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Prussian blue analogues (PBAs), representing the typical faradaic electrode materials for efficient capacitive deionization (CDI) due to their open architecture and high capacity, have been plagued by kinetics issues, leading to insufficient utilization of active sites and poor structure stability. Herein, to address the conflict issue between desalination capacity and stability due to mismatched ionic and electronic kinetics for the PBA-based electrodes, a rational design, including Mn substitution and polypyrrole (ppy) connection, has been proposed for the nickel hexacyanoferrate (Mn-NiHCF/ppy), serving as a model case. Particularly, the theoretical calculation manifests the reduced bandgap and energy barrier for ionic diffusion after Mn substitution, combined with the increased electronic conductivity and integrity through ppy connecting, resulting in enhanced redox kinetics and boosted desalination performance. Specifically, the optimized Mn-NiHCF/ppy demonstrates a remarkable desalination capacity of 51.8 mg g-1 at 1.2 V, accompanied by a high charge efficiency of 81%, and excellent cycling stability without obvious degradation up to 50 cycles, outperforming other related materials. Overall, our concept shown herein provides insights into the design of advanced faradaic electrode materials for high-performance CDI.
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This work reports the use of defect engineering and carbon supporting to achieve metal-doped phosphides with high activities and stabilities for the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER) in alkaline media. Specifically, the nitrogen-doped carbon nanofiber-supported Ni-doped CoP3 with rich P defects (Pv·) on the carbon cloth (p-NiCoP/NCFs@CC) is synthesized through a plasma-assisted phosphorization method. The p-NiCoP/NCFs@CC is an efficient and stable catalyst for the HER and the OER. It only needs overpotentials of 107 and 306 mV to drive 100 mA cm-2 for the HER and the OER, respectively. Its catalytic activities are higher than those of other catalysts reported recently. The high activities of the p-NiCoP/NCFs@CC mainly arise from its peculiar structural features. The density functional theory calculation indicates that the Pv· richness, the Ni doping, and the carbon supporting can optimize the adsorption of the H atoms at the catalyst surface and promote the strong electronic couplings between the carbon nanofiber-supported p-NiCoP with the surface oxide layer formed during the OER process. This gives the p-NiCoP/NCFs@CC with the high activities for the HER and the OER. When used in alkaline water electrolyzers, the p-NiCoP/NCFs@CC shows the superior activity and excellent stability for overall water splitting.
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Generation and manipulation of three-dimensional (3D) optical polarization structures have received considerable interest because of their distinctive optical features and potential applications. However, the realization of multiple 3D polarization structures in a queue along the light propagation direction has not yet been reported. We propose and experimentally demonstrate a metalens to create longitudinally variable 3D polarization knots. A single metalens can simultaneously generate three distinct 3D polarization knots, which are indirectly validated with a rotating polarizer. The 3D polarization profiles are dynamically modulated by manipulating the linear polarization direction of the incident light. We further showcase the 3D image steganography with the generated 3D polarization structures. The ultrathin nature of metasurfaces and unique properties of the developed metalenses hold promise for lightweight polarization systems applicable to areas such as 3D image steganography and virtual reality.
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The open NASICON framework and high reversible capacity enable Na3V2(PO4)3 (NVP) to be a highly promising cathode candidate for sodium-ion batteries (SIBs). Nevertheless, the unsatisfied cyclic stability and degraded rate capability at low temperatures due to sluggish ionic migration and poor conductivity become the main challenges. Herein, excellent sodium storage performance for the NVP cathode can be received by partial potassium (K) substitution and multiwalled carbon nanotube (MWCNT) cross-linking to modify the ionic diffusion and electronic conductivity. Consequently, the as-fabricated Na3-xKxV2(PO4)3@C/MWCNT can maintain a capacity retention of 79.4% after 2000 cycles at 20 C. Moreover, the electrochemical tests at -20 °C manifest that the designed electrode can deliver 89.7, 73.5, and 64.8% charge of states, respectively, at 1, 2, and 3 C, accompanied with a capacity retention of 84.3% after 500 cycles at 20 C. Generally, the improved electronic conductivity and modified ionic diffusion kinetics resulting from K doping and MWCNT interconnecting endows the resultant Na3-xKxV2(PO4)3@C/MWCNT with modified electrochemical polarization and improved redox reversibility, contributing to superior performance at low temperatures. Generally, this study highlights the potential of alien substitution and carbon hybridization to improve the NASICON-type cathodes toward high-performance SIBs, especially at low temperatures.
