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1.
Annu Rev Microbiol ; 77: 111-129, 2023 09 15.
Artigo em Inglês | MEDLINE | ID: mdl-37018842

RESUMO

Infections caused by malaria parasites place an enormous burden on the world's poorest communities. Breakthrough drugs with novel mechanisms of action are urgently needed. As an organism that undergoes rapid growth and division, the malaria parasite Plasmodium falciparum is highly reliant on protein synthesis, which in turn requires aminoacyl-tRNA synthetases (aaRSs) to charge tRNAs with their corresponding amino acid. Protein translation is required at all stages of the parasite life cycle; thus, aaRS inhibitors have the potential for whole-of-life-cycle antimalarial activity. This review focuses on efforts to identify potent plasmodium-specific aaRS inhibitors using phenotypic screening, target validation, and structure-guided drug design. Recent work reveals that aaRSs are susceptible targets for a class of AMP-mimicking nucleoside sulfamates that target the enzymes via a novel reaction hijacking mechanism. This finding opens up the possibility of generating bespoke inhibitors of different aaRSs, providing new drug leads.


Assuntos
Aminoacil-tRNA Sintetases , Antimaláricos , Malária , Humanos , Antimaláricos/farmacologia , Antimaláricos/uso terapêutico , Aminoacil-tRNA Sintetases/química , Aminoacil-tRNA Sintetases/genética , Aminoacil-tRNA Sintetases/metabolismo , Plasmodium falciparum/genética , Malária/tratamento farmacológico , RNA de Transferência/genética , RNA de Transferência/metabolismo , RNA de Transferência/uso terapêutico
2.
Proc Natl Acad Sci U S A ; 121(22): e2401656121, 2024 May 28.
Artigo em Inglês | MEDLINE | ID: mdl-38787880

RESUMO

Understanding the dynamics of electric-double-layer (EDL) charging in porous media is essential for advancements in next-generation energy storage devices. Due to the high computational demands of direct numerical simulations and a lack of interfacial boundary conditions for reduced-order models, the current understanding of EDL charging is limited to simple geometries. Here, we present a network model to predict EDL charging in arbitrary networks of long pores in the Debye-Hückel limit without restrictions on EDL thickness and pore radii. We demonstrate that electrolyte transport is described by Kirchhoff's laws in terms of the electrochemical potential of charge (the valence-weighted average of the ion electrochemical potentials) instead of the electric potential. By employing the equivalent circuit representation suggested by these modified Kirchhoff's laws, our methodology accurately captures the spatial and temporal dependencies of charge density and electric potential, matching results obtained from computationally intensive direct numerical simulations. Our network model provides results up to six orders of magnitude faster, enabling the efficient simulation of a triangular lattice of five thousand pores in 6 min. We employ the framework to study the impact of pore connectivity and polydispersity on electrode charging dynamics for pore networks and discuss how these factors affect the time scale, energy density, and power density of capacitive charging. The scalability and versatility of our methodology make it a rational tool for designing 3D-printed electrodes and for interpreting geometric effects on electrode impedance spectroscopy measurements.

3.
Proc Natl Acad Sci U S A ; 121(8): e2312870121, 2024 Feb 20.
Artigo em Inglês | MEDLINE | ID: mdl-38349875

RESUMO

Oxidation self-charging batteries have emerged with the demand for powering electronic devices around the clock. The low efficiency of self-charging has been the key challenge at present. Here, a more efficient autoxidation self-charging mechanism is realized by introducing hemoglobin (Hb) as a positive electrode additive in the polyaniline (PANI)-zinc battery system. The heme acts as a catalyst that reduces the energy barrier of the autoxidation reaction by regulating the charge and spin state of O2. To realize self-charging, the adsorbed O2 molecules capture electrons of the reduced (discharged state) PANI, leading to the desorption of zinc ions and the oxidation of PANI to complete self-charging. The battery can discharge for 12 min (0.5 C) after 50 self-charging/discharge cycles, while there is nearly no discharge capacity in the absence of Hb. This biology-inspired electronic regulation strategy may inspire new ideas to boost the performance of self-charging batteries.

