Chemosensors
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2022
·Vol. 10
·期 10
·423
·
IF 4.229
Chao Liu,Shenhao Wang,Xuan Dong,Qing Huang
Due to the increasing importance of food quality/safety control, there is an imminent need to develop efficient methods for the rapid detection of pesticide residues in agricultural products. Herein, we proposed a simple and rapid detection approach to the in situ detection of residual pesticides on fruit/vegetable using surface-enhanced Raman spectroscopy (SERS). Flexible and transparent SERS substrates were fabricated by transferring Au@Ag core-shell nanorods (Au@Ag NRs) arrays to silicone membranes, with the single-layer Au@Ag NRs arrays prepared by the liquid–liquid interface self-assembly method. The as-prepared SERS sensor showed excellent SERS activity and repeatability, and it could be readily pasted onto the surface of fruit and vegetables for residual pesticide detection. For the inspection of thiram in contaminated strawberries, apples, and mushrooms, the limit of detection (LOD) could reach 2 ng/cm2with high measurement recovery and reproducibility. In general, this work provides an effective way for the preparation and application of flexible and transparent SERS substrates in food-safety control.Keywords:surface-enhanced Raman spectroscopy (SERS);Au@Ag nanorods;flexible substrates;rapid detection;pesticide detection
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MICROPOROUS AND MESOPOROUS MATERIALS
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2022
·
IF 5.876
Shuai Wang,Hao Wang,Shixing Wang,Libo Zhang,Likang Fu
The gold recovery from wastewater is not only beneficial to environmental protection, but also to alleviate the shortage of resources. Chitosan is considered as an excellent adsorption material, but its application in gold recovery is always some shortcomings including low adsorption capacity and selectivity. This work developed an efficient biosorbent (CS-ES) by functionalizing chitosan with poly(ethylene sulfide) for gold recovery from simulated wastewater. The properties and adsorption mechanism of CS-ES were investigated using SEM, EDS , XRD , FT-IR, BET and XPS . The results of experiments revealed that the adsorption efficiency of CS-ES for Au(III) reaches more than 90% in a wide pH range (2.0–6.0) and the highest adsorption efficiency about 99.07% was achieved at pH = 5.0. At 318 K, the highest adsorption ability of CS-ES for gold ions was 657.49 mg/g. The adsorption findings supported the Langmuir and pseudo-second-order models, suggesting that monolayer chemisorption is the dominant adsorption mechanism. The thermodynamic performance ( ΔH° and ΔS° > 0, ΔG° <0) showed that gold ion adsorption by CS-ES is spontaneous exothermic reaction. CS-ES shows an excellent reproducibility after four adsorption-desorption cycles and selectivity against six metal ions. Moreover, a variety of physicochemical and spectroscopic tests demonstrate the extremely effective adsorption and in-situ reduction of gold by CS-ES are based on electrostatic attraction, chelation, and reduction between gold and nitrogen/sulfur groups. In this work, a novel adsorbent for recovering Au(III) from wastewater was devised with great efficiency, selectivity and repeatability.
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Journal of Materials Chemistry B
·
2022
·Vol. 10
·期 34
·6532-6545
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IF 7.571
Zhe Tang,Israt Ali,Yike Hou,Ozioma Udochukwu Akakuru,Quan Zhang,Asim Mushtaq,Han Zhang,Yuguang Lu,Xuehua Ma,Jian Ge,M. Zubair Iqbal,Xiangdong Kong
Nanotheranostic agents based on plasmonic nanostructures with their resonance wavelengths located in the second near-infrared window (NIR-II) have gained significant attention in profound tumor photothermal therapy. However, the modulation of localized surface plasmon resonance of gold nanomaterials from the first near-infrared (NIR-I) window to the NIR-II window is still challenging. The structures and compositions of the plasmonic nanomaterials have demonstrated promising characteristics in controlling the optical properties of plasmonic nanostructures. Here, gold nanorod (Au NR) coated with an ultrathin palladium (Pd) shell was developed for tumor-targeted NIR-II photothermal-augmented nanocatalytic therapy through the combination of compositional manipulation and structural evolution strategies. These Au@Pd core–shell hybrid NRs (HNRs) were functionalized with biocompatible chitosan (CS) to acquire lower toxicity and higher stability in physiological systems. Further, Au@Pd–CS HNRs were endowed with an excellent targeting ability by conjugating with folic acid (FA). The as-synthesized Au@Pd–CS–FA HNRs show efficient and complete photothermal ablation of tumor cells upon 1064 nm laser irradiation. The remarkable photothermal conversion efficiency of 69.0% was achieved, which is superior to many reported photothermal agents activated in the NIR-II region. Excitingly, Au@Pd–CS–FA HNRs have peroxidase and catalase activities, simultaneously producing ˙OH for catalytic therapy and O2 for relieving tumor hypoxia and photodynamic therapy. Additionally, in vivo tumor photothermal therapy was carried out, where the biocompatible Au@Pd–CS–FA HNRs penetrate intensely into the tumor cells and consequently show remarkable therapeutic effects. The idea about plasmonic modulation behind the bimetallic core–shell nanostructure in this report can be extended to construct new classes of metal-based nanotheranostic agents with dual-modal combined therapy as an alternative to traditional chemotherapy.
