The exponentially increasing heat generation in electronic devices, induced by high power density and miniaturization, has become a dominant issue that affects carbon footprint, cost, performance, reliability, and lifespan. Liquid metals (LMs) with high thermal conductivity are promising candidates for effective thermal management yet are facing pump-out and surface-spreading issues. Confinement in the form of metallic particles can address these problems, but apparent alloying processes elevate the LM melting point, leading to severely deteriorated stability. Here, we propose a facile and sustainable approach to address these challenges by using a biogenic supramolecular network as an effective diffusion barrier at copper particle-LM (EGaIn/Cu@TA) interfaces to achieve superior thermal conduction. The supramolecular network promotes LM stability by reducing unfavorable alloying and fluidity transition. The EGaIn/Cu@TA exhibits a record-high metallic-mediated thermal conductivity (66.1 W m(-1) K-1) and fluidic stability. Moreover, mechanistic studies suggest the enhanced heat flow path after the incorporation of copper particles, generating heat dissipation suitable for computer central processing units, exceeding that of commercial silicone. Our results highlight the prospects of renewable macromolecules isolated from biomass for the rational design of nanointerfaces based on metallic particles and LM, paving a new and sustainable avenue for high-performance thermal management.

Various water contaminants raise concerns about potential negative effects on aquatic ecosystems and human health, which demand breakthrough technologies for the effective removal of a wide range of water contaminants. Recently, nitrogen-doped biochar has shown promise in the removal of various contaminants due to its merits of having a high surface area, versatile surface functionality, and variable surface charge. However, obtaining nitrogen-doped biochar with a high nitrogen content and large surface area simultaneously is challenging. Herein, we developed a nitrogen-rich magnetic and porous biochar (NMPC) via facile pyrolysis of polyphenol and metal ions cofunctionalized collagen. Benefiting from a large surface area (1194.4 m2 g–1) and a high nitrogen content (8.35 wt %), NMPC exhibited high adsorption performance for broad-spectrum water contaminants, including dyes, antibiotics, and heavy metal ions. Besides, NMPC could be magnetically separated for easy recycling with the embedded magnetic iron carbide (Fe3C) and still maintained a high removal performance even in a six-cycle test. This work provides new possibilities for the fabrication of nitrogen-rich magnetic biochar which holds great potential in efficient removal of broad-spectrum water contaminants.

Achieving food sustainability is one of the biggest challenges in the new millennium. Plant factory cultivation systems provide an alternative for food sustainability, while they often suffer from algal blooms. The overuse of conventional algaecides has caused significant environmental pollution and concerns about food security. Here, we design a nanoenabled metal-organic algaecide that is self-assembled from natural polyphenols and two functional metal ions for providing shading effects and delivering active ingredients synergistically to suppress algal blooms. Black wattle tannin (BWT) and Fe3+ ions are utilized to develop self-assembled FeBWT nanoalgaecides with significant shading effects for decreasing light transmission (up to 97 %) and effectively inhibiting algal photosynthesis. Further, the FeBWT is functionalized with Cu2+ ions (bimetallic Cu/FeBWT) to target the algal cells and release Cu2+ ions via phenolic-mediated cell surface interactions, thus enhancing the inhibition efficiency. Importantly, the biosafety of Cu/FeBWT is demonstrated through toxicity tests on zebrafish and NIH3T3 cells. In our real-world field test, the Cu/FeBWT demonstrates high algal inhibition performance (>95 %, over 30 days), and enhances the accumulation of food nutrients in model plant lettuces. Collectively, the supramolecular metal-organic nanoalgaecide provides a promise for nanoagrochemical application and promotes food sustainability and security.

Ubiquitous antibiotics threaten human health and ecosystem sustainability, and existing removal strategies, especially conventional multistep water treatments, are primarily limited by the antibiotic-specific removal capability. Here, we explore the natural biomass, plant polyphenols, in the capture of various antibiotics with a facile treatment-polyphenol-mediated antibiotic-independent supramolecular coagulation (PMAC). The PMAC shows a superior performance in removing five tetracyclines and quinolones (up to 98.54%), even under complex environmental parameters, including different pH, the presence of inorganic particles and ionic strength, and the presence of conventional colloid-associated contaminants. Our mechanistic studies suggested that PMAC is capable of exerting multiple molecular interactions with various antibiotics, and the coordination-driven self-assembly further destabilizes the phenolic-antibiotic nanocomplexes, enabling an antibiotic-independent coagulation. Collectively, the combination of efficient remediation with inexpensive biomass suggests a simple and scalable method for the sustainable removal of antibiotics. Our strategy shows great promise as a cost-effective, facile approach to eliminate antibiotics capable of being integrated into the currently existing water treatment systems.

