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OBJECTIVES: To investigate the effect of the L-arginine metabolism on arthritis and inflammation-mediated bone loss. METHODS: L-arginine was applied to three arthritis models (collagen-induced arthritis, serum-induced arthritis and human TNF transgenic mice). Inflammation was assessed clinically and histologically, while bone changes were quantified by µCT and histomorphometry. In vitro, effects of L-arginine on osteoclast differentiation were analysed by RNA-seq and mass spectrometry (MS). Seahorse, Single Cell ENergetIc metabolism by profilIng Translation inHibition and transmission electron microscopy were used for detecting metabolic changes in osteoclasts. Moreover, arginine-associated metabolites were measured in the serum of rheumatoid arthritis (RA) and pre-RA patients. RESULTS: L-arginine inhibited arthritis and bone loss in all three models and directly blocked TNFα-induced murine and human osteoclastogenesis. RNA-seq and MS analyses indicated that L-arginine switched glycolysis to oxidative phosphorylation in inflammatory osteoclasts leading to increased ATP production, purine metabolism and elevated inosine and hypoxanthine levels. Adenosine deaminase inhibitors blocking inosine and hypoxanthine production abolished the inhibition of L-arginine on osteoclastogenesis in vitro and in vivo. Altered arginine levels were also found in RA and pre-RA patients. CONCLUSION: Our study demonstrated that L-arginine ameliorates arthritis and bone erosion through metabolic reprogramming and perturbation of purine metabolism in osteoclasts.
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Artrite Experimental , Artrite Reumatoide , Reabsorção Óssea , Humanos , Camundongos , Animais , Osteoclastos , Artrite Reumatoide/patologia , Artrite Experimental/patologia , Inflamação/metabolismo , Camundongos Transgênicos , Arginina/farmacologia , Inosina/metabolismo , Inosina/farmacologia , Hipoxantinas/metabolismo , Hipoxantinas/farmacologia , Purinas/farmacologiaRESUMO
Solar-energy-driven photoreduction of CO2 is promising in alleviating environment burden, but suffers from low efficiency and over-reliance on sacrificial agents. Herein, rhenium (Re) is atomically dispersed in In2O3 to fabricate a 2Re-In2O3 photocatalyst. In sacrificial-agent-free photoreduction of CO2 with H2O, 2Re-In2O3 shows a long-term stable efficiency which is enhanced by 3.5 times than that of pure In2O3 and is also higher than those on Au-In2O3, Ag-In2O3, Cu-In2O3, Ir-In2O3, Ru-In2O3, Rh-In2O3 and Pt-In2O3 photocatalysts. Moreover, carbon-based product of the photoreduction overturns from CO on pure In2O3 to CH3OH on 2Re-In2O3. Re promotes charge separation, H2O dissociation and CO2 activation, thus enhancing photoreduction efficiency of CO2 on 2Re-In2O3. During the photoreduction, CO is a key intermediate. CO prefers to desorption rather than hydrogenation on pure In2O3, as CO binds to pure In2O3 very weakly. Re strengthens the interaction of CO with 2Re-In2O3 by 5.0 times, thus limiting CO desorption but enhancing CO hydrogenation to CH3OH. This could be the origin for photoreduction product overturn from CO on pure In2O3 to CH3OH on 2Re-In2O3. The present work opens a new way to boost sacrificial-agent-free photoreduction of CO2.
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Unstable Zn interface with serious detrimental parasitic side-reactions and uncontrollable Zn dendrites severely plagues the practical application of aqueous zinc-ion batteries. The interface stability was closely related to the electrolyte configuration and Zn2+ depositional behavior. In this work, a unique Zn-ion anchoring strategy is originally proposed to manipulate the coordination structure of solvated Zn-ions and guide the Zn-ion depositional behavior. Specifically, the amphoteric charged ion additives (denoted as DM), which act as zinc-ion anchors, can tightly absorb on the Zn surface to guide the uniform zinc-ion distribution by using its positively charged -NR4 + groups. While the negatively charged -SO3 - groups of DM on the other hand, reduces the active water molecules within solvation sheaths of Zn-ions. Benefiting from the special synergistic effect, Zn metal exhibits highly ordered and compact (002) Zn deposition and negligible side-reactions. As a result, the advanced Zn||Zn symmetric cell delivers extraordinarily 7000â hours long lifespan (0.25â mA cm-2, 0.25â mAh cm-2). Additionally, based on this strategy, the NH4V4O10||Zn pouch-cell with low negative/positive capacity ratio (N/P ratio=2.98) maintains 80.4 % capacity retention for 180â cycles. A more practical 4â cm*4â cm sized pouch-cell could be steadily cycled in a high output capacity of 37.0â mAh over 50â cycles.
