Anti-inflammatory compounds, delivered as a payload to the gastrointestinal tract (GIT) by carriers, still cannot treat inflammatory bowel diseases without avoiding side effects. Here, we developed payload-free protein nanoparticles (PNPs) that crossed GIT to retain in the colon and treat colitis by restoring intestinal barrier integrity by modulating gut microbiome and metabolome. Specifically, PNPs, orally administered to mice with acute colitis, reached the colon within three hours. Consequently, PNPs improve gut microbiota dysbiosis to reverse metabolism balance, suppressing the expression of tumor-necrosis factor α and toll-like receptor 4 that restores the intestinal barrier integrity. PNPs then ameliorated colon inflammation and attenuated gut microbiota dysbiosis by exerting probiotic effects on gut microbiota, treating colitis in a week more effectively than the clinically often used 5-aminosalicylic acid without causing undesired side effects. Such PNPs represent safe, sustainable, and cost-effective therapeutics for treating inflammatory and metabolic diseases by eliminating microbial and metabolomic imbalance.

Two series of 3d-Gd mixed-metal phosphonate complexes with either only two gadolinium centers such as {Gd₂}, {Ni₂Gd₂}, {Co₄Gd₂}, {Co₈Gd₂}, {Fe₆Gd₂}, and {Fe₁₇Gd₂} or more than two gadoliniums such as {Co₈Gd₄}, {Mn₈Gd₄}, {Co₄Gd₆}, {Mn₄Gd₆}, {Co₆Gd₈}, {Ni₅Gd₈}, {Ni₆Gd₆}, {Co8Gd₈}, and {Mn₉Gd₉} have been solvothermally prepared and magnetothermally studied. The nearly identical environments of the Gd(III) dimer in the first series allow us to qualitatively analyze the effect of magnetic exchange coupling on the magnetocaloric effect (MCE). By doubling, tripling, or quadrupling of the Gd(III) centers, the second series of 3d-Gd mixed-metal complexes was built to further test the other effects of exchange couplings on MCE in more complicated circumstances. For the antiferromagnetic coupling cases, the results are nearly identical but diversify when topological spin frustrations are created, whose massive low-lying excited spin states help enhance MCE. For presumably ferromagnetically coupled ones, albeit are rare in phosphonate complexes, they do exhibit excellent MCE. Meanwhile, the complexes with weakly coupled metal centers serve as excellent examples for studying the effect of molecular mass on MCE when its magnitude is expressed in the unit of Joule per kilogram, from which we can see the values are directly proportional to the percentage of the Gd(III) ions in molecular weight.

Electrochemical devices allow the conversion and storage of renewable energy into high-value chemicals to mitigate carbon emissions, such as hydrogen production by water electrolysis, carbon dioxide reduction, and the electrochemical synthesis of ammonia. Independent regulation of the electrode pH environment is essential for optimizing the electrode reaction kinetics and enriching the catalyst species. The in situ water dissociation (WD, H₂O → H⁺ + OH⁻) in bipolar membranes (BPMs) offers the possibility of realizing this pH adjustment. Here, the design principles of high-performance polymeric BPMs in electrochemical device applications are presented by analyzing and connecting WD principles and current-voltage curves. The structure-transport property relationships and membrane durability, including the chemical and mechanical stability of the anion- and cation-exchange layers as well as the integrality of the interfacial junction, are systematically discussed. The advantages of BPMs in new electrochemical devices and major challenges to break through are also highlighted. The improved ion and water transport in the membrane layer and the minimized WD overpotential and ohmic loss at high current densities are expected to facilitate the promotion of BPMs from conventional chemical production to novel electrochemical applications.

Incorporating metal nanoparticles (MNPs) in metal-organic frameworks (MOFs) demonstrated great potential in the field of photo-/photothermal-catalysis. However, the oriented design and optimization of the 3D nano-architectures of MOF substrates to achieve high-efficiency light harvesting remains a challenge. Herein, guided on theoretical simulation, a facile etching strategy was employed to fabricate a 3D orderly-stacked-MOF-nanosheet-structure (CASFZU-1) with a high electric field energy-density-distribution; well-dispersed MNPs were afterwards encapsulated onto the MOF support. The unique nanosheet structure improved the light absorbance over the broadband spectrum, thereby enhancing the plasmonic photothermal effects of the MNPs@CASFZU-1 composites. Based on the plasmondriven photothermal conversion, the MNPs@CASFZU-1 composites exhibited approximately twofold catalytic efficiency in the hydrogenation reaction and a lower temperature for the full conversion of carbon monoxide, compared to their bulk-type composites. The surface-plasmon-driven photothermal effects can be exploited in innovative MNPs@MOF platforms for various applications.

