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1.
Proc Natl Acad Sci U S A ; 121(10): e2313981121, 2024 Mar 05.
Artigo em Inglês | MEDLINE | ID: mdl-38412129

RESUMO

Real-time characterization of microresonator dynamics is important for many applications. In particular, it is critical for near-field sensing and understanding light-matter interactions. Here, we report camera-facilitated imaging and analysis of standing wave patterns in optical ring resonators. The standing wave pattern is generated through bidirectional pumping of a microresonator, and the scattered light from the microresonator is collected by a short-wave infrared (SWIR) camera. The recorded scattering patterns are wavelength dependent, and the scattered intensity exhibits a linear relation with the circulating power within the microresonator. By modulating the relative phase between the two pump waves, we can control the generated standing waves' movements and characterize the resonator with the SWIR camera. The visualized standing wave enables subwavelength distance measurements of scattering targets with nanometer-level accuracy. This work opens broad avenues for applications in on-chip near-field (bio)sensing, real-time characterization of photonic integrated circuits, and backscattering control in telecom systems.

2.
Proc Natl Acad Sci U S A ; 120(20): e2300544120, 2023 05 16.
Artigo em Inglês | MEDLINE | ID: mdl-37155910

RESUMO

Indirect reciprocity is a mechanism that explains large-scale cooperation in humans. In indirect reciprocity, individuals use reputations to choose whether or not to cooperate with a partner and update others' reputations. A major question is how the rules to choose their actions and the rules to update reputations evolve. In the public reputation case where all individuals share the evaluation of others, social norms called Simple Standing (SS) and Stern Judging (SJ) have been known to maintain cooperation. However, in the case of private assessment where individuals independently evaluate others, the mechanism of maintenance of cooperation is still largely unknown. This study theoretically shows for the first time that cooperation by indirect reciprocity can be evolutionarily stable under private assessment. Specifically, we find that SS can be stable, but SJ can never be. This is intuitive because SS can correct interpersonal discrepancies in reputations through its simplicity. On the other hand, SJ is too complicated to avoid an accumulation of errors, which leads to the collapse of cooperation. We conclude that moderate simplicity is a key to stable cooperation under the private assessment. Our result provides a theoretical basis for the evolution of human cooperation.


Assuntos
Comportamento Cooperativo , Modelos Psicológicos , Humanos , Normas Sociais , Evolução Biológica
3.
Proc Natl Acad Sci U S A ; 120(11): e2217703120, 2023 Mar 14.
Artigo em Inglês | MEDLINE | ID: mdl-36877847

RESUMO

The release of wastewaters containing relatively low levels of nitrate (NO3-) results in sufficient contamination to induce harmful algal blooms and to elevate drinking water NO3- concentrations to potentially hazardous levels. In particular, the facile triggering of algal blooms by ultra-low concentrations of NO3- necessitates the development of efficient methods for NO3- destruction. However, promising electrochemical methods suffer from weak mass transport under low reactant concentrations, resulting in long treatment times (on the order of hours) for complete NO3- destruction. In this study, we present flow-through electrofiltration via an electrified membrane incorporating nonprecious metal single-atom catalysts for NO3- reduction activity enhancement and selectivity modification, achieving near-complete removal of ultra-low concentration NO3- (10 mg-N L-1) with a residence time of only a few seconds (10 s). By anchoring Cu single atoms supported on N-doped carbon in a carbon nanotube interwoven framework, we fabricate a free-standing carbonaceous membrane featuring high conductivity, permeability, and flexibility. The membrane achieves over 97% NO3- removal with high N2 selectivity of 86% in a single-pass electrofiltration, which is a significant improvement over flow-by operation (30% NO3- removal with 7% N2 selectivity). This high NO3- reduction performance is attributed to the greater adsorption and transport of nitric oxide under high molecular collision frequency coupled with a balanced supply of atomic hydrogen through H2 dissociation during electrofiltration. Overall, our findings provide a paradigm of applying a flow-through electrified membrane incorporating single-atom catalysts to improve the rate and selectivity of NO3- reduction for efficient water purification.

