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MICROCHEMICAL JOURNAL · 2022 · IF 5.304

Ultrasensitive “signal-on” sandwich electrochemiluminescence immunosensor based on Pd@Au-L-cysteine enabled multiple-amplification strategy for Apolipoprotein-A1 detection

Jilan Qi,Xiaolei Zhang,Qiangyan Zhang,Ying Xue,Fei Meng,Yuanhua Liu,Gongjun Yang

In this work, a “signal on” electrochemiluminescence (ECL) strategy was proposed to detect Apolipoprotein-A1 (Apo-A1), a common tumor biomarker for bladder cancer. The tris(2,2′-bipyridyl)-ruthenium(II) [Ru(bpy) 3 2+ ] was used as luminophor captured by three-dimensional (3D) zinc oxalate metal–organic frameworks (MOFs), which constructed as the ECL nanoprobe (Ru-MOF) for detecting Apo-A1. Meanwhile, L-cysteine (L-Cys) as the co-reactant was connected to the [email protected] core–shell nanostructure through Au-S bond, which was directly modified on the glassy carbon electrode (GCE) to significantly reduce the electron transfer distance between the luminophor and co-reactant. The ECL intensity was “signal on” when the ECL probe of Ru-MOF was linked to the electrode by the immunoreaction of antigen–antibody. Based on these principles, the quantitative relationship between the concentration of Apo-A1 and the ECL intensity was obtained in the range of 1.00 fg·mL −1 to 1.00 ng·mL −1 with a linear coefficient of 0.9968. The proposed ECL immunosensor showed some great advantages, such as simplification, rapidity, stability and selectivity. It was also successfully applied for the determination of Apo-A1 in real serum and urine samples with the recovery of 98.0% ∼ 115.0% (RSD < 5.2%). To sum up, a “signal on” ECL immunosensor was successfully constructed for Apo-A1 detection, and it may facilitate the diagnosis of bladder cancer in clinic.

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NEW JOURNAL OF CHEMISTRY · 2022 ·Vol. 46 ·期 20 ·9595-9601 · IF 3.925

The controllable synthesis of orange-red emissive Au nanoclusters and their use as a portable colorimetric fluorometric probe for dopamine

Hongbo Wu,Yingjie Xu,Ruyan Xie,Mingyu Tang,Lihua Chen,Fengyu Qu,Changhong Guo,Fang Chai

Facile and accurate detection of dopamine (DA) in biological samples is crucial for diagnostic needs. This study reports a portable colorimetric fluorescent probe for the tracing of DA based on orange-red emitting Au nanoclusters (AuNCs). The AuNCs were reduced and stabilized with L-methionine by strictly controlling the reaction conditions. The resultant L-methionine capped AuNCs (M-AuNCs) exhibit bright and stable orange-red emission with a quantum yield of 31.08%. The excitation/emission wavelength is located at 420 nm/610 nm, and the large Stoke's shift of 190 nm endows the M-AuNCs with great potential as a late-model sensing probe for life studies and environmental science. The M-AuNCs exhibit unique specificity and excellent sensitivity for tracing DA by an “on–off” strategy with a lower limit of detection (LOD) of 3.96 nM (S/N = 3) within a linear range of 10–100 nM. Notably, the colorimetric detection results can be explored as a visual sensor for sensitive, reliable and real-time/on-site detection of DA with the assistance of a smartphone. The LOD can be determined as 81.94 nM within a wide linear range of 0.1–1.0 μM by a smartphone. Furthermore, the M-AuNCs as a late-model potable probe allow simple and rapid discrimination of DA in serum, and the cellular imaging of the M-AuNCs indicated that the detection of DA can also be achieved in living cells, demonstrating their great feasibility for the tracing of DA in real samples.

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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY · 2022 · IF 7.129

A highly parallel DTT/MB-DNA/Au electrochemical biosensor for trace Hg monitoring by using configuration occupation approach and SECM

Dandan Kong,Xinyue Li,Yang Tang,Ming Sui,Jinping Li,Yonggui Ma,Gaofeng Wang,Wei Gu,Xuegang Guo,Meihua Yang