To combat the dwindling supply of freshwater, solar-driven desalination using plasmonic nanomaterials has emerged as a promising and renewable solution. Refractory plasmonic carbide nanomaterials are exciting candidates that are inexpensive and chemically robust but have not been widely explored. Herein, plasmonic carbide interfaces made of TiC, ZrC, and HfC nanoparticle aggregates loaded onto to a mixed cellulose ester (MCE) membrane were explored to gain insight into their solar-vapor generation and desalination potential. Desalination using Atlantic Ocean water under 1 sun intensity yielded rates of 1.26 ± 0.01, 1.18 ± 0.02, and 1.40 ± 0.01 kg m⁻² h⁻¹, with efficiencies of 86%, 80%, and 96% for TiC, ZrC, and HfC, respectively. Carbide interfaces showed good stability and effectively removed heavy metal ions and salt from solutions with concentrations up to 35%. PVA hydrogel based TMC evaporators afforded rates of 3.31 ± 0.03 and 3.22 ± 0.03 kg m⁻² h⁻¹ for TiC and ZrC, respectively. The HfC-PVA interface afforded a high solar desalination rate of 3.69 ± 0.04 kg m⁻² h⁻¹, corresponding to an efficiency of 97% under 1-sun illumination. The hydrogel evaporators also retained their strong salt rejection action over time.

Controlling the growth of bacterial biofilms in a specific pattern greatly enhances the study of cell-to-cell interactions and paves the way for expanding their biological applications. However, the development of simple, cost-effective, and highly resolved biopatterning approaches remains a persistent challenge. Herein, a pioneering photodynamic biopatterning technique for the creation of living bacterial biofilms with customized geometries at high resolutions is presented. First of all, an outstanding aggregation-induced emission photosensitizer is synthesized to enable efficient photodynamic bacterial killing at a low concentration. By combining with custom-designed photomasks featuring both opaque and transparent patterns, the viability of photosensitizer-coated bacteria is successfully manipulated by controlling the degree of light transmittance. This process leads to the formation of living bacterial biofilms with specific patterns replicated from the photomask. Such an innovative strategy can be employed to generate living bacterial biofilms composed of either mono- or multispecies, with a spatial resolution of approximately 24 µm. Furthermore, its potential applications in information storage/encryption and antibiotic screening are explored. This study provides an alternative way to understand and investigate the intricate interactions among bacteria within 3D biofilms, holding great promise in the controlled fabrication of dynamic biological systems for advanced applications.

The “laboratory” of cells has the capacity to polymerize monosaccharides, amino acids, and nucleotides. Tumor cells, characterized by the overexpression of multiple enzymes and existing in a slightly acidic and highly redox-potent environment, have attracted the attention of chemists aiming to transfer chemical reactions from the traditional laboratory flask to this “cellular laboratory”. Polymers, resulting from the repetitive linkage of monomers, have garnered extensive utility in the biomedical field due to their diverse structural and physicochemical properties. When the polymerization reaction proceeds in situ within the tumor cells, this in situ transformation from small-to-large combines the rapid uptake of monomeric molecules with the strong retention ability of polymers, exerting a profound impact on drug delivery within tumors. Moreover, it shows promising applications in the regulation of cell behavior, imaging, therapy, and theranostics. Given the diverse functions of in situ polymerization in relation to tumor cells, this review focuses on a comprehensive examination of various strategies for in situ polymerization within tumor cells, categorizing these strategies based on the formation mechanisms of polymers. The applications in this domain concerning in situ polymerization within tumor cells are also explored. Moreover, a discussion of specific limitations in current research and insights into potential future directions from the authors’ perspective are provided.

Reactive oxygen species (ROS) have certain effect in cancer treatment, thus many studies have been focused on developing functional systems to generate ROS in tumor. Here, inspired by the multi-enzyme biocatalysis in organisms, novel ultrasound-triggered temporospatial catalytic cascades systems are presented based on barium titanate (BTO) and platinum (Pt) co-loaded multi-component microparticles (Pt/BTO@MCMPs) to successively achieve oxygen and ROS production for tumor sonodynamic therapy. By using a customized capillary microfluidic device, the Pt/BTO@MCMPs are fabricated with Pt nanoparticles located in their core part and BTO nanocubes located in their peripheral part, alternating with blank porous hydrogel components for increasing interaction areas between the encapsulated nanomaterials and the ambient substrates. In the microparticles, the Pt can catalyze hydrogen peroxide from the tumor microenvironment to generate O₂ and H₂O serving as substrates for piezoelectric catalytic reactions, contributing to additional generation of ROS under US activation. Based on the system, it is demonstrated that the Pt/BTO@MCMPs are featured with excellent biocompatibility under normal biological conditions and show desired tumor eradication properties under ultrasound irradiation in mice carrying pancreatic tumors. These results indicate that the proposed ultrasound-triggered temporospatial catalytic cascades systems are promising for clinic anti-tumor applications.

Solar-driven interfacial evaporation is a promising technology for desalination. The photothermal conversion materials are at the core and play a key role in this field. Design of photothermal conversion materials based on organic dyes for desalination is still a challenge due to lack of efficient guiding strategy. Herein, a new D (donor)-A (acceptor) type conjugated tetraphenylpyrazine (TPP) luminophore (namely TPP-2IND) was prepared as a photothermal conversion molecule. It exhibited a broad absorption spectrum and strong π-π stacking in the solid state, resulting in efficient sunlight harvesting and boosting nonradiative decay. TPP-2IND powder exhibited high photothermal efficiency upon 660 nm laser irradiation (0.9 W cm⁻²), and the surface temperature can reach to 200°C. Then, an interfacial heating system based on TPP-2IND is established successfully. The water evaporation rate and the solar-driven water evaporation efficiency were evaluated up to 1.04 kg m⁻² h⁻¹ and 65.8% under 1 sunlight, respectively. Thus, this novel solar-driven heating system shows high potential for desalination and stimulates the development of advanced photothermal conversion materials.

