Showing papers in "ACS Applied Materials & Interfaces in 2022"
TL;DR: In this paper , a layered cationic framework with phosphonate was first fabricated by a facile intercalation method to capture hazardous metals from an aqueous solution, and a new concept named the interaction region indicator was used to characterize weak interaction and coordinate bonds.
Abstract: Sorption methodologies play a pivotal role in heavy metal removal to meet the global requirements for uninterrupted access to drinkable water. Standard sorption technologies lack efficiency due to weak adsorbent-metal interaction. To this end, a layered cationic framework material loaded with phosphonate was first fabricated by a facile intercalation method to capture hazardous metals from an aqueous solution. To inquire the removal mechanisms, batch experiments, detection technologies, and simulation calculations were employed to study the interactions at the interface of clay/water. Specifically, the functionalized layered double hydroxide possessed excellent chelation adsorption properties with Zn2+ (281.36 mg/g) and Fe3+ (206.03 mg/g), in which model fitting results revealed that the adsorption process was chemisorption and monolayer interaction. Further, the interfacial interaction between the phosphonate and clay surface was evaluated by molecular dynamics simulation, and a new concept named the interaction region indicator was used to characterize weak interaction and coordinate bonds. The deep insight into the chelation mechanism was visually presented via the orbital interaction diagram. In addition, the regeneration of the spent adsorbent, adsorption column test, and acute toxicity analysis demonstrated that the synthesized material has immense potential in terms of practical usage for the treatment of toxic pollutants. These results provide a novel path for researchers to properly understand the adsorption behavior.
TL;DR: A respiration-driven triboelectric sensor was devised for simultaneous respiratory biomechanical monitoring and exhaled acetone concentration analysis, which has led to the development of a novel real-time active respiratory monitoring system and strengthened tribOElectric-chemisorption coupling sensing mechanism.
Abstract: The high moisture level of exhaled gases unavoidably limits the sensitivity of breath analysis via wearable bioelectronics. Inspired by pulmonary lobe expansion/contraction observed during respiration, a respiration-driven triboelectric sensor (RTS) was devised for simultaneous respiratory biomechanical monitoring and exhaled acetone concentration analysis. A tin oxide-doped polyethyleneimine membrane was devised to play a dual role as both a triboelectric layer and an acetone sensing material. The prepared RTS exhibited excellent ability in measuring respiratory flow rate (2-8 L/min) and breath frequency (0.33-0.8 Hz). Furthermore, the RTS presented good performance in biochemical acetone sensing (2-10 ppm range at high moisture levels), which was validated via finite element analysis. This work has led to the development of a novel real-time active respiratory monitoring system and strengthened triboelectric-chemisorption coupling sensing mechanism.
TL;DR: In this article , the authors focus on the recent five years of advances in ET-LMOF-based sensing materials, with an emphasis on photochemical and photophysical mechanisms, and discuss in detail possible energy transfer processes within a MOF structure or between MOFs and guest materials.
Abstract: The development of materials with outstanding performance for sensitive and selective detection of multiple analytes is essential for the development of human health and society. Luminescent metal–organic frameworks (LMOFs) have controllable surface and pore sizes and excellent optical properties. Therefore, a variety of LMOF-based sensors with diverse detection functions can be easily designed and applied. Furthermore, the introduction of energy transfer (ET) into LMOFs (ET-LMOFs) could provide a richer design concept and a much more sensitive and accurate sensing performance. In this review, we focus on the recent five years of advances in ET-LMOF-based sensing materials, with an emphasis on photochemical and photophysical mechanisms. We discuss in detail possible energy transfer processes within a MOF structure or between MOFs and guest materials. Finally, the possible sensing applications of the ET-LMOF-based sensors are highlighted.
TL;DR: A new efficient synthetic strategy to prepare cationic hydrogels (PHCI) with intrinsically efficient antimicrobial properties by chemically cross-linking trans-1,4-cyclohexanediamine with 1,3-dibromo-2-propanol using a condensation reaction without the use of toxic cross- linking agents is developed.
Abstract: Bacterial infections are a common problem associated with wound treatment that imposes a significant burden on healthcare systems and patients. As a result, healthcare providers urgently need new treatment strategies to protect people. Hydrogel biomaterials with inherent antimicrobial properties offer an attractive and viable solution to this issue. Here, for the first time, we have developed a new efficient synthetic strategy to prepare cationic hydrogels (PHCI) with intrinsically efficient antimicrobial properties by chemically cross-linking trans-1,4-cyclohexanediamine with 1,3-dibromo-2-propanol using a condensation reaction without the use of toxic cross-linking agents. As expected, the prepared PHCI hydrogel possessed an inherent antibacterial ability that can adsorb and kill Staphylococcus aureus and Escherichia coli electrostatically. Notably, in vivo experiments on normal and diabetic rat models confirmed that the PHCI hydrogel can quickly stop bleeding, efficiently kill bacteria, promote the conversion of macrophages from the proinflammatory M1 phenotype to the repaired M2 phenotype, and accelerate collagen deposition and blood vessel formation, thereby achieving rapid wound healing. Overall, this work presents an effective antibacterial dressing that might provide a facile but effective approach for clinical wound management.
TL;DR: In this paper , Ni-embedded porous graphitic carbon fiber (PGCF@Ni) was used as the scaffold to construct a novel cathode and anode for lithium-sulfur batteries.
