Abstract
Four kinds of Ag3PO4 materials were prepared by controlling the experimental conditions, which were developed as oxidase mimics. Experimental results showed that different synthesis methods led to distinct crystal structures, morphologies, and surface properties, which contributed to diverse oxidase-like activities of Ag3PO4 materials. Among them, Ag3PO4 microcubes (APMCs) can efficiently catalyze the oxidation of colorless 3,3′,5,5′-tetramethylbenzidine in the presence of dissolved oxygen to form a blue-colored oxide, presenting the best intrinsic oxidase mimetic ability. The higher-energy [110] facets with more oxygen vacancies exposed and more active sites coupled with more negative charge and larger specific surface area of APMCs contributed to its enhanced oxidase mimetic performance. Besides, mercury ions were proved to remarkably and selectively stimulate the oxidase-like ability of APMCs owing to the formation of Ag–Hg amalgam on its surface. Based on the stimulating effect of Hg2+ towards APMCs, a simple and rapid method for colorimetric determination of Hg2+ was thus established via the significant signal amplification and megascopic color variation. Under the optimal conditions, the sensing system showed a good linear relationship ranging from 0.1 to 7.0 μM and a detection limit of 20 nM for Hg2+, exhibiting high selectivity and good colour stability. Moreover, the colorimetric method was successfully applied to determine Hg2+ in real water samples. Considering these advantages, the developed colorimetric sensing system is expected to hold bright prospects for trace determination of Hg2+ in biological, environmental, and food samples.
Similar content being viewed by others
References
Baughman TA (2006) Elemental mercury spills. Environ Health Perspect 114:147–152. https://doi.org/10.1289/ehp.7048
Chansuvarn W, Tuntulani T, Imyim A (2015) Colorimetric detection of mercury(II) based on gold nanoparticles, fluorescent gold nanoclusters and other gold-based nanomaterials. Trends Anal Chem 65:83–96. https://doi.org/10.1016/j.trac.2014.10.013
Ding YJ, Wang SS, Li JH, Chen LX (2016) Nanomaterial-based optical sensors for mercury ions. Trends Anal Chem 82:175–190. https://doi.org/10.1016/j.trac.2016.05.015
Tchounwou PB, Ayensu WK, Ninashvili N, Sutton D (2003) Review: environmental exposure to mercury and its toxicopathologic implications for public health. Environ Toxicol 18:149–175. https://doi.org/10.1002/tox.10116
McDowell MA, Dillon CF, Osterloh J, Bolger PM, Pellizzari E, Fernando R, de Oca RM, Schober SE, Sinks T, Jones RL (2004) Hair mercury levels in U.S. children and women of childbearing age: reference range data from NHANES 1999-2000. Environ Health Perspect 112:1165–1171. https://doi.org/10.1289/ehp.7046
Onyido I, Norris AR, Buncel E (2004) Biomolecule-mercury interactions: modalities of DNA base-mercury binding mechanisms. Remediation strategies. Chem Rev 104:5911–5929. https://doi.org/10.1021/cr030443w
Christus AAB, Ravikumar A, Panneerselvam P, Radhakrishnan K (2018) A novel Hg(II) sensor based on Fe3O4@ZnO nanocomposite as peroxidase mimics. Appl Surf Sci 449:669–676. https://doi.org/10.1016/j.apsusc.2017.12.089
Farhadi K, Fough M, Molaeia R, Hajizadeha S, Rafipou A (2012) Highly selective Hg2+ colorimetric sensor using green synthesized and unmodified silver nanoparticles. Sensors Actuators B Chem 161:880–885. https://doi.org/10.1016/j.snb.2011.11.052
