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1.
ACS Appl Mater Interfaces ; 16(32): 42109-42117, 2024 Aug 14.
Artigo em Inglês | MEDLINE | ID: mdl-39088819

RESUMO

The electrochemical CO2 reduction reaction (ECO2RR) is a promising strategy for converting CO2 into high-value chemical products. However, the synthesis of effective and stable electrocatalysts capable of transforming CO2 into a specified product remains a huge challenge. Herein, we report a template-regulated strategy for the preparation of a Bi2O3-derived nanosheet catalyst with abundant porosity to achieve the expectantly efficient CO2-to-formate conversion. The resultant porous bismuth nanosheet (p-Bi) not only exhibited marked Faradaic efficiency of formate (FEformate), beyond 91% in a broad potential range from -0.75 to -1.1 V in the H-type cell, but also demonstrated an appreciable FEformate of 94% at a high current density of 262 mA cm-2 in the commercially important gas diffusion cell. State-of-the-art X-ray absorption near edge structure spectroscopy (XANES) and theoretical calculation unraveled the distinct formate production performance of the p-Bi catalyst, which was cocontributed by its smaller size, plentiful porous structure, and stronger Bi-O bond, thus accelerating the absorption of CO2 and promoting the subsequent formation of intermediates. This work provides an avenue to fabricate bismuth-based catalysts with high planar and porous morphologies for a broad portfolio of applications.

2.
FASEB J ; 38(15): e23855, 2024 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-39096134

RESUMO

Astrocytes and microglia undergo dynamic and complex morphological and functional changes following ischemic stroke, which are instrumental in both inflammatory responses and neural repair. While gene expression alterations poststroke have been extensively studied, investigations into posttranscriptional regulatory mechanisms, specifically alternative splicing (AS), remain limited. Utilizing previously reported Ribo-Tag-seq data, this study analyzed AS alterations in poststroke astrocytes and microglia from young adult male and female mice. Our findings reveal that in astrocytes, compared to the sham group, 109 differential alternative splicing (DAS) events were observed at 4 h poststroke, which increased to 320 at day 3. In microglia, these numbers were 316 and 266, respectively. Interestingly, the disparity between DAS genes and differentially expressed genes is substantial, with fewer than 10 genes shared at both poststroke time points in astrocytes and microglia. Gene ontology enrichment analysis revealed the involvement of these DAS genes in diverse functions, encompassing immune response (Adam8, Ccr1), metabolism (Acsl6, Pcyt2, Myo5a), and developmental cell growth (App), among others. Selective DAS events were further validated by semiquantitative RT-PCR. Overall, this study comprehensively describes the AS alterations in astrocytes and microglia during the hyperacute and acute phases of ischemic stroke and underscores the significance of certain hub DAS events in neuroinflammatory processes.


Assuntos
Processamento Alternativo , Astrócitos , AVC Isquêmico , Microglia , Animais , Astrócitos/metabolismo , Astrócitos/patologia , Microglia/metabolismo , Microglia/patologia , Camundongos , AVC Isquêmico/genética , AVC Isquêmico/metabolismo , AVC Isquêmico/patologia , Masculino , Feminino , Camundongos Endogâmicos C57BL
3.
CNS Neurosci Ther ; 30(6): e14815, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38922778

RESUMO

AIMS: Colony stimulating factor 1 receptor (CSF1R)-related leukoencephalopathy is a rapidly progressing neurodegenerative disease caused by CSF1R gene mutations. This study aimed to identify and investigate the effect of a novel intronic mutation (c.1754-3C>G) of CSF1R on splicing. METHODS: A novel intronic mutation was identified using whole-exome sequencing. To investigate the impact of this mutation, we employed various bioinformatics tools to analyze the transcription of the CSF1R gene and the three-dimensional structure of its encoded protein. Furthermore, reverse transcription polymerase chain reaction (RT-PCR) was performed to validate the findings. RESULTS: A novel mutation (c.1754-3C>G) in CSF1R was identified, which results in exon 13 skipping due to the disruption of the 3' splice site consensus sequence NYAG/G. This exon skipping event was further validated in the peripheral blood of the mutation carrier through RT-PCR and Sanger sequencing. Protein structure prediction indicated a disruption in the tyrosine kinase domain, with the truncated protein showing significant structural alterations. CONCLUSIONS: Our findings underscore the importance of intronic mis-splicing mutations in the diagnosis and management of CSF1R-related leukoencephalopathy.