Abstract: The rational electrode design is one of the most important ways to enhance the electrochemical properties of lithium-sulfur batteries (LSBs). In this contribution, we use Ni-embedded porous graphitic carbon fiber (PGCF@Ni) as the scaffold to construct a novel cathode and anode for LSBs. With the help of elaborate surface engineering, the constructed solid electrolyte interface (SEI)@Li/PGCF@Ni anodes can effectively restrain the growth of lithium dendrites during the cycle, exhibiting an ultralow overpotential of ∼10 mV for 2000 h at 1 mA cm-2/1 mA h cm-2. The underlying mechanism is further investigated by COMSOL Multiphysics simulations. Additionally, the PGCF@Ni/S cathode fabricated by the molten sulfurizing method manifests superior rate performance and stability. Ultimately, the assembled SEI@Li/PGCF@Ni||PGCF@Ni/S full battery exhibits prominent electrochemical property with a high capacity retention of about 77.9% after 600 cycles at 1 C. Such success at the performance improvement in LSBs may open up avenues toward other rational designs of high-quality electrodes in electrochemical energy storage.
TL;DR: In this article , a highly stretchable, sensitive, and multifunctional polysaccharide-based dual-network hydrogel sensor was constructed using dialdehyde carboxymethyl cellulose (DCMC), chitosan (CS), poly(acrylic acid) (PAA), and aluminum ions (Al3+).
Abstract: Tough, biocompatible, and conductive hydrogel-based strain sensors are attractive in the fields of human motion detection and wearable electronics, whereas it is still a great challenge to simultaneously integrate underwater adhesion and self-healing properties into one hydrogel sensor. Here, a highly stretchable, sensitive, and multifunctional polysaccharide-based dual-network hydrogel sensor was constructed using dialdehyde carboxymethyl cellulose (DCMC), chitosan (CS), poly(acrylic acid) (PAA), and aluminum ions (Al3+). The obtained DCMC/CS/PAA (DCP) composite hydrogels exhibit robust mechanical strength and good adhesive and self-healing properties, due to the reversible dynamic chemical bonds and physical interactions such as Schiff base bonds and metal coordination. The conductivity of hydrogel is 2.6 S/m, and the sensitivity (gauge factor (GF)) is up to 15.56. Notably, the DCP hydrogel shows excellent underwater repeatable adhesion to animal tissues and good self-healing properties in water (self-healing rate > 90%, self-healing time < 10 min). The DCP hydrogel strain sensor can sensitively monitor human motion including finger bending, smiling, and wrist pulse, and it can steadily detect human movement underwater. This work is expected to provide a new strategy for the design of high-performance intelligent sensors, particularly for applications in wet and underwater environments.
TL;DR: In this article , a mesopore-adjustable hierarchically porous carbon nanosheets are fabricated based on a micelle-size-mediated spatial confinement strategy, where trimethylbenzene in different volumes of the solvent can mediate the interfacial assembly with a carbon precursor and porogen segment through π-π bonding and van der Waals interaction.
Abstract: Commercial supercapacitors using available carbon products have long been criticized for the under-utilization of their prominent specific surface area (SSA). In terms of carbonaceous electrode optimization, excessive improvement in SSA observed in the gaseous atmosphere might have little effect on the final performance because cracked/inaccessible pore alleys considerably block the direct electrolyte ion transport in a practical electrochemical environment. Herein, mesopore-adjustable hierarchically porous carbon nanosheets are fabricated based on a micelle-size-mediated spatial confinement strategy. In this strategy, hydrophobic trimethylbenzene in different volumes of the solvent can mediate the interfacial assembly with a carbon precursor and porogen segment through π-π bonding and van der Waals interaction to yield micelles with good dispersity and the diameter varying from 119 to 30 nm. With an increasing solvent volume, the corresponding diffusion coefficient (3.1-14.3 m2 s-1) of as-obtained smaller micelles increases, which makes adjacent micelles gather rapidly and then grow along the radial direction of oligomer aggregates to eventually form mesopores on hierarchically porous carbon nanosheets (MNC150-4.5). Thanks to the pore-expansion effect of trimethylbenzene, the mesoporous volume can be adjusted from 28.8 to 40.0%. Mesopores on hierarchically porous carbon nanosheets endow MNC150-4.5 with an enhanced electrochemically active surface area of 819.5 m2 g-1, which gives rise to quick electrolyte accessibility and a correspondingly immediate capacitive response of 338 F g-1 at 0.5 A g-1 in a three-electrode system. Electrolyte transport through pathways within MNC150-4.5 ultimately enables the symmetric cell to deliver a high energy output of 50.4 Wh kg-1 at 625 W kg-1 in a 14 m LiOTF electrolyte and 95% capacitance retention after 100,000 cycles, which show its superior electrochemical performance over representative carbon-based supercapacitors with aqueous electrolytes in recent literature.
TL;DR: In this paper , a typical bilayer-conductive structure Ti3C2Tx MXene/CNTs/TPU composite film was developed by a simple and scalable vacuum filtration process utilizing a porous electrospun thermoplastic polyurethane (TPU) mat as a skeleton.
Abstract: The universal application of wearable strain sensors in various situations for human-activity monitoring is considerably limited by the contradiction between high sensitivity and broad working range. There still remains a huge challenge to design sensors featuring simultaneous broad working range and high sensitivity. Herein, a typical bilayer-conductive structure Ti3C2Tx MXene/carbon nanotubes (CNTs)/thermoplastic polyurethane (TPU) composite film was developed by a simple and scalable vacuum filtration process utilizing a porous electrospun thermoplastic polyurethane (TPU) mat as a skeleton. The MXene/CNTs/TPU strain sensor is composed of two parts: a brittle densely stacked MXene upper lamella and a flexible MXene/CNT-decorated fibrous network lower layer. Benefiting from the synergetic effect of the two parts along with hydrogen-bonding interactions between the porous TPU fiber mat and MXene sheets, the MXene/CNTs/TPU strain sensor possesses both a broad working range (up to 330%) and high sensitivity (maximum gauge factor of 2911) as well as superb long-term durability (2600 cycles under the strain of 50%). Finally, the sensor can be successfully employed for human movement monitoring, from tiny facial expressions, respiration, and pulse beat to large-scale finger and elbow bending, demonstrating a promising and attractive application for wearable devices and human-machine interaction.
