N-doping has significant influence in manipulating the properties of TiO_(2),and this has stimulated the development of N-donor-functionalized titanium-oxo clusters(TOCs)as molecular models to study the structure-prop...N-doping has significant influence in manipulating the properties of TiO_(2),and this has stimulated the development of N-donor-functionalized titanium-oxo clusters(TOCs)as molecular models to study the structure-property relationship.However,the structural type and photoresponsive application are still limited for such TOCs,especially regarding the high-nuclearity TOCs that contain structure unit of TiO_(2)for photocatalysis.Herein,we showed the synthesis of a series of high-nuclearity TOCs 1-3 compounds usingπ-conjugated 1,10-phenanthroline(phen)as chromophore and N-donor functional ligand.Compound 1 features cocrystal structure composed of one[Ti_(26)]~(2+)and half[Ti_(22)]~(2+),which renders it as the first cocrystallized TOC containing two positively charged species and phen-functionalized TOC showing the highest nuclearity up to 37 Ti centers.By adjusting the synthetic conditions,the individual{Ti_(22)}and{Ti_(26)}clusters can also be isolated as Compounds 2 and 3,respectively.The core structure of{Ti_(22)}is mainly constructed from four lacunary{Ti_(4)}derived from pentagonal{Ti(Ti)_5}unit,while{Ti_(26)}is built from four complete{Ti(Ti)_5}unit.Notably,a{Ti_8O_(14)}structure unit of anatase TiO_(2)can be identified in{Ti_(26)}.Based on the unique structural features and proper photophysical and photochemical properties of Compounds 1-3,they are applied for photocatalytic sulfoxidation.Owing to the presence of anatase structure unit in{Ti_(26)}and the synergistic effect from{Ti_(22)}and{Ti_(26)},the catalytic performance presents in the order of Compound 1>Compound 3>Compound 2.This work provides excellent models to understand the structureproperty relationship from the perspective of cocrystallization and Ti-O binding model and will further promote the application of TOCs as functional catalysts for organic transformation.展开更多
Photoactive functionalized titanium-oxo clusters(TOCs)are regarded as an important model compound for dye-sensitized titanium dioxide solar cells.However,the dyes used for sensitizing TOCs are still limited.Herein,two...Photoactive functionalized titanium-oxo clusters(TOCs)are regarded as an important model compound for dye-sensitized titanium dioxide solar cells.However,the dyes used for sensitizing TOCs are still limited.Herein,two cyclic TOCs are reported,namely,[Ti_(6)(μ_(3)-O)_(2)(Oi-Pr)_(8))(LA)_(2)]·i-PrOH(S1)and[Ti_(6)(μ_(3)-O)2(Oi-Pr)_(8))(LV)_(2)]·i-PrOH(S2),which are functionalized by photoactive naphthalene diimide(NDI)chromophores.Their molecular structures and photophysical and photochemical properties were systematically studied.As shown by ultraviolet-visible(UV-vis)spectra and photocurrent study results,the band gap and the photocurrent response of S1 and S2 were derived from NDI ligands which extend the absorption edge of S1 and S2 approaching 500 nm and afford high photocurrent densities of 2.12μA/cm^(2)and 1.95μA/cm^(2)for S1 and S2,respectively,demonstrating the significance of the photoactive ligand in modulating photoresponse of TOCs.This work is expected to enrich the structural library of photoactive TOCs and provide insights into understanding the structure-property relationships of sensitized clusters.展开更多
Supramolecular transformations of coordination cage or capsule have received much attention recently,which help elucidate this natural self-assembly behavior in biological systems.The current study describes the first...Supramolecular transformations of coordination cage or capsule have received much attention recently,which help elucidate this natural self-assembly behavior in biological systems.The current study describes the first supramolecular transformation of titanium-o rganic coordination capsule triggered by phenol(and H_(3) PO_(3)).The structural alterations are accompanied by the reconstruction of 5-coordinated Ti centers to 6-coordinated ones.Meanwhile,different amounts of encapsulated phenol vip molecules can be identified,dependent on the sizes of the obtained cavities.In addition,they display much better visible light absorption and air stability than the isopropanol stabilized ones.展开更多
