The organic photoelectrochemical transistor (OPECT) has been proven to be a promising platform to study the rich light-matter-bio interplay toward advanced biomolecular detection, yet current OPECT ...is highly restrained to its intrinsic electronic amplification. Herein, this work first combines chemical amplification with electronic amplification in OPECT for dual-amplified bioanalytics with high current gain, which is exemplified by human immunoglobulin G (HIgG)-dependent sandwich immunorecognition and subsequent alkaline phosphatase (ALP)-mediated chemical redox cycling (CRC) on a metal-organic framework (MOF)-derived BiVO
/WO
gate. The target-dependent redox cycling of ascorbic acid (AA) acting as an effective electron donor could lead to an amplified modulation against the polymer channel, as indicated by the channel current. The as-developed bioanalysis could achieve sensitive HIgG detection with a good analytical performance. This work features the dual chemical and electronic amplification for OPECT bioanalysis and is expected to stimulate further interest in the design of CRC-assisted OPECT bioassays.
Sensitive photoelectrochemical (PEC) bioanalysis usually relies on enzyme-assisted signal amplification. This work describes the first proof-of-concept study for liposome-based PEC bioanalysis. ...Specifically, unilamellar liposomes were prepared and then utilized to carry the enediol-ligands and antibodies within their internal cavities and upon their external surfaces, respectively. On the other hand, the 96-well plate was used for accommodating the sandwich immunocomplexing, and then the confined liposomes were directed to release the encapsulated enediol-ligands into an individual well. The subsequent in situ sensitization of the TiO2 nanoparticles (NPs) electrode was then used to transduce the recognition events. This facile strategy allows for sensitive immunoassay without the involvement of laborious electrode fabrication and enzymatic amplification. Importantly, the protocol can be extended as a general PEC method for numerous other targets of interest. We believe this work could offer a new perspective for the rational implementation of various liposome complexes for novel PEC bioanalysis.
Purpose
We aimed to evaluate the impact of preoperative local symptoms on prognosis after radical nephroureterectomy in patients with upper tract urothelial carcinoma (UTUC).
Methods
This ...retrospective study consisted of 2,662 UTUC patients treated at 15 institutions in Taiwan from 1988 to 2019. Clinicopathological data were retrospectively collected for analysis by the Taiwan UTUC Collaboration Group. The Kaplan-Meier method was used to calculate overall survival (OS), cancer-specific survival (CSS), disease-free survival (DFS), and bladder recurrence-free survival (BRFS). The prognostic value of preoperative local symptoms in OS, CSS, DFS, and BRFS was investigated using Cox proportional hazards models.
Results
The median follow-up was 36.6 months. Among 2,662 patients, 2,130 (80.0%) presented with hematuria and 398 (15.0%) had symptomatic hydronephrosis at diagnosis. Hematuria was associated with less symptomatic hydronephrosis (
p <
0.001), more dialysis status (
p
= 0.027), renal pelvic tumors (
p <
0.001), and early pathological tumor stage (
p
= 0.001). Symptomatic hydronephrosis was associated with female patients (
p <
0.001), less dialysis status (
p
= 0.001), less bladder cancer history (
p <
0.001), ureteral tumors (
p <
0.001), open surgery (
p
= 0.006), advanced pathological tumor stage (
p <
0.001), and postoperative chemotherapy (
p
= 0.029). Kaplan-Meier analysis showed that patients with hematuria or without symptomatic hydronephrosis had significantly higher rates of OS, CSS, and DFS (all
p <
0.001). Multivariate analysis confirmed that presence of hematuria was independently associated with better OS (HR 0.789, 95% CI 0.661–0.942) and CSS (HR 0.772, 95% CI 0.607–0.980), while symptomatic hydronephrosis was a significant prognostic factor for poorer OS (HR 1.387, 95% CI 1.142–1.683), CSS (HR 1.587, 95% CI 1.229–2.050), and DFS (HR 1.378, 95% CI 1.122–1.693).
Conclusions
Preoperative local symptoms were significantly associated with oncological outcomes, whereas symptomatic hydronephrosis and hematuria had opposite prognostic effects. Preoperative symptoms may provide additional information on risk stratification and perioperative treatment selection for patients with UTUC.
Developing nanoscale ratiometric techniques capable of biochemical response should prove of significance for precise applications with stringent spatial and biological restrictions. Here we present ...and devise the concept of θ-nanopore ratiometry, which uses ratiometric signals that could well address the serious concerns about device deviation in fabrication and nonspecific adsorption in the detection. As exemplified by a 200 nm θ-nanopore toward miRNA detection, the ±20 nm aperture drift could be mitigated and the issue of nonspecific adsorption could be minimized in the complex cytosolic environment. Practical application of this θ-nanopore ratiometry realizes the measurements of cytosolic miRNA-10b. This work has not only established a nanoscopic ratiometric technique but also enriched the extant armory of nanotools for single-cell studies and beyond.
This work reported the photoelectrochemical (PEC) pH sensor for sensitive and broad-range pH measurement on the basis of semiconducting polymer dots (Pdots). The sensor was fabricated by immobilizing ...Pdots onto the surface of indium tin oxide (ITO). Experimental results revealed that the carboxylic acid groups of Pdots were sensitive to pH variation, which could result in conformational changes and further diffusion of carriers. Besides, different pH value could change the redox properties of the Pdots, and the photocurrent response was hence altered by the carriers produced on the Pdots. Further results demonstrated that the developed sensor exhibited variable photocurrent sensitively by responding to different pH values. This pH sensor is of high sensitivity, stability, and reversibility, which provides a bright prospect for future pH measurements in the bioanalytical field.