Dynamic manipulation of enzymatic activity is a challenging task for applications in chemical and pharmaceutical industries due to the difficult modification and variable conformation of various enzymes.Here, we report a new strategy for reversible dynamic modulation of enzymatic activity by near-infrared light-induced photothermal conversion based on polyphenol-functionalized liquid metal nanodroplets（LM）. The metal-phenolic nanocoating not only provides colloidal stability of LM nanodroplets but also generates nanointerfaces for the assembly of various enzymes on the LM nanodroplets. Upon near infrared（NIR） irradiation, the localized microenvironmental heating through photothermal effect of the LM nanodroplets allows tailoring the enzymatic activity without affecting the bulk temperature. A library of functional enzymes, including proteinase K, glucoamylase, glucose oxidase, and Bst DNA polymerase, is integrated to perform a reversible control and enhanced activities even after five times of cycles, demonstrating great potential in bacterial fermentation, bacteriostasis, and target gene amplification.

The production of high-valued organonitrogen chemicals, especially N-heterocycles, requires artificial N 2 fixation accompanied by the consumption of fossil resources. To avoid the use of these energy- and resource-intensive processes, we develop a sustainable strategy to convert nitrogen-rich animal biomass into N-heterocycles through a thermochemical conversion process (TCP) under atmospheric pressure. A high percentage of N-heterocycles (87.51%) were obtained after the TCP of bovine skin due to the abundance of nitrogen-containing amino acids (e.g., glycine, proline, and l -hydroxyproline). Animal biomass with more diverse amino acid composition (e.g., muscles) yielded higher concentrations of amines/amides and nitriles after TCP. In addition, by introducing catalysts (KOH for pyrrole and Al 2 O 3 for cyclo-Gly–Pro) to TCP, the production quantities of pyrrole and cyclo-Gly–Pro increased to 30.79 mg g −1 and 38.88 mg g −1 , respectively. This approach can be used to convert the significant animal biomass waste generated annually from animal culls into valued organonitrogen chemicals while circumventing NH 3 -dependent and petrochemical-dependent synthesis routes. Graphical Abstract

Nano-/microplastics accumulate in aquatic bodies and raise increasing threats to ecosystems and human health. The limitation of existing water cleanup strategies, especially in the context of nano-/microplastics, primarily arises from their complexity (morphological, compositional, and dimensional). Here, highly efficient and bio-based flowthrough capturing materials (bioCap) are reported to remove a broad spectrum of nano-/microplastics from water: polyethylene terephthalate (anionic, irregular shape), polyethylene (net neutral, irregular shape), polystyrene (anionic and cationic, spherical shape), and other anionic and spherical shaped particles (polymethyl methacrylate, polypropylene, and polyvinyl chloride). Highly efficient bioCap systems that adsorb the ubiquitous particles released from beverage bags are demonstrated. As evidence of removal from drinking water, the in vivo biodistribution of nano-/microplastics is profiled, confirming a significant reduction of particle accumulation in main organs. The unique advantage of phenolic-mediated multi-molecular interactions is employed in sustainable, cost-effective, and facile strategies based on wood sawdust support for the removal of challenging nano-/microplastics pollutions.

The size and shape of the mesocrystals directly determine their properties, making the associated morphogenesis a means to engineer advanced materials from biogenic molecules. Unfortunately, the promise of the latter has been scarcely demonstrated, given their inherent anisotropic covalent bonding and limited tendency to form ordered structures. Herein, we report a library of mesocrystals derived from 3,4,5-tri-O-galloylquinic acid, which is a naturally occurring polyphenol. The direct structural characterization uncovers the crystallization path as the initial densification of prenucleated nanoscale intermediates and the followed continuous ordering into the final morphological changes. We demonstrate the possibility of affording biogenic mesocrystals with tailorable colloidal behavior by gaining control of the competitive intermolecular interactions that direct the self-assembly process.