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Photocatalytic overall splitting of pure water (H2O) without sacrificial reagent to hydrogen (H2) and oxygen (O2) holds a great potential for achieving carbon neutrality. Herein, by anchoring cobalt sulfide (Co9S8) as cocatalyst and cadmium sulfide (CdS) as light absorber to channel wall of a porous polymer microreactor (PP12), continuous violent H2 and O2 bubbling productions from photocatalytic overall splitting of pure H2O without sacrificial reagent is achieved, with H2 and O2 production rates as high as 4.41 and 2.20 mmol h-1 gcat.-1 respectively. These are significantly enhanced than those in the widely used stirred tank-type reactor in which no O2 is produced and H2 production rate is only 0.004 mmol h-1 gcat.-1. Besides improved charge separation and interaction of H2O with photocatalyst in PP12, bonding interaction of Co9S8 with PP12 creates abundant catalytic active sites for simultaneous productions of H2 and O2, thus leading to the significantly enhanced H2 and O2 bubbling productions in PP12. This offers a new strategy to enhance photocatalytic overall splitting of pure H2O without sacrificial reagent.
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Lithium-metal shows promising prospects in constructing various high-energy-density lithium-metal batteries (LMBs) while long-lasting tricky issues including the uncontrolled dendritic lithium growth and infinite lithium volume expansion seriously impede the application of LMBs. In this work, it is originally found that a unique lithiophilic magnetic host matrix (Co3 O4 -CCNFs) can simultaneously eliminate the uncontrolled dendritic lithium growth and huge lithium volume expansion that commonly occur in typical LMBs. The magnetic Co3 O4 nanocrystals which inherently embed on the host matrix act as nucleation sites and can also induce micromagnetic field and facilitate a targeted and ordered lithium deposition behavior thus, eliminating the formation of dendritic Li. Meanwhile, the conductive host can effectively homogenize the current distribution and Li-ion flux, thus, further relieving the volume expansion during cycling. Benefiting from this, the featured electrodes demonstrate ultra-high coulombic efficiency of 99.1% under 1 mA cm-2 and 1 mAh cm-2 . Symmetric cell under limited Li (10 mAh cm-2 ) inspiringly delivers ultralong cycle life of 1600 h (under 2 mA cm-2 , 1 mAh cm-2 ). Moreover, LiFePO4 ||Co3 O4 -CCNFs@Li full-cell under practical condition of limited negative/positive capacity ratio (2.3:1) can deliver remarkably improved cycling stability (with 86.6% capacity retention over 440 cycles).
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Water-induced parasitic reactions and uncontrolled dendritic Zn growth are long-lasting tricky problems that severely hinder the development of aqueous zinc-metal batteries. Those notorious issues are closely related to electrolyte configuration and zinc-ion transport behavior. Herein, through constructing aligned dipoles induced electric-field on Zn surface, both the solvation structure and transport behavior of zinc-ions are fundamentally changed. The vertically ordered zinc-ion migration trajectory and gradually concentrated zinc-ion achieved inside the polarized electric-field remarkably eliminate water related side-reactions and Zn dendrites. Zn-metal under the polarized electric-field demonstrated significantly improve reversibility and a dendrite-free surface with strong (002) Zn deposition texturing. Zn||Zn symmetric cell delivers greatly prolonged lifespan up to 1400 h (17 times longer than that of the cell based on bare Zn) while the Zn||Cu half-cell demonstrate ultrahigh 99.9% coulombic efficiency. NH4 V4 O10 ||Zn half-cell delivered exceptional-high 132 mAh g-1 capacity after ultralong 2000 cycles (≈100% capacity retention). In addition, MnO2 ||Zn pouch-cell under aligned dipoles induced electric-field maintains 87.9% capacity retention after 150 cycles under practical condition of high MnO2 mass loading (≈10 mg cm-2 ) and limited N/P ratio. It is considered that this new strategy can also be implemented to other metallic batteries and spur the development of batteries with long-lifespan and high-energy-density.