Yang HG, Xiong YH, Zhang P, Su LJ, Ye FG (2015) Colorimetric detection of mercury ions using MnO2 nanorods as enzyme mimics. Anal Methods 7:4596–4601. https://doi.org/10.1039/c5ay00633c
Lu Y, Yu J, Ye WC, Yao X, Zhou PP, Zhang HX, Zhao SQ, Jia LP (2016) Spectrophotometric determination of mercury(II) ions based on their stimulation effect on the peroxidase-like activity of molybdenum disulfide nanosheets. Microchim Acta 183:2481–2489. https://doi.org/10.1007/s00604-016-1886-4
Zhang JR, Huang WT, Zeng AL, Luo HQ, Li NB (2015) Ethynyl and π-stacked thymine-Hg2+-thymine base pairs enhanced fluorescence quenching via photoinduced electron transfer and simple and sensitive mercury ion sensing. Biosens Bioelectron 64:597–604. https://doi.org/10.1016/j.bios.2014.09.092
Zaib M, Athar MM, Saeed A, Farooq U (2015) Electrochemical determination of inorganic mercury and arsenic—a review. Biosens Bioelectron 74:895–908. https://doi.org/10.1016/j.bios.2015.07.058
de Souza SS, Campiglia AD, Barbosa F Jr (2013) A simple method for methylmercury, inorganic mercury and ethylmercury determination in plasma samples by high performance liquid chromatography-cold-vapor-inductively coupled plasma mass spectrometry. Anal Chim Acta 761:11–17. https://doi.org/10.1016/j.aca.2012.11.038
Shah AQ, Kazi TG, Baig JA, Afridi HI, Arain MB (2012) Simultaneously determination of methyl and inorganic mercury in fish species by cold vapor generation atomic absorption spectrometry. Food Chem 134:2345–2349. https://doi.org/10.1016/j.foodchem.2012.03.109
Rodrigues JL, Torres DP, Souza VCD, Batista BL, de Souza SS, Curtius AJ, Barbosa F (2009) Determination of total and inorganic mercury in whole blood by cold vapor inductively coupled plasma mass spectrometry (CV ICP-MS) with alkaline sample preparation. J Anal At Spectrom 24:1414–1420. https://doi.org/10.1039/B910144F
Kandjani AE, Sabri YM, Mohammad-Taheri M, Bansal V, Bhargava SK (2015) Detect, remove and reuse: a new paradigm in sensing and removal of Hg (II) from wastewater via SERS-active ZnO/Ag nanoarrays. Environ Sci Technol 49:1578–1584. https://doi.org/10.1021/es503527e
Cai Y, Jaffe R, Alli A, Jones RD (1996) Determination of organomercury compounds in aqueous samples by capillary gas chromatography-atomic fluorescence spectrometry following solid-phase extraction. Anal Chim Acta 334:251–259. https://doi.org/10.1016/S0003-2670(96)00309-1
Nolan EM, Lippard SJ (2008) Tools and tactics for the optical detection of mercuric ion. Chem Rev 108:3443–3480. https://doi.org/10.1021/cr068000q
Xu X, Li YF, Zhao J, Li Y, Lin J, Li B, Gao Y, Chen C (2015) Nanomaterial-based approaches for the detection and speciation of mercury. Analyst 140:7841–7853. https://doi.org/10.1039/C5AN01519G
Lee JS, Han MS, Mirkin CA (2007) Colorimetric detection of mercuric ion (Hg2+) in aqueous media using DNA-functionalized gold nanoparticles. Angew Chem Int Ed 46:4093–4096. https://doi.org/10.1002/ange.200700269
Rastogi L, Sashidhar RB, Karunasagar D, Arunachalam J (2014) Gum kondagogu reduced/stabilized silver nanoparticles as direct colorimetric sensor for the sensitive detection of Hg2+ in aqueous system. Talanta 118:111–117. https://doi.org/10.1016/j.talanta.2013.10.012
Wei H, Wang EK (2013) Nanomaterials with enzyme-like characteristics (nanozymes): next generation artificial enzymes. Chem Soc Rev 42:6060–6093. https://doi.org/10.1039/c3cs35486E
Wang QQ, Wei H, Zhang ZQ, Wang EK, Dong SJ (2018) Nanozyme: an emerging alternative to natural enzyme for biosensing and immunoassay. Trends Anal Chem 105:218–224. https://doi.org/10.1016/j.trac.2018.05.012
