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1.
Proc Natl Acad Sci U S A ; 121(19): e2318652121, 2024 May 07.
Artigo em Inglês | MEDLINE | ID: mdl-38687781

RESUMO

Water oxidation on magnetic catalysts has generated significant interest due to the spin-polarization effect. Recent studies have revealed that the disappearance of magnetic domain wall upon magnetization is responsible for the observed oxygen evolution reaction (OER) enhancement. However, an atomic picture of the reaction pathway remains unclear, i.e., which reaction pathway benefits most from spin-polarization, the adsorbent evolution mechanism, the intermolecular mechanism (I2M), the lattice oxygen-mediated one, or more? Here, using three model catalysts with distinguished atomic chemistries of active sites, we are able to reveal the atomic-level mechanism. We found that spin-polarized OER mainly occurs at interconnected active sites, which favors direct coupling of neighboring ligand oxygens (I2M). Furthermore, our study reveals the crucial role of lattice oxygen participation in spin-polarized OER, significantly facilitating the coupling kinetics of neighboring oxygen radicals at active sites.

2.
Chem Rev ; 123(23): 13489-13692, 2023 Dec 13.
Artigo em Inglês | MEDLINE | ID: mdl-37962496

RESUMO

As a key structural parameter, phase depicts the arrangement of atoms in materials. Normally, a nanomaterial exists in its thermodynamically stable crystal phase. With the development of nanotechnology, nanomaterials with unconventional crystal phases, which rarely exist in their bulk counterparts, or amorphous phase have been prepared using carefully controlled reaction conditions. Together these methods are beginning to enable phase engineering of nanomaterials (PEN), i.e., the synthesis of nanomaterials with unconventional phases and the transformation between different phases, to obtain desired properties and functions. This Review summarizes the research progress in the field of PEN. First, we present representative strategies for the direct synthesis of unconventional phases and modulation of phase transformation in diverse kinds of nanomaterials. We cover the synthesis of nanomaterials ranging from metal nanostructures such as Au, Ag, Cu, Pd, and Ru, and their alloys; metal oxides, borides, and carbides; to transition metal dichalcogenides (TMDs) and 2D layered materials. We review synthesis and growth methods ranging from wet-chemical reduction and seed-mediated epitaxial growth to chemical vapor deposition (CVD), high pressure phase transformation, and electron and ion-beam irradiation. After that, we summarize the significant influence of phase on the various properties of unconventional-phase nanomaterials. We also discuss the potential applications of the developed unconventional-phase nanomaterials in different areas including catalysis, electrochemical energy storage (batteries and supercapacitors), solar cells, optoelectronics, and sensing. Finally, we discuss existing challenges and future research directions in PEN.

3.
Alzheimers Dement ; 20(4): 2516-2525, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38329281

RESUMO

INTRODUCTION: The objective of this study is to investigate the incremental value of amyloid positron emission tomography (Aß-PET) in a tertiary memory clinic setting in China. METHODS: A total of 1073 patients were offered Aß-PET using 18F-florbetapir. The neurologists determined a suspected etiology (Alzheimer's disease [AD] or non-AD) with a percentage estimate of their confidence and medication prescription both before and after receiving the Aß-PET results. RESULTS: After disclosure of the Aß-PET results, etiological diagnoses changed in 19.3% of patients, and diagnostic confidence increased from 69.3% to 85.6%. Amyloid PET results led to a change of treatment plan in 36.5% of patients. Compared to the late-onset group, the early-onset group had a more frequent change in diagnoses and a higher increase in diagnostic confidence. DISCUSSION: Aß-PET has significant impacts on the changes of diagnoses and management in Chinese population. Early-onset cases are more likely to benefit from Aß-PET than late-onset cases. HIGHLIGHTS: Amyloid PET contributes to diagnostic changes and its confidence in Chinese patients. Amyloid PET leads to a change of treatment plans in Chinese patients. Early-onset cases are more likely to benefit from amyloid PET than late-onset cases.


Assuntos
Doença de Alzheimer , Disfunção Cognitiva , Humanos , Amiloide , Doença de Alzheimer/diagnóstico por imagem , Tomografia por Emissão de Pósitrons/métodos , Proteínas Amiloidogênicas , Compostos de Anilina , China , Peptídeos beta-Amiloides , Disfunção Cognitiva/diagnóstico
4.
Eur J Nucl Med Mol Imaging ; 50(8): 2394-2408, 2023 07.
Artigo em Inglês | MEDLINE | ID: mdl-36929211

