Joule-Heating-Driven Synthesis of a Honeycomb-Like Porous Carbon Nanofiber/High Entropy Alloy Composite as an Ultralightweight Electromagnetic Wave Absorber.

High entropy alloys (HEA) have garnered significant attention in electromagnetic wave (EMW) absorption due to their efficient synergism among multiple components and tunable electronic structures. However, their high density and limited chemical stability hinder their progress as lightweight absorbers. Incorporating HEA with carbon offers a promising solution, but synthesizing stable HEA/carbon composite faces challenges due to the propensity for phase separation during conventional heat treatments. Moreover, EMW absorption mechanisms in HEAs may be different from established empirical models due to their high-entropy effect. This underscores the urgent need to synthesize stable and lightweight HEA/carbon absorbers and uncover their intrinsic absorption mechanisms. Herein, we successfully integrated a quinary FeCoNiCuMn HEA into a honeycomb-like porous carbon nanofiber (HCNF) using electrostatic spinning and the Joule-heating method. Leveraging the inherent lattice distortion effects and honeycomb structure, the HCNF/HEA composite demonstrates outstanding EMW absorption properties at an ultralow filler loading of 2 wt %. It achieves a minimum reflection loss of -65.8 dB and boasts a maximum absorption bandwidth of up to 7.68 GHz. This study not only showcases the effectiveness of combining HCNF with HEA, but also underscores the potential of Joule-heating synthesis for developing lightweight HEA-based absorbers.

Entropy engineering enhances the electromagnetic wave absorption of high-entropy transition metal dichalcogenides/N-doped carbon nanofiber composites.

Entropy engineering strategies provide a broader platform for exploring the behavior of electromagnetic wave (EMW) absorption materials and their absorption mechanisms on the microscopic scale. In this work, a novel entropy engineering strategy was developed to improve the EMW absorption properties of MoS2. A hierarchical N-doped carbon nanofiber/MoS2 (NCNF/MS) composite was synthesized using the electrospinning and hydrothermal methods. Then, the conformational entropy of MoS2 was increased by sequentially integrating elements such as W, Se, and Te. Although MoS2 maintains a single 2H-phase structure throughout the entropy increase process, it triggers a series of complex changes at the microscopic level, including lattice distortion, ingenious electronic structure adjustments, and an increase in defect density. These changes provide more possibilities for the EMW interaction with the absorber, which significantly enhances the dielectric behavior of the composites, including conduction and polarization losses. Owing to the unique hierarchical structure and rich defect structure, the obtained entropy-increased NCNF/MWSST exhibits excellent EMW absorption performance. The minimum reflection loss reaches -60.7 dB, and the maximum effective absorption bandwidth is 6.48 GHz, which is improved by almost 584% and 810% compared to NCNF/MS. This study provides a new way to design efficient and high-performance MoS2-based absorbers and provides valuable insights for exploring the entropy-increasing strategies to optimize the EMW absorption properties.

Preparation of bicyclo[1.1.1]pentane-derived nucleoside analogues.

Nucleoside analogues are prevalent in drug design and call for more diversified structures. Bicyclo[1.1.1]pentane (BCP) structure has recently found wide applications in drug discovery. However, incorporation of BCP fragment into nucleoside analogues is hitherto unknown. Thus, from readily available BCP-containing building blocks, six new compounds, including pyrimidine nucleoside analogues, purine nucleoside analogues, and C-nucleoside analogues were prepared in 1-4 steps, generally with good yields.

Designing flower-like MOFs-derived N-doped carbon nanotubes encapsulated magnetic NiCo composites with multi-heterointerfaces for efficient electromagnetic wave absorption.

