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Hospital redevelopment projects are among the largest and most costly changes undertaken in health systems. Despite abundant methodologies and frameworks that offer theoretical guidance, the literature reports persistent gaps in managing change of this scale effectively. To examine this gap between theory and implementation of change management in practice, we explored change managers' experiences of leading change in hospital redevelopment projects across one Australian state, using a qualitative approach. We aimed to understand the change management approaches used, the perceived value and limitations of those approaches, the capabilities change managers need to lead change, and the barriers and enablers encountered through the change cycle. Semi-structured interviews were conducted with 28 change managers of varying levels of experience and project scope in hospital redevelopments. Data were analysed using the Framework method. Subthemes were developed inductively from the interviews and then mapped deductively onto the three stages (planning, implementing, and sustaining change) of a statewide health infrastructure change management framework that guided practice in this setting. Inductive subthemes not able to be classified using the framework formed a fourth theme on change managers' capabilities. Four themes were developed: 1) Planning for change, 2) Implementing change, 3) Sustaining and reinforcing change, and 4) Change managers' capabilities and support. Participants described several effective approaches to managing change in hospital redevelopment, including progress tracking, prototypes, site visits, and ongoing stakeholder consultations, with local staff central to facilitating engagement. Executive sponsorship was repeatedly identified as an enabler of change, although securing it early and sustaining it across the project proved a recurring challenge. Further challenges included aligning change plans with broader project processes, transitioning change into business as usual once the project ended, and evaluating whether the change delivered its intended benefits. Some participants reported not being aware of available resources and how to utilise them. Change management frameworks offered useful guidance particularly for less experienced change managers. However, participants often described challenges utilising these frameworks for effective stakeholder engagement, for sustaining change in long-term projects, or where change management and project processes were misaligned. The findings have practical implications for successful change management in redevelopment projects, including the importance of structured training and mentoring for change managers, a need for early and sustained executive and stakeholder engagement, planned transition to business as usual, and closer alignment of change management with project delivery so that the people side of change is supported throughout the project lifecycle.
Inflammatory Bowel Diseases (IBD) are challenging conditions to manage due to the heterogeneity of the disease, diverse treatment options, and nuances of care over a range of ages. Clinical care pathways (CCPs) developed by experts enable health care providers (HCPs) to deliver standardized, high-quality, evidence-based care. In order to remain useful and valuable, these pathways need to evolve alongside changing treatment recommendations. Standardizing IBD care is a priority of Crohn's Colitis Canada's Promoting Access and Care through Centres of Excellence (PACE) network. To describe the process of nationalizing IBD CCP's, including development, standardization, maintenance, and dissemination. This project was based on a previously developed structured framework for review and maintenance. The CCP team consisted of a leadership group, advisory council and a working group with diverse representation from the country and areas of expertise. The work was tracked with a database with coordination completed by staff of the national organization. The nationalization process lasted 14 months, with input from 23 HCPs from 14 academic and community institutions across Canada. Sixteen CCPs for IBD care were developed and approved by the CCP team. Challenges encountered included outdated guidelines, differing clinical opinions, and busy clinical schedules of the team members. Translation into French is complete. Support of Crohn's and Colitis Canada was invaluable. Despite anticipated challenges, 16 CCPs received approval from the advisory council and are publicly available to HCPs across Canada. Our approach to this undertaking and the lessons learned may be valuable for experts undertaking similar projects for patients with chronic diseases.