RESUMO

PURPOSE: TSPO PET with radioligand [18F]DPA-714 is an emerging molecular imaging technique that reflects cerebral inflammation and microglial activation, and it has been recently used in central nervous system diseases. In this study, we aimed to investigate the neuroinflammation pattern of anti-leucine-rich glioma-inactivated 1 (LGI1) protein autoimmune encephalitis (AIE) and to evaluate its possible correlation with clinical phenotypes. METHODS: Twenty patients with anti-LGI1 encephalitis from the autoimmune encephalitis cohort in Huashan Hospital and ten with other AIE and non-inflammatory diseases that underwent TSPO PET imaging were included in the current study. Increased regional [18F]DPA-714 retention in anti-LGI1 encephalitis was detected on a voxel basis using statistic parametric mapping analysis. Multiple correspondence analysis and hierarchical clustering were conducted for discriminate subgroups in anti-LGI1 encephalitis. Standardized uptake value ratios normalized to the cerebellum (SUVRc) were calculated for semiquantitative analysis of TSPO PET features between different LGI1-AIE subgroups. RESULTS: Increased regional retention of [18F]DPA-714 was identified in the bilateral hippocampus, caudate nucleus, and frontal cortex in LGI1-AIE patients. Two subgroups of LGI1-AIE patients were distinguished based on the top seven common symptoms. Patients in cluster 1 had a high frequency of facio-brachial dystonic seizures than those in cluster 2 (p = 0.004), whereas patients in cluster 2 had a higher frequency of general tonic-clonic (GTC) seizures than those in cluster 1 (p < 0.001). Supplementary motor area and superior frontal gyrus showed higher [18F]DPA-714 retention in cluster 2 patients compared with those in cluster 1 (p = 0.024; p = 0.04, respectively). CONCLUSIONS: Anti-LGI1 encephalitis had a distinctive molecular imaging pattern presented by TSPO PET scan. LGI1-AIE patients with higher retention of [18F]DPA-714 in the frontal cortex were more prone to present with GTC seizures. Further studies are required for verifying its value in clinical application.


Assuntos
Doenças Autoimunes do Sistema Nervoso , Encefalite , Glioma , Humanos , Doenças Neuroinflamatórias , Leucina , Peptídeos e Proteínas de Sinalização Intracelular , Encefalite/diagnóstico por imagem , Convulsões , Tomografia por Emissão de Pósitrons/métodos , Receptores de GABA
5.
Eur J Nucl Med Mol Imaging ; 51(1): 159-167, 2023 12.
Artigo em Inglês | MEDLINE | ID: mdl-37668706

RESUMO

PURPOSE: The exact phenoconversion time from isolated rapid eye movement (REM) sleep behavior disorder (iRBD) to synucleinopathies remains unpredictable. This study investigated whole-brain dopaminergic damage pattern (DDP) with disease progression and predicted phenoconversion time in individual patients. METHODS: Age-matched 33 iRBD patients and 20 healthy controls with 11C-CFT-PET scans were enrolled. The patients were followed up 2-10 (6.7 ± 2.0) years. The phenoconversion year was defined as the base year, and every 2 years before conversion was defined as a stage. Support vector machine with leave-one-out cross-validation strategy was used to perform prediction. RESULTS: Dopaminergic degeneration of iRBD was found to occur about 6 years before conversion and then abnormal brain regions gradually expanded. Using DDP, area under curve (AUC) was 0.879 (90% sensitivity and 88.3% specificity) for predicting conversion in 0-2 years, 0.807 (72.7% sensitivity and 83.3% specificity) in 2-4 years, 0.940 (100% sensitivity and 84.6% specificity) in 4-6 years, and 0.879 (100% sensitivity and 80.7% specificity) over 6 years. In individual patients, predicted stages correlated with whole-brain dopaminergic levels (r = - 0.740, p < 0.001). CONCLUSION: Our findings suggest that DDP could accurately predict phenoconversion time of individual iRBD patients, which may help to screen patients for early intervention.


Assuntos
Transtorno do Comportamento do Sono REM , Humanos , Transtorno do Comportamento do Sono REM/diagnóstico por imagem , Encéfalo/diagnóstico por imagem , Dopamina , Progressão da Doença
6.
Eur J Nucl Med Mol Imaging ; 50(5): 1395-1405, 2023 04.
Artigo em Inglês | MEDLINE | ID: mdl-36627498

RESUMO

PURPOSE: Human post mortem studies have described the topographical patterns of tau pathology in progressive supranuclear palsy (PSP). Recent advances in tau PET tracers are expected to herald the next era of PSP investigation for early detection of tau pathology in living brains. This study aimed to investigate whether 18F-Florzolotau PET imaging may capture the distribution patterns and regional vulnerability of tau pathology in PSP, and to devise a novel image-based staging system. METHODS: The study cohort consisted of 148 consecutive patients with PSP who had undergone 18F-Florzolotau PET imaging. The PSP rating scale (PSPrs) was used to measure disease severity. Similarities and differences of tau deposition among different clinical phenotypes were examined at the regional and voxel levels. An 18F-Florzolotau pathological staging system was devised according to the scheme originally developed for post mortem data. In light of conditional probabilities for the sequence of events, an 18F-Florzolotau modified staging system by integrating clusters at the regional level was further developed. The ability of 18F-Florzolotau staging systems to reflect disease severity in terms of PSPrs score was assessed by analysis of variance. RESULTS: The distribution patterns of 18F-Florzolotau accumulation in living brains of PSP showed a remarkable similarity to those reported in post mortem studies, with the binding intensity being markedly higher in Richardson's syndrome. Moreover, 18F-Florzolotau PET imaging allowed detecting regional vulnerability and tracking tau accumulation in an earlier fashion compared with post mortem immunostaining. The 18F-Florzolotau staging systems were positively correlated with clinical severity as reflected by PSPrs scores. CONCLUSIONS: 18F-Florzolotau PET imaging can effectively capture the distribution patterns and regional vulnerability of tau pathology in PSP. The 18F-Florzolotau modified staging system holds promise for early tracking of tau deposition in living brains.


