have been adopted for the determinationof amikacin, including immunoassay,[2] spectrophotometry,[3]

fluorescence method,[4–6] liquid chromatography,[1,7–11] capillaryelectrophoresis[12] and CL[13] voltammetry.[14] Because of lack ofvolatility and chromophore, most methods use derivatization toproduce volatile, UV–vis absorbing or fluorescent derivatives.These methods often suffer from a variety of disadvantages,such as being sophisticated, time-consuming or expensive. CL

analysis has been widely used in many fields such as pharma-ceutical science, environmental science and life science owingto its attracting features, including wide linear dynamic range,low detection limit, simple and inexpensive instruments and rapidanalysis speed. Although the CL method has been reported, ithas suffered from the disadvantage of low sensitivity. The oxida-tion of luminol (3-aminophthalhydrazide) in alkaline mediumis one of the most efficient CL reactions. In this CL system, thecommon oxidants used include hydrogen peroxide, oxygen,potassium permanganate, ferricyanide, periodate and oxygenfree radicals.[15–21] Some transition metals in the highest oxida-tion states, such as trivalent silver, can be stabilized by chelatingwith suitable polydentate ligands. Diperiodatoargentate (III)(DPA) is a powerful oxidizing agent in alkaline medium, with areduction potential of 1.74 V.[22] P. J. Rao et al.[22,23] have used DPAas an oxidizing agent to study kinetics of oxidation of variousorganic substrates. In the later part of the twentieth century, thekinetics of oxidation of various organic and inorganic substrateswere studied by Ag (III) species, which may be due to the strongversatile nature of the two electron oxidants. Although thereare many reports concerning the use of DPA as an oxidant inalkaline medium, the use of DPA in CL analysis was never studied.In this paper, it was found that the reaction of DPA and luminolcan emit chemiluminescence with a low concentration of luminol,but CL is hardly observed when luminol with the same concen-tration reacts with other oxidants. In the experiments, it wasfound that the CL intensity of the luminol–DPA reaction can begreatly enhanced by AKS. In the same condition, the CL intensity

Figure 1. The structure of AKS.

* Correspondence to: Zhujun Zhang, College of Chemistry and MaterialsScience, Shaanxi Normal University, Xi’an 710062, People’s Republic ofChina. E-mail: zhangzhujun18@yahoo.com.cn

College of Chemistry and Materials Science, Shaanxi Normal University,Xi’an 710062, People’s Republic of China

New luminol chemiluminescence reaction

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of the luminol–H2O2–metal ion system, which is one of the mostimportant luminol CL systems, is much lower than the luminol–DPA–AKS CL intensity. Therefore, a new method for the determi-nation of AKS with high sensitivity and selectivity was developedand successfully applied to determine AKS in serum.

Experimental

Materials

Luminol (5-amino-2, 3-dihydro-1, 4-phthalazinedione, 99%) wasobtained from Shaanxi Normal University, Xi’an, China, amikacinsulfate from Drug and Biological Products Examination Bureauof China, Beijing, potassium persulfate from Shanghai AijianChemical Reagent Company, and potassium hydroxide, hydrogenperoxide, sodium nitrate, sodium periodate and silver nitratefrom Shanghai Chemical Reagent Company. All the reagents wereof analytical grade and deionized and double-distilled waterwas used throughout.

A stock solution of 1.3 × 10−4 mol L−1 AKS was prepared bydissolving an appropriate amount of AKS in double-distilledwater and diluting to the mark with water. The 1.0 × 10−2 mol L−1

luminol stock solution was prepared by dissolving 1.772 g luminolin 1 L 0.1 mol L−1 carbonate buffer and left to stand for approxi-mately 24 h before use. The luminol solution was stable for atleast 1 month when stored in the dark.