Assuntos
Íntrons , Leucoencefalopatias , Mutação , Receptores de Fator Estimulador das Colônias de Granulócitos e Macrófagos , Humanos , Leucoencefalopatias/genética , Mutação/genética , Receptores de Fator Estimulador das Colônias de Granulócitos e Macrófagos/genética , Íntrons/genética , Feminino , Masculino , Adulto , Splicing de RNA/genética , Receptor de Fator Estimulador de Colônias de Macrófagos
4.
Adv Sci (Weinh) ; : e2404513, 2024 Jun 27.
Artigo em Inglês | MEDLINE | ID: mdl-38937993

RESUMO

Zinc anodes of zinc metal batteries suffer from unsatisfactory plating/striping reversibility due to interfacial parasitic reactions and poor Zn2+ mass transfer kinetics. Herein, methoxy polyethylene glycol-phosphate (mPEG-P) is introduced as an electrolyte additive to achieve long anti-calendar aging and high-rate capabilities. The polyanionic of mPEG-P self-assembles via noncovalent-interactions on electrode surface to form polyether-based cation channels and in situ organic-inorganic hybrid solid electrolyte interface layer, which ensure rapid Zn2+ mass transfer and suppresses interfacial parasitic reactions, realizing outstanding cycling/calendar aging stability. As a result, the Zn//Zn symmetric cells with mPEG-P present long lifespans over 9000 and 2500 cycles at ultrahigh current densities of 120 and 200 mA cm-2, respectively. Besides, the coulombic efficiency (CE) of the Zn//Cu cell with mPEG-P additive (88.21%) is much higher than that of the cell (36.4%) at the initial cycle after the 15-day calendar aging treatment, presenting excellent anti-static corrosion performance. Furthermore, after 20-day aging, the Zn//MnO2 cell exhibits a superior capacity retention of 89% compared with that of the cell without mPEG-P (28%) after 150 cycles. This study provides a promising avenue for boosting the development of high efficiency and durable metallic zinc based stationary energy storage system.

5.
Angew Chem Int Ed Engl ; : e202407439, 2024 May 28.
Artigo em Inglês | MEDLINE | ID: mdl-38807433

RESUMO

The reversibility and stability of aqueous zinc-ion batteries (AZIBs) are largely limited by water-induced interfacial parasitic reactions. Here, dimethyl(3,3-difluoro-2-oxoheptyl)phosphonate (DP) is introduced to tailor primary solvation sheath and inner-Helmholtz configurations for robust zinc anode. Informed by theoretical guidance on solvation process, DP with high permanent dipole moments can effectively substitute the coordination of H2O with charge carriers through relatively strong ion-dipolar interactions, resulting in a water-lean environment of solvated Zn2+. Thus, interfacial side reactions can be suppressed through a shielding effect. Meanwhile, lone-pair electrons of oxygen and fluorinated features of DP also reinforce the interfacial affinity of metallic zinc, associated with exclusion of neighboring water to facilitate reversible zinc planarized deposition. Thus, these merits endow the Zn anode with a high-stability performance exceeds 3800 hours at 0.5 mA cm-2 and 0.5 mAh cm-2 for Zn||Zn batteries and a high average Coulombic efficiency of 99.8 % at 4 mA cm-2 and 1 mAh cm-2 for Zn||Cu batteries. Benefiting from the stable zinc anode, the Zn||NH4V4O10 cell maintains 80.3 % of initial discharge capacity after 3000 cycles at 5 A g-1 and exhibits a high retention rate of 99.4 % against to the initial capacity during the self-discharge characterizations.