4.
Proc Natl Acad Sci U S A ; 119(32): e2200567119, 2022 08 09.
Artigo em Inglês | MEDLINE | ID: mdl-35914131

RESUMO

Evolution of resistance is a major barrier to successful deployment of gene-drive systems to suppress natural populations, which could greatly reduce the burden of many vector-borne diseases. Multiplexed guide RNAs (gRNAs) that require resistance mutations in all target cut sites are a promising antiresistance strategy since, in principle, resistance would only arise in unrealistically large populations. Using stochastic simulations that accurately model evolution at very large population sizes, we explore the probability of resistance due to three important mechanisms: 1) nonhomologous end-joining mutations, 2) single-nucleotide mutants arising de novo, or 3) single-nucleotide polymorphisms preexisting as standing variation. Our results explore the relative importance of these mechanisms and highlight a complexity of the mutation-selection-drift balance between haplotypes with complete resistance and those with an incomplete number of resistant alleles. We find that this leads to a phenomenon where weakly deleterious naturally occurring variants greatly amplify the probability of multisite resistance compared to de novo mutation. This key result provides design criterion for antiresistance multiplexed systems, which, in general, will need a larger number of gRNAs compared to de novo expectations. This theory may have wider application to the evolution of resistance or evolutionary rescue when multiple changes are required before selection can act.


Assuntos
Tecnologia de Impulso Genético , Variação Genética , Modelos Genéticos , Alelos , Deriva Genética , Variação Genética/genética , Haplótipos , Mutação , Polimorfismo de Nucleotídeo Único/genética , RNA Guia de Cinetoplastídeos/genética , Seleção Genética , Processos Estocásticos
5.
Proc Natl Acad Sci U S A ; 119(30): e2122153119, 2022 07 26.
Artigo em Inglês | MEDLINE | ID: mdl-35858397

RESUMO

Speciation is the process by which barriers to gene flow evolve between populations. Although we now know that speciation is largely driven by natural selection, knowledge of the agents of selection and the genetic and genomic mechanisms that facilitate divergence is required for a satisfactory theory of speciation. In this essay, we highlight three advances/problems in our understanding of speciation that have arisen from studies of the genes and genomic regions that underlie the evolution of reproductive isolation. First, we describe how the identification of "speciation" genes makes it possible to identify the agents of selection causing the evolution of reproductive isolation, while also noting that the link between the genetics of phenotypic divergence and intrinsic postzygotic reproductive barriers remains tenuous. Second, we discuss the important role of recombination suppressors in facilitating speciation with gene flow, but point out that the means and timing by which reproductive barriers become associated with recombination cold spots remains uncertain. Third, we establish the importance of ancient genetic variation in speciation, although we argue that the focus of speciation studies on evolutionarily young groups may bias conclusions in favor of ancient variation relative to new mutations.


Assuntos
Especiação Genética , Isolamento Reprodutivo , Seleção Genética , Fluxo Gênico , Genoma
6.
Eur Heart J ; 45(6): 458-471, 2024 Feb 07.
Artigo em Inglês | MEDLINE | ID: mdl-37950859

