Synergistic changes between tumor-associated macrophages (TAMs) and cancer-associated fibroblasts (CAFs) aggravated immune evasion of hepatocellular carcinoma (HCC), however, the underlying molecular mechanisms remain elusive. Their continuous and dynamic interactions are subject to bioactive molecule changes. A real-time and in situ monitoring method suitable for in vivo research of these processes would be indispensable but is scarce. In this study, a dual imaging strategy that tracing the TAMs and CAFs simultaneously was developed using a new arginase-specific probe and established CAFs-specific probe. The emerging roles of arginase in mediating CAFs activation in mice were explored. Results showed arginase up-regulation in TAMs, followed by proline increase. Subsequently, proline produced by TAMs initiated the activation of CAFs. Through the JAK-STAT signaling, CAFs up-regulated the PD-L1 and CTLA-4, ultimately promoting immune evasion of HCC. This study revealed a new mechanism by which TAMs and CAFs collaborate in immune evasion, providing new targets for HCC immunotherapy.

Near-infrared (NIR)-II fluorescence imaging-guided photothermal therapy (PTT) has attracted great research interest, and constructing donor-acceptor (D-A) electronic configurations has become an established approach to lower bandgap and realize NIR-II emission. However, very few π-conjugated phototheranostic agents can realize efficient NIR-II guided PTT using a clinically safe laser power density, implying that sufficient photothermal performance is still desired. In addition to the continuously refreshed photothermal conversion efficiency levels, the strategies that focus on enhancing light absorptivity have been rarely discussed and endow a new direction for enhancing PTT. Herein, a dimerization π-extension strategy is raised to synthesize π-conjugated dimers with A-D-A monomers. We observe that the light absorptivity (ϵ) of the dimers is strengthened three times owing to the enhanced electronic coupling effect as a result of the π-conjugation extension, thereby surpassing the 2-fold increase in chromophore numbers from the monomer to dimers. Thanks to the enhancement in light absorption, the dimers could generate much more photothermal heat than the monomer in in vivo PTT treatments. Therefore, an efficient anti-tumor outcome has been fulfilled by using dimers under a low laser power (0.3 W/cm²). Moreover, the dimers with extended π-conjugation structures become more favorable to the radiative excited state decay, thus exhibiting a distinguishing improvement in NIR-II imaging compared with monomer. Collectively, due to the improved light absorptivity, the dimers can gain superior NIR-II fluorescence brightness and photothermal performance over the recently reported material, which goes beyond the monomer in double doses for in vivo applications. All these results prove that dimerization is an effective strategy for designing high-performance phototheranostic materials.

Urinary microalbumin (mALB) serves as an exceptionally sensitive indicator for the early detection of kidney damage, playing a pivotal role in identifying chronic renal failure and kidney lesions in individuals. Nevertheless, the current fluorescent methodologies for point-of-care (POC) diagnosis of mALB in real urine still exhibit suboptimal performance. Herein, the development and synthesis of QM-N2, an albumin-activated near-infrared (NIR) aggregation-induced emission (AIE) fluorescent probe, are presented. The strategic incorporation and positioning of quaternary ammonium salts within the quinoline-malononitrile (QM) scaffold significantly influence solubility and luminescence characteristics. Specifically, the quaternary ammonium salt-free variant, QM-OH, and the quaternary ammonium salt integrated at the donor function group (DFG) site, QM-N1, display limited solubility in aqueous solutions while demonstrating a distinct fluorescence signal. Conversely, the incorporation of quaternary ammonium salt at the conformational functional group (CFG) site in QM-N2 imparts superior dispersibility in water and reduces the initial fluorescence. Furthermore, the integration of a well-defined D-π-A structure within QM-N2 enables itself with near-infrared emission, which is crucial for mitigating interference from autofluorescence present in urine samples. Upon interaction with albumin, QM-N2 forms a tight bond with the IIA site of the subdomain of human serum albumin (HSA), inducing alterations in protein configuration and constraining the intrinsic motion of fluorescent molecules. This interaction induces fluorescence, facilitating the sensitive detection of trace albumin. Ultimately, QM-N2 is applied for POC testing of mALB using portable equipment, particularly in the diagnosis of mALB-related diseases, notably chronic renal failure. This positioning underscores its potential as an ideal candidate for self-health measurement at home or in community hospitals.