Assuntos
Paralisia Supranuclear Progressiva , Humanos , Encéfalo/metabolismo , Tomografia por Emissão de Pósitrons/métodos , Paralisia Supranuclear Progressiva/diagnóstico por imagem , Proteínas tau/metabolismo
7.
Mov Disord ; 38(4): 579-588, 2023 04.
Artigo em Inglês | MEDLINE | ID: mdl-36750757

RESUMO

BACKGROUND: Recent development in tau-sensitive tracers has sparkled significant interest in tracking tauopathies using positron emission tomography (PET) biomarkers. However, the ability of 18 F-florzolotau PET imaging to topographically characterize tau pathology in corticobasal syndrome (CBS) remains unclear. Further, the question as to whether disease-level differences exist with other neurodegenerative tauopathies is still unanswered. OBJECTIVE: To analyze the topographical patterns of tau pathology in the living brains of patients with CBS using 18 F-florzolotau PET imaging and to examine whether differences with other tauopathies exist. METHODS: 18 F-florzolotau PET imaging was performed in 20 consecutive patients with CBS, 20 cognitively healthy controls (HCs), 20 patients with Alzheimer's disease (AD), and 16 patients with progressive supranuclear palsy-Richardson's syndrome (PSP-RS). Cerebrospinal fluid (CSF) levels of ß-amyloid biomarkers were quantified in all patients with CBS. 18 F-florzolotau uptake was quantitatively assessed using standardized uptake value ratios. RESULTS: Of the 20 patients with CBS, 19 (95%) were negative for CSF biomarkers of amyloid pathology; of them, three had negative 18 F-florzolotau PET findings. Compared with HCs, patients with CBS showed increased 18 F-florzolotau signals in both cortical and subcortical regions. In addition, patients with CBS were characterized by higher tracer retentions in subcortical regions compared with those with AD and showed a trend toward higher signals in cortical areas compared with PSP-RS. An asymmetric pattern of 18 F-florzolotau uptake was associated with an asymmetry of motor severity in patients with CBS. CONCLUSIONS: In vivo 18 F-florzolotau PET imaging holds promise for distinguishing CBS in the spectrum of neurodegenerative tauopathies. © 2023 International Parkinson and Movement Disorder Society.


Assuntos
Degeneração Corticobasal , Tomografia por Emissão de Pósitrons , Tauopatias , Humanos , Doença de Alzheimer/diagnóstico por imagem , Encéfalo/diagnóstico por imagem , Encéfalo/patologia , Degeneração Corticobasal/diagnóstico por imagem , Radioisótopos de Flúor , Tomografia por Emissão de Pósitrons/métodos , Paralisia Supranuclear Progressiva/diagnóstico por imagem , Paralisia Supranuclear Progressiva/patologia , Proteínas tau/metabolismo , Tauopatias/diagnóstico por imagem
8.
Angew Chem Int Ed Engl ; 62(26): e202301721, 2023 Jun 26.
Artigo em Inglês | MEDLINE | ID: mdl-37130000

RESUMO

The reaction kinetics of spin-polarized oxygen evolution reaction (OER) can be enhanced by ferromagnetic (FM) catalysts under an external magnetic field. However, applying a magnetic field necessitates additional energy consumption and creates design difficulties for OER. Herein, we demonstrate that a single-domain FM catalyst without external magnetic fields exhibits a similar OER increment to its magnetized multi-domain one. The evidence is given by comparing the pH-dependent increment of OER on multi- and single-domain FM catalysts with or without a magnetic field. The intrinsic activity of a single-domain catalyst is higher than that of a multi-domain counterpart. The latter can be promoted to approach the former by the magnetization effect. Reducing the FM catalyst size into the single-domain region, the spin-polarized OER performance can be achieved without a magnetic field, illustrating an external magnetic field is not a requirement to reap the benefits of magnetic catalysts.


