High-pressure(HP)or ultrahigh-pressure(UHP)rutile-quartz veins that form at mantle depths due to fluid-rock interaction can be used to trace the properties and behavior of natural fluids in subduction zones.To explore...High-pressure(HP)or ultrahigh-pressure(UHP)rutile-quartz veins that form at mantle depths due to fluid-rock interaction can be used to trace the properties and behavior of natural fluids in subduction zones.To explore the fluid flow and the associated element mobility during deep subduction and exhumation of the continental crust,we investigated the major and trace elements of Ti-rich minerals.Additionally,U–Pb dating,trace element contents,and Lu–Hf isotopic composition of zircon grains in the UHP eclogite and associated rutile-quartz veins were examined in the North Qaidam UHP metamorphic belt,Yuka terrane.The zircon grains in the rutile-quartz veins have unzoned or weak oscillatory zonings,and show low Th/U ratios,steep chondrite-normalized patterns of heavy rare earth elements(HREEs),and insignificant negative Eu anomalies,indicating their growth in metamorphic fluids.These zircon grains formed in 4313 Ma,which is consistent with the 4322 Ma age of the host eclogite.As for the zircons in the rutile-quartz veins,they showed steep HREE patterns on one hand,and were different from the zircons present in the host eclogite on the other.This demonstrates that their formation might have been related to the breakdown of the early stage of garnet,which corresponds to the abundance of fluids during the early exhumation stage.The core-rim profile analyses of rutile recorded a two-stage rutile growth across a large rutile grain;the rutile core has higher Nb,Ta,W,and Zr contents and lower Nb/Ta ratios than the rim,indicating that the rutile domains grew in different metamorphic fluids from the core towards the rim.The significant enrichment of high field strength elements(HFSEs)in the rutile core suggests that the peak fluids have high solubility and transportation capacity of these HFSEs.Furthermore,variations in the Nb vs.Cr trends in rutile indicate a connection of rutile to mafic protolith.The zircon grains from both the rutile-quartz veins and the host eclogite have similar Hf isotopic compositions,indicating that the vein-forming fluids are internally derived from the host eclogite.These fluids accumulated in the subduction channel and were triggered by local dehydration of the deeply subducted eclogite during the early exhumation conditions.展开更多
As demonstrated by a great amount of geologic and experimental evidences, RE of rock systems may be mobilized during fluid-rock interaction when solutions are rich in F -, Cl -, CO 3 2-, HCO 3 -, CO 2, HPO 4...As demonstrated by a great amount of geologic and experimental evidences, RE of rock systems may be mobilized during fluid-rock interaction when solutions are rich in F -, Cl -, CO 3 2-, HCO 3 -, CO 2, HPO 4 2-, HS -, S 2-, SO 4 2-, though little has been known about the mobilizing mechanism of these anions or ligands. The fractionation of RE resulted from hydrothermal alterations, i. e., fluid-rock interactions, are distinctive. One set of field data implies the preferential mobility of the LRE, while another set of field observations demonstrates the dominant mobilization of the HRE, and some theoretical prediction is not consistent with the field evidence. The Eu anomalies caused by fluid-rock interaction are complex and compelling explanation is not available due to inadequate experimental approaches. To know the exact behavior of RE during fluid-rock interaction and to solve the contradiction between some theoretical predictions and field observations, the following works remain to be done: (1) experimental investigations of RE mobility and fractionation as a function of fluid chemistry, e.g., the activity of F -, Cl -, CO 3 2-, HCO 3 -, CO 2, HPO 4 2-, HS -, S 2-, SO 4 2-, etc.; (2) experimental determination of RE mobility and fractionation as a function of T, P, pH, E h and water/rock ratios; (3) investigation of the mechanism and the controlling factors of RE partitioning between hydrothermal minerals and fluids. It was demonstrated that RE mobility is a potentially useful method for exploration.展开更多
The Koyna region of Maharashtra located in the western part of the~65 Myr old Deccan traps province,overlying the Neoarchean cratonic granitoid basement of peninsular India,has been experiencing recurring seismicity s...The Koyna region of Maharashtra located in the western part of the~65 Myr old Deccan traps province,overlying the Neoarchean cratonic granitoid basement of peninsular India,has been experiencing recurring seismicity since 1962 after the impoundment of the Shivajisagar Reservoir behind the Koyna Dam.展开更多