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RAS mutations are among the most prevalent oncogenic drivers in cancers. RAS proteins propagate signals only when associated with cellular membranes as a consequence of lipid modifications that impact their trafficking. Here, we discovered that RAB27B, a RAB family small GTPase, controlled NRAS palmitoylation and trafficking to the plasma membrane, a localization required for activation. Our proteomic studies revealed RAB27B upregulation in CBL- or JAK2-mutated myeloid malignancies, and its expression correlated with poor prognosis in acute myeloid leukemias (AMLs). RAB27B depletion inhibited the growth of CBL-deficient or NRAS-mutant cell lines. Strikingly, Rab27b deficiency in mice abrogated mutant but not WT NRAS-mediated progenitor cell growth, ERK signaling, and NRAS palmitoylation. Further, Rab27b deficiency significantly reduced myelomonocytic leukemia development in vivo. Mechanistically, RAB27B interacted with ZDHHC9, a palmitoyl acyltransferase that modifies NRAS. By regulating palmitoylation, RAB27B controlled c-RAF/MEK/ERK signaling and affected leukemia development. Importantly, RAB27B depletion in primary human AMLs inhibited oncogenic NRAS signaling and leukemic growth. We further revealed a significant correlation between RAB27B expression and sensitivity to MEK inhibitors in AMLs. Thus, our studies presented a link between RAB proteins and fundamental aspects of RAS posttranslational modification and trafficking, highlighting future therapeutic strategies for RAS-driven cancers.
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Leucemia Mieloide , Lipoilação , Humanos , Animais , Camundongos , Proteômica , Transdução de Sinais , Quinases de Proteína Quinase Ativadas por Mitógeno , Proteínas de Membrana/genética , GTP Fosfo-HidrolasesRESUMO
A lightweight and portable spectrometer is desirable for miniaturization and integration. The unprecedented capability of optical metasurfaces has shown much promise to perform such a task. We propose and experimentally demonstrate a compact high-resolution spectrometer with a multi-foci metalens. The novel metalens is designed based on wavelength and phase multiplexing, which can accurately map the wavelength information into its focal points located on the same plane. The measured wavelengths in the light spectra agree with simulation results upon the illumination of various incident light spectra. The uniqueness of this technique lies in the novel metalens that can simultaneously realize wavelength splitting and light focusing. The compactness and ultrathin nature of the metalens spectrometer render this technology have potential applications in on-chip integrated photonics where spectral analysis and information processing can be performed in a compact platform.
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The piezoelectric effect has been widely observed in biological systems, and its applications in biomedical field are emerging. Recent advances of wearable and implantable biomedical devices bring promise as well as requirements for the piezoelectric materials building blocks. Owing to their biocompatibility, biosafety, and environmental sustainability, natural piezoelectric biomaterials are known as a promising candidate in this emerging field, with a potential to replace conventional piezoelectric ceramics and synthetic polymers. Herein, we provide a thorough review of recent progresses of research on five major types of piezoelectric biomaterials including amino acids, peptides, proteins, viruses, and polysaccharides. Our discussion focuses on their structure- and phase-related piezoelectric properties and fabrication strategies to achieve desired piezoelectric phases. We compare and analyze their piezoelectric performance and further introduce and comment on the approaches to improve their piezoelectric property. Representative biomedical applications of this group of functional biomaterials including energy harvesting, sensing, and tissue engineering are also discussed. We envision that molecular-level understanding of the piezoelectric effect, piezoelectric response improvement, and large-scale manufacturing are three main challenges as well as research and development opportunities in this promising interdisciplinary field.