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Chemosensors
·
2022
·Vol. 10
·期 7
·260
·
IF 4.229
Zhaoxia Shi,Ling Xia,Gongke Li,Yufei Hu
High purity methyl tert-butyl ether (MTBE) can be used to adjust gasoline octane values. However, an isomer, methyl sec-butyl ether (MSBE), is the main by-product of its industrial production, and this affects the purity of MTBE. Pt/Au NPs@Co3O4composites with a hollow dodecahedron three-dimensional structure were synthesized using ZIF-67 as a template, with Pt and Au nanoparticles (NPs) evenly distributed on the shell of the hollow structure. A CTL sensor was established for the determination of MSBE based on the specificity of Pt/Au NPs@Co3O4. The experimental results showed that Pt/Au NPs@Co3O4had a strong specific cataluminescence (CTL) response to MSBE, with no interference from MTBE. The linear range was 0.10–90 mg/L, the limit of detection was 0.031 mg/L (S/N= 3), the RSD was 2.5% (n= 9), and a complete sample test could be completed in five minutes. The sensor was used to detect MSBE in MTBE of different purity grades, with recoveries ranging from 92.0% to 109.2%, and the analytical results were consistent with those determined by gas chromatography. These results indicate that the established method was accurate and reliable, and could be used for rapid analysis of MTBE gasoline additive.Keywords:Pt/Au NPs@Co3O4;cataluminescence sensor;methyl sec-butyl ether;methyl tert-butyl ether;rapid analysis;gasoline additive
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Xian Liu,Like Chen,Yibo Gao,Jiebin Li,Junyong Sun,Tian Gan
In this context, an innovative design of a molecularly imprinted polymer (MIP) capped Au@HKUST− 1 nanocapsules−based electrode was described for highly sensitive and selective detection of isoproturon herbicide. The Au@HKUST− 1 nanocapsules were constructed by in−situ growth of nanoscaled HKUST− 1 crystals on Cu 2 O core materials and subsequent encapsulation of Au nanoparticles inside the hollow HKUST− 1 walls via galvanic replacement reaction between AuCl 4 − and Cu 2 O. After a further surface imprinting−directing polymerization process in the presence of hydrophobic Au@HKUST− 1, a high−performance electrochemical sensing platform was obtained and used for recognition and quantification of isoproturon. Under the optimal experimental conditions, a linear relationship was observed covering the linear range of 0.0010 − 45 μM with an ultra−low detection limit of 0.45 nM. In addition, the Au@HKUST− 1 @MIP modified electrode had higher sensing specificity for isoproturon in the application of water samples with recoveries in the range of 99.07 − 105.8% and a relative standard deviation of < 4%.
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MICROCHIMICA ACTA
·
2022
·Vol. 189
·期 5
·1-9
·
IF 6.408
Zhu Anni,Wang Tiansheng,Jiang Yuning,Hu Sen,Tang Wanxin,Liu Xinling,Guo Xiaoyu,Ying Ye,Wu Yiping,Wen Ying,Yang Haifeng
A specific surface-enhanced Raman scattering (SERS) assay for dopamine (DA) based on an azo derivatization reaction is proposed for the first time by preparation of p-aminothiophenol (PATP)-modified composite SERS substrate, composed of metal–organic framework (MIL-101) decorated with Au and Ag nanoparticles. As the result, the SERS method for detection of the azo reaction between PATP and DA exhibits superior sensitivity, selectivity, and stability. A reasonable linearity in the range 10 −6 to 10 −10 mol∙L −1 is achieved, and the limit of detection is 1.2 × 10 −12 mol∙L −1 . The reactive SERS assay is free from interference in complex physiological fluid. The feasibility of the proposed SERS method for the detection of DA levels in fetal bovine serum (FBS) samples and human serum samples is validated by HPLC–MS methods, displaying promising application potential in early disease diagnosis. Graphical abstract
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JOURNAL OF MOLECULAR LIQUIDS
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2022
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IF 6.633
Yangyang Wang,Xiaoxia Liu,Annie Yang,Ping Lv,Lixin Zhang,Yongnian Li,Yanzhao Yang