New concept for the development of supramolecular assemblies from intricate interactions between different classes of biomacromolecules (polysaccharides, proteins and lipids) is yet to come, due to their intrinsic chemical and structural complexity and incompatibility. Herein, we report an interaction mechanism among multiple biomacromolecules, and the structural and digestive properties of their assemblies using amylose (AM), lauric acid (LA), and β-lactoglobulin (βLG) as exemplars. AM, LA, and βLG interact to form a water-soluble ternary complex through van der Waals forces between AM and LA and high affinity binding between AM and βLG, which can further assemble into uniform-sized, semi-crystalline nanospheres under certain thermodynamic conditions. These nanospheres are substantially resistant to amylolysis, thus can be well utilized by gut microbiota, including increasing short-chain fatty acid levels and shaping bacterial communities. Illustrating the complexation of AM, LA, and βLG and their assemblies from disorder to order, this work offers potential rationale of assemblies for multiple biomacromolecules driven by non-covalent interactions and substantial potentials for supramolecular biomaterials development.

Osteoarthritis has been regarded as a complex and serious degenerative disease. Attempts in this area are focused on improving the curative effect of stem cellbased therapies. In this work, we present a novel inverse opal microcarriers-based cytokines delivery system to induce autologous stem cell homing for osteoarthritis treatment. Considering their important role in stem cell recruitment and chondrogenic differentiation respectively, platelet-derived growth factor BB (PDGF-BB) and transforming growth factor β3 (TGF-β3) are loaded into inverse opal microcarriers as model cytokines. Since cytokine release induces the corresponding variations in characteristic reflection spectra and structural colors, the inverse opal microcarriers possess the optical self-reporting capacity to monitor the release process. In vitro cell experiments reveal that inverse opal microcarriers could successfully recruit the gathering of mesenchymal stem cells through the release of loaded cytokines. Based on these features, we have demonstrated the enhanced therapeutic effect of PDGF-BB and TGF-β3 loaded inverse opal microcarriers in the treatment of rat osteoarthritis models. These results indicate that the multifunctional inverse opal microcarriers-based cytokines delivery system would find broad prospects in osteoarthritis treatment and other biomedical fields.

Plasma protein-induced aggregation of nanoparticles (NPs) is a crucial issue in many applications, such as drug delivery. Although great efforts have been made to investigate the protein adsorption kinetics or protein-induced NPs coalescence in bulk solutions, limited evidence has been uncovered for interfacial circumstances. Diet, disease, medicine, or senility could thoroughly change interfacial physicochemical properties of the inner lining of blood vessels. Implants including stents and artificial heart valves also have varied and evolutionary interfaces. Hence, there is an urgent need to understand the mechanism behind the non-specific protein adsorption and NP-protein aggregation in such interfacial cases. Here, we use evanescent light scattering to observe polystyrene NPs‒fibrinogen aggregation at substrates with varying surface properties. A density-fluctuation correlation function is utilized to reveal the relaxation dynamics of the aggregates. Both time-resolved and spatial-correlated evidence shows that the aging process of such soft materials is out-of-equilibrium, where the dynamics faster and slower than exponential can coexist in one single relaxation process. Besides, corona formation, inner stress, and interconnection together determine the microstructure, local adhesion, and structural relaxation of the aggregates, which can further correspond to the protein-to-NP ratio as well as the surface chemistry of NPs and substrates.

Chirality is one of the fundamental properties of molecules traditionally constructed from atoms. Here, we report for the first time the successful construction of asymmetric chiral structures utilizing highly symmetric endohedral metallofullerene superatoms based on their own bonding properties. Specifically, stable mirror-symmetric sinister and rectus structures are obtained by selecting a superatom capable of forming four chemical bonds as the chiral center. Further analysis shows that the chiral vibration frequency of superatomic assemblies can be as low as a few wavenumbers, which greatly expands the range of chiral spectra compared to atom-based molecules. We term this type of chirality based on superatoms as “superatomic-based chirality”. It is anticipated that this work will significantly expand the variety of chiral structures at the atomic level.

