Plasmonic nanoantennas provide unique opportunities for precise control of light–matter coupling in surface-enhanced infrared absorption(SEIRA)spectroscopy,but most of the resonant systems realized so far suffer from...Plasmonic nanoantennas provide unique opportunities for precise control of light–matter coupling in surface-enhanced infrared absorption(SEIRA)spectroscopy,but most of the resonant systems realized so far suffer from the obstacles of low sensitivity,narrow bandwidth,and asymmetric Fano resonance perturbations.Here,we demonstrated an overcoupled resonator with a high plasmon-molecule coupling coefficient(μ)(OC-Hμresonator)by precisely controlling the radiation loss channel,the resonator-oscillator coupling channel,and the frequency detuning channel.We observed a strong dependence of the sensing performance on the coupling state,and demonstrated that OC-Hμresonator has excellent sensing properties of ultra-sensitive(7.25%nm^(−1)),ultra-broadband(3–10μm),and immune asymmetric Fano lineshapes.These characteristics represent a breakthrough in SEIRA technology and lay the foundation for specific recognition of biomolecules,trace detection,and protein secondary structure analysis using a single array(array size is 100×100μm^(2)).In addition,with the assistance of machine learning,mixture classification,concentration prediction and spectral reconstruction were achieved with the highest accuracy of 100%.Finally,we demonstrated the potential of OC-Hμresonator for SARS-CoV-2 detection.These findings will promote the wider application of SEIRA technology,while providing new ideas for other enhanced spectroscopy technologies,quantum photonics and studying light–matter interactions.展开更多
Catalyst–support interaction plays a crucial role in improving the catalytic activity of oxygen evolution reaction(OER).Here we modulate the catalyst–support interaction in polyaniline-supported Ni_(3)Fe oxide(Ni_(3...Catalyst–support interaction plays a crucial role in improving the catalytic activity of oxygen evolution reaction(OER).Here we modulate the catalyst–support interaction in polyaniline-supported Ni_(3)Fe oxide(Ni_(3)Fe oxide/PANI)with a robust hetero-interface,which significantly improves oxygen evolution activities with an overpotential of 270 mV at 10 mA cm^(-2)and specific activity of 2.08 mA cm_(ECSA)^(-2)at overpotential of 300 mV,3.84-fold that of Ni_(3)Fe oxide.It is revealed that the catalyst–support interaction between Ni_(3)Fe oxide and PANI support enhances the Ni–O covalency via the interfacial Ni–N bond,thus promoting the charge and mass transfer on Ni_(3)Fe oxide.Considering the excellent activity and stability,rechargeable Zn-air batteries with optimum Ni_(3)Fe oxide/PANI are assembled,delivering a low charge voltage of 1.95 V to cycle for 400 h at 10 mA cm^(-2).The regulation of the effect of catalyst–support interaction on catalytic activity provides new possibilities for the future design of highly efficient OER catalysts.展开更多
The primary mechanism of secondary injury after cerebral ischemia may be the brain inflammation that emerges after an ischemic stroke,which promotes neuronal death and inhibits nerve tissue regeneration.As the first i...The primary mechanism of secondary injury after cerebral ischemia may be the brain inflammation that emerges after an ischemic stroke,which promotes neuronal death and inhibits nerve tissue regeneration.As the first immune cells to be activated after an ischemic stroke,microglia play an important immunomodulatory role in the progression of the condition.After an ischemic stroke,peripheral blood immune cells(mainly T cells)are recruited to the central nervous system by chemokines secreted by immune cells in the brain,where they interact with central nervous system cells(mainly microglia)to trigger a secondary neuroimmune response.This review summarizes the interactions between T cells and microglia in the immune-inflammatory processes of ischemic stroke.We found that,during ischemic stroke,T cells and microglia demonstrate a more pronounced synergistic effect.Th1,Th17,and M1 microglia can co-secrete proinflammatory factors,such as interferon-γ,tumor necrosis factor-α,and interleukin-1β,to promote neuroinflammation and exacerbate brain injury.Th2,Treg,and M2 microglia jointly secrete anti-inflammatory factors,such as interleukin-4,interleukin-10,and transforming growth factor-β,to inhibit the progression of neuroinflammation,as well as growth factors such as brain-derived neurotrophic factor to promote nerve regeneration and repair brain injury.Immune interactions between microglia and T cells influence the direction of the subsequent neuroinflammation,which in turn determines the prognosis of ischemic stroke patients.Clinical trials have been conducted on the ways to modulate the interactions between T cells and microglia toward anti-inflammatory communication using the immunosuppressant fingolimod or overdosing with Treg cells to promote neural tissue repair and reduce the damage caused by ischemic stroke.However,such studies have been relatively infrequent,and clinical experience is still insufficient.In summary,in ischemic stroke,T cell subsets and activated microglia act synergistically to regulate inflammatory progression,mainly by secreting inflammatory factors.In the future,a key research direction for ischemic stroke treatment could be rooted in the enhancement of anti-inflammatory factor secretion by promoting the generation of Th2 and Treg cells,along with the activation of M2-type microglia.These approaches may alleviate neuroinflammation and facilitate the repair of neural tissues.展开更多
This article describes a pilot study aiming at generating social interactions between a humanoid robot and adolescents with autism spectrum disorder (ASD), through the practice of a gesture imitation game. The partici...This article describes a pilot study aiming at generating social interactions between a humanoid robot and adolescents with autism spectrum disorder (ASD), through the practice of a gesture imitation game. The participants were a 17-year-old young lady with ASD and intellectual deficit, and a control participant: a preadolescent with ASD but no intellectual deficit (Asperger syndrome). The game is comprised of four phases: greetings, pairing, imitation, and closing. Field educators were involved, playing specific roles: visual or physical inciter. The use of a robot allows for catching the participants’ attention, playing the imitation game for a longer period of time than with a human partner, and preventing the game partner’s negative facial expressions resulting from tiredness, impatience, or boredom. The participants’ behavior was observed in terms of initial approach towards the robot, positioning relative to the robot in terms of distance and orientation, reactions to the robot’s voice or moves, signs of happiness, and imitation attempts. Results suggest a more and more natural approach towards the robot during the sessions, as well as a higher level of social interaction, based on the variations of the parameters listed above. We use these preliminary results to draw the next steps of our research work as well as identify further perspectives, with this aim in mind: improving social interactions with adolescents with ASD and intellectual deficit, allowing for better integration of these people into our societies.展开更多
Deficiency or restriction of Zn absorption in soils is one of the most common micronutrients deficient in cereal plants. To investigate critical micronutrient interaction in zinc deficiency and zinc sufficient in soil...Deficiency or restriction of Zn absorption in soils is one of the most common micronutrients deficient in cereal plants. To investigate critical micronutrient interaction in zinc deficiency and zinc sufficient in soil, a factorial experiment based on completely randomized design (CRD) with three replications was conducted in 2023. Six wheat cultivars with different Zn efficiency were used. The cultivars were grown under Zn deficiency and adequate conditions. Results showed that in Zn deficiency conditions, with increasing Zn concentration in the roots, Fe concentrations were increased too, while the Cu and Mn concentrations decreased. In the same condition and with increasing Zn concentration in shoots, the concentrations of Fe and Mn decreased, while Cu were increased. However, by increasing Zn concentration, Fe, Cu, and Mn concentrations were increased in Zn deficiency condition in grains, as well as Zn sufficient conditions. RST (root to shoot micronutrient translocation) comparison of cultivars showed that in lack of Zn, the ability of translocation of Zn, Fe, and Mn in Zn-inefficient cultivar from root to shoot was higher than inefficient cultivar. In the same conditions, the capability of Zn-inefficient cultivar in Cu translocation from root to shoot was lower than other cultivars. In general, it seems that in Zn deficiency conditions, there are antagonistic effects among Zn, Cu and Mn and synergistic effects between Zn and Fe in the root. Also, in Zn sufficient conditions, there were synergistic effects among all studies micronutrients which include Zn, Fe, Cu, and Mn.展开更多