TL;DR: In vitro and in vivo results indicated that the PHM hydrogel platform effectively ameliorated the inflammatory response, accelerated angiogenesis, and increased tissue remodeling within 20 days, which was better than the nonresponsive PEG-DA/MY (PM) hydrogels platform in promoting diabetic wound healing.
Abstract: Antioxidant hydrogel has exhibited great potential for diabetic wound treatment. However, it is still a difficult challenge to realize reactive oxygen species (ROS) scavenging in an intelligent manner. Herein, we designed a novel glucose-responsive antioxidant hybrid hydrogel for enhanced diabetic wound repair. In this study, phenylboronic acid (PBA) with unique glucose-sensitivity was modified onto a hyaluronic acid (HA) chain by one-step synthesis, which was then incorporated into a polyethylene glycol diacrylates (PEG-DA) hydrogel matrix to obtain a novel hybrid hydrogel (PEG-DA/HA-PBA). Then, myricetin (MY) molecules with strong antioxidant activity were immobilized into the hybrid hydrogel by the formation of a dynamic borate bond between the polyphenol group of MY and the phenylboronic acid group of HA-PBA. The PEG-DA/HA-PBA/MY (PHM) hybrid hydrogel achieved glucose-triggered MY release, efficient ROS-scavenging (>80.0%), and also reshaped the hostile oxidative wound microenvironment (reduced MDA activity and increased SOD and GSH/GSSG levels). Furthermore, in vitro and in vivo results indicated that the PHM hydrogel platform effectively ameliorated the inflammatory response (decreased IL-6 and increased Il-10 expression), accelerated angiogenesis (increased VEGF and CD 31 expression), and increased tissue remodeling within 20 days, which was better than the nonresponsive PEG-DA/MY (PM) hydrogel platform in promoting diabetic wound healing. All results strongly suggested that this novel glucose-responsive antioxidant hybrid hydrogel platform has great potential in diabetic wound repair.
TL;DR: In this article , a wearable strain sensor is fabricated by sandwiching the MAGP hydrogels between two dielectric carbon nanotubes (CNTs)/poly(dimethylsiloxane) (PDMS) layers, which can be utilized to monitor delicate and vigorous human motion.
Abstract: Hydrogels that combine the integrated attributes of being adhesive, self-healable, deformable, and conductive show great promise for next-generation soft robotic/energy/electronic applications. Herein, we reported a dual-network polyacrylamide (PAAM)/poly(acrylic acid) (PAA)/graphene (GR)/poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) (MAGP) conductive hydrogel composed of dual-cross-linked PAAM and PAA as well as PEDOT:PSS and GR as a conducting component that combines these features. A wearable strain sensor is fabricated by sandwiching the MAGP hydrogels between two dielectric carbon nanotubes (CNTs)/poly(dimethylsiloxane) (PDMS) layers, which can be utilized to monitor delicate and vigorous human motion. In addition, the hydrogel-based sensor can act as a deformable triboelectric nanogenerator (D-TENG) for harvesting mechanical energy. The D-TENG demonstrates a peak output voltage and current of 141 V and 0.8 μA, respectively. The D-TENG could easily light 52 yellow-light-emitting diodes (LEDs) simultaneously and demonstrated the capability to power small electronics, such as a hygrometer thermometer. This work provides a potential approach for the development of deformable energy sources and self-powered strain sensors.
TL;DR: In this article , a multifunctional phase change materials (PCM) is proposed for the thermal management of miniaturized and integrated electronic devices. But the development of flexible PCMs possessing heat energy storage, shape memory, and adjustable electromagnetic interference (EMI) shielding properties under complex conditions remains a challenge.
Abstract: Multifunctional phase change materials (PCMs) are highly desirable for the thermal management of miniaturized and integrated electronic devices. However, the development of flexible PCMs possessing heat energy storage, shape memory, and adjustable electromagnetic interference (EMI) shielding properties under complex conditions remains a challenge. Herein, the multifunctional PCM composites were prepared by encapsulating poly(ethylene glycol) (PEG) into porous MXene/silver nanowire (AgNW) hybrid sponges by vacuum impregnation. Melamine foams (MFs) were chosen as a template to coat with MXene/AgNW (MA) to construct a continuous electrical/thermal conductive network. The MF@MA/PEG composites showed a high latent heat (141.3 J/g), high dimension retention ratio (96.8%), good electrical conductivity (75.3 S/m), and largely enhanced thermal conductivity (2.6 times of MF/PEG). Moreover, by triggering the phase change of the PEG, the sponges displayed a significant photoinduced shape memory function with a high shape fixation ratio (∼100%) and recovery ratio (∼100%). Interestingly, the EMI shielding effectiveness (SE) can be adjusted from 12.4 to 30.5 dB by a facile compression-recovery process based on shape memory properties. Furthermore, a finite element simulation was conducted to emphasize the advantage of the MF@MA/PEG composites in the thermal management of chips. Such flexible PCM composites with high latent heat storage, light-actuated shape memory, and adjustable EMI shielding functions exhibit great potential as smart thermal management materials in military and aerospace applications.
TL;DR: In this paper , a micro/nanostructured pore-rich Si/C microsphere consisting of Si nanoparticles tightly immobilized onto a micron-sized cross-linked C matrix that is coated by a thin C layer (denoted P-Si/C@C) is presented.
