The Royal Society of Chemistry最新文献

Pathological macrophage activation orchestrates atherosclerotic plaque progression through sustained inflammation, necrotic core expansion, and plaque destabilization, a process recalcitrant to current targeted therapies. We address this fundamental challenge by engineering a living macrophage-based theranostic cyborg (MφMB-Au) that integrates precision plaque homing with spatiotemporally controlled immunomodulation. This platform exploits the innate inflammatory tropism of functionalized macrophages to co-deliver gold nano-regulator (AuNPs) and real-time tracer microbubbles (MBs). The AuNPs function dually as high-sensitivity photoacoustic imaging agents, enabling deep-tissue quantification of plaque burden, and potent metabolic switches reprogramming macrophage polarization via lipid and energy metabolism pathways. Concurrently, MBs facilitate real-time ultrasonographic tracking with micron-scale spatial resolution. In vivo studies demonstrate sustained plaque-specific accumulation of MφMB-Au, permitting longitudinal dual-modal ultrasound/photoacoustic imaging for over 24 hours. Ultrasound-triggered payload release induced a 5.3-fold increment of M2-repolarization, driving significant plaque regression. Critically, this approach restored efferocytosis capacity and collagen deposition while evading off-target toxicity. As the first cellular cyborg platform unifying longitudinal multimodal imaging, stimuli-responsive cargo deployment, and metabolic reprogramming, this work establishes a paradigm-shifting theranostic strategy to reverse the core pathophysiology of atherosclerosis.

Conventional hydrogels often fail to simultaneously balance the mechanical resilience, tissue adhesion, and electrical conductivity-key requirements for reliable soft bioelectronic interfaces in monitoring scenarios. In this study, we introduce a conductive nanofibrillar double-network hydrogel adhesive that enables real-time, long-term monitoring of human motion and physiological signals, including electrocardiography (ECG), electromyography (EMG), and lung respiration. The double-network matrix, coupled with silver nanoparticle-doped protein nanofibrils, facilitates tunable mechanical properties, tissue-adhesive characteristics, and electrical conductivity of the structural material. The ultra-sensitive strain responsiveness enables precise and reliable detection of various body movements, from finger bending to subtle vocal cord vibration, as well as real-time monitoring of cardiac activity, muscle contractions, and respiratory patterns. Demonstrations in large animal models illustrate its capabilities in sealing lung injury and long-term monitoring lung activity, enabling early detection of abnormalities and facilitating potential personalized healthcare interventions in clinical settings.

The radical anion of amide-functionalized perylene diimide (TFPDIOH˙^-) aggregates into a pimer that is stabilized through pancake bonding. In the presence of primary amines, this pimer can undergo disaggregation, offering potential for responsive organic sensors. In this study, density functional theory calculations were employed to elucidate the sensing mechanism, which can be represented as follows: 1/2[TFPDIOH]₂^2- + nBuNH₂ → [nBuNH₂·TFPDIOH]˙^-. Computational results reveal that steric hindrance from the bulky substituents on the amide positions weakens π-stacking interactions, thereby allowing strong hydrogen bonding to induce pimer disaggregation. The phenolic hydroxyl group on the substituent forms a low-barrier hydrogen bond (LBHB) with nBuNH₂, which is characterized by a short N⋯O distance, high ρ_BCP, 3c-4e bonding pattern, and nearly barrierless proton transfer. The electron-withdrawing fluorine atoms on the substituent enhance hydroxyl acidity, further stabilizing LBHB formation. These findings reveal the LBHB-driven disaggregation mechanism and demonstrate that the rational combination of pancake bonding and LBHB interactions offers a novel strategy for developing π-radical-based organic sensors with enhanced sensitivity.

