Showing papers in "Nano Letters in 2019"
TL;DR: A highly sensitive, flexible, and degradable pressure sensor fabricated by sandwiching porous MXene-impregnated tissue paper between a biodegradable polylactic acid (PLA) thin sheet and an interdigitated electrode-coated PLA thin sheet that exhibits high sensitivity with a low detection limit, broad range, fast response, and robust environmental degradability.
Abstract: Flexible and degradable pressure sensors have received tremendous attention for potential use in transient electronic skins, flexible displays, and intelligent robotics due to their portability, re...
476 citations
TL;DR: The animal studies reveal that the AGL AIE dots have the innate property of fast afterglow signal quenching in normal tissues, including the liver, spleen, and kidney, which enables them to give excellent performance in precise image-guided cancer surgery.
Abstract: Afterglow imaging through the collection of persistent luminescence after the stopping of light excitation holds enormous promise for advanced biomedical uses. However, efficient near-infrared (NIR)-emitting afterglow luminescent materials and probes (particularly the organic and polymeric ones) are still very limited, and their in-depth biomedical applications such as precise image-guided cancer surgery are rarely reported. Here, we design and synthesize a NIR afterglow luminescent nanoparticle with aggregation-induced emission (AIE) characteristics (named AGL AIE dots). It is demonstrated that the AGL AIE dots emit rather-high NIR afterglow luminescence persisting over 10 days after the stopping of a single excitation through a series of processes occurring in the AIE dots, including singlet oxygen production by AIE luminogens (AIEgens), Schaap's dioxetane formation, chemiexcitation by dioxetane decomposition, and energy transfer to NIR-emitting AIEgens. The animal studies reveal that the AGL AIE dots have the innate property of fast afterglow signal quenching in normal tissues, including the liver, spleen, and kidney. After the intravenous injection of AGL AIE dots into peritoneal carcinomatosis bearing mice, the tumor-to-liver ratio of afterglow imaging is nearly 100-fold larger than that for fluorescence imaging. The ultrahigh tumor-to-liver signal ratio, together with low afterglow background noise, enables AGL AIE dots to give excellent performance in precise image-guided cancer surgery.
350 citations
TL;DR: The hole injection barrier of electroluminescent LEDs was effectively eliminated by using alloyed CsPb0.64Zn0.36I3 nanocrystals, and a high peak external quantum efficiency of 15.1% has been achieved.
Abstract: We alloyed Zn2+ into CsPbI3 perovskite nanocrystals by partial substitution of Pb2+ with Zn2+, which does not change their crystalline phase. The resulting alloyed CsPb0.64Zn0.36I3 nanocrystals exhibited an improved, close-to-unity photoluminescence quantum yield of 98.5% due to the increased radiative decay rate and the decreased non-radiative decay rate. They also showed an enhanced stability, which correlated with improved effective Goldschmidt tolerance factors, by the incorporation of Zn2+ ions with a smaller radius than the Pb2+ ions. Simultaneously, the nanocrystals switched from n-type (for CsPbI3) to nearly ambipolar for the alloyed nanoparticles. The hole injection barrier of electroluminescent LEDs was effectively eliminated by using alloyed CsPb0.64Zn0.36I3 nanocrystals, and a high peak external quantum efficiency of 15.1% has been achieved.
342 citations
TL;DR: The analog conductance modulation behavior in the ferroElectric thin-film transistors (FeTFT) that have the nanoscale ferroelectric material and oxide semiconductors is demonstrated to demonstrate linear potentiation and depression characteristics of FeTFTs.
Abstract: Neuromorphic computing is a promising alternative to conventional computing systems as it could enable parallel computation and adaptive learning process. However, the development of energy efficient neuromorphic hardware systems has been hindered by the limited performance of analog synaptic devices. Here, we demonstrate the analog conductance modulation behavior in the ferroelectric thin-film transistors (FeTFT) that have the nanoscale ferroelectric material and oxide semiconductors. Accurate control of polarization changes in the nanoscale ferroelectric layer induces conductance modulation to demonstrate linear potentiation and depression characteristics of FeTFTs. Our devices show potentiation and depression properties, including high linearity, multiple states, and small cycle-to-cycle/device-to-device variations. In simulations with measured properties, a neuromorphic system with FeTFT achieves 91.1% recognition accuracy of handwritten digits. This work may provide a way to realize the neuromorphic hardware systems that use FeTFTs as the synaptic devices.
