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FOOD CHEMISTRY · 2020 · IF 6.306

Bimetallic core shelled nanoparticles (Au@AgNPs) for rapid detection of thiram and dicyandiamide contaminants in liquid milk using SERS

Abid Hussain,Da-Wen Sun,Hongbin Pu

Existing methods for contaminants detection in liquid milk are complex, requires chemicals and time-consuming experimental procedure. In this study, SERS based on bimetallic core shelled nanoparticles was employed for simultaneous and fast detection of thiram and dicyandiamide (DCD) in the milk. Spectra ranging from 400 to 1700 cm −1 were selected to examine thiram (0.5, 1, 2, 5 and 10 ppm) and DCD (20, 40, 80,160 and 320 ppm), by employing 28 nm gold cores and silver-shell thickness of 8 nm. A strong peak at 1379 cm −1 was ascribed to thiram with LOD of 0.21 ppm and R 2 of 0.9896, whereas a band at 929 cm −1 was associated with DCD, delivering LOD of 14.88 ppm and R 2 of 0.9956. The proposed method could achieve results within 34 min and this ecofriendly method can be further employed for simultaneous and rapid screening of other accidental contaminants in milk.

研究领域: 分析化学 · 食品科学 · 环境科学
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Journal of the American Chemical Society · 2017 · IF 13.858

PtPb/PtNi Intermetallic Core/Atomic Layer Shell Octahedra for Efficient Oxygen Reduction Electrocatalysis

Lingzheng Bu,Qi Shao,Bin E,Jun Guo,Jianlin Yao,Xiaoqing Huang

Although explosive studies on pursuing high-performance Pt-based nanomaterials for fuel cell reactions have been carried out, the combined controls of surface composition, exposed facet, and interior structure of the catalyst remains a formidable challenge. We demonstrate herein a facile chemical approach to realize a new class of intermetallic Pt–Pb–Ni octahedra for the first time. Those nanostructures with unique intermetallic core, active surface composition, and the exposed facet enhance oxygen reduction electrocatalysis with the optimized PtPb1.12Ni0.14 octahedra exhibiting superior specific and mass activities (5.16 mA/cm2 and 1.92 A/mgPt) for oxygen reduction reaction (ORR) that are ∼20 and ∼11 times higher than the commercial Pt/C, respectively. Moreover, the PtPb1.12Ni0.14 octahedra can endure at least 15 000 cycles with negligible activity decay, showing a new class of Pt-based electrocatalysts with enhanced performance for fuel cells and beyond.

研究领域: 材料科学 · 电化学
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BIOSENSORS & BIOELECTRONICS · 2018 · IF 8.173

Hierarchical nanocomposites with an N-doped carbon shell and bimetal core: Novel enzyme nanocarriers for electrochemical pesticide detection

Li Ma,Liya Zhou,Ying He,Lihui Wang,Zhihong Huang,Yanjun Jiang,Jing Gao

Core-shell structured nanocomposites (named PtPd@NCS) with N-doped carbon shell and bimetal core (Pt and Pd) were fabricated through a facile strategy for the first time. The PtPd@NCS nanocomposites were obtained through reduction of K 2 PtCl 4 , H 2 PtCl 6 and Na 2 PdCl 4 species, self-polymerization of dopamine (DA) and co-assembly of Pluronic F127 using a one-pot approach. DA serves as a reductant , as well as a carbon and nitrogen source. The core-shell structure of the PtPd@NCS nanocomposites was characterized and the result indicated that Pt-Pd nanoparticle core with a diameter of approximately 15 nm was encased in the N-doped carbon shells with a thickness of approximately 35 nm. The PtPd@NCS nanocomposites were used as an electrode material to prepare acetylcholinesterase (AChE) biosensors for detecting organophosphate pesticides . The obtained AChE biosensor exhibited a linear range of 1 × 10 –14 to 1 × 10 −10 M and 1 × 10 −9 to 1 × 10 −5 M within the detection limit of 7.9 × 10 –15 M for malathion , 1 × 10 –13 to 1 × 10 −6 within the detection limit of 7.1 × 10 –14 M for chlopyrifos, and 1 × 10 –14 to 1 × 10 –11 M and 1 × 10 −10 to 1 × 10 −5 M within the detection limit of 8.6 × 10 –15 M for parathion methyl . The proposed biosensor also exhibited high selectivity, reproducibility and stability. The AChE biosensor was also applied in real samples for detecting organophosphate pesticides and exhibited acceptable recovery. This work demonstrated that the PtPd@NCS had great potential in constructing biosensors to detect organophosphate pesticides and other analytes.