4.
Proc Natl Acad Sci U S A ; 121(5): e2309384121, 2024 Jan 30.
Artigo em Inglês | MEDLINE | ID: mdl-38252835

RESUMO

High-quality specimen preparation plays a crucial role in cryo-electron microscopy (cryo-EM) structural analysis. In this study, we have developed a reliable and convenient technique called the graphene sandwich method for preparing cryo-EM specimens. This method involves using two layers of graphene films that enclose macromolecules on both sides, allowing for an appropriate ice thickness for cryo-EM analysis. The graphene sandwich helps to mitigate beam-induced charging effect and reduce particle motion compared to specimens prepared using the traditional method with graphene support on only one side, therefore improving the cryo-EM data quality. These advancements may open new opportunities to expand the use of graphene in the field of biological electron microscopy.


Assuntos
Grafite , Microscopia Crioeletrônica , Confiabilidade dos Dados , Movimento (Física)
5.
Nano Lett ; 24(5): 1695-1702, 2024 Feb 07.
Artigo em Inglês | MEDLINE | ID: mdl-38261789

RESUMO

To meet the growing demands in both energy and power densities of lithium ion batteries, electrode structures must be capable of facile electron and ion transport while minimizing the content of electrochemically inactive components. Herein, binder-free LiFePO4 (LFP) cathodes are fabricated with a multidimensional conductive architecture that allows for fast-charging capability, reaching a specific capacity of 94 mAh g-1 at 4 C. Such multidimensional networks consist of active material particles wrapped by 1D single-walled carbon nanotubes (CNTs) and bound together using 2D MXene (Ti3C2Tx) nanosheets. The CNTs form a porous coating layer and improve local electron transport across the LFP surface, while the Ti3C2Tx nanosheets provide simultaneously high electrode integrity and conductive pathways through the bulk of the electrode. This work highlights the ability of multidimensional conductive fillers to realize simultaneously superior electrochemical and mechanical properties, providing useful insights into future fast-charging electrode designs for scalable electrochemical systems.

6.
Nano Lett ; 24(31): 9743-9749, 2024 Aug 07.
Artigo em Inglês | MEDLINE | ID: mdl-39072414

RESUMO

The dynamics of ion transport at the interface is the critical factor for determining the performance of an electrochemical energy storage device. While practical applications are realized in concentrated electrolytes and nanopores, there is a limited understanding of their ion dynamic features. Herein, we studied the interfacial ion dynamics in room-temperature ionic liquids by transient single-particle imaging with microsecond-scale resolution. We observed slowed-down dynamics at lower potential while acceleration was observed at higher potential. Combined with simulation, we found that the microstructure evolution of the electric double layer (EDL) results in potential-dependent kinetics. Then, we established a correspondence between the ion dynamics and interfacial ion composition. Besides, the ordered ion orientation within EDL is also an essential factor for accelerating interfacial ion transport. These results inspire us with a new possibility to optimize electrochemical energy storage through the good control of the rational design of the interfacial ion structures.

7.
Nano Lett ; 24(12): 3694-3701, 2024 Mar 27.
Artigo em Inglês | MEDLINE | ID: mdl-38411584

RESUMO

A functional coating layer (FCL) is widely applied in fast-charging lithium-ion batteries to improve the sluggish Li+ transport kinetics of traditional graphite anodes. However, blindly increasing the Li+ conductivity for FCL reduces the overall electron conductivity of the anodes. Herein, we decoupled the effect of La-doping on TiNb2O7 (TNO) in terms of the phase evolution, Li+/electron transport, and lithiation behavior, and then proposed a promising La0.1TNO FCL with balanced Li+/electron transport for a fast-charging graphite anode. By optimizing the doping concentration of La, more holes are introduced into the TNO as electron carriers without causing lattice distortion, thus maintaining the fast Li+ diffusion channel in TNO. As a result, the graphite with La0.1TNO FCL delivers an excellent capacity of 220.2 mAh g-1 (96.3% retention) after 450 cycles at 3 C, nearly twice that of the unmodified one.