Apparatus

The CL-FIA system used in this work is shown in Fig. 2. Two peri-staltic pumps (HL-2, Shanghai Huxi, China) were used to deliverall the chemicals at a flow rate of 1.5 mL min−1. Polytetrafluor-oethylene (PTFF) flow tubes (0.8 mm i.d.) were used to connectall the components in the flow system. Injection was done usingan eight-way injection valve equipped a sample loop (90 μL).The flow cell was made by coiling 20 cm of colorless glass tube(2 mm i.d.) into a spiral disk shape and was located directly fac-ing the window of the photomultiplier tube (PMT). The CL signalwas monitored using an IFFM-A multifunction chemilumines-cence analyzer (Remex Analytical Instrument Co. Ltd. Xian,China). The UV absorbance was detected with the TU1901 UV–visspectrophotometer (Beijing Purkinje General Instrument Co., Ltd.

China). The chemiluminescence spectrum was monitored usingan F-4600 fluorescence spectrophotometer (Shimadzu, Japan).

Synthesis of diperiodatoargentate (III)

In brief, AgNO3 (1.36 g), NaIO4 (3.42 g), K2S2O8 (3 g) and KOH (8 g)were taken in a 500 mL round-bottomed flask. A 100 mL aliquotof demineralized water was added to this mixture. It was heatedto boiling while stirring. After 15 min of boiling an orangish-yellowfroth was obtained and the mixture was heated for another15 min. The mixture was left to cool to room temperature andfiltered through a Gooch crucible (the complex is instantane-ously reduced on a filter paper). The solution was cooled in aniced bath to eliminate as much potassium sulfate as possibleand the solution filtered again while cold. The resultingorangish-red clear filtrate was left to reach room temperature.In order to isolate the complex, 40 mL of NaNO3 solution (50%,in excess) was added to the solution and the mixture left tocrystallize. Almost immediately crystals started appearing andcrystallization was complete when the supernatant liquid wascolorless. The crystals were filtered and washed several timeswith demineralized water until the complex itself started todissolve, indicated by orange-red drops being formed underthe crucible. In this way one can be sure of eliminating sodiumand potassium hydroxide since this complex is insoluble inconcentrated hydroxide solution.[24]

The DPA solutions were freshly prepared by dissolving amountof complex in 1.0 × 10−2 mol L−1 KOH solution before use. Thecomplex was characterized by the UV–visible spectrum, whichshowed two absorption maxima at 362 and 253nm (Fig. 8). Theconcentration of DPA solution was determinated by the absor-bency at 362 nm (molar absorptivity ε = 1.26 × 104 mol−1 L cm−1).

Procedures

The flow injection system used in this work is shown in Fig. 2.The distilled water delivered the AKS or the sample solution in thesample loop to react with the mixture of luminol and DPA in theflow cell to produce strong CL. The CL signal was also detectedby IFFS-A multifunction chemiluminescence analyzer.

Results and discussion

The comparison of CL intensity of luminol with different

oxidant or catalyzer

The oxidation of luminol in alkaline medium is one of the mostimportant CL reactions. Luminol undergoes CL reactions with arange of oxidants. For some oxidants, e.g. hydrogen peroxide,one of the most well-known CL reactions, a catalyst, such asCu2+, Cr3+, Ni2+, is also required for CL. In this paper, it was foundthat DPA has strong redox with luminol to emit chemilumines-cence. The CL intensity was very great, so that the CL was observedeven in the absence of a catalyst, co-oxidant or other enhancerof CL. In particular, the chemiluminescence was obviouslydetected when the concentration of luminol was only up to1.0 × 10−8 mol L−1, but the CL of luminol in same concentrationwith other oxidants could hardly be observed; even when theconcentration of luminol was up to 1.0 × 10−6 mol L−1 (Fig. 3). Inthe experiments, it was found that AKS greatly enhanced theCL intensity of the luminol–DPA reaction. Therefore the reactionof DPA and luminol catalyzed by AKS can emit strong CL intensity

Figure 2. Schematic diagram of the CL–FIA system. a, AKS solution or samples; b,distilled water; c, luminol solution; d, DPA solution; V, injection valve; F, spiral glassflow cell; PMT, photomultiplier tube; pump1 and pump2, peristaltic pumps.