The current landscape of emergency care (EC) is marked by high demand, leading to issues such as emergency department boarding, overcrowding, and subsequent delays that impact the quality and safety of patient care. Integrating data science into EC can enhance decision-making with predictive, preventative, personalized, and participatory approaches. However, gaps in adherence to fairness, accountability, interpretability, and responsibility are evident, particularly due to barriers to data-sharing, which often result in a lack of transparency and robust oversight in these applications. The FAIR-EC (Fair, Accountable, Interpretable, and Responsible-Emergency Care) collaboration adapts the existing Fair, Accountable, Interpretable, and Responsible principles to address emerging challenges as data science integrates with EC. This initiative aims to transform EC by establishing ethical artificial intelligence standards specifically tailored for this integration. By bridging the gap between EC professionals, data scientists, and other stakeholders, the collaboration promotes international cooperation that leverages advanced data science techniques to enhance EC outcomes across different care settings. We propose a federated research design to analyze extensive datasets from various global institutions without compromising patient privacy. This approach transforms epidemiological research with advanced data science techniques, emphasizing the harmonization of data for comprehensive analyses across different health care systems. The FAIR-EC initiative has facilitated the identification and harmonization of datasets from diverse geographical regions, enabling the examination of regional variations in EC practices. As of paper submission, participating sites have identified retrospective EC datasets totaling >2 million records (eg, Duke Health >400,000 and Singapore General Hospital >1.7 million records). Initial projects have demonstrated feasibility and operational readiness, including implementation of federated workflows and ongoing development of a federated scoring system, cross-site evaluation, and adaptation of association studies and predictive models across various regions. Cross-site harmonization and pilot analyses are underway (with local ethics approvals in progress), and first multisite results are expected to be submitted in mid-late 2026, with additional project-level publications anticipated in 2027. These efforts highlight the feasibility of leveraging advanced data science techniques to address the complexities of EC while preserving patient privacy without centralizing individual-level data. This project was funded from September 1, 2022, to August 31, 2023. FAIR-EC integrates data science ethically and effectively into EC, addressing challenges such as fragmented data, real-time handoffs, and public health crises. Its federated design harmonizes diverse data streams while preserving privacy, and its emphasis on ethical artificial intelligence aligns with the dynamic nature of EC. Despite challenges in data variability and system complexity, FAIR-EC establishes a strong foundation for innovation in global EC.
Orthopaedic surgeons routinely consult search engines, journals, and curated websites to stay current on orthopaedic knowledge. The emergence of large language models, such as OpenAI ChatGPT and Google MedGemma, is changing the way we search for information and how residents learn. Although many orthopaedic surgeons are users of artificial intelligence (AI), most are uncertain about how these tools actually work and why they sometimes give impressively accurate explanations alongside glaring factual errors and fabricated citations. This review provides an overview of the underlying preclinical studies behind large language models at the level of detail needed to empower orthopaedic surgeons with the knowledge needed to critically evaluate AI outputs, design future research projects, and effectively incorporate AI tools into clinical practice and resident education. Through clinical examples including a Schatzker VI tibial plateau fracture and an L4 pedicle screw sizing question, we illustrate two distinct classes of AI failure-retrieval failures and reasoning failures-and demonstrate how understanding the preclinical studies behind these errors equips surgeons to evaluate any AI tool regardless of where or how it runs.
The increasing demand for cost-effective, high-performance, and broadband photodetectors motivates the development of novel material systems and device architectures. In this study, compositionally tunable p-(CuS)x(ZnSe)1-x/p-Si isotype heterojunction photodetectors were fabricated via thermal evaporation. The CuS/ZnSe ratio was systematically varied to investigate its impact on the morphological, optical, and electrical properties of the heterojunction. At the optimized x = 0.5 composition, densely and homogeneously distributed nanopillars enhanced light trapping and photon harvesting. Consequently, the device achieved a responsivity of 1.1 A/W, a detectivity of 1.16 × 1011 Jones, and an external quantum efficiency (EQE) of 161% at 850 nm under zero bias. The remarkably high EQE originates from the combined effect of enhanced light harvesting and a trap-assisted internal photoconductive gain mechanism. The valence-band offset at the heterojunction interface acts as a hole-blocking barrier, while copper vacancies identified by XPS serve as hole-trapping centers that prolong carrier lifetime and trigger electron recirculation. This mechanism was further supported by the asymmetric transient response with rise and fall times of 21 and 54 µs, respectively. Ultimately, this convergence of maximized photon absorption and prolonged carrier lifetimes provides a viable strategy for designing high-gain and chalcogenide-based photodetectors for high sensing of light with very low intensity.