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OBJECTIVES: This study aimed to analyse the immune cell profiles of adult-onset Still's disease (AOSD) and to stratify disease-associated endotypes. METHODS: We included 95 cases of treatment-naïve patients with AOSD and 66 cases of healthy controls. Patients with AOSD were classified via an unbiased hierarchical cluster analysis based on circulating immune cells. Their clinical and laboratory characteristics, treatment management, systemic scores and outcomes were then analysed. RESULTS: The proportions of neutrophils and CD8+ T cells were significantly higher while monocytes and natural killer and CD4+ T cells were decreased in patients with AOSD (all P < 0.005). Unbiased hierarchical cluster analysis classified 95 AOSD into three endotype-based groups: group 1 had the highest percentage of neutrophils (neu-dominant group), group 2 had the highest percentage of monocytes (mono-dominant group) and group 3 had the highest percentage of CD8+ T cells (CD8-dominant group). Patients in group 3 had the highest systemic score at diagnosis and were more likely to have pulmonary infiltrates, pericarditis, splenomegaly and poorer treatment responses. A correlation study revealed that the CD4 to CD8 ratio was negatively correlated with the systemic score and positively correlated with treatment response in patients with AOSD (P = 0.001 and P = 0.0091). During the 24.6 (15.2) months of follow-up, the highest total number of disease flares occurred in group 3 (P < 0.0001). CONCLUSION: Hierarchical cluster analysis of peripheral immune cells classified AOSD into three disease-related endotypes. Group 3 showed higher systemic score and poorer treatment responses.
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Doença de Still de Início Tardio , Adulto , Humanos , Doença de Still de Início Tardio/tratamento farmacológico , Biomarcadores , Linfócitos T CD8-Positivos , Monócitos , Análise por ConglomeradosRESUMO
In this study, based on the comparison of two counterparts [Mn- and Cr-modified CeO2 nanobelts (NBs)] with the opposite effects, some novel mechanistic insights into the ethyl acetate (EA) catalytic combustion over CeO2-based catalysts were proposed. The results demonstrated that EA catalytic combustion consisted of three primary processes: EA hydrolysis (C-O bond breakage), the oxidation of intermediate products, and the removal of surface acetates/alcoholates. Rapid EA hydrolysis typically occurs on surface acid/base sites or hydroxyl groups, and the removal of surface acetates/alcoholates resulting from EA hydrolysis is considered the rate-determining step. The deposited acetates/alcoholates like a shield covered the active sites (such as surface oxygen vacancies), and the enhanced mobility of the surface lattice oxygen as an oxidizing agent played a vital role in breaking through the shield and promoting the further hydrolysis-oxidation process. The Cr modification impeded the release of surface-activated lattice oxygen from the CeO2 NBs and induced the accumulation of acetates/alcoholates at a higher temperature due to the increased surface acidity/basicity. Conversely, the Mn-substituted CeO2 NBs with the higher lattice oxygen mobility effectively accelerated the in situ decomposition of acetates/alcoholates and facilitated the re-exposure of surface active sites. This study may contribute to a further mechanistic understanding into the catalytic oxidation of esters or other oxygenated volatile organic compounds over CeO2-based catalysts.