In order to acquire exceptional electromagnetic wave absorption properties, the microstructure design and component modification of composites are essential. Metal-organic frameworks (MOFs), due to the unique metal-organic crystalline coordination, tunable morphology, high surface area, and well-defined pores, have been regarded as promising electromagnetic wave absorption materials precursors. However, the inadequate contact abilities between adjacent MOFs nanoparticles endow it with undesirable electromagnetic wave dissipation capacity at a low filler loading, which is a great challenge to break size effect of nanoparticles to achieve efficient absorption. Herein, NiCo-MOFs derived N-doped carbon nanotubes encapsulated with NiCo nanoparticles anchored on flowers-like composites (denoted as NCNT/NiCo/C) were successfully prepared through facile hydrothermal method followed by thermal chemical vapor deposition with melamine-assisted catalyst. By controlling the Ni/Co ratio in precursor, the tunable morphology and microstructure of MOFs are achieved. Most importantly, the derived N-doped carbon nanotubes tightly connect the adjacent nanosheets to construct the special 3D interconnected conductive network, which effectively accelerates the charge transfer and improves the conduction loss. And notably, the NCNT/NiCo/C composite delivers excellent electromagnetic wave absorption performance with minimum reflection loss of -66.1 dB and wide effective absorption bandwidth up to 4.64 GHz when the Ni/Co ratio is 1:1. This work provides a novel method for the preparation of morphology controllable MOFs-derived composites and realizes high-performance electromagnetic wave absorption properties.

Advances in Electrochemical Energy Storage over Metallic Bismuth-Based Materials.

Bismuth (Bi) has been prompted many investigations into the development of next-generation energy storage systems on account of its unique physicochemical properties. Although there are still some challenges, the application of metallic Bi-based materials in the field of energy storage still has good prospects. Herein, we systematically review the application and development of metallic Bi-based anode in lithium ion batteries and beyond-lithium ion batteries. The reaction mechanism, modification methodologies and their relationship with electrochemical performance are discussed in detail. Additionally, owing to the unique physicochemical properties of Bi and Bi-based alloys, some innovative investigations of metallic Bi-based materials in alkali metal anode modification and sulfur cathodes are systematically summarized for the first time. Following the obtained insights, the main unsolved challenges and research directions are pointed out on the research trend and potential applications of the Bi-based materials in various energy storage fields in the future.

Super-stable SnO2/MoS2 enhanced the electrocatalytic hydrogen evolution in acidic environments.

For electrocatalytic hydrogen evolution in acidic environments, the stability of catalysts has always been a significant factor restricting development. Here, we prepared a superstable SnO2/MoS2 coupled nanosheet array on carbon cloth (CC@SnO2/MoS2), exhibiting an overpotential of 166 mV at a current density of 10 mA cm-2. According to the results of various tests and theoretical calculations, it is shown that the establishment of SnO2/MoS2 interface engineering is to accelerate the electron transmission on the heterogeneous interface and S defects on the edge of MoS2, and finally improve the conductivity and catalytic activity of the catalyst. More importantly, the formation of an SnO2 interface layer during in situ transformation improves the stability and hydrophilicity of the material surface. We have proposed a strategy for engineering an interface with fast electron transport and proton adsorption, providing some new ideas for the design of HER catalysts in acid electrolytes.

Oxidation-Resistant MXene-Based Melamine Foam with Ultralow-Percolation Thresholds for Electromagnetic-Infrared Compatible Shielding.

To effectively avoid the drawbacks of conventional metal-based electromagnetic interference (EMI) shielding materials such as high density and susceptibility to corrosion, a multifunctional melamine foam (MF) consisting of MXene/polydimethylsiloxane (PDMS) layers with ultralow percolation thresholds was designed through the electrostatic self-assembly and impregnation strategies. The prepared lightweight foams simultaneously show multifunctional properties including EMI shielding, infrared (IR) stealth, oxidation-resistance, and compression stability. Typically, this multifunctional foam exhibits an excellent EMI shielding efficiency (EMI SE) of 45.2 dB at X-band (8.2-12.4 GHz) with only 1.131 vol % MXene filler. Moreover, the temperature difference between the upper and lower surfaces of the foam can be maintained at 45 °C due to its unique three-dimensional (3D) porous structure and low infrared emissivity. The MF skeleton with MXene/PDMS (MFMXP) displays high hydrophobicity, which remains stable in EMI SE after 60 days of exposure to air. Additionally, it shows outstanding mechanical stability after 100 cycles of compression experiments. The lightweight stealth nanocomposite foams can operate stably in complex environments and show high potential for applications in high-tech fields such as wearable electronics, the military, and semiconductors, etc.

