http://onlinelibrary.wiley.com/rss/journal/10.1002/(ISSN)1521-4095

A charge density wave (CDW) represents an exotic state in which electrons are arranged in a long range ordered pattern in low-dimensional materials. Although our understanding of the fundamental character of CDW has been enriched after extensive studies, its practical application remains limited. Here, we show an unprecedented demonstration of a tunable charge-spin interconversion (CSI) in graphene/1T-TaS2 van der Waals heterostructures by manipulating the distinct CDW phases in 1T-TaS2. Whereas CSI from spins polarized in all three directions are observed in the heterostructure when the CDW phase does not show commensurability, the output of one of the components disappears and the other two are enhanced when the CDW phase becomes commensurate. The experimental observation is supported by first-principles calculations, which evidence that chiral CDW multidomains in the heterostructure are at the origin of the switching of CSI. Our results uncover a new approach for on-demand CSI in low-dimensional systems, paving the way for advanced spin-orbitronic devices.

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Solution-processable organic conjugated molecules (OCMs) consisted of a series of aromatic units linked by σ-bonds, which present a relatively freedom intramolecular motion and intermolecular re-arrangement under external stimulation. These are influence on the chem-physic, photophysic and electrical property. Cross-linked strategy provided an effective platform to obtain OCMs network, which allow for outstanding optoelectronic, excellent chem-physic property and substantial improvement in device fabrication. Unsaturated double carbon-carbon bond (C = C) is a universal segment to construct crosslinkable OCMs. In this review, we will set C = C cross-linkable units as an example to summarize the development of cross-linkable OCMs for solution-processable optoelectronic applications. First, this review provides a comprehensive of overview of the distinctive chemical, physical, and optoelectronic properties arising from the cross-linking strategies employed in OCMs. Second, the methods for probing the C = C cross-linking reaction also emphasized based on the perturbations of chemical structure and chem-physic property. Third, a series of model C = C cross-linkable units, including styrene, trifluoroethylene, unsaturated acid ester, are further discussed to design and prepare novel OCMs. Furthermore, we present a concise overview of the optoelectronic applications associated with this approach, including light-emitting diodes (LEDs), solar cells (SCs), and field-effect transistors (FETs). Lastly, we offer a concluding perspective and outlook for the improvement of OCMs and their optoelectronic application via cross-linking strategy.

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The sprayable hydrogel coatings that can establish robust adhesion onto diverse materials and devices hold enormous potential; however, a significant challenge persists due to monomer hydration, which impedes even coverage during spraying and induces inadequate adhesion post-gelation. Herein, we present a polycation-reinforced (PCR) surface bridging strategy to achieve tough and sprayable hydrogel coatings onto diverse materials. The polycations offer superior wettability and instant electrostatic interactions with plasma-treated substrates, facilitating an effective spraying application. This PCR-based hydrogel coatings demonstrate tough adhesion performance to inert PTFE and silicone, including remarkable shear strength (161±49 KPa for PTFE), interfacial toughness (198±27 J m−2 for PTFE), and notable tolerance to cyclic tension (10000 cycles, 200% strain, silicone). Meanwhile, this method can be applied to various hydrogel formulations, offering diverse functionalities, including underwater adhesion, lubrication, and drug delivery. Furthermore, the PCR concept enables the conformal construction of durable hydrogel coatings onto sophisticated medical devices like cardiovascular stents. Given its simplicity and adaptability, this approach paves an avenue for incorporating hydrogels onto solid surfaces and potentially promotes untapped applications.

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Development of polymer donors with simple chemical structure and low cost is of great importance for commercial application of organic solar cells (OSCs). Here, side-chain random copolymer PMQ-Si605 with a simply 6,7-difluoro-3-methylquinoxaline-thiophene backbone and 5% siloxane decoration of side chain was synthesized in comparison with its alternating copolymer PTQ11. Relative to molecular weight (M n) of 28.3 kg mol−1 for PTQ11, the random copolymer PMQ-Si605 with minor siloxane decoration is beneficial for achieving higher M n up to 51.1 kg mol−1. In addition, PMQ-Si605 can show stronger aggregation ability and faster charge mobility as well as more efficient exciton dissociation in active layer as revealed by femtosecond transient absorption spectroscopy. With L8-BO-F as acceptor, its PMQ-Si605 based OSCs display power conversion efficiency (PCE) of 18.08%, much higher than 16.21% for PTQ11 based devices. With another acceptor BTP-H2 to optimize the photovoltaic performance of PMQ-Si605, further elevated PCEs of 18.50% and 19.15% can be achieved with the binary and ternary OSCs, respectively. Furthermore, PMQ-Si605 based active layers are suitable for processing in high humidity air, an important factor for massive production of OSCs. Therefore, the siloxane decoration on polymer donors is promising, affording PMQ-Si605 as a high-performing and low cost candidate.