The conversion of the biomass into eco-friendly fuels and chemicals has been extensively recognized as the essential pathway to achieve the sustainable economy and carbon neutral society. Lignin, as a kind of promising biomass energy, has been certified to produce the high-valued chemicals and fuels. Numerous efforts have been made to develop various catalysts for lignin catalytic conversion. Both metalorganic frameworks (MOFs) and covalent organic frameworks (COFs) belong to very important heterogeneous porous catalysts due to their regular porous structures, high specific surface area, and precisely tailored diversities. In the review, the first part focused on the catalytic conversion of lignin, lignin model compounds, and lignin derivatives using the pristine MOFs, functional MOF composites, and MOF-derived materials. The second part summarized the catalytic conversion of lignin model compounds using pristine COFs and functional COF composites. The review here mainly concentrated on the design of the materials, screening of catalytic conditions, and explorations of the corresponded mechanisms. Specifically, (1) we summarized the MOF- and COF-based materials for the effects on the catalytic transformation of lignin-related substances; (2) we emphasized the catalytic mechanism of C–C and C–O bonds cleavage together with the structure–activity relationships; (3) we in-depth realized the relationship between the chemical/electronic/structural properties of the MOF- and COF-based catalysts and their catalytic performance for lignin-related substances. Finally, the challenges and future perspectives were also discussed on the catalytic conversion of lignin-related substances by MOF- and COF-based catalysts.

The silicon carbide (SiC) crystal growth is a multiple-phase aggregation process of Si and C atoms. With the development of the clean energy industry, the 4H-SiC has gained increasing attention as it is an ideal material for new energy automobiles and optoelectronic devices. The aggregation process is normally complex and dynamic due to its distinctive formation energy, and it is hard to study and trace back in a nondestructive and comprehensive way. Here, this work developed a non-destructive and deep learning-enhanced characterization method of 4H-SiC material, which was based on micro-CT scanning, the verification of various optical measurements, and the convolutional neural network (ResNet-50 architecture). Harmful defects at the micro-level, polytypes, micropipes, and carbon inclusions could be identified and orientated with more than 96% high performance on both accuracy and precision. The three-dimensional visual reconstruction with quantitative analyses provided a vivid tracing back of the SiC aggregation process. This work demonstrated a useful tool to understand and optimize the SiC growth technology and further enhance productivity.

Bacterial infection is a major threat to public health. Nanotechnology offers a solution by combining nanomaterials with antibacterial agents. The development of an effective nanocomposite against drug-resistant bacteria such as methicillin-resistant Staphylococcus aureus (MRSA) is highly important yet challenging. Here, an anti- MRSA core-shell structure is designed, containing antibacterial zeolitic imidazolate framework-8 (ZIF-8) as the core and bactericidal benzalkonium chloride (BAC) templated rough-surface mesostructured silica nanocomposite (RMSN) as the shell. The resultant ZIF-8@RMSN nanocomposite exhibits sustained release of BAC and zinc ions, effective disruption of the bacterial membrane, generation of oxidative damage of bacterial DNA, leakage of intracellular components, and finally bacterial death. Furthermore, the synergistic antibacterial mechanisms lead to enhanced biofilm elimination performance. In addition, the ZIF-8@RMSN-modified band-aid effectively combats MRSA infection in vivo. This work has provided a promising nanocomposite against MRSA-related infections.

Flexible wearables have attracted extensive interests for personal human motion sensing, intelligent disease diagnosis, and multifunctional electronic skins. However, the reported flexible sensors, mostly exhibited narrow detection range, low sensitivity, limited degradability to aggravate environmental pollution from vast electronic wastes, and poor antibacterial performance to hardly improve skin discomfort and skin inflammation from bacterial growth under long-term wearing. Herein, bioinspired from human skin featuring highly sensitive tactile sensation with spinous microstructures for amplifying sensing sensitivity between epidermis and dermis, a wearable antibacterial degradable electronics is prepared from degradable elastomeric substrate with MXene-coated spinous microstructures templated from lotus leaf assembled with the interdigitated electrode. The degradable elastomer is facilely obtained with tunable modulus to match the modulus of human skin with improved hydrophilicity for rapid degradation. The as-obtained sensor displays ultra-low detection limit (0.2 Pa), higher sensitivity (up to 540.2 kPa^-1), outstanding cycling stability (>23,000 cycles), a wide detection range, robust degradability, and excellent antibacterial capability. Facilitated by machine learning, the collected sensing signals from the integrated sensors on volunteer’s fingers to the related American Sign Language are effectively recognized with an accuracy up to 99%, showing excellent potential in wireless human movement sensing and smart machine learning-enabled human–machine interaction.

