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1.
Chemosphere ; 357: 142008, 2024 Apr 11.
Artigo em Inglês | MEDLINE | ID: mdl-38614398

RESUMO

The mixture of copper and iron often results in materials with favorable properties. The material production processes involving these metals including electroplating produce hazardous wastewater. In this study, the Fluidized Bed Homogeneous Crystallization (FBHC) process was applied to treat iron and copper-containing wastewater. The initial iron copper particles were successfully recovered from synthetic wastewater with [Fe]0:[Cu]0 of 2:1, the total metal concentration of 3 mM, at effluent pH = 7.75 ± 0.75, with the upflow velocity (U) of 1.76 m/h. The agglomerates hardening process is a crucial step for initial particle synthesis. The SEM analysis reveals the spherical particle's densified crust and porous core. The particle formation mechanism which includes the formation of the nucleus, attachment of precipitate flakes, and densification of particles was proposed after microscopic observation. The initial particles synthesized were used to initiate the treatment of synthetic wastewater at the operating condition pH = 7.75 ± 0.5, [Fe]0:[Cu]0 of 2:1, the total metal concentration of 3 mM, [CO32-]0:[M]0 = 1.2:1, and U of 28.66 m/h which results in the total metal removal of 99% and crystallization ratio of 90% and 88% for iron and copper respectively. The conditions were then applied to treat electroplating wastewater and resulted in the total metal removal of 99% for both iron and copper and a crystallization ratio of 83% and 79% for iron and copper, respectively. The treatment provided advantages in terms of treating larger amounts of sludge while eliminating the need to provide seed thus yielding a higher purity of product.

2.
Angew Chem Int Ed Engl ; 63(15): e202400539, 2024 Apr 08.
Artigo em Inglês | MEDLINE | ID: mdl-38332434

RESUMO

Sodium-ion batteries (SIBs) are recognized as promising energy storage devices. However, they suffer from rapid capacity decay at ultra-low temperatures due to high Na+ desolvation energy barrier and unstable solid electrolyte interphase (SEI). Herein, a weakly solvating electrolyte (WSE) with decreased ion-dipole interactions is designed for stable sodium storage in hard carbon (HC) anode at ultra-low temperatures. 2-methyltetrahydrofuran with low solvating power is incorporated into tetrahydrofuran to regulate the interactions between Na+ and solvents. The reduced Na+-dipole interactions facilitate more anionic coordination in the first solvation sheath, which consistently maintains anion-enhanced solvation structures from room to low temperatures to promote inorganic-rich SEI formation. These enable WSE with a low freezing point of -83.3 °C and faster Na+ desolvation kinetics. The HC anode thus affords reversible capacities of 243.2 and 205.4 mAh g-1 at 50 mA g-1 at -40 and -60 °C, respectively, and the full cell of HC||Na3V2(PO4)3 yields an extended lifespan over 250 cycles with high capacity retention of ~100 % at -40 °C. This work sheds new lights on the ion-dipole regulation for ultra-low temperature SIBs.

3.
Cell Rep Med ; 5(2): 101416, 2024 Feb 20.
Artigo em Inglês | MEDLINE | ID: mdl-38350451

RESUMO

Peripheral T cell lymphoma (PTCL) is a heterogeneous group of non-Hodgkin's lymphomas varying in clinical, phenotypic, and genetic features. The molecular pathogenesis and the role of the tumor microenvironment in PTCL are poorly understood, with limited biomarkers available for genetic subtyping and targeted therapies. Through an integrated genomic and transcriptomic study of 221 PTCL patients, we delineate the genetic landscape of PTCL, enabling molecular and microenvironment classification. According to the mutational status of RHOA, TET2, histone-modifying, and immune-related genes, PTCL is divided into 4 molecular subtypes with discrete patterns of gene expression, biological aberrations, and vulnerabilities to targeted agents. We also perform an unsupervised clustering on the microenvironment transcriptional signatures and categorize PTCL into 4 lymphoma microenvironment subtypes based on characteristic activation of oncogenic pathways and composition of immune communities. Our findings highlight the potential clinical rationale of future precision medicine strategies that target both molecular and microenvironment alterations in PTCL.


