JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Zeyu Jiang,Rui Dong,Mingjiao Tian,Chi He,Yani Wu,Mudi Ma,Shouning Chai
Realizing the simultaneous adsorption and activation of O 2 and reactants over supported noble metal catalysts is crucial for the oxidation of organic hydrocarbons. Herein, we report a facile one-step ethylene glycol reduction method to synthesize difunctional Au(OH)K x sites, which were anchored on a hierarchical hollow MFI support and adopted for acetone decomposition. The alkali ion-associated adjacent surface hydroxyl groups were coordinated with Au nanoparticles , resulting in partially oxidized Au 1+ sites with improved dispersion. The results obtained from exclusive ex situ and in situ experiments illustrated that the proper content of K and hydroxyl groups significantly enhanced the adsorption of surface O 2 and acetone molecules around the Au sites simultaneously, whereas the excess K species inhibited the catalytic performance by blocking the pore structure and decreasing the acidity of catalysts. The Au(OH)K 0.7 /h-MFI catalyst exhibited the highest efficiency for acetone oxidation, over which 1500 ppm acetone can be completely oxidized at just 280 °C with an extremely low activation energy of 32.5 kJ mol −1 . The carbonate species were detected as the main intermediates during acetone decomposition over the difunctional Au(OH)K x sites through a Langmuir − Hinshelwood (L − H) mechanism. This finding paves the way for designing and constructing efficient functional active sites for the complete oxidation of hydrocarbons.
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JOURNAL OF WUHAN UNIVERSITY OF TECHNOLOGY-MATERIALS SCIENCE EDITION
·
2023
·Vol. 38
·期 2
·274-279
·
IF 1.6
Hao Zhenbang,Tian Qihang,Cao Shiyi,Han Xiaoyu,Zhang Jihong,Xie Jun,Zhao Xiujian
Novel hollow Au Ag alloy nano urchins were synthesized via Ag seeds growth method, and self-assembly coated on the wall and end-tip of silica fiber for fiber probe fabrication. The nano urchins homogeneously distributed on fiber surface because of fiber silanization. The sizes and tip sharpness of the nano-urchins could be controlled by Ag seeds. The elements distribution analysis indicated there was high Ag content in tip-top for better surface enhance Raman scattering performance. The detectable concentration could be as low as 10 −8 M using crystal violet molecules as analyte. Moreover, the fiber probes were stable in air, due to Au in the alloy. This fiber probe could be used for low content single molecular analysis.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Zareen Zuhra,Shafqat Ali,Sajjad Ali,Hu Xu,Rongzhen Wu,Yuanyuan Tang
Designing materials for selective recovery of precious metals is a critical challenge in response to recent outbreaks of electronic wastes owing to economic and environmental concerns. We introduced high-performance hybrid materials (MCNTs) comprising of six-amino groups based on hexaaminobenzene metal-organic framework (HAB-MOF) and carbon nano-tube (CNT) sponge for selective recovery of Au(III) and Pd(II). Among all MOFs ever reported in the literature, the particular synthesized 30-MCNT (30 mg HAB-MOF on CNT sponge) exhibited the highest adsorption capacity ( q e ) of 1832 mg/g (45 °C, pH 3.0) for Au(III) and 1651 mg/g (45 °C, pH 1.0) for Pd(II), which can be regarded as a benchmark in the MOF family. The highly selective nature of 30-MCNT was examined in the presence of ten different metal ions and the results showed that the Au(III)/Pd(II) adsorption efficiency was decreased by only 5–10%. Moreover, the Au(III) and Pd(II) recovery was maintained ∼ 100% from the initial solution with metal concentration of 200 mg/L. The superior performance was mainly attributed to the role of abundant amino groups in the hybrid framework, developing several types of interactions with Au(III) and Pd(II) ions such as hydrogen bonding, electrostatic interactions, acid-base affinity and π-π inner sphere complexation. Furthermore, the remarkably high surface area and robust chemical and mechanical stability of CNT-sponge provided an exceptional support for impregnation of HAB-MOF to avail greater active sites and easier handpicked recycle. Density functional theory (DFT) simulation and X-ray photoelectron spectroscopy (XPS) studies were employed to explore the interaction mechanisms during the adsorption processes. Owing to facile and environment-friendly synthesis, excellent recovery and recycling, the material can be possibly considered for industrial application in precious metal recovery.