Assuntos
Campos Magnéticos , Oxigênio , Cinética , Oxirredução , Água
9.
Eur J Nucl Med Mol Imaging ; 49(8): 2798-2811, 2022 07.
Artigo em Inglês | MEDLINE | ID: mdl-35588012

RESUMO

PURPOSE: This work attempts to decode the discriminative information in dopamine transporter (DAT) imaging using deep learning for the differential diagnosis of parkinsonism. METHODS: This study involved 1017 subjects who underwent DAT PET imaging ([11C]CFT) including 43 healthy subjects and 974 parkinsonian patients with idiopathic Parkinson's disease (IPD), multiple system atrophy (MSA) or progressive supranuclear palsy (PSP). We developed a 3D deep convolutional neural network to learn distinguishable DAT features for the differential diagnosis of parkinsonism. A full-gradient saliency map approach was employed to investigate the functional basis related to the decision mechanism of the network. Furthermore, deep-learning-guided radiomics features and quantitative analysis were compared with their conventional counterparts to further interpret the performance of deep learning. RESULTS: The proposed network achieved area under the curve of 0.953 (sensitivity 87.7%, specificity 93.2%), 0.948 (sensitivity 93.7%, specificity 97.5%), and 0.900 (sensitivity 81.5%, specificity 93.7%) in the cross-validation, together with sensitivity of 90.7%, 84.1%, 78.6% and specificity of 88.4%, 97.5% 93.3% in the blind test for the differential diagnosis of IPD, MSA and PSP, respectively. The saliency map demonstrated the most contributed areas determining the diagnosis located at parkinsonism-related regions, e.g., putamen, caudate and midbrain. The deep-learning-guided binding ratios showed significant differences among IPD, MSA and PSP groups (P < 0.001), while the conventional putamen and caudate binding ratios had no significant difference between IPD and MSA (P = 0.24 and P = 0.30). Furthermore, compared to conventional radiomics features, there existed average above 78.1% more deep-learning-guided radiomics features that had significant differences among IPD, MSA and PSP. CONCLUSION: This study suggested the developed deep neural network can decode in-depth information from DAT and showed potential to assist the differential diagnosis of parkinsonism. The functional regions supporting the diagnosis decision were generally consistent with known parkinsonian pathology but provided more specific guidance for feature selection and quantitative analysis.


Assuntos
Aprendizado Profundo , Atrofia de Múltiplos Sistemas , Doença de Parkinson , Transtornos Parkinsonianos , Encéfalo/metabolismo , Diagnóstico Diferencial , Proteínas da Membrana Plasmática de Transporte de Dopamina/metabolismo , Humanos , Atrofia de Múltiplos Sistemas/diagnóstico , Atrofia de Múltiplos Sistemas/metabolismo , Atrofia de Múltiplos Sistemas/patologia , Doença de Parkinson/metabolismo , Transtornos Parkinsonianos/diagnóstico por imagem , Tomografia por Emissão de Pósitrons/métodos
10.
Mov Disord ; 37(9): 1861-1871, 2022 09.
Artigo em Inglês | MEDLINE | ID: mdl-35857319

RESUMO

BACKGROUND: Whether dementia with Lewy bodies (DLB) and Parkinson's disease (PD) dementia (PDD) represent the same disease, distinct entities, or conditions within the same spectrum remains controversial. OBJECTIVE: The objective of this study was to provide new insight into this debate by separately identifying disease-specific metabolic patterns and comparing them with each other and with previously established PD-related pattern (PDRP). METHODS: Patients with DLB (n = 67), patients with PDD (n = 50), and healthy control subjects (HCs; n = 15) with brain 18 F-fluorodeoxyglucose positron emission tomography were enrolled as cohorts A and B for pattern identification and validation, respectively. Patients with PD (n = 30) were included for discrimination. Twenty-one participants had two scans. The principal component analysis was applied for pattern identification (DLB-related pattern [DLBRP], PDD-related pattern [PDDRP]). Similarities and differences among three patterns were assessed by pattern topography, pattern expression, clinical correlations cross-sectionally, and pattern expression changes longitudinally. RESULTS: DLBRP and PDDRP shared highly similar topographies, with relative hypometabolism mainly in the middle temporal gyrus, middle occipital gyrus, lingual gyrus, precuneus, cuneus, angular gyrus, superior and inferior parietal gyrus, middle and inferior frontal gyrus, cingulate, and caudate, and relative hypermetabolism in the cerebellum, putamen, thalamus, precentral/postcentral gyrus, and paracentral lobule, which were more extensive than the PDRP. Patients with DLB and PDD could not be distinguished successfully by any pattern, but patients with PD were easily recognized, especially by DLBRP and PDDRP. The pattern expression of DLBRP and PDDRP showed similar efficacy in cross-sectional disease severity assessment and longitudinal progression monitoring. CONCLUSIONS: The consistent abnormalities in metabolic patterns of DLB and PDD might underline the potential continuum across the clinical spectrum from PD to DLB. © 2022 International Parkinson and Movement Disorder Society.


