Custom-Design of Strong Electron/Proton Extractor on COFs for Efficient Photocatalytic H2O2 Production.

The development of photocatalysts with continuous electron extraction and rapid proton transfer could kinetically accelerate the artificial photosynthesis, but remains a challenge. Herein, we report the topology-guided synthesis of a high-crystalline triazine covalent organic framework (COF) decorated by uniformly distributed polar oxygen functional groups (sulfonic group or carboxyl) as the strong electron/proton extractor for efficient photocatalytic H2O2 production. It was found that the polarity-based proton transfer as well as electron enrichment in as-obtained COFs played a crucial role in improving the H2O2 photosynthesis efficiency (i.e., with an activity order of sulfonic acid- (SO3H-COF)>carboxyl- (COOH-COF)>hydrogen- (H-COF) functionalized COFs). The strong polar sulfonic acid group in the high-crystalline SO3H-COF triggered a well-oriented built-in electric field and more hydrophilic surface, which serves as an efficient carrier extractor enabling a continuous transportation of the photogenerated electrons and interfacial proton to the active sites (i.e., C atoms linked to -SO3H group). As-accelerated proton-coupled electron transfer (PCET), together with the stabilized O2 adsorption finally leads to the highest H2O2 production rate of 4971 µmol g-1 h-1 under visible light irradiation. Meanwhile, a quantum yield of 15 % at 400 nm is obtained, superior to most reported COF-based photocatalysts.

Exploring the pH Sensitivity of Ion-Pair Interactions on a Self-Assembled Monolayer by Scanning Electrochemical Microscopy.

Insights into the chemical essence of weak interactions on the surface of biomacromolecules may help to regulate biological processes. In this work, the pH sensitivity of ion-pair interactions occurring on a cysteine self-assembled monolayer (Cys SAM) that simulates the local surface of a protein was probed by scanning electrochemical microscopy (SECM). Cys SAM and the ion-pair interactions subsequently formed with the introduced aspartic acid (Asp) were both pH-sensitive, as confirmed by the tip current changes in the feedback mode. After continuous pH measurements, the most significant negative feedback was observed at pH 5.50, indicating the most robust ion-pair interactions, which were simultaneously identified by voltammetry. In this case, the extra addition of the inorganic cation (i.e., Ca2+) did not disrupt the existing ion-pair interactions, and the binding constant (K) and Gibbs free energy (ΔGo) of the ion pair were finally determined to be 6.44 × 105 M-1 and -33.14 kJ mol-1, respectively. Overall, the pH sensitivity of ion-pair interactions was found to be mainly attributable to pH-induced changes in the deprotonated/protonated states of the α-amino acid moieties, which may provide insights into the artificial manipulation of complex binding events at the molecular level on the biological surface.

Diabetes and differences in detection of incident invasive breast cancer.

Many women diagnosed with breast cancer have chronic conditions such as diabetes that may impact other health behaviors. Our purpose was to determine if breast cancer screening and detection differs among women with and without diabetes. We conducted a cross-sectional analysis of a retrospective cohort of women aged 52-74 years diagnosed with incident stages I-III breast cancer enrolled in an integrated health plan between 1999 and 2014 with linkage to the Surveillance, Epidemiology and End Results registry (n = 2040). Screening data were taken from electronic health records. We used multivariable modified Poisson regression models with robust standard errors to estimate relative risks (RR) and 95% confidence intervals (CI) for outcomes of (i) receipt of screening in the 2 years prior to diagnosis; (ii) symptom-detected breast cancer; and (iii) diagnosis of locally advanced stage III breast cancer. Compared to women without diabetes, women with diabetes were similar with respect to receipt of screening mammography (78% and 77%), symptom-detected breast cancer (46% and 49%), and stage III diagnosis (7% and 7%). In multivariable models adjusting for age and year of diagnosis, race, BMI, Charlson comorbidity score and depression diagnosis no differences were observed in the outcomes by presence of diabetes. Further investigation is warranted to determine how diabetes acts as a mediating factor in adverse breast cancer outcomes.

Probing a Reversible Cationic Switch on a Mixed Self-Assembled Monolayer Using Scanning Electrochemical Microscopy.

