Angew Chem Int Ed Engl
January 2025
The dynamic response of heterogeneous catalytic materials to their environment opens a wide variety of possible surface states which may have increased catalytic activity. In this work, we find that it is possible to generate a surface state with increased catalytic activity over metallic 2 nm Pt nanoparticles by performing a thermal treatment of the CO*-covered Pt catalyst. This state is characterised by its ability to oxidise CO to CO at room temperature.
View Article and Find Full Text PDFDespite the broad catalytic relevance of metal-support interfaces, controlling their chemical nature, the interfacial contact perimeter (exposed to reactants), and consequently, their contributions to overall catalytic reactivity, remains challenging, as the nanoparticle and support characteristics are interdependent when catalysts are prepared by impregnation. Here, we decoupled both characteristics by using a raspberry-colloid-templating strategy that yields partially embedded PdAu nanoparticles within well-defined SiO or TiO supports, thereby increasing the metal-support interfacial contact compared to nonembedded catalysts that we prepared by attaching the same nanoparticles onto support surfaces. Between nonembedded PdAu/SiO and PdAu/TiO, we identified a support effect resulting in a 1.
View Article and Find Full Text PDFIt is important to maintain confidence in the risk and benefit balance of major caries-preventive programs using fluoride. The ongoing debate about potential effects of early-life exposures to fluoride on cognitive neurodevelopment requires high-quality scientific evidence. This study aimed to investigate the potential effects of fluoride exposure on cognitive neurodevelopment assessed with the Wechsler Adult Intelligence Scale 4th edition (WAIS-IV) in an Australian population-based sample.
View Article and Find Full Text PDFPurpose: The purpose of this study was to identify and test the factor structure of the Agricultural Producer Barriers to Care Scale (APBCS), which assesses barriers to engaging with health care in rural US farmers.
Methods: Respondents (n = 1045) completed an online survey that was distributed digitally and in-person by researchers and community partners at farming events and via farm-related social media. Exploratory and Confirmatory Factor Analysis were used to assess the underlying factor structure of the APBCS, and McDonald's omega coefficients were calculated to test the reliability of each factor and the instrument as a whole.
The catalytic and plasmonic properties of bimetallic gold-palladium (Au-Pd) nanoparticles (NPs) critically depend on the distribution of the Au and Pd atoms inside the nanoparticle bulk and at the surface. Under operating conditions, the atomic distribution is highly dynamic. Analyzing gas induced redistribution kinetics at operating temperatures is therefore key in designing and understanding the behavior of Au-Pd nanoparticles for applications in thermal and light-driven catalysis, but requires advanced characterization strategies.
View Article and Find Full Text PDFInt J Environ Res Public Health
August 2024
The purpose of this study was to explore female farmers' perspectives on barriers to engaging with resources for physical and mental healthcare faced by agriculture producers in the state of Georgia. In-depth interviews were conducted with female farm owners and managers ( = 16) across the state. Interviews were recorded and transcribed, and researchers coded interviews separately before thematic analysis was used to identify common themes.
View Article and Find Full Text PDFBackground: Parents exposed to psychosocial adversities often experience challenges which, combined with the needs of a new-born infant, can be difficult to manage and increase the risk of poor outcomes for both parents and infants. Psychosocial adversity can disrupt the development of parental-foetal attachment to the baby during pregnancy, which can have a negative effect on parental care and quality of interaction during the postnatal period. This intervention is based on the proposition that enhanced parental capacity to mentalise and emotionally connect to unborn children during pregnancy, and better understanding about how to manage distressing infant behaviour (i.
View Article and Find Full Text PDFNanoparticle (NP) size and proximity are two physical descriptors applicable to practically all NP-supported catalysts. However, with conventional catalyst design, independent variation of these descriptors to investigate their individual effects on thermocatalysis remains challenging. Using a raspberry-colloid-templating approach, we synthesized a well-defined catalyst series comprising PdAu alloy NPs of three distinct sizes and at two different interparticle distances.
View Article and Find Full Text PDFThis study introduces a novel iterative Bragg peak removal with automatic intensity correction (IBR-AIC) methodology for X-ray absorption spectroscopy (XAS), specifically addressing the challenge of Bragg peak interference in the analysis of crystalline materials. The approach integrates experimental adjustments and sophisticated post-processing, including an iterative algorithm for robust calculation of the scaling factor of the absorption coefficients and efficient elimination of the Bragg peaks, a common obstacle in accurately interpreting XAS data, particularly in crystalline samples. The method was thoroughly evaluated on dilute catalysts and thin films, with fluorescence mode and large-angle rotation.
View Article and Find Full Text PDFA detailed knowledge of reaction kinetics is key to the development of new more efficient heterogeneous catalytic processes. However, the ability to resolve site dependent kinetics has been largely limited to surface science experiments on model systems. Herein, we can bypass the pressure, materials, and temperature gaps, resolving and quantifying two distinct pathways for CO oxidation over SiO-supported 2 nm Pt nanoparticles using transient pressure pulse experiments.
