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Photosynthesis of CO from CO2 with an iron polypyridyl catalyst at a passivated silicon photoelectrode
Get PDFA first-row transition metal catalyst, [Fe(tpy)(Mebim-py)(NCCH3)]2+ (tpy = 2,2′:6′,2′′-terpyridine, Mebim-py = 1-methylbenzimidazol-2-ylidene-3-(2′-pyridine)) mediates CO2 reduction to CO at passivated p-Si photoelectrodes with applied potentials 240 mV positive of the standard CO2/CO reduction potential. The molecular catalyst's selectivity for CO was retained under photoelectrochemical conditions, with negligible direct proton reduction promoted by the photoelectrode. The faradaic efficiency for CO (44 ± 6%) was slightly enhanced relative to the catalyst performance in the dark (33%). A photosynthetic cell based on this photocathode system, coupled with ferrocene oxidation at the anode, successfully operated at a cell voltage of −1.2 V. The photovoltage generated by illumination of p-Si–CH3 met and surpassed the potential required for CO2 reduction when coupled with ferrocene oxidation. By leveraging a low-overpotential CO2 reduction electrocatalyst, a photo-assisted electrochemical efficiency of 0.15% and applied bias photon-to-current efficiency of 0.05% was achieved for this single-junction cell, ultimately storing 46 kJ mol−1 (11 kcal mol−1) of photon energy.A first-row transition metal catalyst, [Fe(tpy)(Mebim-py)(NCCH3)]2+, mediates CO2 reduction at passivated p-Si photoelectrodes at a cell voltage of –1.2 V, storing 46 kJ mol−1 of photon energy in the CO fuel product
A Parent's Perspective on Systemic Gaps in Supporting Complex Pediatric Care at Home
Get PDFChildren with complex medical needs often require substantial medical care, including at home, where family members perform many procedures typically reserved for licensed nurses. This article presents a caregivers’ perspective of navigating the healthcare system while managing her daughter's care following a diagnosis of Ataxia-Telangiectasia, a rare neurodegenerative disease. It reflects on the systemic gaps in how we prepare and support family caregivers, particularly regarding end-of-life discussions. This article highlights how caregivers are uniquely positioned to identify inefficiencies, safety concerns, and innovative solutions both in hospital and home settings, often before they are recognized by the larger healthcare system. Recommendations include establishing formal caregiver feedback systems, standardizing caregiver training, and developing values-based communication training for clinicians. By integrating caregivers into formal processes, healthcare systems can become more responsive to the needs of children with complex needs and their families
Health workers’ perspectives on barriers and opportunities to optimising quality improvement implementation in urban health facilities in Lilongwe, Malawi
Get PDFEliminating vertical HIV transmission requires high-quality Option B+ services, which provide lifelong antiretroviral therapy to pregnant and breastfeeding women living with HIV. In Malawi, coverage has expanded, but quality remains suboptimal, contributing to challenges in sustaining engagement in care. Quality improvement (QI) approaches can strengthen service delivery and evidence-based practices, with healthcare workers (HCWs) central to implementation. This study explores barriers and opportunities HCWs face in implementing QI in Option B+ within high-volume urban facilities in Lilongwe, Malawi. A descriptive phenomenological qualitative study was conducted between March and June 2021 in five health facilities in Lilongwe, Malawi. Semistructured in-depth interviews were conducted with 30 purposively selected HCWs (4–8 per facility) involved in delivering Option B+ services. Thematic analysis was used, with data coded deductively and inductively. The Consolidated Framework for Implementation Research was applied to map the identified themes into relevant domains and constructs. QI practices among HCWs were hindered by resource constraints, lack of incentives/reimbursement for QI activities conducted beyond working hours, poor communication between QI teams and implementers and resistance or negative attitudes towards QI. Opportunities to enhance QI included increasing meeting frequency, providing mentorship, peer-to-peer learning through exchange visits and securing funding from development partners. Improving QI utilisation in Option B+ requires mobilising resources and having a structured feedback and mentorship mechanisms. Targeted incentives/reimbursements for HCWs and peer-to-peer learning through exchange visits between facilities can further enhance QI. Therefore, a blended QI approach incorporating these recommendations is needed to better support HCWs in delivering evidence-based interventions, strengthen the health system and may improve engagement outcomes
Cation-switchable transposition and hydrogenation of alkenes via interconnected reaction mechanisms.