Aggregate-level photodynamic therapy (PDT) has attracted significant interest and driven substantial advances in multifunction phototheranostic platforms. As exemplified by two typical instances of aggregation-caused quenching of reactive oxygen species (ROS) and aggregation-induced generation of ROS, the aggregation effect plays a significant role on the ROS generation of photosensitizers (PSs), which is worthy of in-depth exploration and full utilization. However, in contrast to the well-developed researches on the aggregation effect on luminescence, the studies concerning the aggregation effect on ROS generation are currently in a relatively nascent and disjointed stage, lacking guidance from a firmly established research paradigm. To advance this regard, this review aims at providing a consolidated overview of the fundamental principles and research status of aggregation effects on the ROS generation. Here, the research status can be organized into two main facets. One involves the comparison between isolated state and aggregated state, which is mainly conducted by two methods of changing solvent environments and adding adjuvants into a given solvent. The other underscores the distinctions between different aggregate states, consisting of three parts, namely comparison within the same or between different categories based on the classification of single-component and multicomponent aggregates. In this endeavor, we will present our views on current research methodologies that explore how aggregation affects ROS generation and highlight the design strategies to leverage the aggregation effect to optimize PS regiments.We aspire this review to propel the advancement of phototheranostic platforms and accelerate the clinical implementation of precision medicine, and inspire more contributions to aggregate-level photophysics and photochemistry, pushing the aggregate science and materials forward.

Polyolefin-b-poly(ethylene oxide) (PEO) represents the most widely investigated amphiphilic block copolymers. So far, one-pot continuous synthesis of such hybrid block copolymers has only been fulfilled by anionic polymerization through sequential addition of vinyl monomers and ethylene oxide (EO). It still remains challenging to achieve altogether high block efficiency, high polymerization efficiency, and high molar mass for PEO. Here, we report a one-pot hybrid block copolymerization approach to polyisoprene/polystyrene(PI/PS)-b-PEO, in which PI/PS are formed by sBuLi-initiated anionic vinyl-addition polymerization, then in situ employed as macroinitiators for the anionic ring-opening polymerization (ROP) of EO aided by an organic Lewis pair. The cooperative (dual-ion-complexing) catalytic effect of organobase and triethylborane is proven, for the first time, effective for lithium alkoxide initiator system, allowing to achieve at room temperature high ROP activity (complete EO conversion and PEO of 3-64 kg/mol reached in 1-6 h), narrow molar mass distribution, controlled block lengths and composition. Density functional theory calculation shows that phosphazene bases are particularly effective, compared with N-heterocyclic bases, for complexing with Li⁺ and enhancing the nucleophilicity of oxyanion. The rate of ROP is also affected by Li⁺-induced aggregation of the chain-end ion pairs, which though can be offset by adequate catalyst loadings. The versatility of this approach is further demonstrated in the one-pot synthesis of tri-/tetrablock ter-/quaterpolymers constituted by PI, PS, PEO, and poly(propylene oxide). Of great interest, PS-b-PI-b-PEO triblock terpolymer with a specific composition is found to form internally microphase-separated micellar aggregates when dispersed in water.

Adsorbents with high adsorption efficiency and excellent biosafety for biomedical applications are highly required. MXene is a promising candidate owning these advantages, yet pristine MXene faces dilemmas including insufficient utility of surface site as well as limited processibility. Here, we develop MXene-encapsulated porous microcapsules via microfluidics. The microcapsules have a biomass hydrogel shell that provides robust support for MXene in the core, by which the microcapsules are endowed with high MXene dosage and remarkable biosafety. Additionally, the MXene nanoflakes assemble into a three-dimensional network via metal ion-induced gelation, thereby avoiding restacking and significantly improving surface utilization. Moreover, a freeze-pretreatment of themicrocapsules during preparation results in the formation of a macroporous structure in the shell, which can facilitate the diffusion of the target molecules. These features, combined with additional magnetoresponsiveness rendered by the incorporation of magnetic nanoparticles, contribute to prominent performances of the microcapsules in cleaning uremia toxins including creatinine, urea, and uric acid. Thus, it is anticipated that the MXene-encapsulated microcapsules will be promising adsorbents in dialysis-related applications, and the combination of microfluidic encapsulation with metal ion gelation will provide a novel approach for construction of hybrid MXene materials with desired functions.

Polar fluorinated arenes can promote organic free radical reactions, which have attracted scientists’ interest in recent years. However, it is still unknown how these solvents interact weakly with organic radical molecules to influence their reactivity. In this study, we investigated how organic free radicals aggregate in five polar fluorocarbon solvents, and demonstrated that different substituents can influence their aggregation behaviors. In these solvents, small organic radicals with simple substituents maintain a homogeneous solution; however, radicals with substituents that form intermolecular hydrogen bonds or with long-chain aliphatic hydrocarbons tend to aggregate in them, whereas substituents of long-chain aliphatic hydrocarbons tend to promote aggregation better. The critical aggregation concentrations of these aggregates are measured by concentration-dependent UV-visible spectroscopy. Their topological morphologies are all spherical based on TEM. The compactness and rotational motivation speed of radical molecules within these aggregates are determined by EPR spectroscopy. The particle sizes of these aggregates are determined by analyzing their cyclic voltammograms. Most excitingly, electrochemical experiments reveal that the aggregation behaviors of free radical molecules with intermolecular hydrogen bonds can significantly increase their catalytic rate for electro-oxidizing benzyl alcohol in such a solvent. The results of this study indicate that in polar fluorinated arenes organic radical molecules’ aggregation behaviors are related to their structures. This may provide guidelines for regulating organic radical reactivity in these solvents in the future.