332 citations
TL;DR: The concise fabrication of biocompatible BSO/GA-Fe(II)@liposome is presented as an effective adjuvant nanomedicine to promote clinically used conventional cancer chemotherapy and radiotherapy, by greatly amplifying the intratumoral oxidative stress.
Abstract: Amplification of intracellular oxidative stress has been found to be an effective strategy to induce cancer cell death. To this end, we prepare a unique type of ultrasmall gallic acid-ferrous (GA–Fe(II)) nanocomplexes as the catalyst of Fenton reaction to enable persistent conversion of H2O2 to highly cytotoxic hydroxyl radicals (•OH). Then, both GA–Fe(II) and l-buthionine sulfoximine (BSO), an inhibitor of glutathione (GSH) synthesis, are coencapsulated within a stealth liposomal nanocarrier. Interestingly, the obtained BSO/GA–Fe(II)@liposome is able to efficiently amplify intracellular oxidative stress via increasing •OH generation and reducing GSH biosynthesis. After chelating with 99mTc4+ radioisotope, such BSO/GA–Fe(II)@liposome could be tracked under in vivo single-photon-emission-computed-tomography (SPECT) imaging, which illustrates the time-dependent tumor homing of such liposomal nanoparticles after intravenous injection. With GA–Fe(II)-mediated •OH production and BSO-mediated GSH depletion, tre...
317 citations
TL;DR: The strategy developed in this work can be generally applied for enhancing the ion storage capacity of metal chalcogenides and other layered materials, making them promising cathodes for challenging multivalent ion batteries.
Abstract: Aqueous Zn-ion batteries present low-cost, safe, and high-energy battery technology but suffer from the lack of suitable cathode materials because of the sluggish intercalation kinetics associated with the large size of hydrated zinc ions. Herein we report an effective and general strategy to transform inactive intercalation hosts into efficient Zn2+ storage materials through intercalation energy tuning. Using MoS2 as a model system, we show both experimentally and theoretically that even hosts with an originally poor Zn2+ diffusivity can allow fast Zn2+ diffusion. Through simple interlayer spacing and hydrophilicity engineering that can be experimentally achieved by oxygen incorporation, the Zn2+ diffusivity is boosted by 3 orders of magnitude, effectively enabling the otherwise barely active MoS2 to achieve a high capacity of 232 mAh g–1, which is 10 times that of its pristine form. The strategy developed in our work can be generally applied for enhancing the ion storage capacity of metal chalcogenides ...
316 citations
TL;DR: A novel Pt-CuS Janus composed of hollow semiconductor CuS and noble metallic Pt was rationally designed and successfully synthesized and develops a versatile nanoplatform for a multifunctional theranostic strategy and broadens the biological applications by rationally designing their structure.
Abstract: As a noninvasive treatment modality, ultrasound (US)-triggered sonodynamic therapy (SDT) shows broad and promising applications to overcome the drawbacks of traditional photodynamic therapy (PDT) in combating cancer. However, the SDT efficacy is still not satisfactory without oxygen (O2) assistance. In addition, there is also much space to explore the SDT-based synergistic therapeutic modalities. Herein, a novel Pt-CuS Janus composed of hollow semiconductor CuS and noble metallic Pt was rationally designed and successfully synthesized. The hollow CuS shows a large inner cavity for loading sonosensitizer molecules (tetra-(4-aminophenyl) porphyrin, TAPP) to implement SDT. Moreover, the deposition of Pt not only enhances photothermal performance compared with those of CuS nanoparticles (NPs) due to the effect of the local electric field enhancement but also possesses nanozyme activity for catalyzing decomposition of endogenous overexpressed hydrogen peroxide (H2O2) to produce O2 that can overcome tumor hypoxia and augment the SDT-induced highly toxic reactive oxygen species (ROS) production for efficient cancer cell apoptosis. Importantly, the generated heat of Pt-CuS by 808 nm laser irradiation can accelerate the catalytic activity of Pt and elevate the O2 level that further facilitates SDT efficacy. Interestingly, the thermally sensitive copolymer coated around the Janus can act as a smart switch to regulate the catalytic ability of Pt and control TAPP release that has a significant effect on modulating the therapeutic effect. The synergistic catalysis-enhanced SDT efficiency and highly photothermal effect almost realized complete tumor resection without obvious reoccurrence and simultaneously displayed a highly therapeutic biosafety. Furthermore, the high optical absorbance allows the as-synthesized Pt-CuS Janus for photoacoustic (PA) imaging and NIR thermal imaging. This work develops a versatile nanoplatform for a multifunctional theranostic strategy and broadens the biological applications by rationally designing their structure.