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Acetatos , Oxigênio , Hidrólise , Oxirredução , Acetatos/químicaRESUMO
BACKGROUND: Older adults are a growing segment of oncology population in China and beyong. However, older cancer patients were vastly underrepresented in clinical trial. To facilitate that all patients with cancer have equal access to the cutting edging treatment and receive evidence-based medication in mainland China, it's of particular importance to fully grasp the proportion of upper age restriction in cancer clinical trials, as well as associated factors. METHODS: Based on clinical trials registered on the China Food and Drug Administration Registration and Information Disclosure Platform, we sought to characterize the overall proportion and trajectory of upper age-restriction among registered cancer drug trials in mainland China from 2009 to 2021, and potential influencing factors were determined by multivariate logistic regression. RESULTS: According to the 3485 trials, upper age restriction proportion of cancer drug trials for patients over 65 years and 75 years was 18.8% (95% CI = 17.5%-20.1%) and 56.5% (95% CI = 51.3%-54.6%), respectively. Phase IV trials, international multicenter trials, or trials initiated by global companies seldom excluded patients over 65 years compared with phase I trials, domestic trials and trials initiated by Chinese enterprise, similar for 75 years and above. Both of 65 and 75 years old age limit sponsored by domestic enterprises showed slowly downward trend, while no such trend was observed for that of foreign companies. Solution to upper age eligibility of cancer drug trials was also provided. CONCLUSIONS: Although there is a certain downward trend, use of eligibility criteria that explicitly exclude older cancer patients in mainland China was remarkably high, especially for trials initiated by domestic enterprise, domestic trials and early-phase trials. Action is urgently needed to promote treatment equity in the older patients while obtaining adequate evidence in clinical trials.
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Antineoplásicos , Ensaios Clínicos como Assunto , Neoplasias , Seleção de Pacientes , Idoso , Humanos , Antineoplásicos/uso terapêutico , China/epidemiologia , Neoplasias/tratamento farmacológico , Neoplasias/epidemiologiaRESUMO
Mobile ad hoc networks (MANETs) are self-configuring networks of wireless nodes, i.e., mobile devices. Since communications in MANETs occur via wireless channels, it is of significance to secure communications among wireless and mobile nodes. Group key management, as a widely used method for securing group communications, has potentially been used in MANETs for years. Most recently, a secure receiver-unrestricted group key management scheme for MANETs has been proposed, which is used to establish a secure channel among a group of wireless nodes without a trusted dealer, which has some advantages such as eliminating the certificate management problem and receiver restriction. However, a formal security analysis of this scheme is still lacking. Therefore, in this paper, we propose the complete security proof to demonstrate that the scheme satisfies the essential security properties including authentication, message confidentiality, known-key security and dynamic secrecy. We also give a brief discussion about the efficiency of the scheme.
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By supporting platinum (Pt) and cadmium sulfide (CdS) nanoparticles on indium oxide (In2 O3 ), we fabricated a CdS/Pt/In2 O3 photocatalyst. Selective photoreduction of carbon dioxide (CO2 ) to methane (CH4 ) was achieved on CdS/Pt/In2 O3 with electronic Pt-In2 O3 interactions, with CH4 selectivity reaching to 100 %, which is higher than that on CdS/Pt/In2 O3 without electronic Pt-In2 O3 interactions (71.7 %). Moreover, the enhancement effect of electronic Pt-(metal-oxide) interactions on selective photoreduction of CO2 to CH4 also occurs by using other common metal oxides, such as photocatalyst supports, including titanium oxide, gallium oxide, zinc oxide, and tungsten oxide. The electronic Pt-(metal-oxide) interactions separate photogenerated electron-hole pairs and convert CO2 into CO2 δ- , which can be easily hydrogenated into CH4 via a CO2 δ- âHCOO*âHCO*âCH*âCH4 path, thus boosting selective photoreduction of CO2 to CH4 . This offers a new way to achieve selective photoreduction of CO2 .
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Photocatalytic hydrogen (H2 ) production is significant to overcome challenges like fossil fuel depletion and carbon dioxide emission, but its efficiency is still far below that which is needed for commercialization. Herein, we achieve long-term stable H2 bubbling production from water (H2 O) and lactic acid via visible-light-driven photocatalysis in a porous microreactor (PP12); the catalytic system benefits from photocatalyst dispersion, charge separation, mass transfer, and dissociation of O-H bonds associated with H2 O. With the widely used platinum/cadmium-sulfide (Pt/CdS) photocatalyst, PP12 leads to a H2 bubbling production rate of 602.5â mmol h-1 m-2 , which is 1000â times higher than that in a traditional reactor. Even when amplifying PP12 into a flat-plate reactor with an area as large as 1â m2 and extending the reaction time to 100â h, the H2 bubbling production rate still remains at around 600.0â mmol h-1 m-2 , offering great potential for commercialization.