The synthesis of titanium oxo clusters(TOCs)with both chirality and photoactivity is urgently needed to expand their applications.However,this remains a significant challenge due to synthetic difficulties and limitati...The synthesis of titanium oxo clusters(TOCs)with both chirality and photoactivity is urgently needed to expand their applications.However,this remains a significant challenge due to synthetic difficulties and limitations in chiral ligand selection.In this work,we have isolated two pairs of enantiomeric TOCs,[Ti_(3)(μ_(3)-O)(R/S-L1)_(2)(^(i)PrO)_(6)](R/S-Ti_(3);^(i)PrOH=isopropanol,R/S-L1=R/S-2'-hydroxy-[1,1'-binaphthalen]-2-yl isopropyl hydrogenphosphate)and[Ti_(4)(μ_(2)-O)(μ_(4)-O)(R/S-L2)_(2)(EtO)_(8)](R/S-Ti4;EtOH=ethanol,R/S-L2=R/S-2'-hydroxy-[1,1'-binaphthalen]-2-yl ethyl hydrogenphosphate),via an in situ ligand transformation approach.The R/S-L1 and R/S-L2 ligands were obtained by alcoholysis of R/S-L(R/S-1,1'-binaphthyl-2,2'-diyl hydrogenphosphate)in different reaction solvents.These ligands,with additional coordination sites,facilitated the formation of novel TOCs and improved their stability.Importantly,these clusters exhibited exceptional stability in solid state and maintained appreciable stability in solution.Furthermore,the introduction of chiral ligands not only imparts a homochiral nature to R/S-Ti3 and R/S-Ti4 but also confers upon them superior photoelectric properties due to ligand-to-metal charge transfer(LMCT)phenomena,as confirmed by theoretical calculations.This study offers a valuable synthetic strategy for preparing photoactive chiral TOCs,and we anticipate it will inspire new discoveries in the field of chiral metal nanoclusters.展开更多
Titanium-based materials have emerged as promising candidates for photo-Fenton-like catalysis,whereas their structural complexities impede precise understanding of the relevant structure–activity relationships.Owing ...Titanium-based materials have emerged as promising candidates for photo-Fenton-like catalysis,whereas their structural complexities impede precise understanding of the relevant structure–activity relationships.Owing to their well-defined and tunable structures,titaniumoxo clusters appear to be facile models for looking into the photophysical and photochemical processes in Ti-H_(2)O_(2) systems.Using PTC-3 as a prototype,we interrogated the relationship between Ti-site coordination environments and photo-Fenton-like behaviors.Through integrated in-situ/exsitu spectroscopic analyses and theoretical simulations,we elucidated light-driven H_(2)O_(2) activation on hexa-coordinated and penta-coordinated Ti sites in PTC-3.The superiority of penta-coordinated Ti site was identified,where extended visible-light absorption and promoted electron transfer could synergistically boost the activation of H_(2)O_(2) into superoxide radicals.This work brightens the role of Ti-site coordination geometry in photo-Fenton-like processes and paves the way for pursuing titanium-based advanced oxidation.展开更多
Under hydrothermal and solvothermal conditions,two novel cobalt-based complexes,{[Co_(2)(CIA)(OH)(1,4-dtb)]·3.2H_(2)O}n(HU23)and{[Co_(2)(CIA)(OH)(1,4-dib)]·3.5H2O·DMF}n(HU24),were successfully construct...Under hydrothermal and solvothermal conditions,two novel cobalt-based complexes,{[Co_(2)(CIA)(OH)(1,4-dtb)]·3.2H_(2)O}n(HU23)and{[Co_(2)(CIA)(OH)(1,4-dib)]·3.5H2O·DMF}n(HU24),were successfully constructed by coordinatively assembling the semi-rigid multidentate ligand 5-(1-carboxyethoxy)isophthalic acid(H₃CIA)with the Nheterocyclic ligands 1,4-di(4H-1,2,4-triazol-4-yl)benzene(1,4-dtb)and 1,4-di(1H-imidazol-1-yl)benzene(1,4-dib),respectively,around Co^(2+)ions.Single-crystal X-ray diffraction analysis revealed that in both complexes HU23 and HU24,the CIA^(3-)anions adopt aκ^(7)-coordination mode,bridging six Co^(2+)ions via their five carboxylate oxygen atoms and one ether oxygen atom.This linkage forms tetranuclear[Co4(μ3-OH)2]^(6+)units.These Co-oxo cluster units were interconnected by CIA^(3-)anions to assemble into 2D kgd-type structures featuring a 3,6-connected topology.The 2D layers were further connected by 1,4-dtb and 1,4-dib,resulting in 3D pillar-layered frameworks for HU23 and HU24.Notably,despite the similar configurations of 1,4-dtb and 1,4-dib,differences in their coordination spatial orientations lead to topological divergence in the 3D frameworks of HU23 and HU24.Topological analysis indicates that the frameworks of HU23 and HU24 can be simplified into a 3,10-connected net(point symbol:(4^(10).6^(3).8^(2))(4^(3))_(2))and a 3,8-connected tfz-d net(point