ANALYTICAL CHEMISTRY
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2021
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IF 6.986
Li Fu,Xuwen Gao,Shuangtian Dong,Hsien-Yi Hsu,Guizheng Zou
Aqueous electrochemiluminescence (ECL) in the second near-infrared biowindow (NIR-II, 900–1700 nm) was anticipated for ECL evolution and spectral multiplexing. Herein, aqueous and monochromatic ECL with a single emission peak beyond 900 nm was achieved by employing methionine (Met)-capped Au–Ag bimetallic nanoclusters (BNCs) as luminophores and triethanolamine (TEOA) as a coreactant. The Met-capped Au–Ag BNCs with surface-defect-induced PL around 756 nm were water-soluble and synthesized via doping Met-capped Au NCs with Ag in a doping-in-growth way. By extensively exploiting the red-shifting nature of surface-defect-induced ECL to PL and the synergetic-effect-enhanced ECL of BNCs, physically surface-confined Au–Ag BNCs exhibited efficient NIR-II ECL around 906 nm in aqueous medium. A spectrum-based NIR-II ECL immunoassay around 915 nm was also achieved by immobilizing the Au–Ag BNCs onto an electrode surface via forming a sandwich immunocomplex, which could selectively determine CA125 from 5 × 10–4 to 1 U/mL with a detection limit of 5 × 10–5 U/mL (S/N = 3). The combined strategy of surface-defect-induced ECL and synergetic-effect-enhanced ECL would enable promising biorelated application of NIR-II ECL.
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ANALYTICA CHIMICA ACTA
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2021
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IF 6.558
Tianze Cong,Jianzhen Wang,Yongpeng Zhao,Dongmei Zhang,Zeng Fan,Lujun Pan
Au Nanostar (NS) monolayer as a surface enhanced Raman scattering (SERS) substrate has been synthesized by self-assembly at a water-oil interface. It is confirmed from the experiment and simulation results that the Au NS monolayer includes lots of “hot spots” at or between the tips of the Au NSs, enhancing the local electromagnetic fields and giving rise to strong SERS signals sequentially. The limit of detection is determined to be down to 4.2 × 10 −12 M for rhodamine 6G . Furthermore, the Au NS monolayer can detect multiple molecules, including thiabendazole , methylene blue , 4-mercaptobenzoic acid, and p-amino thiophenol , indicating that the SERS substrate composed of Au NS monolayer has potential applications in analytical chemistry , food safety, and environmental safety.
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ACS Applied Nano Materials
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2021
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IF 5.097
Shouren Zhang,Wenjing Yi,Yanzhen Guo,Ruibin Jiang,Xiao-Lan Chen,Baocheng Yang,Jianfang Wang
Driving organic reactions by heterogeneous photocatalysts is highly desired in green chemistry. (Plasmonic metal)/semiconductor heterostructures can greatly increase the photocatalytic activity by virtue of effective plasmonic harvesting of sunlight. Herein, we report on the driving of click reactions using (plasmonic Au nanosphere core)@(Cu2O shell) nanostructures under near-infrared light illumination. Upon plasmon excitation, the hybrid nanostructures exhibit excellent catalytic performance for the regioselective production of 1,2,3-triazoles. The yields of the click reactions under light illumination are about two times those of the reactions under sole thermal heating at the same temperatures. The reduced reaction yields in the presence of methanol, a hole scavenging agent, suggest that the plasmonic hot holes play a crucial role in the click reactions. Our results and the gained understanding will be valuable for the design of high-performance plasmonic photocatalysts for different regioselective organic reactions.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2021
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IF 4.464
Shanshan Wei,Haolin Xiao,Miao Gu,Zhencheng Chen,Liangli Cao
In this study, a sensitive and quantitative label-free electrochemical immunosensor based on bimetallic [email protected] nanoparticles , Prussian blue (PB), and reduced graphene oxide-tetraethylene pentamine nanocomposite (rGO-TEPA) was constructed to achieve sensitive detection of HBsAg. A one-pot green method was used to synthesize interlocked rGO-TEPA/PB hybrid composites as high-performance materials with good conductivity . PB was the electron transfer mediator used to provide electrochemical signals. By utilizing rGO-TEPA as supporting material , the stability and intensity of PB were greatly improved. The incorporation of highly conductive [email protected] nanoparticles could further amplify the electrochemical signal, and the high adsorption capacity could provide an efficient substrate for hepatitis B surface antibody (HBsAb) immobilization. Under optimal conditions, the immunoassay had a wide linear range from 0.25 pg mL −1 to 400 ng mL −1 and a low detection limit of 0.08 pg mL −1 (S/N = 3). This method was also applied to the analysis of human serum samples, and the obtained results were on par with those of electrochemiluminescence immunoassay (ECLIA), suggesting significant potential for this new method in clinical research.