Probing a switch on biomimic membrane surfaces would offer some references to the research on permeability of cytomembranes. In this work, a mixed 11-mercaptoundecanoic acid/1-undecanethiol self-assembled monolayer (MUA/UT SAM) was constructed as a model of a biomembrane. In this mixed SAM, the MUA molecules work as functional parts for the switch and the UT molecules work as diluents. The surface coverage, wetting property, and pKa of this mixed SAM all have been well-inspected. The mixed SAM exhibits excellent switchable properties for cations, which is well-monitored by scanning electrochemical microscopy. When the pH of a solution is higher than the pKa, protons would stimulate a shift of dissociation equilibrium of terminal carboxyl groups. The dissociated carboxylate ions would lead to a switch on the state of the SAM. Otherwise, the SAM shows an off state when the pH is lower than the pKa. In addition, the repeatability, applicability, and the mechanism of the switch all have been well-evaluated.

A Cut-Resistant and Highly Restorable Graphene Foam.

High-pressure resistant and multidirectional compressible materials enable various applications but are often hindered by structure-derived collapse and weak elasticity. Here, a super-robust graphene foam with ladder shape microstructure capable of withstanding high pressure is presented. The multioriented ladder arrays architecture of the foam, consisting of thousands of identically sized square spaces, endow it with a great deal of elastic units. It can easily bear an iterative and multidirectional pressure of 44.5 MPa produced by a sharp blade, and may completely recover to its initial state by a load of 180 000 times their own weight even under 95% strain. More importantly, the foam can also maintain structural integrity after experiencing a pressure of 2.8 GPa through siphoning. Computational modeling of the "buckling of shells" mechanism reveals the unique ladder-shaped graphene foam contributes to the superior cut resistance and good resilience. Based on this finding, it can be widely used in cutting resistance sensors, monitoring of sea level, and the detection of oily contaminants in water delivery pipelines.

Antidepressant Medication Management Among Older Patients Receiving Home Health Care.

OBJECTIVE: Antidepressant management for older patients receiving home health care (HHC) may occur through two pathways: nurse-physician collaboration (without patient visits to the physician) and physician management through office visits. This study examines the relative contribution of the two pathways and how they interplay. METHODS: Retrospective analysis was conducted using Medicare claims of 7,389 depressed patients aged 65 years or older who received HHC in 2006-2007 and who possessed antidepressants at the start of HHC. A change in antidepressant therapy (versus discontinuation or refill) was the main study outcome and could take the form of a change in dose, switch to a different antidepressant, or augmentation (addition of a new antidepressant). Logistic regressions were estimated to examine how use of home health nursing care, patient visits to physicians, and their interactions predict a change in antidepressant therapy. RESULTS: About 30% of patients experienced a change in antidepressants versus 51% who refilled and 18% who discontinued. Receipt of mental health specialty care was associated with a statistically significant, 10- to 20-percentage-point increase in the probability of antidepressant change; receipt of primary care was associated with a small and statistically significant increase in the probability of antidepressant change among patients with no mental health specialty care and above-average utilization of nursing care. Increased home health nursing care in absence of physician visits was not associated with increased antidepressant change. CONCLUSIONS: Active antidepressant management resulting in a change in medication occurred on a limited scale among older patients receiving HHC. Addressing knowledge and practice gaps in antidepressant management by primary care providers and home health nurses and improving nurse-physician collaboration will be promising areas for future interventions.

Uniquely arranged graphene-on-graphene structure as a binder-free anode for high-performance lithium-ion batteries.

3D graphene interconnected frameworks homogeneously connected with a few-layer graphene film (3DG/FLG) constitute a novel hierarchical hybrid structure for anodes in lithium-ion batteries. The pore-rich 3D graphene network is favorable for Li(+) diffusion and electron transport, and the FLG is a non-metallic current collector that effectively collects/transports charge carriers from/to the 3D graphene network and provides an excellent scaffold to support the 3DG.

Diffusion of accelerated partial breast radiotherapy in the United States: physician-level and patient-level analyses.