Home-based rehabilitation after arthroscopic rotator cuff repair (ARCR) often lacks objective monitoring. To address this limitation, we developed the ANAPA digital rehabilitation (DR) system, which includes a patient-facing mobile application for clinical efficacy evaluation (ANAPA ME) and a physician-facing measurement application for technical assessment (ANAPA PS). This study compared the safety and preliminary efficacy of ANAPA ME with conventional YouTube-based rehabilitation (CR), with an additional validation of the automated measurement functions in ANAPA PS. This single-center, assessor-blinded, randomized pilot study included 18 patients who had undergone ARCR. The participants were allocated to the DR group (n = 9) or CR group (n = 9) and followed identical postoperative rotator cuff exercise protocols. The program was conducted for 24 weeks postoperatively. The shoulder range of motion (ROM), muscle strength, and clinical outcomes (visual analog scale pain score, Constant shoulder score, Shoulder Pain and Disability Index, and EuroQol-5 Dimension-5 Level questionnaire) were evaluated at baseline and at follow-up up to 24 weeks postoperatively. Ultrasonography was performed at 24 weeks to evaluate the integrity of the repaired tendons. Automated ROM and muscle strength measurements of ANAPA PS were validated against digital goniometry and hand-held dynamometry at the 6-month follow-up, and measurement consistency was assessed using intraclass correlation coefficients (ICCs) and coefficients of variation (CV). Both the DR and CR groups demonstrated significant within-group improvements in ROM and clinical scores (p < 0.05). The DR group showed significantly greater improvements in specific ROM parameters, including forward flexion at 24 weeks and abduction, abduction-external rotation, and internal rotation at 18 and 24 weeks, compared with the CR group (p < 0.05). At 18 weeks, the internal rotation muscle strength was also significantly higher in the DR group than in the CR group (p < 0.05). A significant time-by-group interaction was observed for abduction, side-external rotation, and internal rotation (p < 0.05), suggesting a more consistent improvement pattern over time in the DR group compared with the CR group. In supplementary validation, ANAPA PS measurements showed high agreement with reference instruments (mean absolute error of 3.14° for ROM and 0.15-0.22 kgf for muscle strength). In consistency analysis, ANAPA PS showed higher repeatability and lower variability than digital goniometry (ICC = 0.99 vs. 0.97; CV = 1.61% vs. 11.7%, p < 0.001) and hand-held dynamometry (ICC = 0.97 vs. 0.39; CV = 2.1% vs. 13.8%, p < 0.001). In this exploratory pilot study, the ANAPA DR system demonstrated favorable trends compared with CR in patients after ARCR, suggesting the feasibility and safety of artificial intelligence-based digital therapeutics in postoperative shoulder rehabilitation. The supplementary validation further demonstrated the technical reliability and measurement consistency of the ANAPA PS automated measurement functions for monitoring rehabilitation outcomes.
Minimizing platinum-group metal (PGM) usage in anion-exchange membrane fuel cells (AEMFCs) and proton-exchange membrane fuel cells (PEMFCs) is essential for cost reduction. However, achieving power densities exceeding 1 W cm-2 requires high PGM loadings at the anode, particularly in AEMFCs (>0.1 mg cm-2), to sustain hydrogen oxidation reaction (HOR) kinetics. Nickel-based catalysts offer a low-cost alternative but are typically limited by poor activity and oxidative instability. Here, we address these limitations by developing a core-shell nanoreactor comprising Ni nanoparticles (NPs) encapsulated by N-doped graphitic carbon (NC) that is embedded with atomic Ru and Ni species. With an ultralow Ru loading of 1 µg cm-2, anodes using this catalyst deliver peak power densities of 2.36 and 3.26 W cm-2 in AEMFC and PEMFC, respectively, with negligible structure change after 200 h of continuous operation at 1 A cm-2 in both devices. Mechanistic studies in alkaline media reveal a tandem catalytic pathway in which NPs shielded from the electrolyte dissociate H2 to H*, and adjacent atomic metal species enable H* spillover across the NC shell to react with surface-anchored OH*. This work provides a general strategy for designing tandem electrocatalysts for multi-step catalytic processes.
