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1.
J Am Chem Soc ; 146(26): 17613-17617, 2024 Jul 03.
Artigo em Inglês | MEDLINE | ID: mdl-38885442

RESUMO

Synthesis of high-entropy oxide (HEO) nanocrystals has focused on increasing the temperature in the entropy term (T(ΔS)) to overcome the enthalpy term. However, these high temperatures lead to large, polydisperse nanocrystals. In this work, we leverage the low solubility product (Ksp) of metal oxides and optimize the Lewis-acid-catalyzed esterification reaction for equal rate production of the cation monomers to synthesize HEO nanocrystals at low temperatures, producing the smallest (<4 nm) and most monodisperse (<15% size dispersity) HEOs to date. We apply these HEO nanocrystals as electrocatalysts, exhibiting promising activity toward the oxygen evolution reaction in alkaline media, with an overpotential of 345 mV at 10 mA/cm2.

2.
Nat Commun ; 15(1): 3555, 2024 Apr 26.
Artigo em Inglês | MEDLINE | ID: mdl-38670945

RESUMO

Measuring the three-dimensional (3D) distribution of chemistry in nanoscale matter is a longstanding challenge for metrological science. The inelastic scattering events required for 3D chemical imaging are too rare, requiring high beam exposure that destroys the specimen before an experiment is completed. Even larger doses are required to achieve high resolution. Thus, chemical mapping in 3D has been unachievable except at lower resolution with the most radiation-hard materials. Here, high-resolution 3D chemical imaging is achieved near or below one-nanometer resolution in an Au-Fe3O4 metamaterial within an organic ligand matrix, Co3O4-Mn3O4 core-shell nanocrystals, and ZnS-Cu0.64S0.36 nanomaterial using fused multi-modal electron tomography. Multi-modal data fusion enables high-resolution chemical tomography often with 99% less dose by linking information encoded within both elastic (HAADF) and inelastic (EDX/EELS) signals. We thus demonstrate that sub-nanometer 3D resolution of chemistry is measurable for a broad class of geometrically and compositionally complex materials.

3.
ACS Appl Mater Interfaces ; 16(14): 17757-17765, 2024 Apr 10.
Artigo em Inglês | MEDLINE | ID: mdl-38535523

RESUMO

Controllable synthesis of homochiral nano/micromaterials has been a constant challenge for fabricating various stimuli-responsive chiral sensors. To provide an avenue to this goal, we report electrospinning as a simple and economical strategy to form continuous homochiral microfibers with strain-sensitive chiroptical properties. First, electrospun homochiral microfibers from self-assembled cadmium sulfide (CdS) quantum dot magic-sized clusters (MSCs) are produced. Highly sensitive and reversible strain sensors are then fabricated by embedding these chiroptically active fibers into elastomeric films. The chiroptical response on stretching is indicated quantitatively as reversible changes in magnitude, spectral position (wavelength), and sign in circular dichroism (CD) and linear dichroism (LD) signals and qualitatively as a prominent change in the birefringence features under cross-polarizers. The observed periodic twisted helical fibrils at the surface of fibers provide insights into the origin of the fibers' chirality. The measurable shifts in CD and LD are caused by elastic deformations of these helical fibrillar structures of the fiber. To elucidate the origin of these chiroptical properties, we used field emission-electron microscopy (FE-SEM), atomic force microscopy (AFM), synchrotron X-ray analysis, polarized optical microscopy, as well as measurements to isolate the true CD, and contributions from photoelastic modulators (PEM) and LD. Our findings thus offer a promising strategy to fabricate chiroptical strain-sensing devices with multiple measurables/observables using electric-field-assisted spinning of homochiral nano/microfibers.

