Photothermal Conversion Ability Research Articles

Corrosion resistance and near-infrared light induced self-healing behavior of polycaprolactone coating with MIL-53@TA on magnesium alloy

A novel self-healing composite coating was fabricated on magnesium alloy by using polycaprolactone (PCL) as resin matrix and iron-based metal-organic framework MIL-53 modified with tannic acid (TA) as function filler. The surface morphology, structure and wettability of composite coating were characterized by scanning electron microscopy (SEM), Fourier transform infrared (FT-IR) and sessile water droplet static contact angle. The corrosion resistance and healing performance of PCL coatings was determined by electrochemical impedance spectroscopy (EIS) and photothermal tests. Results indicate that MIL-53@TA/PCL coating possesses a flatter surface, a higher corrosion resistance and better photothermal effect than that of blank PCL coating and MIL-53/PCL coating. Under the near-infrared (NIR) laser irradiation with the wave length of 808 nm, the scratched MIL-53@TA/PCL coating could be healed within 10 min because of the excellent photothermal conversion ability of MIL-53@TA component.

Novel composite phase change material of high heat storage and photothermal conversion ability

Using porous matrix as the supports for phase change materials (PCMs) can effectively eliminate the leakage problem of PCMs during the phase change process. In heat storage utilization, the as-prepared shape-stabilized phase change materials are highly desired to have high latent heat density, rapid heat transfer ability and less supercooling. Although mesoporous silica with large pore volume and specific surface area might be a promising matrix for PCMs, it would be more beneficial if its thermal conductivity and photo-thermal conversion capacity were further improved, especially for the utilization of solar thermal energy. Herein, a composite PCM, namely SA/CNTs@MS, was fabricated successfully using mesoporous silica coated carbon nanotubes (CNTs@MS) as the shape-stabilized matrix for the PCM stearic acid (SA). The results of characterizations showed that CNTs@MS had a core-shell structure with mesoporous silica of a thickness of about 30 nm coated on the outer surface of carbon tubes (CNTs) homogeneously. The melting enthalpy of the obtained SA/CNTs@MS composite was 125.6 J/g. Its thermal conductivity increased 64.7%, and the supercooling degree decreased 3.2 ℃ while compared with those of pure SA. The melting and solidification enthalpies of SA/CNTs@MS decreased 1.1% and 1.3%, respectively after 200 thermal cycles. Besides, it is also confirmed that SA/CNTs@MS had good photo-thermal conversion performance. These imply that the synthesized SA/CNTs@MS composite would be an ideal heat storage material, especially for solar energy utilization.

Photothermally activated self-healing protective coating based on the “close and seal” dual-action mechanisms

In this work, a dual-action self-healing coating with excellent photothermal response to both near-infrared (NIR) laser and sunlight irradiation was prepared. The coating was composed of a shape memory epoxy matrix embedded with poly (ε-caprolactone) (PCL) microspheres, the surface of which was covered by titanium nitride nanoparticles (TiN NPs) to achieve the superior photothermal conversion ability. Upon light irradiation, the [email protected] composite microspheres could efficiently absorb light energy and generate sufficient heat to induce the shape memory recovery of coating defect as well as the melting of PCL to seal the scratch. Morphology observation and electrochemical measurements proved that the coating incorporated with 10 wt% of [email protected] microspheres presented an excellent self-healing performance under 30 s of NIR illumination to recover the barrier property. In addition, the photothermal conversion of [email protected] microspheres could accelerate the evaporation of water around the coating scratch, hence restraining the corrosion activity in the damaged region. The outdoor exposure test on the atmospheric corrosion monitor (ACM) covered by the coating confirmed that sunlight also benefited to achieve the prominent self-healing performance and shorten the water evaporation time, leading to much reduced corrosion current outputs hence improved corrosion protection property.

Dependence of the Nonlinear Photoacoustic Response of Gold Nanoparticles on the Heat-Transfer Process.

Photoacoustic (PA) imaging using the nonlinear PA response of gold nanoparticles (GNPs) can effectively attenuate the interference from background noise caused by biomolecules (e.g., hemoglobin), thus offering a highly potential noninvasive biomedical imaging method. However, the mechanism of the nonlinear PA response of GNPs based on the thermal expansion mechanism, especially the effect of heat-transfer ability, still lacks quantitative investigation. Therefore, this work investigated the effect of heat-transfer ability on the nonlinear PA response of GNPs using the critical energy and fluence concept, taking into account the Au@SiO2 core–shell nanoparticles (weakened heat transfer) and gold nanochains (enhanced heat transfer). The results showed that the stronger the heat transferability, the smaller the critical energy, indicating that the nonlinear PA response of different nanoparticles cannot be contrasted directly through the critical energy. Moreover, the critical fluence can directly contrast the proportion of nonlinear components in the PA response of different GNPs as governed by the combined effect of heat transferability and photothermal conversion ability.