289 citations
TL;DR: The intrinsic ferromagnetism in atomically thin monolayer CrBr3 is reported, directly probed by polarization resolved magneto-photoluminescence and attribute the layer-number-dependent hysteresis loops in thick layers to the magnetic domain structures.
Abstract: Atomically thin magnets are the key element to build up spintronics based on two-dimensional materials. The surface nature of two-dimensional ferromagnet opens up opportunities to improve the device performance efficiently. Here, we report the intrinsic ferromagnetism in atomically thin monolayer CrBr3, directly probed by polarization resolved magneto-photoluminescence. The spontaneous magnetization persists in monolayer CrBr3 with a Curie temperature of 34 K. The development of magnons by the thermal excitation is in line with the spin-wave theory. We attribute the layer-number-dependent hysteresis loops in thick layers to the magnetic domain structures. As a stable monolayer material in air, CrBr3 provides a convenient platform for fundamental physics and pushes the potential applications of the two-dimensional ferromagnetism.
272 citations
TL;DR: A strain-driven 90° lattice rotation is found in the magnetic VSSe monolayer with an extremely high reversal strain, indicating an intrinsic ferroelasticity and the combination of piezoelectricity and valley polarization make magnetic 2D Janus VSSe a tantalizing material for potential applications in nanoelectronics, optoelectronic, and valleytronics.
Abstract: Inspired by recent experiments on the successful fabrication of monolayer Janus transition-metal dichalcogenides [Lu, A.-Y.; Nat. Nanotechnol. 2017, 12, (8), 744 and ferromagnetic VSe2 [Bonilla, M.; Nat. Nanotechnol. 2018, 13, (4), 289], we predict a highly stable room-temperature ferromagnetic Janus monolayer (VSSe) by density functional theory methods and further confirmed the stability by a global minimum search with the particle-swarm optimization method. The VSSe monolayer exhibits a large valley polarization due to the broken space- and time-reversal symmetry. Moreover, its low symmetry C3v point group results in giant in-plane piezoelectric polarization. Most interestingly, a strain-driven 90° lattice rotation is found in the magnetic VSSe monolayer with an extremely high reversal strain (73%), indicating an intrinsic ferroelasticity. The combination of piezoelectricity and valley polarization make magnetic 2D Janus VSSe a tantalizing material for potential applications in nanoelectronics, optoelec...
254 citations
TL;DR: A global optimizer, based on a conditional generative neural network, which can output ensembles of highly efficient topology-optimized metasurfaces operating across a range of parameters, is presented.
Abstract: We present a global optimizer, based on a conditional generative neural network, which can output ensembles of highly efficient topology-optimized metasurfaces operating across a range of parameters. A key feature of the network is that it initially generates a distribution of devices that broadly samples the design space and then shifts and refines this distribution toward favorable design space regions over the course of optimization. Training is performed by calculating the forward and adjoint electromagnetic simulations of outputted devices and using the subsequent efficiency gradients for backpropagation. With metagratings operating across a range of wavelengths and angles as a model system, we show that devices produced from the trained generative network have efficiencies comparable to or better than the best devices produced by adjoint-based topology optimization, while requiring less computational cost. Our reframing of adjoint-based optimization to the training of a generative neural network applies generally to physical systems that can utilize gradients to improve performance.
250 citations
TL;DR: In this paper, it was shown that atomically thin CrCl3 is a layered antiferromagnetic insulator with an easy-plane normal to the c-axis, that is, the polarization is in the plane of each layer and has no preferred direction within it.
Abstract: The recent discovery of magnetism in atomically thin layers of van der Waals (vdW) crystals has created new opportunities for exploring magnetic phenomena in the two-dimensional (2D) limit. In most 2D magnets studied to date, the c-axis is an easy axis, so that at zero applied field the polarization of each layer is perpendicular to the plane. Here, we demonstrate that atomically thin CrCl3 is a layered antiferromagnetic insulator with an easy-plane normal to the c-axis, that is, the polarization is in the plane of each layer and has no preferred direction within it. Ligand-field photoluminescence at 870 nm is observed down to the monolayer limit, demonstrating its insulating properties. We investigate the in-plane magnetic order using tunneling magnetoresistance in graphene/CrCl3/graphene tunnel junctions, establishing that the interlayer coupling is antiferromagnetic down to the bilayer. From the temperature dependence of the magnetoresistance, we obtain an effective magnetic phase diagram for the bilayer. Our result shows that CrCl3 should be useful for studying the physics of 2D phase transitions and for making new kinds of vdW spintronic devices.