4.
ACS Mater Au ; 3(5): 501-513, 2023 Sep 13.
Artigo em Inglês | MEDLINE | ID: mdl-38089098

RESUMO

The thiospinel group of nickel cobalt sulfides (NixCo3-xS4) are promising materials for energy applications such as supercapacitors, fuel cells, and solar cells. Solution-processible nanoparticles of NixCo3-xS4 have advantages of low cost and fabrication of high-performance energy devices due to their high surface-to-volume ratio, which increases the electrochemically active surface area and shortens the ionic diffusion path. The current approaches to synthesize NixCo3-xS4 nanoparticles are often based on hydrothermal or solvothermal methods that are difficult to scale up safely and efficiently and that preclude monitoring the reaction through aliquots, making optimization of size and dispersity challenging, typically resulting in aggregated nanoparticles with polydisperse sizes. In this work, we report a scalable "heat-up" method to colloidally synthesize NixCo3-xS4 nanoparticles that are smaller than 15 nm in diameter with less than 15% in size dispersion, using two inexpensive, earth-abundant sulfur sources. Our method provides a reliable synthetic pathway to produce phase-pure, low-dispersity, gram-scale nanoparticles of ternary metal sulfides. This method enhances the current capabilities of NixCo3-xS4 nanoparticles to meet the performance demands to improve renewable energy technologies.

5.
J Am Chem Soc ; 145(31): 17406-17419, 2023 Aug 09.
Artigo em Inglês | MEDLINE | ID: mdl-37525439

RESUMO

While certain ternary spinel oxides have been well-explored with colloidal nanochemistry, notably the ferrite spinel family, ternary manganese (Mn)-based spinel oxides have not been tamed. A key composition is cobalt (Co)-Mn oxide (CMO) spinel, CoxMn3-xO4, that, despite exemplary performance in multiple electrochemical applications, has few reports in the colloidal literature. Of these reports, most show aggregated and polydisperse products. Here, we describe a synthetic method for small, colloidally stable CMO spinel nanocrystals with tunable composition and low dispersity. By reacting 2+ metal-acetylacetonate (M(acac)2) precursors in an amine solvent under an oxidizing environment, we developed a pathway that avoids the highly reducing conditions of typical colloidal synthesis reactions; these reducing conditions typically push the system toward a monoxide impurity phase. Through surface chemistry studies, we identify organic byproducts and their formation mechanism, enabling us to engineer the surface and obtain colloidally stable nanocrystals with low organic loading. We report a CMO/carbon composite with low organic contents that performs the oxygen reduction reaction (ORR) with a half-wave potential (E1/2) of 0.87 V vs RHE in 1.0 M potassium hydroxide at 1600 rpm, rivaling previous reports for the highest activity of this material in ORR electrocatalysis. We extend the general applicability of this procedure to other Mn-based spinel nanocrystals such as Zn-Mn-O, Fe-Mn-O, Ni-Mn-O, and Cu-Mn-O. Finally, we show the scalability of this method by producing inorganic nanocrystals at the gram scale.

6.
J Chem Phys ; 159(1)2023 Jul 07.
Artigo em Inglês | MEDLINE | ID: mdl-37409702

RESUMO

Cation exchange is a versatile post-synthetic method to explore a wide range of nanoparticle compositions, phases, and morphologies. Recently, several studies have expanded the scope of cation exchange to magic-size clusters (MSCs). Mechanistic studies indicated that MSC cation exchange undergoes a two-stage reaction pathway instead of the continuous diffusion-controlled mechanism found in nanoparticle cation exchange reactions. The cation exchange intermediate, however, has not been well-identified despite it being the key to understanding the reaction mechanism. Only indirect evidence, such as exciton peak shifts and powder x-ray diffraction, has been used to indicate the formation of the cation exchange intermediate. In this paper, we investigate the unusual nature of cation exchange in nanoclusters using our previously reported CdS MSC. High-resolution mass spectra reveal two cation exchanged reaction intermediates [Ag2Cd32S33(L) and AgCd33S33(L), L: oleic acid] as well as the fully exchanged Ag2S cluster. Crystal and electronic structure characterizations also confirm the two-stage reaction mechanism. Additionally, we investigate the Cu/CdS MSC cation exchange reaction and find a similar two-stage reaction mechanism. Our study shows that the formation of dilutely exchanged intermediate clusters can be generally found in the first stage of the MSC cation exchange reaction. By exchanging different cations, these intermediate clusters can access varying properties compared to their unexchanged counterparts.