6.
J Transl Med ; 22(1): 302, 2024 03 24.
Artigo em Inglês | MEDLINE | ID: mdl-38521921

RESUMO

BACKGROUND: Myasthenia gravis (MG) is a chronic autoimmune disorder characterized by fluctuating muscle weakness. Despite the availability of established therapies, the management of MG symptoms remains suboptimal, partially attributed to lack of efficacy or intolerable side-effects. Therefore, new effective drugs are warranted for treatment of MG. METHODS: By employing an analytical framework that combines Mendelian randomization (MR) and colocalization analysis, we estimate the causal effects of blood druggable expression quantitative trait loci (eQTLs) and protein quantitative trait loci (pQTLs) on the susceptibility of MG. We subsequently investigated whether potential genetic effects exhibit cell-type specificity by utilizing genetic colocalization analysis to assess the interplay between immune-cell-specific eQTLs and MG risk. RESULTS: We identified significant MR results for four genes (CDC42BPB, CD226, PRSS36, and TNFSF12) using cis-eQTL genetic instruments and three proteins (CTSH, PRSS8, and CPN2) using cis-pQTL genetic instruments. Six of these loci demonstrated evidence of colocalization with MG susceptibility (posterior probability > 0.80). We next undertook genetic colocalization to investigate cell-type-specific effects at these loci. Notably, we identified robust evidence of colocalization, with a posterior probability of 0.854, linking CTSH expression in TH2 cells and MG risk. CONCLUSIONS: This study provides crucial insights into the genetic and molecular factors associated with MG susceptibility, singling out CTSH as a potential candidate for in-depth investigation and clinical consideration. It additionally sheds light on the immune-cell regulatory mechanisms related to the disease. However, further research is imperative to validate these targets and evaluate their feasibility for drug development.


Assuntos
Predisposição Genética para Doença , Miastenia Gravis , Humanos , Multiômica , Estudo de Associação Genômica Ampla , Miastenia Gravis/genética , Locos de Características Quantitativas/genética , Polimorfismo de Nucleotídeo Único/genética
7.
Small ; 19(45): e2302795, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-37415517

RESUMO

Pyridinic nitrogen has been recognized as the primary active site in nitrogen-doped carbon electrocatalysts for the oxygen reduction reaction (ORR), which is a critical process in many renewable energy devices. However, the preparation of nitrogen-doped carbon catalysts comprised of exclusively pyridinic nitrogen remains challenging, as well as understanding the precise ORR mechanisms on the catalyst. Herein, a novel process is developed using pyridyne reactive intermediates to functionalize carbon nanotubes (CNTs) exclusively with pyridine rings for ORR electrocatalysis. The relationship between the structure and ORR performance of the prepared materials is studied in combination with density functional theory calculations to probe the ORR mechanism on the catalyst. Pyridinic nitrogen can contribute to a more efficient 4-electron reaction pathway, while high level of pyridyne functionalization result in negative structural effects, such as poor electrical conductivity, reduced surface area, and small pore diameters, that suppressed the ORR performance. This study provides insights into pyridine-doped CNTs-functionalized for the first time via pyridyne intermediates-as applied in the ORR and is expected to serve as valuable inspiration in designing high-performance electrocatalysts for energy applications.

8.
J Pain Res ; 16: 2487-2495, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-37497373

RESUMO

Purpose: To determine the effectiveness and safety of venlafaxine in treating persistent idiopathic dentoalveolar pain (PIDP). Patients and Methods: A retrospective analysis was conducted on a cohort comprising 129 patients with a definite diagnosis of PIDP, who were treated with venlafaxine between May 2020 and December 2022 at three different institutions. Baseline characteristics were statistically described, and visual analog scale (VAS) scores before and during treatment were collected. The percentage of pain relief was calculated. Differences in baseline characteristics between responsive and unresponsive patients were evaluated. Additionally, side effects experienced during treatment were also summarized. Results: Among the included patients, 4 suffered immediate side effects following the initial dose of venlafaxine and the treatment was discontinued. 104 (80.6%) patients achieved pain relief. VAS scores of responsive patients at weeks 2, and months 1, 2, and 3 were significantly lower than baseline (p<0.001). Duration of pain was the only factor related to responsiveness (Wilcoxon rank sum test p<0.001, logistic regression p=0.001). 64 patients (49.6%) suffered from mild side effects. No serious side effects were observed during the study. Conclusion: Venlafaxine is potentially effective and safe in the management of PIDP. Early application of venlafaxine following the diagnoses of PIDP can result in a higher possibility of pain relief.