研究领域: 材料科学 · 环境科学 · 分析化学 · 生物技术
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Sulfur dioxide-resistant platinum-based intermetallic nanocatalysts encaged by porous nitrogen-doped carbon for oxygen reduction reaction

Manli Wang,Longsheng Cao,Zhicheng Liu,Wenbing Yang,Shucheng Sun,Ming Hou,Zhigang Shao

SO 2 , one of the considerable air pollutants, exhibits a stronger binding affinity with Pt when compared to O 2 , thereby inducing irreversible degradation of the Oxygen Reduction Reaction (ORR) catalyzed by Pt-based catalysts. Despite this detrimental phenomenon, scarce investigations have delved into the realm of contaminant-tolerant catalysts, and so far, no effective SO 2 -tolerant catalysts have been proposed. To meet this challenge, we designed and synthesized a core–shell structure catalyst equipped with a dual protection mechanism. This was achieved through the in-situ polymerization of aniline monomers, concomitantly reducing Pt 2+ . The resulting shell effectively hinders the transmission of SO 2 to the active sites of Pt, while permitting the unimpeded transmission of O 2 . Simultaneously, the intermetallic core inhibits the adsorption of SO 2 . Therefore, this catalyst exhibits exemplary ORR activity coupled with exceptional resistance to SO 2 resistance. In particular, the PtFe@FeNC/C-10 catalyst, optimized in terms of the quantity of added aniline, demonstrates a mass activity 1.84 times greater and a specific activity 4.03 times higher than that of commercial Pt/C catalysts. Following exposure to SO 2 -induced poisoning, the E 1/2 value of the PtFe@FeNC/C-10 catalyst undergoes a decrease of only 51.7 mV, lower than that observed for the commercial Pt/C catalyst (92.0 mV). Moreover, the results of an accelerated durability test affirm the superior stability of PtFe@FeNC/C-10 in comparison to commercial Pt/C. This stability advantage is attributed to the protective carbon shell, which effectively prevents the detachment and agglomeration of Pt nanoparticles .

研究领域: 材料科学 · 催化化学
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ADVANCED MATERIALS · 2025 · IF 26.8

Synergistic Enhancement of Fluorescence Through Plasmon Resonance and Interfacial Charge Transfer by AgNC@AgAux Core–Shell Quantum Dots

Youlong Chen,Yihua Hu,Yushuang Zhang,Hao Huang,Xing Yang,Youlin Gu,Fanhao Meng,Yuhao Xia,Ziwei Fu,Xinyuan Zhang,Junhao Chu

Bimetallic core–shell quantum dots (QDs) hold great promise in elucidating the bimetallic synergism and optoelectronic devices. The synthesis and properties of AgNC@AgAu x QDs of core–shell heterostructure are reported. Significantly enhanced photoluminescence emission on these heterostructures is observed. These enhancements are attributed to electron injection and the surface plasmon-induced strong local electric field, which are observed through time-resolved transient absorption spectroscopy. X-ray absorption near edge structure spectra and density functional theory confirms the electron injection from the Ag core to the AgAu x shell. On the other hand, the plasmon resonance of the AgNC@AgAu x QDs has been studied by finite-element method analysis and time-resolved photoluminescence spectra. There are 94.06 times fluorescence enhancement and 32.40 times quantum yield improvement of oxygen content correlation compared to AgAu 3 QDs. It shows a perfect correlation coefficient of 98.85% for the detection of heavy metal Cu 2+ ions. Such Bimetallic core–shell heterostructures have great potential for future optoelectronic devices, optical imaging, and other energy-environmental applications.