Assuntos
Doença de Alzheimer , Doença por Corpos de Lewy , Doença de Parkinson , Doença de Alzheimer/metabolismo , Encéfalo/diagnóstico por imagem , Encéfalo/metabolismo , Estudos Transversais , Humanos , Doença por Corpos de Lewy/diagnóstico por imagem , Doença por Corpos de Lewy/metabolismo , Doença de Parkinson/diagnóstico por imagem , Doença de Parkinson/metabolismo , Tomografia por Emissão de Pósitrons/métodos
11.
Mov Disord ; 37(9): 1915-1923, 2022 09.
Artigo em Inglês | MEDLINE | ID: mdl-35861378

RESUMO

BACKGROUND: Anecdotal evidence suggests that patients diagnosed with the parkinsonian subtype of multiple system atrophy (MSA-P) may show uptake of the second-generation tau positron emission tomography (PET) tracer 18 F-Florzolotau (previously known as 18 F-APN-1607) in the putamen. OBJECTIVES: This study systematically investigated the localization and magnitude of 18 F-Florzolotau uptake in a relatively large cohort of patients with MSA-P. METHODS: 18 F-Florzolotau PET imaging was performed in 31 patients with MSA-P, 24 patients with Parkinson's disease (PD), and 20 age-matched healthy controls. 18 F-Florzolotau signal in the striatum was analyzed by visual inspection and classified as either positive or negative. Regional 18 F-Florzolotau binding was also expressed as standardized uptake value ratio (SUVR) to assess whether it was associated with core symptoms of MSA-P after adjustment for potential confounders. RESULTS: By visual inspection and semiquantitative SUVR comparisons, patients with MSA-P showed elevated 18 F-Florzolotau uptake in the putamen, globus pallidus, and dentate-a finding that was not observed in PD. This increased signal was significantly associated with the core symptoms of MSA-P. In addition, patients with MSA-P with cerebellar ataxia showed an elevated 18 F-Florzolotau uptake in the cerebellar dentate. CONCLUSIONS: 18 F-Florzolotau tau PET imaging findings may reflect the clinical severity of MSA-P and can potentially discriminate between this condition and PD. © 2022 International Parkinson and Movement Disorder Society.


Assuntos
Atrofia de Múltiplos Sistemas , Doença de Parkinson , Fluordesoxiglucose F18/metabolismo , Humanos , Atrofia de Múltiplos Sistemas/diagnóstico , Doença de Parkinson/diagnóstico , Tomografia por Emissão de Pósitrons/métodos , Putamen/metabolismo , Tomografia Computadorizada por Raios X
12.
Eur Radiol ; 32(11): 8008-8018, 2022 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-35674825

RESUMO

OBJECTIVES: We proposed a novel deep learning-based radiomics (DLR) model to diagnose Parkinson's disease (PD) based on [18F]fluorodeoxyglucose (FDG) PET images. METHODS: In this two-center study, 255 normal controls (NCs) and 103 PD patients were enrolled from Huashan Hospital, China; 26 NCs and 22 PD patients were enrolled as a separate test group from Wuxi 904 Hospital, China. The proposed DLR model consisted of a convolutional neural network-based feature encoder and a support vector machine (SVM) model-based classifier. The DLR model was trained and validated in the Huashan cohort and tested in the Wuxi cohort, and accuracy, sensitivity, specificity and receiver operator characteristic (ROC) curve graphs were used to describe the model's performance. Comparative experiments were performed based on four other models including the scale model, radiomics model, standard uptake value ratio (SUVR) model and DLR model. RESULTS: The DLR model demonstrated superiority in differentiating PD patients and NCs in comparison to other models, with an accuracy of 95.17% [90.35%, 98.13%] (95% confidence intervals, CI) in the Huashan cohort. Moreover, the DLR model also demonstrated greater performance in diagnosing PD early than routine methods, with an accuracy of 85.58% [78.60%, 91.57%] in the Huashan cohort. CONCLUSIONS: We developed a DLR model based on [18F]FDG PET images that showed good performance in the noninvasive, individualized prediction of PD and was superior to traditional handcrafted methods. This model has the potential to guide and facilitate clinical diagnosis and contribute to the development of precision treatment. KEY POINTS: The DLR method on [18F]FDG PET images helps clinicians to diagnose PD and PD subgroups from normal controls. A prospective two-center study showed that the DLR method provides greater diagnostic accuracy.