Typical and atypical declines in cognitive function, as well as increases in chronic, low-grade inflammation and impaired vascular function are all impacted by the ageing process. Flavonoid-rich foods/beverages have been extensively shown to impact human cognition and to modulate immune and/or vascular function, although the cause-and-effect relationship between these factors is unclear. Here, we examine the acute (2 hours) and short-term (8 days) effects of anthocyanin-rich black rice on cognition, inflammation, and vascular function in older adults. Twenty-four older adults (65 ± 7 years) participated in a randomized, single-blind, crossover trial with one-week washout periods. Participants consumed either 210 g of anthocyanin-rich black rice (208 mg of anthocyanins) or the brown rice control (0 mg of anthocyanins) daily for 9 days. Acute effects were assessed 2 hours after consumption on days 1 and 9, and short-term effects were evaluated after completing 8 days of intake. Cognitive performance (RAVLT, digit span, Stroop, and digit symbol substitution), microvascular blood flow, and blood pressure were measured for both acute and short-term interventions, while serum inflammatory biomarkers were assessed for the short-term intervention. Anthocyanins and phenolic acids in rice were identified by using liquid chromatography-mass spectrometry (LC-MS). Data were analyzed using linear mixed models with Bonferroni-corrected comparisons. Eight days of black rice intake significantly improved verbal memory (RAVLT final recall: 12.64 vs. 11.92, p = 0.04; total recall: 52.57 vs. 49.54, p = 0.02) and enhanced digit span backward (change from baseline (CFB) = 0.83, p = 0.03) compared with brown rice. In parallel, black rice significantly reduced interleukin-6 (IL-6) levels (CFB: -0.67, p = 0.03), an effect not seen with the control. Acute black rice consumption attenuated declines in delayed recall (CFB: -1.17, p = 0.09) and recognition (CFB: -0.67, p = 0.19), while significant reductions were observed following brown rice intake. No significant treatment effects were observed for microvascular blood flow or blood pressure. Consumption of anthocyanin-rich black rice for 8 days improved verbal memory and reduced blood IL-6 in older adults. These data suggest for the first time that cognitive benefits induced by anthocyanin-rich black rice may be mediated by anti-inflammatory mechanisms. The clinical trial registry number is NCT06583785 (https://clinicaltrials.gov).

Cold-pressed almond oil is considered a premium product due to its solvent-free extraction and sensory quality. Its industrial production produces large volumes of a nutrient-rich by-product, namely almond press cake (APC). In this study, this by-product was submitted to supercritical fluid extraction (SFE) with CO2 using two different pressure conditions for extracting residual oil in APC, further generating two residues (APC20 and APC24, from extraction at 20 and 24 MPa, respectively). Except for fat, which, as expected, was reduced in APC20 and APC24, and available carbohydrates, which were higher in the SFE-derived samples, the three residues showed similar contents of the remaining macronutrients (p > 0.05). The residues were particularly rich in total dietary fiber (from 73.7 to 76.2 g per 100 g), presenting also relevant quantities of protein (from 9.3 to 9.5 g per 100 g). APC20 and APC24 showed a strong retention of phenolic compounds, with only about a 10% decrease of total phenols compared to APC. In vitro digestion using the INFOGEST protocol revealed that some phenolic compounds exhibited high bioaccessibility values, with taxifolin, amygdalin, caffeic acid, vanillic acid, protocatechuic acid, and quercetin-3-O-glucoside exceeding 100% bioaccessibility. Moreover, the antioxidant potential of bioaccessible fractions after simulated digestion was superior to that exhibited by non-digested samples. Furthermore, the prebiotic potential of digested residues was evident through the promotion of Lactobacillus and Bifidobacterium growth, comparable to inulin. Altogether, these results highlight the value of almond oilcake and its extraction residues as promising and sustainable functional food ingredients.

