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1.
Angew Chem Int Ed Engl ; 63(22): e202403668, 2024 May 27.
Artigo em Inglês | MEDLINE | ID: mdl-38462892

RESUMO

The electrolyte chemistry is crucially important for promoting the practical application of lithium metal batteries (LMBs). Here, we demonstrate for the first time that 1,3-dimethylimidazolium dimethyl phosphate (DIDP) and trimethylsilyl trifluoroacetate (TMSF) can undergo in situ transesterification in carbonate electrolyte to generate dimethyl trimethylsilyl phosphate (DTMSP) and 1,3-dimethylimidazolium trifluoroacetate (DITFA) as multifunctional additives for LMBs. H2O and HF can be removed by the Si-O group in DTMSP to improve the moisture resistance of electrolyte and the stability of cathode. Furthermore, the dissolution of lithium nitrate (LiNO3) in carbonate electrolyte can be promoted by the trifluoroacetate anion (TFA-) in DITFA, thereby optimizing the solvation structure and transport kinetics of Li+. More importantly, both DTMSP and DITFA tend to preferential redox decomposition due to the low lowest unoccupied molecular orbital (LUMO) and high highest occupied molecular orbital (HOMO). Consequently, a thin and robust layer rich in P/N/Si on the cathode and an inorganic-rich layer (e.g. Li3N/Li3P) on the anode can be constructed and superior electrochemical performances are achieved. This artificial transesterification strategy to introduce favorable additives paves an efficient and ingenious route to high-performance electrolyte for LMBs.

2.
Sensors (Basel) ; 24(1)2023 Dec 20.
Artigo em Inglês | MEDLINE | ID: mdl-38202904

RESUMO

Removing noise from acquired images is a crucial step in various image processing and computer vision tasks. However, the existing methods primarily focus on removing specific noise and ignore the ability to work across modalities, resulting in limited generalization performance. Inspired by the iterative procedure of image processing used by professionals, we propose a pixel-wise crossmodal image-denoising method based on deep reinforcement learning to effectively handle noise across modalities. We proposed a similarity reward to help teach an optimal action sequence to model the step-wise nature of the human processing process explicitly. In addition, We designed an action set capable of handling multiple types of noise to construct the action space, thereby achieving successful crossmodal denoising. Extensive experiments against state-of-the-art methods on publicly available RGB, infrared, and terahertz datasets demonstrate the superiority of our method in crossmodal image denoising.

3.
Artigo em Inglês | MEDLINE | ID: mdl-39033955

RESUMO

BACKGROUND: Brain aging is a complex process that involves functional alterations in multiple subnetworks and brain regions. However, most previous studies investigating aging-related functional connectivity (FC) changes using resting-state functional magnetic resonance images (rs-fMRIs) have primarily focused on the linear correlation between brain subnetworks, ignoring the nonlinear casual properties of fMRI signals. METHODS: We introduced the neural Granger causality technique to investigate the sex-dependent nonlinear Granger connectivity (NGC) during aging on a publicly available dataset of 227 healthy participants acquired cross-sectionally in Leipzig, Germany. RESULTS: Our findings indicate that brain aging may cause widespread declines in NGC at both regional and subnetwork scales. These findings exhibit high reproducibility across different network sparsities, demonstrating the efficacy of static and dynamic analysis strategies. Females exhibit greater heterogeneity and reduced stability in NGC compared to males during aging, especially the NGC between the visual network and other subnetworks. Besides, NGC strengths can well reflect the individual cognitive function, which may therefore work as a sensitive metric in cognition-related experiments for individual-scale or group-scale mechanism understanding. CONCLUSION: These findings indicate that NGC analysis is a potent tool for identifying sex-dependent brain aging patterns. Our results offer valuable perspectives that could substantially enhance the understanding of sex differences in neurological diseases in the future, especially in degenerative disorders.

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