Structure-dependent electrochemical properties of cobalt (II) carbonate hydroxide nanocrystals in supercapacitors.

In this work, we report the structure-dependent electrochemical performance of cobalt carbonate hydroxide (Co2(OH)2CO3) nanocrystals by experimental investigation and theoretical simulation. Different Co2(OH)2CO3 nanostructures including two-dimensional (2D) nanosheets (NSs) and one-dimensional (1D) nanowires (NWs), were synthesized on self-supported carbon cloth substrates by a facile hydrothermal method. Compared to 1D NWs, 2D Co2(OH)2CO3 NSs provided a short ion transfer path, and low electron transfer resistance during the electrochemical reaction. At the current density of 2 mA cm-2, 2D Co2(OH)2CO3 NSs exhibited a higher area capacitance of 2.15F cm-2 and better cycling performance (96.2% retention after 10,000 cycles) than that of 1D NWs (1.15F cm-2 and 90.1% retention). First-principles density functional theory (DFT) calculations revealed that the band gap of the (120) facet in 2D NSs was 0.2 eV, far less than of the (200) facet in 1D NWs (1.04 eV). Electrochemical impedance spectroscopy (EIS) measurements further indicated that the electron transfer and reaction kinetics were more efficient in 2D NSs. This work can provide an important insight in understanding the mechanism of electrochemical energy storage.

Oxygen Vacancy Engineering Synergistic with Surface Hydrophilicity Modification of Hollow Ru Doped CoNi-LDH Nanotube Arrays for Boosting Hydrogen Evolution.

With the development of clean hydrogen energy, the cost effective and high-performance hydrogen evolution reaction (HER) electrocatalysts are urgently required. Herein, a green, facile, and time-efficient Ru doping synergistic with air-plasma treatment strategy is reported to boost the HER performance of CoNi-layered double hydroxide (LDH) nanotube arrays (NTAs) derived from zeolitic imidazolate framework nanorods. The Ru doping and air-plasma treatment not only regulate the oxygen vacancy to optimize the electron structure but also increase the surface roughness to improve the hydrophilicity and hydrogen spillover efficiency. Therefore, the air plasma treated Ru doped CoNi-LDH (P-Ru-CoNi-LDH) nanotube arrays display superior HER performance with an overpotential of 29 mV at a current density of 10 mA cm-2 . Furthermore, by assembling P-Ru-CoNi-LDH as both cathode and anode for two-electrode urea-assisted water electrolysis, a small cell voltage of 1.36 V is needed at 10 mA cm-2 and can last for 100 h without any obvious activity attenuation that showing outstanding durability. In general, the P-Ru-CoNi-LDH can improve the HER performance from intrinsic electronic structure regulation cooperated with extrinsic surface wettability modification. These findings provide an effective intrinsic and extrinsic synergistic effect avenue to develop high performance HER electrocatalysts, which is potential to be applied to other research fields.

Formulating Multiphase Medium Anti-wetting States in an Air-Water-Oil System: Engineering Defects for Interface Chemical Evolutions.

Studies which regulate macroscopic wetting states on determined surfaces in multiphase media are of far-reaching significance but are still in the preliminary stage. Herein, inspired by the wettability subassembly of fish scales, Namib desert beetle shell, and lotus leaf upper side, interfaces in the air-water-oil system are programmed by defect engineering to tailor the anti-wetting evolution from double to triple liquid repellency states. By controlling the visible light irradiation and plasma treatment, surface oxygen vacancies on CuxO@TiO2 nanowires (NWs) can be healed or reconstructed. The original membrane or the membrane after plasma treatment possesses abundant surface oxygen vacancies, and the homogeneous hydrophilic membrane shows only double anti-wetting states in the water-oil system. By the unsaturated visible light irradiation time, the surface oxygen vacancy partially healed, the heterogeneous hydrophilic-hydrophobic components occupied the membrane surface, and the anti-wetting state finally changed from double to triple in the air-water-oil system. After the illumination time reaches saturation, it promotes the healing of all surface oxygen vacancies, and the membrane surface only contains uniform hydrophobic components and only maintains double anti-wetting state in the air-oil system. The mechanism of the triple anti-wetting state on a heterogeneous surface is expounded by establishing a wetting model. The wetting state and the adhesion state of the CuxO@TiO2 NW membrane show regional specificity by controlling the illumination time and region. The underwater oil droplets exhibit the "non-adhesive" and "adhesive" state in a region with unsaturated irradiation time or in an unirradiated region, respectively. Underwater oil droplet manipulation can be accomplished easily based on switchable wettability and adhesion. Current studies reveal that defect engineering can be extended to anti-wetting evolution in the air-water-oil system. Constructing an anti-wetting interface by heterogeneous components provides reference for designing the novel anti-wetting interface.