Assuntos
Linfoma de Células T Periférico , Humanos , Linfoma de Células T Periférico/genética , Linfoma de Células T Periférico/metabolismo , Perfilação da Expressão Gênica , Genômica , Mutação , Microambiente Tumoral/genética
4.
Proc Natl Acad Sci U S A ; 121(5): e2316914121, 2024 Jan 30.
Artigo em Inglês | MEDLINE | ID: mdl-38252828

RESUMO

High-performance sodium storage at low temperature is urgent with the increasingly stringent demand for energy storage systems. However, the aggravated capacity loss is induced by the sluggish interfacial kinetics, which originates from the interfacial Na+ desolvation. Herein, all-fluorinated anions with ultrahigh electron donicity, trifluoroacetate (TFA-), are introduced into the diglyme (G2)-based electrolyte for the anion-reinforced solvates in a wide temperature range. The unique solvation structure with TFA- anions and decreased G2 molecules occupying the inner sheath accelerates desolvation of Na+ to exhibit decreased desolvation energy from 4.16 to 3.49 kJ mol-1 and 24.74 to 16.55 kJ mol-1 beyond and below -20 °C, respectively, compared with that in 1.0 M NaPF6-G2. These enable the cell of Na||Na3V2(PO4)3 to deliver 60.2% of its room-temperature capacity and high capacity retention of 99.2% after 100 cycles at -40 °C. This work highlights regulation of solvation chemistry for highly stable sodium-ion batteries at low temperature.

5.
Angew Chem Int Ed Engl ; 63(8): e202316949, 2024 Feb 19.
Artigo em Inglês | MEDLINE | ID: mdl-38169133

RESUMO

The sodium extraction/insertion in layered transition-metal oxide (TMO) cathode materials are typically accompanied by slab sliding and lattice changes, leading to microstructure destruction and capacity decay. Herein, negative lattice expansion is observed in an O3 type Ni-based layered cathode of Na0.9 Ni0.32 Zn0.08 Fe0.1 Mn0.3 Ti0.2 O2 upon Na+ extraction. It is attributed to the weak Zn2+ -O2- orbital hybridization and increased electron density of the surrounding oxygen for reinforced interlayer O-O repulsive force. This enables gliding of TMO slabs for the intergrowth phase transition of P3→OP2 to alleviate lattice strain with moderate lattice shrinkage, which exhibits general interslab spacings and volume changes as low as 2.4 % and 1.9 %, respectively. The strong Ti-O bonds accommodate the internal distortion of TMO6 octahedra due to the flexibility of TiO6 octahedra during cycling. These endow a high specific capacity of 144.9 mAh g-1 and excellent cycling performance of pouch-type sodium-ion batteries with 93 % capacity retention after 3600 cycles.

6.
Angew Chem Int Ed Engl ; 63(1): e202315314, 2024 Jan 02.
Artigo em Inglês | MEDLINE | ID: mdl-38009311

RESUMO

Aprotic Li-O2 battery has attracted considerable interest for high theoretical energy density, however the disproportionation of the intermediate of superoxide (O2 - ) during discharge and charge leads to slow reaction kinetics and large voltage hysteresis. Herein, the chemically stable ruthenium tris(bipyridine) (RB) cations are employed as a soluble catalyst to alternate the pathway of O2 - disproportionation and its kinetics in both the discharge and charge processes. RB captures O2 - dimer and promotes their intramolecular charge transfer, and it decreases the energy barrier of the disproportionation reaction from 7.70 to 0.70 kcal mol-1 . This facilitates the discharge and charge processes and simultaneously mitigates O2 - and singlet oxygen related side reactions. These endow the Li-O2 battery with reduced discharge/charge voltage gap of 0.72 V and prolonged lifespan for over 230 cycles when coupled with RuO2 catalyst. This work highlights the vital role of superoxide disproportionation for Li-O2 battery.

