ORCID Profile
0000-0001-8049-516X
Current Organisations
Huazhong Agricultural University
,
Massachusetts General Hospital
,
Brigham and Women's Hospital
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Publisher: Research Square Platform LLC
Date: 17-10-2022
DOI: 10.21203/RS.3.RS-2131354/V1
Abstract: Dual-atom catalysts possess a significant potential for promoting CO 2 photoreduction to lucrative solar fuels. However, the precise construction of the diatomic sites that simultaneously foster light absorption and catalytic activity is a formidable challenge, as both processes follow distinct pathways in the photocatalyst. Herein, a facile electrostatic-driven self-assembling approach is employed to realize a bifunctional architecture of a diatomic LaNi-Phen (Phenanthroline)/covalent organic framework (COF-5) photocatalyst. The La site acts as an optically active center for the photoinduced generation of carriers, while the Ni site serves as the catalytically active center for highly selective CO 2 -to-CO reduction enabled by directional charge transfer via COF-5. Density functional theory (DFT) calculations and in-situ characterization reveal the efficient synergistic effect of the La-Ni double-atomic sites, leading to decreased reaction energy barriers of *COOH intermediate and enhanced CO 2 -to-CO conversion. As a result, in the absence of any additional photosensitizers, a 15.2 times enhancement of the CO 2 reduction rate (605.8 µmol·g − 1 ·h − 1 ) over that of pristine COF-5 colloid (39.9 µmol·g − 1 ·h − 1 ) and an improvement in CO selectivity to 98.2% are achieved. This work presents a novel strategy for integrating optically and catalytically active centers, which results in a diatomic synergy effect enabling high-performance photocatalytic CO 2 reduction.
Publisher: Springer Science and Business Media LLC
Date: 14-09-2020
DOI: 10.1038/S41467-020-18350-7
Abstract: Exploring photocatalysts to promote CO 2 photoreduction into solar fuels is of great significance. We develop TiO 2 erovskite (CsPbBr 3 ) S-scheme heterojunctions synthesized by a facile electrostatic-driven self-assembling approach. Density functional theory calculation combined with experimental studies proves the electron transfer from CsPbBr 3 quantum dots (QDs) to TiO 2 , resulting in the construction of internal electric field (IEF) directing from CsPbBr 3 to TiO 2 upon hybridization. The IEF drives the photoexcited electrons in TiO 2 to CsPbBr 3 upon light irradiation as revealed by in-situ X-ray photoelectron spectroscopy analysis, suggesting the formation of an S-scheme heterojunction in the TiO 2 /CsPbBr 3 nanohybrids which greatly promotes the separation of electron-hole pairs to foster efficient CO 2 photoreduction. The hybrid nanofibers unveil a higher CO 2 -reduction rate (9.02 μmol g –1 h –1 ) comparing with pristine TiO 2 nanofibers (4.68 μmol g –1 h –1 ). Isotope ( 13 CO 2 ) tracer results confirm that the reduction products originate from CO 2 source.
Publisher: Springer Science and Business Media LLC
Date: 11-09-2019
Publisher: American Society of Neuroradiology (ASNR)
Date: 22-06-2023
DOI: 10.3174/AJNR.A7894
Publisher: Springer Science and Business Media LLC
Date: 26-10-2022
DOI: 10.1038/S41537-022-00293-1
Abstract: Brain iron is central to dopaminergic neurotransmission, a key component in schizophrenia pathology. Iron can also generate oxidative stress, which is one proposed mechanism for gray matter volume reduction in schizophrenia. The role of brain iron in schizophrenia and its potential link to oxidative stress has not been previously examined. In this study, we used 7-Tesla MRI quantitative susceptibility mapping (QSM), magnetic resonance spectroscopy (MRS), and structural T 1 imaging in 12 in iduals with chronic schizophrenia and 14 healthy age-matched controls. In schizophrenia, there were higher QSM values in bilateral putamen and higher concentrations of phosphocreatine and lactate in caudal anterior cingulate cortex (caCC). Network-based correlation analysis of QSM across corticostriatal pathways as well as the correlation between QSM, MRS, and volume, showed distinct patterns between groups. This study introduces increased iron in the putamen in schizophrenia in addition to network-wide disturbances of iron and metabolic status.
