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SENSORS AND ACTUATORS B-CHEMICAL · 2024 · IF 8

Photoinduced defective MIL-100-NH2 as SERS substrate with charge-transfer resonances for direct, sensitive and simultaneous detection of small-molecule biothiols

Siqi Wei,Renjie Li,Ling Li,Dan Huang,Li Wu,Xiandeng Hou

The development of a rapid and accurate assay for the detection of biothiols is critical for early diagnosis and prevention of diseases. Herein, we report that the preparation of photoinduced defective MIL-100-NH 2 (PID-MIL-100-NH 2 ) with oxygen vacancy defects as a surface-enhanced Raman scattering (SERS) substrate by high-energy light irradiation. The substrate exhibited excellent SERS activity to Cys, Hcy and GSH with limits of detection (LODs) as low as 30, 23 and 18 nM, respectively, notably lowering the detectable concentration by at least 10 5 times compared to the Au NP substrate. Such superior SERS activity is attributed to the energy level matching of the PID-MIL-100-NH 2 substrate and the biothiol molecules, which results in efficient multiple charge-transfer resonances, such as photoinduced charge-transfer (PICT), ground-state charge-transfer (GSCT), and exciton resonances. Making good use of the rich fingerprint information, selective identification and simultaneous quantitation of biothiols in complex biological environment can be achieved. Trace biothiols in human serum samples have been successfully determined using this method. This work provides a feasible strategy to construct efficient charge-transfer resonances, enabling high-performance direct SERS sensing of biological small molecules.

研究领域: 分析化学 · 材料科学 · 生物医学工程 · 纳米技术
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ACS Applied Materials & Interfaces · 2021 · IF 9.229

Targeting Enrichment and Correlation Studies of Glutathione and Homocysteine in IgAVN Patient Urine Based on a Core–Shell Zr-Based Metal–Organic Framework

Xue Ma,Jinghua Zhang,Chong Zhang,Xiaoqing Yang,Ajuan Yu,Yanjie Huang,Shusheng Zhang,Gangfeng Ouyang

Aminothiols are closely related to chronic kidney disease, but little is known regarding levels of related aminothiols in the urine of immunoglobulin A vasculitis with nephritis (IgAVN) patients. Herein, a well-defined core–shell Zr-based metal–organic framework (Zr-MOF) composite SiO2@50Benz-Cys was constructed as a mercury ion affinity material via a solvent-assisted ligand exchange strategy for the selective extraction and enrichment of low-concentration aminothiols in IgAVN patient urine. SiO2@50Benz-Cys was competent to enrich the total glutathione (GSH) and total homocysteine (Hcy) in virtue of the excellent affinity after chelation with mercury ions. The extraction efficiencies were closely related to the pH, dithiothreitol amount, and the dose of functional Zr-MOF. Coupled with HPLC–MS/MS in optimized conditions, GSH and Hcy were determined with low detection limits of 0.5 and 1 nmol L–1, respectively. The recoveries of GSH and Hcy for the urine sample at three spiked levels were in the range of 85.3–105% and 79.5–103%, which showed good precision and accuracy. Benefiting from the matrix interference elimination in the process of extraction, the simultaneous detection of aminothiols in the urine of the healthy group and immunoglobulin A vasculitis (IgAV) and IgAVN patients was successfully carried out, suggesting that the Zr-MOF and the robust method together provided a potential application in the analysis of urinary biomolecules. The analysis of variance (ANOVA) showed that the levels of GSH and Hcy had significant differences between the patients and the control. This work is very valuable as it provides a better understanding of concentration alterations of GSH and Hcy in urine involved with IgAVN for clinical research.

研究领域: 分析化学 · 临床化学 · 肾病学 · 生物标志物分析
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY · 2024 · IF 5.7

A Clickase-Mediated Immunoassay Based on Nanopore and Bionic Signal Labels for Ultrasensitive, Portable, and On-Site Detection of Ricin

Jianing Chen,Zhuoqun Su,Wenrui Li,Ziye Pei,Di Wu,Lin Li,Yongning Wu,Guoliang Li

It is of particular importance to develop an effective method that possesses several merits simultaneously of rapid, ultrasensitive, portable, and on-site detection potential for food safety detection. Herein, we propose a clickase-mediated immunoassay based on nanopore and bionic signal labels for the detection of ricin. The introduction of Cu/Cys clickase and nanopore simultaneously effectively addressed the inherent limitations of natural enzymes and colorimetric signal output, respectively. Using this method, bionic signal labels can be easily formed through DNA and Gram-positive bacterial cell wall terminal peptide fragments (labeled by alkynyl and azide, respectively) and vancomycin. Translocation of the D-P@vancomycin through the nanopore generated highly specific oscillation current traces. This method showed a great on-site detection potential and superior analytical performance owing to the combination of the specificity of antibodies, high CuAAC click reaction catalytic efficiency of clickase, ultrasensitivity of the nanopore, and high signal resolution of D-P@vancomycin. Moreover, the practical applicability of the established method was also verified, achieving a limit of detection (LOD) down to 200.9 ag/mL with a wide linear relationship under the optimized conditions. In conclusion, this method is promising for rapid, portable, ultrasensitive, and on-site food safety detection.

研究领域: 分析化学 · 纳米技术 · 食品安全 · 生物传感器 · 免疫测定
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Journal of Materials Chemistry B · 2022 ·Vol. 10 ·期 22 ·4261-4273 · IF 7.571

Dual-responsive nano-prodrug micelles for MRI-guided tumor PDT and immune synergistic therapy

Hui Guo,Fangzhe Liu,Enqi Liu,Shanshan Wei,Wenbo Sun,Baoqiang Liu,Guoying Sun,Lehui Lu

Micelles as nanocarriers not only offer new opportunities for early diagnosis and treatment of malignant cancers but also encounter numerous barriers in the path of efficient delivery of drugs to diseased areas in the body. To address these issues, we developed a pH/GSH responsive nano-prodrug micelle (NLG919/PGA–Cys–PPA@Gd) with a high drug-loading ratio and controlled drug release performance for MRI-guided tumor photodynamic therapy (PDT) and immune synergistic therapy. Under normal conditions, theranostic nanomicelles remained stable and in a photo-quenched state. Upon accumulation in the tumor site, however, the micelles demonstrated tumor microenvironment (TME) triggered photoactive formed-PPA (a photosensitizer) and NLG919 (an indoleamine 2,3-dioxygenase (IDO) inhibitor) release because the amide bonds of PGA–Cys–PPA and the disulfide linkage of Cys were sensitive to pH and GSH, respectively. More importantly, these micelles could avoid the undesired PPA leakage in blood circulation due to the conjugation between PPA and polymers. Furthermore, the obtained micelles could also enhance the contrast of T1-weighted MRI of tumors by virtue of their high relaxivity (r1 = 29.85 mM−1 s−1). In vitro and in vivo results illustrated that the micelles had good biocompatibility and biosafety. On the basis of the efficient drug delivery strategies in PDT and IDO pathway inhibition, this intelligent dual-drug delivery system could serve as an effective approach for MRI guided combination therapy of cancer.

研究领域: 纳米技术 · 癌症治疗 · 磁共振成像(MRI) · 药物递送系统 · 光动力疗法 · 免疫疗法
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