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Artificial molecular motors have the potential to generate mechanical work on their environment by producing autonomous unidirectional motions when supplied with a source of energy. However, the harnessing of this mechanical work to subsequently activate various endoenergetic processes that can be useful in materials science remains elusive. Here we show that by integrating a light-driven rotary motor through hydrogen bonds in a β-amyloid-like structure forming supramolecular hydrogels, the mechanical work generated during the constant rotation of the molecular machine under UV irradiation is sufficient to disrupt the β-amyloid fibers and to trigger a gel-to-sol transition at macroscopic scale. This melting of the gel under UV irradiation occurs 25°C below the temperature needed to melt it by solely using thermal activation. In the dark, a reversible sol-gel transition is observed as the system fully recovers its original microstructure, thus illustrating the possible access to new kinds of motorized materials that can be controlled by advanced out-of-equilibrium thermodynamics.

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Dielectrophoresis (DEP) particle separation has label-free, well-controllable, and low-damage merits. Sidewall microelectrodes made of liquid metal alloy (LMA) inherits the additional advantage of thick electrodes to generate impactful DEP force. However, existing LMA electrode-based devices lack the ability to integrate large-array electrodes in a compact footprint, severely limiting flow rate and thus throughput. Herein, a facile and versatile method is proposed to integrate high-density thick LMA electrodes in microfluidic devices, taking advantage of the passive control ability of capillary burst valves (CBVs). CBVs with carefully designed burst pressures are co-designed in microfluidic channels, allowing self-assembly of LMA electrode array through simple hand-push injection. The arrayed electrode configuration brings the accumulative DEP deflection effect. Specifically, we demonstrate to fabricate 5000 pairs of sidewall electrodes in a compact chip to achieve 10 times higher throughput in DEP deflection. We applied the 5000-electrode-pair device to successfully separate the mixed sample of human peripheral blood mononuclear cells (PBMCs) and A549 cells with the flow rate of 70 µL min−1. It is envisioned that this work can greatly facilitate LMA electrode array fabrication and offer a robust and versatile platform for DEP separation applications.

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Alternating current (AC)-driven quantum-dot light-emitting diodes (QLEDs) are superior to direct current-driven QLEDs because they can be directly integrated into household AC electricity and have high stability. However, achieving high-performance AC-driven QLEDs remains challenging. In this work, a bipolar QLED with coplanar electrodes is realized by horizontally connecting a regular QLED and an inverted QLED in series using an Al bridging layer. The bipolar QLED can be turned on with either a positive or a negative bias voltage, with a high external quantum efficiency (EQE) of 22.9%. By replacing the Al with Ag, the resistances of the electron transport layers are effectively reduced, and thus the bipolar QLED shows an enhanced brightness of 16370 cd/m2 at 15 V. By connecting multiple bipolar QLEDs in series, the resulting light source can be directly driven by a 220 V/50 Hz household power supply without the need for back-end electronics. The bipolar QLED can also be realized by vertically stacking a regular QLED and an inverted QLED with a metallic intermediate connection layer. We demonstrate that the coplanar or vertical bipolar QLEDs could find potential applications in household AC electricity play-and-plug solid-state lighting and single- or double-sided displays.

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Spin-polarized bands in pristine and proximity-induced magnetic materials are promising building blocks for future devices. Conceptually new memory, logic, and neuromorphic devices have been conceived based on atomically thin magnetic materials and the manipulation of their spin-polarized bands via electrical and optical methods. A critical remaining issue is the direct probe and the optimized use of the magnetic coupling effect in van der Waals heterostructures, which requires further delicate design of atomically thin magnetic materials and devices. Here, we report a spin-selective memtransistor with magnetized single-layered graphene on a reactive antiferromagnetic material, CrI3. The spin-dependent hybridization between graphene and CrI3 atomic layers enables the spin-selective bandgap opening in the single-layered graphene and the electric field control of magnetization in a specific CrI3 layer. The microscopic working principle is clarified by our first-principles calculations and theoretical analysis of our transport data. We achieved reliable memtransistor operations (i.e., memory and logic device-combined operations) as well as a spin-selective probe of Landau levels in the magnetized graphene by using the subtle manipulation of the magnetic proximity effect via electrical means.