Interface engineering of a hierarchical ZnxCd1-xS architecture with favorable kinetics for high-performance solar water splitting.

Manipulating the charge carrier transport in photoactive materials is a big challenge toward high efficiency solar water splitting. Herein, we designed a hierarchical ZnxCd1-xS architecture for tuning the interfacial charge transfer kinetics. The in situ growth of ZnxCd1-xS nanoflakes on ZnO backbones provided low interfacial resistance for charge separation. With this special configuration, the optimized Zn0.33Cd0.67S photoanode achieved significantly enhanced performance with a photocurrent density of 10.67 mA cm-2 at 1.23 V versus RHE under AM1.5G solar light irradiation, which is about 14.1 and 2.5 times higher than that of the pristine ZnO and CdS nanoparticle decorated ZnO photoanodes, respectively. After coating a thin SiO2 layer, the photostability of the hierarchical Zn0.33Cd0.67S photoanode is greatly enhanced with 92.33% of the initial value retained under 3600 s continuous light illumination. The prominent PEC activity of the hierarchical ZnxCd1-xS nanorod arrays can be ascribed to an enhanced charge transfer rate aroused by the binder-free interfacial heterojunction, and the improved reaction kinetics at the electrode-electrolyte interface, which is evidenced by electrochemically active surface area measurements and intensity modulated photocurrent spectroscopy analysis. This interfacial heterojunction strategy provides a promising pathway to prepare high performance photoelectrodes.

Ultrathin ZIF-8 wrapping on Au-dotted Ag-nanowires for highly selective SERS-based CO2 gas detection.

Ultrathin ZIF-8 wrapping was constructed on Au-dotted Ag-nanowires to obtain Ag@Au@ZIF-8. A thin film (Ag@Au@ZIF-8 NWs/TF) was constructed to selectively adsorb and enrich CO2 molecules, which solved the problem that SERS signals could not be detected due to the poor affinity of the metal surface and the low concentration of gas molecules.

Solar-Heating Crassula perforata-Structured Superoleophilic CuO@CuS/PDMS Nanowire Arrays on Copper Foam for Fast Remediation of Viscous Crude Oil Spill.

In nature, leaf photosynthesis is the most common solar energy conversion system, which involves light absorption and conversion processes. Most interestingly, the leaves of a green plant are almost lamellar. Herein, inspired by the structure and light conversion capacity of plants, we developed a Crassula perforata-structured CuO@CuS/poly(dimethylsiloxane) (CuO@CuS/PDMS) nanowire arrays (NWAs) on copper foam (CF) with effective light-to-heat conversion to clean up viscous crude oil (∼105 mPa s) by in situ reducing the viscosity of crude oil. The C. perforata-structured CuO@CuS/PDMS core/shell NWAs were grown on copper foam with high density and uniformity, exhibiting excellent light adsorption and photothermal conversion efficiency. When simulated sunlight was irradiated on the structure of the CuO@CuS/PDMS NWAs/CF, abundant heat was generated and in situ reduced the viscosity of crude oil, which prominently increased the oil diffusion coefficient and sped up the oil sorption rate. The oil recovery procedure can realize a continuous clean up with the assistance of a pump device, and the crude oil adsorption capacity can reach up to 15.57 × 105 g/m3 during a 5 min adsorption process. The high-performance photothermal self-heated superoleophilic CuO@CuS/PDMS NWAs/CF has a promise of promoting the practical applications of the sorbents in the clean up of viscous crude oil spills.