The concept of neuroimmune interactions has shown significant advancements over the years. Modern research has revealed many areas of connection between fields, which were previously viewed as distinct disciplines. Fo...The concept of neuroimmune interactions has shown significant advancements over the years. Modern research has revealed many areas of connection between fields, which were previously viewed as distinct disciplines. For example, the nervous system can sense changes in the external environment and convey these changes through molecules and mediators with receptors in the immune system to modulate immune responses. Neuromediators can act on different receptors in the same group of cells, producing antipodal effects. Identification of the anti-inflammatory role of glucocorticoids highlighted that the body functions properly in an integrated manner. These interactions and crosstalk are not unidirectional, as the immune system can also influence various aspects of the nervous system, such as synaptic plasticity and fever. Strict integration of neuro-immuno-endocrine circuits is indispensable for homeostasis. Understanding these circuits and molecules can lead to advances in the understanding of various immune diseases, which will offer promising therapeutic options.展开更多
Maintaining the integrity and longevity of structures is essential in many industries,such as aerospace,nuclear,and petroleum.To achieve the cost-effectiveness of large-scale systems in petroleum drilling,a strong emp...Maintaining the integrity and longevity of structures is essential in many industries,such as aerospace,nuclear,and petroleum.To achieve the cost-effectiveness of large-scale systems in petroleum drilling,a strong emphasis on structural durability and monitoring is required.This study focuses on the mechanical vibrations that occur in rotary drilling systems,which have a substantial impact on the structural integrity of drilling equipment.The study specifically investigates axial,torsional,and lateral vibrations,which might lead to negative consequences such as bit-bounce,chaotic whirling,and high-frequency stick-slip.These events not only hinder the efficiency of drilling but also lead to exhaustion and harm to the system’s components since they are difficult to be detected and controlled in real time.The study investigates the dynamic interactions of these vibrations,specifically in their high-frequency modes,usingfield data obtained from measurement while drilling.Thefindings have demonstrated the effect of strong coupling between the high-frequency modes of these vibrations on drilling sys-tem performance.The obtained results highlight the importance of considering the interconnected impacts of these vibrations when designing and implementing robust control systems.Therefore,integrating these compo-nents can increase the durability of drill bits and drill strings,as well as improve the ability to monitor and detect damage.Moreover,by exploiting thesefindings,the assessment of structural resilience in rotary drilling systems can be enhanced.Furthermore,the study demonstrates the capacity of structural health monitoring to improve the quality,dependability,and efficiency of rotary drilling systems in the petroleum industry.展开更多
This study addresses security and ethical challenges in LLM-based Multi-Agent Systems, as exemplified in a blockchain fraud detection case study. Leveraging blockchain’s secure architecture, the framework involves sp...This study addresses security and ethical challenges in LLM-based Multi-Agent Systems, as exemplified in a blockchain fraud detection case study. Leveraging blockchain’s secure architecture, the framework involves specialized LLM Agents—ContractMining, Investigative, Ethics, and PerformanceMonitor, coordinated by a ManagerAgent. Baseline LLM models achieved 30% accuracy with a threshold method and 94% accuracy with a random-forest method. The Claude 3.5-powered LLM system reached an accuracy of 92%. Ethical evaluations revealed biases, highlighting the need for fairness-focused refinements. Our approach aims to develop trustworthy and reliable networks of agents capable of functioning even in adversarial environments. To our knowledge, no existing systems employ ethical LLM agents specifically designed to detect fraud, making this a novel contribution. Future work will focus on refining ethical frameworks, scaling the system, and benchmarking it against traditional methods to establish a robust, adaptable, and ethically grounded solution for blockchain fraud detection.展开更多
Background:Triple-negative breast cancer(TNBC),characterized by its lack of traditional hormone receptors and HER2,presents a significant challenge in oncology due to its poor response to conventional therapies.Autoph...Background:Triple-negative breast cancer(TNBC),characterized by its lack of traditional hormone receptors and HER2,presents a significant challenge in oncology due to its poor response to conventional therapies.Autophagy is an important process for maintaining cellular homeostasis,and there are currently autophagy biomarkers that play an effective role in the clinical treatment of tumors.In contrast to targeting protein activity,intervention with proteinprotein interaction(PPI)can avoid unrelated crosstalk and regulate the autophagy process with minimal interference pathways.Methods:Here,we employed Naive Bayes,Decision Tree,and k-Nearest Neighbors to elucidate the complex PPI network associated with autophagy in TNBC,aiming to uncover novel therapeutic targets.Meanwhile,the candidate proteins interacting with Beclin 2 were initially screened in MDA-MB-231 cells using Beclin 2 as bait protein by immunoprecipitation-mass spectrometry assay,and the interaction relationship was verified by molecular docking and CO-IP experiments after intersection.Colony formation,cellular immunofluorescence,cell scratch and 3-(4,5-Dimethylthiazol-2-yl)-2,5-diphenyltetrazolium bromide(MTT)tests were used to predict the clinical therapeutic effects of manipulating candidate PPI.Results:By developing three PPI classification models and analyzing over 13,000 datasets,we identified 3733 previously unknown autophagy-related PPIs.Our network analysis revealed the central role of Beclin 2 in autophagy regulation,uncovering its interactions with 39 newly identified proteins.Notably,the CO-IP studies identified the substantial interaction between Beclin 2 and Ubiquilin 1,which was anticipated by our model and discovered in immunoprecipitation-mass spectrometry assay results.Subsequently,in vitro investigations showed that overexpressing Beclin 2 increased Ubiquilin 1,promoted autophagy-dependent cell death,and inhibited proliferation and metastasis in MDA-MB-231 cells.Conclusions:This study not only enhances our understanding of autophagy regulation in TNBC but also identifies the Beclin 2-Ubiquilin 1 axis as a promising target for precision therapy.These findings open new avenues for drug discovery and offer inspiration for more effective treatments for this aggressive cancer subtype.展开更多
BACKGROUND Disorders of gut-brain interaction(DGBI)are common,but knowledge about their physiopathology is still poor,nor valid tools have been used to evaluate them in childhood.AIM To develop a psycho-gastroenterolo...BACKGROUND Disorders of gut-brain interaction(DGBI)are common,but knowledge about their physiopathology is still poor,nor valid tools have been used to evaluate them in childhood.AIM To develop a psycho-gastroenterological questionnaire(PGQ)to assess the psycho-gastroenterological profile and social characteristics of a pediatric population with and without DGBI.METHODS One hundred and nineteen Italian children(age 11-18)were included:28 outpatient patients with DGBI(Rome IV criteria)and 91 healthy controls.They filled the PGQ,faces pain scale revised(FPS-R),Bristol stool chart,ga-strointestinal symptoms rating scale,state-trait anxiety inventory,Toronto alexithymia scale 20,perceived self-efficacy in the management of negative emotions and expression of positive emotions(APEN-G,APEP-G),irritable bowel syndrome-quality of life questionnaire,school performances,tobacco use,early life events,degree of digital-ization.RESULTS Compared to controls,patients had more medical examinations(35%of them went to the doctor more than five times),a higher school performance(23%vs 13%,P<0.05),didn’t use tobacco(never vs 16%,P<0.05),had early life events(28%vs 1%P<0.05)and a higher percentage of pain classified as 4 in the FPS-R during the examination(14%vs 7%,P<0.05).CONCLUSION Pediatric outpatients with DGBI had a higher prevalence of early life events,a lower quality of life,more medical examinations rising health care costs,lower anxiety levels.展开更多