Environmental pollution and medicine safety have aroused increasing public concerns due to human health. Amongst various contaminants, mercury is of special attention owing to their environmental persistence and biogeochemical recycling and ecological risks. Herein, a simple and highly parallel electrochemical biosensor for Hg determination was designed and investigated. The proposed biosensor was prepared and compared between (1) DTT/MB-DNA/Au with configuration occupation approach and (2) MCH/MB-DNA/Au with passivation approach. According to the combined results of scanning electrochemical microscope (SECM) and Randles-Sevcik equation, the DTT modified electrode exhibited high uniformity on DNA distribution and superb stability on electron transfer in Hg 2+ detection. Evidentially, the response value of proposed DTT/MB-DNA/Au was increased from 57.518% to 97.607%, while RSD% between duplicate runs had dropped from 22.658% to 0.223% (n = 3). Moreover, the increased proportion of effective working area was 467.380% compared with general sensors. Besides, DTT concentration, DNA concentration as well as assembly time were optimized, utilizing electrochemical impedance spectroscopy (EIS), Cyclic Voltammetry (CV) and Square Wave Anode Stripping Voltammetry (SWASV). This optimized biosensor exhibited an excellent selectivity toward Hg 2+ over Cu 2+ , As 2+ , Cd 2+ , Pb 2+ , Cr 3+ , Ni 2+ and Zn 2+ etc., and the stability of DTT/MB-DNA/Au were at least two times better even after 3 days under room temperature. Also, a linear relation was observed between the peak current and Hg 2+ concentrations in a range from 0.25 nM to 2.00 μM with a detection limit of 53.00 pM under optimal conditions. Finally, DTT/MB-DNA/Au was applied for plants and medical products analysis. In all, this optimized DTT/MB-DNA/Au with advantages of high repeatability and sensitivity would provide a new insight into the design and application of biosensor for reliable sensing in safeguarding plant protection and medicinal safety.

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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY · 2022 · IF 4.831

Rapid and sensitive SERS detection of opioids in solutions based on the solid chip Au-coated Si nano-cone array

Lingyi Zhao,Ruiqin Yang,Yi Wei,Yujing Guo,Qian Zhao,Hongwen Zhang,Weiping Cai

Rapid and flexible detection or accurate recognition of trace drugs is of great importance in cracking down on drug crimes, but it remains to be expected. Here, a solid chip is presented for the efficient detection and recognition of trace opioids (typically morphine) in aqueous solutions based on surface-enhanced Raman spectroscopy (SERS). Firstly, a Au-coated Si nano-cone array (Au-SNCA) is designed and fabricated via Si-based organic colloidal template etching and Au deposition. This Au-SNCA shows three-dimensional nanostructure with high densities of nanotips and deep nanogaps as well as high structural consistency, which exhibits strong SERS activity to morphine and outstanding stability. Then, such Au-SNCA is used as solid SERS chip to detect morphine in aqueous solutions. It has been demonstrated that using such solid chip, trace morphine in solutions could be recognized and detected within 1 min, and the detection limit is 10 -5 mg/mL (∼10 ppb), showing rapid and sensitive detection , which is much better than the previous reports. Meanwhile, the Au-SNCA chip also can be utilized to detect trace morphine in tap water and reservoir water, the recoveries range from 90.4% to 102.4%. Such excellent SERS performance of this Au-SNCA chip is attributed to its special structure which enhances not only local electromagnetic field but also molecular adsorption . The experimental results about the effects of immersion time and concentration show that the adsorption behavior of morphine molecules on such Au-SNCA chip can be explained by the pseudo-second-order kinetic model and Freundlich adsorption mode. Moreover, the Au-SNCA chip is also suitable for the identification of morphine homologues and the broad-spectrum detection of various common drugs. This study presents a practical solid chip and a simple approach for the efficient SERS detection and recognition of trace drugs in solutions. This is of significance to on-site detect drugs in forensic science.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

A dual-functional fluorescent probe for simultaneous visualization and quantification of Au and Pd species in environmental and biological systems

Yabing Gan,Guoxing Yin,Zhaomin Xu,Huyang Zhou,Ting Yu,Haitao Li,Peng Yin

Gold (Au) and palladium (Pd) species have been widely used in synthetic chemistry, biology, and environmental sciences, raising hard-to-ignore health and environment risks due to their potential toxicity. Herein, a novel dual-functional fluorescent probe was rationally designed and developed for simultaneous quantification and visualization of Au 3+ and Pd species in the environmental and biological systems. Significant fluorescence enhancement at 484 and 606 nm and color changes were observed upon addition of Au 3+ and Pd 0 with high sensitivity. The detection limit for Au 3+ and Pd 0 was as low as 68 nM and 7 nM, respectively. Combined with smartphone chromaticity and dual-channel fluorescence imaging analysis, this probe was successfully applied to the quantification and visualization of Au 3+ and Pd species in real water samples. Thus, simultaneous naked-eye visualization and quantification of Au 3+ and Pd 0 in real water samples was achieved using this probe. The probe was also successfully applied to fluorescence imaging of Au 3+ and Pd 0 in HeLa cells and zebrafish, promoting the monitor and understanding about gold and palladium species in environmental and biological systems.