Effective photodynamic therapy of polymer hydrogel on tumor cells prepared using methylene blue sensitized mesoporous titania nanocrystal.

A novel hydrogel shell on cancer cells was prepared via in situ photopolymerization of polyethyleneglycol diacrylate (PEGDA) using methylene blue (MB) sensitized mesoporous titania nanocrystal for effective photodynamic therapy (PDT). TiO2 in this system served as an effective photosensitizer and initiator for the formation of hydrogel, also can protect the MB from being degraded into an inactive form. While MB was used as a significant photosensitive additive to improve the photochemistry effects of TiO2 and widen its optical response area to near infrared region (660-900 nm). The PEGDA hydrogel with peritumoral injectability shows competitive advantages, i.e. good biocompatibility and hydrophily, selective and minimally invasive delivery of TiO2@MB, maintaining a high PDT drug concentration for inducing tumor apoptosis, localized and sustainable release under 660 nm laser irradiation for reducing side effect. The hydrogel also could load chemo-therapy drugs, and serve as a versatile platform for multimode antitumor treatment.

High-Flux Oil/Water Separation with Interfacial Capillary Effect in Switchable Superwetting Cu(OH)2@ZIF-8 Nanowire Membranes.

Highly ordered architectures with roughness and porous surface are the key challenges toward developing smart superwetting membranes. We prepared switchable superwetting Cu(OH)2@ZIF-8 core/shell nanowire membranes for high-flux oil/water separation as well as simultaneous heavy-metal ions removal in one step. The well-defined Cu(OH)2@ZIF-8 core/shell nanowire grown on copper mesh with average length of ca. 15 µm and diameter of ca. 162 nm exhibits high water contact angle (CA) of ca. 153 ± 0.6°. After modified by ethanol, the membrane holds the reverse superwettability with oil (dichloromethane as an example) CA of ca. 155 ± 0.8° underwater. The separation efficiencies of the membranes are higher than that of 97.2% with a remarkable flux rate higher than 90 000 L m-2 h-1 for the immiscible oil/water mixture. And the removal efficiency for Cr3+ ions at 10 ppb can arrive at 99.2 wt % in the toluene-in-water emulsion. The high performances of the smart superwetting membranes can be attributed to the interfacial capillary effects of the hierarchical Cu(OH)2@ZIF-8 core/shell nanostructures. This work may provide a new insight into the design of smart superwetting surfaces for oil/water separation and target adsorption in one step.

Hierarchical core-shell structures of P-Ni(OH)2 rods@MnO2 nanosheets as high-performance cathode materials for asymmetric supercapacitors.

The hierarchical porous structure with phosphorus-doped Ni(OH)2 (P-Ni(OH)2) rods as the core and MnO2 nanosheets as the shell is fabricated directly by growth on a three-dimensional (3D) flexible Ni foam (NF) via a two-step hydrothermal process. As a binder-free electrode material, this unique hybrid structure exhibits excellent electrochemical properties, including an ultrahigh areal capacitance of 5.75 F cm-2 at a current density of 2 mA cm-2 and great cyclic stability without capacitance loss at a current density of 20 mA cm-2 after 10 000 cycles. Moreover, an all-solid-state asymmetric supercapacitor (AAS) based on a P-Ni(OH)2@MnO2 hybrid structure on Ni foam as the cathode and activated carbon (AC) as the anode is successfully assembled to enhance value the electrochemical properties. The AAS device also shows excellent electrochemical properties including a large potential window of 0∼1.6 V, an areal capacitance is 911.3 mF cm-2 at a current density of 1 mA cm-2 and long-term cycling performance. Meanwhile, the AAS device also delivers a high energy density of 0.324 mW h cm-2 at a power density of 0.8 mW cm-2; and can easily light colorful light-emitting diode (LED) lights, suggesting that 3D P-Ni(OH)2@MnO2 hybrid composite has promising potential for practical use in high-performance supercapacitors.