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BIOSENSORS & BIOELECTRONICS
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2021
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IF 10.618
Fubin Pei,Shasha Feng,Yi Wu,Xuchu Lv,Hualai Wang,Shen-Ming Chen,Qingli Hao,Yang Cao,Wu Lei,Zhaoyang Tong
Aflatoxin B1 (AFB1) is the most toxic mycotoxin , is widely found in foods and animal feeds, and can pose a serious threat to our lives. A label-free photoelectrochemical (PEC) immunosensor was fabricated for the sensitive detection of AFB1. A Z-scheme heterojunction of gold nanoparticles (Au NPs) loaded on graphitic carbon nitride sheet and tungsten trioxide sphere composite (g-C 3 N 4 /Au/WO 3 ) acted as the highly sensitive platform. The g-C 3 N 4 /Au/WO 3 is capable, not only of immobilizing antibodies via Au NPs, but also enhancing the separation of electron-hole pairs due to its good energy band matching efficiency. The mechanism of photo-generated electron/hole transfer on g-C 3 N 4 /Au/WO 3 was explored using scavengers to eliminate active components. On this basis, an electron transfer pathway for the immunosensor was deduced. The PEC immunosensor displayed a linear concentration range from 1.0 pg mL −1 to 100 ng mL −1 and a low detection limit of 0.33 pg mL −1 (S/N = 3) for AFB1. Good reproducibility, stability, and specificity provide a solid foundation for the practical application of this immunosensor.
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Journal of Energy Chemistry
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2021
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IF 9.676
Zhiguo Zhu,Xiongjie Gao,Xiuming Wang,Mengdie Yin,Qingyao Wang,Wanzhong Ren,Bo Wang,Hongying Lü,Weiping Liao
The selective aerobic oxidation of biomass-derived 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid (FDCA, a potential renewable substitution of fossil-based terephthalic acid to produce polyethylene 2,5-furandicarboxylate plastic) is an appealing transformation for constructing eco-friendly and sustainable chemical processes. Au supported catalysts have showed encouraging performances for this well-received conversion, whose catalytic behavior was greatly affected by the adopted support derived from the existence of metal-support interactions. Herein, a series of Mg-Beta zeolites were hydrothermally synthesized via developed structural reconstruction, which were employed as basic supports for Au catalysts to construct bifunctional catalysts. The relationship between structure (Au particle size, basicity within zeolites and Au δ+ contents) and FDCA yield was concretely established. The conclusion was made that the utilization of Mg-Beta zeolites with strong basicity as the support could not only improve the FDCA yield but also decrease the amount of additional base. Furthermore, the possible reaction mechanism was also proposed via tracking time-dependent variations of corresponding organics and controlled experiment. This work provides some guidance for rationally designing multifunctional catalysts in the view of integrating metal catalysts with metallosilicate zeolites, which was beneficial to the catalytic upgrading of organic compounds with multiple functional groups.
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ANALYTICAL BIOCHEMISTRY
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2020
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IF 2.877
Zui Tao,Liting Wei,Shijia Wu,Nuo Duan,Xiang Li,Zhouping Wang
In this work, a colorimetric aptamer-based method for detection of cadmium using gold nanoparticles modified MoS 2 nanocomposites as enzyme mimic is established. In short, biotinylated Cd 2+ aptamers are immobilized by biotin-avidin binding on the bottoms of the microplate, the complementary strands of Cd 2+ aptamers are connected to the Au–MoS 2 nanocomposites which have the function of enhanced peroxidase-like activity. The csDNA-Au-MoS 2 signal probe and target Cd 2+ compete for binding Cd 2+ aptamer , the color change can be observed by addition of chromogenic substrate, thereby realizing visual detection of Cd 2+ . The absorbance of the solution at 450 nm has a clear linear relationship with the Cd 2+ concentration. The linear range is 1–500 ng/mL, and the limit of detection is 0.7 ng/mL. The assay was used to test white wine samples, the results are consistent with those of atomic absorption spectrometry ; which prove that this method can be used for detection of Cd 2+ in real samples.