Get PDFCation-switchable catalysis is a promising strategy for modulating reaction rates or selectivity using external stimuli, with potential applications including polymer synthesis and tandem catalysis. This study establishes a deeper understanding of the mechanistic origins of cation rate promotion in systems where a hemilabile crown ether affixed to the catalyst serves as a cation receptor site, which in turn enables reactivity extensions of this platform to introduce cation-switchable alkene hydrogenation. The mechanistic study hinges on the synthesis of two previously unreported iridium(iii) complexes, bearing either bis(2-methoxyethyl)amine or diethylamine groups, which could be compared in catalysis with and without cation promoters. Only the catalyst containing a crown ether exhibits switchable catalysis, providing support for a "substrate gating" mechanism in which cations tune the hemilability of the crown ether donors to enable alkene binding. The generality of the substrate gating mechanism is established through the extension of catalytic reactivity to cation-switchable alkene hydrogenation. The crown-ether-containing catalyst was found to be an effective hydrogenation catalyst capable of reducing internal and trisubstituted olefins. The isomerization and hydrogenation reactions occur at similar rates in some cases, and kinetic and labeling studies provide insight into the implications of competitive reactivity
Serum Arginase−1 is a predictive biomarker for melanoma patients and a surrogate indicator of systemic myeloid cell fitness
Get PDFWhile recent advances in immuno-oncology have revolutionized cancer therapy, only a subset patients benefit from these treatments and achieve durable clinical responses. Biomarker-guided identification of patients likely to respond to immunotherapy could enable more effective management of various malignancies. To explore this, we took advantage of a Phase I trial evaluating the efficacy of antigen-engineered dendritic cell (DC) vaccine, administered either as monotherapy or in combination with high-dose interferon-α2b, in promoting anti-tumor immunity in melanoma patients. Liquid biopsies, including serum and peripheral blood mononuclear cells, and tumor biopsies were previously analyzed for predictive markers using Luminex, NanoString gene expression profiling and flow cytometry. Here, in vitro stimulation assays were conducted to assess arginase−1 production by circulating myeloid subsets. Of 73 serum analytes, serum arginase−1 (sArg1) most effectively distinguished melanoma patients with measurable disease from healthy donors. Elevated sArg1 levels in patients with active disease correlated with favorable responses to the vaccine and were associated with longer overall and progression-free survival. Integrated phenotypic, functional and metabolic analyses identified circulating CD14-CD11c+ DC3 as the likely source of sArg1. These findings support the hypothesis that sArg1 may serve as a biomarker for responsiveness to cancer vaccine immunotherapy and reflect systemic myeloid cell fitness associated with enhanced anti-tumor immunity. Given the stability and accessibility of serum compared to cells or tissues, this assay could offer a method for assessing patient status, potentially improving stratification and clinical decision-making
University Students Implement a Nutrition and Cooking Education Curriculum With Fidelity
Get PDFObjective To assess the ability of trained university students to implement Cooking Matters for Kids, a hands-on nutrition and cooking education curriculum for third through fifth-grade children. Methods Process evaluation data were collected from 6 Cooking Matters for Kids courses led by university students in the fall of 2019 and spring of 2020 at 6 afterschool programs in Orange County, North Carolina. Trained research assistants observed lessons and reported whether key intervention components were implemented as planned, the level of participant engagement, what worked well, and what could be improved on. Results University students implemented the curriculum with high fidelity and kept most participants engaged during lessons. Dividing children into smaller groups and assigning instructor roles worked well. Limited completion of take-home challenge activities was an area to improve on. Conclusions and Implications University students may be effective instructors for Cooking Matters for Kids and other related programs
Exploring prefrontal alpha modulation as a mechanistic treatment target in lupus-associated depression: A transcranial alternating current stimulation study.