7.
Dev Neurosci ; : 1-10, 2023 Sep 27.
Artigo em Inglês | MEDLINE | ID: mdl-37757768

RESUMO

Glioblastoma (GBM) is the most prevalent and fatal form of brain tumor, which is associated with a poor prognosis. ATP-binding cassette subfamily F member 1 (ABCF1) is an E2 ubiquitin-conjugating enzyme, which is implicated in regulating immune responses and tumorigenesis. Aberrant E3 ubiquitylation has been evidenced in GBM. However, the role of ABCF1 in GBM needs to be further explored. The expression of ABCF1, CXC chemokine ligand 12 (CXCL12), and CXC chemokine receptor 4 (CXCR4) in GBM tissues was examined by the GEPIA tool, real-time PCR and Western blotting. HMC3, U251MG, and LN-229 cells were cultured and transfected with shRNA targeting ABCF1 and ABCF1 plasmids. The proliferative, migrative, and invasive ability of cells was detected. Western blotting was used to detect the levels of phosphorylated phosphatidylinositol 3-kinase (PI3K) and phosphorylated protein kinase B (AKT). We observed that GBM tissues had higher ABCF1, CXCL12, and CXCR4 expression levels. The expression levels of CXCL12 and CXCR4 were enhanced by ABCF1 overexpression, which were significantly reversed by silence of ABCF1 in GBM cells. Silencing ABCF1 or CXCR4 inhibition weakened the capacity of GBM cell growth, migration, and invasion, while ectopic ABCF1 expression or CXCL12 treatment enhanced the cellular function of GBM cells. Furthermore, p-PI3K and p-AKT protein levels were downregulated by ABCF1 knockdown or CXCR4 blockade, which were prompted by ABCF1 overexpression or CXCL12 supplement. The ABCF1-CXCL12-CXCR4 axis was identified as a key player in GBM cell survival and metastasis by activating the PI3K/AKT signaling pathway in GBM cells.

8.
Chemosphere ; 343: 140268, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-37758073

RESUMO

This study aims to explore the reusability of wastewater treatment by-product for photo-Fenton process to treat an organic pollutant model. The optimal condition, reactive oxygen species (ROS), and kinetic approach in photo-Fenton process was discussed. The Metal oxide crystal pellets from are a by-product of the Fluidized-Bed Crystallization (FBC) process and can be used as a catalyst in the Photo-Fenton process. Electroplating wastewater containing iron and copper was treated via the FBC process using granulated Al(OH)3 as carrier seeds. The binary oxide of FeOOH and Cu2O on the Al(OH)3 surface (Fe0.66Cu0.33@Al(OH)3) was identified as the FBC by-product after characterization using FTIR and XPS analysis. In the photo-Fenton process, visible light from a fluorescence lamp with a wavelength of 400-610 nm was chosen as an irradiation source. Oxalic acid was added as chelating agent to form photosensitive iron oxalate species and hydrogen peroxide was applied as oxidant to generate active radical to decolorize and mineralize RB5 synthesized solution (100 mg/L). The operating conditions including the oxalic acid to pollutant ratio ([OA]0/[RB5]0) of 4.5-13.0, reaction pH (pHr) of 3-7 and initial to theoretical hydrogen peroxide molar ratio [H2O2]0/[ H2O2]theoretical of 35%-120% were optimized. Under the optimal conditions, pHr = 5.0; [H2O2]0/[RB5]0 at 75% stoichiometric and [OA]0/[RB5]0 = 9, the RB5 is almost completely decolorized after 210 min of operation and the mineralization efficiency is 58%. The contribution of •OH, O2•-, and O21 to the Photo-Fenton system was determined using ESR analysis with the addition of DMPO and TEMP as spin trap agents. The kinetic analysis reveals the observed rate constants kRB5, kOA and kR from fitting are 0.0120, 0.0054 and 0.0001 M-1s-1, respectively.


Assuntos
Poluentes Ambientais , Peróxido de Hidrogênio , Peróxido de Hidrogênio/química , Cobre , Compostos Azo , Cinética , Luz , Óxidos/química , Ácido Oxálico , Oxirredução
9.
Small ; 19(49): e2304187, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-37603387