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A dual-acceptor strategy in all-polymer photovoltaic blends pushes the efficiency up to 18.81%, with decent changes in maximal power point (MPP) tracked and thermal stress applied stability tests, where a new phenomenon in that donor aggregation is modulated by the acceptor component is focused on and carefully analyzed. The experience of ternary blend design from here is also expected to be instructive for other organic photovoltaics systems.

Using two structurally similar polymer acceptors in constructing high-efficiency ternary all-polymer solar cells is a widely acknowledged strategy; however, the focus thus far has not been on how polymer acceptor(s) would tune the aggregation of polymer donors, and furthermore film morphology and device performance (efficiency and stability). Herein, it is reported that matching of the celebrity acceptor PY-IT and the donor PBQx-TCl results in enhanced H-aggregation in PBQx-TCl, which can be finely tuned by controlling the amount of the second acceptor PY-IV. Consequently, the efficiency-optimized PY-IV weight ratio (0.2/1.2) leads to a state-of-the-art power conversion efficiency of 18.81%, wherein light-illuminated operational stability is also enhanced along with well-protected thermal stability. Such enhancements in the efficiency and operational and thermal stabilities of solar cells can be attributed to morphology optimization and the desired glass transition temperature of the target active layer based on comprehensive characterization. In addition to being a high-power conversion efficiency case for all-polymer solar cells, these enhancements are also a successful attempt for using combined acceptors to tune donor aggregation toward optimal morphology, which provides a theoretical basis for the construction of other types of organic photovoltaics beyond all-polymer solar cells.

The development of X-ray scintillators with ultrahigh light yields and ultrafast response times is a long sought-after goal. In this work, we theoretically predict and experimentally demonstrate a fundamental mechanism that pushes the frontiers of ultrafast X-ray scintillator performance: the use of nanoscale-confined surface plasmon polariton modes to tailor the scintillator response time via the Purcell effect. By incorporating nanoplasmonic materials in scintillator devices, this work predicts over 10-fold enhancement in decay rate and 38% reduction in time resolution even with only a simple planar design. we experimentally demonstrate the nanoplasmonic Purcell effect using perovskite scintillators, enhancing the light yield by over 120% to 88 ±$\pm$ 11 ph/keV, and the decay rate by over 60% to 2.0 ±$\pm$ 0.2 ns for the average decay time, and 0.7 ±$\pm$ 0.1 ns for the ultrafast decay component, in good agreement with the predictions of our theoretical framework. we perform proof-of-concept X-ray imaging experiments using nanoplasmonic scintillators, demonstrating 182% enhancement in the modulation transfer function at 4 line pairs per millimeter spatial frequency. This work highlights the enormous potential of nanoplasmonics in optimizing ultrafast scintillator devices for applications including time-of-flight X-ray imaging and photon-counting computed tomography.

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Multicatalytic synergistic chemical transformation is a highly efficient and imperative approach for engineering gels in a sustainable way. Through Lignin aluminum nanoparticles (AlNPs)-aluminum ions (Al3+) catalytic system, a sustainable, environmentally adaptable, flame-retardant, conductive, self-healing, and multifaceted organohydrogel is engineered. The organohydrogel concurrently combines the advantages of both hydrogels and organogels, broadening the scope and applications of the gel-system into a wide range of industries.