Assuntos
Aprendizado Profundo , Doença de Parkinson , Humanos , Fluordesoxiglucose F18/farmacologia , Doença de Parkinson/diagnóstico por imagem , Estudos Prospectivos , Tomografia por Emissão de Pósitrons
13.
J Am Chem Soc ; 143(11): 4387-4396, 2021 Mar 24.
Artigo em Inglês | MEDLINE | ID: mdl-33703893

RESUMO

Phase engineering of nanomaterials (PEN) enables the preparation of metal nanomaterials with unconventional phases that are different from their thermodynamically stable counterparts. These unconventional-phase nanomaterials can serve as templates to construct precisely controlled metallic heterostructures for wide applications. Nevertheless, how the unconventional phase of templates affects the nucleation and growth of secondary metals still requires systematic explorations. Here, two-dimensional (2D) square-like Au nanosheets with an unconventional 2H/face-centered cubic (fcc) heterophase, composing of two pairs of opposite edges with 2H/fcc heterophase and fcc phase, respectively, and two 2H/fcc heterophase basal planes, are prepared and then used as templates to grow one-dimensional (1D) Rh nanorods. The effect of different phases in different regions of the Au templates on the overgrowth of Rh nanorods has been systematically investigated. By tuning the reaction conditions, three types of 1D/2D Rh-Au heterostructures are prepared. In the type A heterostructure, Rh nanorods only grow on the fcc defects including stacking faults and/or twin boundaries (denoted as fcc-SF/T) and 2H phases in two 2H/fcc edges of the Au nanosheet. In the type B heterostructure, Rh nanorods grow on the fcc-SF/T and 2H phases in two 2H/fcc edges and two 2H/fcc basal planes of the Au nanosheet. In the type C heterostructure, Rh nanorods grow on four edges and two basal planes of the Au nanosheet. Furthermore, the type C heterostructure shows promising performance toward the electrochemical hydrogen evolution reaction (HER) in acidic media, which is among the best reported Rh-based and other noble-metal-based HER electrocatalysts.

14.
Eur J Neurol ; 28(9): 2927-2939, 2021 09.
Artigo em Inglês | MEDLINE | ID: mdl-34110063

RESUMO

BACKGROUND AND PURPOSE: The diagnosis and monitoring of semantic variant primary progressive aphasia (sv-PPA) are clinically challenging. We aimed to establish a distinctive metabolic pattern in sv-PPA for diagnosis and severity evaluation. METHODS: Fifteen sv-PPA patients and 15 controls were enrolled to identify sv-PPA-related pattern (sv-PPARP) by principal component analysis of 18 F-fluorodeoxyglucose positron emission tomography. Eighteen Alzheimer disease dementia (AD) and 14 behavioral variant frontotemporal dementia (bv-FTD) patients were enrolled to test the discriminatory power. Correspondingly, regional metabolic activities extracted from the voxelwise analysis were evaluated for the discriminatory power. RESULTS: The sv-PPARP was characterized as decreased metabolic activity mainly in the bilateral temporal lobe (left predominance), middle orbitofrontal gyrus, left hippocampus/parahippocampus gyrus, fusiform gyrus, insula, inferior orbitofrontal gyrus, and striatum, with increased activity in the bilateral lingual gyrus, cuneus, calcarine gyrus, and right precentral and postcentral gyrus. The pattern expression had significant discriminatory power (area under the curve [AUC] = 0.98, sensitivity = 100%, specificity = 94.4%) in distinguishing sv-PPA from AD, and the asymmetry index offered complementary discriminatory power (AUC = 0.91, sensitivity = 86.7%, specificity = 92.9%) in distinguishing sv-PPA from bv-FTD. In sv-PPA patients, the pattern expression correlated with Boston Naming Test scores at baseline and showed significant increase in the subset of patients with follow-up. The voxelwise analysis showed similar topography, and the regional metabolic activities had equivalent or better discriminatory power and clinical correlations with Boston Naming Test scores. The ability to reflect disease progression in longitudinal follow-up seemed to be inferior to the pattern expression. CONCLUSIONS: The sv-PPARP might serve as an objective biomarker for diagnosis and progression evaluation.


Assuntos
Doença de Alzheimer , Afasia Primária Progressiva , Demência Frontotemporal , Afasia Primária Progressiva/diagnóstico por imagem , Humanos , Testes Neuropsicológicos , Tomografia por Emissão de Pósitrons , Semântica
15.
Angew Chem Int Ed Engl ; 60(49): 25884-25890, 2021 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-34561927

RESUMO

The efficiency of electrolytic hydrogen production is limited by the slow reaction kinetics of oxygen evolution reaction (OER). Surface-reconstructed ferromagnetic (FM) catalysts with a spin-pinning effect at the FM/oxyhydroxide interface could enhance the spin-dependent OER kinetics. However, in real-life applications, electrolyzers are operated at elevated temperature, which may disrupt the spin orientations of FM catalysts and limit their performance. In this study, we prepared surface-reconstructed SmCo5 /CoOx Hy , which possesses polarized spins at the FM/oxyhydroxide interface that lead to excellent OER activity. These interfacial polarized spins could be further aligned through a magnetization process, which further enhanced the OER performance. Moreover, the operation temperature was elevated to mimic the practical operation conditions of water electrolyzers. It was found that the OER activity enhancement of the magnetized SmCo5 /CoOx Hy catalyst could be preserved up to 60 °C.