Selective recovery of gold and platinum from secondary resources is of great significance under the crisis of resource shortage. Hence, the optimal extractant 1-(2-(dimethylamino) ethyl)-4-methyl-piperazin bis(trifluoromethylsulfonyl)imide ([C 6 -Et-TMEDA-PIP][Tf 2 N] 2 ) was synthesized and screened out from five piperazine-based ionic liquids (ILs) to construct an IL-water system for Au(III) and Pt(IV) extraction. ILs have high hydrophobicity and low viscosity at room temperature, which can be used as both extractant and hydrophobic phase. The effects of IL dosage, metal concentration and acidity on the extraction efficiency were investigated. Under the optimal conditions, the extraction efficiency of 98.5% (Au(III)) and 97.5% (Pt(IV)) can be achieved. The anion exchange mechanism was verified through the combination of Ultraviolet visible spectroscopy (UV–vis), Nuclear magnetic spectra (NMR) and quantum chemical calculations. Besides that, the two-factor optimization of the extractant dosage and HCl concentration was carried out by Response surface methodology (RSM), and the effective separation of Au(III) and Pt(IV) was successfully achieved. Au(III)/ Pt(IV) was extracted into the IL phase as [Et-TMEDA-PIP + ][AuCl 4 - ] and can easily be stripped by reduction to Au(0)/Pt(Ⅱ) with H 2 C 2 O 4 /CS(NH 2 ) 2 -HCl, and each extraction ability maintained after 5 turns of extraction cycle experiments. Since the excellent behaviors showed in the multi-metal selective extraction and cycle experiments, the [C 6 -Et-TMEDA-PIP][Tf 2 N] 2 was regarded as the most potential system for Au(III) and Pt(IV) recovery from HCI medium.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2022
·
IF 9.221
Shuang Li,Jiawei Zhang,Cherie S. Tan,Chong Chen,Chang Hu,Yongchang Bai,Dong Ming
As important biomarkers for prostate cancer, total prostate specific antigen (tPSA) and free prostate specific antigen (fPSA) levels in serum play essential roles in early diagnosis. In this study, hybrid molybdenum disulfide (MoS 2 )/Pt@Au-nanoprism/polydopamine (PDA)-modified screen-printed electrodes were utilized to detect both fPSA and tPSA in serum simultaneously. MoS 2 generated by the hydrothermal method assembled on the electrode to provide binding sites for further modification. Au nanoprisms were obtained by reducing chloroauric acid with sodium thiosulfate to achieve uniformity. Pt nanoparticles covered on Au nanoprisms by the displacement method, and the generated Pt@Au-nanoprism structure was then deposited onto the electrode to enhance the electrochemical signals. An electropolymerization-synthesized PDA film further modified the electrode to increase antibody binding sites. The results demonstrated that the proposed electrochemical immunosensor for fPSA and tPSA analysis in serum using differential pulse voltammetry (DPV) had a wide linear range from 0.0001 ng/mL to 100 ng/mL, with limits of detection (3 SD/slope) at 0.1 pg/mL and 1.1 fg/mL, respectively. For clinical patient samples, the proposed biosensor demonstrated good accuracy according to the clinical electrochemiluminescence immunoassay and improved the diagnostic specificity of tPSA concentrations in the “gray zone", suggesting promising prospects for clinical applications of our multiplex biosensors.
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MICROCHEMICAL JOURNAL
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2022
·
IF 5.304
Xueyuan Li,Xuezhong Du
Surface enhanced electrochemiluminescence (SEECL) emission of the Ru(bpy) 3 2+ (bpy = 2,2′-bipyridyl)/tripropylamine (TPA) system by [email protected] 2 core/shell nanoparticles (NPs) was achieved owing to the electromagnetic field enhancement induced by localized surface plasmon resonance (LSPR) of internal Au cores. The Ru(bpy) 3 2+ /TPA system in electrolyte solution showed a maximum ECL enhancement when a glassy carbon electrode (GCE) was modified with [email protected] 2 NPs ( [email protected] 2 /GCE; Au core, ca. 68 nm; silica shell, 12 nm). The ECL emission of the system in the case of [email protected] 2 /GCE was 29 fold stronger than the ECL emission in the case of bare GCE, ca. 39 fold stronger than the ECL emission in the case of hollow silica NP-modified GCE, and 100 fold stronger than the ECL emission in the case of AuNP-modified GCE. To the best of our knowledge, the respective folds of ECL enhancement in the Ru(bpy) 3 2+ /TPA system by the LSPR-induced electromagnetic field of AuNPs are the largest reported to date. The ECL emission of TPA •+ radical cations was detected for the first time taking the advantage of the electromagnetic field enhancement. A SEECL platform based on the [email protected] 2 /GCE in the Ru(bpy) 3 2+ /TPA system was constructed for the detection of dopamine (DA). This is the first example that the AuNP-enhanced ECL emission was quenched by DA for the selective detection of DA, and a wide linear range of 0.01–600 μM directly relevant to DA concentration was obtained with a low detection limit of 0.004 μM and high sensitivity and accuracy. The mechanism that the ECL emission of the Ru(bpy) 3 2+ /TPA system was quenched by DA for the detection of DA was clearly elaborated. The level of DA in human serum was determined using the SEECL platform.