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Analytical Methods
·
2021
·Vol. 14
·期 3
·278-285
·
IF 2.896
Ting Zhou,Meijuan Li,Na Li,Yulin Dong,Dan Liu,Xiaosong Hu,Zhizhong Xie,Deyu Qu,Xi Li,Chaocan Zhang
An ultrasensitive and specific-selection electrochemical sensor was constructed for Hg2+ detection based on Au nanoparticles and molybdenum selenide (Au NPs@MoSe2) as well as the thymine–Hg2+–thymine (T–Hg2+–T) coordination. Herein, Au NPs@MoSe2 not only could improve the sensitivity due to the large surface area and good electrical conductivity but also offered more sites to immobilize thiol-labeled T-rich hairpin DNA probes (P-1), which has a specific recognition for Hg2+ and methylene blue-labeled T-rich DNA probes (MB-P). When Hg2+ and MB-P exist, P-1 and MB-P can form a stable T–Hg2+–T complex. Then, methylene blue can be close to the electrode and detectable via differential pulse voltammetry (DPV). Benefiting from the specific recognition of T–Hg2+–T and the merits of Au NPs and MoSe2, the fabricated biosensor presented an ultrasensitive and highly selective performance. The DPV responses had a positive linear relationship with Hg2+ concentrations over ten orders of magnitude from 1.0 × 10−16 to 1.0 × 10−7 mol L−1. The detection limit was down to 1.1 × 10−17 mol L−1. Moreover, the developed sensor exhibited a promising application for trace Hg2+determination in water samples.
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ANALYTICAL CHEMISTRY
·
2026
·
IF 7.3
Yingfang Zhang,Sihai Luo,Sen Jiang,Hao Sun,Hongyi Shen,Lijuan Chen,Qi Yuan,Xiaoliang Chen,Nan Zhang,Fang Mi,Yi Lv,Fenggang Ren,Jinyou Shao
Abstract The confinement of light into nanometer-sized (typically <10 nm) metallic nanogaps can generate extremely high near-field enhancement, dramatically boosting absorption, emission, and Raman scattering of target molecules situated within the gaps. However, the scarcity of cost-effective, reliable, and high-throughput nanofabrication techniques capable of fabricating sub-10 nm gaps, particularly in binary nanostructures, has significantly hindered their practical applications. Here, a high-throughput nanofabrication strategy that combines anodic aluminum oxide (AAO) templates, molecular self-assembly, and glancing-angle ion-beam etching (IBE) is proposed to controllably produce large-scale bimetallic gold–silver (Au–Ag) arrays with approximately 5 nm gaps. These arrays serve as exceptional surface-enhanced Raman spectroscopy (SERS) substrates, allowing for the ultrasensitive detection of target molecules with limits of detection (LODs) as low as 10–11 M for rhodamine 6G (R6G) and 4-mercaptobenzoic acid (4-MBA) and 10–8 M for bilirubin. The bimetallic Au–Ag nanogap arrays leverage the synergistic effects of gold’s strong absorption and silver’s superior plasmonic properties, achieving significantly enhanced electromagnetic fields compared to monolithic Au–Au nanogap arrays. This cost-effective and efficient nanofabrication approach overcomes the limitations of conventional methods for fabricating binary nanostructures, providing a viable solution for developing high-sensitive and reliable SERS-based detection platforms toward chemical-/bio-sensing.
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ANALYST
·
2023
·Vol. 148
·期 21
·5435-5444
·
IF 4.2
Yuqiu Wang,Shuchang Liu,Yongjun Hu,Cuicui Fu,Weiqiang Chen
We developed a highly sensitive and stable SERS-active substrate of Au@Ag@Ag core/shell/shell nanorods, formed by encapsulating Au nanorods (Au NRs) into a bilayer silver shell with Raman reporter molecules (4-mercaptobenzoic acid (4-MBA) and thiram) in the shell–shell gap. The core/shell/shell nanostructures demonstrated a high SERS enhancement and easy assembly. The important role of the bilayer silver shell in boosting the SERS intensity and detection sensitivity was revealed by comparing the performances of the Au@Ag@4-MBA@Ag NRs, Au@Ag@4-MBA NRs, and Au@4-MBA NRs. The obtained Au@Ag@4-MBA@Ag NRs exhibited a significantly promoted SERS intensity, which could reach around 2.6 times and 240 times that of the Au@Ag@4-MBA NRs and Au@4-MBA NRs, where the enhancement factor was found to be strongly correlated with the shell thickness. The controllable plasma properties and SERS effect of the Au@Ag@4-MBA@Ag NRs could be optimized by adjusting the dose of silver nitrate. The SERS substrate comprising core/shell/shell nanorods was highly reproducible and stable (retaining 83% SERS intensity after one month). Moreover, the highly sensitive detection of the pesticide thiram with a detection limit as low as 1.74 × 10−9 M was achieved by taking advantage of the great SERS response of the core/shell/shell nanostructures, which was 1–2 orders of magnitude lower than for other SERS substrates. The developed SERS substrate could be readily extended to embed other target analytes into the core/shell/shell nanostructure for novel and sensitive detection. This study could enable fresh approaches toward next-generation ultrasensitive analyte detection.