Stereotactic arrhythmia radioablation (STAR) has been proposed to treat refractory ventricular tachycardia (VT) in patients with structural heart disease (SHD). The aim of the STAR-VT-2020 (Stereotactic Ablative Radiosurgery of Recurrent Ventricular Tachycardia in Structural Heart Disease) randomized trial was to compare the efficacy of STAR and catheter ablation (CA) after a failure of previous CA. Patients with VT recurrences were randomized at 2 centers (June 2020 to January 2024) to the STAR or CA group in a 1:1 fashion using a covariate-adaptive algorithm. In the STAR group, the arrhythmogenic substrate was irradiated by a single dose of 25 Gy delivered by a robotic system (CyberKnife). The planning target volume was delineated by coregistering the electroanatomical substrate map (CARTO 3) with the planning computed tomographic scan. In the CA group, CA was performed using substrate modification strategies. The primary endpoint was VT recurrence, while repeated CA was one of the secondary endpoints. A total of 22 patients (68% men, mean age 67 ± 11 years, 27% with ischemic cardiomyopathy, mean left ventricular ejection fraction 31% ± 9%, 3.0 ± 1.3 previous CAs) were enrolled (11 in each group) and followed for 28 ± 17 months. The STAR patients exhibited a nonsignificantly higher risk for VT recurrence (HR: 2.5; 95% CI: 0.97-6.6) than those who underwent CA, and a significantly higher risk of repeated CA for VT (HR: 4.0; 95% CI: 1.2-13.8). Throughout the trial, 13 patients died, 3 underwent heart transplantation, and 3 received left ventricular assist devices, with no significant differences between the 2 groups. The STAR-VT-2020 trial suggests a potential clinical benefit of repeated CA over STAR in patients with SHD, despite prior failed CA at specialized centers. Because of the small study cohort of highly selected patients and several methodological limitations, the results of the prematurely terminated trial should be considered exploratory and interpreted strictly as hypothesis generating. Larger trials with optimized design are warranted. (Stereotactic Ablative Radiosurgery of Recurrent Ventricular Tachycardia in Structural Heart Disease; NCT04612140).
Formamidinium (FA) based perovskites have evolved as a promising candidate for high performance optoelectronic devices due to their near-ideal band structure. However, demonstration of high performance field effect transistors with FA based perovskites remains largely unexplored due to the inherent phase instability of the photoactive FA phase and field induced ionic defect migration. Here, we developed an α-phase-assisted anti-solvent method which utilizes facet-rich CsPbBr3 nanocrystals (NCs) to demonstrate hysteresis-free field effect transistors with n-type transport at least 30 times higher than pristine FAPbI3 reaching values > 1 cm2/Vs. These devices demonstrate exceptional operational bias stress stability with a marginal threshold voltage shift (∆Vth) ∼ 0.7 V for 10 h of continuous operation which self-heals, > 1500 h of ambient stability and > 8500 h of performance retention under nitrogen atmosphere making them one of the champion n-type perovskite compositions till date in terms of stable devices for practical applications. Interestingly, these composite perovskites do not exhibit significant ion migration indicated by an activated temperature dependence in the mobility which is generally not observed in 3D Pb-based perovskite compositions. By integrating electronic/ionic transport studies along with terahertz time-domain spectroscopy, single-particle blinking measurements, and structure-property correlations, we establish the microscopic mechanism through which facet polarity stabilizes the thermodynamically elusive α-phase of FAPbI3 without affecting the band-structure, ultimately yielding desirable long-term operational stability of the field effect devices. Our findings establish facet engineering of NCs as a transformative route toward developing reliable and stable perovskite based optoelectronic devices.