C. Yang et al.

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with lower concentration of luminol than other luminol–oxidant–catalyst systems. For example, the luminol–DPA–AKS systemcan obtain excellent experimental results with lower luminolconcentration than luminol–H2O2–metal ion (Cu2+, Cr3+, Ni2+)systems, which is one of the most well-known luminol CLreactions (Fig. 4). Therefore this method possesses a particularadvantage, which is lower reagent consumption than otherluminol CL systems.

Kinetics curve of the CL reaction

Before carrying out the flow-injection method, the kineticcharacteristics of the proposed CL reaction were studied byusing the batch method. In the batch mode, the experimentalparameters were kept constant; the typical response curve(intensity vs times) of luminol (3.0 × 10−7 mol L−1) CL reactioncatalyzed by AKS (1.0 × 10−5 mol L−1) in the present DPA (1.0 ×10−4 mol L−1) was recorded to study the kinetic characteristic of

the CL reaction. Figure 5 demonstrates that the CL reaction wasa very quick reaction. The CL intensity peak appeared within 3 ssince the AKS solution was injected. The CL signals woulddecrease to baseline at within 10 s. The kinetic curve indicatedthat the CL system was rapid, sensitive enough and suitable forperforming determination of AKS.

Optimization of CL reaction conditions

Stability of DPA. Trivalent argentine is in the highest oxidationstate, which should be stabilized by chelating with suitablepolydentate ligand due to the fact of its limited stability, butDPA with low concentration in aqueous solution is also notstable. The stability of DPA in aqueous solution was studiedby varying CL intensity within 2 h (Fig. 6). As can be seen, the CLintensity varied little within 2 h when the DPA concentrationwas up to 1.0 × 10−6 mol L−1. The time of stability met the testrequirement.

Figure 3. The comparison of CL intensity of luminol with different oxidant. A,DPA, 5.0 × 10−5 mol L−1; B, H2O2, 5.0 × 10−5 mol L−1; C, KIO4, 5.0 × 10−5 mol L−1; D,K3Fe(CN)6, 5.0 × 10−5 mol L−1; negative high voltage, 450 V.

Figure 4. Effect of luminol concentration on CL intensity in luminol–DPA–AKSand luminol–H2O2–metal ion system. A, Luminol + DPA (5.0 × 10−5 mol L−1) + AKS(5.0 × 10−5 mol L−1); B–D, luminol + H2O2 (5.0 × 10−5 mol L−1) + Co (II), Cu (II), Cr (III)(5.0 × 10−5 mol L−1); negative high voltage, 450 V.

Figure 5. Kinetics curves of luminol–DPA catalyzed by AKS. Luminol: 3.0 ×10−7 mol L−1; DPA: 1.0 × 10−4 mol L−1; AKS: 1.0 × 10−5 mol L−1.

Figure 6. The stability of DPA. Luminol, 2.0 × 10−7 mol L−1; AKS, 1.0 × 10−6 mol L−1;DPA, 6.0 × 10−7 mol L−1 (A); 8.0 × 10−7 mol L−1 (B); 1.0 × 10−6 mol L−1 (C); 2.0 × 10−6 mol L−1

(D); 4.0 × 10−6 mol L−1 (E).

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The effect of DPA concentration. The effect of DPA concentrationon the CL intensity was examined in the range from 1.0 × 10−5

to 2.5 × 10−4 mol L−1. It was found that the CL intensity increasedwith DPA concentration up to 5.0 × 10−5 mol L−1; decreasingthereafter because the higher concentration of DPA resultedin self-absorption. Therefore, 5.0 × 10−5 mol L−1 of DPA wasselected.

The effect of potassium hydroxide concentration in DPA solu-

tion. DPA can be used as an oxidant in aqueous alkaline medium.The effect of potassium hydroxide in DPA solution on the CLintensity was examined. The concentration of potassium hydrox-ide was studied at different concentrations from 8.0 × 10−4 to4.0 × 10−2 mol L−1. It was found that the CL intensity increaseswith potassium hydroxide concentration up to 2.0 × 10−3 mol L−1,thereafter increasing little. To obtain the highest sensitivity andaccuracy, 2.0 × 10−3 mol L−1 potassium hydroxide was selected asan optimum concentration.