Photonic Hydrogels for Synergistic Visual Bacterial Detection and On-Site Photothermal Disinfection.

Rapid and sensitive diagnostics in the early stage of bacterial infection and immediate treatment play critical roles in the control of infectious diseases. However, it remains challenging to develop integrated systems with both rapid detection of bacterial infection and timely on-demand disinfection ability. Herein, we demonstrate a photonic hydrogel platform integrating visual diagnosis and on-site photothermal disinfection by incorporating Fe3O4@C nanoparticles into a poly(hydroxyethyl methacrylate)-co-polyacrylamide (PHEMA-co-PAAm) matrix. In vitro experiments demonstrate that such a hydrogel can respond to pH variation caused by bacterial metabolism and generate the corresponding color changes to realize naked-eye observation. Meanwhile, its excellent photothermal conversion ability enables it to effectively kill bacteria by destroying cell membranes under near-infrared irradiation. Moreover, the pigskin infection wound model also verifies the bacterial detection performance and disinfection ability of the hydrogel in vivo. Our strategy demonstrates a new approach for visual diagnosis and treatment of bacterial infections.

Polydopamine-Induced Multilevel Engineering of Regenerated Silk Fibroin Fiber for Photothermal Conversion.

Solid photothermal materials with favorable biocompatibility and modifiable mechanical properties demonstrate obvious superiority and growing demand. In this work, polydopamine (PDA) induced functionalization of regenerated silk fibroin (RSF) fibers has satisfactory photothermal conversion ability and flexibility. Based on multilevel engineering, RSF solution containing PDA nanoparticles is wet spun to PDA-incorporating RSF (PDA@RSF) fibers, and then the fibers are coated with PDA via oxidative self-polymerization of dopamine to form PDA@RSF-PDA (PRP) fibers. During the wet spinning process, PDA is to adjust the mechanical properties of RSF by affecting its hierarchical structure. Meanwhile, coated PDA gives the PRP fibers extensive absorption of near-infrared light and sunlight, which is further fabricated into PRP fibrous membranes. The temperature of PRP fibrous membranes can be adjusted and increases to about 50°C within 360 s under 808nm laser irradiation with a power density of 0.6Wcm-2 , and PRP fibrous membranes exhibit effective photothermal cytotoxicity both in vitro and in vivo. Under the simulated sunlight, the temperature of PRP fiber increases to more than 200°C from room temperature and the material can generate 4.5V voltage when assembled with a differential thermal battery, which means that the material also has the potential for flexible wearable electronic devices.

Robust multifunctional superhydrophobic, photocatalytic and conductive fabrics with electro-/photo-thermal self-healing ability

The fabrication of superhydrophobic and conductive fabrics that can conveniently and repeatedly restore the lost superhydrophobicity, caused by either the surface accumulation of trace organic contaminants or the chemical damage to surface components, remains challenging. Herein, we report a multifunctional superhydrophobic and conductive cotton fabric that integrates not only the photocatalytic activity for cleaning organic contaminants, but also the self-healing ability enabled by either electro-thermal or photo-thermal heating besides convection oven heating. The fabric was fabricated through the polydopamine (PDA)-assisted deposition of photocatalyst Ag/CdS and the subsequent thiol-Ag self-assembly. Either UV or visible light irradiation is able to decompose the surface organic contaminants, and the photocatalysis-induced slight damage on super water-repellency is curable by heating. The Ag layer endows the fabric with antibacterial property and conductivity along with the electro-/photo-thermal conversion ability, which offers relatively convenient ways of heating for curing the surface chemical damages caused by O2 plasma etching or accelerated washing. Of particular importance is that the fabric still shows super water-repellency even after 18 cycles of accelerated washing, which equals to 90 normal home laundering cycles. The combination of these multiple functions makes this fabric very promising for a wide range of wearable applications.