16.
Angew Chem Int Ed Engl ; 60(13): 7418-7425, 2021 Mar 22.
Artigo em Inglês | MEDLINE | ID: mdl-33372346

RESUMO

A rational design for oxygen evolution reaction (OER) catalysts is pivotal to the overall efficiency of water electrolysis. Much work has been devoted to understanding cation leaching and surface reconstruction of very active electrocatalysts, but little on intentionally promoting the surface in a controlled fashion. We now report controllable anodic leaching of Cr in CoCr2 O4 by activating the pristine material at high potential, which enables the transformation of inactive spinel CoCr2 O4 into a highly active catalyst. The depletion of Cr and consumption of lattice oxygen facilitate surface defects and oxygen vacancies, exposing Co species to reconstruct into active Co oxyhydroxides differ from CoOOH. A novel mechanism with the evolution of tetrahedrally coordinated surface cation into octahedral configuration via non-concerted proton-electron transfer is proposed. This work shows the importance of controlled anodic potential in modifying the surface chemistry of electrocatalysts.

17.
Eur J Nucl Med Mol Imaging ; 47(12): 2753-2764, 2020 11.
Artigo em Inglês | MEDLINE | ID: mdl-32318784

RESUMO

PURPOSE: Positron emission tomography (PET) with 18F-fluorodeoxyglucose (FDG) reveals altered cerebral metabolism in individuals with mild cognitive impairment (MCI) and Alzheimer's dementia (AD). Previous metabolic connectome analyses derive from groups of patients but do not support the prediction of an individual's risk of conversion from present MCI to AD. We now present an individual metabolic connectome method, namely the Kullback-Leibler Divergence Similarity Estimation (KLSE), to characterize brain-wide metabolic networks that predict an individual's risk of conversion from MCI to AD. METHODS: FDG-PET data consisting of 50 healthy controls, 332 patients with stable MCI, 178 MCI patients progressing to AD, and 50 AD patients were recruited from ADNI database. Each individual's metabolic brain network was ascertained using the KLSE method. We compared intra- and intergroup similarity and difference between the KLSE matrix and group-level matrix, and then evaluated the network stability and inter-individual variation of KLSE. The multivariate Cox proportional hazards model and Harrell's concordance index (C-index) were employed to assess the prediction performance of KLSE and other clinical characteristics. RESULTS: The KLSE method captures more pathological connectivity in the parietal and temporal lobes relative to the typical group-level method, and yields detailed individual information, while possessing greater stability of network organization (within-group similarity coefficient, 0.789 for sMCI and 0.731 for pMCI). Metabolic connectome expression was a superior predictor of conversion than were other clinical assessments (hazard ratio (HR) = 3.55; 95% CI, 2.77-4.55; P < 0.001). The predictive performance improved further upon combining clinical variables in the Cox model, i.e., C-indices 0.728 (clinical), 0.730 (group-level pattern model), 0.750 (imaging connectome), and 0.794 (the combined model). CONCLUSION: The KLSE indicator identifies abnormal brain networks predicting an individual's risk of conversion from MCI to AD, thus potentially constituting a clinically applicable imaging biomarker.


Assuntos
Doença de Alzheimer , Disfunção Cognitiva , Conectoma , Doença de Alzheimer/diagnóstico por imagem , Encéfalo/diagnóstico por imagem , Disfunção Cognitiva/diagnóstico por imagem , Progressão da Doença , Fluordesoxiglucose F18 , Humanos , Tomografia por Emissão de Pósitrons , Tomografia Computadorizada por Raios X
18.
Chemistry ; 25(20): 5113-5127, 2019 Apr 05.
Artigo em Inglês | MEDLINE | ID: mdl-30484919

RESUMO

Core-shell noble metal catalysts have gained significant attention in the past few decades, as they not only reduce the use of noble metals effectively but also exhibit unique properties derived from the synergistic effect between core and shell metals. In particular, regulating the surface structure of shells to maximize the atomic utilization efficiency of noble metals is critically important. Controlling the shell thickness of noble metal catalysts at the atomic level as an efficient approach to realize this goal has been attracting growing attention; this approach involves the formation of ultrathin shells (typically 2-6 atomic layers), monolayers, or even atomically dispersed noble metals embedded in the host metal. These strategies drive the core/support metals to improve the number of active sites and the intrinsic activity of the deposited noble metals remarkably, meanwhile minimizing the usage of noble metals. Herein, recent advances regarding atomic control of the core-shell noble metal catalysts is reviewed, with focus on the surface regulation. First, synthesis methods and surface structures are summarized, and then catalytic applications of these architectures are highlighted.