The effect of luminol concentration. The effect of luminolconcentration on the signal/noise (S/N) ratio was investigatedfor the range 6.0 × 10−8 to 1.0 × 10−6 mol L−1. It was found that theS/N ratio reached the maximum value when the concentrationof luminol was 6.0 × 10−7 mol L−1. Therefore 6.0 × 10−7 mol L−1 lumi-nol was used as an optimum concentration.

The effect of potassium hydroxide concentration in luminol

solution. The CL reaction occurred in alkaline solution. In theexperiments, the alkalinity of the reaction medium was adjustedby preparing luminol with a suitable concentration of potassiumhydroxide. The effect of potassium hydroxide concentrationin the range 6.0 × 10−4 to 4.0 × 10−3 mol L−1 was examined. When2.0 × 10−3 mol L−1 potassium hydroxide was used, the CL reactionhad the maximum CL intensity.

Analytical parameters

Under the optimum experimental conditions, the CL intensityshowed linearly with the amikacin sulfate concentration from5.1 × 10−8 to 5.1 × 10−6 mol L−1 and the detection limit was 1.9 ×10−8 mol L−1 (3σ) with a relative standard deviation for 5.1 ×10−7 mol L−1 amikacin sulfate solution 2.8% (n = 7). The regres-sion equation was ΔI = 18.431c − 29.859 [c being the amikacinsulfate concentration (1.0 × 10−8 mol L−1) and ΔI being the rela-tive height of the CL intensity] with R2 = 0.994 (n = 11).

Interferences study

In order to assess the analytical applicability of the method, theinterference of some substances existing in serum was studiedby analyzing synthetic samples containing 1.3 × 10−7 mol L−1 AKSand various additives. The tolerable limit of an interferingspecies was taken as a relative error less than 5%. It showedthat, more than 1000-fold excess of K+, Na+, Ca2+, Cl−, SO4

2−, creat-inine, pyruvic acid, 100-fold starch, carbamide, oxalate, 50-foldFe3+, 10-fold citrate, lactose, glucose, xanthine, 1-fold ascorbicacid and 0.1-fold uric acid did not affect determination. Interfer-ence of protein in human serum could also be ignored whenhuman serum was ultrafiltered, thus implying that the presentmethod may be directly applied to the determination of AKS inhuman serum.

Applications

The proposed method was utilized for the determination of AKSin human serum. A 2 mL blank serum sample was collected andtransferred into an ultra-filtration tube, then centrifuged at10 000 rpm for 10 min at 4°C. Then 1 mL filtrate was transferredinto a 100 mL volumetric flask and diluted to the mark with double-distilled water. The blank serum was injected to the CL system,and then the blank signal recorded. A known amount of AKSstandard solution was added to 10 mL diluted serum. The amountof AKS in human serum and the recovery obtained are shown inTable 1. The results of the proposed method agree well withthose obtained by the spectrophotometric method[25] (Table 2).

Mechanism discussion

In order to explore the possible mechanism of this CL enhancingphenomena, the following experiments were performed. Firstly,the CL spectrum was drawn using an F-4600 fluorescence spec-trophotometer (Shimadzu, Japan) combined with a flow-injectionsystem, whose light entrance slot was shut. The maximum emissionspectra of luminol–DPA CL reaction in the absence and presenceof AKS appeared at 425 nm, and a much higher CL peak wasobserved in the AKS presence (Fig. 7). It is well known that 3-aminophthalate is the luminophor, and the maximum emissionof CL reaction is at 425 nm. This indicated that the CL spectrawere independent of AKS. Therefore the CL emitter in the bothCL reactions between luminol and DPA with and without AKS is3-aminophthalate, which is the oxidation product of luminol.