PURPOSE: To evaluate diffusion of brachytherapy-based accelerated partial breast radiotherapy (RT) in the United States, a new breast cancer treatment requiring 5 days twice daily, rather than daily treatment for 6-7 weeks. It has limited long-term effectiveness data compared with standard whole breast RT. DATA AND METHODS: We used 2005-2008 Medicare claims for female Medicare beneficiaries receiving RT after breast-conserving surgery merged with physician and area-based data (n=74,254 patient-subjects; n=1901 physicians), applying logistic regression to estimate: (1) proportion of patients for whom the radiation oncologist used brachytherapy-based accelerated RT, and (2) probability a patient received brachytherapy-based accelerated RT, clustering on physician. RESULTS: Use of accelerated partial breast RT increased over time (8% in 2005 to 17% in 2008). Physician-level analysis indicates rural physicians were less likely to perform accelerated RT [odds ratio (OR): 0.35-0.49; P<0.002)]; as were those licensed 20+years [OR: 0.54; 95% confidence interval (CI), 0.39-0.74]. Overall, 11.7% of patients received accelerated RT. Treatment post 2005 was associated with increasing odds of receiving accelerated RT (P<0.0001). Older age was associated with lower odds of receiving accelerated RT (reference, 66-69 years old, OR: 0.90, P<0.006), as was black (OR: 0.73;95% CI, 0.63-0.85) or other race (OR: 0.80; 95% CI, 0.65-1.00), living in rural areas (OR: 0.8; P<0.0001), or seeing an older physician [20+years postgraduation (OR: 0.7; 95% CI, 0.5-0.9)]. Patients living in counties with more hospitals with advanced RT facilities were more likely to undergo accelerated RT (OR: 1.4; 95% CI, 1.1-1.8). DISCUSSION: This new technology appears to be in the early phase of diffusion across the United States and is more rapidly being taken up in younger, white patients living in urban and suburban areas with availability of advanced RT facilities. Rural and older patient populations are not tending to undergo the treatment.

Graphene quantum dots-three-dimensional graphene composites for high-performance supercapacitors.

Graphene quantum dots (GQDs) have been successfully deposited onto the three-dimensional graphene (3DG) by a benign electrochemical method and the ordered 3DG structure remains intact after the uniform deposition of GQDs. In addition, the capacitive properties of the as-formed GQD-3DG composites are evaluated in symmetrical supercapacitors. It is found that the supercapacitor fabricated from the GQD-3DG composite is highly stable and exhibits a high specific capacitance of 268 F g(-1), representing a more than 90% improvement over that of the supercapacitor made from pure 3DG electrodes (136 F g(-1)). Owing to the convenience of the current method, it can be further used in other well-defined electrode materials, such as carbon nanotubes, carbon aerogels and conjugated polymers to improve the performance of the supercapacitors.

Graphene quantum dots-carbon nanotube hybrid arrays for supercapacitors.

Graphene quantum dots (GQDs) have been successfully deposited onto aligned carbon nanotubes (CNTs) by a benign electrochemical method and the capacitive properties of the as-formed GQD/CNT hybrid arrays were evaluated in symmetrical supercapacitors. It was found that supercapacitors fabricated from GQD/CNT hybrid arrays exhibited a high capacitance of 44 mF cm(-2), representing a more than 200% improvement over that of bare CNT electrodes.

An all-cotton-derived, arbitrarily foldable, high-rate, electrochemical supercapacitor.

The pure natural cotton provides a low-cost material platform for the facile assembly of all-cotton-derived electrochemical supercapacitors (allC-ECs) with a remarkable character of arbitrary foldability and high response rate, which can be bent, rolled-up, and fully folded without loss of high-rate (<50 ms) capacitive performance.

Lung Cancer Patients' and Caregivers' Satisfaction With Multidisciplinary Versus Serial Care in a Community Healthcare Setting: A Prospective Comparative-Effectiveness Cohort Study.