RESUMO

Layered manganese-based oxides (LMOs) are promising cathode materials for sodium-ion batteries (SIBs) due to their versatile structures. However, the Jahn-Teller effect of Mn3+ induces severe distortion of MnO6 octahedra, and the resultant low symmetry is responsible for the gliding of MnO2 layers and then inferior multiple-phase transitions upon Na+ extraction/insertion. Here, hexagonal P2-Na0.643 Li0.078 Mn0.827 Ti0.095 O2 is synthesized through the incorporation of Li and Ti into the distorted orthorhombic P'2-Na0.67 MnO2 to function as a phase-transition-free oxide cathode. It is revealed that Li in both the transition-metal and Na layers enhances the covalency of Mn-O bonds and allows degeneracy of Mn 3d eg orbitals to favor the formation of hexagonal phase, and the high strength of Ti-O bonds reduces the electrostatic interaction between Na and O for suppressed Na+ /vacancy rearrangements. These collectively lead to a whole-voltage-range solid-solution reaction between 1.8 and 4.3 V with a small volume variation of 1.49%. This rewards its excellent cycling stability (capacity retention of 90% after 500 cycles) and rate capability (89 mAh g-1 at 2000 mA g-1 ).

10.
Front Physiol ; 14: 1225638, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-37534367

RESUMO

Background and aims: Blood glucose prediction (BGP) has increasingly been adopted for personalized monitoring of blood glucose levels in diabetic patients, providing valuable support for physicians in diagnosis and treatment planning. Despite the remarkable success achieved, applying BGP in multi-patient scenarios remains problematic, largely due to the inherent heterogeneity and uncertain nature of continuous glucose monitoring (CGM) data obtained from diverse patient profiles. Methodology: This study proposes the first graph-based Heterogeneous Temporal Representation (HETER) network for multi-patient Blood Glucose Prediction (BGP). Specifically, HETER employs a flexible subsequence repetition method (SSR) to align the heterogeneous input samples, in contrast to the traditional padding or truncation methods. Then, the relationships between multiple samples are constructed as a graph and learned by HETER to capture global temporal characteristics. Moreover, to address the limitations of conventional graph neural networks in capturing local temporal dependencies and providing linear representations, HETER incorporates both a temporally-enhanced mechanism and a linear residual fusion into its architecture. Results: Comprehensive experiments were conducted to validate the proposed method using real-world data from 112 patients in two hospitals, comparing it with five well-known baseline methods. The experimental results verify the robustness and accuracy of the proposed HETER, which achieves the maximal improvement of 31.42%, 27.18%, and 34.85% in terms of MAE, MAPE, and RMSE, respectively, over the second-best comparable method. Discussions: HETER integrates global and local temporal information from multi-patient samples to alleviate the impact of heterogeneity and uncertainty. This method can also be extended to other clinical tasks, thereby facilitating efficient and accurate capture of crucial pattern information in structured medical data.

11.
Chemosphere ; 338: 139509, 2023 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-37459934

RESUMO

Response surface methodology (RSM) is an effective tool for process optimization with multi-complex operational factors. The present work aims to model and optimize the photocatalytic oxidation (PCO) parameters of Reactive Red 195 (RR195) dye decoloration with the SiO2-supported Fe-Co catalyst (FCS) derived from a novel catalyst synthesis method, fluidized-bed crystallization (FBC) process, using Box-Behnken design (BBD) as the RSM statistical model. The Fe-Co@SiO2 catalyst was successfully fabricated using the FBC process, and it showed good catalytic activity and performance toward the degradation of RR195. The extent of the effects of pH, H2O2 dosage (HD), catalyst loading (CL), and operating time (t) on the decoloration of RR195 was studied. Hence, the order of variable significance follows the sequence: pH > t > CL > HD. pH has the most significant effect among the variables for RR195 decoloration. The decoloration efficiency predicted by the BBD model was 88.3% under the optimized operation conditions of initial pH of 3.15, 0.76 mM H2O2, 1.18 g L-1 FCS and 59.4 min of operating time. The actual decoloration efficiency was very close to the predicted value indicating that BBD can efficiently be utilized to optimize RR195 degradation with FCS under the PCO system.