AuAg nanocages/graphdiyne for rapid elimination and detection of trace pathogenic bacteria

We prepared a biocompatible AuAg nanocages/graphdiyne @ polyethylene glycol (AuAg/GDY@PEG) composite. The combination of AuAg and GDY to obtain a synergistically enhanced photothermal effect, and the antibacterial effect of GDY and AuAg are used in combined anti-infective therapy. The in vitro antibacterial activity of AuAg/GDY@PEG was investigated, showing an impressive broad-spectrum antibacterial activity with the killing rate > 99.999%. Based on the photothermal conversion ability of AuAg/GDY@PEG, a simple photothermal immunoassay for pathogenic bacteria was successfully established. Sandwich immune response was performed on a microporous plate, the microplate containing the antibody binds specifically to the bacterium being tested, which then binds to the material with the antibody on its surface, and the signal was a change in temperature under 808 nm near-infrared light. The limit of detection (LOD) for S. typhimurium detection is 103 CFU mL−1, with a range of 103–107 CFU mL−1. This method is accurate, rapid and low-cost, which can be used for on-site detection of pathogenic bacteria in food.

A dynamic nano-coordination protein hydrogel for photothermal treatment and repair of infected skin injury.

In this work, a dynamic photothermal hydrogel based on copper disulfide nanoparticles and thiolated gelatin was reported. The resultant hydrogel enabled rapid photothermal sterilization and the sterilization rate could reach 99.9% after 10 minutes of near-infrared irradiation. In addition, the hydrogel exhibited typical dynamic properties with self-recovery, injectability and photothermal conversion ability, showing great potential as a highly adaptable and antibacterial wound dressing for infected tissue injuries.

A tumour microenvironment-mediated Bi2-xMnxO3 hollow nanospheres via glutathione depletion for photothermal enhanced chemodynamic collaborative therapy.

Photothermal-enhanced chemodynamic therapy (CDT) has been attracting increasing attention for effective tumour treatment. Nevertheless, even though Mn-based nanostructures are promising CDT agents, their photothermal conversion capacities are not good enough for an ideal combination therapy. In this work, a bifunctional Bi2-xMnxO3 nanoplatform was developed, with tumour microenvironment (TME)-triggered photothermal therapy (PTT)-enhanced CDT, for a collaborative therapy for tumours. The doping of a small amount of Bi tuned the photothermal and CDT performance of Bi2-xMnxO3, thus promoting the photothermal conversion ability as well as accelerating the ˙OH generation. The existence of reductive Mn4+ could disrupt the internal tumour redox balance by enhancing glutathione (GSH) consumption to improve the CDT effect. Meanwhile, the mild photothermal effect could accelerate the depletion of GSH and the generation of ˙OH in the tumour region after laser irradiation, thus promoting the CDT effect. This manganese-based nanoplatform provides a good strategy for tumour therapy via TME-mediated PTT-enhanced CDT.

Sensitive Micro-Breathing Sensing and Highly-Effective Photothermal Antibacterial Cinnamomum camphora Bark Micro-Structural Cotton Fabric via Electrostatic Self-Assembly of MXene/HACC.

Natural fabrics are gradually becoming the ideal substrate for flexible smart wearable devices due to their excellent moisture absorption, softness, and skin-friendliness. However, the bonding fastness of the conductive layer and the corresponding durability during service have not yet been well satisfied. In this report, we successfully prepared a smart wearable multifunctional protective cotton fabric with microbreathing monitoring and rapid-photothermal antibacterial abilities of Cinnamomum camphora bark microstructure, by combining chitosan quaternary ammonium salt (HACC) with MXene nanosheets through electrostatic self-assembly. Impressively, MXene nanosheets and HACC established a strong interaction using the electrostatic attraction, endowing the fiber surface with ordered nanosheets. Meanwhile, the fabric decorated with MXene/HACC retains its original characteristics of outstanding breathability and softness, and its conductivity exhibits noticeable stability in terms of resistances to oxidation, washing, various solvents, and long-term bending cycles. On the basis of the principle of adsorption and release of water molecules in the MXene multilayer structures, the MXene/HACC fabric could accurately monitor the physiological health activities of users according to their breathing frequency and depth. Benefiting from the local surface plasmon resonance (LSPR) effect, the MXene/HACC shows encouraging photothermal conversion ability, photothermal stability under long time irradiation, washing resistance, and cycle stability. In addition, the fabric achieved an antibacterial efficiency of nearly 100% against Gram-negative Escherichia coli and Gram-positive Staphylococcus aureus within 5 min under an irradiation intensity of 400 mW/cm2. More importantly, after 10 washes, the antibacterial efficiency against the two bacteria could still reach 99.975% and 99.98%, respectively. This multifunctional protective MXene/HACC cotton fabric is expected to play a unique role in the new generation of smart wearable microbreathing sensing and against to bacterial attack, and shows a broad application prospect.