研究领域: 材料科学 · 光学 · 环境科学
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Nano Research · 2019 ·Vol. 13 ·期 5 ·1354-1362 · IF 8.515

(Metal yolk)/(porous ceria shell) nanostructures for high-performance plasmonic photocatalysis under visible light

Jiang Nina,Li Danyang,Liang Lili,Xu Qing,Shao Lei,Wang Shi-Bin,Chen Aizheng,Wang Jianfang

We describe a route to the preparation of (metal yolk)/(porous ceria shell) nanostructures through the heterogeneous growth of ceria on porous metal nanoparticles followed by the calcination-induced shrinkage of the nanoparticles. The approach allows for the control of the ceria shell thickness, the metal yolk composition and size, which is difficult to realize through common templating approaches. The yolk/shell nanostructures with monometallic Pt and bimetallic PtAg yolks featuring plasmon-induced broadband light absorption in the visible region are rationally designed and constructed. The superior photocatalytic activities of the obtained nanostructures are demonstrated by the selective oxidation of benzyl alcohol under visible light. The excellent activities are ascribed to the synergistic effects of the metal yolk and the ceria shell on the light absorption, electron-hole separation and efficient mass transfer. Our synthesis of the (metal yolk)/(porous ceria shell) nanostructures points out a way to the creation of sophisticated heteronanostructures for high-performance photocatalysis.

CAS / MDL: 31175-20-9
研究领域: 材料科学 · 化学工程 · 纳米技术
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Journal of Environmental Chemical Engineering · 2024 · IF 7.4

Enhanced peroxymonosulfate activation via MOF-derived bimetal core-shell Co-Fe@NC hybrids to degrade emerging pollutants

Hui Li,Xinlei Ren,Wenxue Pan,Shiting Zhu,Jin Zhang,Zhiyuan Yang,Liu Qian,Yueying Wang,Yujing Huang,Lin Guo,Minghui Xiang

The reasonable control of the structure of metal–organic frameworks (MOFs) is a promising strategy for improving their peroxymonosulfate (PMS) activation activity. In this study, ZIF-67 @ZIF-8 was used as a template to prepare bimetallic core–shell Co-Fe@NC via Fe doping and high-temperature carbonization . Co-Fe@NC maintained the core–shell structure of the original MOF, in which cobalt was uniformly distributed in the nitrogen-doped graphite carbon skeleton and the surface of the graphite carbon skeleton was covered with iron. With the synergistic effect of the nitrogen-doped graphite carbon skeleton, iron, and cobalt, 100% of tetrabromobisphenol S (TBBPS) was removed in 60 min with k obs = 0.062 min −1 in Co-Fe@NC-0.2/PMS system. The addition of iron increased the graphitization degree with I D /I G value increased from 0.98 (Co@NC) to 1.034 (Co-Fe@NC-0.2) and electron transfer rate of the carbon skeleton. Besides, the Co leaching was effectively attenuated from 1.86 mg/L(Co@NC) to 0.78 mg/L (Co-Fe@NC-0.2) by the core-shell structure and bimetal strategy. Both O 2 · - and 1 O 2 contributed to the degradation of TBBPS according to quenching experiments. TBBPS was deeply degraded into small-molecule compounds through three degradation pathways by the Co-Fe@NC-0.2/PMS system. This study provides a new strategy for designing highly efficient bimetal–carbon composites for environmental remediation.

研究领域: 环境科学 · 材料科学 · 化学工程
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Nature Communications · 2023 ·Vol. 14 ·期 1 ·1-12 · IF 16.6

Suppression of kernel vibrations by layer-by-layer ligand engineering boosts photoluminescence efficiency of gold nanoclusters

Zhong Yuan,Zhang Jiangwei,Li Tingting,Xu Wenwu,Yao Qiaofeng,Lu Min,Bai Xue,Wu Zhennan,Xie Jianping,Zhang Yu

The restriction of structural vibration has assumed great importance in attaining bright emission of luminescent metal nanoclusters (NCs), where tremendous efforts are devoted to manipulating the surface landscape yet remain challenges for modulation of the structural vibration of the metal kernel. Here, we report efficient suppression of kernel vibration achieving enhancement in emission intensity, by rigidifying the surface of metal NCs and propagating as-developed strains into the metal core. Specifically, a layer-by-layer triple-ligands surface engineering is deployed to allow the solution-phase Au NCs with strong metal core-dictated fluorescence, up to the high absolute quantum yields of 90.3 ± 3.5%. The as-rigidified surface imposed by synergistic supramolecular interactions greatly influences the low-frequency acoustic vibration of the metal kernel, resulting in a subtle change in vibration frequency but a reduction in amplitude of oscillation. This scenario therewith impedes the non-radiative relaxation of electron dynamics, rendering the Au NCs with strong emission. The presented study exemplifies the linkage between surface chemistry and core-state emission of metal NCs, and proposes a strategy for brighter emitting metal NCs by regulating their interior metal core-involved motion.