BACKGROUND: Multidisciplinary Care is recommended for complex oncologic conditions. We compared lung cancer patients' and caregivers' satisfaction with Multidisciplinary Care to routine, serial care. MATERIALS AND METHODS: We analyzed validated surveys administered at baseline, 3 and 6 months to patients and their caregivers enrolled in a prospective cohort comparative-effectiveness study of Multidisciplinary versus Serial Care (clinicaltrials.gov NCT02123797). Multivariate mixed linear models examined the cross-group differences, time-related variances, and how interaction between groups and time-periods influenced satisfaction. RESULTS: Compared to serial care (N = 297), the Multidisciplinary Care cohort (N = 159), was older (69 vs. 66 years), had earlier clinical stage (41% vs. 33% stage I/II), and less severe symptoms (45% vs. 35% asymptomatic). Demographic and social-economic characteristics of caregivers (N = 99 for Multidisciplinary and 123 for Serial Care, respectively) were similar. Multidisciplinary Care patients and caregivers were more likely to perceive their care to be better than that of other patients (p < .01). Although Serial Care patients and caregivers expressed greater satisfaction with their treatment plan (p < .01 patients, p = 0.04 caregivers), Multidisciplinary Care patients showed greater improvement at 6-months (p < .01). Multidisciplinary Care patients and caregivers reported better overall satisfaction with team members (p < .01) while Serial Care patients had greater improvement in their satisfaction with team members at 6-months (p = .04). Multidisciplinary Care patients perceived more financial burden at 6-months compared to Serial Care patients (p = .04). CONCLUSION: Patient-caregiver dyads had mixed perceptions of their care experience. Recipients of Multidisciplinary Care perceived better experience with care and team members; Serial Care recipients expressed greater satisfaction with their treatment plan.

Cerebrovascular reserve and stroke risk in patients with carotid stenosis or occlusion: a systematic review and meta-analysis.

BACKGROUND AND PURPOSE: Impairments in cerebrovascular reserve (CVR) have been variably associated with increased risk of ischemic events and may stratify stroke risk in patients with high-grade internal carotid artery stenosis or occlusion. The purpose of this study is to perform a systematic review and meta-analysis to summarize the association of CVR impairment and stroke risk. METHODS: We performed a literature search evaluating the association of impairments in CVR with future stroke or transient ischemic attack in patients with high-grade internal carotid artery stenosis or occlusion. We included studies with a minimum of 1-year patient follow-up with baseline CVR measures performed by any modality and primary outcome measures of stroke and/or transient ischemic attack. A meta-analysis with assessment of study heterogeneity and publication bias was performed. Results were presented in a forest plot and summarized using a random-effects model. RESULTS: Thirteen studies met the inclusion criteria, representing a total of 1061 independent CVR tests in 991 unique patients with a mean follow-up of 32.7 months. We found a significant positive relationship between impairment of CVR and development of stroke with a pooled random effects OR of 3.86 (95% CI, 1.99-7.48). Subset analysis showed that this association between CVR impairment and future risk of stroke/transient ischemic attack remained significant regardless of ischemic outcome measure, symptomatic or asymptomatic disease, stenosis or occlusion, or CVR testing method. CONCLUSIONS: CVR impairment is strongly associated with increased risk of ischemic events in carotid stenosis or occlusion and may be useful for stroke risk stratification.

Inappropriate medication in a national sample of US elderly patients receiving home health care.

BACKGROUND: With substantial morbidity and functional impairment, older patients receiving home health care are especially susceptible to the adverse effects of unsafe or ineffective medications. Home health agencies' medication review and reconciliation services, however, provide an added mechanism of medication safety that could offset this risk. OBJECTIVE: To estimate the prevalence of potentially inappropriate medications (PIMs) among current elderly home health patients in the US. DESIGN: Cross-sectional analysis using data from the 2007 National Home and Hospice Care Survey. SUBJECTS: 3,124 home health patients 65 years of age or older on at least one medication. MAIN MEASURES: Prevalence and classification of PIM use and the association between PIM use and patient and home health agency characteristics.Key Results In 2007, 38% (95% CI: 36-41) of elderly home health patients were taking at least one PIM. Polypharmacy was associated with an increased risk of PIM use; admission to home health care from a nursing home or other sub-acute facility (compared to admission from the community) and a payment source other than Medicare or Medicaid were associated with a decreased risk of PIM use. CONCLUSIONS: The prevalence of PIM use in older home health patients is high despite potential mechanisms for improved safety. Policies to improve the review and reconciliation processes within home health agencies and to improve physician-home health clinician collaboration are likely needed to lower the prevalence of PIM use in older home health patients.