7.
Chirality ; 35(11): 846-855, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-37331723

RESUMO

Chiral materials with strong linear anisotropies are difficult to accurately characterize with circular dichroism (CD) because of artifactual contributions to their spectra from linear dichroism (LD) and birefringence (LB). Historically, researchers have used a second-order Taylor series expansion on the Mueller matrix to model the LDLB interaction effects on the spectra in conventional materials, but this approach may no longer be sufficient to account for the artifactual CD signals in emergent materials. In this work, we present an expression to model the measured CD using a third-order expansion, which introduces "pairwise interference" terms that, unlike the LDLB terms, cannot be averaged out of the signal. We find that the third-order pairwise interference terms can make noticeable contributions to the simulated CD spectra. Using numerical simulations of the measured CD across a broad range of linear and chiral anisotropy parameters, the LDLB interactions are most prominent in samples that have strong linear anisotropies (LD, LB) but negligible chiral anisotropies, where the measured CD strays from the chirality-induced CD by factors greater than 103 . Additionally, the pairwise interactions are most significant in systems with moderate-to-strong chiral and linear anisotropies, where the measured CD is inflated twofold, a figure that grows as linear anisotropies approach their maximum. In summary, media with moderate-to-strong linear anisotropy are in great danger of having their CD altered by these effects in subtle manners. This work highlights the significance of considering distortions in CD measurements through higher-order pairwise interference effects in highly anisotropic nanomaterials.

8.
ACS Nano ; 16(12): 20457-20469, 2022 Dec 27.
Artigo em Inglês | MEDLINE | ID: mdl-36395373

RESUMO

Chiroptically active, hierarchically structured materials are difficult to accurately characterize due to linear anisotropic contributions (i.e., linear dichroism (LD) and linear birefringence (LB)) and parasitic ellipticities that produce artifactual circular dichroism (CD) signals, in addition to chiral analyte contributions ranging from molecular-scale clusters to micron-sized assemblies. Recently, we have shown that CdS magic-sized clusters (MSC) can self-assemble into ordered films that have a hierarchical structure spanning seven orders of length-scale. These films have a strong CD response, but the chiral origins are obfuscated by the hierarchical architecture and LDLB contributions. Here, we derive and demonstrate a method for extracting the "pure" CD signal (CD generated by structural dissymmetry) from hierarchical MSC films and identified the chiral origin. The theory behind the method is derived using Mueller matrix and Stokes vector conventions and verified experimentally before being applied to hierarchical MSC and nanoparticle films with varying macroscopic orderings. Each film's extracted "true CD" shares a bisignate profile aligned with the exciton peak, indicating the assemblies adopt a chiral arrangement and form an exciton coupled system. Interestingly, the linearly aligned MSC film possesses one of the highest g-factors (0.05) among semiconducting nanostructures reported. Additionally, we find that films with similar electronic transition dipole alignment can possess greatly different g-factors, indicating chirality change rather than anisotropy is the cause of the difference in the CD signal. The difference in g-factor is controllable via film evaporation geometry. This study provides a simple means to measure "true" CD and presents an example of experimentally understanding chiroptic interactions in hierarchical nanostructures.

9.
Nat Mater ; 21(5): 518-525, 2022 05.
Artigo em Inglês | MEDLINE | ID: mdl-35422509

RESUMO

Spontaneous hierarchical self-organization of nanometre-scale subunits into higher-level complex structures is ubiquitous in nature. The creation of synthetic nanomaterials that mimic the self-organization of complex superstructures commonly seen in biomolecules has proved challenging due to the lack of biomolecule-like building blocks that feature versatile, programmable interactions to render structural complexity. In this study, highly aligned structures are obtained from an organic-inorganic mesophase composed of monodisperse Cd37S18 magic-size cluster building blocks. Impressively, structural alignment spans over six orders of magnitude in length scale: nanoscale magic-size clusters arrange into a hexagonal geometry organized inside micrometre-sized filaments; self-assembly of these filaments leads to fibres that then organize into uniform arrays of centimetre-scale bands with well-defined surface periodicity. Enhanced patterning can be achieved by controlling processing conditions, resulting in bullseye and 'zigzag' stacking patterns with periodicity in two directions. Overall, we demonstrate that colloidal nanomaterials can exhibit a high level of self-organization behaviour at macroscopic-length scales.