With the rapid development of flexible electronics and human-computer interaction technologies, the demand for high-performance flexible strain sensors for human motion and physiological signal monitoring has grown sharply. This study developed a sandwich-structured flexible strain sensor based on multi-walled carbon nanotube/halloysite nanotube (MWCNT/HNT) nanocomposites. A polydopamine (PDA) modification layer was first formed on the polydimethylsiloxane (PDMS) film via in situ polymerization of dopamine (DA), which significantly improved the surface hydrophilicity and enhanced interfacial adhesion between PDMS and the subsequent conductive layer. The MWCNT/HNT mixed conductive layer was then uniformly sprayed onto the PDA@PDMS film, followed by PDMS encapsulation to form the final structure. The sensor integrates the excellent conductivity of MWCNTs and the mechanical reinforcement capability of HNTs, achieving a wide strain-sensing range, high sensitivity with GF values of 14.46 at 0-40% strain and 35.55 at 40-85% strain, fast response/recovery times of 250/300 ms, and excellent cyclic stability over 7500 cycles. It can sensitively detect physiological signals such as swallowing, pulse and breathing, as well as motion signals including joint bending and mouse clicking. Moreover, it can distinguish subtle finger movements during English letter writing, showing broad application potential in wearable healthcare devices and human-computer interaction systems.
Obtaining host DNA from the blood meals of their invertebrate parasites (invertebrate-derived DNA, iDNA) has proven to be a powerful tool in terrestrial ecology for detecting vertebrates to answer questions relating to host community diversity. However, the use of iDNA in the marine environment is limited. Here, we assessed the efficacy of sampling parasites from the critically endangered flapper skate (Dipturus intermedius) to determine whether iDNA could (i) identify the host species and (ii) obtain host haplotype sequences. In total, 34 copepods (Trebius caudatus specimens, n = 30; Caligus elongatus specimens, n = 4) were processed from 20 flapper skates. Fin-clips were also taken from each flapper for comparison. iDNA identified the host species with 91% success. The host haplotype sequenced from multiple T. caudatus specimens sampled from the same host matched in all cases. A bias-reduced logistic regression found a positive but non-significant association between copepod gut length (z-score) and host-copepod haplotype match success (β = 0.67, p = 0.34). These findings demonstrate the utility of iDNA for confirming the identity and the haplotype of a cryptic conservation-listed batoid and its potential to transform community-led genetic sampling.
The steady increase in laboratory testing volume burdens the health care system with substantial costs, contributes to patient dissatisfaction, and generates adverse environmental effects. Beyond financial expenditure, unnecessary testing poses medical risks and affects patient well-being. Our quality improvement (QI) project aimed to employ a multimodal intervention to enhance appropriate laboratory utilization amongst residents and hospitalists. This QI initiative used a multimodal intervention to enhance appropriate lab utilization among residents and hospitalists. It involved evaluating baseline knowledge gaps, implementing targeted education, and integrating daily structured discussions on lab necessity. In addition, an electronic dashboard was utilized with real-time data on lab ordering volume and labs ordered per attending. The intervention led to a net decrease of 4657 lab orders over the 3-month period. Specifically, there were significant reductions in comprehensive metabolic panel (CMP) (19.5%), serum Mg (11.8%), serum Phos (14.1%), and complete blood count (CBC) (11.2%) orders, alongside a 20% increase in basic metabolic panel (BMP) orders. Patient satisfaction improved, with affirmative "rest and recover" responses rising from 51.8% to 63.2%. This reduction generated an estimated $10,645 in cost savings and a 1304.61 kg reduction in CO2 emissions. This multifaceted QI approach, integrating systemic interventions and education, effectively reduced unnecessary lab testing. It simultaneously improved patient experience, yielded cost savings, and mitigated environmental impact, offering a transferable framework.