8.
Small ; 20(16): e2307027, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38018336

RESUMO

Fast charging lithium (Li)-ion batteries are intensively pursued for next-generation energy storage devices, whose electrochemical performance is largely determined by their constituent electrode materials. While nanosizing of electrode materials enhances high-rate capability in academic research, it presents practical limitations like volumetric packing density and high synthetic cost. As an alternative to nanosizing, microscale electrode materials cannot only effectively overcome the limitations of the nanosizing strategy but also satisfy the requirement of fast-charging batteries. Therefore, this review summarizes the new emerging microscale electrode materials for fast charging from the commercialization perspective. First, the fundamental theory of electronic/ionic motion in both individual active particles and the whole electrode is proposed. Then, based on these theories, the corresponding optimization strategies are summarized toward fast-charging microscale electrode materials. In addition, advanced functional design to tackle the mechanical degradation problems related to next generation high capacity alloy- and conversion-type electrode materials (Li, S, Si et al.) for achieving fast charging and stable cycling batteries. Finally, general conclusions and the future perspective on the potential research directions of microscale electrode materials are proposed. It is anticipated that this review will provide the basic guidelines for both fundamental research and practical applications of fast-charging batteries.

9.
Small ; : e2402774, 2024 May 28.
Artigo em Inglês | MEDLINE | ID: mdl-38805741

RESUMO

2D layered molybdenum disulfide (MoS2) has garnered considerable attention as an attractive electrode material in sodium-ion batteries (SIBs), but sluggish mass transfer kinetic and capacity fading make it suffer from inferior cycle capability. Herein, hierarchical MoS2 nanosheets decorated porous TiO2 nanofibers (MoS2 NSs@TiO2 NFs) with rich oxygen vacancies are engineered by microemulsion electrospinning method and subsequent hydrothermal/heat treatment. The MoS2 NSs@TiO2 NFs improves ion/electron transport kinetic and long-term cycling performance through distinctive porous structure and heterogeneous component. Consequently, the electrode exhibits excellent long-term Na storage capacity (298.4 mAh g-1 at 5 A g-1 over 1100 cycles and 235.6 mAh g-1 at 10 A g-1 over 7200 cycles). Employing Na3V2(PO4)3 as cathode, the full cell maintains a desirable capacity of 269.6 mAh g-1 over 700 cycles at 1.0 A g-1. The stepwise intercalation-conversion and insertion/extraction endows outstanding Na+ storage performance, which yields valuable insight into the advancement of fast-charging and long-cycle life SIBs anode materials.

10.
Small ; 20(26): e2310201, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38243889

RESUMO

Enhancing the mobility of lithium-ions (Li+) through surface engineering is one of major challenges facing fast-charging lithium-ion batteries (LIBs). In case of demanding charging conditions, the use of a conventional artificial graphite (AG) anode leads to an increase in operating temperature and the formation of lithium dendrites on the anode surface. In this study, a biphasic zeolitic imidazolate framework (ZIF)-AG anode, designed strategically and coated with a mesoporous material, is verified to improve the pathways of Li+ and electrons under a high charging current density. In particular, the graphite surface is treated with a coating of a ZIF-8-derived carbon nanoparticles, which addresses sufficient surface porosity, enabling this material to serve as an electrolyte reservoir and facilitate Li+ intercalation. Moreover, the augmentation in specific surface area proves advantageous in reducing the overpotential for interfacial charge transfer reactions. In practical terms, employing a full-cell with the biphasic ZIF-AG anode results in a shorter charging time and improved cycling performance, demonstrating no evidence of Li plating during 300 cycles under 3.0 C-charging and 1.0 C-discharging. The research endeavors to contribute to the progress of anode materials by enhancing their charging capability, aligning with the increasing requirements of the electric vehicle applications.

11.
Small ; 20(29): e2311250, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38431938

RESUMO

Ultrafast high-capacity lithium-ion batteries are extremely desirable for portable electronic devices, where Si is the most promising alternative to the conventional graphite anode due to its very high theoretical capacity. However, the low electronic conductivity and poor Li-diffusivity limit its rate capability. Moreover, high volume expansion/contraction upon Li-intake/uptake causes severe pulverization of the electrode, leading to drastic capacity fading. Here, interface and morphology-engineered amorphous Si matrix is being reported utilizing a few-layer vertical graphene (VG) buffer layer to retain high capacity at both slow and fast (dis)charging rates. The flexible mechanical support of VG due to the van-der-Waals interaction between the graphene layers, the weak adhesion between Si and graphene, and the highly porous geometry mitigated stress, while the three-dimensional mass loading enhanced specific capacity. Additionally, the high electronic conductivity of VG boosted rate-capability, resulting in a reversible gravimetric capacity of ≈1270 mAh g-1 (areal capacity of ≈37 µAh cm-2) even after 100 cycles at an ultrafast cycling rate of 20C, which provides a fascinating way for conductivity and stress management to obtain high-performance storage devices.