CAS / MDL: 3326-32-7
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APPLIED SURFACE SCIENCE · 2022 · IF 7.392

Electrochemical fabrication of Ru[bpy]32+@Cu-MOF(-SH)/Au photo/electrochemical coupling interface and its DNA-based biosensing performance

Xianda Han,Zhigang Yu,Yangkejia Xiang,Fengqin Li,Xiaoping Tan,Lan Xu,Guiling Zhang

An electrochemical fabrication method of Ru[bpy] 3 2+ @Cu-MOF(-SH)/Au (MOF = metal–organic framework) was developed with a photo/electrochemical information characterization and a DNA-based biosensing validation for the proposed interface. Applying an anodic synthesis method, a modification layer of Ru[bpy] 3 2+ encapsulated with MOF was formed on the Au electrode surface to fabricate an interface with photo/electrochemical dual-signal response. Combining the scanning electrochemical microscopy (SECM) imaging technology with electrochemical and electrochemiluminescence (ECL) detection, the information about the interfacial photo/electrochemical bi-functional properties was explored from three aspects of the parameter variable, intensity variable, and morphology variable. The results show that the effect of parameter variables on the interfacial response follows an “interference effect” mechanism. Under the optimized conditions, the background and the saturation ECL intensities are 610.0 and 24.0 with a quenching efficiency of 96.1% and a detection limit of 30 fM. The saturation current is 48.8 µA with a detection limit of 330.0 nM. Both ECL and electrochemical imaging methods can corroborate each other, validating the logical correlation between the interface fabrication and the response performance in the regional interfacial distribution and laying a methodological foundation for evaluating the interface fabrication quality based on imaging morphology qualitatively. The proposed interface can construct photo/electrochemical dual-signal DNA-based biosensors.

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VIBRATIONAL SPECTROSCOPY · 2022 · IF 2.382

Thermal annealing-boosted photoinduced electron transfer efficiency of g-C3N4/Au NPs hybrids for promoting SERS detection of uric acids

Chang Wang,Qingqiang Cui,Tian Yue,Anxin Jiao,Hui Ma,Mengya Zhang,Linqi Zheng,Shuang Li,Guanhua Li,Ming Chen

As for the ultrasensitive diagnosis of biomolecules via surface-enhanced Raman scattering spectroscopy (SERS), the primary requirement is to effectively enhance the activity of nano-substrates. Herein, we report an interesting strategy for further boosting SERS activity by thermal annealing treatment of as-prepared hybrid substrates. Initially, highly dense and monodisperse plasmonic Au nanoparticles (NPs) were loaded on two-dimensional (2D) graphitic carbon nitride (g-C 3 N 4 ) nanosheets . By adopting uric acids (UAs) as probe biomolecules, the g-C 3 N 4 /Au NPs with appropriate ~2.1% Au compositions exhibit much higher Raman signals than that of the hybrids with other Au contents. Besides the enhancement by routinely controlling hybrid components, the further maximizing SERS activity with a ~2.6-fold improvement than the original one can be obtained by thermal annealing of g-C 3 N 4 /Au NPs at 350 ℃ condition. It enables the thermal modified g-C 3 N 4 /Au NPs to be applied for highly sensitive monitoring of UAs in artificial urine. The corresponding detection limit is achieved at the ultralow level of 10 −11 M, which is nearly two orders of magnitude better than that of the unannealed sample. It should be attributed to the stronger synergistic coupling effect by thermal annealing treatment that gives rise to the higher-efficiency photoinduced electron transfer (PIET) between g-C 3 N 4 supports and plasmonic Au NPs. The present work provides a new opportunity for further promoting the SERS activity of prefabricating nano-substrates, holding great potential for practical monitoring of ultra-trace biomolecules in the near future.