In situ growth of UIO-66-NH2 on thermally stabilized electrospun polyacrylonitrile nanofibers for visible-light driven Cr (VI) photocatalytic reduction

UIO-66-NH2 was successfully deposited on electrospun polyacrylonitrile (PAN) nanofibers treated by thermal oxidative stabilization (TOS) via a simple and effective in situ growth method. Owing to the formation of acridone rings, naphthyridinering rings and hydronaphthyridine rings during the TOS process, the thermally stabilized electrospun PAN (TSPAN) nanofibers were greatly improved in stability and heat resistance and could provide adequate nucleation points for MOFs growth, indicating an ideal MOFs deposition support without additional surface modifications. The results demonstrated that UIO-66-NH2 crystals distributed relatively uniform and dense on the TSPAN nanofibers with mass loading up to 28.1 ​wt%. Compared with powdered UIO-66-NH2, the formed UIO-66-NH2@TSPAN nanofibers showed enhanced visible light driven photocatalytic activity towards reduction of Cr(VI) due to the improvement of visible light response, more excellent photothermal conversion ability and the increase of exposed active sites. The photocatalytic reduction rate of Cr(VI) over UIO-66-NH2@TSPAN was up to 93% within 180 ​min and the rate constant (k ​= ​0.1362) was 2.3 times that of powdered UIO-66-NH2 (k ​= ​0.00576). Significantly, the mechanical flexibility and structural stability endowed the nanofibrous photocatalyst easy operation and outstanding reusable capability. The photocatalytic activity for Cr(VI) reduction still preserved 90% after five cycles. This work proposes a facile strategy for preparation of free-standing MOFs nanofibers and provides MOFs-based photocatalysts a new opportunitie for broad applications in water treatment.

Organelle‐Specific Anchored Delivery System Stretching a Reversal of Tumor Hypoxia Microenvironment to a Combinational Chemo‐Photothermal Therapy

AbstractDirect delivery to an organelle‐specific point can boost the efficacy of therapy procedures to new heights. Among other subcellular organelles, mitochondria generate ATP as intracellular powerhouse, and are associated with multiple aspects of tumorigenesis and tumor development. Here, a mitochondrial anchored biomimetic nanoplatform (CZACN) is designed and its reversal of tumor hypoxia microenvironment underlying the mitochondria‐located chemo‐photothermal therapy is studied. After shuttling into cancer cells, therapeutic payloads including cisplatin (CDDP) and Au nanozymes are controllably released in the ATP‐overexpressed mitochondria. CDDP generates O2•−, forms H2O2 for a chemical fuel in the next reaction, and damages mitochondrial DNA. Meanwhile, the catalase‐like Au nanozymes catalyze the produced hydrogen peroxide for oxygen supply to relieve hypoxic tumor microenvironment, offering cytotoxic singlet oxygen against cancer cells under NIR treatment. As a result of cancer‐cell self‐recognition, mitochondria‐targeted therapy, and photothermal conversion ability, the fabricated CZACNs obtained 89.2 ± 3.70% of tumor growth inhibition under NIR irradiation and constrained the dose‐limiting toxicity of CDDP, as well. These findings reinforce the synergistic effect of organelle‐specific navigation and in situ oxygen self‐sufficiency for combinational chemo‐photothermal therapy.

ICG-Loaded PEG-Modified Black Phosphorus Nanosheets for Fluorescence Imaging-Guided Breast Cancer Therapy.