Assuntos
Nanoestruturas , Nanoestruturas/química
10.
J Chem Phys ; 155(14): 144702, 2021 Oct 14.
Artigo em Inglês | MEDLINE | ID: mdl-34654287

RESUMO

Efforts to improve energy storage depend greatly on the development of efficient electrode materials. Recently, strain has been employed as an alternate approach to improve ion mobility. While lattice strain has been well-researched in catalytic applications, its effects on electrochemical energy storage are largely limited to computational studies due to complexities associated with strain control in nanomaterials as well as loss of strain due to the phase change of the active material during charging-discharging. In this work, we overcome these challenges and investigate the effects of strain on supercapacitor performance in Li-ion-based energy devices. We synthesize epitaxial Fe3O4@MnFe2O4 (core@shell) nanoparticles with varying shell thickness to control the lattice strain. A narrow voltage window for electrochemical testing is used to limit the storage mechanism to lithiation-delithiation, preventing a phase change and maintaining structural strain. Cyclic voltammetry reveals a pseudocapacitive behavior and similar levels of surface charge storage in both strained- and unstrained-MnFe2O4 samples; however, diffusive charge storage in the strained sample is twice as high as the unstrained sample. The strained-MnFe2O4 electrode exceeds the performance of the unstrained-MnFe2O4 electrode in energy density by ∼33%, power density by ∼28%, and specific capacitance by ∼48%. Density functional theory shows lower formation energies for Li-intercalation and lower activation barrier for Li-diffusion in strained-MnFe2O4, corresponding to a threefold increase in the diffusion coefficient. The enhanced Li-ion diffusion rate in the strained-electrodes is further confirmed using the galvanostatic intermittent titration technique. This work provides a starting point to using strain engineering as a novel approach for designing high performance energy storage devices.

11.
Clin Exp Emerg Med ; 8(1): 55-64, 2021 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-33845524

RESUMO

OBJECTIVE: Burnout is a common occurrence among healthcare providers and has been associated with provider wellness culture. However, this association has not been extensively studied among emergency medicine (EM) providers. We aim to determine the association between EM provider burnout and their culture of wellness, and to elicit the independent wellness culture domains most predictive of burnout prevention. METHODS: This was a multi-center observational study. We enrolled EM physicians and advanced practice providers from sixteen different emergency departments (EDs). Provider wellness culture and burnout surveys were performed. The wellness culture domains included in this study are personal/organizational value alignment, provider appreciation, leadership quality, self-controlled scheduling, peer support, and family support. Correlations between each wellness culture domain and burnout were analyzed by Pearson correlation co-efficiency, and their associations were measured by multivariate logistic regression with adjustments of other confounders. RESULTS: A total of 242 ED provider surveys were entered for final analysis. The overall burnout rate was 54% (130/242). Moderate correlations were found between burnout and two wellness culture domains (value alignment: r=-0.43, P<0.001 and provider appreciation: r=-0.49, P<0.001). The adjusted odds ratio of provider appreciation associated with burnout was 0.44 (95% confidence interval, 0.25-0.77; P=0.004), adjusted odds ratio of family support was 0.67 (95% confidence interval, 0.48-0.95; P=0.025). CONCLUSION: ED providers have a relatively high burnout rate. Provider burnout might have certain associations with wellness culture domains. Provider appreciation and family support seem to play important roles in burnout protection.