Assuntos
Peróxido de Hidrogênio , Dióxido de Silício , Peróxido de Hidrogênio/química , Oxirredução , Modelos Estatísticos
12.
Environ Res ; 236(Pt 1): 116782, 2023 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-37517497

RESUMO

Sulfide-containing wastewater, characterized by its foul odor, corrosiveness, and toxicity, can endanger human health. Fluidized-bed homogeneous crystallization (FBHC) avoids the excessive sludge production commonly associated with conventional chemical precipitation methods. In this study, FBHC is used to treat sulfur-containing synthetic wastewater. Furthermore, nickel-containing wastewater was utilized as a precipitant in the system, hence the advantage of simultaneous sulfur and nickel removal from the wastewater. The operating parameters, including pH, a precipitant dosage of [Ni2+]0/[S2-]0, and cross-sectional surface loading (LS, kg/m2h) are optimized. The optimum operating conditions of pH 9.8 ± 0.3, [Ni2+]0/[S2-]0 = 0.8, and LS = 1.5 kg/m2h results in total sulfur removal (TR) of 95.7% and crystallization ratio (CR) of 94.8%. The effect of organic compounds (acetic acid, oxalic acid, EDTA, and citric acid) and inorganic ions (NO3-, CO32-, PO43-, F-, and Cl-) on the nickel sulfide granulation process was discussed.

13.
Inorg Chem ; 62(26): 10120-10130, 2023 Jul 03.
Artigo em Inglês | MEDLINE | ID: mdl-37347205

RESUMO

Sulfide-sulfoxide aerobic photo-oxidation is of great interest in organic and medicinal chemistry; however, developing efficient and facile heterogeneous photocatalytic systems without additional additives remains challenging. Herein, we intentionally designed and synthesized two polyoxometalate (POM)-based metalloviologen frameworks, formulated as [MII(4-PBPY)2(H2O)][MII(H2O)4][CoIII2MoVI10H4O38]·nH2O (M = Cu, n = 10 for 1; M = Co, n = 11 for 2), prepared by the mild one-step synthesis strategy and characterized in detail. X-ray single-crystal diffraction analysis shows that they present a two-dimensional layered structure formed by two parallel metalloviologen layers pillared by dimeric Evans-Showell-type POMs. The connection of POM to the metalloviologen framework enables easier flow of electrons to the POM port, which can theoretically further induce O2 to generate reactive oxygen species (O2•-) to oxidize substrates to form target products. As expected, both 1 and 2 exhibit outstanding photocatalytic activity in the oxidation of sulfides. Within 6 h, methyl phenyl sulfide can be quantitatively converted into methyl phenyl sulfoxide. The in-depth mechanism reveals that there is also a synergistic energy-transfer pathway in the catalytic system in addition to the electron-transfer pathway. In addition, the corresponding catalytic activity and structure can be well maintained after at least 10 cycle experiments.

14.
Angew Chem Int Ed Engl ; 62(30): e202306236, 2023 Jul 24.
Artigo em Inglês | MEDLINE | ID: mdl-37285514

RESUMO

Li-O2 batteries have garnered much attention due to their high theoretical energy density. However, the irreversible lithium plating/stripping on the anode limits their performance, which has been paid little attention. Herein, a solvation-regulated strategy for stable lithium anodes in tetraethylene glycol dimethyl ether (G4) based electrolyte is attempted in Li-O2 batteries. Trifluoroacetate anions (TFA- ) with strong Li+ affinity are incorporated into the lithium bis(fluorosulfonyl)imide (LiTFSI)/G4 electrolyte to attenuate the Li+ -G4 interaction and form anion-dominant solvates. The bisalt electrolyte with 0.5 M LiTFA and 0.5 M LiTFSI mitigates G4 decomposition and induces an inorganic-rich solid electrolyte interphase (SEI). This contributes to decreased desolvation energy barrier from 58.20 to 46.31 kJ mol-1 , compared with 1.0 M LiTFSI/G4, for facile interfacial Li+ diffusion and high efficiency. It yields extended lifespan of 120 cycles in Li-O2 battery with a limited Li anode (7 mAh cm-2 ). This work gains comprehensive insights into rational electrolyte design for Li-O2 batteries.