Functional microspheres of graphene quantum dots.

Graphene-quantum-dot microspheres (GQDSs) have been prepared by assembly of graphene quantum dots (GQDs) via a water-in-oil (W/O) emulsion technique without the addition of any surfactants. Although made of quantum-sized graphene dots, the as-formed GQDSs are solid and remain intact after slight ultrasonication. The versatile W/O emulsion method allows the in situ intercalation of functional nanocomponents into the GQDSs for specific applications. As exemplified by the Fe(3)O(4)-containing GQDSs, Fe(3)O(4)-GQDSs exhibit a large magnetic response. Furthermore, the embedded Fe(3)O(4) nanoparticles in GQDSs can act as the catalysts for the growth of carbon nanotubes (CNTs), which opens the opportunities for fabricating new complex structures of CNTs surrounding GQDSs by simple chemical vapor deposition.

Radiation Without Endocrine Therapy in Older Women With Stage I Estrogen-Receptor-Positive Breast Cancer is Not Associated With a Higher Risk of Second Breast Cancer Events.

PURPOSE: The omission of radiation therapy (RT) in older women with stage 1 estrogen-receptor-positive (ER+) breast cancer receiving endocrine therapy (ET) is an acceptable strategy based on randomized trial data. Less is known about the omission of ET with or without RT. METHODS AND MATERIALS: We analyzed surveillance, epidemiology, and end results (SEER)-Medicare data for 13,321 women age 66 years or older with stage I ER+ breast cancer from 2007 to 2012 who underwent breast-conserving surgery. Patients were classified into 4 groups: (1) ET + RT (reference); (2) ET alone; (3) RT alone; and (4) neither RT nor ET (NT). Second breast cancer events (SBCEs) were captured using the Chubak high-specificity algorithm. We used χ2 tests for descriptive statistics, multivariable multinomial logistic regression to estimate relative risk of undergoing a treatment, and multivariable, propensity-weighted competing-risks survival regression to estimate standardized hazard ratio (SHR) of SBCE. We set significance at P ≤ .01. RESULTS: Most women underwent both treatments, with 44% undergoing ET + RT, 41% RT alone, 6.6% ET alone, and 8.6% NT, but practice patterns varied over time. From 2007 to 2012, RT decreased from 49% to 30%, whereas ET alone and ET + RT increased (ET alone, 5.4%-9.6%; ET + RT, 38%-51%). Compared with patients age 66 to 69 years, patients age 80 to 85 years were more likely to receive NT (odds ratio [OR], 8.9), RT (OR, 1.9), or ET (OR, 8.8) versus ET + RT (P < .01). Three percent of subjects had an SBCE (2.2% ET + RT, 3.0% RT alone, 3.2% ET alone, 7.0% NT). Relative to ET + RT, NT and ET alone were associated with higher SBCE (NT: SHR, 3.7, P < .001; ET alone: SHR, 2.2, P = .008), whereas RT was not associated with a higher SBCE (SHR 1.21; P = .137). Clinical factors associated with higher SBCE were HER2 positivity and pT1c (SHR, 1.7; P = .006). CONCLUSIONS: Treatment with RT alone in older women with stage I ER+ disease is decreasing. RT alone is not associated with an increased risk for SBCE. By contrast, NT and ET are both associated with higher SBCE in multivariable analysis with propensity weighting. Further study of the omission of endocrine therapy in this patient population is warranted.

Reborn Three-Dimensional Graphene with Ultrahigh Volumetric Desalination Capacity.