12.
Small ; : e2405731, 2024 Aug 13.
Artigo em Inglês | MEDLINE | ID: mdl-39136416

RESUMO

Localized high-concentration electrolytes (LHCEs) have emerged as a promising class of electrolytes to improve the cycle life and energy density of lithium-ion batteries (LIBs). While their application in batteries with lithium-metal anodes is extensively investigated, their behavior in systems with graphite anodes has received less research attention. Herein, the behaviors of four electrolytes in Graphite | LiNiO2 cells are compared. By systematically varying the electrolyte compositions, the impacts of the solvation structure, solvent composition, and salt composition of LHCEs are identified on the rate capability, stability, and propensity for lithium plating in LIB full-cells. It is found that while the solvation structure and solvent composition each play an important role in determining rate capability, the substitution of LiPF6 salt with LiFSI maximizes the rate capability and suppresses irreversible lithium plating. It is now demonstrated via constant-potential cycling, that an appropriately formulated LHCE can, therefore, maintain high reversible capacity and safety under arbitrarily fast charging conditions.

13.
Small ; : e2404583, 2024 Jul 30.
Artigo em Inglês | MEDLINE | ID: mdl-39077979

RESUMO

In recent years, there have been extensive debates regarding the charging mechanism of MnO2 cathodes in aqueous Zn electrolytes. The discussion centered on several key aspects including the identity of the charge carriers contributing to the overall capacity, the nature of the electrochemical process, and the role of the zinc hydroxy films that are reversibly formed during the charging/discharging. Intense studies are also devoted to understanding the effect of the Mn2+ additive on the performance of the cathodes. Nevertheless, it seems that a consistent explanation of the α-MnO2 charging mechanism is still lacking. To address this, a step-by-step analysis of the MnO2 cathodes is conducted. Valuable information is obtained by using in situ electrochemical quartz crystal microbalance with dissipation (EQCM-D) monitoring, supplemented by solid-state nuclear magnetic resonance (NMR), X-ray diffraction (XRD) in Characterization of Materials, and pH measurements. The findings indicate that the charging mechanism is dominated by the insertion of H3O+ ions, while no evidence of Zn2+ intercalation is found. The role of the Mn2+ additive in promoting the generation of protons by forming MnOOH, enhancing the stability of Zn/α-MnO2 batteries is thoroughly investigated. This work provides a comprehensive overview on the electrochemical and the chemical reactions associated with the α-MnO2 electrodes, and will pave the way for further development of aqueous cathodes for Zn-ion batteries.

14.
Small ; : e2404879, 2024 Aug 05.
Artigo em Inglês | MEDLINE | ID: mdl-39101287

RESUMO

Traditional ethylene carbonate (EC)-based electrolytes constrain the applications of silicon carbon (Si-C) anodes under fast-charging and low-temperature conditions due to sluggish Li+ migration kinetics and unstable solid electrolyte interphase (SEI). Herein, inspired by the efficient water purification and soil stabilization of aquatic plants, a stable SEI with a 3D desolvation interface is designed with gel polymer electrolyte (GPE), accelerating Li+ desolvation and migration at the interface and within stable SEI. As demonstrated by theoretical simulations and experiment results, the resulting poly(1,3-dioxolane) (PDOL), prepared by in situ ring-opening polymerization of 1,3-dioxolane (DOL), creates a 3D desolvation area, improving the Li+ desolvation at the interface and yielding an amorphous GPE with a high Li+ ionic conductivity (5.73 mS cm-1). Furthermore, more anions participate in the solvated structure, forming an anion-derived stable SEI and improving Li+ transport through SEI. Consequently, the Si-C anode achieves excellent rate performance with GPE at room temperature (RT) and low temperature (-40 °C). The pouch full cell coupled with LiFePO4 cathode obtains 97.42 mAh g-1 after 500 cycles at 5 C/5 C. This innovatively designed 3D desolvation interface and SEI represent significant breakthroughs for developing fast-charging and low-temperature batteries.