12.
Acc Chem Res ; 54(3): 509-519, 2021 Feb 02.
Artigo em Inglês | MEDLINE | ID: mdl-33434011

RESUMO

ConspectusChemically induced transformations are postsynthetic processing reactions applied to first generation (as-synthesized) nanomaterials to modify property-defining factors such as atomic structure, chemical composition, surface chemistry, and/or morphology. Compared with conditions for direct synthesis of colloidal nanocrystals, postsynthetic chemical transformations can be conducted in relatively mild conditions with a more controllable process, which makes them suitable for the precise manipulation of nanomaterials and for trapping metastable phases that are typically inaccessible from the conventional synthetic routes. Each of the chemically induced transformations methods can result in substantial restructuring of the atomic structure, but their transformation pathways can be very different. And the converse is also true: the atomic structure of the parent material plays a large role in the pathway toward and the resulting chemically transformed product. Additionally, the characteristic length of the parent material greatly affects the structure, which affects the outcome of the reaction.In this Account, we show how the atomic structure and nanoscale size directs the product formation into materials that are inaccessible from analogous chemically transformations in bulk materials. Through examples from the three chemical transformation processes (cation/anion exchange, redox reactions, and ligand exchange and ligand etching), the effect of the atomic structure on chemical transformations is made apparent, and vice versa. For cation exchange, an anisotropic atomic lattice results in a unidirectional exchange boundary. And because the interface can extend through the full crystal, a substantial strain field can form, influencing the phase of the material. In the redox reaction that leads to the nanoscale Kirkendall effect, the atomic structure is the key to inverting the diffusion rates in a diffusion couple to form the hollow cores. And for ligand etching, if one of the materials in a heterostructure has a defected and\or defect-tolerant atomic structure, it can be preferentially etched and its atomic structure can undergo phase transformations while the other composition remains intact. For length scales, we show how the chemically induced transformations greatly differ between bulk, nanocrystal, and nanocluster characteristic sizes. For instance, the structural transformation on relatively large nanocrystals (2-100 nm) can be a continuous process when the activation volume is smaller than the nanocrystal, while for smaller nanoclusters (<2 nm) the transformation kinetics could be swift resulting in only discrete thermodynamic states. Comparing the two nanosystems (nanocrystals to small nanoclusters), we address how their atomic structural differences can direct the divergent transformation phenomena and the corresponding mechanisms. Understanding the nanoscale mechanisms of chemically induced transformations and how they differ from bulk processes is key to unlocking new science and for implementing this processing for functional materials.

13.
Adv Mater ; 32(49): e2004490, 2020 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-33084168

RESUMO

The small-polaron hopping model has been used for six decades to rationalize electronic charge transport in oxides. The model was developed for binary oxides, and, despite its significance, its accuracy has not been rigorously tested for higher-order oxides. Here, the small-polaron transport model is tested by using a spinel system with mixed cation oxidation states (Mnx Fe3- x O4 ). Using molecular-beam epitaxy (MBE), a series of single crystal Mnx Fe3- x O4 thin films with controlled stoichiometry, 0 ≤ x ≤ 2.3, and lattice strain are grown, and the cation site-occupation is determined through X-ray emission spectroscopy (XES). Density functional theory + U analysis shows that charge transport occurs only between like-cations (Fe/Fe or Mn/Mn). The site-occupation data and percolation models show that there are limited stoichiometric ranges for transport along Fe and Mn pathways. Furthermore, due to asymmetric hopping barriers and formation energies, the Mn O h 2 + polaron is energetically preferred to the Fe O h 2 + polaron, resulting in an asymmetric contribution of Mn/Mn pathways. All of these findings are not contained in the conventional small-polaron hopping model, highlighting its inadequacy. To correct the model, new parameters in the nearest-neighbor hopping equation are introduced to account for percolation, cross-hopping, and polaron-distribution, and it is found that a near-perfect correlation can be made between experiment and theory for the electronic conductivity.