The inhibition effects of copper（Ⅱ）-phenolic nanocomplexes on algal growth and its effect on lettuce in hydroponics were studied. In this study, natural polyphenols（Bayberry tannin, Valonia tannin, Tara tannin, and Tannin acid） and functional metal ions（copper ions） were used as building blocks to engineer self-assembled copper（Ⅱ）-phenolic nanocomplexes, and the inhibition experiment of copper（Ⅱ）-phenolic nanocomplexes for Chlorella vulgaris and application of copper（Ⅱ）-phenolic nanocomplexes on actual hydroponic lettuce were designed. The results showed that: 1) The polyphenol-induced interface interaction enabled the attachment of copper（Ⅱ）-phenolic nanocomplexes on the surface of algal cells, which continuously and precisely delivered metal ions（copper ions） to algae, resulting in oxidative damage and cell death. Thus, the copper（Ⅱ）-phenolic nanocomplexes presented long-lasting inhibition for algae, and the corresponding inhibition rate of Cu Ⅱ -BT still reached 99% on the 7th day for C.vulgaris. 2) The algal inhibition experiments showed that the inhibition ability of Cu Ⅱ -BT and Cu Ⅱ -VT for C.vulgaris was better than that of Cu Ⅱ -Tr and Cu Ⅱ -TA. 3) Plant experiments showed that copper（Ⅱ）-phenolic nanocomplexes could inhibit algae during actual production, and there was no difference in fresh weight of lettuce seedlings compared with the control group. These results demonstrate the copper（Ⅱ）-phenolic nanocomplexes had greater biosafety. Thus, the self-assembled copper（Ⅱ）-phenolic nanocomplexes could inhibit algal blooms in actual hydroponic production, which contributed to reduce the problem of loss of crop yield caused by algal blooms.

The growing global population necessitates substantial increases in food production. Hydroponic cultivation systems afford a critical alternative for food sustainability and enable stable annual production regardless of the climatic and geographical variations. However, the overgrowth of harmful algal blooms significantly threatens the crop yield by competing with nutrition in the solution and producing contaminants. The conventional practice of algaecides fails to control algal proliferation due to the limited efficiency and food safety concerns. Nanopesticides can deliver active ingredients responsively to suppress crop diseases and offer solutions to current practical challenges and difficulties. Inspired by prospects of nanotechnology for agricultural applications, we have utilized natural polyphenols and copper ions (Cu2+ ions) to develop self-assembled nanoalgaecides referred to as CuBes. The nanoalgaecide attached to algal cells via phenolic surface interactions, enabling localized Cu2+ ion release. This cell-targeted delivery suppressed Chlorella vulgaris for over 30 days (99% inhibition). Transcriptomics revealed that the nanoalgaecide disrupted algal metabolism by downregulating photosynthesis and chlorophyll pathways. In a solar-illuminated plant factory, the nanoalgaecide showed higher algal inhibition and lettuce biosafety versus the commercial Kocide 3000. Notably, the use of nanoalgaecide can enhance the nutrient value of lettuces, which meets the daily supply of Cu for adults. By integrating smart nanotechnology design with selective delivery mechanisms, this metal-phenolic nanoalgaecide provides a nanoenabled solution for controlling harmful algal blooms in hydroponics to advance food production.

The wide-spread overuse and misuse of antibiotics has led to major risks to human health, which demands breakthrough technologies for elimination of antibiotics from water streams. Membrane-based water purification has drawn substantial interest for this purpose. However, high permeance and high antibiotic removal efficiency remain extremely challenging. In this work, the use of polyphenol-based nanoengineering to functionalize conventional microporous membranes capable of ultrafast removal of 10 different antibiotics in an in-line flow-through purification system is explored. The high adsorption kinetics of these nanocoatings enable a record-high permeance (9774 L m−2 h−1 bar−1) with exceptional removal rate and efficiency, at a relatively low energy cost (0.09 kWh m−3), even in a real-world wastewater treatment. Molecular dynamics simulations provide detailed insights into the role of polyphenol-based nanocoatings and their multiple molecular interactions with antibiotics. This work provides a promising and sustainable platform for engineering the next-generation adsorption-based membranes for clean water production.