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The aim of this Policy Review was to compare China's overall and synchronous participation in clinical trials for innovative anticancer drugs with that of the USA, the EU, Japan, and South Korea, and to assess changes in the participation rate trends in these five regions. Relevant data from the top 20 international pharmaceutical companies from 2011 to 2021 were systematically collected from the Trialtrove and Pharmaprojects databases. Among the 8260 trials for 954 new anticancer drugs identified, China was involved in 8·8% of the trials and with 20·4% of the drugs being trialled. These participation rates are significantly lower than those for South Korea (14·5% of trials and 36·3% of drugs), Japan (16·1% of trials and 38·7% of drugs), the EU (40·6% of trials and 67·7% of drugs), and the USA (65·7% of trials and 91·2% of drugs; p<0·0001 for all). Similar results were found for the synchronous participation rate, defined as the proportion of drugs or trials at the highest development stage internationally, for the 803 tested drugs, which ranged from 9·0% in China to 87·7% in the USA. China's participation rate in early phase trials (4·4%) and in synchronous trials (5·4%) was even lower, in stark contrast to that of the USA (66·1% for early phase trials and 89·1% for synchronous trials). The fastest growing annual rate of participation in trials was observed in China (15·7%), followed by South Korea (8·2%) and Japan (6·8%); no change was detected in the USA or the EU. This Policy Review shows that Chinese participation in the clinical development of innovative cancer drugs by international pharmaceutical companies has increased over the past decade, but an obvious gap persists in comparison with the USA, the EU, Japan, and South Korea, especially in its synchronous participation and early participation rates.
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Antineoplásicos , Humanos , Antineoplásicos/uso terapêutico , China , Japão , República da Coreia/epidemiologia , Indústria FarmacêuticaRESUMO
The frequent occurrence of single-phase grounding faults affects the reliable operation of power systems. When a single-phase grounding fault occurs, it is difficult to accurately identify the fault type because of the weak characterization and subtle distinction between different fault types. Therefore, this paper proposes a single-phase grounding fault type identification method based on the multi-feature transformation and fusion. Firstly, the Hilbert-Huang transform (HHT) was used to preprocess the fault recorded wave data to highlight the characteristics between different fault types. Secondly, the deep learning model ResNet18 and the long short-term memory (LSTM) are designed to extract the complex abstract features and time-series correlation features from the preprocessed data set separately. Finally, it designs a fusion model to combine the advantages of heterogeneous models to identify the type of single-phase grounding fault. Experiments validate that the method is good at fully mining the characteristics of the fault types contained in the fault recorded wave data, so it can identify multiple types of faults with strong robustness and provide a reliable basis for the subsequent formulation of targeted fault-handling measures.
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BACKGROUND: Unsaturated fatty acids used to form unstable micro-vesicles, while conjugate linoleic acid (CLA)-sodium dodecyl sulfate (SDS) can self-assembly to stable nano-conjugate linoleic acid vesicles (nano-CLAVs). Generally, micro-capsule could geometrically provide higher loading capacity but also generate concerns in construction convenience, sustained release, bioaccessibility and stability. Hence there is a contradiction between loading capacity and encapsulation efficiency. Therefore, the study of the factors that decide the capsule size falling in nano or micron size with same capsule material would be a benefit to food or drug delivery science. RESULTS: The micron- and nano-CLAVs were constructed for encapsulation and sustained release of ginsenoside Rg3. The formation mechanism of nano or micron capsule,s the effect of vesicle sizes on encapsulation efficiency, drug loading efficiency and stability of the encapsulated Rg3 were investigated. It was found that with the addition of salt (PBS), the size of CLAVs jumped from nano to micron. Furthermore, the salt concentration is the key factor that decides the vesicle size of nano or micron. The pH at fabrication triggers the vesiculation and dramatically affects the vesicle size over the nano and micron scales. CONCLUSION: Compared to the nano-CLAVs, micron vesicles enhanced the loading capacity to 137.6% and the encapsulation efficiency to 138.4%, respectively. Meanwhile, the micron-CLAVs performed similar sustained release of Rg3 as the nano-CLAVs did, and was stable for 120 days at room temperature or sustained 98.9% of capsules after centrifuge at 6090 × g for 20 min. © 2022 Society of Chemical Industry.