14.
J Am Chem Soc ; 142(34): 14495-14503, 2020 08 26.
Artigo em Inglês | MEDLINE | ID: mdl-32786802

RESUMO

Self-assembly of three-dimensional structures with order across multiple length scales-hierarchical assembly-is of great importance for biomolecules for the functions of life. Creation of similar complex architectures from inorganic building blocks has been pursued toward artificial biomaterials and advanced functional materials. Current research, however, primarily employs only large, nonreactive building blocks such as Au colloids. By contrast, sulfur-bridged transition metal clusters (<2 nm) are able to offer more functionality in catalytic and biochemical reactions. Hierarchical assembly of these systems has not been well researched because of the difficulty in obtaining single-phase clusters and the lack of suitable ligands to direct structure construction. To overcome these challenges, we employ a rigid planar ligand with an aromatic ring and bifunctional bond sites. We demonstrate the synthesis and assembly of 1.2 nm sulfur-bridged copper (SB-Cu) clusters with tertiary hierarchical complexity. The primary structure is clockwise/counterclockwise chiral cap and core molecules. They combine to form clusters, and due to the cap-core interaction (C-H···π), only two enantiomeric isomers are formed (secondary structure). A tertiary hierarchical architecture is achieved through the self-assembly of alternating enantiomers with hydrogen bonds as the intermolecular driving force. The SB-Cu clusters are air stable and have a distribution of oxidation states ranging from Cu(0) to Cu(I), making them interesting for redox and catalytic activities. This study shows that structural complexity at different length scales, mimicking biomolecules, can occur in active-metal clusters and provides a new platform for investigation of those systems and for the design of advanced functional materials.

15.
Obes Res Clin Pract ; 14(4): 350-359, 2020.
Artigo em Inglês | MEDLINE | ID: mdl-32684413

RESUMO

BACKGROUND: An obesity survival paradox has been reported among obese patients with pneumonia. AIMS: To determine the impact of obesity on pneumonia outcomes and analyze the correlation between in-hospital all-cause mortality and obesity among patients with pneumonia. METHODS: The United States Nationwide Readmissions Database (NRD) was retrospectively analyzed for patients with pneumonia from 2013 to 2014. We used a step-wise restricted and propensity score matching cohort model (dual model) to compare mortality rates and other outcomes among pneumonia patients based on BMI. Mortality was calculated by a Cox proportional hazard model, adjusted for potential confounders with propensity score matched analysis. RESULTS: A total of 70,886,775 patients were registered in NRD during the study period. Of these, 7,786,913 patients (11.0%) were considered obese and 1,652,456 patients (2.3%) were admitted to the hospital with pneumonia. Based on the step-wise restricted cohort model, the hazard ratio comparing the mortality rates among obese pneumonia patients to mortality rates among normal BMI pneumonia patients was 0.75 (95% CI 0.60-0.94). The propensity score matched analysis estimated a hazard rate of 0.84 (95% CI 0.79-0.90) and the hazard ratio estimated from the dual model was 0.82 (95% CI 0.63-1.07). CONCLUSIONS: With the application of a dual model, there appears to be no significant difference in mortality of obese patients with pneumonia compared to normal BMI patients with pneumonia.


Assuntos
Obesidade , Pneumonia , Índice de Massa Corporal , Estudos de Coortes , Humanos , Obesidade/complicações , Obesidade/mortalidade , Pneumonia/complicações , Pneumonia/mortalidade , Modelos de Riscos Proporcionais , Estudos Retrospectivos , Estados Unidos
16.
PLoS One ; 15(2): e0228719, 2020.
Artigo em Inglês | MEDLINE | ID: mdl-32023302

RESUMO

BACKGROUND AND OBJECTIVE: Attending physician productivity and efficiency can be affected when working simultaneously with Residents. To gain a better understanding of this effect, we aim to compare productivity, efficiency, and overall performance differences among Attendings working solo versus working with Residents in an Emergency Department (ED). METHODS: Data were extracted from the electronic medical records of all patients seen by ED Attendings and/or Residents during the period July 1, 2014 through June 30, 2017. Attending productivity was measured based on the number of new patients enrolled per hour per provider. Attending efficiency was measured based on the provider-to-disposition time (PDT). Attending overall performance was measured by Attending Performance Index (API). Furthermore, Attending productivity, efficiency, and overall performance metrics were compared between Attendings working solo and Attendings working with Residents. The comparisons were analyzed after adjusting for confounders via propensity score matching. RESULTS: A total of 15 Attendings and 266 Residents managing 111,145 patient encounters over the study period were analyzed. The mean (standard deviation) of Attending productivity and efficiency were 2.9 (1.6) new patients per hour and 2.7 (1.8) hours per patient for Attendings working solo, in comparison to 3.3 (1.9) and 3.0 (2.0) for Attendings working with Residents. When paired with Residents, the API decreased for those Attendings who had a higher API when working solo (average API dropped from 0.21 to 0.19), whereas API increased for those who had a lower API when working solo (average API increased from 0.13 to 0.16). CONCLUSION: In comparison to the Attending working solo staffing model, increased productivity with decreased efficiency occurred among Attendings when working with Residents. The overall performance of Attendings when working with Residents varied inversely against their performance when working solo.