Micrometer-sized silicon oxide(SiO)anodes encounter challenges in large-scale applications due to significant volume expansion during the alloy/de-alloy process.Herein,an innovative deep eutectic electrolyte derived f...Micrometer-sized silicon oxide(SiO)anodes encounter challenges in large-scale applications due to significant volume expansion during the alloy/de-alloy process.Herein,an innovative deep eutectic electrolyte derived from succinonitrile is introduced to enhance the cycling stability of SiO anodes.Density functional theory calculations validate a robust ion-dipole interaction between lithium ions(Li^(+))and succinonitrile(SN).The cosolvent fluoroethylene carbonate(FEC)optimizes the Li^(+)solvation structure in the SN-based electrolyte with its weakly solvating ability.Molecular dynamics simulations investigate the regulating mechanism of ion-dipole and cation-anion interaction.The unique Li^(+)solvation structure,enriched with FEC and TFSI^(-),facilitates the formation of an inorganic-organic composite solid electrolyte interphase on SiO anodes.Micro-CT further detects the inhibiting effect on the SiO volume expansion.As a result,the SiO|LiCoO_(2) full cells exhibit excellent electrochemical performance in deep eutectic-based electrolytes.This work presents an effective strategy for extending the cycle life of SiO anodes by designing a new SN-based deep eutectic electrolyte.展开更多
RNA molecules play crucial roles in various biological processes. Their regulation and function are mediated by interacting with other molecules. Among them RNA-RNA interactions （RRIs） are important in many basic ce...RNA molecules play crucial roles in various biological processes. Their regulation and function are mediated by interacting with other molecules. Among them RNA-RNA interactions （RRIs） are important in many basic cellular activities including transcription, RNA processing, localization, and translation. However, we just start to unveil the complexity of the knowledge and underlying mechanisms of RRIs. Results： In this review, we will summarize approaches for RRI identifications, including both conventional, focused biophysical and biochemical methods and recently developed large scale sequencing-based techniques. We will also discuss discoveries per RRI type revealed by using these technologies, as well as challenges towards a systematic and functional understanding of RRIs. Conclusions： The development of sequencing-based techniques has revolutionized the study of RRIs. Applying these techniques in multiple organisms has identified thousands of RRls, many of which could potentially regulate multiple aspects of gene expression. However, despite the great breakthrough, the RNA-RNA interactome of any species remains far from complete due to intrinsic complex nature of RRI and limitations in current techniques. More efficient experimental methods and computational framework are needed to obtain the full image of RRI networks, and their possible regulatory roles in biology and medicine.展开更多
Ultrasmall gold nanoparticles(AuNPs)typically includes atomically precise gold nanoclusters(AuNCs)and AuNPs with a core size below 3 nm.Serving as a bridge between small molecules and traditional inorganic nanoparticl...Ultrasmall gold nanoparticles(AuNPs)typically includes atomically precise gold nanoclusters(AuNCs)and AuNPs with a core size below 3 nm.Serving as a bridge between small molecules and traditional inorganic nanoparticles,the ultrasmall AuNPs show the unique advantages of both small molecules(e.g.,rapid distribution,renal clearance,low non-specific organ accumulation)and nanoparticles(e.g.,long blood circulation and enhanced permeability and retention effect).The emergence of ultrasmall AuNPs creates significant opportunities to address many challenges in the health field including disease diagnosis,monitoring and treatment.Since the nano–bio interaction dictates the overall biological applications of the ultrasmall AuNPs,this review elucidates the recent advances in the biological interactions and imaging of ultrasmall AuNPs.We begin with the introduction of the factors that influence the cellular interactions of ultrasmall AuNPs.We then discuss the organ interactions,especially focus on the interactions of the liver and kidneys.We further present the recent advances in the tumor interactions of ultrasmall AuNPs.In addition,the imaging performance of the ultrasmall AuNPs is summarized and discussed.Finally,we summarize this review and provide some perspective on the future research direction of the ultrasmall AuNPs,aiming to accelerate their clinical translation.展开更多
The high throughput prediction of the thermodynamic phase behavior of active pharmaceutical ingredients(APIs)with pharmaceutically relevant excipients remains a major scientific challenge in the screening of pharmaceu...The high throughput prediction of the thermodynamic phase behavior of active pharmaceutical ingredients(APIs)with pharmaceutically relevant excipients remains a major scientific challenge in the screening of pharmaceutical formulations.In this work,a developed machine-learning model efficiently predicts the solubility of APIs in polymers by learning the phase equilibrium principle and using a few molecular descriptors.Under the few-shot learning framework,thermodynamic theory(perturbed-chain statistical associating fluid theory)was used for data augmentation,and computational chemistry was applied for molecular descriptors'screening.The results showed that the developed machine-learning model can predict the API-polymer phase diagram accurately,broaden the solubility data of APIs in polymers,and reproduce the relationship between API solubility and the interaction mechanisms between API and polymer successfully,which provided efficient guidance for the development of pharmaceutical formulations.展开更多
Ruthenium(Ru)has been regarded as one of the most promising alternatives to substitute Pt for catalyzing alkaline hydrogen evolution reaction(HER),owing to its inherent high activity and being the cheapest platinum-gr...Ruthenium(Ru)has been regarded as one of the most promising alternatives to substitute Pt for catalyzing alkaline hydrogen evolution reaction(HER),owing to its inherent high activity and being the cheapest platinum-group metal.Herein,based on the idea of strong metal–support interaction(SMSI)regulation,Ru/TiN catalysts with different degrees of TiN overlayer over Ru nanoparticles were fabricated,which were applied to the alkaline electrolytic water.Characterizations reveal that the TiN overlayer would gradually encapsulate the Ru nanoparticles and induce more electron transfer from Ru nanoparticles to TiN support by the Ru–N–Ti bond as the SMSI degree increased.Further study shows that the exposed Ru–TiN interfaces greatly promote the H_(2) desorption capacity.Thus,the Ru/TiN-300 with a moderate SMSI degree exhibits excellent HER performance,with an overpotential of 38 mV at 10 mA cm^(−2).Also,due to the encapsulation role of TiN overlayer on Ru nanoparticles,it displays super long-term stability with a very slight potential change after 24 h.This study provides a deep insight into the influence of the SMSI effect between Ru and TiN on HER and offers a novel approach for preparing efficient and stable HER electrocatalysts through SMSI engineering.展开更多