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Ginsenosídeos , Ácidos Linoleicos Conjugados , Preparações de Ação Retardada , Sistemas de Liberação de MedicamentosRESUMO
Introduction: Psoriasis is an immune-mediated systemic disease. Neutrophils are enriched in psoriasis lesions and can form neutrophil extracellular traps (NETs) to activate keratinocytes. Receptor-interacting protein kinase RIPK1 and RIPK3 are involved in necroptosis and NET formation. Aim: To elucidate whether RIPK1 regulates circulating neutrophils to form NETs and inflammation in psoriasis. Material and methods: Blood samples of psoriasis patients (n = 20) and healthy controls (n = 20) were detected by flow cytometry. The expression level of RIPK1/3 in isolated circulating neutrophils from psoriasis patients (n = 17) and healthy controls (n = 17) was examined by quantitative real-time PCR. SYTOX Green dye and PicoGreen reagent were used to detect NET formation and DNA release in neutrophils under the stimulation of phorbol 12-myristate 13-acetate (PMA) and necrostain-1 (Nec-1). Correlation analysis was performed between RIPK1/3 expression and Psoriasis Area Severity Index (PASI), neutrophil-to-lymphocyte ratio (NLR). Results: RIPK1 and RIPK3 expression in protein levels were decreased in monocytes and neutrophils from peripheral blood of psoriasis patients. In isolated psoriasis neutrophils, RIPK1 and Caspase8 mRNA were downregulated while RIPK3 and MLKL mRNA were elevated, leading to the necroptosis pathway. In addition, RIPK1-inhitor-necrostatin-1 (Nec-1) enhanced NETosis in psoriasis neutrophils in vitro. More importantly, there is a negative correlation between RIPK1 and psoriasis disease severity. Conclusions: Our data demonstrated that downregulated RIPK1 expression in psoriasis neutrophils may enhance NET generation. RIPK1 may be identified as a novel therapeutic target in psoriasis.
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Searching for novel anode materials to address the issues of poor cycle stability in the aqueous lithium-ion battery system is highly desirable. In this work, ammonium vanadium bronze (NH4 )2 V7 O16 with brick-like morphology has been investigated as an anode material for aqueous lithium-ion batteries and Li+ /Na+ hybrid ion batteries. The two novel full cell systems (NH4 )2 V7 O16 ||Li2 SO4 ||LiMn2 O4 and (NH4 )2 V7 O16 ||Na2 SO4 ||LiMn2 O4 both demonstrate good rate capability and excellent cycling performance. A capacity retention of 78.61 % after 500 cycles at 300â mA g-1 was demonstrated in the (NH4 )2 V7 O16 ||Li2 SO4 ||LiMn2 O4 system, whereas no capacity attenuation is observed in the (NH4 )2 V7 O16 ||Na2 SO4 ||LiMn2 O4 system. The reaction mechanisms of the (NH4 )2 V7 O16 electrode and impedance variation of the two full cells were also researched. The excellent cycling stability suggests that layered (NH4 )2 V7 O16 can be a promising anode material for aqueous rechargeable lithium-ion batteries.