Rare earths in ores, altered and unaltered sericite phyllite, altered and unaltered dacite porphyry were determined in order to examine behaviors of rare earths in hydrothermal alteration associating with ore-forming ...Rare earths in ores, altered and unaltered sericite phyllite, altered and unaltered dacite porphyry were determined in order to examine behaviors of rare earths in hydrothermal alteration associating with ore-forming processes of Yinshan deposit. It is not sufficient to show the mobility only by the absolute abundance of trace elements changes before and after alteration. This can simply result from dilution or concentration if other elements are added to or removed from the rock. As shown by that in Yinshan deposit, less than 20% of the increment of RE was caused by the 'condensed' of leaching some of major elements (e.g. Si, Na) from the rock. The principal factor which should be responsible for the higher contents of RE in altered rock is the addition of RE into the rock by hydrothermal fluids. Eu is selectively leached from the altered sericite phyllite by a mild acidity and reducing fluid which is characterized by much lower LRE/HRE ratio and a large positive Eu anomaly. A major effect on the RE patterns is the tendency to develop relatively flatter chondrite-normalized patterns. The RE characteristics may be used to distinguish between small and large ore bodies at a later stage of exploration.展开更多
Recently,many researchers have focused on the usage of electromagnetic waves in oil production and well stimulation,but so far the effect of these waves on the fluid and rock interaction and its simultaneous effect wi...Recently,many researchers have focused on the usage of electromagnetic waves in oil production and well stimulation,but so far the effect of these waves on the fluid and rock interaction and its simultaneous effect with nanoparticles have not been investigated.Fluid-rock interaction is one of the most important factors affecting fluid distribution in the reservoirs.In this study,the oil reservoir rock wettability alteration under electromagnetic heating and the presence of nanoparticles has been investigated.Three nanoparticles of TiO_2,Fe_(3)O_(4),and TiO_2/Fe_(3)O_(4)have been utilized.TiO_2 nanoparticles are commercially available,and the other mentioned nanoparticles are synthesized via a co-precipitation method.Citric acid has been used to modify surfaces of nanoparticles and stabilize them in water as the base fluid.Also,the adsorption of the nanoparticles on the rock surface has been determined.In the next step,the amount of oil outflow from the rock has been measured and reported as the external fluid imbibition.In this process,the nanoparticle performance in wettability alteration was investigated using pH and inductively coupled plasma(ICP)analyses.To better understand the governing mechanisms,oil viscosity was measured by mixing the oil with nanoparticles and put under irradiation.The results reveal that the microwave has a great ability to reduce oil contact angle with carbonate rock.In the presence of0.2 wt%Fe_(3)O_(4)nanoparticles,the contact angle was reduced from 155°to 19°after 28 min of irradiation,indicating strong rock hydrophilicity.Furthermore,microwave irradiation on Fe_(3)O_(4)nanofluid extracts75%of the oil from the rock.With microwave radiation,the pH of the nanofluid increases and hence,more nanoparticles are adsorbed on the rock which subsequently causes more rock dissolution.The viscosity change results prove that there is an optimal irradiation time of 5 min in which oil viscosity reduces from 481 cP to 410 cP and then increases to 827 cP.Moreover,the application of further nanoparticles diminishes the oil viscosity at optimum irradiation time in which Fe_(3)O_(4)has the most oil viscosity reduction,representing 481 cP to 200 cP at 50%microwave power level.展开更多
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
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
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
Hydrogen and oxygen isotope studies were carried out on mineral separates from high to ultrahigh pressure metamorphic rocks at Huangzhen and Shuanghe in the eastern Dabie Mountains, East China. The δ18O values of ecl...Hydrogen and oxygen isotope studies were carried out on mineral separates from high to ultrahigh pressure metamorphic rocks at Huangzhen and Shuanghe in the eastern Dabie Mountains, East China. The δ18O values of eclogites cover a wide range of ?5‰ to+9‰, but the δD values of micas fall within a narrow range of ?85% to ?70‰. Both equilibrium and disequilibrium oxygen isotope fractionations were observed between quartz and the other minerals, with reversed fractionations between omphacite and garnet in some eclogite samples. The δ18 O values of ?5‰ to ?1‰ for some of the eclogites represent the oxygen isotope compositions of their protoliths which underwent meteoric water-rock interaction prior to plate subduction. The preservation of oxygen isotope heterogeneity in the eclogites implies a channelized flow of fluids during progressive metamorphism caused by rapid subduction. Retrograde metamorphism has caused oxygen and hydrogen isotope disequilibria between some of the minerals, but the fluid for retrograde reactions was internally buffered in the stable isotope compositions.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