Organic solar cells (OSCs) have attracted much interest in the past few decades because of their advantages, such as being lightweight, low cost, simple preparation process, and environmental friendliness. While researchers have made significant progress on the active layer materials of OSCs, the interface engineering is another entry point for upgrading the photovoltaic performance of OSCs. Significantly, the interface modification materials, including anode interfacial materials and cathode interfacial materials, are two essential parts of interfacial layers for OSCs, in which the excellent interfacial materials can realize the very high-performance photovoltaic cells. Among these interfacial materials, the anode interfacial layers (AILs) play a crucial role in improving photovoltaic performance. This review expresses a detailed conclusion of the development of anode interfacial materials and an outlook on future trends for OSCs.

PD-1/PD-L1 inhibitors have emerged as standard treatments for advanced solid tumors; however, challenges such as a low overall response rate and systemic side effects impede their implementation. Hypoxia drives the remodeling of the tumor microenvironment, which is a leading reason for the failure of immunotherapies. Despite some reported strategies to alleviate hypoxia, their individual limitations constrain further improvements. Herein, a novel two-pronged strategy is presented to efficiently address hypoxia by simultaneously adopting atovaquone (ATO, inhibiting oxygen consumption) and oxyhemoglobin (HbO₂, directly supplementing oxygen) within a multifunctional aggregate termed NPs-aPD-1/HbO₂/ATO. In addition to eliminating hypoxia with these two components, this smart aggregate also includes albumin and an ROS-responsive cross-linker as a controlled release scaffold, along with PD-1 antibody (aPD-1) for immunotherapy. Intriguingly, NPs-aPD-1/HbO₂/ATO demonstrates exceptional tumor targeting in vivo, exhibiting ≈4.2 fold higher accumulation in tumors than in the liver. Consequently, this aggregate not only effectively mitigates hypoxia and significantly assists aPD-1 immunotherapy but also simultaneously resolves the targeting and systemic toxicity issues associated with individual administration of each component. This study proposes substantial implications for drug-targeted delivery, addressing tumor hypoxia and advancing immunotherapy, providing valuable insights for advancing cancer treatment strategies.

J-aggregation and H-aggregation are identified as two classical models of functionally oriented non-covalent interactions, and significant attention has been drawn by researchers. However, due to the scarcity of single-crystal examples of Haggregation, a comprehensive understanding of the relationship between its stacking mode and optical behaviour has been hindered. In recent studies, two polyaromatic Schiff base compounds, Cl-Salmphen and H-Salmphen, were successfully synthesized, and both were found to exhibit H-aggregation. In the findings, H-Salmphen was shown to display typical C─H···π interactions, characteristic of Aggregation-Induced Emission (AIE) active molecules, whereas its halogenated counterpart was identified as behaving similar to Aggregation-Caused Quenching (ACQ) active molecules. These types of results suggest that identical intermolecular interactions can produce differing optical behaviours. Light was shed, at least in part, on the formation mechanisms of H-type aggregates and their luminescence properties from these observations. Additionally, the high optical signal-to-noise ratio inherent to H-aggregates was utilized for the exploration of water content detection. As an outcome, a high-performance fluorescent filter paper was developed, enabling easy real-time detection using a smartphone.

Currently three major problems seriously limit the practical application of cancer photodynamic therapy (PDT): (i) the hypoxic tumor microenvironment (TME); (ii) low generation efficiency of toxic reactive oxygen species (ROS) in aggregates and (iii) shallow tissue penetration depth of excitation light. Very limited approaches are available for addressing all the above three problems with a single design. Herein, a rational “three birds with one stone” molecular and nanoengineering strategy is demonstrated: a photodynamic nanoplatform U-Ir@PAA-ABS based on the covalent combination of lanthanide-doped upconversion nanoparticles (UCNPs) and an AIE-active dinuclear Ir(III) complex provides a low oxygen concentration-dependent type-I photochemical process upon 980 nm irradiation by Föster resonance energy transfer (FRET). U-Ir@PAA-ABS targets mitochondria and has excellent phototoxicity even in severe hypoxia environments upon 980 nm irradiation, inducing a dual-mode cell death mechanism by apoptosis and ferroptosis. Taken together, the in vitro and in vivo results demonstrate a successful strategy for improving the efficacy of PDT against hypoxic tumors.

Structures in nature are often multi-material, and their structures have a fine balance between segregation and aggregation (mixed, but not scrambled) that provides functionality. Chaotic fabrication, a technology that exploits the ability of chaotic advection to create predictable and reproducible multilayered structures, excels at producing materials where this balance can be achieved and finely tuned. This method is based on the use of chaotic mixing systems, which can produce constructs with highly organized internal micro-architecture in a simple and cost-effective way. This manuscript provides a perspective on how chaotic printing can be a great enabler in the manufacture of advanced materials, including living tissues. Chaotic printing may overcome many of the critical hurdles that are currently faced in manufacturing and biofabrication (e.g., creating a wide array of interfaces, reaching high resolutions rapidly and at low cost, and producing densely vascularized tissues). The manuscript introduces the technology, explains how the idea originated, presents a timeline that provides a recapitulation of the milestones achieved so far, describes the main characteristics, advantages, limitations, and challenges of the technology, and concludes with future perspectives on the evolution and use of this versatile method.