View Article and Find Full Text PDFObjectives: The purposes of this study were to explore behavioral and mental health outcomes among a sample of farmers living in the United States and to compare differences between male and female farmers.
Methods: An online cross-sectional survey was distributed within the farming community by researchers, farming consultants, and community partners. χ 2 and analysis or variance analyses were used to explore relationships between variables of interest.
Herein, we present a design for a transient flow reactor system with high detection sensitivity and minimal dead volume, such that it is capable of sub-second switching of the gas stream flowing through a catalytic bed. We demonstrate the reactor's capabilities for step transient, pulse, and stream oscillation experiments using the model system of CO oxidation over Pd catalysts, and we find that we are able to precisely model step transients for CO oxidation using a pseudo-homogenous-packed bed reactor model. The design principles leading to minimal gas hold-up time and increased sensitivity that are described in this paper can be implemented into existing flow reactor designs with minimal cost, providing a readily accessible alternative to the existing transient instrumentation.
View Article and Find Full Text PDFComplex regional pain syndrome (CRPS) is a relatively rare, but debilitating condition that may occur after limb or peripheral nerve trauma. Typical symptoms of CRPS include swelling, allodynia, hyperalgesia, and skin temperature changes. Although a variety of pharmacological and non-pharmacological approaches are commonly used in caring for individuals with CRPS, they are frequently ineffective and often associated with side effects and/or additional risks.
View Article and Find Full Text PDFMyocardial strain offers new insights into ventricular performance, There are software packages from several different companies used to ascertain this, and little data is available in patients with single right ventricle (sRV) physiology. We aimed to compare the analysis of two strain software applications using a cohort of patients with sRV for both inter-vendor and inter-observer variability. Echocardiograms from 85 patients with sRV (122 separate studies) were prospectively evaluated.
View Article and Find Full Text PDFAccurate assessment of the right ventricular (RV) volume and function is important in patients with hypoplastic left heart syndrome (HLHS). We sought to investigate the effect of ventriculotomy on the correlation of RV functional assessments by two-dimensional echocardiography (2DE) to cardiac magnetic resonance (CMR)-derived RV ejection fraction (EF) in patients with HLHS. A retrospective re-analysis of CMR imaging with matched 2DE was performed from the institutional HLHS registry.
View Article and Find Full Text PDFLeft ventricular (LV) morphology may affect right ventricular (RV) function before and after Fontan palliation in patients with hypoplastic left heart syndrome (HLHS). We sought to assess the potential impact of LV morphology on RV function in patients with HLHS using cardiac magnetic resonance (CMR) imaging. A retrospective analysis of available CMR scans from all patients with HLHS was performed.
View Article and Find Full Text PDFSuperconducting radio frequency niobium cavities are the building blocks of modern accelerators for scientific applications. Lower surface resistance, higher fields, and high operating temperatures advance the reach of the future accelerators for scientific discovery as well as potentially enabling cost-effective industrial solutions. We describe the design and performance of an NbSn coating system that converts the inner surface of niobium cavities to an NbSn film.
View Article and Find Full Text PDFControlling the selectivity of catalytic reactions is a critical aspect of improving energy efficiency in the chemical industry; thus, predictive models are of key importance. Herein the performance of a heterogeneous, nanoporous Au catalyst is predicted for the complex catalytic self-coupling of the series of C -C alkyl alcohols, based solely on the known kinetics of the elementary steps of the catalytic cycle for methanol coupling, using scaling methods augmented by density functional theory. Notably, a sharp decrease in selectivity for ester formation with increasing molecular weight to favor the aldehyde due to van der Waals interactions of reaction intermediates with the surface was predicted and subsequently verified quantitatively by experiment.
View Article and Find Full Text PDFBackground And Purpose: The purpose was to determine the test-retest reliability, practice effects, convergent validity and sensitivity to multiple sclerosis (MS) disability of neuroperformance subtests from the patient self-administered Multiple Sclerosis Performance Test (MSPT) designed to assess low contrast vision (Contrast Sensitivity Test, CST), upper extremity motor function (Manual Dexterity Test, MDT) and lower extremity motor function (Walking Speed Test, WST) and to introduce the concept of regression-based norms to aid clinical interpretation of performance scores using the MSPT cognition test (Processing Speed Test, PST) as an example.
Methods: Substudy 1 assessed test-retest reliability, practice effects and convergent validity of the CST, MDT and WST in 30 MS patients and 30 healthy controls. Substudy 2 examined sensitivity to MS disability in over 600 MS patients as part of their routine clinic assessment.
Introduction: In the clinic, the assessment of patients with multiple sclerosis (MS) is typically qualitative and non-standardized.
Objectives: To describe the MS Performance Test (MSPT), an iPad Air 2 (Apple, Cupertino, CA, USA)-based neurological assessment platform allowing patients to input relevant information without the aid of a medical technician, creating a longitudinal, clinically meaningful, digital medical record. To report results from human factor (HF) and usability studies, and the initial large-scale implementation in a practice setting.