TL;DR: A vertical Memristor that sandwiches two MoS2 monolayers between an active Cu top electrode and an inert Au bottom electrode achieves consistent bipolar and analogue switching, and thus exhibits the synapse-like learning behavior such as the spike-timing dependent plasticity (STDP), the very first STDP demonstration among all 2D-material-based vertical memristors.
Abstract: Atomically thin two-dimensional (2D) materials-such as transition metal dichalcogenide (TMD) monolayers and hexagonal boron nitride (hBN)-and their van der Waals layered preparations have been actively researched to build electronic devices such as field-effect transistors, junction diodes, tunneling devices, and, more recently, memristors. Two-dimensional material memristors built in lateral form, with horizontal placement of electrodes and the 2D material layers, have provided an intriguing window into the motions of ions along the atomically thin layers. On the other hand, 2D material memristors built in vertical form with top and bottom electrodes sandwiching 2D material layers may provide opportunities to explore the extreme of the memristive performance with the atomic-scale interelectrode distance. In particular, they may help push the switching voltages to a lower limit, which is an important pursuit in memristor research in general, given their roles in neuromorphic computing. In fact, recently Akinwande et al. performed a pioneering work to demonstrate a vertical memristor that sandwiches a single MoS2 monolayer between two inert Au electrodes, but it could neither attain switching voltages below 1 V nor control the switching polarity, obtaining both unipolar and bipolar switching devices. Here, we report a vertical memristor that sandwiches two MoS2 monolayers between an active Cu top electrode and an inert Au bottom electrode. Cu ions diffuse through the MoS2 double layers to form atomic-scale filaments. The atomic-scale thickness, combined with the electrochemical metallization, lowers switching voltages down to 0.1-0.2 V, on par with the state of the art. Furthermore, our memristor achieves consistent bipolar and analogue switching, and thus exhibits the synapse-like learning behavior such as the spike-timing dependent plasticity (STDP), the very first STDP demonstration among all 2D-material-based vertical memristors. The demonstrated STDP with low switching voltages is promising not only for low-power neuromorphic computing, but also from the point of view that the voltage range approaches the biological action potentials, opening up a possibility for direct interfacing with mammalian neuronal networks.
TL;DR: This work proposes a novel fabrication method to introduce kirigami approach to pattern a highly conductive and transparent electrode into diverse shapes of stretchable electronics with multivariable configurability for E-skin applications and demonstrates human-machine-interface using stretchable transparent kirigsami electrodes.
Abstract: Recent research progress of relieving discomfort between electronics and human body involves serpentine designs, ultrathin films, and extraordinary properties of nanomaterials. However, these strat...
TL;DR: This work realized unprecedented long cycle life with high reversible capacity as well as outstanding rate capability for KIBs by embedding red P into free-standing nitrogen-doped porous hollow carbon nanofibers (red P@N-PHCNFs).
Abstract: Potassium-ion batteries (KIBs) are a promising alternative to lithium-ion batteries (LIBs) for large-scale renewable energy storage owning to the natural abundance and low cost of potassium. However, the biggest challenge for KIBs application lies in the lack of suitable electrode materials that can deliver long cycle life and high reversible capacity. In this work, we realized unprecedented long cycle life with high reversible capacity (465 mAh g–1 at 2 A g–1 after 800 cycles) as well as outstanding rate capability (342 mAh g–1 at 5 A g–1) for KIBs by embedding red P into free-standing nitrogen-doped porous hollow carbon nanofibers (red P@N-PHCNFs). This design circumvents the problems of pulverization and aggregation of P particles. The in situ transmission electron microscopy (TEM) investigation reveals the structural robustness of the composite fibers during potassiation. The formation of P–C chemical bonds as well as nitrogen doping in the carbon matrix can facilitate the sturdy contact and enhance t...
TL;DR: This work highlights a rationally designed tumor microenvironment-specific nanoreactor for opening improved researches in nanozymes and provides a means to design a catalytic cascade model for practical applications.