The development of bioinspired gradient hydrogels with self-sensing actuated capabilities for remote interaction with soft-hard robots remains a challenging endeavor. Here, we propose a novel multifunctional self-sens...The development of bioinspired gradient hydrogels with self-sensing actuated capabilities for remote interaction with soft-hard robots remains a challenging endeavor. Here, we propose a novel multifunctional self-sensing actuated gradient hydrogel that combines ultrafast actuation and high sensitivity for remote interaction with robotic hand. The gradient network structure, achieved through a wettability difference method involving the rapid precipitation of MoO_(2) nanosheets, introduces hydrophilic disparities between two sides within hydrogel. This distinctive approach bestows the hydrogel with ultrafast thermo-responsive actuation(21° s^(-1)) and enhanced photothermal efficiency(increase by 3.7 ℃ s^(-1) under 808 nm near-infrared). Moreover, the local cross-linking of sodium alginate with Ca^(2+) endows the hydrogel with programmable deformability and information display capabilities. Additionally, the hydrogel exhibits high sensitivity(gauge factor 3.94 within a wide strain range of 600%), fast response times(140 ms) and good cycling stability. Leveraging these exceptional properties, we incorporate the hydrogel into various soft actuators, including soft gripper, artificial iris, and bioinspired jellyfish, as well as wearable electronics capable of precise human motion and physiological signal detection. Furthermore, through the synergistic combination of remarkable actuation and sensitivity, we realize a self-sensing touch bioinspired tongue. Notably, by employing quantitative analysis of actuation-sensing, we realize remote interaction between soft-hard robot via the Internet of Things. The multifunctional self-sensing actuated gradient hydrogel presented in this study provides a new insight for advanced somatosensory materials, self-feedback intelligent soft robots and human–machine interactions.展开更多
Thermoelectric(TE)generators capable of converting thermal energy into applicable electricity have gained great popularity among emerging energy conversion technologies.Biopolymer-based ionic thermoelectric(i-TE)mater...Thermoelectric(TE)generators capable of converting thermal energy into applicable electricity have gained great popularity among emerging energy conversion technologies.Biopolymer-based ionic thermoelectric(i-TE)materials are promising candidates for energy conversion systems because of their wide sources,innocuity,and low manufacturing cost.However,common physically crosslinked biopolymer gels induced by single hydrogen bonding or hydrophobic interaction suffer from low differential thermal voltage and poor thermodynamic stability.Here,we develop a novel i-TE gel with supramolecular structures through multiple noncovalent interactions between ionic liquids(ILs)and gelatin molecular chains.The thermopower and thermoelectric power factor of the ionic gels are as high as 2.83 mV K-1 and 18.33μW m^(-1)K^(-2),respectively.The quasi-solid-state gelatin-[EMIM]DCA i-TE cells achieve ultrahigh 2 h output energy density(E_(2h)=9.9 mJ m^(-2))under an optimal temperature range.Meanwhile,the remarkable stability of the supramolecular structure provides the i-TE hydrogels with a thermal stability of up to 80℃.It breaks the limitation that biopolymer-based i-TE gels can only be applied in the low temperature range and enables biopolymer-based i-TE materials to pursue better performance in a higher temperature range.展开更多
Water electrolysis poses a significant challenge for balancing catalytic activity and stability of oxygen evolution reaction(OER)electrocatalysts.In this study,we address this challenge by constructing asymmetric redo...Water electrolysis poses a significant challenge for balancing catalytic activity and stability of oxygen evolution reaction(OER)electrocatalysts.In this study,we address this challenge by constructing asymmetric redox chemistry through elaborate surface OO–Ru–OH and bulk Ru–O–Ni/Fe coordination moieties within single-atom Ru-decorated defective NiFe LDH nanosheets(Ru@d-NiFe LDH)in conjunction with strong metal-support interactions(SMSI).Rigorous spectroscopic characterization and theoretical calculations indicate that single-atom Ru can delocalize the O 2p electrons on the surface and optimize d-electron configurations of metal atoms in bulk through SMSI.The^(18)O isotope labeling experiment based on operando differential electrochemical mass spectrometry(DEMS),chemical probe experiments,and theoretical calculations confirm the encouraged surface lattice oxygen,stabilized bulk lattice oxygen,and enhanced adsorption of oxygen-containing intermediates for bulk metals in Ru@d-NiFe LDH,leading to asymmetric redox chemistry for OER.The Ru@d-NiFe LDH electrocatalyst exhibits exceptional performance with an overpotential of 230 mV to achieve 10 mA cm^(−2)and maintains high robustness under industrial current density.This approach for achieving asymmetric redox chemistry through SMSI presents a new avenue for developing high-performance electrocatalysts and instills confidence in its industrial applicability.展开更多
Metal-organic framework(MOF)-derived carbon composites have been considered as the promising materials for energy storage.However,the construction of MOF-based composites with highly controllable mode via the liquid-l...Metal-organic framework(MOF)-derived carbon composites have been considered as the promising materials for energy storage.However,the construction of MOF-based composites with highly controllable mode via the liquid-liquid synthesis method has a great challenge because of the simultaneous heterogeneous nucleation on substrates and the self-nucleation of individual MOF nanocrystals in the liquid phase.Herein,we report a bidirectional electrostatic generated self-assembly strategy to achieve the precisely controlled coatings of single-layer nanoscale MOFs on a range of substrates,including carbon nanotubes(CNTs),graphene oxide(GO),MXene,layered double hydroxides(LDHs),MOFs,and SiO_(2).The obtained MOF-based nanostructured carbon composite exhibits the hierarchical porosity(V_(meso)/V_(micro)∶2.4),ultrahigh N content of 12.4 at.%and"dual electrical conductive networks."The assembled aqueous zinc-ion hybrid capacitor(ZIC)with the prepared nanocarbon composite as a cathode shows a high specific capacitance of 236 F g^(-1)at 0.5 A g^(-1),great rate performance of 98 F g^(-1)at 100 A g^(-1),and especially,an ultralong cycling stability up to 230000 cycles with the capacitance retention of 90.1%.This work develops a repeatable and general method for the controlled construction of MOF coatings on various functional substrates and further fabricates carbon composites for ZICs with ultrastability.展开更多
Two suites of mafic dykes,T1193-A and T1194-A,outcrop in Gyangze area,southeast Tibet.They are in the area of Comei LIP and have indistinguishable field occurrences with two other dykes in Gyangze,T0902 dyke with 137....Two suites of mafic dykes,T1193-A and T1194-A,outcrop in Gyangze area,southeast Tibet.They are in the area of Comei LIP and have indistinguishable field occurrences with two other dykes in Gyangze,T0902 dyke with 137.7±1.3 Ma zircon age and T0907 dyke with 142±1.4 Ma zircon age reported by Wang YY et al.(2016),indicating coeval formation time.Taking all the four diabase dykes into consideration,two different types,OIB-type and weak enriched-type,can be summarized.The“OIB-type”samples,including T1193-A and T0907 dykes,show OIB-like geochemical features and have initial Sr-Nd isotopic values similar with most mafic products in Comei Large Igneous Provinces(LIP),suggesting that they represent melts directly generated from the Kerguelen mantle plume.The“weak enriched-type”samples,including T1194-A and T0902 dykes,have REEs and trace element patterns showing withinplate affinity but have obvious Nb-Ta-Ti negative anomalies.They show uniform lowerεNd(t)values(−6‒−2)and higher 87Sr/86Sr(t)values(0.706‒0.709)independent of their MgO variation,indicating one enriched mantle source.Considering their closely spatial and temporal relationship with the widespread Comei LIP magmatic products in Tethyan Himalaya,these“weak enriched-type”samples are consistent with mixing of melts from mantle plume and the above ancient Tethyan Himalaya subcontinental lithospheric mantle(SCLM)in different proportions.These weak enriched mafic rocks in Comei LIP form one special rock group and most likely suggest large scale hot mantle plume-continental lithosphere interaction.This process may lead to strong modification of the Tethyan Himalaya lithosphere in the Early Cretaceous.展开更多
基金supported by A*STAR under the“Nanosystems at the Edge”program(Grant No.A18A4b0055)Ministry of Education(MOE)under the research grant of R-263-000-F18-112/A-0009520-01-00+1 种基金National Research Foundation Singapore grant CRP28-2022-0038the Reimagine Re-search Scheme(RRSC)Project(Grant A-0009037-02-00&A0009037-03-00)at National University of Singapore.