研究领域: 材料科学 · 纳米技术 · 光学 · 化学
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Materials Chemistry Frontiers · 2023 ·Vol. 7 ·期 6 ·1100-1109 · IF 7

Highly homogeneous bimetallic core–shell Au@Ag nanoparticles with embedded internal standard fabrication using a microreactor for reliable quantitative SERS detection

Suyang Li,Junjie Chen,Wanbing Xu,Biao Sun,Jiechen Wu,Qiang Chen,Pei Liang

Bimetallic gold core–silver shell (Au@Ag) surface-enhanced Raman scattering tags draw broad interest in the fields of biological and environmental analyses. Herein, an efficient hybrid microfluidic chip was designed to prepare uniform Au@Ag core–shell nanoparticles, and DTNB was used as the internal standard tag molecule to prepare Au@DTNB@Ag for SERS detection. Homogeneous core–shell nanoparticles with a particle size of 90 nm were prepared by mixing a silver precursor and a gold core in a microfluidic chip. The relative standard deviation (RSD) of the particle size distribution was close to 10%, and the detection limit of 4-MBA was as low as 10-10 M. In order to solve the influence of SERS signal fluctuation, a uniform Au@DTNB@Ag core–molecule–shell structure was synthesized in a microfluidic chip, and the characteristic peak of the analyte was corrected by the relative intensity of the DTNB characteristic peak (1335 cm−1). The experimental results showed that the SERS detection was achieved with high reproducibility, and the SERS peak intensity had a good linear correlation with the concentration. The homogeneous SERS substrate prepared using a microfluidic chip has potential for sensitive and reliable detection of environmental chemical contaminants.

研究领域: 纳米技术 · 分析化学 · 环境科学 · 材料科学
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BIOMATERIALS · 2019 · IF 10.273

A sandwich-type electrochemical aptasensor for Mycobacterium tuberculosis MPT64 antigen detection using C60NPs decorated N-CNTs/GO nanocomposite coupled with conductive PEI-functionalized metal-organic framework

Yuhan Chen,Xinzhu Liu,Shuliang Guo,Jun Cao,Jing Zhou,Jianli Zuo,Lijuan Bai

The present work described a novel sandwich-type electrochemical aptasensor for rapid and sensitive determination of Mycobacterium tuberculosis MPT64 antigen. Herein, a novel carbon nanocomposite composed of fullerene nanoparticles , nitrogen-doped carbon nanotubes and graphene oxide (C 60 NPs-N-CNTs/GO) was facilely synthesized for the first time, which not only possessed a large specific surface area and excellent conductivity , but also exhibited outstanding inherent electroactive property, and therefore served as nanocarrier and redox nanoprobe simultaneously. Gold nanoparticles (AuNPs) was then uniformly anchored onto the surface of such nanocomposite via Au–N bonds to bind with MPT64 antigen aptamer Ⅱ (MAA Ⅱ), forming the tracer label to realize generation and amplification of electrochemical signal. Additionally, conductive polyethyleneimine (PEI)-functionalized Fe-based metal-organic framework (P-MOF) was used as a sensing platform to absorb bimetallic core-shell Au–Pt nanoparticles ( [email protected] ), which could accelerate electron transfer and increase the immobilization of MPT64 antigen aptamer Ⅰ (MAA Ⅰ). After the typical sandwich-type protein-aptamer recognition, the inherent electroactivity of the tracer label was provoked by tetraoctylammonium bromide (TOAB), leading to a well-defined current response. Under the optimum condition, the proposed aptasensor showed a wide linear range for MPT64 detection from 1 fg/mL to 1 ng/mL with a limit of detection (LOD) as low as 0.33 fg/mL. More importantly, it was successfully used for MPT64 antigen detection in human serum, exhibiting a promising prospect for TB diagnosis in clinical practice.

研究领域: 分析化学 · 纳米技术 · 生物医学工程 · 电化学 · 生物传感器 · 医疗诊断
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