A sustainable and efficient multicatalytic chemical transformation approach is devised for the development of all-biobased environmentally adaptable polymers and gels with multifunctional properties. The catalytic system, utilizing Lignin aluminum nanoparticles (AlNPs)-aluminum ions (Al3+), synergistically combines multiple catalytic cycles to create robust, mechanically stable, and versatile organohydrogels. Single catalytic cycles alone fail to achieve desired results, highlighting the importance of cooperatively combining different cycles for successful outcomes. The transformation involves free radical crosslinking, reversible quinone-catechol reactions, and an autocatalytic mechanism, resulting in a dual crosslinking strategy that incorporates both covalent and ionic crosslinking. This approach creates a dynamic gel system with combined energy dissipation and storage mechanisms. The engineered organohydrogels demonstrate vital multifunctionalities such as good thermal stability, self-healing, and adhesive properties, flame-retardancy, mechanical resilience and durability, conductivity, viscoelastic properties, environmental adaptability, and resistance to extreme conditions such as freezing and drying. The developed catalytic technology and resulting gels hold significant potential for applications in flexible electronics, energy storage, actuators, and sensors.

Poly(2-vinylpyridine) (P2VP) limits the unrestricted 2D diffusion of zinc ions through soft coordination and the partially quaternized derivative (q-P2VP) further enables a balance between coordination trapping and ion transporting, leading to a rapid ion migration speed and a lower capacity decay.

Decorating Zn anodes with functionalized polymers is considered as an effective strategy to inhibit dendrite growth. However, this normally brings extra interfacial resistance rendering slow reaction kinetics of Zn2+. Herein, a poly(2-vinylpyridine) (P2VP) coating with modulated coordination strength and ion conductivity for dendrite-free Zn anode is reported. The P2VP coating favors a high electrolyte wettability and rapid Zn2+ migration speed (Zn2+ transfer number, t Zn 2+ = 0.58). Electrostatic potential calculation shows that P2VP mildly coordinates with Zn2+ (adsorption energy = −0.94 eV), which promotes a preferential deposition of Zn along the (002) crystal plane. Notably, the use of partially (26%) quaternized P2VP (q-P2VP) further reduces the interfacial resistance to 126 Ω, leading to a high ion migration speed (t Zn 2+ = 0.78) and a considerably low nucleation overpotential (18 mV). As a result of the synergistic effect of mild coordination and partial electrolysis, the overpotential of the q-P2VP-decorated Zn anode retains at a considerably low level (≈46 mV) over 1000 h at a high current density of 10 mA cm−2. The assembled (NH4)2V6O16·1.5H2O || glass fiber || q-P2VP-Zn full cell reveals a lower average capacity decay rate of only 0.018% per cycle within 500 cycles at 1 A g−1.

Fully saturated polymeric carbon nitrides are one of the holy grails of material sciences due to their expected exceptional superhardness. Here, the high-pressure synthesis of three novel carbon nitrides comprised of corner-sharing CN4 tetrahedra is reported. They are recoverable to ambient conditions and stable in air, feature ultra-incompressibility, superhardness, and other attractive properties such as piezoelectricity and fluorescence.

Carbon nitrides featuring three-dimensional frameworks of CN4 tetrahedra are one of the great aspirations of materials science, expected to have a hardness greater than or comparable to diamond. After more than three decades of efforts to synthesize them, no unambiguous evidence of their existence has been delivered. Here, the high-pressure high-temperature synthesis of three carbon–nitrogen compounds, tI14-C3N4, hP126-C3N4, and tI24-CN2, in laser-heated diamond anvil cells, is reported. Their structures are solved and refined using synchrotron single-crystal X-ray diffraction. Physical properties investigations show that these strongly covalently bonded materials, ultra-incompressible and superhard, also possess high energy density, piezoelectric, and photoluminescence properties. The novel carbon nitrides are unique among high-pressure materials, as being produced above 100 GPa they are recoverable in air at ambient conditions.

Functional unit combination strategy is developed to fabricate purely organic room-temperature phosphorescent (RTP) materials. In this strategy, the folding units are responsible for spin–orbit coupling enhancement while diverse luminescent core units contribute to tunable color/lifetime, which facilitates the construction of a series of new molecules with high-efficiency, color/lifetime-tunable, and photo-responsive dynamic RTP.

A rational molecular design strategy facilitates the development of a purely organic room-temperature phosphorescence (RTP) material system with precisely regulated luminescence properties, which surely promotes its functional integration and intelligent application. Here, a functional unit combination strategy is proposed to design novel RTP molecules combining a folding unit with diverse luminescent cores. The different luminescent cores are mainly responsible for tunable RTP properties, while the folding unit contributes to the spin–orbit coupling (SOC) enhancement, which makes the RTP material design as workable as the building block principle. By this strategy, a series of color/lifetime-tunable RTP materials is achieved with unique photo-responsive RTP enhancement when subjected to UV irradiation, which expands their application scenarios in reusable privacy tags, advanced “4D” encryption, and phase separation analysis of blended polymers. This work suggests a simple and effective strategy to design purely organic RTP materials with tunable color and lifetime, and also provides new application options for photo-responsive dynamic RTP materials.