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Materiais Biocompatíveis , Engenharia Tecidual , Materiais Biocompatíveis/química , Polímeros/química , Aminoácidos/química , ProteínasRESUMO
Polarization as an important degree of freedom for light plays a key role in optics. Structured beams with controlled polarization profiles have diverse applications, such as information encoding, display, medical and biological imaging, and manipulation of microparticles. However, conventional polarization optics can only realize two-dimensional polarization structures in a transverse plane. The emergent ultrathin optical devices consisting of planar nanostructures, so-called metasurfaces, have shown much promise for polarization manipulation. Here we propose and experimentally demonstrate color-selective three-dimensional (3D) polarization structures with a single metasurface. The geometric metasurfaces are designed based on color and phase multiplexing and polarization rotation, creating various 3D polarization knots. Remarkably, different 3D polarization knots in the same observation region can be achieved by controlling the incident wavelengths, providing unprecedented polarization control with color information in 3D space. Our research findings may be of interest to many practical applications such as vector beam generation, virtual reality, volumetric displays, security, and anti-counterfeiting.
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We present a tunable plasmon-induced transparency (PIT) metamaterial for manipulating the group velocity of terahertz (THz) waves. The metamaterial is composed of metal split rings and photoconductive silicon strips. The strong PIT effect with slowing down THz waves is generated by the bright-bright mode coupling between the high-order plasmon mode and the lattice surface mode via electromagnetic destructive interference. By varying the conductivity of silicon strips, the group slowing performance is dynamically tunable. The group delay can achieve beyond 20 ps with the group index as high as 592, showing the promising application for THz signal manipulation.
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Computer-generated holography typically generates terahertz (THz) holographic images with a pixel size larger than wavelength. We propose a multi-foci metalens model to reconstruct THz holographic images with subwavelength resolution. The designed devices are realized based on dielectric metasurfaces consisting of silicon micropillars with spatially variant orientations. By exploiting quasi-continuous profile of focal points as the pixels of a holographic image, a metalens can reconstruct a high-resolution target image on its focal plane. The effects of size and pitch of each sub-diffraction focal point on imaging quality and pixel resolution are discussed. The intensity distribution at each focal point indicates that the reconstructed images have subwavelength resolution. In comparison with conventional hologram designs, this design method can be used to reconstruct THz holographic images with subwavelength resolution, which have potential applications in THz communication, information security and anti-counterfeiting.
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Nanostructured piezoelectric semiconductors offer unprecedented opportunities for high-performance sensing in numerous catalytic processes of biomedical, pharmaceutical, and agricultural interests, leveraging piezocatalysis that enhances the catalytic efficiency with the strain-induced piezoelectric field. Here, a cost-efficient, high-performance piezo-electrocatalytic sensor for detecting l-ascorbic acid (AA), a critical chemical for many organisms, metabolic processes, and medical treatments, is designed and demonstrated. Zinc oxide (ZnO) nanorods and nanosheets are prepared to characterize and compare their efficacy for the piezo-electrocatalysis of AA. The electrocatalytic efficacy of AA is significantly boosted by the piezoelectric polarization induced in the nanostructured semiconducting ZnO catalysts. The charge transfer between the strained ZnO nanostructures and AA is elucidated to reveal the mechanism for the related piezo-electrocatalytic process. The low-temperature synthesis of high-quality ZnO nanostructures allows low-cost, scalable production, and integration directly into wearable electrocatalytic sensors whose performance can be boosted by otherwise wasted mechanical energy from the working environment, for example, human-generated mechanical signals.