Fibre-based wearables for embroidery, chemosensing, and biofluid’s unidirectional draining with good flexibility, tunability, and designability drive technological advance. However, synthetic polymer fibres are non-degradable, threatening the environment and human health. Herein, we have developed versatile microfibrebased wearables by combining many advantages in one platform of biodegradable polylactic acid (PLA) and melt electrowriting strategy. Diverse potential applications of PLA wearables are achieved by flexibly designing their printing files, components and structures. Three-dimensional printing files are generated from two-dimensional images to fabricate ‘embroidery-like’ patterns. PLA/aggregation-induced emission fluorogens (AIE) chemosensors exhibit colorimetric and fluorescent colour changes upon exposure to amine vapours. Janus PLA-cotton textiles with a hydrophobic/ hydrophilic structure could facilitate unidirectional draining of sweats which is favourable for the management of temperature and humidity on the surface of skin. The proposed platform can not only broaden the design possibilities in 3D/4D printing but also offer wide potential applications for functional wearables.

Fluorescent-patterned materials are widely used in information storage and encryption. However, preparing a patterned fluorescent display on a matrix currently requires a time-consuming (hours or even days) and complex multi-step process. Herein, a rapid and mild technique developed for the in-situ controllable synthesis of fluorescent nitrogen-doped carbon dots (NCDs) on eco-friendly transparent wood films (TEMPO-oxidized carboxyl wood film [TOWF]) within a few minutes was developed. A wood skeleton was employed as the carbon precursor for NCD synthesis as well as the matrix for the uniform and controlled distribution of NCDs. Moreover, the in-situ synthesis mechanism for preparing NCDs in TOWF was proposed. The resulting fluorescent wood films have excellent tensile strength (310.00 ± 15.57 MPa), high transmittance (76.2%), high haze (95.0%), UV-blocking properties in the full ultraviolet (UV) range, and fluorescent performance that can be modified by changing the heating parameters. Fluorescent patterning was simply achieved by regulating the in-situ NCD synthesis regions, and the fluorescent patterns were formed within 10 s. These fluorescent-patterned wood films can effectively store and encrypt information, and they can interact with external information through a transparent matrix. This work provides a green and efficient strategy for fabricating fluorescent information storage and encryption materials.

Aggregation-induced emission (AIE) materials exhibit remarkable emission in the aggregated or solid state while demonstrating minimal emission in dilute solutions. In contrast to conventional luminescent materials, AIE luminogens (AIEgens) offer several advantages in the aggregate state, including high quantum yield, excellent photostability, and low background signals, making them highly promising for diverse applications. Integrating AIEgens into designable metal–organic frameworks (MOFs) enables tunable and well-ordered AIE materials, allowing for precise control over photophysical properties and deeper exploration of AIE mechanisms. Numerous AIE MOFs have been constructed and investigated, and several reviews focus on their structure design and applications in sensing and bioimaging. This review highlights the state-of-the-art advancements in AIE MOFs, including mechanisms, design strategies, and applications in chemical sensing, bioimaging, and disease therapy. The challenges associated with practical applications of AIE MOFs are also addressed, with an emphasis on their large-scale production involved interdisciplinary collaboration. This comprehensive review aims at guiding further development of AIE MOFs and promoting their practical applications in analysis, healthcare, and other luminescence related fields.