15.
Front Med ; 17(4): 699-713, 2023 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-37060525

RESUMO

Anti-CD19 chimeric antigen receptor (CAR)-T cell therapy has achieved 40%-50% long-term complete response in relapsed or refractory diffuse large B-cell lymphoma (DLBCL) patients. However, the underlying mechanism of alterations in the tumor microenvironments resulting in CAR-T cell therapy failure needs further investigation. A multi-center phase I/II trial of anti-CD19 CD28z CAR-T (FKC876, ChiCTR1800019661) was conducted. Among 22 evaluable DLBCL patients, seven achieved complete remission, 10 experienced partial remissions, while four had stable disease by day 29. Single-cell RNA sequencing results were obtained from core needle biopsy tumor samples collected from long-term complete remission and early-progressed patients, and compared at different stages of treatment. M2-subtype macrophages were significantly involved in both in vivo and in vitro anti-tumor functions of CAR-T cells, leading to CAR-T cell therapy failure and disease progression in DLBCL. Immunosuppressive tumor microenvironments persisted before CAR-T cell therapy, during both cell expansion and disease progression, which could not be altered by infiltrating CAR-T cells. Aberrant metabolism profile of M2-subtype macrophages and those of dysfunctional T cells also contributed to the immunosuppressive tumor microenvironments. Thus, our findings provided a clinical rationale for targeting tumor microenvironments and reprogramming immune cell metabolism as effective therapeutic strategies to prevent lymphoma relapse in future designs of CAR-T cell therapy.

16.
Community Dent Oral Epidemiol ; 51(3): 519-526, 2023 06.
Artigo em Inglês | MEDLINE | ID: mdl-36440596

RESUMO

OBJECTIVES: This study investigated the association between the decline of the decayed, missing, and filled teeth (DMFT) index and several family-level and individual-level factors among 6- to 18-year-old Taiwanese children from 2012 to 2020. METHODS: This study used data from the 2012 and 2020 Taiwan National Oral Health Survey of Children and Adolescents. Both surveys used similar methods and were performed in the same study age group. A structured questionnaire was used to collect data on parents' sociodemographic background; the number of children in the family; oral health-related knowledge, attitudes, and behaviours; and children's dietary habits. Dental caries was recorded through standardized oral examinations. Multivariable multilevel zero-inflated negative binomial regression models were used to determine the association between family-level and individual-level factors and the DMFT index from 2012 to 2020. RESULTS: A total of 10 217 and 10 436 schoolchildren completed the oral examinations and questionnaires in the 2012 and 2020 surveys, respectively. The adjusted mean DMFT index of 12-year-old Taiwanese schoolchildren in 2020 was 2.01, denoting a significant decline from 2.50 in 2012 (adjusted mean ratio = 0.20, 95% confidence interval [CI] = 0.17, 0.23, p < .0001). Furthermore, children who often consumed sugar-rich drinks had a significantly higher risk (mean ratio = 1.05, 95% CI = 1.01, 1.10) of having DMFT than those who seldom consumed such drinks (p = .017). CONCLUSIONS: In the period of 2012-2020, the DMFT index among Taiwanese children significantly declined. Children who often consumed sugar-rich drinks had a higher DMFT index than those who seldom consumed such drinks. Our findings are valuable to paediatricians, dentists, nutritionists, and public health policymakers.


Assuntos
Cárie Dentária , Criança , Adolescente , Humanos , Cárie Dentária/epidemiologia , Cárie Dentária/etiologia , Taiwan/epidemiologia , Estudos Transversais , Inquéritos de Saúde Bucal , Açúcares , Índice CPO , Prevalência
17.
Angew Chem Int Ed Engl ; 62(2): e202214717, 2023 Jan 09.
Artigo em Inglês | MEDLINE | ID: mdl-36369628

RESUMO

Hard carbon (HC) is a promising anode material for sodium-ion batteries, yet still suffers from low initial Coulombic efficiency (ICE) and unstable solid electrolyte interphase (SEI). Herein, sodium diphenyl ketone (Na-DK) is applied to realize dual-function presodiation for HC anodes. It compensates the irreversible Na uptake at the oxygen-containing functional groups and reacts with carbon defects of five/seven-membered rings for quasi-metallic sodium in HC. The as-formed sodium induces robust NaF-rich SEI on HC in 1.0 M NaPF6 in diglyme, favoring the interfacial reaction kinetics and stable Na+ insertion and extraction. This renders the presodiated HC (pHC) with high ICE of ≈100 % and capacity retention of 82.4 % after 6800 cycles. It is demonstrated to couple with Na3 V2 (PO4 )3 cathodes in full cells to show high capacity retention of ≈100 % after 700 cycles. This work provides in-depth understanding of chemical presodiation and a new strategy for highly stable sodium-ion batteries.