Abstract: The efficiency of chemical intercommunication between enzymes in natural networks can be significantly enhanced by the organized catalytic cascades. Nevertheless, the exploration of two-or-more-enzymes-engineered nanoreactors for catalytic cascades remains a great challenge in cancer therapy because of the inherent drawbacks of natural enzymes. Here, encouraged by the catalytic activity of the individual nanozyme for benefiting the treatment of solid tumors, we propose an organized in situ catalytic cascades-enhanced synergistic therapeutic strategy driven by dual-nanozymes-engineered porphyrin metal-organic frameworks (PCN). Precisely, catalase-mimicking platinum nanoparticles (Pt NPs) were sandwiched by PCN, followed by embedding glucose oxidase-mimicking ultrasmall gold nanoparticles (Au NPs) within the outer shell, and further coordination with folic acid (P@Pt@P-Au-FA). The Pt NPs effectively enabled tumor hypoxia relief by catalyzing the intratumoral H2O2 to O2 for (1) enhancing the O2-dependent photodynamic therapy and (2) subsequently accelerating the depletion of β-d-glucose by Au NPs for synergistic starving-like therapy with the self-produced H2O2 as the substrate for Pt NPs. Consequently, a remarkably strengthened antitumor efficiency with prevention of tumor recurrence and metastasis was achieved. This work highlights a rationally designed tumor microenvironment-specific nanoreactor for opening improved research in nanozymes and provides a means to design a catalytic cascade model for practical applications.
TL;DR: This 3D interpenetrating structure demonstrates the superiority for energy storage applications and the Galvanostatic intermittent titration (GITT) measurement and the first-principles calculations reveal that the interconnected macroporous are more beneficial to the diffusion of the K+.
Abstract: The biggest challenge of potassium-ion batteries (KIBs) application is to develop high-performance electrode materials to accommodate the potassium ions large size. Herein, by rational design, we c...
TL;DR: New design principles of hydrogel-based solar evaporator provides a useful means for surface-enhanced water evaporation to inspire scalable and processable solar evaporators from accessible raw materials.
Abstract: Solar vapor generation, which can separate the soluble or dispersing contaminants from water, is particularly desirable owing to its green energy utilization for water purification technology. Here, we present a concept of enhancing solar vapor generation by tailoring surface topography of the hydrogel-based solar evaporator. Via nanotexture-enhanced heat flux at the evaporation front, the obtained solar evaporator achieves a water evaporation rate of ∼2.6 kg m–2 h–1 at ∼91% energy efficiency under one sun (1 kW m–2). An easy-to-install solar still based on this solar evaporator consisting of cost-effective poly(vinyl alcohol) and activated carbon is deployed to demonstrate the potential for domestic or urgent water purification purposes. Such new design principles of hydrogel-based solar evaporators provides a useful means for surface-enhanced water evaporation to inspire scalable and processable solar evaporators from accessible raw materials.
TL;DR: It is theoretically disclosed that the external potential provided by photogenerated electrons for NRR/HER endowing B@g-CN spontaneous NRR and inaccessible HER may provide a promising lead for designing efficient and robust metal-free single atom catalysts toward photocatalytic NRR under visible/infrared spectrum.
Abstract: Conversion of naturally abundant dinitrogen (N2) to ammonia (NH3) is one of the most attractive and challenging topics in chemistry. Current studies mainly focus on electrocatalytic nitrogen reduction reaction (NRR) using metal-based electrocatalysts, while metal-free and solar-driven photocatalysts have been rarely explored. Here, on the basis of the "σ donation-π* back-donation" concept, single B atom supported on holey g-CN (B@g-CN) can serve as metal-free photocatalyst for highly efficient N2 fixation and reduction under visible and even infrared spectra. Our results reveal that N2 can be efficiently activated and reduced to NH3 with extremely low overpotential of 0.15 V and activation barrier of 0.61 eV, lower than most of metal-based NRR catalysts, thereby guaranteeing low energy cost and fast kinetics of NRR. The inherent properties of B@g-CN, such as centralized spin-polarization on the B atom, efficient prohibition of competitive hydrogen evolution reaction (HER), and reduced exciton binding energy, are responsible for the high selectivity and Faradaic efficiency for NRR under ambient conditions. Moreover, for the first time, we theoretically disclose that the external potential provided by photogenerated electrons for NRR/HER endowing B@g-CN spontaneous NRR and inaccessible HER. This work may provide a promising lead for designing efficient and robust metal-free single atom catalysts toward photocatalytic NRR under visible/infrared spectrum.
TL;DR: A stimuli-responsive "all-in-one" nanocarrier that realizes bimodal imaging diagnosis and chemo- photothermal synergistic therapy and the strong NIR region absorbance endows the Au@MOF of NIR thermal imaging and photoacoustic imaging properties.