Indocyanine green (ICG) has been used in various surgical navigation systems and plays an important role in intraoperative imaging diagnosis. However, the poor photostability and unsatisfactory tumor-targeting ability have limited its broad application prospects. In the decades, the construction of a nanodrug delivery system for tumor-targeting diagnosis and therapy has become a research hotspot. Black phosphorus nanosheets (BPNS), as a new kind of biodegradable nanomaterials, have the advantages of high loading capacity, good biocompatibility, tumor targeting, and photothermal effect over other two-dimensional (2D) reported nanomaterials. Herein, ICG-loaded poly(ethylene glycol) (PEG)-modified BPNS (ICG@BPNS-PEG) nanocomposites are constructed to improve the tumor-targeting capacity and guide photothermal therapy through real-time fluorescence imaging. In this study, ICG@BPNS-PEG nanocomposites with a suitable size (240 ± 28 nm) have been successfully constructed. The photostability of ICG@BPNS-PEG nanocomposites surpassed that of free ICG after four on–off cycles of near laser irradiation (NIR). Moreover, ICG@BPNS-PEG nanocomposites have enhanced photothermal conversion ability. The cellular uptake result through flow cytometry showed that ICG@BPNS-PEG nanocomposites could be swallowed easily owing to the suitable size and passive cellular uptake. In addition, the cytotoxicity evaluation of MCF-7, 4T1 breast cancer cells, and healthy RPE cells through the MTT assay demonstrated that ICG@BPNS-PEG nanocomposites have lower cytotoxicity and good cellular compatibility without irradiation. However, the cytotoxicity and live/dead staining proved that ICG@BPNS-PEG nanocomposites have satisfactory photothermal therapeutic effects when irradiated. In the 4T1-bearing mice model, the fluorescence imaging after intravenous injection of nanocomposites showed that ICG@BPNS-PEG nanocomposites have superior passive tumor targeting accumulation through the enhanced permeability and retention (EPR) effect compared with that of free ICG. Also, changes in tumor volume showed a remarkable tumor growth inhibition effect compared with other groups. Moreover, the results of hematoxylin–eosin (H&E) staining of major organs in 4T1-bearing mice also demonstrated that the nanocomposites have good biocompatibility. Therefore, the constructed ICG@BPNS-PEG nanocomposites have substantial potential in breast cancer therapy.

MXene-Coated Wrinkled Fabrics for Stretchable and Multifunctional Electromagnetic Interference Shielding and Electro/Photo-Thermal Conversion Applications.

Stretchability and multifunctional heating abilities are highly desired for wearable electromagnetic interference (EMI) shielding fabrics to tackle the growing electromagnetic pollution for special crowd, such as pregnant women. Herein, we fabricated stretchable MXene-coated thermoplastic polyurethane (TPU) fabrics by simple uniaxial prestretching and spraying methods. The obtained unique wrinkled structure endowed the film with effective strain-invariant electrical conductivity and EMI shielding properties. Specifically, the prepared stretchable film with an extremely low MXene loading (0.417 mg cm-2) exhibited a stable EMI shielding effectiveness of approximately 30 dB under 50% tensile strain and durability during stretching and bending cycles. More importantly, owing to the high electrical conductivity and localized surface plasmon resonance (LSPR) effect of the MXene layer, the stretchable fabrics exhibited excellent Joule heating (up to 104 °C at a voltage of 5 V) and superior photothermal conversion abilities. Moreover, the unique wrinkled MXene-coating layer not only endows the fabrics with stretchable heat abilities but also enhances the photothermal conversion performance by increasing the light absorption area and travel path. We believe that this study offers a novel strategy for the versatile design of stretchable and multifunctional wearable shielding fabrics.

Ultrarobust Photothermal Materials via Dynamic Crosslinking for Solar Harvesting.

Highly efficient and mechanically durable photothermal materials are urgently needed for solar harvesting, but their development still remains challenging. Here, inspired by the hierarchically oriented architecture of natural spider silk, an ultrarobust liquid metals (LMs)/polymer composite is presented via dynamic crosslinking based on the unique mechanical deformable characteristic of LMs. Dynamically cross-linked core-shell structured LMs droplets can be squeezed along with the orientational crystallization of polymer chains during drawing, thus enabling LMs nanoparticles to be uniformly programmed in the rigid polyethylene nanofiber skeleton. The resultant composite exhibits an unprecedented combination of strong broad-band light absorption (96.9-99.3%), excellent photothermal conversion ability, remarkable mechanical property (tensile strength of 283.7MPa, which can lift 200000 times its own weight), and long-term structural reliability (bearing 100000 bending cycles). A powerful and durable solar thermoelectric generator system for real-environmental solar-heat-electricity conversion is further demonstrated, providing a valuable guidance for the design and fabrication of high-performance solar-harvesting materials.

Boosting Photothermal Theranostics via TICT and Molecular Motions for Photohyperthermia Therapy of Muscle‐Invasive Bladder Cancer (Adv. Healthcare Mater. 24/2021)

Photothermal Therapies In article number 2101063 by Qian Liu, Guangxue Feng, Dan Ding, and co-workers, a small photothermal molecule with active intramolecular motions and a dark state twisted intramolecular charge transfer feature is designed to boost the photothermal conversion ability. Such a design strategy enables the effective low-temperature photo-hyperthermia treatment of muscle-invasive bladder cancers at low drug and laser dosages with minimal side effects.