The constructing of 3D materials with optimal performance is urgently needed to meet the growing demand of advanced materials in the high-tech sector. A distinctive 3D graphene (3DG) is designed based on a repeated rebirth strategy to obtain a better body and performance after each round of rebirth, as if it is Phoenix Nirvana. The properties of reborn graphene, namely 3DG after Nirvana (NvG), has been dramatically upgraded compared to 3DG, including high density (3.36 times) together with high porosity, as well as better electrical conductivity (1.41 times), mechanical strength (32.4 times), and ultrafast infiltration behavior. These advantages of NvG make it a strong intrinsic motivation for application in capacitive deionization (CDI). Using NvG directly as the CDI electrode, it has an extremely high volumetric capacity of 220 F cm-3 at 1 A cm-3 and a maximum salt absorption capacity of 8.02~9.2 mg cm-3 (8.9-10.2 times), while the power consumption for adsorption of the same mass of salt is less than a quarter of 3DG. The "Phoenix Nirvana"-like strategy of manufacturing 3D structures will undoubtedly become the new engine to kick-start the development of innovative carbon materials through an overall performance upgrade.

Prophylactic central neck dissection and local recurrence in papillary thyroid cancer: a meta-analysis.

BACKGROUND: The effectiveness of prophylactic central neck dissection (pCND) in the treatment of patients with papillary thyroid carcinoma (PTC) to prevent local recurrence is controversial. We performed a meta-analysis to assess the effect of pCND on local recurrence in PTC. METHODS: Exhaustive search of online search engines identified five retrospective studies that compared the local recurrence rates of PTC in patients without clinically detectable nodal disease in patients undergoing thyroidectomy + pCND (group A) to those undergoing thyroidectomy alone (group B). A meta-analysis was performed by the fixed effects method. Recurrence was documented by imaging, thyroglobulin detection, or reoperation. Location of recurrence was identified in either the central or lateral neck compartment. RESULTS: A total of 1264 patients were included, 396 in group A and 868 in group B. Follow-up ranged from 6 months to 27 years. The overall recurrence rate was 2.02% in group A versus 3.92% in group B (odds ratio [OR] = 1.05, 95% confidence interval [95% CI] 0.48-2.31). The recurrence rate in the central neck compartment in group A was 1.86% compared to 1.68% in group B (OR = 1.31, 95% CI 0.44-3.91). The recurrence rate in the lateral neck compartment in group A was 3.73% compared to 3.79% in group B (OR = 1.21, 95% CI 0.52-2.75). There was no statistically significant difference in the OR in the local recurrence between the two groups. CONCLUSIONS: This meta-analysis indicates that pCND does not greatly reduce local recurrence in thyroid cancer. However, the available studies have substantial limitations and a prospective multicenter study to determine the indications for pCND is warranted.

Frontiers of carbon materials as capacitive deionization electrodes.

Capacitive deionization (CDI), which is based on ion electrosorption on the surface of electrically charged electrodes, has attracted widespread attention as a novel, cost-effective and environment-friendly desalination technology. Carbon materials are widely used as CDI electrodes due to their high specific surface area (SSA), superior conductivity, and better stability. Many research efforts have been made to further enhance the CDI performance of carbon materials. In this review, the performance-enhancing strategies of various carbon materials including activated carbon, porous carbon, carbon aerogels, carbon nanotubes and graphene are systematically presented. We also explain the significance of the development of CDI technology and identify where further work is urgently required and where challenges are still faced.

Controllable release of dopamine from simulated enzyme-containing biomembrane by biased potential.

Controllable release of dopamine (DA) is worth studying for its significant in physiological metabolic process. ß-cyclodextrin/11-mercaptoundecanoic acid self-assembled monolayer (ß-CD/MUA SAM) based on hydrogen bonds network was constructed as simulated enzyme-containing biomembrane. DA interacted with ß-CD based on intermolecular hydrogen bond and formed inclusion complexes in SAM, namely DA@ß-CD/MUA SAM. The desorption process of DA from DA@ß-CD/MUA SAM revealed the release behavior of DA from enzyme-containing biomembrane at molecular level. Positive biased potential as external stimulus was applied at DA@ß-CD/MUA SAM, reducing the negative charge density of SAM. The decrease of negative charge density of SAM resulted in the weakening of hydrogen bond between DA and ß-CD, which in turn caused DA to be released. Using scanning electrochemical microscopy, positive biased potential not only had specificity induction for the release of DA, but also was able to monitor the release quantitatively in real time. These results showed that positive biased potential as external stimulus was favorable for the controllable release of DA, suggesting the possible application of biased potential in controllable regulation field.