Assuntos
Eficiência , Serviço Hospitalar de Emergência/estatística & dados numéricos , Internato e Residência , Corpo Clínico Hospitalar/estatística & dados numéricos , Admissão e Escalonamento de Pessoal , Feminino , Humanos , Masculino , Corpo Clínico Hospitalar/psicologia , Estudos Retrospectivos
17.
Obes Res Clin Pract ; 13(6): 561-570, 2019.
Artigo em Inglês | MEDLINE | ID: mdl-31635969

RESUMO

BACKGROUND: An obesity survival paradox has been reported among obese patients with pneumonia. AIMS: To determine the impact of obesity on pneumonia outcomes and analyze the correlation between in-hospital all-cause mortality and obesity among patients with pneumonia. METHODS: The United States Nationwide Readmissions Database (NRD) was retrospectively analyzed for patients with pneumonia from 2013 to 2014. We used a step-wise restricted and propensity score matching cohort model (dual model) to compare mortality rates and other outcomes among pneumonia patients based on BMI. Mortality was calculated by a Cox proportional hazard model, adjusted for potential confounders with propensity score matched analysis. RESULTS: A total of 70,886,775 patients were registered in NRD during the study period. Of these, 7,786,913 patients (11.0%) were considered obese and 1,652,456 patients (2.3%) were admitted to the hospital with pneumonia. Based on the step-wise restricted cohort model, the hazard ratio comparing the mortality rates among obese pneumonia patients to mortality rates among normal BMI pneumonia patients was 0.75 (95% CI 0.60-0.94). The propensity score matched analysis estimated a hazard rate of 0.84 (95% CI 0.79-0.90) and the hazard ratio estimated from the dual model was 0.82 (95% CI 0.63-1.07). CONCLUSIONS: With the application of a dual model, there appears to be no significant difference in mortality of obese patients with pneumonia compared to normal BMI patients with pneumonia.


Assuntos
Obesidade/mortalidade , Pneumonia/mortalidade , Adolescente , Adulto , Idoso , Idoso de 80 Anos ou mais , Estudos de Coortes , Comorbidade , Bases de Dados Factuais , Feminino , Mortalidade Hospitalar , Humanos , Masculino , Pessoa de Meia-Idade , Modelos Teóricos , Reprodutibilidade dos Testes , Estudos Retrospectivos , Fatores de Risco , Análise de Sobrevida , Estados Unidos/epidemiologia , Adulto Jovem
18.
AEM Educ Train ; 3(3): 209-217, 2019 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-31360813

RESUMO

OBJECTIVES: Provider efficiency has been reported in the literature but there is a lack of efficiency analysis among emergency medicine (EM) residents. We aim to compare efficiency of EM residents of different training levels and determine if EM resident efficiency is affected by emergency department (ED) crowding. METHODS: We conducted a single-center retrospective observation study from July 1, 2014, to June 30, 2017. The number of new patients per resident per hour and provider-to-disposition (PTD) time of each patient were used as resident efficiency markers. A crowding score was assigned to each patient upon the patient's arrival to the ED. We compared efficiency among EM residents of different training levels under different ED crowding statuses. Dynamic efficiency changes were compared monthly through the entire academic year (July to next June). RESULTS: The study enrolled a total of 150,920 patients. A mean of 1.9 patients/hour was seen by PGY-1 EM residents in comparison to 2.6 patients/hour by PGY-2 and -3 EM residents. Median PTD was 2.8 hours in PGY-1 EM residents versus 2.6 hours in PGY-2 and -3 EM residents. There were no significant differences in acuity across all patients seen by EM residents. When crowded conditions existed, residency efficiency increased, but such changes were minimized when the ED became overcrowded. A linear increase of resident efficiency was observed only in PGY-1 EM residents throughout the entire academic year. CONCLUSION: Resident efficiency improved significantly only during their first year of EM training. This efficiency can be affected by ED crowding.