Abstract Constructing versatile metal nanoclusters (NCs) assemblies through noncovalent weak interactions between inter‐ligands is a long‐standing challenge in interfacial chemistry, while compelling ...interfacial hydrogen‐bond‐driven metal NCs assemblies remain unexplored so far. Here, the study reports an amination‐ligand o ‐phenylenediamine‐coordinated copper NCs (CuNCs), demonstrating the impact of interfacial hydrogen‐bonds (IHBs) motifs on the luminescent behaviors of metal NCs as the alteration of protic solvent. Experimental results supported by theoretical calculation unveil that the flexibility of interfacial ligand and the distance of cuprophilic Cu I ···Cu I interaction between intra‐/inter‐NCs can be tailored by manipulating the cooperation between the diverse IHBs motifs reconstruction, therewith the IHBs‐modulated fundamental structure‐property relationships are established. Importantly, by utilizing the IHBs‐mediated optical polychromatism of aminated CuNCs, portable visualization of humidity sensing test‐strips with fast response is successfully manufactured. This work not only provides further insights into exploring the interfacial chemistry of NCs based on inter‐ligands hydrogen‐bond interactions, but also offers a new opportunity to expand the practical application for optical sensing of metal NCs.
Literature regarding the impacts of heavy metal exposure on erectile dysfunction (ED) is scarce. We aimed to evaluate the correlation between 10 urinary metals and ED in a large, nationally ...representative adult male sample. The dataset was extracted from the National Health and Nutrition Examination Survey (NHANES) during the period of 2001-2002 and 2003-2004. Weighted proportions and multivariable logistic regression analysis adjusted for confounding variables were utilized to determine the relationship between metal exposure and ED. Weighted quantile sum (WQS) regression was utilized to evaluate the impact of a mixture of urinary metals on ED. A total of 1328 participants were included in our study. In multivariable logistic regression analysis, cobalt (Co) and antimony (Sb) were positively associated with ED (odds ratio OR: 1.36, 95% confidence interval CI: 1.10-1.73, P = 0.020; and OR: 1.41, 95% CI: 1.12-1.77, P = 0.018, respectively) after full adjustment. Men in tertile 4 for Co (OR: 1.49, 95% CI: 1.02-2.41, P for trend = 0.012) and Sb (OR: 1.53, 95% CI: 1.08-2.40, P for trend = 0.041) had significantly higher odds of ED than those in tertile 1. Furthermore, the WQS index was significantly linked with increased odds of ED after full adjustment (OR: 1.31, 95% CI: 1.04-1.72, P < 0.05). Our study expanded on previous literature indicating the possible role of heavy metal exposure in the etiology of ED. The evaluation of heavy metal exposure should be included in the risk assessment of ED.
Confined and free diffusion of phenol occur in the electric double layer (EDL) and extra‐EDL region in the nanochannels of porous anodic alumina (see picture). The inductive effect of the EDL ...electric field on the phenol molecules slows their diffusion, but it is negligible in the free‐diffusion region. The extent of the two regions depends on EDL thickness, and hence the diffusion flux increases with increasing ionic strength of the electrolyte.
Ninety-three women with urodynamic stress incontinence (USI) and a mean age of 60.8 ± 10.7 (36-83) years were retrospectively enrolled. According to their VUDS, 31 (33%) were grouped into USI and ...detrusor overactivity (DO), 28 (30.1%) were grouped into USI and hypersensitive bladder (HSB), and 34 (36.6%) were controls (USI and stable bladder). The USI and DO group had significantly increased 8-isoprostane (mean, 33.3 vs. 10.8 pg/mL) and 8-hydroxy-2-deoxyguanosine (8-OHdG; mean, 28.9 vs. 17.4 ng/mL) and decreased interleukin (IL)-2 (mean, 0.433 vs. 0.638 pg/mL), vascular endothelial growth factor (mean, 5.51 vs. 8.99 pg/mL), and nerve growth factor (mean, 0.175 vs. 0.235 pg/mL) levels compared to controls. Oxidative stress biomarkers were moderately diagnostic of DO from controls, especially 8-isoprostane (area under the curve (AUC) > 0.7). Voided volume was highly diagnostic of DO from either controls or non-DO patients (AUC 0.750 and 0.915, respectively). The proposed prediction model with voided volume, 8-OHdG, and 8-isoprostane (cutoff values 384 mL, 35 ng/mL, and 37 pg/mL, respectively) had an accuracy of 81.7% (sensitivity, 67.7%; specificity, 88.7%; positive predictive value, 75.0%; negative predictive value, 84.6%). Combined with voided volume, urinary oxidative stress biomarkers have the potential to be used to identify urodynamic DO in patients with USI.
Understanding and managing hot electrons in metals are of fundamental and practical interest in plasmonic studies and applications. A major challenge for the development of hot electron devices ...requires the efficient and controllable generation of long-lived hot electrons so that they can be harnessed effectively before relaxation. Here, we report the ultrafast spatiotemporal evolution of hot electrons in plasmonic resonators. Using femtosecond-resolution interferometric imaging, we show the unique periodic distributions of hot electrons due to standing plasmonic waves. In particular, this distribution can be flexibly tuned by the size, shape, and dimension of the resonator. We also demonstrate that the hot electron lifetimes are substantially prolonged at hot spots. This appealing effect is interpreted as a result of the locally concentrated energy density at the antinodes in standing hot electron waves. These results could be useful to control the distributions and lifetimes of hot electrons in plasmonic devices for targeted optoelectronic applications.