Gao L, Zhuang J, Nie L, Zhang J, Zhang Y, Gu N, Wang T, Feng J, Yang D, Perrett S, Yan X (2007) Intrinsic peroxidase-like activity of ferromagnetic nanoparticles. Nat Nanotechnol 2:577–583. https://doi.org/10.1038/nnano.2007.260
Ju P, Yu YZ, Wang M, Zhao Y, Zhang D, Sun CJ, Han XX (2016) Synthesis of EDTA-assisted CeVO4 nanorods as robust peroxidase mimics towards colorimetric detection of H2O2. J Mater Chem B 4:316–6325. https://doi.org/10.1039/C6TB01881E
Ju P, Ding JF, Wang B, Li W, Jiang FH, Han XX, Sun CJ, Wu CC (2019) Intrinsic peroxidase-like activity of Cu2ZnSn(SxSe1-x)4 nanocrystals and their application to the colorimetric detection of H2O2. Microchim Acta 186:118. https://doi.org/10.1007/s00604-018-3185-8
Liu HY, Zhu LL, Ma H, Wen JJ, Xu HX, Qiu YB, Zhang LN, Li LH, Gu CC (2019) Copper(II)-coated Fe3O4 nanoparticles as an efficient enzyme mimic for colorimetric detection of hydrogen peroxide. Microchim Acta 186:518. https://doi.org/10.1007/s00604-019-3599-y
Liu HY, Ma H, Xu HX, Wen JJ, Huang ZH, Qiu YB, Fan K, Li DJ, Gu CC (2019) Hollow and porous nickel sulfide nanocubes prepared from a metal-organic framework as an efficient enzyme mimic for colorimetric detection of hydrogen peroxide. Anal Bioanal Chem 411:129–137. https://doi.org/10.1007/s00216-018-1423-x
Sui N, Li S, Wang YK, Zhang QB, Liu SF, Bai Q, Xiao HL, Liu M, Wang LN, Yu WW (2019) Etched PtCu nanowires as a peroxidase mimic for colorimetric determination of hydrogen peroxide. Microchim Acta 186:186. https://doi.org/10.1007/s00604-019-3293-0
Wu TT, Hou WL, Ma ZY, Liu ML, Liu XY, Zhang YY, Yao SZ (2019) Colorimetric determination of ascorbic acid and the activity of alkaline phosphatase based on the inhibition of the peroxidase-like activity of citric acid-capped Prussian blue nanocubes. Microchim Acta 186:123. https://doi.org/10.1007/s00604-018-3224-5
Yang Z, Ji H (2013) 2-Hydroxypropyl-β-cyclodextrin polymer as a mimetic enzyme for mediated synthesis of benzaldehyde in water. ACS Sustain Chem Eng 1:1172–1179. https://doi.org/10.1021/sc4001059
Tan B, Zhao HM, Wu WH, Liu X, Zhang YB, Quan X (2017) Fe3O4-AuNPs anchored 2D metal-organic framework nanosheets with DNA regulated switchable peroxidase-like activity. Nanoscale 9:18699–18710. https://doi.org/10.1039/C7NR05541B
Wang Q, Yang Z, Zhang X, Xiao X, Chang CK, Xu B (2007) A supramolecular-hydrogel-encapsulated hemin as an artificial enzyme to mimic peroxidase. Angew Chem Int Ed 46:4285–4289. https://doi.org/10.1002/anie.200700404
Lin Y, Ren J, Qu X (2014) Catalytically active nanomaterials: a promising candidate for artificial enzymes. Acc Chem Res 47:1097–1105. https://doi.org/10.1021/ar400250z
Nasir M, Nawaz MH, Latif U, Yaqub M, Hayat A, Rahim A (2017) An overview on enzyme-mimicking nanomaterials for use in electrochemical and optical assays. Microchim Acta 184:323–342. https://doi.org/10.1007/s00604-016-2036-8
Wei H, Wang EK (2008) Fe3O4 magnetic nanoparticles as peroxidase mimetics and their applications in H2O2 and glucose detection. Anal Chem 80:2250–2254. https://doi.org/10.1021/ac702203f
Qiao FM, Qi QQ, Wang ZZ, Xu K, Ai SY (2016) MnSe-loaded g-C3N4 nanocomposite with synergistic peroxidase-like catalysis: synthesis and application toward colorimetric biosensing of H2O2 and glucose. Sensors Actuators B Chem 229:379–386. https://doi.org/10.1016/j.snb.2015.12.109
Yu YZ, Ju P, Zhang D, Han XX, Yin XF, Zheng F, Sun CJ (2016) Peroxidase-like activity of FeVO4 nanobelts and its analytical application for optical detection of hydrogen peroxide. Sensors Actuators B Chem 233:162–172. https://doi.org/10.1016/j.snb.2016.04.041