15.
Small ; 20(34): e2402108, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38586916

RESUMO

Lithium metal is a highly promising anode for next-generation high-energy-density rechargeable batteries. Nevertheless, its practical application faces challenges due to the uncontrolled lithium dendrites growth and infinite volumetric expansion during repetitive cycling. Herein, a composite lithium anode is designed by mechanically rolling and pressing a cerium oxide-coated carbon textile with lithium foil (Li@CeO2/CT). The in situ generated cerium dioxide (CeO2) and cerium trioxide (Ce2O3) form a heterojunction with a reduced lithium-ion migration barrier, facilitating the rapid lithium ions migration. Additionally, both CeO2 and Ce2O3 exhibit higher adsorbed energy with lithium, enabling faster and more distributed interfacial transport of lithium ions. Furthermore, the high specific surface area of 3D skeleton can effectively reduce local current density, and alleviate the lithium volumetric changes upon plating/stripping. Benefiting from this unique structure, the highly compact and uniform lithium deposition is constructed, allowing the Li@CeO2/CT symmetric cells to maintain a stable cycling for over 500 cycles at an exceptional high current density of 100 mA cm-2. When paired with LiNi0.91Co0.06Mn0.03O2 (NCM91) cathode, the cell achieves 74.3% capacity retention after 800 cycles at 1 C, and a remarkable capacity retention of 81.1% after 500 cycles even at a high rate of 4  C.

16.
Small ; 20(23): e2310809, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38154097

RESUMO

Triboelectric nanogenerator (TENG) as a means of energy harvesting can effectively harvest ocean wave energy, but the energy conversion efficiency and stability of the device during long-term operations are still problems that must be solved for TENGs. Decreasing the frictional resistance between two triboelectric material surfaces is one of the critical approaches for improving the device efficiency and durability. In this work, a novel stacked disc-type rolling triboelectric nanogenerator (SDR-TENG) is designed and fabricated for low-frequency water wave energy harvesting. After 860 000 working cycles, the electrical output attenuation of the SDR-TENG basic unit is less than 5%, showing excellent device durability. Under the simulated water wave conditions, the SDR-TENG with four rolling TENG units can produce an output current of 84.4 µA and an output power of 7.6 mW, corresponding to an effective power density of 16.8 W m-3. This work not only proposes a strategy to effectively enhance the durability of the devices, but also provides a feasible solution for monitoring the surrounding environment of the charging buoys of unmanned ships.

17.
Small ; : e2405432, 2024 Sep 19.
Artigo em Inglês | MEDLINE | ID: mdl-39295569

RESUMO

LiNi0.8Mn0.1Co0.1O2 (NMC811) is the most promising cathode material for future Li-ion batteries (LIBs). However, the bulk and surface structural instabilities retard its commercial success. Surface chemical instability toward exposure to moisture (H2O and CO2) leads to the formation of residual lithium compounds (RLCs: Li2CO3, LiOH) on the surface. The alkaline RLCs form a resistive layer on the surface of NMC811 by undergoing parasitic side reactions with electrolytes. Herein, an "Adverse-to-Beneficial" approach is proposed to eliminate RLCs by chemically transforming them into a LixPOy (Li3PO4 and LiPO3) interface. The interface protects the NMC811 surface from moisture attack and unwanted side reactions with electrolytes. It enhances the cycle life by retaining 70% of the initial capacity after 300 cycles at a 0.5C rate and 60% after 500 cycles, even at a 5C rate in a voltage window of 3.0-4.3 V versus Li+/Li. The coexistence of two Li-conducting phases lowers the voltage polarization of the kinetically sluggish H1 → M phase transition to unlock fast cycling, reduces cationic disorder, improves coulombic efficiency, enhances ion diffusion kinetics, and minimizes particle crack formation after long-term cycling. Hence, the LixPOy interface yields multifaceted benefits in the storage, processing, and electrochemistry of NMC811.