Microfibers from natural products are endowed with remarkable biocompatibility, biodegradability, sustainable utilization as well as environmental protection characteristics etc. Benefitting from these advantages, microfibers have demonstrated their prominent values in biomedical applications. This review comprehensively summarizes the relevant research progress of sustainable microfibers from natural products and their biomedical applications. To begin, common natural elements are introduced for the microfiber fabrication. After that, the focus is on the specific fabrication technology and process. Subsequently, biomedical applications of sustainable microfibers are discussed in detail. Last but not least, the main challenges during the development process are summarized, followed by a vision for future development opportunities.

Surgical resection is the preferred option for hepatocellular carcinoma (HCC), but surgical navigation technology using indocyanine green still has some drawbacks such as non-specific imaging, thus it is very important to develop new fluorescence imaging technology. All-cis hexaphenyl-1,3-butadiene derivative (ZZ-HPB-NC) with aggregation-induced emission (AIE) feature has been reported to be quickly turned-on fluorescent response in the intraoperative frozen-section slides of HCC. However, the probe did not respond to normal liver tissue around HCC. In order to enhance the diagnostic rate and elucidate the response mechanism, all-trans configuration EE-HPB-NC, was furtherly synthesized. Within two minutes, non-cancer tissues could be fluorescently labeled by EE-HPB-NC by spraying, showing the same effect with ZZ-HPB-NC to HCC. The results indicated that the configurationinduced cross-identification fluorescence imaging strategy was achieved through the combination of ZZ- and EE-HPB-NC. Then the mechanism of HPB-NC localization in HCC lesions was explored, and the binding of HPB-NC with specific proteins in cells resulted in the AIE effect to label HCC cells. On this basis, the accuracy of specific fluorescence imaging for HCC was further verified on the mouse hepatic neoplasm models, indicating that it has clinical application potential for surgical fluorescence real-time navigation.

Accurate and sensitive near-infrared (NIR) luminescent lateral flow immunoassay (LFIA) has attracted considerable attention in the field of point-of-care testing (POCT). However, the detection accuracy and sensitivity are often compromised by the low fluorescence quantum efficiency (<10%) of the NIR fluorescent probe. Herein, ultrabright NIR AIEgen nanoparticles (PS@AIE830NPs) composed of polystyrene (PS) nanoparticles and NIR aggregation-induced emission luminogen (AIEgen) with the maximum emission at 830 nm (AIE₈₃₀) is reported, and its potential to promote an accurate and sensitive detection of complex samples by LFIA is described. The relative quantum yield (QY) of the PS@AIE₈₃₀NPs was 14.76%, which was superior to that of the polymer embedding method and indocyanine green (ICG)-based NIR nanoparticles. The PS@AIE830NPs immunolabeled-LFIA combined with laboratory-built NIR-LFIA portable quantitative instruments (detected light range > 800 nm) completely eliminated background interference and allowed highly accurate and sensitive detection without any pre-treatment steps. The limits of detection (LODs) for aflatoxin B₁ (AFB₁) in soy sauce, alpha hemolysin (Hla) of Staphylococcus aureus biomarker in joint fluid, and C-reactive protein (CRP) in human haemolysed samples were 0.01 ng mL⁻¹, 0.02 µg mL⁻¹, and 0.156 mg L⁻¹, respectively, commensurating with those of the corresponding gold standard assays and covering the detection range of interests. It is anticipated that the ultrabright NIR AIEgen nanoparticles will serve as a universally applicable signal probe for NIRLFIA diagnostics, promising to expand the range of applications for quantitative detection of complex samples.

The efficacy of transarterial chemoembolization (TACE) has been limited by insufficient embolization and a high incidence of tumor recurrence. Herein, we identified that aberrant metabolic reprogramming and immunosuppression contribute to TACE refractoriness and Rhein, as a potential glycolytic metabolism inhibitor and immunoactivation inducer, was optimized to sensitize tumors to TACE therapy. To achieve efficient embolization, we developed an oil-in-water lipiodol embolic emulsion by stabilizing the self-assembled Rhein nanogel. The assembled Rhein exhibited a nanofiber network, and its integration enhanced the mechanical stability and viscoelasticity of the lipiodol embolic agent. With the synergistic advantages of solid and liquid embolic agents, this carrier-free Pickering emulsion exhibits efficient embolization and sustained drug release in models of unilateral renal artery embolization, rabbit ear tumor embolization, rabbit orthotopic liver cancer, and rat orthotopic liver cancer. Compared to conventional three-way catheter mixing methods, multimodal imaging corroborates a marked enhancement in local drug retention and tumor suppression. Importantly, the incorporation of Rhein-mediated synergistic immunoembolization in this strategy achieved efficient embolization while robustly activating anti-tumor immune responses, including inducing immunogenic cell death, dendritic cell activation, and major histocompatibility complex class I presentation to CD8+ T cells for tumor killing. Together, these findings reveal a novel strategy for the application of self-assembled Rhein nanofiber-stabilized lipiodol emulsion to control metabolic signaling and immunoactivation in TACE.