Table 1. Results of recovery tests on human serum

Sample Found (10−8 mol L−1)

Added (10−8 mol L−1)

Total found (10−8 mol L−1)

Recovery(%)

RSD(%)

7.7 15.6 105 3.11 7.5 10.2 17.1 94 2.5

12.8 20.7 103 3.325.6 45.0 104 3.0

2 18.5 51.2 68.1 97 3.776.7 96.2 101 1.576.7 114.9 103 3.9

3 35.8 102.3 135.7 98 1.3127.9 166.0 102 1.4

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Series experiments have been performed to determine somemore detail of the AKS enhanced luminol–DPA CL reaction.Firstly, the UV absorption spectra of AKS, DPA and their mixturein basic solution were studied. The results showed (Fig. 8) thatthe absorption peaks of AKS and DPA almost disappear as theyare mixed. Secondly, when DPA and AKS were mixed in alkalinemedium, the color of DPA faded. However, when strong oxidant(K2S2O8 or HNO3) was added into this near-colorless solution, theprimary color of DPA recovered. Considering above experiment,it is obvious that a redox reaction takes place between AKS andDPA. What is more, when the mixture of AKS and DPA wasinjected into luminol, hardly any CL enhancement could be

observed. The observation implied the existence of a mediumproduct, which may be a free radical (AKSox.) in AKS oxidation,although more evidence is not available. Based on above analy-sis, reactions (1) and (2) are proposed.

More experiments to evaluate reactions (1) and (2) were car-ried out. When AKS standard solution was firstly mixed with DPAflow instead of luminol in the present flow system (Fig. 2), the CLintensity was much lower than that obtained without the aboveflow system change. By varying the tube length from DPA–AKSconfluence point to luminol confluence point, it was found that,the longer the tube length, the weaker the CL observed. Thesetwo experiment results coincide with what has been suggestedin reactions (1) and (2). It can be concluded the CL differenceobserved in above experiments is attributable to the instabilityof proposed AKSox..

It is known that luminol forms the dianion of luminol (I) asshown in reaction (3) in basic aqueous solution. In this paper, itis considered that the dianion (I) can be oxidized by DPA to thesemidione structure shown in one of its resonance forms [reac-tion (4)].[22,23,26–28] The semidione (II) reacts with oxygen to givethe proxy radical; the proxy radical is subsequently reduced in afast step to give proxy anion (III) [reaction (5)]. The proxy aniondecomposes to electronically excited (IV) with loss of nitrogenand then contributes CL emission [reaction (6)].[29] Based onthe CL enhancement of AKS on the DPA–luminol reaction, it issuggested that AKSox. could oxidize the luminol dianion (I) tosemidione structure (II) as shown in reaction (7), and this reac-tion performs as the competing reaction with reaction (4). Itenabled us to conclude that K1K7 >> K4 and K1 > K2, otherwisethe CL enhancement from AKS should not be observed. Basedon the above discussion, the most probable reaction mecha-nism is shown in Fig. 9, although more evidence is not available.

Conclusions

A sensitive and novel CL method has been proposed. Combinedwith the flow injection system, the enhanced luminol–DPA CLintensity was utilized for the determination of AKS in humanserum. The proposed method has prominent advantages includinginstrumental simplicity, lower reagent consumption, high sensi-tivity and selectivity, analytical efficiency and an easy handlingprocedure. The result of the proposed method agrees well withthose obtained by the spectrophotometric method.

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Table 2. Results of determination of AKS in human serum

Sample Amount added(10−5 mol L−1)

Amount found (10−5 mol L−1) ± RSD(%)

Proposedmethod

Spectrophotometricmethod

1 1.10 1.09 ± 3.2 1.13 ± 0.722 1.39 1.42 ± 2.7 1.43 ± 0.76

Figure 7. CL spectrum of luminol and DPA catalyzed by AKS in the absence (A)and presence (B) conditions. Luminol, 1.0 × 10−4 mol L−1; DPA, 1.0 × 10−4 mol L−1;AKS, 5.1 × 10−5 mol L−1.

Figure 8. UV–vis absorption spectra. A, DPA (2.0 × 10−5 mol L−1); B, AKS (5.1 ×10−4 mol L−1; C, DPA (2.0 × 10−5mol L−1) + AKS (5.1 × 10−4 mol L−1).

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Figure 9. The most possible reaction mechanism.

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