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Spatial manipulation of nanoparticles (NPs) in a controlled manner is critical for the fabrication of 3D hybrid materials with unique functions. However, traditional fabrication methods such as electron-beam lithography and stereolithography are usually costly and time-consuming, precluding their production on a large scale. Herein, for the first time the ultrafast laser direct writing is combined with external magnetic field (MF) to massively produce graphene-coated ultrafine cobalt nanoparticles supported on 3D porous carbon using metal-organic framework crystals as precursors (5 × 5 cm2 with 10 s). The MF-confined picosecond laser scribing not only reduces the metal ions rapidly but also aligns the NPs in ultrafine and evenly distributed order (from 7.82 ± 2.37 to 3.80 ± 0.84 nm). ≈400% increment of N-Q species within N compositionis also found as the result of the special MF-induced laser plasma plume. (). The importance of MF is further exmined by electrochemical water-splitting tests. Significant overpotential improvements of 90 and 150 mV for oxygen evolution reaction and hydrogen evolution reaction are observed, respectively, owing to the MF-induced alignment of the NPs and controlled elemental compositions. This work provides a general bottom-up approach for the synthesis of metamaterials with high outputs yet a simple setup.
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Elemental two-dimensional (2D) materials have emerged as promising candidates for energy and catalysis applications due to their unique physical, chemical, and electronic properties. These materials are advantageous in offering massive surface-to-volume ratios, favorable transport properties, intriguing physicochemical properties, and confinement effects resulting from the 2D ultrathin structure. In this review, we focus on the recent advances in emerging energy and catalysis applications based on beyond-graphene elemental 2D materials. First, we briefly introduce the general classification, structure, and properties of elemental 2D materials and the new advances in material preparation. We then discuss various applications in energy harvesting and storage, including solar cells, piezoelectric and triboelectric nanogenerators, thermoelectric devices, batteries, and supercapacitors. We further discuss the explorations of beyond-graphene elemental 2D materials for electrocatalysis, photocatalysis, and heterogeneous catalysis. Finally, the challenges and perspectives for the future development of elemental 2D materials in energy and catalysis are discussed.
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Three-dimensional (3D) light fields with spatially inhomogeneous polarization and intensity distributions play an increasingly important role in photonics due to their peculiar optical features and extra degrees of freedom for carrying information. However, it is very challenging to simultaneously control the intensity profile and polarization profile in an arbitrary manner. Here we experimentally demonstrate a metalens that can focus light into an arbitrarily shaped focal curve with a predefined polarization distribution. The efficacy of this approach is exemplified through the demonstration of focused curves in 3D space ranging from simple shapes such as a circle to topologically nontrivial objects such as a 3D knot with controlled local polarization states. This powerful control of the light field would be technically challenging with their conventional counterparts. Our demonstration may find applications in beam engineering and integration optics.
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We present a tunable plasmon-induced transparency (PIT) structure that is composed of dielectric grating and a graphene system to manipulate terahertz (THz) waves. The graphene system consists of a graphene sheet and a graphene ribbon layer, with a spacer between them. By exploiting the diffraction coupling of THz wave with dielectric grating, graphene plasmonic resonance is efficiently excited on both graphene sheet and graphene ribbons. This leads to the surface plasmon mode of the graphene sheet and the localized plasmon mode of the graphene ribbons. The coupling between the two-plasmon modes via near-field destructive interference generates a strong PIT effect with slowing the group velocity of THz waves. A group delay over 0.2 ps and group index beyond 170 can be achievable. The group slowing effect is dynamically tunable with varying the Fermi level of graphene. The work suggests a promising scheme for on-chip graphene slow-wave devices at the THz regime.