RESUMO

BACKGROUND AND AIMS: Physical inactivity, sedentary behaviour (SB), and inadequate sleep are key behavioural risk factors of cardiometabolic diseases. Each behaviour is mainly considered in isolation, despite clear behavioural and biological interdependencies. The aim of this study was to investigate associations of five-part movement compositions with adiposity and cardiometabolic biomarkers. METHODS: Cross-sectional data from six studies (n = 15 253 participants; five countries) from the Prospective Physical Activity, Sitting and Sleep consortium were analysed. Device-measured time spent in sleep, SB, standing, light-intensity physical activity (LIPA), and moderate-vigorous physical activity (MVPA) made up the composition. Outcomes included body mass index (BMI), waist circumference, HDL cholesterol, total:HDL cholesterol ratio, triglycerides, and glycated haemoglobin (HbA1c). Compositional linear regression examined associations between compositions and outcomes, including modelling time reallocation between behaviours. RESULTS: The average daily composition of the sample (age: 53.7 ± 9.7 years; 54.7% female) was 7.7 h sleeping, 10.4 h sedentary, 3.1 h standing, 1.5 h LIPA, and 1.3 h MVPA. A greater MVPA proportion and smaller SB proportion were associated with better outcomes. Reallocating time from SB, standing, LIPA, or sleep into MVPA resulted in better scores across all outcomes. For example, replacing 30 min of SB, sleep, standing, or LIPA with MVPA was associated with -0.63 (95% confidence interval -0.48, -0.79), -0.43 (-0.25, -0.59), -0.40 (-0.25, -0.56), and -0.15 (0.05, -0.34) kg/m2 lower BMI, respectively. Greater relative standing time was beneficial, whereas sleep had a detrimental association when replacing LIPA/MVPA and positive association when replacing SB. The minimal displacement of any behaviour into MVPA for improved cardiometabolic health ranged from 3.8 (HbA1c) to 12.7 (triglycerides) min/day. CONCLUSIONS: Compositional data analyses revealed a distinct hierarchy of behaviours. Moderate-vigorous physical activity demonstrated the strongest, most time-efficient protective associations with cardiometabolic outcomes. Theoretical benefits from reallocating SB into sleep, standing, or LIPA required substantial changes in daily activity.


Assuntos
Doenças Cardiovasculares , Postura Sentada , Humanos , Feminino , Adulto , Pessoa de Meia-Idade , Masculino , HDL-Colesterol , Hemoglobinas Glicadas , Estudos Transversais , Estudos Prospectivos , Exercício Físico , Triglicerídeos , Sono , Doenças Cardiovasculares/epidemiologia , Doenças Cardiovasculares/prevenção & controle
7.
Nano Lett ; 24(13): 4012-4019, 2024 Apr 03.
Artigo em Inglês | MEDLINE | ID: mdl-38527220

RESUMO

The measurement of in-plane mechanical properties, such as Young's modulus and strength, of thin and stretchable materials has long been a challenge. Existing measurements, including wrinkle instability and nano indentation, are either indirect or destructive, and are inapplicable to meshes or porous materials, while the conventional tension test fails to measure the mechanical properties of nanoscale films. Here, we report a technique to test thin and stretchable films by loading a thin film afloat via differential surface tension and recording its deformation. We have demonstrated the method by measuring the Young's moduli of homogeneous films of soft materials including polydimethylsiloxane and Ecoflex and verified the results with known values. We further measured the strain distributions of meshes, both isotropic and anisotropic, which were otherwise nearly impossible to measure. The method proposed herein is expected to be generally applicable to many material systems that are thin, stretchable, and water-insoluble.

8.
Diabetologia ; 67(6): 1051-1065, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38478050

RESUMO

AIMS/HYPOTHESIS: The aim of this study was to examine the dose-response associations of device-measured physical activity types and postures (sitting and standing time) with cardiometabolic health. METHODS: We conducted an individual participant harmonised meta-analysis of 12,095 adults (mean ± SD age 54.5±9.6 years; female participants 54.8%) from six cohorts with thigh-worn accelerometry data from the Prospective Physical Activity, Sitting and Sleep (ProPASS) Consortium. Associations of daily walking, stair climbing, running, standing and sitting time with a composite cardiometabolic health score (based on standardised z scores) and individual cardiometabolic markers (BMI, waist circumference, triglycerides, HDL-cholesterol, HbA1c and total cholesterol) were examined cross-sectionally using generalised linear modelling and cubic splines. RESULTS: We observed more favourable composite cardiometabolic health (i.e. z score <0) with approximately 64 min/day walking (z score [95% CI] -0.14 [-0.25, -0.02]) and 5 min/day stair climbing (-0.14 [-0.24, -0.03]). We observed an equivalent magnitude of association at 2.6 h/day standing. Any amount of running was associated with better composite cardiometabolic health. We did not observe an upper limit to the magnitude of the dose-response associations for any activity type or standing. There was an inverse dose-response association between sitting time and composite cardiometabolic health that became markedly less favourable when daily durations exceeded 12.1 h/day. Associations for sitting time were no longer significant after excluding participants with prevalent CVD or medication use. The dose-response pattern was generally consistent between activity and posture types and individual cardiometabolic health markers. CONCLUSIONS/INTERPRETATION: In this first activity type-specific analysis of device-based physical activity, ~64 min/day of walking and ~5.0 min/day of stair climbing were associated with a favourable cardiometabolic risk profile. The deleterious associations of sitting time were fully attenuated after exclusion of participants with prevalent CVD and medication use. Our findings on cardiometabolic health and durations of different activities of daily living and posture may guide future interventions involving lifestyle modification.