Atomic distance has an important influence on the symmetry and electronic structure of active metal atom. It is classified into three types, namely, the bond length between metal and coordination atom, the distance between single-atom sites and the arrangement spacing of metal atoms, and their corresponding design strategies and improvement on catalytic performance are systematically summarized and discussed.

It is very important to understand the structure–performance relationship of metal catalysts by adjusting the microstructure of catalysts at the atomic scale. The atomic distance has an essential influence on the composition of the environment of active metal atom, which is a key factor for the design of targeted catalysts with desired function. In this review, we discuss and summarize strategies for changing the atomic distance from three aspects and relate their effects on the reactivity of catalysts. First, the effects of regulating bond length between metal and coordination atom at one single-atom site on the catalytic performance are introduced. The bond lengths are affected by the strain effect of the support and high-shell doping and can evolve during the reaction. Next, the influence of the distance between single-atom sites on the catalytic performance is discussed. Due to the space matching of adsorption and electron transport, the catalytic performance can be adjusted with the shortening of site distance. In addition, the effect of the arrangement spacing of the surface metal active atoms on the catalytic performance of metal nanocatalysts is studied. Finally, a comprehensive summary and outlook of the relationship between atomic distance and catalytic performance is given.

The controllable synthesis of transition metal phosphorous chalcogenides (TMPCs) based on subtracting elements mechanism is reported. Among them, the SnPS3 exhibits effective nonlinear susceptibility χ (2) of 8.41 × 10−11 m V−1. The CdPSe3 photodetector displays high responsivity (582 mA W−1) and detectivity (3.19 × 1011 Jones). This research will pave the way for exploration of ternary TMPCs in optical and photoelectric detection.

The 2D ternary transition metal phosphorous chalcogenides (TMPCs) have attracted extensive research interest due to their widely tunable band gap, rich electronic properties, inherent magnetic and ferroelectric properties. However, the synthesis of TMPCs via chemical vapor deposition (CVD) is still challenging since it is difficult to control reactions among multi-precursors. Here, a subtractive element growth mechanism is proposed to controllably synthesize the TMPCs. Based on the growth mechanism, the TMPCs including FePS3, FePSe3, MnPS3, MnPSe3, CdPS3, CdPSe3, In2P3S9, and SnPS3 are achieved successfully and further confirmed by Raman, second-harmonic generation (SHG), and scanning transmission electron microscopy (STEM). The typical TMPCs–SnPS3 shows a strong SHG signal at 1064 nm, with an effective nonlinear susceptibility χ (2) of 8.41 × 10−11 m V−1, which is about 8 times of that in MoS2. And the photodetector based on CdPSe3 exhibits superior detection performances with responsivity of 582 mA W−1, high detectivity of 3.19 × 1011 Jones, and fast rise time of 611 µs, which is better than most previously reported TMPCs-based photodetectors. These results demonstrate the high quality of TMPCs and promote the exploration of the optical properties of 2D TMPCs for their applications in optoelectronics.

The dynamic solvent exchange process within the silica nanoparticles is monitored with millisecond time resolution by embedding rotor-based fluorophores in the silica matrix. The additional validations is further demonstrated the effectiveness of this approach as a promising strategy for investigating nanoscale transport diffusion in micropores.

Measuring the diffusivity of molecules is the first step toward understanding their dependence and controlling diffusion, but the challenge increases with the decrease of molecular size, particularly for non-fluorescent and non-reactive molecules such as solvents. Here, the capability to monitor the solvent exchange process within the micropores of silica with millisecond time resolution is demonstrated, by simply embedding a rotor-based fluorophore (thioflavin T) in colloidal silica nanoparticles. Basically, the silica provides an extreme case of viscous microenvironment, which is affected by the polarity of the solvents. The fluorescence intensity traces can be well fitted to the Fickian diffusion model, allowing analytical solution of the diffusion process, and revealing the diffusion coefficients. The validation experiments, involving the water-to-ethanol and ethanol-to-water solvent exchange, the comparison of different drying conditions, and the variation in the degree of cross-linking in silica, confirmed the effectiveness and sensitivity of this method for characterizing diffusion in silica micropores. This work focuses on the method development of measuring diffusivity and the high temporal resolution in tracking solvent exchange dynamics over a short distance (within 165 nm) opens enormous possibilities for further studies.