The multi-component strategy has proven effective in advancing the performance of organic photovoltaics (OPVs), enhancing photocurrent and fill factor through spectral complementarity and morphology optimization. However, the open-circuit voltage (V_OC) mechanism in multi-component systems lacks systematic investigation. In this study, we explore the influence of alloy-like phases on energy level distribution and energy loss mechanisms in multi-component OPVs. Appropriate modulation of donor alloy-like phases maintains the original intermolecular stacking, enhances component compatibility, reduces acceptor aggregation, and improves acceptor phase purity, mitigating non-radiative recombination losses. Additionally, suitable alloy-like phase modulation elevates charge transfer (CT) states, reducing the gap between CT and local exciton state, lowering reorganization energy, and alleviating radiative recombination loss below the bandgap. Through synergistic optimization (layer-by-layer method with solid additive), ternary devices based on Y6 acceptor achieve a notable 19.41% power conversion efficiency, offering new insights for the analysis of the energy loss of the multi-component OPVs.

The unfavorable photochemical processes at the molecular level have become a barrier limiting the use of aromatic amides as high-performance luminescent materials. Herein, we propose a reliable strategy for manipulating noncovalent conformational lock (NCL) via side-chain engineering to burst out eye-catching luminescence at the aggregate level. Contrary to the invisible emission in dilute solutions, dyad OO with a three-centered H-bond gave the wondrous crystallization-induced emission with a quantum yield of 66.8% and clusterization-triggered emission, which were much brighter than those of isomers. Theoretical calculations demonstrate that crystallization-induced planarized intramolecular charge transfer (PICT), conformation rigidification, and through-space conjugation (TSC) are responsible for aggregate-state luminescence. Robust NCL composed of intramolecular N-H···O interactions could boost molecular rigidity and planarity, thus greatly facilitating PICT and TSC. This study would inspire researchers to design efficient luminescent materials at the aggregate level via rational conformational control.

Silver sulfide thin film, with excellent thermoelectric properties, is few reported due to the complex and time-consuming high-temperature or high-pressure synthesis process. Here, a fast ionic conductor n-type Ag₂S film with good crystallinity and uniform density is prepared by sputtering metal Ag films of different thicknesses on glass and then reacting in S precursor solution at low temperature. At 450 K, β-Ag₂S films can be obtained and underwent a phase transition from α-Ag₂S monoclinic, which had a significant effect on their electrical and thermal properties. The grain size of Ag₂S films increases with the increase of film thickness. Before and after the phase transition, the carrier concentration and mobility cause obvious changes in the electrical properties of Ag₂S. The carrier concentration of body-centered cubic phase β-Ag₂S is about three orders of magnitude higher than that of monoclinic phase α-Ag₂S, and the mobility is also 2-3 times that of the latter. Especially, after the phase transition, the conductivity of β-Ag₂S rises exponentially from the zero conductivity of α-Ag₂S and increases with the increase of temperature. The Ag₂S film shows the highest figure of merit of 0.83 ± 0.30 at 600 K from the sample with~1600 nm thickness, which is the highest record among Ag₂S-based thermoelectric materials reported so far.

Avoiding the tedious process of crystal cultivation and directly obtaining organic crystals with desirable phosphorescent performance is of great significance for studying their structure and properties. Herein, a set of benzophenone-cored phosphors with bright green afterglow are obtained on a large scale through in-situ generation via an end-capping strategy to suppress non-radiative triplet excitons and reinforce the intermolecular interactions. The ordered arrangement of phosphors with alkyl-cyano groups as regulators is crucial for the enhancement of roomtemperature phosphorescence (RTP) emission, which has been further verified by the attenuated lifetimes in isolated states through the formation of inclusion complexes upon binding with pillar[5]arenes. Moreover, the hierarchical interactions of phosphors, including hydrogen bonding, π-π stacking interactions, and van der Waals forces, are quantified by crystal structures and theoretical calculation to deeply interpret the origins of RTP emission. With this study, we provide a potential strategy for the direct acquisition of crystalline organic phosphors and modulation of RTP.

Acute liver failure is a life-threatening syndrome, for which liver transplantation is presently the most effective treatment. Unfortunately, such treatment is extremely limited by a shortage of donor organs. Stem cell therapy offers a promising treatment strategy for acute liver failure. Yet, therapeutic efficacy and potential are hampered by administration route and safety concerns. In this work, we fabricated menstrual blood-derived stem cells-conditioned medium/polymersome hybrid nanoparticles that were self-assembled from amphiphilic block copolymers via the direct hydration method and encapsulated therapeutic bioactive factors within the aqueous core of vesicles. The merit of vesicular architecture enabled the loading capacity of distinct proteins and the maintenance of biological activity. These hybrid nanoparticles can be steadily taken up into cytoplasm and promote hepatocyte proliferation in vitro. Prolonged in vivo circulation time brought higher accumulation in livers. The therapeutic nanoparticles alleviated hepatic injury and promoted liver recovery in mice with carbon tetrachloride-induced liver failure. Considering the feasibility and benefit of the hybrid nanoparticle therapy, it provided a potential strategy to treat acute liver failure.