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Applied Materials Today
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2020
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IF 8.352
Xueqin Wang,Tiandi Xiong,Miao Cui,Xinglei Guan,Jiacheng Yuan,Zichao Wang,Ruifang Li,Huiru Zhang,Shaofeng Duan,Fang Wei
Catalytic nanozyme-based tumor therapy is currently considered as a promising strategy in anti-tumor treatment, but it also has some disadvantages such as systemic toxicity, off-target, and non-specificity, leading to lowered therapeutic precision and efficacy in clinical curability. To overcome these limitations, herein we report a distinct strategy of nanocatalytic tumor precision therapy via tumor cell-specific CD44 targeted nanozyme-catalyzed cascade reactions. Briefly, the composite nanozyme CD44 MMSN/AuNPs were assembled with two self-activable nanocatalysts including the inner core peroxidase-mimic Fe 3 O 4 magnetic nanoparticles (MNPs), and the outer glucose oxidase-mimic AuNPs situated within large aperture mesoporous silicon (MMSN/AuNPs), and then functionalized with cell ligand hyaluronic acid (HA), which can specifically target transmembrane CD44 receptor of HepG2 tumor cells. In terms of catalysis, we found the coupled AuNPs effectively catalyzed glucose to produce H 2 O 2 , which was inversely catalyzed by Fe 3 O 4 NPs and AuNPs to produce more hydroxyl radicals (•OH) in tumor microenvironment (TME). That is, this composite nanozyme performed self-activable reactive oxygen species (ROS)-mediated cascade reactions, and thereby resulted in significantly specific growth inhibition of hepatocellular carcinoma HepG2 cells. The present results also showed that the composite nanozyme CD44 MMSN/AuNPs could specifically induce a greater number of HepG2 cell apoptosis and death. More importantly, we elucidated the mechanism of the composite nanozyme CD44 MMSN/AuNPs via inducing HepG2 cell apoptosis and death from subcellular level. Therefore, this study represents an insightful paradigm for achieving nanocatalytic tumor precision therapy through rationally designing tumor cell-targeting inorganic nanozyme with self-activable cascade reactions.
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ANALYTICAL CHEMISTRY
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2020
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IF 6.785
Guohua Qi,Dandan Wang,Chuanping Li,Kongshuo Ma,Ying Zhang,Yongdong Jin
Molecular diagnosis and accurate damage analysis of complex genomic DNAs in tumor cells are crucial to the theranostics of cancers but still a huge challenge. Herein, by designed preparation of a uniform plasmonic sunflower-like assembly gold (Au) nanostructure that is capable of efficient DNA capture and providing high-density gap-plasmon “hot spots” for adequate surface-enhanced Raman spectroscopy (SERS) enhancement, we succeeded in sensitive and reliable label-free SERS detection of DNA damage in electrostimulus-induced apoptotic cancer cells at the DNA base level for the first time. The SERS results showed that the external electrostimulus (at 1.2 V, for 5 min) was almost harmless to normal healthy cells, but it caused pronounced double strand break and adenine base damage in cancer cell DNAs, which effectively destroyed the reproduction and transcription of DNAs and ultimately induced cell apoptosis. The developed sensing platform and method are promising for cell study of genetically related diseases.