Get PDFObjective This study explored whether modulating prefrontal alpha oscillations using transcranial alternating current stimulation (tACS) could alleviate depressive symptoms in individuals with systemic lupus erythematosus (SLE). Methods Over the course of 5 days, three individuals underwent daily 40-min sessions of 2 mA bifrontal individual alpha frequency tACS (IAF-tACS) while watching a relaxing video. Resting-state 128-channel electroencephalography (EEG) was recorded on Day 1 and Day 5 before each tACS session. Self-reported assessments of depression, anxiety, insomnia, and fatigue were administered on Day 1, Day 5, and at the 2- and 4-week follow-ups. Results Two out of three participants showed a reduction in left prefrontal alpha power after 5 days of IAF-tACS. Only those with this reduction reported short-term improvements in depression, insomnia, anxiety, and well-being. Conclusion These preliminary results suggest that modulating prefrontal alpha oscillations through tACS may offer a potential approach for alleviating depressive symptoms in individuals with SLE
Alzheimer’s disease plasma biomarkers are associated with cognitive performance among Hispanic/Latino adults
Get PDFBackground Blood-based biomarkers hold promise as a minimally invasive tool for identifying early signs of Alzheimer’s disease pathology and neurodegeneration. We investigated associations between plasma biomarkers of amyloid-beta, tau, neuroaxonal injury, and glial activation with cognitive performance among community-dwelling Hispanic/Latino adults in the United States. Methods We analyzed cross-sectional data from 5730 adults aged 50 years and older (unweighted; mean [SD], 63.5 [8.2] years) in the Study of Latinos-Investigation of Neurocognitive Aging (SOL-INCA; 2016–2018). Plasma concentrations of amyloid-beta (Aβ42/40), phosphorylated tau-181 (pTau-181), neurofilament light chain (NfL), and glial fibrillary acidic protein (GFAP) were quantified (Quanterix Simoa HD-X) and log-transformed (ln). Cognitive performance was assessed across domain-specific scores (learning, memory, verbal fluency, and executive functioning/processing speed) used to calculate global cognitive performance. Survey-weighted linear regression models were used to examine associations between plasma biomarkers and cognitive performance, adjusting for sociodemographic, cardiometabolic, kidney, and APOE ε4 covariates. Results Here we show higher ln(pTau-181) and ln(NfL) are associated with lower global cognitive performance (bpTau-181 = −0.06; 95%CI = [−0.12;−0.01]; p = 0.022; bNfL = −0.07; 95%CI = [−0.12;−0.02]; p = 0.005). Lower ln(Aβ42/40) is associated with poorer verbal fluency, higher ln(pTau-181) is associated with poorer learning and memory, and higher ln(NfL) is associated with learning and executive functioning/processing speed. We find ln(GFAP) is not significantly associated with cognitive performance. Conclusions Plasma biomarkers related to Alzheimer’s disease pathophysiology and broader neurodegenerative processes are associated with cognitive performance among Hispanic/Latino adults. These findings highlight the potential utility of blood-based biomarkers for identifying early cognitive vulnerability in this population
Criminalizing free Black migrants in antebellum North Carolina: State law, the planter class, and lived experience
Get PDFThis article examines an 1826 North Carolina Act that criminalized the migration of free Black people into the state, using forced labor and confinement as punitive mechanisms. Through archival and legal analysis, I show how the Act functioned as a tool of racialized mobility control, reinforcing white planter power. The study situates state-level migration law within the broader history of migration law, highlighting its role in racial subordination through legal frameworks, private capital-state entanglements, and economic incentives tied to confinement and forced labor. Further, I analyze ways that free Black people navigated and contested these restrictions, exposing the limits of legal enforcement and the agency of those subject to it. Attending to these dynamics expands epistemologies of migration by foregrounding state-level regimes of migration control of the antebellum United States and contributes to centering Black mobility within migration narratives
Simultaneous initiation of finerenone and empagliflozin across the spectrum of kidney risk in the CONFIDENCE trial.
Get PDFThe CONFIDENCE (COmbinatioN effect of FInerenone anD EmpaglifloziN in participants with CKD and type 2 diabetes using a UACR Endpoint) trial investigated the safety and efficacy of simultaneously initiating finerenone and empagliflozin for patients with chronic kidney disease (CKD) and type 2 diabetes. This prespecified analysis aimed to determine if the predicted risk of kidney disease progression, based on KDIGO risk categories, influenced the benefits and safety of this combination therapy.The double-blind, double-dummy trial randomized 818 adults with CKD and type 2 diabetes [urine albumin-creatinine ratio (UACR) ≥100 to <5000 mg/g] to receive once-daily finerenone plus empagliflozin, finerenone alone or empagliflozin alone, all in addition to a renin-angiotensin system inhibitor. The relative change in UACR from baseline to day 180 (primary endpoint) and a >30% reduction in UACR (secondary endpoint) across KDIGO risk categories was assessed.At baseline, among 781 with available data, 11.3% of participants were classified as low/moderate risk, 29.6% as high risk and 59.2% as very high risk. At 180 days, combination therapy significantly reduced UACR levels across all KDIGO risk categories (low/moderate: -61.7%; high: -60.7%; very high: -52.4%). This reduction was consistently greater than that achieved with either monotherapy alone. More than half of patients on combination therapy experienced UACR reductions of >30% (low/moderate: 58.1%; high: 74.2%; very high: 70.6%), again outperforming monotherapies across all risk groups. While hyperkalemia was more common with combination therapy, early eGFR declines (>30% within 30 days) were less frequent in individuals with higher KDIGO risk compared with lower risk. Overall, the safety profile of combination therapy remained consistent across all KDIGO risk categories, with no unexpected safety signals.The CONFIDENCE trial demonstrates that the relative efficacy and safety of simultaneous finerenone and empagliflozin combination therapy are consistent across a wide spectrum of predicted kidney disease risk.NCT05254002; EudraCT 2021-003037-11