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Biosensors-Basel
·
2023
·Vol. 13
·期 10
·932
·
IF 5.4
Gang Peng,Mengxue Guo,Yuting Liu,Han Yang,Zuorui Wen,Xiaojun Chen
Hg2+, a highly toxic heavy metal, poses significant environmental and health risks, necessitating rapid detection methods. In this study, we employed an electrochemical aptasensor for rapid and sensitive detection of Hg2+based on DNA strands (H2 and H3) immobilized graphene aerogels-Au nanoparticles (GAs-AuNPs) hybrid recognition interface and exonuclease III (Exo III)-mediated cyclic amplification. Firstly, Gas-AuNPs were modified on the surface of the ITO electrode to form a sensing interface to increase DNA loading and accelerate electron transfer. Then, DNA helper was generated with the addition of Hg2+via Exo III-mediated cycling. Finally, the hairpin structures of H2 and H3 were opened with the DNA helper, and then the methylene blue (MB) functionalized DNA (A1 and A2) combined with the H2 and H3 to form an H-shaped structure. The current response of MB as an electrochemical probe was proportional to the concentration of Hg2+. Under optimal conditions, the aptasensor showed excellent performance for Hg2+, achieving a linear range from 1 fM to 10 nM and a detection limit of 0.16 fM. Furthermore, the aptasensor was used to detect Hg2+in spiked milk samples, achieving a high recovery rate and demonstrating promising application prospects.Keywords:graphene aerogels–Au nanoparticles;Hg2+;H-shaped;aptasensor;milk sample
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SENSORS AND ACTUATORS B-CHEMICAL
·
2021
·
IF 7.46
Muhammad Muhammad,Chang-sheng Shao,Qing Huang
A label-free, highly sensitive, and selective biosensor for detection of interleukin-6 (IL-6), which is an important inflammatory and cancer progression cytokine, has been achieved by combining gold nanoparticles (NPs) array surface-enhanced Raman spectroscopy (SERS) substrate and DNA aptamer. The SERS substrate consisted of Au NPs array is functionalized with the aptamer which is composed of the IL-6 recognition sequence and the output signal reporter. Upon recognition of target IL-6 in serum, the aptamer changes its conformation, resulting in the corresponding change of the output Raman intensity ratio (I 660 /I 736 ), with which the quantitative evaluation of IL-6 in 10 -12 -10 -7 M range can be realized. This SERS approach was employed to detect IL-6 in mice serum for inspecting the effect of drug and bacterial infection, and particularly, the radiation injury in the treated animals. This work therefore exemplifies that the aptamer-based SERS biosensor can serve as a promising tool for quick and convenient medical diagnosis applications.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Linsen Huang,Deyu Bao,Junhua Li,Xiaoqing Jiang,Xiaosong Sun
The residual antibiotics in water has become an environmental problem and is now deeply concerned. Z-scheme g-C 3 N 4 /defective ZnO heterojunction embellished with Au nanoparticles (Au-g-C 3 N 4 -ZnO) was synthesized by three sequential procedures, in-situ the preparation of g-C 3 N 4 , the guided cultivation of ZnO nanorods on g-C 3 N 4 nanosheets and the deposition of Au nanoparticles. The tailored photocatalysts, imbuing with inherent oxygen vacancies and outstanding light absorption capacity, exhibits unprecedented photocatalysis efficiency for tetracycline (TC) degradation. The formed Au-g-C 3 N 4 -ZnO implements broad-spectrum response, intensifying capacity of light harvest and utilization and promoting the separation and transmission efficiency of carriers. Remarkably, the photocatalytic degradation for TC by 2%Au-g-C 3 N 4 -ZnO achieves the best degradation efficiency of 74.7% within 30 min under Xe lamp irradiation. It displays excellent stability and acid or alkaline resistance. Besides, the TC degradation pathways are elucidated in line with intermediate degradation products. Finally, a novel Z-scheme heterojunction photocatalytic mechanism is rationally proposed based on the band structure, surface plasmon resonance effect, oxygen vacancies, charge transfer behaviors and active species generation.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Jun Cao,Qing Sun,Ai-Guo Shen,Bing Fan,Ji-Ming Hu