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APPLIED SURFACE SCIENCE
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2020
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IF 6.182
Guanhua Zhang,Tiantian Dai,Yue Meng,Lianyang Zhang,Chao Yang,Guoxiang Pan,Zheming Ni,Shengjie Xia
Z-scheme heterojunction catalysts are novel photocatalytic materials with wide application prospects because of their promise for the engineering of band structure to achieve high-speed hot carrier-transfer and strong redox tunability. A bridged-Au Z-scheme heterojunction catalyst (ZnO-Au-ZnAl 2 O 4 ) was synthesized using layered double hydroxides (LDHs) as the backbone. The atomistic and architectural structures, elemental composition and and visible-light absorption of as-prepared photocatalysts were systematically investigated and characterized. The presence of Z-scheme heterojunctions in ZnO-Au-ZnAl 2 O 4 can significantly improve the photocatalytic activity under visible light irradiation with a reaction rate constant of 0.5503 h −1 (ZnO-Au(2%)-ZnAl 2 O 4 ), 27.2 times that of pure ZnO (0.0202 h −1 ) and 9.8 times that of ZnO-ZnAl 2 O 4 (0.0389 h −1 ). We further investigated the reaction kinetics of the heterostructure catalyst in the photodegradation of catechol , where the effect of the catalyst dosage, initial pH, irradiation intensity and reaction temperature were discussed. Based on the mechanism study in the capture and detection of photo-generated radicals and the calculation of band structures by DFT (work function), the successful construction of bridged-Au Z-scheme heterojunction was further proven. Au nanoparticles sandwiched between ZnO and ZnAl 2 O 4 play a vital role for the formation of a built-in electric field (BIEF) between ZnO and ZnAl 2 O 4 , which can significantly facilitate the transfer of hot carriers in the photocatalytic system.
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ANALYTICA CHIMICA ACTA
·
2021
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IF 6.558
Yingzhou Tao,Yisheng Lin,Fang Luo,Caili Fu,Cuiying Lin,Yu He,Zongwei Cai,Bin Qiu,Zhenyu Lin
Hydrogen sulfide (H 2 S), as a hazardous gas, is often found around dump areas. Long term exposure can cause harm to health, it is highly necessary to develop some simple and sensitive methods for on-site H 2 S detection. Herein, a convenient photothermal assay has been designed for the quantitation of H 2 S using a handheld thermometer as readout. Au@Ag nanocubes (Au@Ag NCs), a core-shell nanocomposite with strong light absorption at ∼450 nm, was chosen as a novel photothermal agent in this study. Under the laser irradiation at 450 nm, the Au@Ag NCs show a strong photothermal effect, and a significant temperature enhancement can be measured by the thermometer easily. The presence of H 2 S can lead to the deposition of sulfur onto Au@Ag NCs, altering the localized surface plasmon resonance absorption, size, surface composition, and morphology of Au@Ag NCs and hence leading to the reduction of photothermal effect. The change of the temperature has a linear relationship with the H 2 S concentration in the range of 0.5–80.0 μM with a detection limit of 0.35 μM. By combining with simple sample purification procedures, the developed method has been applied to detect H 2 S in garbage odor gas with satisfactory results.
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BIOELECTROCHEMISTRY
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2020
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IF 4.722
Qingshan Yang,Ping Wang,Enhui Ma,Haoxuan Yu,Kaiwei Zhou,Chunyuan Tang,Jie Ren,Yueyun Li,Qing Liu,Yunhui Dong
In this work, a sandwich-type electrochemical immunosensor was fabricated to the effective detection of hepatitis B surface antigen (HBsAg). The designed electrochemical immunosensor was based on Au core and Pd shell nanodendrites loaded on amino functionalized molybdenum dioxide nanosheets (Au@Pd NDS/NH 2 –MoO 2 NSs) as the secondary antibody (Ab 2 ) label and silver nanoparticles were loaded by electrodeposited (D-Ag NPs) on the surface of electrode as the platform. Because of the synergistic effect and abundant catalytic activity sites provided by surface dendrite structure, Au@Pd NDs were more effective than single gold and palladium nanoparticles in catalytic reduction of hydrogen peroxide (H 2 O 2 ). MoO 2 had the good catalytic capacity for reduction of H 2 O 2 and favourable electrical conductivity . Hence, the obtained Au@Pd NDS/NH 2 –MoO 2 NSs were more effective than Au@Pd NDs and NH 2 –MoO 2 NSs in catalytic reduction of hydrogen peroxide attribute to a synergistic effect. Also, Ag NPs with admirable electrical conductivity and biocompatibility were used as sensing platforms and primary antibodies (Ab 1 ) carriers, which can accelerate the electron transfer and improve the sensitivity of the immunosensor. Here, the proposed electrochemical immunosensor offered a wide linear interval from 10 fg mL −1 to 100 ng mL −1 and the lower limit of detection of 3.3 fg mL −1 (S/N = 3) for detection of HBsAg under optimal experimental conditions. Furthermore, the accuracy of the actual serum sample analysis was satisfactory, which showed that the electrochemical immunosensor possessed a good application prospect in clinical detection.
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