9.
Materials (Basel) ; 16(9)2023 May 06.
Artigo em Inglês | MEDLINE | ID: mdl-37176437

RESUMO

The low oil recovery rate observed in current oil fields is largely attributed to the presence of remaining oil trapped in the pores of porous media during waterflooding. To improve the recovery rate, it is imperative to gain an understanding of the oil-water flow characteristics and displacement mechanisms during waterflooding, as well as to elucidate the underlying mobilization mechanisms of residual oil at the pore scale. In this paper, we explore these issues in depth by numerically investigating the influence of factors such as water injection velocities, oil-water viscosity ratios, and wettability conditions on pore-scale oil-water flow characteristics and oil recovery rate. To this end, we employ a direct numerical simulation (DNS) method in conjunction with the volume of fluid (VOF) method to study the microscopic displacement mechanisms of waterflooding in a reconstructed two-dimensional digital rock core based on micro-CT technology. In addition, the particle tracing method is adopted to identify the flow path and dominant areas during waterflooding in order to mobilize the residual oil within the pores. The findings indicate that the oil-water flow characteristics in porous media are determined by the interplay between capillary and viscous forces. Furthermore, the oil recovery rate is 10.6% and 24.7% lower under strong water-wet and oil-wet conditions than that (32.36%) under intermediate wettability conditions, and the final oil recovery rate is higher under water-wet conditions than under oil-wet conditions. The seepage path and the dominant areas are directly linked to the capillarity formed during waterflooding. The findings of this study are significant in terms of enhancing the recovery rate of residual oil and provide a novel perspective for understanding the waterflooding process.

10.
J Neuroinflammation ; 20(1): 63, 2023 Mar 08.
Artigo em Inglês | MEDLINE | ID: mdl-36890539

RESUMO

Vitamin D deficiency is associated with worse clinical outcomes after ischemic stroke; nevertheless, the pathophysiological mechanisms remain largely unexplored. In this study, we characterized the molecular mechanisms of how vitamin D signaling modulated stroke progression in male mouse ischemia-reperfusion stroke models. We found that vitamin D receptor (VDR) exhibited a predominant upregulation in peri-infarct microglia/macrophages following cerebral ischemia. Conditional Vdr inactivation in microglia/macrophages markedly augmented infarct volumes and neurological deficits. VDR-deficient microglia/macrophages exhibited a more primed proinflammatory phenotype with substantial secretion of TNF-α and IFN-γ. These inflammatory cytokines further enhanced CXCL10 release from endothelial cells and blood-brain barrier disruption, and ultimately infiltration of peripheral T lymphocytes. Notably, blocking TNF-α and IFN-γ significantly ameliorated stroke phenotypes in Vdr conditional knockout mice. Collectively, VDR signaling in microglia/macrophages plays a crucial role in restraining ischemia-elicited neuroinflammation and stroke progression. Our findings delineate a novel mechanism underlying the association between vitamin D deficiency and poor stroke outcomes, and underline the significance of maintaining a functional vitamin D signaling in the management of acute ischemic stroke.


Assuntos
Lesões Encefálicas , Isquemia Encefálica , AVC Isquêmico , Acidente Vascular Cerebral , Deficiência de Vitamina D , Camundongos , Masculino , Animais , Microglia , AVC Isquêmico/complicações , Doenças Neuroinflamatórias , Fator de Necrose Tumoral alfa , Vitamina D , Células Endoteliais , Macrófagos , Acidente Vascular Cerebral/complicações , Isquemia Encefálica/complicações , Isquemia Encefálica/genética , Lesões Encefálicas/complicações , Modelos Animais de Doenças , Camundongos Knockout , Infarto , Deficiência de Vitamina D/complicações , Infarto da Artéria Cerebral Média/complicações
11.
Pain Physician ; 25(7): E1121-E1128, 2022 10.
Artigo em Inglês | MEDLINE | ID: mdl-36288599