Publisher: Springer Science and Business Media LLC
Date: 17-10-2017
DOI: 10.1038/MP.2017.170
Publisher: Springer Science and Business Media LLC
Date: 10-02-2022
DOI: 10.1038/S41380-022-01460-7
Abstract: Brain morphology differs markedly between in iduals with schizophrenia, but the cellular and genetic basis of this heterogeneity is poorly understood. Here, we sought to determine whether cortical thickness (CTh) heterogeneity in schizophrenia relates to interregional variation in distinct neural cell types, as inferred from established gene expression data and person-specific genomic variation. This study comprised 1849 participants in total, including a discovery (140 cases and 1267 controls) and a validation cohort (335 cases and 185 controls). To characterize CTh heterogeneity, normative ranges were established for 34 cortical regions and the extent of deviation from these ranges was measured for each in idual with schizophrenia. CTh deviations were explained by interregional gene expression levels of five out of seven neural cell types examined: (1) astrocytes (2) endothelial cells (3) oligodendrocyte progenitor cells (OPCs) (4) excitatory neurons and (5) inhibitory neurons. Regional alignment between CTh alterations with cell type transcriptional maps distinguished broad patient subtypes, which were validated against genomic data drawn from the same in iduals. In a predominantly neuronal/endothelial subtype (22% of patients), CTh deviations covaried with polygenic risk for schizophrenia (sczPRS) calculated specifically from genes marking neuronal and endothelial cells ( r = −0.40, p = 0.010). Whereas, in a predominantly glia/OPC subtype (43% of patients), CTh deviations covaried with sczPRS calculated from glia and OPC-linked genes ( r = −0.30, p = 0.028). This multi-scale analysis of genomic, transcriptomic, and brain phenotypic data may indicate that CTh heterogeneity in schizophrenia relates to inter-in idual variation in cell-type specific functions. Decomposing heterogeneity in relation to cortical cell types enables prioritization of schizophrenia subsets for future disease modeling efforts.
Publisher: Springer Science and Business Media LLC
Date: 29-04-2023
DOI: 10.1038/S41467-023-37545-2
Abstract: The precise construction of photocatalysts with diatomic sites that simultaneously foster light absorption and catalytic activity is a formidable challenge, as both processes follow distinct pathways. Herein, an electrostatically driven self-assembly approach is used, where phenanthroline is used to synthesize bifunctional LaNi sites within covalent organic framework. The La and Ni site acts as optically and catalytically active center for photocarriers generation and highly selective CO 2 -to-CO reduction, respectively. Theory calculations and in-situ characterization reveal the directional charge transfer between La-Ni double-atomic sites, leading to decreased reaction energy barriers of *COOH intermediate and enhanced CO 2 -to-CO conversion. As a result, without any additional photosensitizers, a 15.2 times enhancement of the CO 2 reduction rate (605.8 μmol·g −1 ·h −1 ) over that of a benchmark covalent organic framework colloid (39.9 μmol·g −1 ·h −1 ) and improved CO selectivity (98.2%) are achieved. This work presents a potential strategy for integrating optically and catalytically active centers to enhance photocatalytic CO 2 reduction.
Publisher: Springer Science and Business Media LLC
Date: 03-07-2019
DOI: 10.1038/S41467-019-11031-0
Abstract: Age- and sex-related alterations in gene transcription have been demonstrated, however the underlying mechanisms are unresolved. Neuroepigenetic pathways regulate gene transcription in the brain. Here, we measure in vivo expression of the epigenetic enzymes, histone deacetylases (HDACs), across healthy human aging and between sexes using [ 11 C]Martinostat positron emission tomography (PET) neuroimaging ( n = 41). Relative HDAC expression increases with age in cerebral white matter, and correlates with age-associated disruptions in white matter microstructure. A post mortem study confirmed that HDAC1 and HDAC2 paralogs are elevated in white matter tissue from elderly donors. There are also sex-specific in vivo HDAC expression differences in brain regions associated with emotion and memory, including the amygdala and hippoc us. Hippoc us and white matter HDAC expression negatively correlates with emotion regulation skills ( n = 23). Age and sex are associated with HDAC expression in vivo, which could drive age- and sex-related transcriptional changes and impact human behavior.
Publisher: Springer Science and Business Media LLC
Date: 24-05-2021
Location: Denmark
Location: United States of America
No related grants have been discovered for Amanda E Lyall.