文摘Plasmonic nanoantennas provide unique opportunities for precise control of light–matter coupling in surface-enhanced infrared absorption(SEIRA)spectroscopy,but most of the resonant systems realized so far suffer from the obstacles of low sensitivity,narrow bandwidth,and asymmetric Fano resonance perturbations.Here,we demonstrated an overcoupled resonator with a high plasmon-molecule coupling coefficient(μ)(OC-Hμresonator)by precisely controlling the radiation loss channel,the resonator-oscillator coupling channel,and the frequency detuning channel.We observed a strong dependence of the sensing performance on the coupling state,and demonstrated that OC-Hμresonator has excellent sensing properties of ultra-sensitive(7.25%nm^(−1)),ultra-broadband(3–10μm),and immune asymmetric Fano lineshapes.These characteristics represent a breakthrough in SEIRA technology and lay the foundation for specific recognition of biomolecules,trace detection,and protein secondary structure analysis using a single array(array size is 100×100μm^(2)).In addition,with the assistance of machine learning,mixture classification,concentration prediction and spectral reconstruction were achieved with the highest accuracy of 100%.Finally,we demonstrated the potential of OC-Hμresonator for SARS-CoV-2 detection.These findings will promote the wider application of SEIRA technology,while providing new ideas for other enhanced spectroscopy technologies,quantum photonics and studying light–matter interactions.
基金Research Institute for Smart Energy(CDB2)the grant from the Research Institute for Advanced Manufacturing(CD8Z)+4 种基金the grant from the Carbon Neutrality Funding Scheme(WZ2R)at The Hong Kong Polytechnic Universitysupport from the Hong Kong Polytechnic University(CD9B,CDBZ and WZ4Q)the National Natural Science Foundation of China(22205187)Shenzhen Municipal Science and Technology Innovation Commission(JCYJ20230807140402006)Start-up Foundation for Introducing Talent of NUIST and Natural Science Foundation of Jiangsu Province of China(BK20230426).
文摘Catalyst–support interaction plays a crucial role in improving the catalytic activity of oxygen evolution reaction(OER).Here we modulate the catalyst–support interaction in polyaniline-supported Ni_(3)Fe oxide(Ni_(3)Fe oxide/PANI)with a robust hetero-interface,which significantly improves oxygen evolution activities with an overpotential of 270 mV at 10 mA cm^(-2)and specific activity of 2.08 mA cm_(ECSA)^(-2)at overpotential of 300 mV,3.84-fold that of Ni_(3)Fe oxide.It is revealed that the catalyst–support interaction between Ni_(3)Fe oxide and PANI support enhances the Ni–O covalency via the interfacial Ni–N bond,thus promoting the charge and mass transfer on Ni_(3)Fe oxide.Considering the excellent activity and stability,rechargeable Zn-air batteries with optimum Ni_(3)Fe oxide/PANI are assembled,delivering a low charge voltage of 1.95 V to cycle for 400 h at 10 mA cm^(-2).The regulation of the effect of catalyst–support interaction on catalytic activity provides new possibilities for the future design of highly efficient OER catalysts.
基金supported by the National Natural Science Foundation of China,Nos.82104560(to CL),U21A20400(to QW)the Natural Science Foundation of Beijing,No.7232279(to XW)the Project of Beijing University of Chinese Medicine,No.2022-JYB-JBZR-004(to XW)。
文摘The primary mechanism of secondary injury after cerebral ischemia may be the brain inflammation that emerges after an ischemic stroke,which promotes neuronal death and inhibits nerve tissue regeneration.As the first immune cells to be activated after an ischemic stroke,microglia play an important immunomodulatory role in the progression of the condition.After an ischemic stroke,peripheral blood immune cells(mainly T cells)are recruited to the central nervous system by chemokines secreted by immune cells in the brain,where they interact with central nervous system cells(mainly microglia)to trigger a secondary neuroimmune response.This review summarizes the interactions between T cells and microglia in the immune-inflammatory processes of ischemic stroke.We found that,during ischemic stroke,T cells and microglia demonstrate a more pronounced synergistic effect.Th1,Th17,and M1 microglia can co-secrete proinflammatory factors,such as interferon-γ,tumor necrosis factor-α,and interleukin-1β,to promote neuroinflammation and exacerbate brain injury.Th2,Treg,and M2 microglia jointly secrete anti-inflammatory factors,such as interleukin-4,interleukin-10,and transforming growth factor-β,to inhibit the progression of neuroinflammation,as well as growth factors such as brain-derived neurotrophic factor to promote nerve regeneration and repair brain injury.Immune interactions between microglia and T cells influence the direction of the subsequent neuroinflammation,which in turn determines the prognosis of ischemic stroke patients.Clinical trials have been conducted on the ways to modulate the interactions between T cells and microglia toward anti-inflammatory communication using the immunosuppressant fingolimod or overdosing with Treg cells to promote neural tissue repair and reduce the damage caused by ischemic stroke.However,such studies have been relatively infrequent,and clinical experience is still insufficient.In summary,in ischemic stroke,T cell subsets and activated microglia act synergistically to regulate inflammatory progression,mainly by secreting inflammatory factors.In the future,a key research direction for ischemic stroke treatment could be rooted in the enhancement of anti-inflammatory factor secretion by promoting the generation of Th2 and Treg cells,along with the activation of M2-type microglia.These approaches may alleviate neuroinflammation and facilitate the repair of neural tissues.
文摘This article describes a pilot study aiming at generating social interactions between a humanoid robot and adolescents with autism spectrum disorder (ASD), through the practice of a gesture imitation game. The participants were a 17-year-old young lady with ASD and intellectual deficit, and a control participant: a preadolescent with ASD but no intellectual deficit (Asperger syndrome). The game is comprised of four phases: greetings, pairing, imitation, and closing. Field educators were involved, playing specific roles: visual or physical inciter. The use of a robot allows for catching the participants’ attention, playing the imitation game for a longer period of time than with a human partner, and preventing the game partner’s negative facial expressions resulting from tiredness, impatience, or boredom. The participants’ behavior was observed in terms of initial approach towards the robot, positioning relative to the robot in terms of distance and orientation, reactions to the robot’s voice or moves, signs of happiness, and imitation attempts. Results suggest a more and more natural approach towards the robot during the sessions, as well as a higher level of social interaction, based on the variations of the parameters listed above. We use these preliminary results to draw the next steps of our research work as well as identify further perspectives, with this aim in mind: improving social interactions with adolescents with ASD and intellectual deficit, allowing for better integration of these people into our societies.