Chai DF, Ma Z, Qiu YF, Lv YG, Liu H, Song CY, Gao GG (2016) Oxidase-like mimic of Ag@Ag3PO4 microcubes as a smart probe for ultrasensitive and selective Hg2+ detection. Dalton Trans 4:3048–3054. https://doi.org/10.1039/C5DT04192A
Ma CM, Ma Y, Sun YF, Lu Y, Tian EL, Lan JF, Li JL, Ye WC, Zhang HX (2019) Colorimetric determination of Hg2+ in environmental water based on the Hg2+-stimulated peroxidase mimetic activity of MoS2-Au composites. J Colloid Interface Sci 537:554–561. https://doi.org/10.1016/j.jcis.2018.11.069
Li W, Chen B, Zhang HX, Sun YH, Wang J, Zhang JL, Fu Y (2015) BSA-stabilized Pt nanozyme for peroxidase mimetics and its application on colorimetric detection of mercury(II) ions. Biosens Bioelectron 66:251–258. https://doi.org/10.1016/j.bios.2014.11.032
Amanulla B, Perumal KN, Ramaraj SK (2019) Chitosan functionalized gold nanoparticles assembled on sulphur doped graphitic carbon nitride as a new platform for colorimetric detection of trace Hg2+. Sensor Actuat B Chem 281:281–287. https://doi.org/10.1016/j.snb.2018.10.039
Zhang ST, Zhang DX, Zhang XH, Shang DH, Xue ZH, Shan DL, Lu XQ (2017) Ultratrace naked-eye colorimetric detection of Hg2+ in wastewater and serum utilizing mercury-stimulated peroxidase mimetic activity of reduced graphene oxide-PEI-Pd nanohybrids. Anal Chem 89:3538–3544. https://doi.org/10.1021/acs.analchem.6b04805
Lian Q, Liu H, Zheng XF, Li XM, Zhang J, Gao J (2019) Enhanced peroxidase-like activity of CuO/Pt nanoflowers for colorimetric and ultrasensitive Hg2+ detection in water sample. Appl Surf Sci 483:551–561. https://doi.org/10.1016/j.apsusc.2019.03.337
Yang HG, Zha JQ, Zhang P, Xiong YH, Su LJ, Ye FG (2016) Sphere-like CoS with nanostructures as peroxidase mimics for colorimetric determination of H2O2 and mercury ions. RSC Adv 6:66963–66970. https://doi.org/10.1039/C6RA16619A
Zhao Y, Qiang H, Chen ZB (2017) Colorimetric determination of Hg(II) based on a visually detectable signal amplification induced by a Cu@Au-Hg trimetallic amalgam with peroxidase-like activity. Microchim Acta 184:107–115. https://doi.org/10.1007/s00604-016-2002-5
Yi ZG, Ye JH, Kikugawa N, Kako T, Ouyang SX, Stuart-Williams H, Yang H, Cao JY, Luo WJ, Li ZS, Liu Y, Withers RL (2010) An orthophosphate semiconductor with photooxidation properties under visible-light irradiation. Nat Mater 9:559–564. https://doi.org/10.1038/nmat2780
Dong PY, Wang YH, Li HH, Li H, Ma XL, Han LL (2013) Shape-controllable synthesis and morphology-dependent photocatalytic properties of Ag3PO4 crystals. J Mater Chem A 1:4651–4656. https://doi.org/10.1039/c3ta00130j
Wang J, Teng F, Chen MD, Xu JJ, Song YQ, Zhou XL (2013) Facile synthesis of novel Ag3PO4 tetrapods and the {110} facets-dominated photocatalytic activity. CrystEngComm 15:39–42. https://doi.org/10.1039/c2ce26060c
Liang QH, Ma WJ, Shi Y, Li Z, Yang XM (2012) Hierarchical Ag3PO4 porous microcubes with enhanced photocatalytic properties synthesized with the assistance of trisodium citrate. CrystEngComm 14:2966–2973. https://doi.org/10.1039/c2ce06425a
Bi YP, Ouyang SX, Umezawa N, Cao JY, Ye JH (2011) Facet effect of single-crystalline Ag3PO4 sub-microcrystals on photocatalytic properties. J Am Chem Soc 133:6490–6492. https://doi.org/10.1021/ja2002132
Bi YP, Hu HY, Ouyang SX, Lu GX, Cao JY, Ye JH (2012) Photocatalytic and photoelectric properties of cubic Ag3PO4 sub-microcrystals with sharp corners and edges. Chem Commun 48:3748–3750. https://doi.org/10.1039/c2cc30363a