RESUMO

BACKGROUND: Pulsed radiofrequency (PRF) is a percutaneous, micro-invasive, and micro-destructive neuromodulation technology. It has been reported to be useful in the treatment of supraorbital neuralgia (SN). However, the long-term effectiveness and safety of this technique in SN has not been reported yet. OBJECTIVES: To investigate the outcomes of PRF on supraorbital neuralgia (SN) in multi-centers and a long-term perspective. STUDY DESIGN: Retrospective case series. METHODS: Patients who underwent PRF for SN at 4 hospitals in Beijing between Jan 2007 and Jan 2021 were identified and reviewed for inclusion. Their demographic data and baseline conditions were statistically described, and their conditions of pain control were analyzed using Kaplan-Meier survival analyses. A survival curve was plotted, the cumulative proportion of pain-free at specific time points was determined, and the median pain-free time was estimated. Complications related to PRF treatment were summarized. The risk factors for initial pain control and pain-free survival were analyzed using logistic regression and Cox regression. RESULTS: A total of 116 patients were included; 91 (78.4%) patients got initial pain control with just one attempt of PRF. The maximum length of follow-up was 127 months, with a median of 18 months. During follow-up, 29 (31.9%) patients suffered from pain recurrence, and 11 (12.1%) were lost. The cumulative pain-free survival at 6 months, 1 year, 2 years, 3 years, 5 years, 8 years, and 10 years were estimated as 70%, 64%, 59%, 55%, 44%, 37%, and 37%, respectively. The median pain-free time was 52 months. No severe complications were observed or reported. Duration of disease could significantly influence initial pain control, while no risk factors for pain-free survival were recognized. LIMITATIONS: A retrospective study setting without a control group. CONCLUSION: The performance of PRF for the treatment of SN was confirmed to be favorable in a multicentric, relatively large scale, and long-term perspective.


Assuntos
Neuralgia , Tratamento por Radiofrequência Pulsada , Neuralgia do Trigêmeo , Humanos , Tratamento por Radiofrequência Pulsada/métodos , Estudos Retrospectivos , Neuralgia/terapia , Neuralgia do Trigêmeo/terapia , Manejo da Dor/métodos , Resultado do Tratamento
12.
Nat Commun ; 13(1): 6382, 2022 Oct 26.
Artigo em Inglês | MEDLINE | ID: mdl-36289229

RESUMO

Constructing stable electrodes which function over long timescales at large current density is essential for the industrial realization and implementation of water electrolysis. However, rapid gas bubble detachment at large current density usually results in peeling-off of electrocatalysts and performance degradation, especially for long term operations. Here we construct a mechanically-stable, all-metal, and highly active CuMo6S8/Cu electrode by in-situ reaction between MoS2 and Cu. The Chevrel phase electrode exhibits strong binding at the electrocatalyst-support interface with weak adhesion at electrocatalyst-bubble interface, in addition to fast hydrogen evolution and charge transfer kinetics. These features facilitate the achievement of large current density of 2500 mA cm-2 at a small overpotential of 334 mV which operate stably at 2500 mA cm-2 for over 100 h. In-situ total internal reflection imaging at micrometer level and mechanical tests disclose the relationships of two interfacial forces and performance of electrocatalysts. This dual interfacial engineering strategy can be extended to construct stable and high-performance electrodes for other gas-involving reactions.

13.
J Phys Chem A ; 126(42): 7787-7793, 2022 Oct 27.
Artigo em Inglês | MEDLINE | ID: mdl-36240026

RESUMO

Two-photon entangled generation is used to produce an entangled photon source which is a key and core element concerning the technology applications of quantum computing, quantum communication, and quantum precision measurement. In this work, we have deduced the formulas of dynamic susceptibility and phase-matching angle of two-photon entangled generation in nonlinear optical crystals. The formulas are employed to compute the susceptibilities and phase-matching angles of these optical processes for uniaxial and biaxial crystals. The susceptibility magnitude and phase-matching condition of two-photon entangled generation affect the performance of the source. The calculated results by these formulas are employed to study properties and estimate the performance of an entangled photon source. In this way, we discuss the phase matching among waves and working wavelength in an entangled source that affects the efficiency of satellite communication with the ground during the day and night.