A wide bandgap polymer donor based on benzobisthiazole is designed with deep energy level, high planar structure, and good crystallinity, which endows the good complementary absorption, energy level match, and fibril-like morphology with polymer acceptors, and thus realizes high power conversion efficiencies of 17.15% and 18.60% in the binary and ternary blend all-polymer solar cells.

The limited selection of wide bandgap polymer donors for all-polymer solar cells (all-PSCs) is a bottleneck problem restricting their further development and remains poorly studied. Herein, a new wide bandgap polymer, namely PBBTz-Cl, is designed and synthesized by bridging the benzobisthiazole acceptor block and chlorinated benzodithiophene donor block with thiophene units for application as an electron donor in all-PSCs. PBBTz-Cl not only possesses wide bandgap and deep energy levels but also displays strong absorption, high-planar structure, and good crystallinity, making it a promising candidate for application as a polymer donor in organic solar cells. When paired with the narrow bandgap polymer acceptor PY-IT, a fibril-like morphology forms, which facilitates exciton dissociation and charge transport, contributing to a power conversion efficiency (PCE) of 17.15% of the corresponding all-PSCs. Moreover, when introducing another crystalline polymer acceptor BTP-2T2F into the PBBTz-Cl:PY-IT host blend, the absorption ditch in the range of 600–750 nm is filled, and the blend morphology is further optimized with the trap density reducing. As a result, the ternary blend all-PSCs achieve a significantly improved PCE of 18.60%, which is among the highest values for all-PSCs to date.

Following oxidation of Ti3C2T x MXenes, atom probe tomography (APT) reveals that alkalis concentrate in TiO2 nanowires, indicating that their presence influences the oxidation mechanisms and kinetics. These results highlight how APT can be utilized to better understand the functional surface terminations, intercalated ions, or impurities that are inevitable in the wet chemical synthesis of MXenes.

MXenes are a family of 2D transition metal carbides and nitrides with remarkable properties, bearing great potential for energy storage and catalysis applications. However, their oxidation behavior is not yet fully understood, and there are still open questions regarding the spatial distribution and precise quantification of surface terminations, intercalated ions, and possible uncontrolled impurities incorporated during synthesis and processing. Here, atom probe tomography (APT) analysis of as-synthesized Ti3C2T x MXenes reveals the presence of alkali (Li, Na) and halogen (Cl, F) elements as well as unetched Al. Following oxidation of the colloidal solution of MXenes, it is observed that the alkalis are enriched in TiO2 nanowires. Although these elements are tolerated through the incorporation by wet chemical synthesis, they are often overlooked when the activity of these materials is considered, particularly during catalytic testing. This work demonstrates how the capability of APT to image these elements in 3D at the near-atomic scale can help to better understand the activity and degradation of MXenes, in order to guide their synthesis for superior functional properties.

An instant protection spray based on an angle layout can form a hydrogel film on burns in 30 s. The spray-loaded microparticles formed from probiotic extracts and flavones can provide a physical and anti-infection barrier for burns and promote healing, together with the hydrogel film.

Distinct from common injuries, deep burns often require a chronic recovery cycle for healing and long-term antibiotic treatment to prevent infection. The rise of drug-resistant bacteria has caused antibiotics to no longer be perfect, and continuous drug use can easily lead to repeated infection and even death. Inspired by wild animals that chew plants to prevent wound infection, probiotic extracts with a structure similar to the tailspike of phage are obtained from Lactobacillus casei and combined with different flavones to design a series of nonantibiotic bactericides. These novel antibacterial agents are combined with a rapid gelation spray with a novel cross-angle layout to form an instant protection spray (IPS) and provide a physical and anti-infectious barrier for burns within 30 s. This IPS is able to sterilize 100.00% and 96.14% of multidrug-resistant Staphylococcus aureus (MRSA) in vitro and in vivo, respectively. In addition, it is found to effectively reduce inflammation in MRSA-infected burns in rats and to promote tissue healing.