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
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
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
基金funded by the Fundamental Research Funds for National Universities, China University of Geosciences (Wuhan) and China Geological Survey (Grant Nos. 12120113032800, 21201011000150004, DD20190069)
文摘High-pressure(HP)or ultrahigh-pressure(UHP)rutile-quartz veins that form at mantle depths due to fluid-rock interaction can be used to trace the properties and behavior of natural fluids in subduction zones.To explore the fluid flow and the associated element mobility during deep subduction and exhumation of the continental crust,we investigated the major and trace elements of Ti-rich minerals.Additionally,U–Pb dating,trace element contents,and Lu–Hf isotopic composition of zircon grains in the UHP eclogite and associated rutile-quartz veins were examined in the North Qaidam UHP metamorphic belt,Yuka terrane.The zircon grains in the rutile-quartz veins have unzoned or weak oscillatory zonings,and show low Th/U ratios,steep chondrite-normalized patterns of heavy rare earth elements(HREEs),and insignificant negative Eu anomalies,indicating their growth in metamorphic fluids.These zircon grains formed in 4313 Ma,which is consistent with the 4322 Ma age of the host eclogite.As for the zircons in the rutile-quartz veins,they showed steep HREE patterns on one hand,and were different from the zircons present in the host eclogite on the other.This demonstrates that their formation might have been related to the breakdown of the early stage of garnet,which corresponds to the abundance of fluids during the early exhumation stage.The core-rim profile analyses of rutile recorded a two-stage rutile growth across a large rutile grain;the rutile core has higher Nb,Ta,W,and Zr contents and lower Nb/Ta ratios than the rim,indicating that the rutile domains grew in different metamorphic fluids from the core towards the rim.The significant enrichment of high field strength elements(HFSEs)in the rutile core suggests that the peak fluids have high solubility and transportation capacity of these HFSEs.Furthermore,variations in the Nb vs.Cr trends in rutile indicate a connection of rutile to mafic protolith.The zircon grains from both the rutile-quartz veins and the host eclogite have similar Hf isotopic compositions,indicating that the vein-forming fluids are internally derived from the host eclogite.These fluids accumulated in the subduction channel and were triggered by local dehydration of the deeply subducted eclogite during the early exhumation conditions.
文摘As demonstrated by a great amount of geologic and experimental evidences, RE of rock systems may be mobilized during fluid-rock interaction when solutions are rich in F -, Cl -, CO 3 2-, HCO 3 -, CO 2, HPO 4 2-, HS -, S 2-, SO 4 2-, though little has been known about the mobilizing mechanism of these anions or ligands. The fractionation of RE resulted from hydrothermal alterations, i. e., fluid-rock interactions, are distinctive. One set of field data implies the preferential mobility of the LRE, while another set of field observations demonstrates the dominant mobilization of the HRE, and some theoretical prediction is not consistent with the field evidence. The Eu anomalies caused by fluid-rock interaction are complex and compelling explanation is not available due to inadequate experimental approaches. To know the exact behavior of RE during fluid-rock interaction and to solve the contradiction between some theoretical predictions and field observations, the following works remain to be done: (1) experimental investigations of RE mobility and fractionation as a function of fluid chemistry, e.g., the activity of F -, Cl -, CO 3 2-, HCO 3 -, CO 2, HPO 4 2-, HS -, S 2-, SO 4 2-, etc.; (2) experimental determination of RE mobility and fractionation as a function of T, P, pH, E h and water/rock ratios; (3) investigation of the mechanism and the controlling factors of RE partitioning between hydrothermal minerals and fluids. It was demonstrated that RE mobility is a potentially useful method for exploration.
基金conducted under the project sponsored by the Ministry of Earth Sciences,Govt.of India[Project Code-Mo ES/P.O.(Seismo)/1(374)/2019]
文摘The Koyna region of Maharashtra located in the western part of the~65 Myr old Deccan traps province,overlying the Neoarchean cratonic granitoid basement of peninsular India,has been experiencing recurring seismicity since 1962 after the impoundment of the Shivajisagar Reservoir behind the Koyna Dam.