18.
Small ; : e2400824, 2024 May 19.
Artigo em Inglês | MEDLINE | ID: mdl-38764257

RESUMO

Halide perovskite, renowned for its multifunctional properties, shows considerable promise for realizing self-charging power systems. In this study, a lead-free methylammonium bismuth iodide (MA3Bi2I9) perovskite is used to create a self-charging power unit (SPU). This involves constructing a hybrid piezoelectric-triboelectric nanogenerator (Hybrid-TENG) and utilizing MA3Bi2I9 for energy storage as an anode in a lithium-ion battery (LIB). Initially, MA3Bi2I9 nanorods are synthesized and composited with a polystyrene-block-poly(ethylene-ran-butylene)-block-polystyrene polymer. The dielectric and mechanical properties of composite films having perovskite loading content are investigated. The optimized Hybrid-TENG exhibits superior performance, generating a voltage of 537 V, current density of 13.2 µA cm- 2, and maximum power density of 3.04 mW cm-2, which can be attributed to the high piezoelectric coefficient of MA3Bi2I9 nanorods (≈20.6 pm V-1). A MA3Bi2I9 thin film, serving as an electrode in LIB, demonstrates a high specific capacity of 2378.9 mAh cm-3 (578.8 mAh g-1) with a capacity retention of ≈87.5% over 100 cycles, underscoring its stable performance. Furthermore, a Hybrid-TENG is employed to charge the MA3Bi2I9-based LIB, thus realizing an SPU for driving portable electronics. This study highlights the promising potential of perovskites for developing efficient nanogenerators and LIBs, paving the way for sustainable energy solutions in small-scale electronics.

19.
J Synchrotron Radiat ; 31(Pt 1): 55-64, 2024 Jan 01.
Artigo em Inglês | MEDLINE | ID: mdl-37930257

RESUMO

X-ray photon correlation spectroscopy (XPCS) holds strong promise for observing atomic-scale dynamics in materials, both at equilibrium and during non-equilibrium transitions. Here an in situ XPCS study of the relaxor ferroelectric PbMg1/3Nb2/3O3 (PMN) is reported. A weak applied AC electric field generates strong response in the speckle of the diffuse scattering from the polar nanodomains, which is captured using the two-time correlation function. Correlated motions of the Bragg peak are also observed, which indicate dynamic tilting of the illuminated volume. This tilting quantitatively accounts for the observed two-time speckle correlations. The magnitude of the tilting would not be expected solely from the modest applied field, since PMN is an electrostrictive material with no linear strain response to the field. A model is developed based on non-uniform static charging of the illuminated surface spot by the incident micrometre-scale X-ray beam and the electrostrictive material response to the combination of static and dynamic fields. The model qualitatively explains the direction and magnitude of the observed tilting, and predicts that X-ray-induced piezoresponse could be an important factor in correctly interpreting results from XPCS and nanodiffraction studies of other insulating materials under applied AC field or varying X-ray illumination.

20.
RNA ; 2022 Oct 25.
Artigo em Inglês | MEDLINE | ID: mdl-36283829

RESUMO

Each transfer RNA (tRNA) is aminoacylated (charged) with a genetic codon-specific amino acid at its 3' end. Charged tRNAs are primarily used for translation, whereas fluctuations in charged tRNA fractions are known to reflect cellular response to stress. Here we report the development of individual tRNA-acylation using PCR (i-tRAP), a convenient PCR-based method that can specifically quantify individual tRNA charging ratio. In this i-tRAP method, demethylases remove base methylations which are problematic for reverse transcription reaction, and ß-elimination reaction specifically removes the 3' end of adenine residue in uncharged tRNA. Subsequent TaqMan MGB qRT-PCR can distinguish between cDNA of charged tRNA and uncharged tRNA. By using this method, we revealed that the charging ratio of tRNAGln(CUG) was changed in response to amino acid starvation and also the charging ratio of tRNAGln(CUG) in senescent cells was lower than in young cells under starvation conditions. i-tRAP can be applicable to the quantification of charging ratio of various tRNAs, and provides a simple and convenient method for analyzing tRNA charging.

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