14.
J Chem Phys ; 157(7): 074704, 2022 Aug 21.
Artigo em Inglês | MEDLINE | ID: mdl-35987593

RESUMO

Developing efficient catalysts for electrochemical CO2 reduction reaction (ECO2RR) to hydrocarbons is becoming increasingly important but still challenging due to their high overpotential and poor selectivity. Here, the famous Heusler alloys are investigated as ECO2RR catalysts for the first time by means of density functional theory calculations. The linear scaling relationship between the adsorption energies of CHO (and COOH) and CO intermediates is broken and, thus, the overpotential can be tuned regularly by chemically permuting different 3d, 4d, or 5d transition metals (TMs) in Heusler alloy Cu2TMAl. Cu2ZnAl shows the best activity among all the 30 Heusler alloys considered in the present study, with 41% improvement in energy efficiency compared to pure Cu electrode. Cu2PdAl, Cu2AgAl, Cu2PtAl, and Cu2AuAl are also good candidates. The calculations on the competition between hydrogen evolution reaction and CO2RR indicate that Cu2ZnAl is also the one having the best selectivity toward hydrocarbons. This work identifies the possibility of applying the Heusler alloy as an efficient ECO2RR catalyst. Since thousands of Heusler alloys have been found in experiments, the present study also encourages the search for more promising candidates in this broad research area.

15.
Comput Intell Neurosci ; 2022: 5941395, 2022.
Artigo em Inglês | MEDLINE | ID: mdl-35990140

RESUMO

Once virtual reality technology (Virtual Reality, VR) came out, it has received a lot of attention; in recent years, it has been widely used in the study of psychology. Because it can improve the ecological validity of experimental research, the level of conditional control, reproducibility, and avoid the dangers of field operations, it has been introduced into the field of psychology by many researchers. Compared with traditional sports psychology research methods, virtual reality technology has the characteristics of multiperception, immersion, interaction, and imagination to get a better, more realistic feel and increase people's interest in sports. Taking the application of virtual reality technology in table tennis teaching in colleges and universities as an example, this study aims to review the application of virtual reality technology in sports psychology; summarize the theory, practice, and prospect of the application of virtual reality technology in sports psychology; and add new content to the research of sports psychology. It aims to review the principles, characteristics, and application of virtual reality technology in sports psychology; summarize the advantages and disadvantages of the application of virtual reality technology in sports and point out the problems that need to be paid attention to when using this method; explore the application of virtual reality technology in sports psychology; and add new content to the research of sports psychology.


Assuntos
Tênis , Realidade Virtual , Humanos , Psicologia do Esporte , Reprodutibilidade dos Testes , Tecnologia
16.
Front Psychol ; 13: 940431, 2022.
Artigo em Inglês | MEDLINE | ID: mdl-35967614

RESUMO

Among primary and secondary school teachers in China, 70% of teachers believe that they are facing greater occupational pressure. 63.8% of teachers clearly stated that occupational pressure has caused a great or great impact on themselves. And this has had negative effects on them such as mental, physical and personal development. This article studies the group of public-funded normal students from the perspective of psychological support. This article uses the SCL-90 form to investigate the professional psychology of teachers for the psychological support of public-funded normal students engaged in the teaching profession. And it conducts a survey on the curriculum setting and satisfaction of the public-funded normal students during their study stage. The experimental results of this article show that only 11.9% of public-funded normal students are very willing to take root and serve township education. Moreover, the psychological pressure of teachers at different educational stages is quite different.

17.
Small ; 18(32): e2201051, 2022 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-35841344

RESUMO

2D material-based heterostructures are constructed by stacking or spicing individual 2D layers to create an interface between them, which have exotic properties. Here, a new strategy for the in situ growth of large numbers of 2D heterostructures on the centimeter-scale substrate is developed. In the method, large numbers of 2D MoS2 , MoO2 , or their heterostructures of MoO2 /MoS2 are controllably grown in the same setup by simply tuning the gap distance between metal precursor and growth substrate, which changes the concentration of metal precursors feed. A lateral force microscope is used first to identify the locations of each material in the heterostructures, which have MoO2 on the top of MoS2 . Noteworthy, the creation of a clean interface between atomic thin MoO2 (metallic) and MoS2 (semiconducting) results in a different electronic structure compared with pure MoO2 and MoS2 . Theoretical calculations show that the charge redistribution at such an interface results in an improved HER performance on the MoO2 /MoS2 heterostructures, showing an overpotential of 60 mV at 10 mA cm-2 and a Tafel slope of 47 mV dec-1 . This work reports a new strategy for the in situ growth of heterostructures on large-scale substrates and provides platforms to exploit their applications.