The blockade of cytoprotective autophagy has been demonstrated to effectively enhance the efficacy of sonodynamic therapy (SDT). However, the limited recognition of antiautophagy agents for autophagosomes impedes the clinical application of autophagy inhibition. To efficiently deliver hydroxychloroquine (HCQ), an autophagy inhibitor, to autophagosomes, we utilized a strategy based on in situ click chemistry between sulfhydryl (-SH) and maleimide (Mal) groups to trigger autophagosomes tracking and suppress tumor growth synergistically. A cascade nanoreactor was synthesized by encapsulating Mal-modified HCQ (^MHCQ) into a manganese porphyrin-based metal-organic framework with sonosensitizer properties, followed by poly(ethylene glycol)ylated liposomal membrane coating. After ultrasound irradiation, SDT-induced apoptotic cells released damaged proteins with free -SH groups, which ^MHCQ rapidly captured in situ via a Mal-thiol click reaction. When autophagosomes actively wrapped damaged proteins for detoxification, they simultaneously internalized HCQ anchored on proteins. In this scenario, antiautophagy drugs could actively track intracellular autophagosomes instead of undergoing passive diffusion in the cytosol. The interaction between HCQ and autophagic vesicles was greatly enhanced, which strengthened the blocking efficiency of autophagy and resulted in complete cell death. Overall, this study with smart design provides a promising strategy for improving intracellular targeted delivery to autophagosomes, thereby enhancing antitumor therapy.

Developing the sensitive point-of-care testing (POCT) of oncogenic nucleic acids from human papillomavirus (HPV) infection is essential in preventing cervical cancer, especially in resource-limited settings. Rolling circle amplification (RCA) is attractive in achieving POCT via nucleic acid-based aggregation under isothermal conditions. However, the influence of RCA product structure on the aggregation remains unexplored resulting in limited sensitivity. Here, a minimum secondary structured RCA technique (MSS-RCA) is developed by designing a unique circular template, demonstrating significantly enhanced detection sensitivity with only one amplification step and one primer under isothermal conditions. The amplification efficiency of MSS-RCA could be kinetically manipulated by controlling the secondary structure of the circular template. Introducing the invertase probe to MSSRCA, HPV16 E6/E7 nucleic acid target was detected with a personal glucose meter (PGM) with a sensitivity of 5 fM (50 zmol in 10 µL). This integrated MSS-RCAPGM detection system was successfully applied to detect HPV16 E6/E7 mRNA extracted from 54 cervical swab samples reaching a positive predictive value of 100.00% and negative predictive values of 96.00% (77.77% to 99.40%, 95% CI). MSS-RCA-PGM provides a sensitive POCT platform for the detection of nucleic acid biomarkers for screening of cervical cancer or other diseases.

The hydrothermal/soft templating method is an effective way to synthesize ordered mesoporous carbon (OMC), yet the mechanism of this strategy is not well illustrated. Herein, a hydrothermal temperature-controlled approach is developed to precisely synthesize OMCs with well-defined morphologies from liquefied wood (LW). As the hydrothermal temperature increases from 130 to 210°C, the hydrophilicity of the hydrophilic blocks decreases accompanied by the increase of the relative volume of the hydrophobic block, resulting in the packing parameter p of micelles changing from p ≤ 1/3 to 1/3 < p < 1/2, which transforms the micelle’s structure from spherical to cylindrical. Additionally, accelerated nucleation occurred with the increased hydrothermal temperature. When the rate of nucleation is matched to the self-assembly of the composite micelles, the composite micelles grow into worm-like morphology and an ordered p6m mesostructure. This hydrothermal temperature-controlled strategy provides a straightforward and effective approach for synthesizing OMCs with various morphologies from LW, addressing the previously insufficiently elucidated micelle formation mechanism in the hydrothermal/soft templating method.

Integrated multimodal imaging in theranostics nanomaterials offers extensive prospects for precise and noninvasive cancer treatment. Precisely controlling the structural evolution of plasmonic nanoparticles is crucial in the development of photothermal agents. However, previous successes have been limited to static assemblies and single-component structures. Here, an activatable plasmonic theranostics system utilizing self-assembled 1D silver-coated gold nanochains (1D nanochains) is presented for precise tumor diagnosis and effective treatment. The absorbance of the adaptable core-shell chain structure can shift from visible to near-infrared (NIR) regions due to the fusion between nearby Au@Ag nanoparticles induced by elevated H₂O₂ levels in the tumor microenvironment (TME), resulting in the creation of a novel 3D aggregates with strong NIR absorption. With a high photothermal conversion efficiency of 60.2% at 808 nm, nanochains utilizing the TME-activated characteristics show remarkable qualities for photoacoustic imaging and significantly limit tumor growth in vivo. This study may pave the way for precise tumor diagnosis and treatment through customizable, optically tunable adaptive plasmonic nanostructures.