19.
Eur J Pediatr ; 178(8): 1161-1169, 2019 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-31218401

RESUMO

Congenital hyperinsulinism (CHI) is a clinically, genetically, and morphologically heterogeneous disorder. 18F DOPA-PET CT scanning greatly improves its clinical outcome. Here, we presented the first Chinese 18F DOPA-PET CT scanning-based CHI cohort highlighting the variable ethic clinical phenotypes and genotypes. Fifty CHI patients were recruited. Median age at presentation was 2 days. Median fasting time was 2 h. Mean insulin level was 25.6 µIU/ml. Fifty-two percent of patients were diazoxide-unresponsive with significantly shorter fasting tolerance time and higher serum insulin level compared with the responsive patients. Seventy-four percent of patients experienced at least one adverse drug reaction. Tremendously increased focal lesions (32%) were detected and 75% of them were cured through surgery. Thirty-one nucleotide sequence changes were identified in 48% patients. Four novel variants (Q608X, Q1347X, Q289X, F1489S) in ABCC8 gene and 2 novel variants (G132A, V138E) in KCNJ11 gene were detected. Of the variants, 87.1% harbored in ABCC and KCNJ11 genes. T1042Qfs*75 in ABCC8 gene was the most common mutation.Conclusion: Highly increased portion of focal lesion was presented in Chinese CHI patients compared with that of the previous reports. Intolerance to diazoxide was much more evident in Chinese or East Asian than other populations. Certain hotspot mutations harbored in Chinese CHI patients. What is Known: • 18F DOPA-PET CT scanning can provide informative guidance for surgical procedure when medical therapy is not well responded in CHI patients. What is New: • Intolerance to diazoxide is much more evident in Chinese and East Asian CHI patients compared with the other ethnic populations. • Novel mutations were detected in ABCC8 and KCNJ11 gene. Hotspot mutations such as T1042Qfs*75, I1511K, E501K, G111R in ABCC8 gene, and R34H in KCNJ11 gene are predominantly responsible for Chinese CHI patients.


Assuntos
Hiperinsulinismo Congênito/diagnóstico por imagem , Hiperinsulinismo Congênito/genética , Genótipo , Fenótipo , Tomografia por Emissão de Pósitrons combinada à Tomografia Computadorizada/métodos , Canais de Potássio Corretores do Fluxo de Internalização/genética , Receptores de Sulfonilureias/genética , Povo Asiático , Criança , Pré-Escolar , China , Hiperinsulinismo Congênito/etnologia , Hiperinsulinismo Congênito/terapia , Di-Hidroxifenilalanina/análogos & derivados , Feminino , Marcadores Genéticos , Testes Genéticos , Humanos , Lactente , Recém-Nascido , Masculino , Mutação , Compostos Radiofarmacêuticos , Resultado do Tratamento
20.
Hum Brain Mapp ; 39(7): 2842-2858, 2018 07.
Artigo em Inglês | MEDLINE | ID: mdl-29536636

RESUMO

Progressive supranuclear palsy (PSP) is a rare movement disorder and often difficult to distinguish clinically from Parkinson's disease (PD) and multiple system atrophy (MSA) in early phases. In this study, we report reproducible disease-related topographies of brain network and regional glucose metabolism associated with PSP in clinically-confirmed independent cohorts of PSP, MSA, and PD patients and healthy controls in the USA and China. Using 18 F-FDG PET images from PSP and healthy subjects, we applied spatial covariance analysis with bootstrapping to identify a PSP-related pattern (PSPRP) and estimate its reliability, and evaluated the ability of network scores for differential diagnosis. We also detected regional metabolic differences using statistical parametric mapping analysis. We produced a highly reliable PSPRP characterized by relative metabolic decreases in the middle prefrontal cortex/cingulate, ventrolateral prefrontal cortex, striatum, thalamus and midbrain, covarying with relative metabolic increases in the hippocampus, insula and parieto-temporal regions. PSPRP network scores correlated positively with PSP duration and accurately discriminated between healthy, PSP, MSA and PD groups in two separate cohorts of parkinsonian patients at both early and advanced stages. Moreover, PSP patients shared many overlapping areas with abnormal metabolism in the same cortical and subcortical regions as in the PSPRP. With rigorous cross-validation, this study demonstrated highly comparable and reproducible PSP-related metabolic topographies at network and regional levels across different patient populations and PET scanners. Metabolic brain network activity may serve as a reliable and objective marker of PSP, although cross-validation applying recent diagnostic criteria and classification is warranted.


Assuntos
Mapeamento Encefálico/métodos , Encéfalo/metabolismo , Glucose/metabolismo , Atrofia de Múltiplos Sistemas/metabolismo , Rede Nervosa/metabolismo , Doença de Parkinson/metabolismo , Tomografia por Emissão de Pósitrons/métodos , Paralisia Supranuclear Progressiva/metabolismo , Idoso , Encéfalo/diagnóstico por imagem , China , Diagnóstico Diferencial , Feminino , Fluordesoxiglucose F18/farmacocinética , Humanos , Masculino , Pessoa de Meia-Idade , Atrofia de Múltiplos Sistemas/diagnóstico por imagem , Rede Nervosa/diagnóstico por imagem , Doença de Parkinson/diagnóstico por imagem , Compostos Radiofarmacêuticos/farmacocinética , Paralisia Supranuclear Progressiva/diagnóstico por imagem , Estados Unidos
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