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FOOD CHEMISTRY · 2022 · IF 9.231

Development of a Nafion-MWCNTs and in-situ generated Au nanopopcorns dual-amplification electrochemical aptasensor for ultrasensitive detection of OTA

Yujiao Hou,Nan Long,Qingbin Xu,Ying Li,Pengyue Song,Minghan Yang,Jiabo Wang,Lidong Zhou,Ping Sheng,Weijun Kong

Trace detection of ochratoxin A (OTA) in foods is essential to mitigate risks to human health. Herein, a label-free electrochemical (EC) aptasensor based on dual-signal amplification of Nafion dispersed multi-walled carbon nanotubes (Nafion-MWCNTs) and Au nanopopcorns was developed for ultrasensitive detection of OTA. Nafion solution prevented the leaching of MWCNTs, and the Nafion-MWCNTs modified screen-printed carbon electrode (SPCE) acted as the sensing substrate which facilitated the uniform distribution of the electrodeposited Au nanopopcorns. The in-situ generated Au nanopopcorns could not only load a large amount of aptamers for specific identification of OTA, but also promote the electron transfer of the sensing platform. The incorporation of Nafion-MWCNTs and Au nanopopcorns realized dual-amplification of the aptasensor due to the enhanced conductivity and the increased electroactive surface area of the electrode. The modified electrodes were characterized through scanning electron microscopy, X-ray photoelectron spectroscopy and EC evaluation. Under optimal conditions, the electrochemical impedance spectroscopy (EIS) was measured for the determination of OTA. The as-fabricated Au nanopopcorns/Nafion-MWCNTs impedimetric aptasensor displayed excellent sensitivity with a detection limit as low as 1 pg/mL and a wide linear range of 1 pg/mL-10 ng/mL for OTA. Practical application of the aptasensor in the spiked malt samples achieved satisfactory recoveries of 89.82–95.65 %, which was also successfully verified to detect OTA in eleven batches of actual malt samples collected from the local market. The creative aptasensor is simple, cost-effective, sensitive, and accurate, showing great promise for on-site monitoring of other trace contaminants in foods by simply replacing the aptamers.

CAS / MDL: 51805-45-9
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

N-hexane-assisted synthesis of plasmonic Au-mediated polymeric carbon nitride photocatalyst for remarkable H2 evolution under visible-light irradiation

Manyi Gao,Weiwei Yang,Yongsheng Yu,Jiaming Li,Yequn Liu

Plasmonic Au-mediated polymeric carbon nitride (PCN) has been recognized as one of the promising materials for photocatalytic applications due to its excellent properties in wide visible light spectrum, however it is still hindered by low catalytic efficiency. In this work, it was established that strong metal-support interactions (MSI) at the interface between plasmonic Au nanoparticles (NPs) and PCN nanosheets (PCNS) improves its photocatalytic efficiency. The resulting Au/PCNS 2.5 exhibits excellent photocatalytic activity with H 2 evolution rate up to 4.84 mmol g -1 h -1 under visible light, 12.4 times higher than that of bulk PCN. Such strong MSI significantly strengthens the localized surface plasmon resonance (LSPR) effect of Au NPs and the charge “pump” role of Schottky junctions at Au-PCNS interface, resulting in broad light absorption range as well as effective separation and transfer of charge carrier. This work provides a new way to design the plasmonic photocatalysts for splitting water as well as other plasmon-driven chemical reactions.

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Applied Materials Today · 2021 · IF 10.041

Antisense oligonucleotides-Laden UiO-66@Au nanohybrid for enhanced radiotherapy against hypoxic tumor by dual-inhibition of carbonic anhydrase IX

Kai Wang,Shuaishuai Ding,Lijuan Zeng,Jingrong Zhou,Yuhua Cao,Jiaqian Wu,Lu Lu,Xiu-wu Bian,Gan Tian

Hypoxia-acquired radioresitance is considered to be a major factor responsible for the clinical failure of radiotherapy. Carbonic anhydrase IX (CA IX), a hypoxia-induced cell-surface enzyme involved in pH regulation of hypoxic solid tumors, has been acknowledged as a desirable target for cancer therapy. Herein, we developed a dual exogenous/endogenous CA IX inhibition strategy using core/satellite-like metal-organic framework (UiO-66)/gold nanoparticles (Au NPs) nanohybrids as a therapeutic platform for hypoxia-relief enhanced RT of triple negative breast cancer. The UiO-66 matrix supported the Au NPs generation in situ and would decompose inside tumor cells by the high-concentration phosphates to release p -phthalic acid (PTA), a original building skeleton of the UiO-66 matrix, to inhibit CA IX, while the decorated Au NPs served as radiosensitizers to potentiate the sensitivity of tumor cells to X-ray and yet provided active sites for CA IX antisense oligonucleotide (ASO) loading via formation of stable Au-S bond to knockdown CA IX. The dual inhibitory manner, exogenous inhibition from PTA and endogenous inhibition from CA IX ASO, largely alleviated the hypoxia-induced resistance and synergized with Au NPs-mediated radiosensitization to afford super therapeutic outcome in vitro and in vivo , supporting the feasibility of our synergistic RT strategy in hypoxic tumor management.