Killing harmful bacteria in biofilms is a major challenge for current root canal therapy. Although traditional chemical disinfectants have a good bactericidal effect on plankton, they have little efficiency for the removal and sterilization of bacterial biofilms, and even lead to the emergence of bacterial resistance and high toxic side effects. Herein, we propose for the first time biosafe nanocomposites that integrate photothermal and peroxidase-like catalytic activity for efficient removal and killing of bacterial biofilms in root canals. The integration of gold (core) and copper (Ⅰ, Ⅱ) sulfide (shell) shows excellent catalytic effect, which can catalyze the decomposition of hydrogen peroxide at biosafe concentrations to hydroxyl radicals for efficient removal of biofilms. Moreover, studies on the mechanism of antibiofilm showed that the nanocomposites ( [email protected] 2-x S) have significant degradation effects on proteins and polysaccharides-the main components of biofilm. The in vitro results indicated that the synergism of free radical and heat shows higher sterilization rate against both gram-positive Enterococcus faecalis and gram-negative Fusobacterium nucleus , compared with free radical and heat treatment alone. More importantly, the bactericidal results on isolated dental slices and in root canal models and beagle dog demonstrated the [email protected] 2-x S is highly effective in inactivating the bacteria in biofilms. Hence this safe and synergistic antimicrobial system has great potential in antibiofilm-oriented root canal therapy.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2021
·
IF 4.098
Ruyi Tang,Xuemin Xia,Xia Zhang,Huan Jiang,Baihui Wang,Peilei Zhang,Yujin Zhang,Yanxue Tang,Yi Zhou
A novel Au NPs/GeO 2 nanozymes are developed as Surface-Enhanced Raman Scattering (SERS) substrates with the promising prospect for detection ChI. Herein, it is discovered that both Au NPs and GeO 2 nanozymes have peroxidase-like activity, catalyzing colorless 3,3′,5,5′-tetramethylbenzidine (TMB) to produce blue TMB ox . Interestingly, compared with single Au NPs or GeO 2 nanozymes, the Au NPs/GeO 2 nanozymes show stronger peroxidase-like activity, and significantly ameliorated SERS signal of TMB ox . The mentioned two enhancements are ascribed to a positive synergistic function of Au NPs/GeO 2 nanozymes. Surprisingly, choline iodide (ChI) can inhibit the positive synergy in Au NPs/GeO 2 nanozymes, and slow down the reaction of TMB-H 2 O 2 -Au NPs/GeO 2 system. On this foundation, a new Au NPs/GeO 2 SERS technique with high sensitivity, label-free detection method of choline iodide (ChI) is established, suggesting that Au NPs/GeO 2 nanozymes have the potential application of water environment.
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Analytical Methods
·
2021
·Vol. 13
·期 20
·2290-2296
·
IF 2.896
Qianqian Zhao,Datong Wu,Zheng-Zhi Yin,Wenrong Cai,Haifeng Zhou,Yong Kong
A fluorescent chiral sensor is proposed based on the inner filter effect (IFE) of chiral Au nanoparticles (AuNPs) on MoS2 quantum dots (MoS2 QDs), which can be used for the discrimination of the isomers of tyrosine (Tyr). L-Tyrosine (L-Tyr) can induce obvious agglomeration of the chiral AuNPs, leading to an attenuated IFE of the chiral AuNPs and greatly restored fluorescence of the MoS2 QDs, and thus the enantioselective recognition of the Tyr isomers can be achieved. Also, L-Tyr but not D-Tyr induced agglomeration of the chiral AuNPs is confirmed by the larger association constant between L-Tyr and the chiral sensor.
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