Cardiovascular-kidney-metabolic (CKM) syndrome poses a major health risk. This study assessed the impact of a healthy lifestyle on all-cause and cardiovascular disease (CVD) mortality in CKM individuals. We analyzed 306 831 and 9823 CKM individuals from UK Biobank and NHANES (2007-2018). A healthy lifestyle score was created based on seven factors: no current smoking, moderate drinking, healthy diet, regular physical activity, adequate sleep, low sedentary behavior and appropriate social connection. Primary outcomes were all-cause and CVD mortality from linked health records and death registries. Cox regression models showed that higher lifestyle scores were associated with reduced risks of all-cause (hazard ratio [HR]: 0.81, 95% confidence interval [CI]: 0.80-0.82) and CVD mortality (HR: 0.82, 95% CI: 0.80-0.84) in UK Biobank. In NHANES, higher scores were associated with 15% (95% CI: 0.80-0.90) and 11% (95% CI: 0.81-0.99) lower mortality risks. Both regular physical activity (HRs: 0.85 and 0.89 for UK Biobank, 0.76 and 0.73 for NHANES) and low sedentary behavior (HRs: 0.85 and 0.91 for UK Biobank, 0.79 and 0.67 for NHANES) were related to reduced mortality risks (p < 0.05). Participants with non-advanced CKM syndrome and a favorable lifestyle had the lowest mortality risks compared to those with advanced CKM syndrome and an unfavorable lifestyle. A healthy lifestyle, particularly regular physical activity and low sedentary behavior, was significantly associated with lower all-cause and CVD mortality in individuals with CKM syndrome. These associations were stronger in the early stages, highlighting the importance of timely and targeted lifestyle interventions.
Wide-bandgap transparency and large optical anisotropy are mutually exclusive in most solar-blind birefringent crystals, severely limiting the miniaturization of solar-blind polarization optics. Here, we show that this long-standing trade-off can be broken by a complementary hydrogen-bond co-assembly strategy, in which interstitial water molecules act as directional locks to compress the dihedral angles between urea building blocks and align their dipole moments. This yields two crystals, C2H5N3O2 and its hydrated derivative C2H5N3O2·0.75 H2O, which deliver birefringence values of 0.224 and 0.283 at 546 nm while maintaining absorption edges of 210 and 202 nm in the solar-blind ultraviolet region, respectively. The hydrated phase achieves a 2.5-fold birefringence enhancement over pristine urea, overcoming the inherent anisotropy bottleneck of the classical hydrogen-bonded network. Our findings establish a rational paradigm, from excellent structural units to the ordered arrangement of complementary weak bonds, and then to outstanding optical anisotropy, showing that weak interactions can actively regulate polar units to drive birefringence close to its theoretical limit, offering a widely applicable design platform for the next generation of solar-blind photonic materials.
Developing efficient, stable, low-cost bifunctional ORR/OER electrocatalysts remains challenging. Methods such as morphological design, element doping and interface engineering are common and effective strategies to effectively improve oxygen electrocatalytic activity. On this basis, we designed and prepared the transition metal selenide heterojunction supported conductive hierarchical porous carbon nanofibers electrocatalyst (CoCuSe/Cu2-xSe@PCNFs). The obtained Cu2-xSe exhibits well electronic conductivity, and bimetallic selenides also can enhance the dispersion and stability of active sites, thus greatly improving ORR and OER activities. The theoretical calculations also indicate that a novel interface can be formed between the two components in the heterojunction, and an internal electric field also is generated at the interfaces. The result can effectively adjust the electron distribution of the active material, optimize the adsorption and desorption of reaction intermediates and subsequently enhance the catalytic performance. Benefiting from the synergistic effect between components and unique morphological structure, the CoCuSe/Cu2-xSe@PCNFs exhibits excellent bifunctional activity for oxygen reduction reaction (ORR) (E1/2 = 0.85 V) and oxygen evolution reaction (OER) (Ej = 10 = 300 mV) in alkaline electrolyte, and demonstrates superior stability (>1000 h) for high-performance zinc-air batteries. This study combines experiment and theory to provide a new approach for exploring multifunctional electrocatalysts.
Analyzing spatial frequency domain features is essential for capturing diverse in-depth features of targets, thereby enhancing the adaptability to unstructured environments for embodied intelligence. Digital approaches suffer from limited efficiency due to frequent data transfer, while neuromorphic ones lack dedicated frequency-domain processing hardware. Here, we report a Fourier neuromorphic visual (FIVE) system integrating a Fourier optical system and Fourier optoelectronic synapses (FOSs). The FIVE system extracts frequency-domain cues optically with negligible time latency and computational energy consumption, and these cues are then filtered based on nonlinearity to the light intensity of FOSs. Furthermore, such a FOS device exhibits multilevel memory tunability by light intensity of single-wavelength. This property enables the implementation of multilayer perceptron for further classification of frequency domain features. The FIVE system achieves a high accuracy of ∼90% in the image noise classification task and outperforms convolutional neural network (CNN)-based approaches by orders of magnitude in parameter count.