文摘Rare earths in ores, altered and unaltered sericite phyllite, altered and unaltered dacite porphyry were determined in order to examine behaviors of rare earths in hydrothermal alteration associating with ore-forming processes of Yinshan deposit. It is not sufficient to show the mobility only by the absolute abundance of trace elements changes before and after alteration. This can simply result from dilution or concentration if other elements are added to or removed from the rock. As shown by that in Yinshan deposit, less than 20% of the increment of RE was caused by the 'condensed' of leaching some of major elements (e.g. Si, Na) from the rock. The principal factor which should be responsible for the higher contents of RE in altered rock is the addition of RE into the rock by hydrothermal fluids. Eu is selectively leached from the altered sericite phyllite by a mild acidity and reducing fluid which is characterized by much lower LRE/HRE ratio and a large positive Eu anomaly. A major effect on the RE patterns is the tendency to develop relatively flatter chondrite-normalized patterns. The RE characteristics may be used to distinguish between small and large ore bodies at a later stage of exploration.
基金the National Iranian South Oil Company(NISOC)for their financial support。
文摘Recently,many researchers have focused on the usage of electromagnetic waves in oil production and well stimulation,but so far the effect of these waves on the fluid and rock interaction and its simultaneous effect with nanoparticles have not been investigated.Fluid-rock interaction is one of the most important factors affecting fluid distribution in the reservoirs.In this study,the oil reservoir rock wettability alteration under electromagnetic heating and the presence of nanoparticles has been investigated.Three nanoparticles of TiO_2,Fe_(3)O_(4),and TiO_2/Fe_(3)O_(4)have been utilized.TiO_2 nanoparticles are commercially available,and the other mentioned nanoparticles are synthesized via a co-precipitation method.Citric acid has been used to modify surfaces of nanoparticles and stabilize them in water as the base fluid.Also,the adsorption of the nanoparticles on the rock surface has been determined.In the next step,the amount of oil outflow from the rock has been measured and reported as the external fluid imbibition.In this process,the nanoparticle performance in wettability alteration was investigated using pH and inductively coupled plasma(ICP)analyses.To better understand the governing mechanisms,oil viscosity was measured by mixing the oil with nanoparticles and put under irradiation.The results reveal that the microwave has a great ability to reduce oil contact angle with carbonate rock.In the presence of0.2 wt%Fe_(3)O_(4)nanoparticles,the contact angle was reduced from 155°to 19°after 28 min of irradiation,indicating strong rock hydrophilicity.Furthermore,microwave irradiation on Fe_(3)O_(4)nanofluid extracts75%of the oil from the rock.With microwave radiation,the pH of the nanofluid increases and hence,more nanoparticles are adsorbed on the rock which subsequently causes more rock dissolution.The viscosity change results prove that there is an optimal irradiation time of 5 min in which oil viscosity reduces from 481 cP to 410 cP and then increases to 827 cP.Moreover,the application of further nanoparticles diminishes the oil viscosity at optimum irradiation time in which Fe_(3)O_(4)has the most oil viscosity reduction,representing 481 cP to 200 cP at 50%microwave power level.
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.
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.
基金Project supported by the Chinese Ministry of Science and Technology (Grant No. 95-Pre-39)the National Natural Science Foundation of China (Grant Nos. 49794042, 49473173 and 49453003)the Chinese Academy of Sciences (Grant No. KZ951-A1-401-5).
文摘Hydrogen and oxygen isotope studies were carried out on mineral separates from high to ultrahigh pressure metamorphic rocks at Huangzhen and Shuanghe in the eastern Dabie Mountains, East China. The δ18O values of eclogites cover a wide range of ?5‰ to+9‰, but the δD values of micas fall within a narrow range of ?85% to ?70‰. Both equilibrium and disequilibrium oxygen isotope fractionations were observed between quartz and the other minerals, with reversed fractionations between omphacite and garnet in some eclogite samples. The δ18 O values of ?5‰ to ?1‰ for some of the eclogites represent the oxygen isotope compositions of their protoliths which underwent meteoric water-rock interaction prior to plate subduction. The preservation of oxygen isotope heterogeneity in the eclogites implies a channelized flow of fluids during progressive metamorphism caused by rapid subduction. Retrograde metamorphism has caused oxygen and hydrogen isotope disequilibria between some of the minerals, but the fluid for retrograde reactions was internally buffered in the stable isotope compositions.
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.