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PURPOSE: Different non-pharmacological interventions have been considered and applied to patients with colorectal cancer to improve their quality of life and distress symptoms; however, there is little evidence comparing the effectiveness of these strategies. This review aimed at assessing the effect of non-pharmacological interventions on quality of life, anxiety, and depression scores among patients with colorectal cancer. METHODS: A systematic search for articles published until August 1, 2020, in the English language was performed in Medline, EMBASE, Web of Science, and the Cochrane Library; the reference lists of eligible articles were scanned for other potentially eligible publications. A meta-analysis was performed using random-effects models to estimate pooled effect sizes. RESULTS: Twenty studies were included, representing a total of 3438 patients with colorectal cancer. Non-pharmacological interventions were associated with a significant reduction in anxiety (standardized mean difference [SMD] = - 0.157; 95% confidence interval [CI], - 0.312-[- 0.002]) and depression (SMD = - 0.207; 95% CI, - 0.390-[- 0.024]) scores during 5-8 months of follow-up. Subgroup analyses revealed that interventions delivered face-to-face improved patients' quality of life during 1-4 months of follow-up. Moreover, interventions delivered face-to-face but without a behavioral component were associated with improved anxiety scores, whereas interventions with a behavioral component improved the depression scores during 5-8 months of follow-up. CONCLUSIONS: Non-pharmacological interventions were associated with reduced anxiety and depression scores, whereas interventions delivered face-to-face were associated with improved quality of life scores in patients with colorectal cancer. Given the few studies and patients included in this meta-analysis, these conclusions should be interpreted with caution.
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Neoplasias Colorretais , Qualidade de Vida , Ansiedade/etiologia , Ansiedade/terapia , Neoplasias Colorretais/terapia , Depressão/etiologia , Depressão/terapia , Humanos , Ensaios Clínicos Controlados Aleatórios como AssuntoRESUMO
Herein, we present a dual-amplification sensing strategy-based surface-enhanced Raman scattering (SERS) chip, which combines rolling circle amplification (RCA) and polyadenine (PolyA) assembly for sensitive and reproducible determination of the activity of M.SssI, a cytosine-guanine dinucleotide (CpG) methyltransferase (MTase). Typically, in the presence of M.SssI, RCA process is triggered, resulting in long, single-stranded DNA (ssDNA) fragments that are hybridized with thousands of Raman reporters of Cy3. Afterward, the resultant ssDNA fragments are conjugated to SERS-active substrates made of silver core-gold satellite nanocomposites-modified silicon wafer (Ag-Au NPs@Si), with the SERS enhancement factor of â¼5 × 106. The core-satellite nanostructures are assembled relied on the strong affinity of PolyA toward gold/silver surface. Of particular significance, the developed SERS chip displays an ultrahigh sensitivity with a low limit of detection (LOD) of 2.8 × 10-3 U/mL, which is around 2 orders of magnitude higher than most reported methods. In addition, the constructed chip features a broad detection range covering from 0.05 to 50 U/mL. Besides for the ultrahigh sensitivity and broad dynamic range, the chip also features good reproducibility (e.g., the relative standard deviation (RSD) is less than â¼12%). Taking advantages of these merits, the developed chip is feasible for accurate discrimination of M.SssI with various concentrations spiked in human serum samples with good recoveries ranging from 99.6% to 107%.
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DNA-Citosina Metilases/sangue , Análise Espectral Raman/métodos , Carbocianinas , Fragmentação do DNA , DNA de Cadeia Simples , Ouro , Humanos , Limite de Detecção , Nanopartículas Metálicas/química , Poli A/metabolismo , Reprodutibilidade dos Testes , Prata , Análise Espectral Raman/normasRESUMO
The fouling and stability are two most critical limiting factors for practical applications of surface-enhanced Raman scattering (SERS)-based microfluidic electrophoresis device. Herein, we present a novel biomimetic nanoengineering strategy to achieve a SERS substrate featuring antifouling ability, good stability, and reliable quantitative capability. Typically, by employing tea polyphenol as the reducing agent, the substrate made of silver core-gold shell nanostructures in situ grown on silicon wafer surface is fabricated. The core-shell nanostructures are further embedded with internal standard molecules. Remarkably, the fabricated substrate preserves distinct SERS effects, adaptable reproducibility, and reliable quantitative ability even if the substrate is incubated with 15% H2 O2 , 13% HNO3 , or 108 CFU/mL bacteria, or suffered from 12-day continuous vibration at 250 rpm/min in PBS buffer. As a proof-of-concept application, the DNA-functionalized substrate is capable of precise quantification of Hg2+ with a limit of detection down to ca. 1 pM even in sewage water.