Abstract: Silicon/carbon (Si/C) composites have rightfully earned the attention as anode candidates for high-energy-density lithium-ion batteries (LIBs) owing to their advantageous capacity and superior cycling stability, yet their practical application remains a significant challenge. In this study, we report the large-scale synthesis of an intriguing micro/nanostructured pore-rich Si/C microsphere consisting of Si nanoparticles tightly immobilized onto a micron-sized cross-linked C matrix that is coated by a thin C layer (denoted P-Si/C@C) using a low-cost spray-drying approach and a chemical vapor deposition process with inorganic salts as pore-forming agents. The as-obtained P-Si/C@C composite has high porosity that provides sufficient inner voids to alleviate the huge volume expansion of Si. The outer smooth and robust C shells strengthen the stability of the entire structure and the solid-electrolyte interphase. Si nanoparticles embedded in a microsized cross-linked C matrix show excellent electrical conductivity and superior structural stability. By virtue of structural advantages, the as-fabricated P-Si/C@C anode displays a high initial Coulombic efficiency of 89.8%, a high reversible capacity of 1269.6 mAh g-1 at 100 mA g-1, and excellent cycle performance with a capacity of 708.6 mAh g-1 and 87.1% capacity retention after 820 cycles at 1000 mA g-1, outperforming the reported results of Si/C composite anodes. Furthermore, a low electrode swelling of 18.1% at a high areal capacity of 3.8 mAh cm-2 can be obtained. When assembled into a practical 3.2 Ah cylindrical cell, extraordinary long cycling life with a capacity retention of 81.4% even after 1200 cycles at 1C (3.2 A) and excellent rate performance are achieved, indicating significant advantages for long-life power batteries in electric vehicles.
TL;DR: In this paper , a broad-band NIR phosphor-converted light-emitting diode (pc-LED) device was fabricated by using the as-prepared material combined with a 450 nm blue LED chip, which presented a high NIR output power of 32.1 mW and excellent photoelectric conversion efficiency of 11.4% under a drive current of 100 mA.
Abstract: Broad-band near-infrared (NIR) phosphors are essential to assembling portable NIR light sources for applications in spectroscopy technology. However, developing inexpensive, efficient, and thermally stable broad-band NIR phosphors remains a significant challenge. In this work, a phosphate, KAlP2O7, with a wide band gap and suitable electronic environment for Cr3+ equivalent substitution was selected as the host material. The synthesized KAlP2O7:Cr3+ material exhibits a broad-band emission covering 650-1100 nm with a peak centered at 790 nm and a full width at half-maximum (fwhm) of 120 nm under 450 nm excitation. The internal quantum efficiency (IQE) was determined to be 78.9%, and the emission intensity at 423 K still maintains 77% of that at room temperature, implying the high efficiency and excellent thermal stability of this material. Finally, a NIR phosphor-converted light-emitting diode (pc-LED) device was fabricated by using the as-prepared material combined with a 450 nm blue LED chip, which presents a high NIR output power of 32.1 mW and excellent photoelectric conversion efficiency of 11.4% under a drive current of 100 mA. Thus, this work not only provides an inexpensive broad-band NIR material with high performance for applications in NIR pc-LEDs but also highlights some strategies to explore this class of materials.
TL;DR: A safe and effective superoxide radical (O2•-) mediated self-synthesis strategy is developed to prepare Au-doped MoO-x (Au/MoO3-x) plasmonic-semiconductor hybrid for the elimination of MRSA mediated wound infection.
Abstract: A rapid increase in methicillin-resistant Staphylococcus aureus (MRSA) induced infection has been noticed in recent years and the biofilm formed by MRSA further delays wound healing, causing a high mortality rate. Hence, a safe and effective superoxide radical (O2•-) mediated self-synthesis strategy is developed to prepare Au-doped MoO3-x (Au/MoO3-x) plasmonic-semiconductor hybrid for the elimination of MRSA mediated wound infection. The synthesis mechanism of Au NPs is systematically investigated, proving that O2•- plays a key role in reduction of HAuCl4 into Au NPs in the presence of H2O and O2. Au-doped MoO3-x exhibits the improved photothermal conversion efficiency (∼52.40%) compared with MoO3-x (∼41.11%). Moreover, the peroxidase (POD)-like activity of Au/MoO3-x hybrid is higher than that of MoO3-x NPs, resulting in increased yield of highly toxic ·OH. In combination with the enhanced photothermal and POD-like properties, Au/MoO3-x hybrid achieves efficient elimination of MRSA bacteria with eradication ratio of ∼99.76%. Additionally, the as-prepared Au/MoO3-x NPs exhibit excellent biosafety, which is verified via in vitro and in vivo experiments. This study provides the basis for exploring MoO3-x-based hybrids via a green O2•--mediated self-synthesis approach.
TL;DR: In this article , the self-interlocked structures driven by close overlapping and hooking of nanosheets in Fe3O4/expanded graphite (FG) composites remarkably facilitate the construction of phonon and electron transmission channels and improve mechanical strength.
Abstract: High-performance films via layer-by-layer assembly of two-dimensional (2D) materials would provide all possibilities for the development of modern integrated electronics. However, the stacked structure between nanosheets and large-scale fabrication still remain a great challenge. Herein, Fe3O4/expanded graphite (EG) papers are fabricated via in situ oxidation of ferrocene onto EG nanosheets, followed by a continuous roll-in process. Upon mechanical compaction, the self-interlocked structures driven by close overlapping and hooking of nanosheets in Fe3O4/EG (FG) composites remarkably facilitate the construction of phonon and electron transmission channels and improve mechanical strength. FG papers exhibit prominent shielding effectiveness (67.1 dB at ∼100 μm) with enhanced absorptivity (∼0.1, surpassing lots of conductive film materials), stemming from the synergistic effect of electrical and magnetic properties. Also, the electromagnetic interference (EMI) shielding performance shows prominent reliability after bending (2000 cycles) and ultrasonic treatment (30 min). The corresponding tensile strength reaches 35.8 MPa; meanwhile, the corresponding in-plane thermal conductivity coefficient is as high as 191.7 W/(m·K), which can rapidly and efficiently accelerate heat dissipation. In particular, FG papers also reveal rapid response, controllable, and highly stable Joule heating performance and present promising prospects in the fields of radiation-proof clothing, flexible heaters, portable wearable devices, and aerospace.