Abstract: Light-sensitive yolk-shell nanoparticles (YSNs) as remote-controlled and stimuli-responsive theranostic platforms provide an attractive method for synergistic cancer therapy. Herein, a kind of novel stimuli-responsive multifunctional YSNs has been successfully constructed by integrating star-shaped gold (Au star) nanoparticles as the second near-infrared (NIR-II) photothermal yolks and biodegradable crystalline zeolitic imidazolate framework-8 (ZIF-8) as the shells. In this platform, a chemotherapeutic drug (doxorubicin hydrochloride, DOX) was encapsulated into the cavity, which can show the behavior of controlled release due to the degradation process of ZIF-8 in the mildly acidic tumor microenvironment. Upon the 1064 nm (NIR-II biowindow) laser irradiation, gold nanostar@ZIF-8 (Au@MOF) nanoparticles exhibited outstanding synergistic anticancer effect based on their photothermal and promoted cargo release properties. Moreover, the strong NIR region absorbance endows the Au@MOF of NIR thermal imaging and photoacoustic (PA) imaging properties. This work contributes to design a stimuli-responsive "all-in-one" nanocarrier that realizes bimodal imaging diagnosis and chemo-photothermal synergistic therapy.
TL;DR: A biomimetic hybrid nanozyme is reported which integrates natural enzyme glucose oxidase with nanozyme manganese dioxide by mutual promotion for maximizing the enzymatic activity of MnO2 and GOx and would further facilitate the development of biological nanozymes for cancer treatment.
Abstract: Nanozymes as artificial enzymes that mimicked natural enzyme-like activities have received great attention in cancer diagnosis and therapy. Biomimetic nanozymes require more consideration regarding complicated tumor microenvironments to mimic biological enzymes, thus achieving superior nanozyme activity in vivo. Here we report a biomimetic hybrid nanozyme (named rMGB) which integrates natural enzyme glucose oxidase (GOx) with nanozyme manganese dioxide (MnO2) by mutual promotion for maximizing the enzymatic activity of MnO2 and GOx. Under hypoxia environment, we observed that MnO2 could react with endogenous H2O2 to produce O2 for enhancing the catalytic efficiency of GOx for starvation therapy. Meanwhile, we confirmed that glucose oxidation generated gluconic acid and further improved the catalytic efficiency of MnO2 subsequently. The biochemical reaction cycle, consisting of MnO2, O2, GOx, and H+, was triggered by the tumor microenvironment and accelerated each other so as to achieve self-supplied H+ and accelerate O2 generation, enhancing the starvation therapy, alleviating tumor hypoxia and accelerating the reactive oxygen species generation in photodynamic therapy. This biomimetic hybrid nanozyme would further facilitate the development of biological nanozymes for cancer treatment.
TL;DR: It is found that MSC-exo specifically targeted and accumulated in pathologically relevant murine models brains regions up to 96 h post administration, while in healthy controls they showed a diffuse migration pattern and clearance by 24 h, suggesting that the homing mechanism is inflammatory-driven.
Abstract: Exosomes, nanovesicles that are secreted by different cell types, enable intercellular communication at local or distant sites. Alhough they have been found to cross the blood brain barrier, their migration and homing abilities within the brain remain unstudied. We have recently developed a method for longitudinal and quantitative in vivo neuroimaging of exosomes based on the superior visualization abilities of classical X-ray computed tomography (CT), combined with gold nanoparticles as labeling agents. Here, we used this technique to track the migration and homing patterns of intranasally administrated exosomes derived from bone marrow mesenchymal stem cells (MSC-exo) in different brain pathologies, including stroke, autism, Parkinson’s disease, and Alzheimer’s disease. We found that MSC-exo specifically targeted and accumulated in pathologically relevant murine models brains regions up to 96 h post administration, while in healthy controls they showed a diffuse migration pattern and clearance by 24 h. ...
TL;DR: The finding in this work provides a clear clue that a precise composition stoichiometry could guarantee the formation of high quality multicomponent perovskite films.