18.
Proc Natl Acad Sci U S A ; 119(34): e2202835119, 2022 Aug 23.
Artigo em Inglês | MEDLINE | ID: mdl-35969765

RESUMO

Aprotic Li-O2 batteries are a promising energy storage technology, however severe side reactions during cycles lead to their poor rechargeability. Herein, highly reactive singlet oxygen (1O2) is revealed to generate in both the discharging and charging processes and is deterimental to battery stability. Electron-rich triphenylamine (TPA) is demonstrated as an effective quencher in the electrolyte to mitigate 1O2 and its associated parasitic reactions, which has the tertiary amine and phenyl groups to manifest excellent electrochemical stability and chemical reversibility. It reacts with electrophilic 1O2 to form a singlet complex during cycles, and it then quickly transforms to a triplet complex through nonradiative intersystem crossing (ISC). This efficiently accelerates the conversion of 1O2 to the ground-state triplet oxygen to eliminate its derived side reactions, and the regeneration of TPA. These enable the Li-O2 battery with obviously reduced overvoltages and prolonged lifetime for over 310 cycles when coupled with a RuO2 catalyst. This work highlights the ISC mechanism to quench 1O2 in Li-O2 battery.

19.
Comput Biol Med ; 148: 105859, 2022 09.
Artigo em Inglês | MEDLINE | ID: mdl-35930956

RESUMO

Parkinson's disease (PD) is a common neurodegenerative disease in the elderly population. PD is irreversible and its diagnosis mainly relies on clinical symptoms. Hence, its effective diagnosis is vital. PD has the related gene mutation called gene-related PD, which can be diagnosed not only in the specific PD patients, but also in the healthiest people without clinical symptoms of PD. Since mutations in PD-related genes can affect healthy people, and unaffected PD-related gene carriers can develop into PD patients, it is very necessary to distinguish gene-related PD diseases. The magnetic resonance imaging (MRI) has a lot of information about brain tissue, which can distinguish gene-related PD diseases. However, the limited amount of the gene-related cohort in PD is a challenge for further diagnosis. Therefore, we develop a joint learning framework called feature-based multi-branch octave convolution network (FMOCNN), which uses MRI data for gene-related cohort PD diagnosis. FMOCNN performs sample-feature selection to learn discriminative samples and features and contains a deep neural network to obtain high-level feature representation from various feature types. Specifically, we first train a cardinality constrained sample-feature selection (CCSFS) model to select informative samples and features. We then establish a multi-branch octave convolution neural network (MBOCNN) to jointly train multiple feature inputs. High/low-frequency learning in MBOCNN is exploited to reduce redundant feature information and enhance the feature expression ability. Our method is validated on the publicly available Parkinson's Progression Markers Initiative (PPMI) dataset. Experiments demonstrate that our method achieves promising classification performance and outperforms similar algorithms.


Assuntos
Doenças Neurodegenerativas , Doença de Parkinson , Idoso , Algoritmos , Encéfalo , Humanos , Imageamento por Ressonância Magnética
20.
Chemistry ; 28(64): e202202130, 2022 Nov 16.
Artigo em Inglês | MEDLINE | ID: mdl-35960207

RESUMO

Rechargeable lithium-oxygen batteries (LOBs) are considered to be the next-generation energy technology owing to their high theoretical energy density. However, the sluggish cathode kinetics and degradation of Li anodes result in large voltage hysteresis and low coulombic efficiency. Various materials have been applied to promote the electrochemical performance of LOBs. Metal-organic frameworks (MOFs) possessing porous structures, open active sites and adjustable pore sizes have been attempted as promising materials for catalysts and separators of LOBs. This concept presents an overview of different MOF-based catalysts for LOBs, including traditional, conductive, semi-conductive and soluble MOFs, as well as our recently proposed photo-involved LOBs. Recent advances in MOF-based separators to restrain the shuttling of redox mediators between cathodes and anodes and suppress the formation of lithium dendrites are also discussed. Finally, perspectives on the development of MOF-based LOBs for future research are presented.

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