TL;DR: In this paper , a simple metal-organic framework (MOF)-derived synthetic strategy was proposed to fabricate low-dimensional (LD) nanohybrids formed by zero-dimensional ZrO2 nanoparticles and heteroatom-doped two-dimensional carbon nanostructures.
Abstract: The design of alternative earth-abundant van der Waals (vdW) nanoheterostructures for bifunctional oxygen evolution/reduction (OER/ORR) electrocatalysis is of paramount importance to fabricate energy-related devices. Herein, we report a simple metal-organic framework (MOF)-derived synthetic strategy to fabricate low-dimensional (LD) nanohybrids formed by zero-dimensional (0D) ZrO2 nanoparticles (NPs) and heteroatom-doped two-dimensional (2D) carbon nanostructures. The 2D platforms controlled the electronic structures of interfacial Zr atoms, thus producing optimized electron polarization for boron and nitrogen-doped carbon (BCN)/ZrO2 nanohybrids. X-ray photoelectron spectroscopy (XPS) and theoretical studies revealed the key role of the synergistic couple effect of boron (B) and nitrogen (N) in interfacial electronic polarization. The BCN/ZrO2 nanohybrid showed excellent bifunctional electrocatalytic activity, delivering an overpotential (η10) of 301 mV to reach a current density of 10 mA-cm-2 for the OER process and a half-wave potential (E1/2) of 0.85 V vs reversible hydrogen electrode (RHE) for the ORR process, which are comparable to the state-of-the-art LD nanohybrids. Furthermore, BCN/ZrO2 also showed competitive performances for water-splitting and zinc-air battery devices. This work establishes a new route to fabricate highly efficient multifunctional electrocatalysts by tuning the electronic polarization properties of 0D-2D electrochemical interfaces.
TL;DR: In this article , the authors proposed a general method to perfectly control diffraction patterns based on a multi-beam PGM, which can be used to design multiple-beam antennas and that has significance in wireless communication applications.
Abstract: Phase-gradient metasurfaces (PGMs) constitute an efficient platform for deflection of a beam in a desired direction. According to the generalized Snell's law, the direction of the reflected/refracted wave can be tuned by the spatial phase function provided by the PGMs. However, most studies on PGM focus only on a single diffraction order, that is, the incident wave can be reflected or refracted to a single target direction. Even in the case of multiple beams pointing in different directions, the beams are still in the same order mode, and the energy carried by different beams cannot be controlled. In addition, the energy ratio of multiple beams is generally uncontrollable. Here, we propose a general method to perfectly control diffraction patterns based on a multi-beam PGM. An analytical solution for arbitrarily controlling diffraction beams is derived through which the generation and energy distribution in high-order diffraction beams can be achieved. Three metasurfaces with different diffraction orders and energy ratios are designed and fabricated to demonstrate the proposed method. The efficiencies of diffraction for the desired channels are close to 100%. The simulated and measured far-field patterns are in good agreement with theoretical predictions, validating the proposed method that provides a new way to design multi-beam antennas and that has significance in wireless communication applications.
TL;DR: In this paper , a corrosion-resistant graphene-based carbon-coated iron (Fe@C) magnetic composite foam is fabricated via self-assembly of iron phthalocyanine/Fe3O4 (FePc hybrid) on the graphene skeletons under solvothermal conditions and then annealing at high temperature.
Abstract: Designing and fabricating high-performance microwave absorption materials with efficient electromagnetic absorption and corrosion resistance becomes a serious and urgent concern. Herein, novel corrosion-resistant graphene-based carbon-coated iron (Fe@C) magnetic composite foam is fabricated via self-assembly of iron phthalocyanine/Fe3O4 (FePc hybrid) on the graphene skeletons under solvothermal conditions and then annealing at high temperature. As a result, the rational construction of a hierarchical impedance gradient between graphene skeletons and Fe@C particles can facilitate the optimization in impedance matching and attenuation characteristic of the foam, realizing the efficient dissipation for incident electromagnetic waves. Additionally, the performance of electromagnetic absorption can be controllably regulated by optimizing annealing temperature and/or time. More importantly, the formation of a carbon-coated iron structure substantially improves the corrosion resistance of magnetic particles, endowing the composite foam with excellent stability and durability in microwave absorption performance.
TL;DR: In this paper , a biomimetic copper-based metal-organic framework (Cu-Cu(OH)2-MOF) foam sheet with interconnected pores and pine needle-like hierarchical structures consisting of Cu(OH)-2 nanowires and MOF nanowhiskers is fabricated.
Abstract: Solar steam generation has become a hot research topic because of its great potential to alleviate the drinking water crisis without extra energy input. Although some efforts focusing on designing spatial geometry have been made to multiply the evaporation performances of up-to-date three-dimensional evaporators, they still have some shortcomings, such as low material and space utilization efficiencies, complex spatial geometry, energy loss due to the hot solar absorption surface, and salt crystallization due to inefficient water supply. Herein, a biomimetic copper-based metal-organic framework (Cu-Cu(OH)2-MOF) foam sheet with interconnected pores and pine needle-like hierarchical structures consisting of Cu(OH)2 nanowires and MOF nanowhiskers is fabricated. The pine needle-like hierarchical structures of Cu-Cu(OH)2-MOF foam contribute to absorbing solar energy and supplying sufficient water by trapping incident light and enhancing the capillary force, respectively. Inspired by drying clothes outside under solar irradiation, through exposing one end of the Cu-Cu(OH)2-MOF foam to air, the biface evaporator achieves a subambient evaporation surface temperature and an evaporation rate of up to 3.27 kg m-2 h-1 under only one sun illumination. Furthermore, when coupled with an air flow, the biface evaporator realizes an excellent evaporation rate of 11.58 kg m-2 h-1 with an energy efficiency of 160.07% even in seawater, ensuring its great application prospect to be used in drinking water production and seawater desalination.