Abstract: Addressing the toxicity issue in lead-based perovskite compounds by seeking other nontoxic candidate elements represents a promising direction to fabricate lead-free perovskite solar cells. Recently, Cs2AgBiBr6 double perovskite achieved by replacing two Pb2+ with Ag+ and Bi3+ in the crystal lattice has drawn much attention owing to the convenient substitution of its chemical compositions. Herein, the dependence of the optoelectronic properties and corresponding photovoltaic performance of Cs2AgBiBr6 thin films on the deposition methods of vacuum sublimation and solution processing is investigated. Compared to the vacuum sublimation based one, the solution-processed Cs2AgBiBr6 shows inherently higher crystallinity, narrower electronic bandgap, longer photoexcitation lifetime, and higher mobility. The excellent optoelectronic properties are attributed to the accurate composition stoichiometry of Cs2AgBiBr6 films based on solution processing. These merits enable the corresponding perovskite solar cells to d...
TL;DR: A deeper understanding of metal state-dependent enzyme-like and antibacterial activities is provided, and a new approach for designing novel and selective antibacterial therapies based on metal-carbon nanozymes is highlighted.
Abstract: Metal–carbon hybrid materials have shown promise as potential enzyme mimetics for antibacterial therapy; however, the effects of metal states and corresponding antibacterial mechanisms are largely ...
TL;DR: An in situ dynamic surface self-reconstruction that can dramatically improve the catalytic activity of electrocatalysts is reported that is superior to that of the state-of-the-art OER electrocatalysis.
Abstract: The oxygen-evolution reaction (OER) is a key process in water-splitting systems, fuel cells, and metal–air batteries, but the development of highly active and robust OER catalyst by simple methods ...
TL;DR: This work demonstrates the first example of a formamidinium (FA) containing Dion-Jacobson 2D perovskite material characterized by the BFA n-1Pb nI3 n+1 formulation through employing a novel bifunctional organic spacer (B), namely 1,4-phenylenedimethanammonium (PDMA).
Abstract: Three-dimensional (3D) perovskite materials display remarkable potential in photovoltaics owing to their superior solar-to-electric power conversion efficiency, with current efforts focused on improving stability. Two-dimensional (2D) perovskite analogues feature greater stability toward environmental factors, such as moisture, owing to a hydrophobic organic cation that acts as a spacer between the inorganic layers, which offers a significant advantage over their comparatively less stable 3D analogues. Here, we demonstrate the first example of a formamidinium (FA) containing Dion–Jacobson 2D perovskite material characterized by the BFAn–1PbnI3n+1 formulation through employing a novel bifunctional organic spacer (B), namely 1,4-phenylenedimethanammonium (PDMA). We achieve remarkable efficiencies exceeding 7% for (PDMA)FA2Pb3I10 based 2D perovskite solar cells resisting degradation when exposed to humid ambient air, which opens up new avenues in the design of stable perovskite materials.
TL;DR: The current work highlights the contribution of ferroptotic machinery to antitumor PDT via an activatable, adaptable, all-active MOF nanocarrier.
Abstract: Nanoscale photodynamic therapy (PDT) is an appealing antitumor modality for which apoptosis is the major mechanism of toxicity induction. It was postulated that the highly reactive singlet oxygen in PDT could deplete glutathione (GSH) and activate ferroptosis, the extent to which could be further manipulated by a redox-responsive nanocarrier. To validate this, a disulfide-bearing imidazole ligand coordinated with zinc to form an all-active metal organic framework (MOF) nanocarrier where a photosensitizer (chlorin e6/Ce6) was encapsulated. Regardless of light irradiation, the Ce6-loaded nanocarrier caused the depletion of intracellular GSH via the disulfide-thiol exchange reaction in a murine mammary carcinoma cell line (4T1). The GSH depletion further caused the inactivation of glutathione peroxide 4 (GPX4) and the enhancement of cytotoxicity that was alleviated by ferroptosis inhibitors. The superior in vivo antitumor efficacy of the all-active nanocarrier was corroborated in a 4T1 tumor-bearing mice model regarding tumor growth suppression and animal survival rate. The coadministration of an iron chelator weakened the antitumor potency of the nanocarrier due to ferroptosis inhibition, which was supported by the fact of tumor growth upsurge and the recovered GPX4 activity. The current work highlights the contribution of ferroptotic machinery to antitumor PDT via an activatable, adaptable, all-active MOF nanocarrier.
TL;DR: This work unambiguously demonstrates experimentally the spin Hall effect in graphene induced by MoS2 proximity and for varying temperatures up to room temperature, paving the way toward the combination of spin information transport and spin-to-charge conversion in two-dimensional materials.