Assuntos
Exercício Físico , Postura , Postura Sentada , Caminhada , Humanos , Feminino , Exercício Físico/fisiologia , Pessoa de Meia-Idade , Masculino , Caminhada/fisiologia , Postura/fisiologia , Sono/fisiologia , Estudos Prospectivos , Acelerometria , Adulto , Biomarcadores/sangue , Idoso , Circunferência da Cintura/fisiologia , Posição Ortostática , HDL-Colesterol/sangue , Estudos Transversais , Triglicerídeos/sangue , Índice de Massa Corporal , Doenças Cardiovasculares/prevenção & controle , Doenças Cardiovasculares/epidemiologia , Comportamento Sedentário , Subida de Escada/fisiologia
9.
J Physiol ; 602(11): 2601-2614, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38194279

RESUMO

Darwin recognized that 'a grand and almost untrodden field of inquiry will be opened, on the causes and laws of variation.' However, because the Modern Synthesis assumes that the intrinsic probability of any individual mutation is unrelated to that mutation's potential adaptive value, attention has been focused on selection rather than on the intrinsic generation of variation. Yet many examples illustrate that the term 'random' mutation, as widely understood, is inaccurate. The probabilities of distinct classes of variation are neither evenly distributed across a genome nor invariant over time, nor unrelated to their potential adaptive value. Because selection acts upon variation, multiple biochemical mechanisms can and have evolved that increase the relative probability of adaptive mutations. In effect, the generation of heritable variation is in a feedback loop with selection, such that those mechanisms that tend to generate variants that survive recurring challenges in the environment would be captured by this survival and thus inherited and accumulated within lineages of genomes. Moreover, because genome variation is affected by a wide range of biochemical processes, genome variation can be regulated. Biochemical mechanisms that sense stress, from lack of nutrients to DNA damage, can increase the probability of specific classes of variation. A deeper understanding of evolution involves attention to the evolution of, and environmental influences upon, the intrinsic variation generated in gametes, in other words upon the biochemical mechanisms that generate variation across generations. These concepts have profound implications for the types of questions that can and should be asked, as omics databases become more comprehensive, detection methods more sensitive, and computation and experimental analyses even more high throughput and thus capable of revealing the intrinsic generation of variation in individual gametes. These concepts also have profound implications for evolutionary theory, which, upon reflection it will be argued, predicts that selection would increase the probability of generating adaptive mutations, in other words, predicts that the ability to evolve itself evolves.


Assuntos
Variação Genética , Genoma , Animais , Humanos , Evolução Biológica , Meio Ambiente , Seleção Genética , Mutação
10.
Annu Rev Genomics Hum Genet ; 22: 357-383, 2021 08 31.
Artigo em Inglês | MEDLINE | ID: mdl-33909459

RESUMO

The repeated adaptation of oceanic threespine sticklebacks to fresh water has made it a premier organism to study parallel evolution. These small fish have multiple distinct ecotypes that display a wide range of diverse phenotypic traits. Ecotypes are easily crossed in the laboratory, and families are large and develop quickly enough for quantitative trait locus analyses, positioning the threespine stickleback as a versatile model organism to address a wide range of biological questions. Extensive genomic resources, including linkage maps, a high-quality reference genome, and developmental genetics tools have led to insights into the genomic basis of adaptation and the identification of genomic changes controlling traits in vertebrates. Recently, threespine sticklebacks have been used as a model system to identify the genomic basis of highly complex traits, such as behavior and host-microbiome and host-parasite interactions. We review the latest findings and new avenues of research that have led the threespine stickleback to be considered a supermodel of evolutionary genomics.