TL;DR: In this article , the 2D ultrathin bismuth oxychalcogenide (Bi2O2X, X refers to S, Se, and Te) is synthesized by a facile and eco-friendly chemical synthesis method at room temperature.
Abstract: Two-dimensional (2D) bismuth oxychalcogenide (Bi2O2X, X refers to S, Se, and Te) is one type of rising semiconductor with excellent electrical transport properties, high photoresponse, and good air stability. However, the research on 2D Bi2O2S is limited. In this work, ultrathin Bi2O2S nanosheets are synthesized by a facile and eco-friendly chemical synthesis method at room temperature. The thickness and lateral sizes are 2-4 nm and 20-40 nm, respectively. The 2D ultrathin Bi2O2S nanosheets have a broad absorption spectrum from ultraviolet (UV) to near-infrared (NIR). Photoelectrochemical (PEC) photodetectors based on 2D Bi2O2S nanosheets are fabricated by a simple drop-casting method. The 2D Bi2O2S-based PEC photodetectors show excellent photodetection performance with a broad photoresponse spectrum from 365 to 850 nm, a high responsivity of 13.0 mA/W, ultrafast response times of 10/45 ms, and good long-term stability at a bias voltage of 0.6 V, which are superior to most 2D material-based PEC photodetectors. Further, the 2D Bi2O2S PEC photodetector can function as a high-performance self-powered broadband photodetector. Moreover, the photoresponse performance can be effectively tuned by the concentration and the kind of electrolyte. Our results demonstrate that 2D Bi2O2S nanosheets hold great promise for application in high-performance optoelectronic devices.
TL;DR: A one-step laser induction method was proposed to prepare fluorine-doped laser-induced graphene (F-LIG) with stable and superhydrophobic properties by confining a 355 nm ultraviolet laser at the interface between the fluorinated ethylene propylene (FEP) film and polyimide (PI) film.
Abstract: Joule heaters based on flexible thin films have attracted a significant amount of attention in both academia and the industry. However, it has been highly challenging to fabricate such heaters. In this study, a one-step laser induction method was proposed to prepare fluorine-doped laser-induced graphene (F-LIG) with stable and superhydrophobic properties by confining a 355 nm ultraviolet laser at the interface between the fluorinated ethylene propylene (FEP) film and polyimide (PI) film. The superhydrophobic properties of the F-LIG composite films could be attributed to the doping of fluorine elements and the laser-processed microstructures, which could be tuned by laser processing parameters. Based on the processed F-LIG films, Joule deicing heaters were developed and their deicing efficiencies are 7 times higher than that of the undoped LIG-based deicing heater. The method will provide new means and ideas to develop LIG-based flexible devices.
TL;DR: In this paper , a geometric phase-enabled novel design strategy is proposed to break the conventional trade-off between polarization-insensitivity and bandwidth, which ensures the realization of broad-band polarization sensitivity through a simplified design procedure.
Abstract: The remarkable potential of metasurface holography promises revolutionary advancements for imaging, chip-integrated augmented/virtual reality (AR/VR) technology, and flat optical displays. The choice of constituent element geometry constrains many potential applications purveyed through polarization-independent optical response. The limited capabilities and degree of freedoms in commonly used meta-atoms restrict the design flexibility to break the conventional trade-off between polarization-insensitivity and bandwidth. Here, we propose a geometric phase-enabled novel design strategy to break this conventional trade-off. The proposed strategy ensures the realization of broad-band polarization-insensitivity through a simplified design procedure. An identical output wavefront manipulation is achieved by adjusting the phase delay freedom of geometric phase engineering under different incident polarization conditions. For proof of concept, a metahologram device is fabricated by an optimized complementary metal-oxide-semiconductor (CMOS)-compatible material of hydrogenated amorphous silicon (a-Si:H). This metahologram device reproduces the required hologram with high image fidelity and efficiency under different polarization scenarios of white light incidence. Due to the simple design strategy, low computational cost, and easy fabrication, the proposed technique can be an excellent candidate for realizing polarization-insensitive metahologram devices.
TL;DR: In this paper , a self-healing super-hydrophobic coating was fabricated by combining polydopamine (PDA)-functionalized Cu2+-doped graphene oxide (GO), octadecylamine (ODA), and polydimethylsiloxane (PDMS), which can recover the superhydrophobicity and microstructure of the coating after chemical/physical damage.
Abstract: A self-healing coating possesses a broad application prospect in the metal corrosion protection area due to its pleasurable performance. By far, despite a great deal of research studies that have been reported in this field, it is still a challenge to construct an intrinsic self-healing surface that can repair a damaged structure and restore superhydrophobicity simultaneously. Herein, a self-healing superhydrophobic coating was fabricated by combining polydopamine (PDA)-functionalized Cu2+-doped graphene oxide (GO), octadecylamine (ODA), and polydimethylsiloxane (PDMS), which can recover the superhydrophobicity and microstructure of the coating after chemical/physical damage. The as-prepared self-healing coating displayed excellent liquid repellency with a water contact angle of 158.2 ± 2° and a sliding angle of 4 ± 1°, which endowed the Mg alloy with excellent anticorrosion performance. Once the coating is scratched, the local damaged structure will be automatically repaired through the chelation of catechol and Cu2+. Also, the superhydrophobicity of the coating can be rapidly restored under 1-sun irradiation even after being etched by O2 plasma. Furthermore, the as-fabricated self-healing coating still exhibited excellent corrosion protection against a magnesium alloy after immersion in 3.5 wt % NaCl solution for 30 days, which was attributed to the efficient repair of defects in GO by PDA through π-π interactions and the inherent chemical inertia of PDMS. Moreover, the as-fabricated self-healing coating also exhibited favorable mechanical stability, chemical durability, and weather resistance. This study paves a fresh insight into the design of robust self-healing coatings with huge application potential.