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Trigonal tellurium (Te) is a chiral semiconductor that lacks both mirror and inversion symmetries, resulting in complex band structures with Weyl crossings and unique spin textures. Detailed time-resolved polarized reflectance spectroscopy is used to investigate its band structure and carrier dynamics. The polarized transient spectra reveal optical transitions between the uppermost spin-split H4 and H5 and the degenerate H6 valence bands (VB) and the lowest degenerate H6 conduction band (CB) as well as a higher energy transition at the L-point. Surprisingly, the degeneracy of the H6 CB (a proposed Weyl node) is lifted and the spin-split VB gap is reduced upon photoexcitation before relaxing to equilibrium as the carriers decay. Using ab initio density functional theory (DFT) calculations, we conclude that the dynamic band structure is caused by a photoinduced shear strain in the Te film that breaks the screw symmetry of the crystal. The band-edge anisotropy is also reflected in the hot carrier decay rate, which is a factor of two slower along the c-axis than perpendicular to it. The majority of photoexcited carriers near the band-edge are seen to recombine within 30 ps while higher lying transitions observed near 1.2 eV appear to have substantially longer lifetimes, potentially due to contributions of intervalley processes in the recombination rate. These new findings shed light on the strong correlation between photoinduced carriers and electronic structure in anisotropic crystals, which opens a potential pathway for designing novel Te-based devices that take advantage of the topological structures as well as strong spin-related properties.
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We propose a reflective terahertz (THz) metalens with four focal points for polarization detection of THz beams. The metalens is composed of Z-shaped resonators with spatially variant orientations, a reflective gold layer, and a dielectric spacer between them. The polarization states of the focal points include left circular polarization, right circular polarization, an incident polarization state, and a polarization state whose major axis is rotated π/4 in comparison with that of the incident polarization. The handedness, ellipticity, and major axis of the polarization state can be determined based on the light intensities of the focal points. The uniqueness of the designed device renders this technique very attractive for applications in compact THz polarization detection and information processing.
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The capability of sensor systems to efficiently scavenge their operational power from stray, weak environmental energies through sustainable pathways could enable viable schemes for self-powered health diagnostics and therapeutics. Triboelectric nanogenerators (TENG) can effectively transform the otherwise wasted environmental, mechanical energy into electrical power. Recent advances in TENGs have resulted in a significant boost in output performance. However, obstacles hindering the development of efficient triboelectric devices based on biocompatible materials continue to prevail. Being one of the most widely used polymers for biomedical applications, polyvinyl alcohol (PVA) presents exciting opportunities for biocompatible, wearable TENGs. Here, the holistic engineering and systematic characterization of the impact of molecular and ionic fillers on PVA blends' triboelectric performance is presented for the first time. Triboelectric devices built with optimized PVA-gelatin composite films exhibit stable and robust triboelectricity outputs. Such wearable devices can detect the imperceptible skin deformation induced by the human pulse and capture the cardiovascular information encoded in the pulse signals with high fidelity. The gained fundamental understanding and demonstrated capabilities enable the rational design and holistic engineering of novel materials for more capable biocompatible triboelectric devices that can continuously monitor vital physiological signals for self-powered health diagnostics and therapeutics.
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Materiais Biocompatíveis/química , Fenômenos Fisiológicos Cardiovasculares , Engenharia , Monitorização Fisiológica/instrumentação , Álcool de Polivinil/química , Dispositivos Eletrônicos Vestíveis , Fontes de Energia Elétrica , Fenômenos MecânicosRESUMO
We present, by simulations, a metastructured graphene/liquid crystal hybrid tuning terahertz perfect absorber that consists of graphene disk resonator arrays above a metallic layer separated with liquid crystal substrate. The liquid crystal refractive index and the graphene Fermi level are utilized to implement double-tuning operation to push the spectra scanning limit of the terahertz absorber. Our simulations demonstrate high performance of a near-linear broad tuning region and near-unity absorbance with wide incident angle and polarization independence. The range of the resonant frequency scan is notably enlarged at a spectral ratio of as high as Δf/f=50% while ensuring absorbance beyond 90%. Such graphene/liquid crystal hybrid tuning scheme would be preferable to push the working-band limit of terahertz perfect absorbers.