文摘Deficiency or restriction of Zn absorption in soils is one of the most common micronutrients deficient in cereal plants. To investigate critical micronutrient interaction in zinc deficiency and zinc sufficient in soil, a factorial experiment based on completely randomized design (CRD) with three replications was conducted in 2023. Six wheat cultivars with different Zn efficiency were used. The cultivars were grown under Zn deficiency and adequate conditions. Results showed that in Zn deficiency conditions, with increasing Zn concentration in the roots, Fe concentrations were increased too, while the Cu and Mn concentrations decreased. In the same condition and with increasing Zn concentration in shoots, the concentrations of Fe and Mn decreased, while Cu were increased. However, by increasing Zn concentration, Fe, Cu, and Mn concentrations were increased in Zn deficiency condition in grains, as well as Zn sufficient conditions. RST (root to shoot micronutrient translocation) comparison of cultivars showed that in lack of Zn, the ability of translocation of Zn, Fe, and Mn in Zn-inefficient cultivar from root to shoot was higher than inefficient cultivar. In the same conditions, the capability of Zn-inefficient cultivar in Cu translocation from root to shoot was lower than other cultivars. In general, it seems that in Zn deficiency conditions, there are antagonistic effects among Zn, Cu and Mn and synergistic effects between Zn and Fe in the root. Also, in Zn sufficient conditions, there were synergistic effects among all studies micronutrients which include Zn, Fe, Cu, and Mn.
文摘The concept of neuroimmune interactions has shown significant advancements over the years. Modern research has revealed many areas of connection between fields, which were previously viewed as distinct disciplines. For example, the nervous system can sense changes in the external environment and convey these changes through molecules and mediators with receptors in the immune system to modulate immune responses. Neuromediators can act on different receptors in the same group of cells, producing antipodal effects. Identification of the anti-inflammatory role of glucocorticoids highlighted that the body functions properly in an integrated manner. These interactions and crosstalk are not unidirectional, as the immune system can also influence various aspects of the nervous system, such as synaptic plasticity and fever. Strict integration of neuro-immuno-endocrine circuits is indispensable for homeostasis. Understanding these circuits and molecules can lead to advances in the understanding of various immune diseases, which will offer promising therapeutic options.
文摘Maintaining the integrity and longevity of structures is essential in many industries,such as aerospace,nuclear,and petroleum.To achieve the cost-effectiveness of large-scale systems in petroleum drilling,a strong emphasis on structural durability and monitoring is required.This study focuses on the mechanical vibrations that occur in rotary drilling systems,which have a substantial impact on the structural integrity of drilling equipment.The study specifically investigates axial,torsional,and lateral vibrations,which might lead to negative consequences such as bit-bounce,chaotic whirling,and high-frequency stick-slip.These events not only hinder the efficiency of drilling but also lead to exhaustion and harm to the system’s components since they are difficult to be detected and controlled in real time.The study investigates the dynamic interactions of these vibrations,specifically in their high-frequency modes,usingfield data obtained from measurement while drilling.Thefindings have demonstrated the effect of strong coupling between the high-frequency modes of these vibrations on drilling sys-tem performance.The obtained results highlight the importance of considering the interconnected impacts of these vibrations when designing and implementing robust control systems.Therefore,integrating these compo-nents can increase the durability of drill bits and drill strings,as well as improve the ability to monitor and detect damage.Moreover,by exploiting thesefindings,the assessment of structural resilience in rotary drilling systems can be enhanced.Furthermore,the study demonstrates the capacity of structural health monitoring to improve the quality,dependability,and efficiency of rotary drilling systems in the petroleum industry.
文摘This study addresses security and ethical challenges in LLM-based Multi-Agent Systems, as exemplified in a blockchain fraud detection case study. Leveraging blockchain’s secure architecture, the framework involves specialized LLM Agents—ContractMining, Investigative, Ethics, and PerformanceMonitor, coordinated by a ManagerAgent. Baseline LLM models achieved 30% accuracy with a threshold method and 94% accuracy with a random-forest method. The Claude 3.5-powered LLM system reached an accuracy of 92%. Ethical evaluations revealed biases, highlighting the need for fairness-focused refinements. Our approach aims to develop trustworthy and reliable networks of agents capable of functioning even in adversarial environments. To our knowledge, no existing systems employ ethical LLM agents specifically designed to detect fraud, making this a novel contribution. Future work will focus on refining ethical frameworks, scaling the system, and benchmarking it against traditional methods to establish a robust, adaptable, and ethically grounded solution for blockchain fraud detection.
基金the National Natural Science Foundation of China(Nos.22307009,82374155,82073997,82104376)the Sichuan Science and Technology Program(Nos.2023NSFSC1108,2024NSFTD0023)+1 种基金the Postdoctoral Research Project of Sichuan Provincethe Xinglin Scholar Research Promotion Project of Chengdu University of TCM.
文摘Background:Triple-negative breast cancer(TNBC),characterized by its lack of traditional hormone receptors and HER2,presents a significant challenge in oncology due to its poor response to conventional therapies.Autophagy is an important process for maintaining cellular homeostasis,and there are currently autophagy biomarkers that play an effective role in the clinical treatment of tumors.In contrast to targeting protein activity,intervention with proteinprotein interaction(PPI)can avoid unrelated crosstalk and regulate the autophagy process with minimal interference pathways.Methods:Here,we employed Naive Bayes,Decision Tree,and k-Nearest Neighbors to elucidate the complex PPI network associated with autophagy in TNBC,aiming to uncover novel therapeutic targets.Meanwhile,the candidate proteins interacting with Beclin 2 were initially screened in MDA-MB-231 cells using Beclin 2 as bait protein by immunoprecipitation-mass spectrometry assay,and the interaction relationship was verified by molecular docking and CO-IP experiments after intersection.Colony formation,cellular immunofluorescence,cell scratch and 3-(4,5-Dimethylthiazol-2-yl)-2,5-diphenyltetrazolium bromide(MTT)tests were used to predict the clinical therapeutic effects of manipulating candidate PPI.Results:By developing three PPI classification models and analyzing over 13,000 datasets,we identified 3733 previously unknown autophagy-related PPIs.Our network analysis revealed the central role of Beclin 2 in autophagy regulation,uncovering its interactions with 39 newly identified proteins.Notably,the CO-IP studies identified the substantial interaction between Beclin 2 and Ubiquilin 1,which was anticipated by our model and discovered in immunoprecipitation-mass spectrometry assay results.Subsequently,in vitro investigations showed that overexpressing Beclin 2 increased Ubiquilin 1,promoted autophagy-dependent cell death,and inhibited proliferation and metastasis in MDA-MB-231 cells.Conclusions:This study not only enhances our understanding of autophagy regulation in TNBC but also identifies the Beclin 2-Ubiquilin 1 axis as a promising target for precision therapy.These findings open new avenues for drug discovery and offer inspiration for more effective treatments for this aggressive cancer subtype.
文摘BACKGROUND Disorders of gut-brain interaction(DGBI)are common,but knowledge about their physiopathology is still poor,nor valid tools have been used to evaluate them in childhood.AIM To develop a psycho-gastroenterological questionnaire(PGQ)to assess the psycho-gastroenterological profile and social characteristics of a pediatric population with and without DGBI.METHODS One hundred and nineteen Italian children(age 11-18)were included:28 outpatient patients with DGBI(Rome IV criteria)and 91 healthy controls.They filled the PGQ,faces pain scale revised(FPS-R),Bristol stool chart,ga-strointestinal symptoms rating scale,state-trait anxiety inventory,Toronto alexithymia scale 20,perceived self-efficacy in the management of negative emotions and expression of positive emotions(APEN-G,APEP-G),irritable bowel syndrome-quality of life questionnaire,school performances,tobacco use,early life events,degree of digital-ization.RESULTS Compared to controls,patients had more medical examinations(35%of them went to the doctor more than five times),a higher school performance(23%vs 13%,P<0.05),didn’t use tobacco(never vs 16%,P<0.05),had early life events(28%vs 1%P<0.05)and a higher percentage of pain classified as 4 in the FPS-R during the examination(14%vs 7%,P<0.05).CONCLUSION Pediatric outpatients with DGBI had a higher prevalence of early life events,a lower quality of life,more medical examinations rising health care costs,lower anxiety levels.