Traditional techniques for pollutant removal (e.g., static absorption and membrane nanofiltration) are either time consuming or energy intensive with limited permeances. Here, we demonstrate a protocol to fabricate polyamide (PA) -based regenerable adsorption-based membranes (PArab) for ultrafast removal of antibiotics. This protocol describes how to determine the distribution of nano-coatings through the membrane. We also detail the antibiotics removal performance and the regeneration tests. For complete details on the use and execution of this protocol, please refer to Wang et al. (2023).1

Tissue (re)vascularization strategies face various challenges, as therapeutic cells do not survive long enough in situ, while the administration of pro-angiogenic factors is hampered by fast clearance and insufficient ability to emulate complex spatiotemporal signaling. Here, we propose to address these limitations by engineering a functional biomaterial capable of capturing and concentrating the pro-angiogenic activities of mesenchymal stem cells (MSCs). In particular, dextran sulfate, a high molecular weight sulfated glucose polymer, supplemented to MSC cultures, interacts with MSC-derived extracellular matrix (ECM) components and facilitates their co-assembly and accumulation in the pericellular space. Upon decellularization, the resulting dextran sulfate-ECM hybrid material can be processed into MIcroparticles of SOlidified Secretome (MIPSOS). The insoluble format of MIPSOS protects protein components from degradation, while facilitating their sustained release. Proteomic analysis demonstrates that MIPSOS are highly enriched in pro-angiogenic factors, resulting in an enhanced pro-angiogenic bioactivity when compared to naïve MSC-derived ECM (cECM). Consequently, intravital microscopy of full-thickness skin wounds treated with MIPSOS demonstrates accelerated revascularization and healing, far superior to the therapeutic potential of cECM. Hence, the microparticle-based solidified stem cell secretome provides a promising platform to address major limitations of current therapeutic angiogenesis approaches.

Designing a hemoperfusion adsorbent for the excretion therapy of toxic heavy metals still remains a great challenge due to the biosafety risks of non-biological materials and the desired highly efficient removal capacity. Herein, inspired from the homeostasis mechanism of plants, natural polyphenols are integrated with collagen matrix to construct a polyphenol-functionalized collagen-based artificial liver (PAL) for heavy metals excretion and free radicals scavenging therapy. PAL presents high adsorption capacities for Cu2+, Pb2+, and UO22+ ions, up to 76.98 mu mol g(-1), 106.70 mu mol g(-1), and 252.48 mu mol g(-1), respectively. Remarkably, PAL possesses a high binding affinity for UO22+, Pb2+, and Cu2+ ions even in the complex serum environment with the presence of biologically-relevant ions (e.g., Mg2+, Ca2+ ions). Low hemolysis ratio (1.77%), high cell viability (> 85%), high plasma recalcification time (17.4 min), and low protein adsorption (1.02 mu mol g(-1)) indicate outstanding biocompatibility of this material. This natural polyphenol/collagen-based fully bio-derived hemoperfusion adsorbent provides a novel and potentially applicable strategy for constructing a hemoperfusion adsorbent for heavy metal ions excretion therapy with efficiency and biosafety.

Face masks are effective response to address this havoc pandemic caused by respiratory infection virus, but they are lack of reusable, antibacterial, and antiviral abilities due to their simple filtration mechanism, bringing to a supply shortage and severe plastic pollution globally. Herein, we designed reusable, antiviral, and antibacterial masks (referred to as R2A masks) that transformed from commonly-used standard masks and household fabrics based on the polyphenol-based surface functionalization. R2A nanocoatings are mainly composed of supramolecular complexation of natural polyphenols and metal ions, possessing a high performance of antibacterial property and comprehensive recyclability. Interfacial interaction of R2A nanocoating can effectively capture the spreading of particulate matters and aerosols containing virus-mimic nanoparticles even after 10 recycles. Moreover, R2A masks exist antibacteria and antivirus for severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2). Collectively, this simple functional enhancement of masks provides a sustainable and strategic preparation for combating the infectious respiratory diseases.

New materials for combating bacteria-caused infection and promoting the formation of microvascular networks during wound healing are of vital importance. Although antibiotics can be used to prevent infection, treatments that can disinfect and accelerate wound healing are scarce. Herein, we engineer a coating that is both highly compatible with current wound dressing substrates and capable of simultaneously disinfecting and revascularizing wounds using a metal-phenolic nanoplatform containing an alloyed nanostructured architecture (Ag@Cu-MPNNC). The alloyed nanostructure is formed by the spontaneous co-reduction and catalytic disproportionation reaction of multiple metal ions on a foundation metal-phenolic supramolecular layer. This synergistic presence of metals greatly improves the antibacterial activity against both Gram-negative and Gram-positive pathogenic bacteria, while demonstrating negligible cytotoxicity to normal tissue. In infected rat models, the Ag@Cu-MPNNC could kill bacteria efficiently, promoting revascularization and accelerate wound closure with no adverse side effects in infected in vivo models. In other words, this material acts as a combination therapy by inhibiting bacterial invasion and modulating bio-nano interactions in the wound.