Liu YJ, Zhu GX, Yang J, Yuan AH, Shen XP (2014) Peroxidase-like catalytic activity of Ag3PO4 nanocrystals prepared by a colloidal route. PLoS One 9:e109158. https://doi.org/10.1371/journal.pone.0109158
Li CJ, Zhang P, Lv R, Lu JW, Wang T, Wang SP, Wang HF, Gong JL (2013) Selective deposition of Ag3PO4 on monoclinic BiVO4 (040) for highly efficient photocatalysis. Small 9:3951–3956. https://doi.org/10.1002/smll.201301276
Shang J, Gao XH (2014) Nanoparticle counting: towards accurate determination of the molar concentration. Chem Soc Rev 43:7267–7278. https://doi.org/10.1039/C4CS00128A
Chen GH, Chen WY, Yen YC, Wang CW, Chang HT, Chen CF (2014) Detection of mercury (II) ions using colorimetric gold nanoparticles on paper-based analytical devices. Anal Chem 86:6843–6849. https://doi.org/10.1021/ac5008688
Chen X, Zhai N, Snyder JH, Chen Q, Liu P, Jin L, Zheng Q, Lin F, Hu J, Zhou H (2015) Colorimetric detection of Hg2+ and Pb2+ based on peroxidase-like activity of graphene oxide-gold nanohybrids. Anal Methods 7:1951–1957. https://doi.org/10.1039/C4AY02801E
Kamali KZ, Pandikumar A, Jayabal S, Ramaraj R, Lim HN, Ong BH, Bien CSD, Kee YY, Huang NM (2016) Amalgamation based optical and colorimetric sensing of mercury(II) ions with silver@graphene oxide nanocomposite materials. Microchim Acta 183:369–377. https://doi.org/10.1007/s00604-015-1658-6
Rameshkumar P, Manivannan S, Ramaraj R (2013) Silver nanoparticles deposited on amine-functionalized silica spheres and their amalgamation-based spectral and colorimetric detection of Hg(II) ions. J Nanopart Res 15:1639–1164. https://doi.org/10.1007/s11051-013-1639-9
Zhu RC, Zhou Y, Wang X, Liang L, Long Y, Wang Q, Zhang H, Huang X, Zheng H (2013) Detection of Hg2+ based on the selective inhibition of peroxidase mimetic activity of BSA-Au clusters. Talanta 117:127–132. https://doi.org/10.1016/j.talanta.2013.08.053
Funding
This work was supported by National Natural Science Foundation of China (51702328 and 41706080), the Basic Scientific Fund for National Public Research Institutes of China (2019Y03 and 2020S02), Shandong Provincial Natural Science Foundation (ZR2017BD002), the Key Research and Development Program of Shandong Province (2018GHY115029), CAS “Light of West China” Program, Open Fund of Shandong Key Laboratory of Corrosion Science (KLCS201906), Open Fund of Laboratory for Marine Ecology and Environmental Science, Pilot National Laboratory for Marine Science and Technology (Qingdao) (LMEES201802), Open Foundation of Pilot National Laboratory for Marine Science and Technology (Qingdao) (QNLM2016ORP0410), and The Aoshan Scientific and Technological Innovation Project Financially Supported by Pilot National Laboratory for Marine Science and Technology (Qingdao) (2016ASKJ14).
Author information
Authors and Affiliations
Corresponding authors
Ethics declarations
Conflict of interest
The authors declare that they have no competing interests.
Additional information
Publisher’s note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Electronic supplementary material
ESM 1
(DOC 6861 kb)
Rights and permissions
About this article
Cite this article
Zhang, Y., Ju, P., Sun, L. et al. Colorimetric determination of Hg2+ based on the mercury-stimulated oxidase mimetic activity of Ag3PO4 microcubes. Microchim Acta 187, 422 (2020). https://doi.org/10.1007/s00604-020-04399-0
Received:
Accepted:
Published:
DOI: https://doi.org/10.1007/s00604-020-04399-0