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J Hazard Mater ; 405: 124642, 2020 Nov 21.
Artigo em Inglês | MEDLINE | ID: mdl-33301972


Total removal of organic mercury in industrial wastewater is a crucially important task facing environmental pollution in the current world. Herein, we demonstrate the fabrication of Au-NiFe layered double hydroxide (LDH)/rGO nanocomposite as not only an efficient nanozyme with oxidase-like activity but also an efficient surface-enhanced Raman spectroscopy (SERS) substrate to determine organic mercury, with the minimum detection concentration as low as 1 × 10-8 M. According to the binding energy of X-Ray photoelectron spectrometer (XPS) and the free radicals of electron paramagnetic resonance (EPR) spectra, the mechanism of catalytic enhanced degradation is the production of Au-amalgam on Au surface, accelerating the electron transfer and the generation of O2•- radicals from oxygen molecules and •CH3 radicals from the methyl group in MeHg to participate the oxidase-like reaction. Furthermore, the Au-NiFe LDH/rGO nanocomposite is able to degrade and remove 99.9% of organic mercury in two hours without the secondary pollution by Hg2+. In addition, the material can be used for the multiple degradation-regeneration cycles in actual applications, which is significant in terms of the environmental and economic point of view. This work may open a new horizon for both highly sensitive detection and thorough degradation of organic mercury in environmental science and technology.

Anal Chem ; 92(17): 11763-11770, 2020 09 01.
Artigo em Inglês | MEDLINE | ID: mdl-32697077


Surface-enhanced Raman scattering (SERS) is a supersensitive technique for monitoring catalytic reactions. However, building a SERS-kinetics model to investigate catalytic efficiency on the surface or interface of the catalyst remains a great challenge. In the present study, we successfully obtained an excellent semiconducting SERS substrate, reduced MnCo2O4 (R-MnCo2O4) nanotubes, whose favorable SERS sensitivity is mainly related to the promoted interfacial charge transfer caused by the introduction of oxygen vacancies as well as the electromagnetic enhancement effect. Furthermore, the R-MnCo2O4 nanotubes showed a favorable oxidase-like activity toward oxidation with the aid of molecular oxygen. It was also showed the oxidase-like catalytic process could be monitored using the SERS technique. A new SERS-kinetics model to monitor the catalytic efficiency of the oxidase-like reaction was developed, and the results demonstrate that the Vm values measured by the SERS-kinetics method are close to that obtained by the UV-vis approach, while the Km values measured by the SERS-kinetics method are much lower, demonstrating the better affinity between the enzyme and the substrate from SERS results and further confirming the high sensitivity of the SERS-kinetics approach and the actual enzyme-like reaction on the surface of nanozymes, which provides guidance in understanding the kinetics process and catalytic mechanism of natural enzymatic and other artificial enzymatic reactions. This work demonstrated the improved SERS sensitivity of defective semiconductors for the application of enzyme mimicking, providing a new frontier to construct highly sensitive biosensors.

Nanotechnology ; 31(31): 315501, 2020 Jul 31.
Artigo em Inglês | MEDLINE | ID: mdl-32303010


In-situ and real-time ultra-sensitive monitoring for the degradation process of environmental pollutants is always an important issue of concern to many people. Herein, a multifunctional magnetic metal-organic framework (MOF)-based composite has been successfully constructed and applied in monitoring the disposal of cationic dyes. Owing to its particular MOFs shell and internal gold particles, the composite can be used as an efficient SERS substrate to ultra-sensitively detect the cationic dyes. Furthermore, the prepared MOF-based composite is also a peroxidase-like nanozyme, which can catalytically degrade the adsorbed cationic dyes. Additionally, the magnetic core in the MOF-based composite offers a good magnetic separation capacity, which makes a facile and rapid separation of the catalyst from the reacted solution for recyclability. This work has provided a new way to monitor the catalytic degradation process by SERS technique in the co-existence of catalyst and dye molecules in the reaction system, which can effectively eliminate the absorption of the catalyst compared with the UV-vis technique, showing promising applications in in-situ and real-time pollution disposal monitoring.