19.
BMC Health Serv Res ; 19(1): 451, 2019 Jul 04.
Artigo em Inglês | MEDLINE | ID: mdl-31272442

RESUMO

BACKGROUND: It is critical to understand whether providing health insurance coverage, assigning a dedicated Primary Care Physician (PCP), and arranging timely post-Emergency Department (ED) clinic follow-up can improve compliance with clinic visits and reduce ED discharge failures. We aim to determine the benefits of providing these common step-wise interventions and further investigate the necessity of urgent PCP referrals on behalf of ED discharged patients. METHODS: This is a single-center retrospective observational study. All patients discharged from the ED over the period Jan 1, 2015 through Dec 31, 2017 were included in the study population. Step-wise interventions included providing charity health insurance, assigning a dedicated PCP, and providing ED follow-up clinics. PCP clinic compliance and ED discharge failures were measured and compared among groups receiving different interventions. RESULT: A total of 227,627 patients were included. Fifty-eight percent of patients receiving charity insurance had PCP visits in comparison to 23% of patients without charity insurance (p < 0.001). Seventy-seven percent of patients with charity insurance and PCP assignments completed post-ED discharge PCP visits in comparison to only 4.5% of those with neither charity insurance nor PCP assignments (p < 0.001). CONCLUSIONS: Step-wise interventions increased patient clinic follow-up compliance while simultaneously reducing ED discharge failures. Such interventions might benefit communities with similar patient populations.


Assuntos
Assistência Ambulatorial/estatística & dados numéricos , Serviço Hospitalar de Emergência/estatística & dados numéricos , Alta do Paciente/estatística & dados numéricos , Adulto , Feminino , Humanos , Masculino , Pessoa de Meia-Idade , Cooperação do Paciente , Melhoria de Qualidade , Estudos Retrospectivos
20.
BMJ Open ; 9(6): e028051, 2019 06 27.
Artigo em Inglês | MEDLINE | ID: mdl-31248927

RESUMO

OBJECTIVES: Identifying patients who are at high risk for discharge failure allows for implementation of interventions to improve their care. However, discharge failure is currently defined in literature with great variability, making targeted interventions more difficult. We aim to derive a screening tool based on the existing diverse discharge failure models. DESIGN, SETTING AND PARTICIPANTS: This is a single-centre retrospective cohort study in the USA. Data from all patients discharged from the emergency department were collected from 1 January 2015 through 31 December 2017 and followed up within 30 days. METHODS: Scoring systems were derived using modified Framingham methods. Sensitivity, specificity and area under the receiver operational characteristic (AUC) were calculated and compared using both the broad and restricted discharge failure models. RESULTS: A total of 227 627 patients were included. The Screening for Healthcare fOllow-Up Tool (SHOUT) scoring system was derived based on the broad and restricted discharge failure models and applied back to the entire study cohort. A sensitivity of 80% and a specificity of 71% were found in SHOUT scores to identify patients with broad discharge failure with AUC of 0.83 (95% CI 0.83 to 0.84). When applied to a 3-day restricted discharge failure model, a sensitivity of 86% and a specificity of 60% were found to identify patients with AUC of 0.79 (95% CI 0.78 to 0.80). CONCLUSION: The SHOUT scoring system was derived and used to screen and identify patients that would ultimately become discharge failures, especially when using broad definitions of discharge failure. The SHOUT tool was internally validated and can be used to identify patients across a wide spectrum of discharge failure definitions.


Assuntos
Serviço Hospitalar de Emergência/normas , Alta do Paciente/estatística & dados numéricos , Assistência ao Convalescente/normas , Assistência ao Convalescente/estatística & dados numéricos , Feminino , Hospitais Urbanos , Humanos , Tempo de Internação/estatística & dados numéricos , Masculino , Estudos Retrospectivos , Fatores de Risco , Centros de Atenção Terciária , Estados Unidos
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