TL;DR: In this article , a broad-band polarization-insensitive flexible metasurface for the security of sensitive packages in the transport industry is proposed, which employs both the propagation and the geometric phase of novel TiO2 resin-based anisotropic nanoresonators.
Abstract: Secure packaging and transportation of light-sensitive chemical and biomedical test tubes are crucial for environmental protection and public health. Benefiting from the compact form factor and high efficiency of optical metasurfaces, we propose a broad-band polarization-insensitive flexible metasurface for the security of sensitive packages in the transport industry. We employ both the propagation and the geometric phase of novel TiO2 resin-based anisotropic nanoresonators to demonstrate a flexible and broad-band polarization-insensitive metasurface in the visible domain. The ultraviolet nanoimprint lithographic technique (UV-NIL) is used to fabricate high-index TiO2 nanoparticle-embedded-resin (nano-PER) structures that are patterned on a flexible substrate. This novel approach provides swift single-step fabrication without secondary fabrication steps such as deposition and etching. Moreover, replicating and transforming patterns over flexible substrates make the proposed technique highly suitable for large-throughput commercial manufacturing. As the proposed metahologram manifests high transmission efficiency in the visible domain, such flexible metaholographic platforms could find several exciting applications in bendable/curved displays, wearable devices, and holographic labeling for interactive displays.
TL;DR: In vivo experiments showed that QCS/TA2.5 hydrogel dressing not only rapidly stopped the bleeding of arterial and deep incompressible wounds in mouse tail amputation, femoral artery hemorrhage, and liver incision models but also significantly accelerated wound healing in a full-thickness skin wound model.
Abstract: Engineered wound dressing materials with excellent injectability, self-healing ability, tissue-adhesiveness, especially the ones possessing potential therapeutic effects have great practical significance in healthcare. Herein, an injectable quaternary ammonium chitosan (QCS)/tannic acid (TA) hydrogel based on QCS and TA was designed and fabricated by facile mixing of the two ingredients under physiological conditions. In this system, hydrogels were mainly cross-linked by dynamic ionic bonds and hydrogen bonds between QCS and TA, which endows the hydrogel with excellent injectable, self-healing, and adhesive properties. Benefitting from the inherent antioxidative, antibacterial, and hemostatic abilities of TA and QCS, this hydrogel showed superior reactive oxygen species scavenging activity, broad-spectrum antibacterial ability, as well as rapid hemostatic capability. Moreover, the QCS/TA2.5 hydrogel (containing 2.5% TA) exhibited excellent biocompatibility. The in vivo experiments also showed that QCS/TA2.5 hydrogel dressing not only rapidly stopped the bleeding of arterial and deep incompressible wounds in mouse tail amputation, femoral artery hemorrhage, and liver incision models but also significantly accelerated wound healing in a full-thickness skin wound model. For the great potentials listed above, this multifunctional QCS/TA2.5 hydrogel offers a promising network as a dressing material for both rapid hemostasis and skin wound repair.
TL;DR: A high-performance Ni2+-doped garnet solid-solution broadband SWIR emitter is fabricated and a synergetic enhancement strategy, adding a fluxing agent and a charge compensator simultaneously, is proposed to deliver a more than 20-fold increase of the SWIR emission intensity and nearly 2-fold improvement of the thermal quenching behavior.
Abstract: Broadband shortwave infrared (SWIR) light-emitting diodes (LEDs), capable of advancing the next-generation solid-state smart invisible lighting technology, have sparked tremendous interest and will launch ground-breaking spectroscopy and instrumental applications. Nevertheless, the device performance is still suppressed by the low quantum efficiency and limited emission bandwidth of the critical phosphor layer. Herein, we report a high-performance Ni2+-doped garnet solid-solution broadband SWIR emitter centered at ∼1450 nm with a large full-width at half-maximum of ∼300 nm, thereby fabricating, for the first time, a directly excited Ni2+-doped garnet solid-solution phosphor-converted broadband SWIR LED device. A synergetic enhancement strategy, adding a fluxing agent and a charge compensator simultaneously, is proposed to deliver a more than 20-fold increase of the SWIR emission intensity and nearly 2-fold improvement of the thermal quenching behavior. The site occupation and mechanism behind the synergetic enhancement strategy are elucidated by a combination of experimental study and theoretical calculation. A prototype of the SWIR LED with a radiation flux of 1.25 mW is fabricated and utilized as an invisible SWIR light source to demonstrate the SWIR spectroscopy applications. This work not only opens a window to explore novel broadband SWIR phosphors but also provides a synergetic strategy to remarkably improve the performance of artificial SWIR LED light sources.
TL;DR: In this article , a blue light-excited, green-emitting Ce3+-activated CaY2ZrScAl3O12:1%Ce3+ phosphor was presented.