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Analytical Methods
·
2023
·Vol. 15
·期 35
·4494-4505
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IF 3.1
Chao Sun,Lizheng Wang,Naiyu Guo,Runze Hu,Li Ye,Zhiming Hu,Jianjun Ding
Surface-enhanced Raman scattering (SERS) has a unique fingerprint spectrum, which allows for rapid, highly sensitive, and non-destructive detection without the need for sample pretreatment. However, SERS substrates have disadvantages such as short storage time and poor reproducibility. In this study, carbon nanotubes, gold, and silver were combined to take advantage of their inherent structural and characteristic properties that enhance the Raman effect. A new type of SERS composite substrate, CNTs/Ag@Au/SiO2, was prepared using a hydrothermal method and seed growth method. The substrate was characterized using transmission electron microscopy (TEM), and the average distance between the core–shell nanoparticles was found to be 3.1 nm, which is more suitable than other gold–silver combined core–shell structures and significantly improves the SERS enhancement factor. The substrate demonstrated high sensitivity even at low concentrations of probe molecules and good uniformity at five randomly selected locations. After storage for 45 days, the substrate still exhibited good stability. In most gold–silver combined core–shell structures, the detection limit for Rhodamine 6G (R6G) is 10−9 mol L−1, while in this substrate, the detection limit for R6G is 10−11 mol L−1. Furthermore, the contribution of the substrate's enhancement was deeply investigated using finite-difference time-domain (FDTD), which revealed that the substrate's hotspots were present in two forms: the “hotspots generated between Ag@Au nanoparticles” and the “hotspots generated between Ag@Au nanoparticles and carbon nanotubes”. These two forms of hotspots also demonstrated that the performance brought about by the preparation of the substrate structure was reliable. The simulation results were compared with the experimental results, and the analysis showed that the real environment would have an impact on the substrate's structure during the actual substrate preparation process. Finally, the substrate was used for detecting the pesticide fipronil, and the results showed clear peaks even at a concentration of 0.1 mg L−1. The results indicated that the Raman intensity was linearly exponential with the fipronil solution concentration, with a determination coefficient of R2 = 0.991. This study provides a new SERS substrate for pesticide residue detection and further explores the improvement of pesticide detection limits.
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MICROCHEMICAL JOURNAL
·
2021
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IF 4.821
Ruru Wang,Xuerui Liu,Yiwei Zhao,Jianhua Qin,Hui Xu,Lina Dong,Shanmin Gao,Linlin Zhong
A novel carbon composite was integrated with Au@Pt core–shell nanoparticles (Au@Pt NPs) to construct a sensing interface for enzyme-free electrochemical detection of glucose. As surfactant, graphene oxide (GO) was used to disperse multi-walled carbon nanotubes (MWCNTs). After the glassy carbon electrode (GCE) was modified with the mixture of GO and MWCNTs, the Au@Pt NPs were decorated on it. The prepared novel three-dimensional sensor interface was applied to detect glucose without enzyme at a remarkable negative potential (at about −0.013 V vs. Ag/AgCl), demonstrating a low detection limit (4.2 × 10 −8 M) and two wide linear range from 5 × 10 −8 to 1 × 10 −4 M and 1 × 10 −4 M to 2.5 × 10 −3 M. In addition, the non-enzymatic glucose sensing platform can be realized for practical application.
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Jiabin Shen,Shanshan Xu,Cheng Zhao,Xiaopeng Qiao,Haiquan Liu,Yong Zhao,Jing Wei,Yongheng Zhu
In this work, we present a new metal oxide semiconductor gas sensor for detecting trimethylamine (TMA) by bimetal Au@Pt-modified α-Fe2O3 hollow nanocubes (NCs) as sensing materials. The structure and morphological characteristics of Au@Pt/α-Fe2O3 were evaluated through multiple analyses, and their gas-sensitive performance was investigated. Compared with the pristine α-Fe2O3 NC sensor, the sensor based on Au@Pt/α-Fe2O3 NCs exhibited faster response time (5 s) and higher response (Ra/Rg = 32) toward 100 ppm TMA gas at a lower temperature (150 °C). Furthermore, we also assessed the Au@Pt/α-Fe2O3 NC sensor for detecting the freshness of Larimichthys crocea which have been observed by headspace solid-phase microextraction and gas chromatography–mass spectrometry. The high performance of the Au@Pt/α-Fe2O3 NCs is attributed to the special hollow morphology with a high specific surface area (212.9 m2/g) and the synergistic effect of the Au@Pt bimetal. The Au@Pt/α-Fe2O3 sensor shows promising application prospects in estimating seafood freshness on the spot.
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