18.
Nat Commun ; 13(1): 4181, 2022 Jul 19.
Artigo em Inglês | MEDLINE | ID: mdl-35854015

RESUMO

Poly(ethylene oxide)-based solid-state electrolytes are widely considered promising candidates for the next generation of lithium and sodium metal batteries. However, several challenges, including low oxidation resistance and low cation transference number, hinder poly(ethylene oxide)-based electrolytes for broad applications. To circumvent these issues, here, we propose the design, synthesis and application of a fluoropolymer, i.e., poly(2,2,2-trifluoroethyl methacrylate). This polymer, when introduced into a poly(ethylene oxide)-based solid electrolyte, improves the electrochemical window stability and transference number. Via multiple physicochemical and theoretical characterizations, we identify the presence of tailored supramolecular bonds and peculiar morphological structures as the main factors responsible for the improved electrochemical performances. The polymeric solid electrolyte is also investigated in full lithium and sodium metal lab-scale cells. Interestingly, when tested in a single-layer pouch cell configuration in combination with a Li metal negative electrode and a LiMn0.6Fe0.4PO4-based positive electrode, the polymeric solid-state electrolyte enables 200 cycles at 42 mA·g-1 and 70 °C with a stable discharge capacity of approximately 2.5 mAh when an external pressure of 0.28 MPa is applied.

19.
Nanoscale ; 14(22): 7957-7973, 2022 Jun 09.
Artigo em Inglês | MEDLINE | ID: mdl-35635464

RESUMO

To mitigate excessively accumulated carbon dioxide (CO2) in the atmosphere and tackle the associated environmental concerns, green and effective approaches are necessary. The electrocatalytic CO2 reduction reaction (CO2RR) using sustainable electricity under benign reaction conditions represents a viable way to produce value-added and profitable chemicals. In this minireview, recent studies regarding unary Bi electrocatalysts and binary BiSn electrocatalysts are symmetrically categorized and reviewed, as they disclose high faradaic efficiencies toward the production of formate/formic acid, which has a relatively higher value of up to 0.50 $·per kg and has been widely used in the chemical and pharmaceutical industry. In particular, the preparation methodologies, electrocatalyst morphologies, catalytic performances and the corresponding mechanisms are comprehensively presented. The use of solid-state electrolytes showing high economic prospects for directly obtaining high-purity formic acid is highlighted. Finally, the remaining questions and challenges for CO2RR exploitations using Bi-related electrocatalysts are proposed, while perspectives and the corresponding strategies aiming to enhance their entire catalytic functionalities and boost their performance are provided.

20.
Nature ; 604(7907): 689-696, 2022 04.
Artigo em Inglês | MEDLINE | ID: mdl-35444276

RESUMO

The structure of the human neocortex underlies species-specific traits and reflects intricate developmental programs. Here we sought to reconstruct processes that occur during early development by sampling adult human tissues. We analysed neocortical clones in a post-mortem human brain through a comprehensive assessment of brain somatic mosaicism, acting as neutral lineage recorders1,2. We combined the sampling of 25 distinct anatomic locations with deep whole-genome sequencing in a neurotypical deceased individual and confirmed results with 5 samples collected from each of three additional donors. We identified 259 bona fide mosaic variants from the index case, then deconvolved distinct geographical, cell-type and clade organizations across the brain and other organs. We found that clones derived after the accumulation of 90-200 progenitors in the cerebral cortex tended to respect the midline axis, well before the anterior-posterior or ventral-dorsal axes, representing a secondary hierarchy following the overall patterning of forebrain and hindbrain domains. Clones across neocortically derived cells were consistent with a dual origin from both dorsal and ventral cellular populations, similar to rodents, whereas the microglia lineage appeared distinct from other resident brain cells. Our data provide a comprehensive analysis of brain somatic mosaicism across the neocortex and demonstrate cellular origins and progenitor distribution patterns within the human brain.


Assuntos
Células Clonais , Mosaicismo , Neocórtex , Linhagem da Célula , Células Cultivadas , Humanos , Microglia , Neocórtex/citologia , Neocórtex/crescimento & desenvolvimento
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