Assuntos
Smegmamorpha , Animais , Mapeamento Cromossômico , Genômica , Humanos , Fenótipo , Locos de Características Quantitativas , Smegmamorpha/genética
11.
Small ; 20(26): e2310829, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38258407

RESUMO

The pursuit of highly-active and stable catalysts in anodic oxygen evolution reaction (OER) is desirable for high-current-density water electrolysis toward industrial hydrogen production. Herein, a straightforward yet feasible method to prepare WFeRu ternary alloying catalyst on nickel foam is demonstrated, whereby the foreign W, Fe, and Ru metal atoms diffuse into the Ni foam resulting in the formation of inner immobilized ternary alloy. Thanks to the synergistic impact of foreign metal atoms and structural robustness of inner immobilized alloying catalyst, the well-designed WFeRu@NF self-standing anode exhibits superior OER activities. It only requires overpotentials of 245 and 346 mV to attain current densities of 20 and 500 mA cm-2, respectively. Moreover, the as-prepared ternary alloying catalyst also exhibits a long-term stability at a high-current-density of 500 mA cm-2 for over 45 h, evidencing the inner-immobilization strategy is promising for the development of highly active and stable metal-based catalysts for high-density-current water oxidation process.

12.
Small ; 20(35): e2400646, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38686673

RESUMO

The elastic interaction between kinks (and antikinks) within domain walls plays a pivotal role in shaping the domain structure, and their dynamics. In bulk materials, kinks interact as elastic monopoles, dependent on the distance between walls (d-1) and typically characterized by a rigid and straight domain configuration. In this work the evolution of the domain structure is investigated, as the sample size decreases, by the means of in situ heating microscopy techniques on free-standing samples. As the sample size decreases, a significant transformation is observed: domain walls exhibit pronounced curvature, accompanied by an increase in both domain wall and junction density. This transformation is attributed to the pronounced influence of kinks, inducing sample warping, where "dipole-dipole" interactions are dominant (d-2). Moreover, a critical thickness range that delineates a crossover between the monopolar and dipolar regimens is experimentally identified and corroborated by atomic simulations. These findings are relevant for in situ TEM studies and for the development of novel devices based on free-standing ferroic thin films and nanomaterials.

13.
Small ; : e2404307, 2024 Sep 06.
Artigo em Inglês | MEDLINE | ID: mdl-39240072

RESUMO

Free-standing micro-supercapacitor (MSC) devices without substrate or current collectors are promising for practical applications. However, it is still difficult to prepare high-performance free-standing MSC devices because of the requirement of optimized active sites, conductivity, ion diffusion, controlled patterns, moisture susceptibility, etc. Here, it is proposed that the optimization of oxygen level on graphene is promising to solve these requirements because of the balance of sp2 and sp3 hybridization. Using the medium-oxidized graphene, the flexible, conductive, hydro-stable, easy-processing film can be facilely obtained, which facilitates the preparation of free-standing MSC electrodes. After constructing with gel electrolyte, the free-standing MSC device shows a high capacitance of 898.4 mF cm-2 using aqueous-gel electrolyte and 383.6 mF cm-2 using ion-gel electrolyte with mass loading of ca. 10 mg cm-2. Correspondingly, the MSC device can achieve a landmark energy density of 42.6 µWh cm-2 at 0.85 mW cm-2 (7.1 mWh cm-3 at 141.7 mW cm-3). The advantages of high performance, facile preparation, and low inactive components make the free-standing MSC device promising for practical applications.