Photoluminescence (PL) mechanisms of nontraditional luminogens (NTLs) have attracted great interest, and they are generally explained with intra/intermolecular through-space conjugation (TSC) of nonconventional chromophores. Here a new concept of nonaromatic through-bond conjugation (TBC) is proposed and it is proved that it plays an important role in the PL of NTLs. The PL behaviors of the three respective isomers of cyclohexanedione and gemdimethyl-1,3- cyclohexanedione were studied and correlated with their chemical and aggregate structures. These compounds show different fluorescence emissions as well as different concentration, excitation and solvent-dependent emissions. The compounds which undergo keto-enol tautomerism and hence with a conjugated ketone-enol structure (i.e., nonaromatic TBC) show more red-shifted emissions. TBC effect reduces the energy gaps and facilitates the formation of stronger TSC in the aggregate state. The compounds in the ketone-enol form are also prone to occur excited state intra/intermolecular proton transfer (ESIPT). The cooperative effect of nonaromatic TBC and TSC determines the PL behaviors of NTLs. This work provides a novel understanding of the PL mechanisms of NTLs and is of great importance for directing the design and synthesis of novel NTLs.

Lipid droplets (LDs), which are the hubs of lipid metabolism, play a critical role in maintaining cellular energy homeostasis. The construction of advanced photosensitizers (PSs) capable of manipulating LD-mediated cell fate regulation is highly desirable though rarely reported. In this study, a near-infrared emissive PS (DPCMP) with LDs specificity was synthesized and successfully applied to induce ferroptosis and apoptosis. DPCMP exhibited typical aggregation-induced emission characteristics owing to its twisted molecular conformation. Excellent biocompatibility and suitable lipophilicity allowed DPCMP to specifically stain the LDs in living cells. Under white light illumination, the DPCMP displayed potent reactive oxygen species (ROS) generation capacity through both type I and II photochemistry. The massive accumulation of lethal ROS generated by DPCMP-mediated photosensitization initiated lipid peroxidation, impaired cellular redox homeostasis, and led to endoplasmic reticulum oxidative stress, ultimately inhibiting cellular proliferation via concurrent ferroptosis and apoptosis in both living cancer cells and multicellular tumor spheroids.

Phototherapeutic nanoplatforms that combine photodynamic therapy (PDT) and photothermal therapy (PTT) with the guidance of photoacoustic (PA) imaging are an effective strategy for the treatment of tumors, but establishing a universal method for this strategy has been challenging. In this study, we present a supramolecular assembly strategy based on Förster resonance energy transfer to construct a supramolecular nanostructured phototherapeutic agent (PcDA) via the anion and cation supramolecular interaction between two water-soluble phthalocyanine ramifications, PcD and PcA. This approach promotes the absorption of energy, thus enhancing the generation of reactive oxygen species (ROS) and heat by PcDA, improving its therapeutic efficacy, and overcoming the low photon utilization efficiency of conventional PSs. Notably, after the intravenous injection of PcDA, neoplastic sites could be clearly visualized using PA imaging, with a PA signal-to-liver ratio as high as 11.9. Due to these unique features, PcDA exhibits excellent antitumor efficacy in a preclinical model at a low dose of light irradiation. This study thus offers a general approach for the development of efficient phototherapeutic agents based on the simultaneous effect of PDT and PTT against tumors with the assistance of PA imaging.

The management of infected wounds is always of great significance and urgency in clinical and biomedical fields. Recent efforts in this area are focusing on the development of functional wound patches with effective antibacterial, drug delivery, and sensor properties. Here, we present novel hyaluronic acid (HA) microneedle patches with these features by encapsulating aminobenzeneboronic acid-modified gold nanoclusters (A-GNCs) for infected wound management. The A-GNCs loaded microneedle patches were derived from negative-mold replication and showed high mechanical strength to penetrate the skin. The release of the A-GNCs was realized by the degradation of HA, and the self-monitor of the released actives was based on the dynamic bright orange fluorescence emitted from A-GNCs under ultraviolet radiation. As the A-GNCs could destroy bacteria membranes, the microneedle patches were with excellent in vitro antibiosis ability. Based on these features, we have demonstrated the bacteria inhibition, residual drug self-monitoring, and wound healing promotion abilities of the microneedle patches in Escherichia coli-or Staphylococcus aureus-infected wound management. These results indicated the great potential of such A-GNCs loaded microneedle patches for clinical applications.