CAS / MDL: 100-21-0
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ACS Nano · 2021 · IF 15.881

Wide-Range and Highly Sensitive Chiral Sensing by Discrete 2D Chirality Transfer on Confined Surfaces of Au(I)-Thiolate Nanosheets

Yang Yu,Guojian Yang,Shengrui Zhang,Mo Liu,Shujue Xu,Chunyu Wang,Minjie Li,Sean Xiao-An Zhang

Circular dichroism (CD) chiral sensing is very promising to meet the ever-increasing demands for high-throughput chiral analysis in asymmetric synthesis. However, it is still very challenging to sensitively quantify the composition of enantiomers in a wide concentration range because the existing sensing systems show either linear CD response resultant from stoichiometric chiral transfer or nonlinear CD response resultant from amplified chiral transfer and thus have the drawbacks of low sensitivity and narrow quantification range, respectively. Herein, we propose a sensing system of two-dimensional (2D) Au(I)-thiolate nanosheets. The disordered interligand interactions on the confined surfaces of nanosheets enable the formation of discrete amplified chiral domains around the adsorbed chiral analytes, resulting in a linearly amplified chiral transfer behavior, which provides a solution for highly sensitive and wide-range quantification of enantiomer compositions. Taking (1R, 2R)-(−)- and (1S, 2S)-(+)-1,2-diamino cyclohexanes as example analytes, the concentration and full-range enantiomeric excess (ee) values have been quickly determined by adsorbing them on the surface of Au(I)-MPA (MPA: 3-mercaptopropionic acid) nanosheets in the concentration range of 1.0 × 10–6 to 4.0 × 10–5 M. By engineering the surface functional groups, Au(I)-thiolate nanosheets can be extended to sense other types of analytes, and several polyols with multiple chiral centers have been sensed by boronic acid functionalized nanosheets at the 10–7 M level. The high performances, good extendibility, and one-pot high-yield aqueous synthesis ensure these Au(I)-thiolate nanosheets can be developed as a practical and powerful chiral sensing platform.

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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2021 · IF 4.539

Highly sensitive determination of acetaminophen and 4-aminophenol based on COF/3D NCNF-T/Au NPs composite electrochemical sensing platform

Qixia Guan,Hao Guo,Ning Wu,Yujuan Cao,Mingyue Wang,Longwen Zhang,Wu Yang

As a new kind of porous organic material, covalent organic framework materials (COFs) have many advantages and have been widely used in catalysis, sensing, drug delivery, gas separation and other fields. In this paper, A COF was successfully prepared based on Schiff base reaction of 1, 3, 6, 8-tetrakis(4-formyl phenyl) pyrene (TFPPy) and 1, 3, 6, 8-tetrakis(4-amino phenyl) pyrene (PyTTA) named as TF-Py COF, and its structure was characterized in detail. By physically combining a pre-prepared three-dimensional carbon material containing nitrogen (3D NCNF-T) and TF-Py COF, followed by deposition of AuNPs, relatively poor conductivity of TF-Py COF was efficiently overcome and a novel electrochemical sensing platform with high sensitivity and high selectivity for simultaneous detection of acetaminophen (ACOP) and 4-aminophenol (4-AP) was successfully constructed. The synergistic effect between TF-Py COF, 3D NCNF-T and AuNPs effectively improves the analytical sensitivity of target analytes. Under optimized experimental conditions, the electrochemical sensing platform has a sensitive volt-ampere response and a wide linear range to both ACOP and 4-AP, and the detection limits are 0.13 μM and 0.05 μM (S/N = 3), respectively. The sensor has been successfully applied to the determination of ACOP and 4-AP in acetaminophen tablets and Yellow River water samples, with high recovery rate, good selectivity and reproducibility, and strong anti-interference ability. It is expected to be widely used in the actual sample detection.

CAS / MDL: 504-24-5
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