14.
Small ; : e2403915, 2024 Jul 07.
Artigo em Inglês | MEDLINE | ID: mdl-38973115

RESUMO

In 2D materials, a key engineering challenge is the mass production of large-area thin films without sacrificing their uniform 2D nature and unique properties. Here, it is demonstrated that a simple fluid phenomenon of water/alcohol solvents can become a sophisticated tool for self-assembly and designing organized structures of 2D nanosheets on a water surface. In situ, surface characterizations show that water/alcohol droplets of 2D nanosheets with cationic surfactants exhibit spontaneous spreading of large uniform monolayers within 10 s. Facile transfer of the monolayers onto solid or flexible substrates results in high-quality mono- and multilayer films with high coverages (>95%) and homogeneous electronic/optical properties. This spontaneous spreading is quite general and can be applied to various 2D nanosheets, including metal oxides, graphene oxide, h-BN, MoS2, and transition metal carbides, enabling on-demand smart manufacture of large-size (>4 inchϕ) 2D nanofilms and free-standing membranes.

15.
Small ; 20(29): e2310978, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38513253

RESUMO

Rechargeable sodium chloride (Na-Cl2) batteries have emerged as promising alternatives for next-generation energy storage due to their superior energy density and sodium abundance. However, their practical applications are hindered by the sluggish chlorine cathode kinetics related to the aggregation of NaCl and its difficult transformation into Cl2. Herein, the study, for the first time from the perspective of electrode level in Na-Cl2 batteries, proposes a free-standing carbon cathode host with customized vertical channels to facilitate the SOCl2 transport and regulate the NaCl deposition. Accordingly, electrode kinetics are significantly enhanced, and the deposited NaCl is distributed evenly across the whole electrode, avoiding the blockage of pores in the carbon host, and facilitating its oxidation to Cl2. With this low-polarization cathode, the Na-Cl2 batteries can deliver a practically high areal capacity approaching 4 mAh cm-2 and a long cycle life of over 170 cycles. This work demonstrates the significance of pore engineering in electrodes for mediating chlorine conversion kinetics in rechargeable alkali-metal-Cl2 batteries.

16.
Small ; 20(28): e2400222, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38477688

RESUMO

Proton-conducting metal-organic frameworks (MOFs) have attracted attention as potential electrolytes for fuel cells. However, research progress in utilizing MOFs as electrolytes for fuel cells has been limited, mainly due to challenges associated with issues such as the fabrication of MOF membranes, and hydrogen crossover through the MOF's pores. Here, proton conductivity and fuel cell performance of a self-standing membrane prepared from of a bismuth subgallate MOF nanosheets with non-porous structure are reported. The fabricated MOF nanosheet membrane with no binding agent exhibits structural anisotropy. The proton conductivity in the membrane thickness direction (4.4 × 10-3 S cm-1) at 90 °C and RH 100% is observed to be higher than that in the in-plane direction of the membrane (3.3 × 10-5 S cm-1). The open circuit voltage (OCV) of a fuel cell with ≈120 µm proton conducting membrane is 1.0 V. The non-porous nature of the MOF nanosheets contributes to the relatively high OCV. A fuel cell using ≈40 µm membrane as proton conducting electrolyte records a maximum of 25 mW cm-2 power density and a maximum of 109 mA cm-2 current density with 0.91 V OCV at 80 °C in humid conditions.

17.
Small ; 20(31): e2311675, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38441359

RESUMO

The high oxygen electrocatalytic overpotential of flexible cathodes due to sluggish reaction kinetics result in low energy conversion efficiency of wearable zinc-air batteries (ZABs). Herein, lignin, as a 3D flexible carbon-rich macromolecule, is employed for partial replacement of polyacrylonitrile and constructing flexible freestanding air electrodes (FFAEs) with large amount of mesopores and multi-hollow channels via electrospinning combined with annealing strategy. The presence of lignin with disordered structure decreases the graphitization of carbon fibers, increases the structural defects, and optimizes the pore structure, facilitating the enhancement of electron-transfer kinetics. This unique structure effectively improves the accessibility of graphitic-N/pyridinic-N with oxygen reduction reaction (ORR) activity and pyridinic-N with oxygen evolution reaction (OER) activity for FFAEs, accelerating the mass transfer process of oxygen-active species. The resulting N-doped hollow carbon fiber films (NHCFs) exhibit superior bifunctional ORR/OER performance with a low potential difference of only 0.60 V. The rechargeable ZABs with NHCFs as metal-free cathodes possess a long-term cycling stability. Furthermore, the NHCFs can be used as FFAEs for flexible ZABs which have a high specific capacity and good cycling stability under different bending states. This work paves the way to design and produce highly active metal-free bifunctional FFAEs for electrochemical energy devices.