Highly efficient solar vapour generation via self-floating three-dimensional Ti2O3-based aerogels

To reduce the shortage of water resources, solar-driven water evaporation is considered as a sustainable solution. High efficiency solar steam generation (SSG) with the good light absorption, sufficient water transmission, high thermal management and freely floating photothermal materials is highly desirable. Herein, a simple solar desalination strategy was proposed and a new type three-dimensional Ti2O3-based aerogel with high porosity and low thermal conductivity was prepared. In short, polydopamine (PDA)-modified Ti2O3 nanoparticles were uniformly dispersed in chitosan (CS) solution and a porous Ti2O3-based aerogel was formed after freeze-drying. The evaporation rate of this solar steam generator is as high as 1.31 kg m−2 h−1 at 1.0 solar irradiance (1.0 kW m−2), and the photothermal conversion efficiency is about 81.7%. The optical absorption at 250–2500 nm was 94.49%. In addition, the aerogel has a porosity of 97.50% and a density of 0.025 g cm−3, making it freely float on the surface of water. Besides, its thermal conductivity is 0.037 W m−1 K−1, indicating it has excellent thermal insulation performance. The porous Ti2O3-based aerogel can maintain stable evaporation rate and high evaporation efficiency after 10 repeated evaporation cycles. Additionally, the seawater after desalination was tested and the removal rates of ions and carbon-containing organic matter reached 99.80% and 75.45%, respectively. Therefore, the interfacial water evaporator prepared in this work has excellent photothermal conversion ability and is expected to be a candidate material for solar seawater desalination.

Synthesis and in Vitro anticancer properties of Cu2–xSe–AIPH nanomaterials

The Cu2–xSe nanoparticles were synthesized by high temperature pyrolysis, modified with aminated polyethylene glycol in aqueous solution and loaded with compound 2,2′–azobis[2–(2–imidazolin–2–yl)propane] dihydrochloride (AIPH). The obtained nanomaterials can induce photothermal effect and use heat to promote the generation of toxic AIPH radicals under the irradiation of near-infrared laser (808 nm), which can effectively kill cancer cells. A series of in vitro experiments can preliminarily prove that Cu2–xSe–AIPH nanomaterials have strong photothermal conversion ability, good biocompatibility and anticancer properties.

Design of a Smart Self-Healing Coating with Multiple-Responsive Superhydrophobicity and Its Application in Antibiofouling and Antibacterial Abilities.

Inspired by the restoration of the superhydrophobic surfaces after the damage in nature such as lotus leaf and clover, smart self-healing coating with controllable release of loaded healing agents is both of scientific and technological interest. Herein, a smart self-healing coating with superhydrophobicity was gained through blending UV/NIR/acid/base multiple-responsive ZnO-encapsulated mesoporous polydopamine (MPDA) microspheres (zinc oxide-encapsulated mesoporous polydopamine microspheres) with silicone latex and hydrophobic nanoparticles. The hydrophobic and micro/nanostructured ZnO-encapsulated MPDA microspheres provided UV/NIR/acid/base multiple response sources for the smart self-healing coating, combining the photocatalytic activity and acid/base solubility of ZnO nanoparticles, zwitterionic characteristic of amino-modified silicone oil (ASO), as well as the photothermal conversion abilities and charge characteristics of PDA. The ZnO nanoparticles simultaneously acted as the protective layer for the stimuli-responsive microspheres and functional filler in the coating, contributing to realize the controllable and long-period release of loaded hydrophobic ASO and the further antibacterial functionalization for the coating. The super/high hydrophobicity and antibiofouling performances of the coating could be self-healed by UV, NIR, acid, or base stimuli, attributing to the release of ASO from the microspheres. Then, large-area, rapid, and controllable healing superiority could be achieved on the coating with the combined multiple responses under different conditions. Robust environmental endurances for superhydrophobic coating were also confirmed under harsh environments by directly exposing to UV-accelerated weathering and immersing into various solutions (including strong acid/base, salt, and artificial seawater solution). This smart coating has high application prospects due to its environmentally friendly nature, excellent self-healing, and multifunctional characteristics, and the multiple-responsive ZnO-encapsulated MPDA microspheres can be used for the functionalization of other materials.