Abstract: Graphene is an excellent material for long-distance spin transport but allows little spin manipulation. Transition-metal dichalcogenides imprint their strong spin–orbit coupling into graphene via the proximity effect, and it has been predicted that efficient spin-to-charge conversion due to spin Hall and Rashba–Edelstein effects could be achieved. Here, by combining Hall probes with ferromagnetic electrodes, we unambiguously demonstrate experimentally the spin Hall effect in graphene induced by MoS2 proximity and for varying temperatures up to room temperature. The fact that spin transport and the spin Hall effect occur in different parts of the same material gives rise to a hitherto unreported efficiency for the spin-to-charge voltage output. Additionally, for a single graphene/MoS2 heterostructure-based device, we evidence a superimposed spin-to-charge current conversion that can be indistinguishably associated with either the proximity-induced Rashba–Edelstein effect in graphene or the spin Hall effect...
TL;DR: With its roll-to-roll compatible fabrication procedure, WGC serves as a highly promising material for the practical realization of Li metal anodes in next-generation high energy density secondary batteries.
Abstract: Lithium (Li) metal has long been considered the “holy grail” of battery anode chemistry but is plagued by low efficiency and poor safety due to its high chemical reactivity and large volume fluctuation, respectively. Here we introduce a new host of wrinkled graphene cage (WGC) for Li metal. Different from recently reported amorphous carbon spheres, WGC show highly improved mechanical stability, better Li ion conductivity, and excellent solid electrolyte interphase (SEI) for continuous robust Li metal protection. At low areal capacities, Li metal is preferentially deposited inside the graphene cage. Cryogenic electron microscopy characterization shows that a uniform and stable SEI forms on the WGC surface that can shield the Li metal from direct exposure to electrolyte. With increased areal capacities, Li metal is plated densely and homogeneously into the outer pore spaces between graphene cages with no dendrite growth or volume change. As a result, a high Coulombic efficiency (CE) of ∼98.0% was achieved u...
TL;DR: The present study demonstrates MMV as a promising and rich material, with which to mimic macrophages, and demonstrates that MNP is an efficient biomimetic vehicle for RA targeting and treatment.
Abstract: The targeted delivery of therapeutics to sites of rheumatoid arthritis (RA) has been a long-standing challenge. Inspired by the intrinsic inflammation-targeting capacity of macrophages, a macrophage-derived microvesicle (MMV)-coated nanoparticle (MNP) was developed for targeting RA. The MMV was efficiently produced through a novel method. Cytochalasin B (CB) was applied to relax the interaction between the cytoskeleton and membrane of macrophages, thus stimulating MMV secretion. The proteomic profile of the MMV was analyzed by iTRAQ (isobaric tags for relative and absolute quantitation). The MMV membrane proteins were similar to those of macrophages, indicating that the MMV could exhibit bioactivity similar to that of RA-targeting macrophages. A poly(lactic-co-glycolic acid) (PLGA) nanoparticle was subsequently coated with MMV, and the inflammation-mediated targeting capacity of the MNP was evaluated both in vitro and in vivo. The in vitro binding of MNP to inflamed HUVECs was significantly stronger than ...
TL;DR: The interface modulation of superlattices providing a promising approach for designing advanced electrocatalysts is heralded, with high activity and stability toward the overall water splitting on the MoS2/NiFe-LDHsuperlattice bifunctional electrocatalyst, outperforming the commercial Pt/C-RuO2 couple.
Abstract: Molecular-scale modulation of interfaces between different unilamellar nanosheets in superlattices is promising for efficient catalytic activities. Here, three kinds of superlattices from alternate restacking of any two of the three unilamellar nanosheets of MoS2, NiFe-layered double hydroxide (NiFe-LDH), and graphene are systematically investigated for electrocatalytic water splitting. The MoS2/NiFe-LDH superlattice exhibits a low overpotential of 210 and 110 mV at 10 mA cm-2 for oxygen evolution reaction (OER) and alkaline hydrogen evolution reaction (HER), respectively, superior than MoS2/graphene and NiFe-LDH/graphene superlattices. High activity and stability toward the overall water splitting are also demonstrated on the MoS2/NiFe-LDH superlattice bifunctional electrocatalyst, outperforming the commercial Pt/C-RuO2 couple. This outstanding performance can be attributed to optimal adsorption energies of both HER and OER intermediates on the MoS2/NiFe-LDH superlattice, which originates from a strong electronic coupling effect at the heterointerfaces. These results herald the interface modulation of superlattices providing a promising approach for designing advanced electrocatalysts.