18.
Small ; : e2400845, 2024 Jun 16.
Artigo em Inglês | MEDLINE | ID: mdl-38881161

RESUMO

Na2Ti3O7-based anodes show great promise for Na+ storage in sodium-ion batteries (SIBs), though the effect of Na2Ti3O7 morphology on battery performance remains poorly understood. Herein, hydrothermal syntheses is used to prepare free-standing Na2Ti3O7 nanosheets or Na2Ti3O7 nanotubes on Ti foil substrates, with the structural and electrochemical properties of the resulting electrodes explored in detail. Results show that the Na2Ti3O7 nanosheet electrode (NTO NSs) delivered superior performance in terms of reversible capacity, rate capability, and especially long-term durability in SIBs compared to its nanotube counterpart (NTO NTs). Electrochemical impedance spectroscopy (EIS) and scanning electron microscopy (SEM) investigations, combined with density functional theory calculations, demonstrated that the flexible 2D Na2Ti3O7 nanosheets are mechanically more robust than the rigid Na2Ti3O7 nanotube arrays during prolonged battery cycling, explaining the superior durability of the NTO NSs electrode. This work prompts the use of anodes based on Na2Ti3O7 nanosheets in the future development of high-performance SIBs.

19.
Small ; 20(20): e2307621, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38111987

RESUMO

Layered double hydroxides (LDHs) are a class of functional materials that exhibit exceptional properties for diverse applications in areas such as heterogeneous catalysis, energy storage and conversion, and bio-medical applications, among others. Efforts have been devoted to produce millimeter-scale LDH structures for direct integration into functional devices. However, the controlled synthesis of self-supported continuous LDH materials with hierarchical structuring up to the millimeter scale through a straightforward one-pot reaction method remains unaddressed. Herein, it is shown that millimeter-scale self-supported LDH structures can be produced by means of a continuous flow microfluidic device in a rapid and reproducible one-pot process. Additionally, the microfluidic approach not only allows for an "on-the-fly" formation of unprecedented LDH composite structures, but also for the seamless integration of millimeter-scale LDH structures into functional devices. This method holds the potential to unlock the integrability of these materials, maintaining their performance and functionality, while diverging from conventional techniques like pelletization and densification that often compromise these aspects. This strategy will enable exciting advancements in LDH performance and functionality.

20.
Small ; : e2400812, 2024 Jun 07.
Artigo em Inglês | MEDLINE | ID: mdl-38845480

RESUMO

Manufacturing high-performance and cost-affordable non-metallic, electroactive 1D carbon material for energy storage and hydrogen evolution reaction (HER) is of foremost importance to respond positively to the impending energy crisis. Porous N-doped carbon nanofiber (PNCNF) is successfully synthesized by electrospinning, using selenium nanoparticles as a sacrificial template (where Se is reutilized for ZIF-67 selenization as a bi-process, and the surface of PNCNF is modified with poly(3,4-ethylenedioxythiophene) (PNCNT/PEDOT) by electropolymerization. The prepared materials are found ideal for energy storage (supercapacitor) and electrocatalysis (HER). The bi-functional material has shown excellent energy storage capability with the specific capacitance (CS) of 230 F g-1 (PNCNF) and 395 F g-1 (PNCNF/PEDOT), and the symmetric supercapacitor device, PNCNF/PEDOT//PEDOT/PNCNF, exhibits 32.4 Wh kg-1 energy density at 14400 W kg-1 power density with 96.6% Coulombic efficiency and 106% CS at the end of 5000 charge-discharge cycles. The rate capability of the symmetric supercapacitor cell of PNCNF/PEDOT is 51% for the current density increase from 1 to 8 A g-1, while that of PNCNF is a meager 29% only. Electrocatalytic HER at the PNCNF electrode is achieved with an overpotential of 281 mV@10 mA cm-2 relative to the Pt/C electrode and a low Tafel slop value of 96 mV dec-1.

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