基金supported by the National Natural Science Foundation of China(22279026)the National Key Research and Development Program of China(2022YFE0138900)+2 种基金the Young Elite Scientist sponsorship program by CAST(no.20200148)the Natural Science Funds of Heilongjiang Province(YQ2021B003)the Fundamental Research Funds for the Central Universities(grant no.HIT.OCEF.2022017).
文摘Micrometer-sized silicon oxide(SiO)anodes encounter challenges in large-scale applications due to significant volume expansion during the alloy/de-alloy process.Herein,an innovative deep eutectic electrolyte derived from succinonitrile is introduced to enhance the cycling stability of SiO anodes.Density functional theory calculations validate a robust ion-dipole interaction between lithium ions(Li^(+))and succinonitrile(SN).The cosolvent fluoroethylene carbonate(FEC)optimizes the Li^(+)solvation structure in the SN-based electrolyte with its weakly solvating ability.Molecular dynamics simulations investigate the regulating mechanism of ion-dipole and cation-anion interaction.The unique Li^(+)solvation structure,enriched with FEC and TFSI^(-),facilitates the formation of an inorganic-organic composite solid electrolyte interphase on SiO anodes.Micro-CT further detects the inhibiting effect on the SiO volume expansion.As a result,the SiO|LiCoO_(2) full cells exhibit excellent electrochemical performance in deep eutectic-based electrolytes.This work presents an effective strategy for extending the cycle life of SiO anodes by designing a new SN-based deep eutectic electrolyte.
文摘RNA molecules play crucial roles in various biological processes. Their regulation and function are mediated by interacting with other molecules. Among them RNA-RNA interactions （RRIs） are important in many basic cellular activities including transcription, RNA processing, localization, and translation. However, we just start to unveil the complexity of the knowledge and underlying mechanisms of RRIs. Results： In this review, we will summarize approaches for RRI identifications, including both conventional, focused biophysical and biochemical methods and recently developed large scale sequencing-based techniques. We will also discuss discoveries per RRI type revealed by using these technologies, as well as challenges towards a systematic and functional understanding of RRIs. Conclusions： The development of sequencing-based techniques has revolutionized the study of RRIs. Applying these techniques in multiple organisms has identified thousands of RRls, many of which could potentially regulate multiple aspects of gene expression. However, despite the great breakthrough, the RNA-RNA interactome of any species remains far from complete due to intrinsic complex nature of RRI and limitations in current techniques. More efficient experimental methods and computational framework are needed to obtain the full image of RRI networks, and their possible regulatory roles in biology and medicine.
基金the National Natural Science Foundation of China(Grant 22022403 and 22274058)Fundamental Research Funds for the Central Universities.
文摘Ultrasmall gold nanoparticles(AuNPs)typically includes atomically precise gold nanoclusters(AuNCs)and AuNPs with a core size below 3 nm.Serving as a bridge between small molecules and traditional inorganic nanoparticles,the ultrasmall AuNPs show the unique advantages of both small molecules(e.g.,rapid distribution,renal clearance,low non-specific organ accumulation)and nanoparticles(e.g.,long blood circulation and enhanced permeability and retention effect).The emergence of ultrasmall AuNPs creates significant opportunities to address many challenges in the health field including disease diagnosis,monitoring and treatment.Since the nano–bio interaction dictates the overall biological applications of the ultrasmall AuNPs,this review elucidates the recent advances in the biological interactions and imaging of ultrasmall AuNPs.We begin with the introduction of the factors that influence the cellular interactions of ultrasmall AuNPs.We then discuss the organ interactions,especially focus on the interactions of the liver and kidneys.We further present the recent advances in the tumor interactions of ultrasmall AuNPs.In addition,the imaging performance of the ultrasmall AuNPs is summarized and discussed.Finally,we summarize this review and provide some perspective on the future research direction of the ultrasmall AuNPs,aiming to accelerate their clinical translation.
基金the financial support from the National Natural Science Foundation of China(22278070,21978047,21776046)。
文摘The high throughput prediction of the thermodynamic phase behavior of active pharmaceutical ingredients(APIs)with pharmaceutically relevant excipients remains a major scientific challenge in the screening of pharmaceutical formulations.In this work,a developed machine-learning model efficiently predicts the solubility of APIs in polymers by learning the phase equilibrium principle and using a few molecular descriptors.Under the few-shot learning framework,thermodynamic theory(perturbed-chain statistical associating fluid theory)was used for data augmentation,and computational chemistry was applied for molecular descriptors'screening.The results showed that the developed machine-learning model can predict the API-polymer phase diagram accurately,broaden the solubility data of APIs in polymers,and reproduce the relationship between API solubility and the interaction mechanisms between API and polymer successfully,which provided efficient guidance for the development of pharmaceutical formulations.
基金supported by the National Natural Science Foundation of China(Grant Nos.22075159,22002066)Shandong Taishan Scholars Project(Grant Nos.ts20190932,tsqn202103058)+1 种基金Open Fund of Hubei Key Laboratory of Processing and Application of Catalytic Materials(Grant No.202203404)Postdoctoral Applied Research Project in Qingdao,and the Youth Innovation Team Project of Shandong Provincial Education Department(Grant No.2019KJC023).
文摘Ruthenium(Ru)has been regarded as one of the most promising alternatives to substitute Pt for catalyzing alkaline hydrogen evolution reaction(HER),owing to its inherent high activity and being the cheapest platinum-group metal.Herein,based on the idea of strong metal–support interaction(SMSI)regulation,Ru/TiN catalysts with different degrees of TiN overlayer over Ru nanoparticles were fabricated,which were applied to the alkaline electrolytic water.Characterizations reveal that the TiN overlayer would gradually encapsulate the Ru nanoparticles and induce more electron transfer from Ru nanoparticles to TiN support by the Ru–N–Ti bond as the SMSI degree increased.Further study shows that the exposed Ru–TiN interfaces greatly promote the H_(2) desorption capacity.Thus,the Ru/TiN-300 with a moderate SMSI degree exhibits excellent HER performance,with an overpotential of 38 mV at 10 mA cm^(−2).Also,due to the encapsulation role of TiN overlayer on Ru nanoparticles,it displays super long-term stability with a very slight potential change after 24 h.This study provides a deep insight into the influence of the SMSI effect between Ru and TiN on HER and offers a novel approach for preparing efficient and stable HER electrocatalysts through SMSI engineering.