Collagen, the main component of mammal skin, has been traditionally used in leather manufacturing for thousands of years due to its diverse physicochemical properties. Collagen is the most abundant protein in mammals and the main component of the extracellular matrix (ECM). The properties of collagen also make it an ideal building block for the engineering of materials for a range of biomedical applications. Reproductive medicine, especially human fertility preservation strategies and reproductive organ regeneration, has attracted significant attention in recent years as it is key in resolving the growing social concern over aging populations worldwide. Collagen-based biomaterials such as collagen hydrogels, decellularized ECM (dECM), and bioengineering techniques including collagen-based 3D bioprinting have facilitated the engineering of reproductive tissues. This review summarizes the recent progress in applying collagen-based biomaterials in reproductive. Furthermore, we discuss the prospects of collagen-based materials for engineering artificial reproductive tissues, hormone replacement therapy, and reproductive organ reconstruction, aiming to inspire new thoughts and advancements in engineered reproductive tissues research. Graphical abstract

The development of bioadhesives is an important, yet challenging task as seemingly mutually exclusive properties need to be combined in one material, that is, strong adhesion, water resistance, and high biocompatibility. Here, a biocompatible and biodegradable protein-based bioadhesive patch (PBP) with high adhesion strength and low immunogenic response is reported. PBP exists as a strong adhesion for biological surfaces, which is higher than some conventional bioadhesives (i.e., polyethylene glycol and fibrin). Robust adhesion and strength are realized through the removal of interfacial water and fast formation of multiple supramolecular interactions induced by metal ions. The PBP's high biocompatibility is evaluated and immunogenic response in vitro and in vivo is neglected. The strong adhesion on soft biological tissues qualifies the PBP as biomedical glue outperforming some commercial products for applications in hemostasis performance, accelerated wound healing, and sealing of defected organs, anticipating to be useful as a tissue adhesive and sealant.

Rationale: The combination of photosensitizers, oxygen supply agents, and adjuvant therapy drugs in a single nano-drug delivery system for photodynamic therapy (PDT) has been showing great promises to overcome the inherent challenges of PDT for tumor treatment. However, the complicated preparation of integrating multiple components hampers their further developments. Here, we describe a self-assembly nanomicelle with rationally designed building blocks, which shows a high efficiency of synergistic chemo-photodynamic therapy in the animal modal. Methods: The nanomicelle was prepared by a coordination-driven self-assembly based on a rationally designed ferrocene cyclopalladated compound coupled with photosensitizers and hyaluronic acid (referred to as FCP-Tph/HA). The morphology, targeting drug delivery, pharmacokinetics, hemolysis, and multimodal synergistic therapy of FCP-Tph/HA were investigated. Results: The formation of nanomicelles presents a low hemolysis rate and a prolonged blood circulation time. FCP-Tph/HA possesses an enhanced antitumor effect in vitro through the specific binding of HA to CD44 and combining chemotherapy with oxygen self-supplying PDT. Simultaneously, the nanomicelle facilitates a significantly improved antitumor efficacy (>90% tumor regression) on a breast cancer model in vivo. Conclusion: Our results present a modular self-assembled nanomicellar platform with synergistic chemo-photodynamic therapy for challenging PDT-based tumor treatment.

Highly efficient removal of bilirubin from blood by hemoperfusion for liver failure therapy remains a great challenge in the clinical field due to the unsatisfied biocompatibility of non-biological materials and the slow adsorption kinetics of currently used bilirubin adsorbents. Here, inspired by the natural collagen-supported multiscale structures of the liver for bilirubin removal, a natural collagen-based artificial liver, named ColAL, was successfully constructed via a biomimetic synthetic strategy. ColAL exhibited a record-high adsorption capacity of 102.32 mg g(-1) for bilirubin in the presence of 40.0 g L-1 bovine serum albumin. The ColAL also presented excellent bilirubin adsorption capacity in the complex serum. Importantly, the total bilirubin (TBIL) removal rate was higher than 69.17% and the direct bilirubin (DBIL) removal rate was 75.31% by immersing the ColAL in ex vivo blood samples. No damages were observed in the major organs after the injection of ColAL extract solution subcutaneously in vivo, indicating high biocompatibility and biostability of these natural collagen-based materials. This facile approach provides a new avenue to develop collagen-based high-performance hemoperfusion adsorbent for the removal of bilirubin, showing great promise to the translational therapy of hyperbilirubinemia.