To systematically review and analyze the impact of proprotein convertase subtilisin/kexin type 9 (PCSK9) inhibitors on circulating inflammation, focusing on their underlying mechanisms and clinical application prospects, this review comprehensively summarizes recent studies addressing the molecular basis, nonclassical pathologic mechanisms, clinical evidence in multisystem diseases, therapeutic advances, and combined intervention strategies associated with PCSK9 and its inhibitors, highlighting their anti-inflammatory potential and personalized management strategies. PCSK9 participates in circulating inflammation primarily through multiple signaling pathways, including the NOD-like receptor family pyrin domain containing 3 inflammasome and the Toll-like receptor 4/nuclear factor kappa B axis. Clinical evidence indicates that PCSK9 inhibitors have limited direct effects on traditional inflammatory biomarkers. However, they show benefits in improving atherosclerotic plaque stability and modulating immune-inflammatory gene expression. The anti-inflammatory effects of PCSK9 inhibitors in circulating inflammation might not be directly reflected through changes in conventional inflammatory biomarkers. Future research should further explore their nonclassical mechanisms and optimize personalized risk stratification strategies, integrating multiomics and multiple biomarkers for precise inflammation management.
Atherosclerosis (AS) is a risk factor for various cardiovascular diseases (CVD), and early diagnosis and plaque removal are challenges in the management of AS and CVD. To address these challenges, we designed a tungsten‑doped polydopamine nanoparticle (W-PDA NPs). The near-infrared (NIR) optical absorption and enzymatic properties of W-PDA were tuned by adjusting the ratio of W6+ to PDA. It was found that the W-PDA NPs contain a mixture of W6+ and W5+, which generated large amounts of free electrons, thus conferring both second near-infrared (NIR-II) light absorption capability and superoxide dismutase (SOD)- and catalase (CAT)-like activities. Plaque-targeting was conferred by appending an anti-osteopontin antibody via coordination between carboxyl moieties of the antibody with W6+ ions on the W-PDA surface. The NIR-II light absorption ability can be utilized for photoacoustic diagnosis of AS, while the SOD- and CAT-like activities facilitate the conversion of superoxide into H2O2 and subsequently O2, thereby clearing reactive oxygen species and mitigating inflammation, enabling therapy of AS. Thus, the proposed theranostic agent not only can dynamically report the progression of AS but also can effectively treat AS plaques. This strategy holds broad application prospects in the early and accurate diagnosis and treatment of AS.
Imine-linked covalent organic frameworks (COFs) are promising cathodes for rechargeable magnesium batteries (RMBs), yet their abundant imine linkages (C═N) typically remain electrochemically inert, serving merely as structural connectors. Here, we reveal that the redox inactivity of imine linkages arises from insufficient π-electron delocalization, and we demonstrate that enhancing local delocalization can switch these bonds into highly reversible redox centers. Through precise fluorine substitution in a triazine-based COF, we achieve localized π-delocalization without disrupting the overall conjugated framework. This delocalization-driven activation lowers the LUMO level and stabilizes the reduced state of imine linkages (C-N-), enabling a reversible C═N ⇄ C-N- conversion-a function never realized before in magnesium batteries. The activated imine sites become kinetically preferred Mg2+ migration channels, cutting the diffusion barrier by half (from 1.61 to 0.81 eV) and switching the transport pathway from triazine to imine. Consequently, the optimized COF cathode delivers a high specific capacity of 203.6 mAh g-1, outstanding rate capability, and exceptional cycling stability (72.9% retention after 9000 cycles). This work establishes π-delocalization engineering as a general strategy and a redox switch to unlock latent redox functions in organic frameworks, providing a mechanistic blueprint for activating inert bonds in multivalent energy storage systems beyond magnesium batteries.