Photosensitive multifunctional poly(vinyl alcohol) micelles for enhanced antitumor effect.

Polyvinyl alcohol (PVA) micelles were firstly synthesized by using hemin molecules as novel crosslinked bridges (PVA-H crosslinked micelles). On one hand, the crosslinked micelles can allow high stability against extensive dilution (1800-fold) to reduce side-effects; On the other hand, the bridges not only can destruct by means of laser irradiation (405nm, 200mw), but also can induce the production of singlet oxygen (1O2) and the release of 5-fluorouracil (5FU) (i.e. 46% release in 360min). But above all, that 5FU-loaded PVA-H crosslinked micelles irradiating by laser is more efficient than PVA-H crosslinked micelles and free 5FU in killing tumor cells, suggest the effective synergistic antitumor effect about chemotherapy and photodynamic therapy (PDT).

A novel porous aspirin-loaded (GO/CTS-HA)n nanocomposite films: Synthesis and multifunction for bone tissue engineering.

A novel porous graphene oxide (GO)/chitosan (CTS)-hydroxyapatite (HA) nanocomposite film was successfully prepared for the first time by combining layer-by-layer (LBL) assembly technology with biomimetic mineralization method. The LBL technology was used to control the thickness of film as well as induce the biomimetic mineralization of biocompatible HA. The obtained (GO/CTS-HA)n film provided ideal platform for the proliferation of mouse mesenchymal stem cells (mMSCs). The pore size in the film is about 300nm, and the porous architecture made the film have high aspirin loading efficiency. Also the accumulated loading dosage could be adjusted by the film thickness, and the sustained release of aspirin could ensure well anti-inflammatory effect. The above advantages may alleviate the pain of patients and give the better environment for bone regeneration. This multifunctional aspirin-loaded (GO/CTS-HA)n film provided an inspiration for the synthesis of novel porous inorganic/biomacromolecule nanocomposite films as the biocoatings applied in bone tissue engineering.

Nitrogen-doped nanoporous carbon derived from waste pomelo peel as a metal-free electrocatalyst for the oxygen reduction reaction.

The development of a new catalyst for the low-cost, environmentally friendly and highly efficient oxygen reduction reaction (ORR) is important for the commercialization of fuel cells. Herein, a smart strategy was proposed for the preparation of a novel nitrogen-doped nanoporous carbon (N-PC) using resource-rich pomelo peel, a type of waste, as starting material. The typical product (N-PC-1000) possesses a high BET surface area (up to 1444.9 m2 g(-1)), porous structure and high graphitic N content. In alkaline and acidic media, the N-PC-1000 shows not only decent catalytic activities in terms of onset potential and current density, but also has excellent tolerance to methanol poisoning effects and durability. This study provides worthy inspiration for using other environmental wastes to prepare related functional carbon materials with a variety of promising practical applications such as supercapacitors and lithium-ion batteries.

An ordered and porous N-doped carbon dot-sensitized Bi2O3 inverse opal with enhanced photoelectrochemical performance and photocatalytic activity.

A novel ordered porous Bi2O3 inverse opal structure (IOS) was prepared using a polystyrene (PS) photonic crystal as the template for the first time. Nitrogen-doped carbon dots (N-CDs) were chosen to sensitize the as-prepared Bi2O3 IOS for improving photoelectrochemical performance and photocatalytic activity. The photocurrent density of the fabricated N-CDs/Bi2O3 IOS with favorable visible light absorption properties can achieve 0.75 mA cm(-2), which significantly enhanced performance two-, seven-, and thirty-fold compared with that of the CDs/Bi2O3 IOS, Bi2O3 IOS, and Bi2O3 nanoparticles (NPs), respectively. The N-CDs/Bi2O3 IOS also has increased photocatalytic activity for the decolorization of Rhodamine B (RhB), 4 times higher than Bi2O3 NPs. The above performance enhancement of N-CDs/Bi2O3 IOS is caused by the synergistic effect of N-CDs sensitization and the highly ordered IOS, which make it a promising material to be used in clean energy, solar cells, potential applications in water purification and so on.