基金The financial support from the National Natural Science Foundation of China (32201179)Guangdong Basic and Applied Basic Research Foundation (2020A1515110126 and 2021A1515010130)+1 种基金the Fundamental Research Funds for the Central Universities (N2319005)Ningbo Science and Technology Major Project (2021Z027) is gratefully acknowledged。
文摘The development of bioinspired gradient hydrogels with self-sensing actuated capabilities for remote interaction with soft-hard robots remains a challenging endeavor. Here, we propose a novel multifunctional self-sensing actuated gradient hydrogel that combines ultrafast actuation and high sensitivity for remote interaction with robotic hand. The gradient network structure, achieved through a wettability difference method involving the rapid precipitation of MoO_(2) nanosheets, introduces hydrophilic disparities between two sides within hydrogel. This distinctive approach bestows the hydrogel with ultrafast thermo-responsive actuation(21° s^(-1)) and enhanced photothermal efficiency(increase by 3.7 ℃ s^(-1) under 808 nm near-infrared). Moreover, the local cross-linking of sodium alginate with Ca^(2+) endows the hydrogel with programmable deformability and information display capabilities. Additionally, the hydrogel exhibits high sensitivity(gauge factor 3.94 within a wide strain range of 600%), fast response times(140 ms) and good cycling stability. Leveraging these exceptional properties, we incorporate the hydrogel into various soft actuators, including soft gripper, artificial iris, and bioinspired jellyfish, as well as wearable electronics capable of precise human motion and physiological signal detection. Furthermore, through the synergistic combination of remarkable actuation and sensitivity, we realize a self-sensing touch bioinspired tongue. Notably, by employing quantitative analysis of actuation-sensing, we realize remote interaction between soft-hard robot via the Internet of Things. The multifunctional self-sensing actuated gradient hydrogel presented in this study provides a new insight for advanced somatosensory materials, self-feedback intelligent soft robots and human–machine interactions.
基金financially supported by the National Natural Science Foundation of China(NNSFC grants 52125301)the Fundamental Research Funds for the Central Universities
文摘Thermoelectric(TE)generators capable of converting thermal energy into applicable electricity have gained great popularity among emerging energy conversion technologies.Biopolymer-based ionic thermoelectric(i-TE)materials are promising candidates for energy conversion systems because of their wide sources,innocuity,and low manufacturing cost.However,common physically crosslinked biopolymer gels induced by single hydrogen bonding or hydrophobic interaction suffer from low differential thermal voltage and poor thermodynamic stability.Here,we develop a novel i-TE gel with supramolecular structures through multiple noncovalent interactions between ionic liquids(ILs)and gelatin molecular chains.The thermopower and thermoelectric power factor of the ionic gels are as high as 2.83 mV K-1 and 18.33μW m^(-1)K^(-2),respectively.The quasi-solid-state gelatin-[EMIM]DCA i-TE cells achieve ultrahigh 2 h output energy density(E_(2h)=9.9 mJ m^(-2))under an optimal temperature range.Meanwhile,the remarkable stability of the supramolecular structure provides the i-TE hydrogels with a thermal stability of up to 80℃.It breaks the limitation that biopolymer-based i-TE gels can only be applied in the low temperature range and enables biopolymer-based i-TE materials to pursue better performance in a higher temperature range.
基金supported by the Guangdong Basic and Applied Basic Research Foundation(2021B1515120072)the Natural Science Foundation of China(22279096 and T2241003)the Fundamental Research Funds for the Central Universities(WUT:2023IVA094).
文摘Water electrolysis poses a significant challenge for balancing catalytic activity and stability of oxygen evolution reaction(OER)electrocatalysts.In this study,we address this challenge by constructing asymmetric redox chemistry through elaborate surface OO–Ru–OH and bulk Ru–O–Ni/Fe coordination moieties within single-atom Ru-decorated defective NiFe LDH nanosheets(Ru@d-NiFe LDH)in conjunction with strong metal-support interactions(SMSI).Rigorous spectroscopic characterization and theoretical calculations indicate that single-atom Ru can delocalize the O 2p electrons on the surface and optimize d-electron configurations of metal atoms in bulk through SMSI.The^(18)O isotope labeling experiment based on operando differential electrochemical mass spectrometry(DEMS),chemical probe experiments,and theoretical calculations confirm the encouraged surface lattice oxygen,stabilized bulk lattice oxygen,and enhanced adsorption of oxygen-containing intermediates for bulk metals in Ru@d-NiFe LDH,leading to asymmetric redox chemistry for OER.The Ru@d-NiFe LDH electrocatalyst exhibits exceptional performance with an overpotential of 230 mV to achieve 10 mA cm^(−2)and maintains high robustness under industrial current density.This approach for achieving asymmetric redox chemistry through SMSI presents a new avenue for developing high-performance electrocatalysts and instills confidence in its industrial applicability.
基金financial support from Project funded by National Natural Science Foundation of China(52172038,22179017)funding from Dalian University of Technology Open Fund for Large Scale Instrument Equipment
文摘Metal-organic framework(MOF)-derived carbon composites have been considered as the promising materials for energy storage.However,the construction of MOF-based composites with highly controllable mode via the liquid-liquid synthesis method has a great challenge because of the simultaneous heterogeneous nucleation on substrates and the self-nucleation of individual MOF nanocrystals in the liquid phase.Herein,we report a bidirectional electrostatic generated self-assembly strategy to achieve the precisely controlled coatings of single-layer nanoscale MOFs on a range of substrates,including carbon nanotubes(CNTs),graphene oxide(GO),MXene,layered double hydroxides(LDHs),MOFs,and SiO_(2).The obtained MOF-based nanostructured carbon composite exhibits the hierarchical porosity(V_(meso)/V_(micro)∶2.4),ultrahigh N content of 12.4 at.%and"dual electrical conductive networks."The assembled aqueous zinc-ion hybrid capacitor(ZIC)with the prepared nanocarbon composite as a cathode shows a high specific capacitance of 236 F g^(-1)at 0.5 A g^(-1),great rate performance of 98 F g^(-1)at 100 A g^(-1),and especially,an ultralong cycling stability up to 230000 cycles with the capacitance retention of 90.1%.This work develops a repeatable and general method for the controlled construction of MOF coatings on various functional substrates and further fabricates carbon composites for ZICs with ultrastability.
基金supported by National Science Foundation of China(42102059 and 92055202)the China Geological Survey(DD20221817 and DD20190057)+1 种基金the basic scientific research funding in CAGS(J2204)the Second Tibetan Plateau Scientific Expedition and Research(2019QZKK0702).
文摘Two suites of mafic dykes,T1193-A and T1194-A,outcrop in Gyangze area,southeast Tibet.They are in the area of Comei LIP and have indistinguishable field occurrences with two other dykes in Gyangze,T0902 dyke with 137.7±1.3 Ma zircon age and T0907 dyke with 142±1.4 Ma zircon age reported by Wang YY et al.(2016),indicating coeval formation time.Taking all the four diabase dykes into consideration,two different types,OIB-type and weak enriched-type,can be summarized.The“OIB-type”samples,including T1193-A and T0907 dykes,show OIB-like geochemical features and have initial Sr-Nd isotopic values similar with most mafic products in Comei Large Igneous Provinces(LIP),suggesting that they represent melts directly generated from the Kerguelen mantle plume.The“weak enriched-type”samples,including T1194-A and T0902 dykes,have REEs and trace element patterns showing withinplate affinity but have obvious Nb-Ta-Ti negative anomalies.They show uniform lowerεNd(t)values(−6‒−2)and higher 87Sr/86Sr(t)values(0.706‒0.709)independent of their MgO variation,indicating one enriched mantle source.Considering their closely spatial and temporal relationship with the widespread Comei LIP magmatic products in Tethyan Himalaya,these“weak enriched-type”samples are consistent with mixing of melts from mantle plume and the above ancient Tethyan Himalaya subcontinental lithospheric mantle(SCLM)in different proportions.These weak enriched mafic rocks in Comei LIP form one special rock group and most likely suggest large scale hot mantle plume-continental lithosphere interaction.This process may lead to strong modification of the Tethyan Himalaya lithosphere in the Early Cretaceous.