Int Immunopharmacol ; 72: 437-444, 2019 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-31030100


BACKGROUND: Immune thrombocytopenia (ITP) is an immune-mediated acquired autoimmune hemorrhagic disease. About one-third of patients are unresponsive to first-line therapies. Thalidomide (THD) as an immunomodulatory agent is now used to treat several autoimmune disorders. Therefore, we assessed the safety and efficacy of THD in corticosteroid-resistant or relapsed ITP patients, and preliminarily explore its mechanism. METHODS: 50 newly-diagnosed ITP patients and 47 healthy volunteers were enrolled in this study. Additionally, 17 corticosteroid-resistant or relapsed ITP patients were recruited, with 7 cases in the rhTPO + THD group and 10 cases in the THD monotherapy group. Overall response rate at 6, 12, and 24 months were assessed. Levels of Neuropilin-1(NRP-1), regulatory T cells (Tregs) and regulatory B cells (Bregs) were detected. RESULTS: Expression of NRP-1, Tregs and Bregs were reduced in newly-diagnosed ITP patients. In vitro, THD treatment upregulated expression of NRP-1and Tregs only in ITP patients. As for corticosteroid-resistant or relapsed ITP patients, overall response rate at 6, 12, and 24 months was 85.7%, 57.1% and 100% in the rhTPO + THD group and 60%, 75% and 83.3% in the THD group, respectively. Additionally, rhTPO plus THD or THD therapy significantly increased the levels of NRP-1, Tregs and Bregs in responders. CONCLUSIONS: Our study shows for the first time that NRP-1 is involved in the pathogenesis of ITP, THD could induce response in ITP patients by upregulating NRP-1 expression and restoring the proportion of Tregs and Bregs. THD might be served as a novel therapeutic agent in corticosteroid-resistant or relapsed ITP patients.

Imunossupressores/uso terapêutico , Neuropilina-1/imunologia , Púrpura Trombocitopênica Idiopática/tratamento farmacológico , Talidomida/uso terapêutico , Adolescente , Corticosteroides/uso terapêutico , Adulto , Linfócitos B Reguladores/efeitos dos fármacos , Linfócitos B Reguladores/imunologia , Resistência a Medicamentos , Feminino , Humanos , Imunossupressores/farmacologia , Masculino , Pessoa de Meia-Idade , Neuropilina-1/genética , Púrpura Trombocitopênica Idiopática/genética , Púrpura Trombocitopênica Idiopática/imunologia , Linfócitos T Reguladores/efeitos dos fármacos , Linfócitos T Reguladores/imunologia , Talidomida/farmacologia , Regulação para Cima/efeitos dos fármacos , Adulto Jovem
ACS Appl Mater Interfaces ; 10(30): 25726-25736, 2018 Aug 01.
Artigo em Inglês | MEDLINE | ID: mdl-29987930


Fabrication of multifunctional nanocatalysts with surface-enhanced Raman scattering (SERS) activity is of vital importance for monitoring catalytic courses in situ and studying the reaction mechanisms. Herein, SERS-active magnetic metal-organic framework (MOF)-based nanocatalysts were successfully prepared via a three-step method, including a solvothermal reaction, an Au seed-induced growth process, and a low-temperature cycling self-assembly technique. The as-synthesized magnetic MOF-based nanocatalysts not only exhibit outstanding peroxidase-like activity, but can also be applied as a SERS substrate. Owing to these features, they can be used for monitoring in situ catalytic oxidation of 3,3',5,5'-tetramethylbenzidine (TMB) by H2O2 via a SERS technique, and the concentration of H2O2 was determined. Owing to the intrinsic character of the Fe-based MOF material (MIL-100(Fe)), a novel photoinduced enhanced catalytic oxidation effect was demonstrated, in which the catalytic oxidation of TMB and o-phenylenediamine was accelerated. This study provides a versatile approach for the fabrication of functional MOF-based nanocomposites as a promising SERS substrate with a unique photoinduced enhanced peroxidase-like activity for potential applications in ultrasensitive monitoring, biomedical treatment, and environmental evaluation.