Abstract: Phosphor-containing white light-emitting diodes (LEDs) with low color-correlated temperatures (CCTs) and high color rendering indexes (CRIs) are highly desirable for energy-efficient and environmentally friendly solid-state light sources. Here, we report a new and efficient blue light-excited, green-emitting Ce3+-activated CaY2ZrScAl3O12 phosphor, which underpins the fabrication of high-color quality and full-visible-spectrum warm-white LED devices with ultrahigh CRI values (Ra > 96 and R9 > 96). A family of CaY2ZrScAl3O12:Ce3+ phosphors with different Ce3+ dopant concentrations were prepared by high-temperature solid-state synthesis. X-ray diffraction and corresponding Rietveld refinement reveal a garnet structure with an Ia3̅d space group and crystallographic parameters a = b = c = 12.39645(8) Å, α = β = γ = 90°, and V = 1904.99(4) Å3. Luminescence properties were studied in detail as a function of Ce3+ with the optimal concentration 1% mol. Impressively, CaY2ZrScAl3O12:1%Ce3+ exhibits a broad excitation band from 370 to 500 nm, peaking at ∼421 nm, which is well matched with emission from commercial blue LED chips. Under 421 nm excitation, the CaY2ZrScAl3O12:1%Ce3+ phosphor produces dazzling green light in a wide emission band from 435 to 750 nm (emission peak: 514 nm; full width at half-maximum: 113 nm), with a high internal quantum efficiency of 63.1% and good resistance to thermal quenching (activation energy of 0.28 eV). A white LED device combining a 450 nm blue LED chip with CaY2ZrScAl3O12:1%Ce3+ green phosphor and commercial CaAlSiN3:Eu2+ red phosphor as color converters demonstrates bright warm-white light with excellent CIE color coordinates of (0.3938, 0.3819), low CCT of 3696 K, high CRI (Ra = 96.9, R9 = 98.2), and high luminous efficacy of 45.04 lm W-1 under a 20 mA driving current. New green phosphors enable the design and implementation of efficient luminescent materials for healthy solid-state lighting.
TL;DR: A multifunctional Janus electrospun nanofiber dressing, which can inhibit methicillin-resistant Staphylococcus aureus, drain excessive biofluid to promote wound healing, and simultaneously monitor wound pH level, is developed.
Abstract: Wound healing greatly affects patients' health and produces medical burden. Therefore, we developed a multifunctional electrospun nanofiber dressing, which can inhibit methicillin-resistant Staphylococcus aureus (MRSA), drain excessive biofluid to promote wound healing, and simultaneously monitor wound pH level. The polyoxometalate (α-K6P2W18O62·14H2O, P2W18) and oxacillin (OXA) are encapsulated in hydrophobic polylactide (PLA) nanofiber to synergistically inhibit MRSA. The phenol red (PSP) is encapsulated in hydrophilic polyacrylonitrile (PAN) nanofiber to sensitively indicate wound pH in situ. The PSP/PAN nanofiber is directly electrospun on the patterning OXA/P2W18/PLA nanofiber layer to form a Janus dressing. By taking advantage of the wettability difference between the two layers, the excess biofluid can be drained away from the wound. In addition, the Janus dressing exhibits good biocompatibility and accelerates wound healing via its antimicrobial activity and skin repairing function. This multifunctional Janus electrospun nanofiber dressing would be beneficial for wound management and treatment.
TL;DR: In this article , the feasibility of optimizing the dielectric properties of the SmNbO4 (SN) ceramics by substituting Bi3+ ions at the A site was studied.
Abstract: Microwave dielectric ceramics exhibiting a low dielectric constant (εr), high quality factor (Q × f), and thermal stability, specifically in an ultrawide temperature range (from -40 to +120 °C), have attracted much attention. In addition, the development of 5G communication has caused an urgent demand for electronic devices, such as dielectric resonant antennas. Hence, the feasibility of optimizing the dielectric properties of the SmNbO4 (SN) ceramics by substituting Bi3+ ions at the A site was studied. The permittivity principally hinges on the contribution of Sm/Bi-O to phonon absorption in the microwave range, while the reduced sintering temperature results in a smaller grain size and slightly lower Q × f value. The expanded and distorted crystal cell indicates that Bi3+ doping effectively regulates the temperature coefficient of resonant frequency (TCF) by adjusting the strains (causing the distorted monoclinic structure) of monoclinic fergusonite besides correlating with the permittivity. Moreover, a larger A-site radius facilitates the acquisition of near-zero TCF values. Notably, the (Sm0.875Bi0.125)NbO4 (SB0.125N) ceramic with εr ≈ 21.9, Q × f ≈ 38 300 GHz (at ∼8.0 GHz), and two different near-zero TCF values of -9.0 (from -40 to +60 °C) and -6.6 ppm/°C (from +60 to +120 °C), respectively, were obtained in the microwave band. A simultaneous increase in the phase transition temperature (Tc) and coefficients of thermal expansion (CTEs) by A-site substitution provides the possibility for promising thermal barrier coating (TBC) materials. Then, a cylindrical dielectric resonator antenna (CDRA) with a resonance at 4.86 GHz and bandwidth of 870 MHz was fabricated by the SB0.125N specimen. The exceptional performance shows that the SB0.125N material is a possible candidate for the sub-6 GHz antenna owing to the advantages of low loss and stable temperature.
TL;DR: In this article , a 3D hybrid nanostructure (CNT/FeCoNi@C) comprising MOF-derived magnetic nanospheres and Fe-filled carbon nanotube sponge has been controllably fabricated to enhance the absorption ability and broaden the effective absorption bandwidth (EAB).
Abstract: Metal-organic frameworks (MOFs) are booming as a promising precursor for constructing lightweight, high-efficiency microwave absorbing (MA) material. However, it is still a challenge to rationally design three-dimensional (3D), porous MOF-derived MA materials with a stable structure and strong and wideband MA performance. Herein, a 3D hybrid nanostructure (CNT/FeCoNi@C) comprising MOF-derived magnetic nanospheres and Fe-filled carbon nanotube (CNT) sponge has been controllably fabricated to enhance the absorption ability and broaden the effective absorption bandwidth (EAB). The magnetic nanospheres are uniformly anchored on the CNT skeleton, forming hybrid network structures, which enhance interface polarization, electron transportation, and impedance matching. The minimum reflection loss (RL) and EAB of the as-prepared CNT/FeCoNi@C sponges reach -51.7 dB and 6.0 GHz, respectively, outperforming most reported MOF-based wave absorbers. This work provides not only a novel design of MOF-derived 3D nanostructures but also an effective guide for the optimization of electromagnetic properties and absorbing performance in MA material.