Ageing is associated with attenuated type-2 bitter-taste receptor (TAS2R) signalling and contributes to metabolic, inflammatory and barrier decline, but its system-wide impact along the gut remains undefined. We combined transcription analysis, physiology, metabolomics and microbiota profiling to test whether a brief grape-seed proanthocyanidin extract (GSPE) intervention can counter age-related dysfunction by long-term modulation of intestinal Tas2r expression. Female Wistar rats were distributed into young (2 months, n = 10) or aged (21 months, n = 24) groups; eleven aged animals received GSPE (500 mg kg^-1, oral gavage) for 10 days, followed by a 75-day wash-out. After sacrifice, we quantified Tas2r mRNA in five gut segments, assessed ex vivo permeability, enteroendocrine outputs, systemic metabolites, inflammatory markers, 16S microbiota and the untargeted plasma metabolome. An elastic-net/PLS-DA/random-forest pipeline ranked variables discriminating age and GSPE effects, and GeneNet partial correlations generated an integrated network. Ageing suppressed Tas2r gene expression across the small intestine and the distal colon, while the proximal colon was largely unchanged. Despite the long wash-out, the brief GSPE treatment restored small-intestinal Tas2r transcription of some receptors while paradoxically down-regulating a subset in the distal colon. Consensus variable selection highlighted enterohormone expression and its ex vivo secretion, intestinal barrier dysfunction indices, some microbiota genera and several Tas2r transcripts among the 34 strongest discriminators. Tas2rs formed high-betweenness hubs linking epithelial integrity, inflammatory tone and butyrate-producing taxa. These findings indicate that intestinal type-2 bitter taste receptors (Tas2rs) may integrate multisystem regulatory networks fundamental to healthy ageing. Brief administration of grape-seed proanthocyanidin extract (GSPE) is sufficient to durably reprogramme Tas2r expression and the surrounding microbiota-endocrine-barrier landscape in aged rats.

Chlorogenic acid (CGA) is a polyphenol widely found in plants with a wide range of biological activities, especially anti-inflammatory effects. The mechanism by which CGA improves colitis by regulating the gut microbiota has not been fully investigated. This study aimed to explore the anti-inflammatory properties of CGA on dextran sodium sulfate (DSS) treated mice. CGA supplementation attenuated the severity of colitis by reducing the disease activity index (DAI), repairing colonic histological damage and suppressing the abnormal inflammatory response. Sequencing analysis indicated that intake of CGA alleviated DSS-induced gut microbiota dysbiosis, including reducing the F/B value and stimulating the growth of potentially beneficial bacteria, such as Akkermansia muciniphila, Odoribacter and Muribaculaceae. CGA (100 mg per kg body weight) supplementation also reversed the generation of short-chain fatty acids (SCFAs), especially propionic acid, butyric acid, isobutyric acid and 4-methylvaleric acid. Consequently, these findings demonstrated that supplementation of CGA attenuated the severity of intestinal inflammation by ameliorating gut microbiota dysbiosis and promoting the growth of butyrate-producing gut microbiota.

The pyrolysis of lignocellulosic biomass yields biochar consisting of high-carbon scaffolds bearing a variety of functional groups. As produced, the biochar is mechanically fragile and lacks the structural cohesion needed for making structural materials. To enhance both its chemical stability and mechanical strength, elemental sulfur is here introduced to induce a vulcanization reaction with biochar. Heating a biochar-sulfur (BS) mixture up to 185 °C under pressure induces effective crosslinking within the carbon network of biochar, a reaction attributed to free-radical sulfur polymerization and addition to functional groups attached to the carbon network of biochar. The synthesis method yields a crosslinked biochar with markedly enhanced mechanical strength. Depending on the synthesis conditions, the compressive strength and Young's modulus can reach values between 22-382.5 MPa and 6-165 GPa, respectively. With the density of only 1.4 g cm^-3, the mechanical properties of the best synthesized materials closely match that of structural steel. The BS materials can potentially be used as sustainable materials in parts and products for human infrastructure and transport. Alternatively, this method may also provide an alternative pathway for biomass-derived carbon storage contributing to climate change mitigation.

Cysteine fluorescent probes are specialized molecular tools that facilitate highly sensitive detection of cysteine via alterations in fluorescent signals. Currently, these probes have been widely employed in fields including disease biomarker monitoring, redox balance research, and drug toxicity assessment, thereby exhibiting substantial application potential in biochemical and biomedical studies. In this study, a novel fluorescent probe was designed for detecting cysteine based on the thiopyrone structure. Through characterization of its properties, it was found that this fluorescent probe exhibits a large Stokes shift (217 nm), excellent sensitivity (13.60 nM), rapid response time (3.0 min), high stability and selectivity. Furthermore, this cysteine fluorescent probe demonstrates excellent applications in RAW 264.7 cells, zebrafish, and actual samples. This study also proposes a more convenient method for testing cysteine levels using mobile phone software, and the findings indicate that the fluorescent probe under investigation has considerable potential for use in cysteine detection.