symbol:(4^(3))_(2)((4^(6).6^(18).8^(4)))),respectively.This structural differentiation confirms the precise regulatory role of ligands on the topology of metal-organic frameworks.Moreover,the ultraviolet-visible absorption spectra confirmed that HU23 and HU24 have strong absorption capabilities for ultraviolet and visible light.According to the Kubelka-Munk method,their bandwidths were 2.15 and 2.08 eV,respectively,which are consistent with those of typical semiconductor materials.Variable-temperature magnetic susceptibility measurements(2-300 K)revealed significant antiferromagnetic coupling in both complexes,with their effective magnetic moments decreasing markedly as the temperature lowered.CCDC:2457554,HU23;2457553,HU24.展开更多
This paper proposes an equivalent modeling method for photovoltaic(PV)power stations via a particle swarm optimization(PSO)K-means clustering(KMC)algorithm with passive filter parameter clustering to address the compl...This paper proposes an equivalent modeling method for photovoltaic(PV)power stations via a particle swarm optimization(PSO)K-means clustering(KMC)algorithm with passive filter parameter clustering to address the complexities,simulation time cost and convergence problems of detailed PV power station models.First,the amplitude–frequency curves of different filter parameters are analyzed.Based on the results,a grouping parameter set for characterizing the external filter characteristics is established.These parameters are further defined as clustering parameters.A single PV inverter model is then established as a prerequisite foundation.The proposed equivalent method combines the global search capability of PSO with the rapid convergence of KMC,effectively overcoming the tendency of KMC to become trapped in local optima.This approach enhances both clustering accuracy and numerical stability when determining equivalence for PV inverter units.Using the proposed clustering method,both a detailed PV power station model and an equivalent model are developed and compared.Simulation and hardwarein-loop(HIL)results based on the equivalent model verify that the equivalent method accurately represents the dynamic characteristics of PVpower stations and adapts well to different operating conditions.The proposed equivalent modeling method provides an effective analysis tool for future renewable energy integration research.展开更多
Compared with nanoparticle-aspect relatives titanium dioxide(TiO2),titanium-oxo clusters(TOCs)are atomically structural-determined and can be further precisely modified through coordination and supramolecular chemistr...Compared with nanoparticle-aspect relatives titanium dioxide(TiO2),titanium-oxo clusters(TOCs)are atomically structural-determined and can be further precisely modified through coordination and supramolecular chemistry.Another parallel research direction is titanium-based metal-organic frameworks,and those based on TOC have attracted particular attention because of their high optical performances resulting from the cluster aggregation effect.Though challenging,assembling macro-materials from specific clusters helps establish the assembly chemistry of clusters and incorporates porous andflexible characteristics into a single bulk material.Although separate reviews are reported in these two branches,no com-prehensive review is available to highlight the bridges between them.Herein,we review and summarize the development and progress of new aggregation of TOCs,from intramolecular unique cluster aggregation to hierarchical intermolecular aggre-gation via covalent forces,coordination bonds,and non-covalent forces using the specific clusters as precursors.We hope this reviewfills the gap in the methodology of assembling particular-aggregated TOCs and their derived frameworks,providing general guidance to researchers interested in this area.展开更多
Molecular solid solutions of metal clusters containing different metal centers with well-defined structures can accurately regulate the HOMO-LUMO gap,but are rarely available.Herein,a series of colorless lanthanide-ti...Molecular solid solutions of metal clusters containing different metal centers with well-defined structures can accurately regulate the HOMO-LUMO gap,but are rarely available.Herein,a series of colorless lanthanide-titanium-oxo clusters Ln_(2)Ti_4(μ_(2)-O)_(2)(μ_(3)-O)_4(Piv)_(10)(THF)_(2)(Ln_(2)Ti_4,Ln = Eu,Gd,Tb,and Ce,HPiv = pivalic acid) were synthesized by the reaction of pivalic acid with Ln(Ac)_(3) and titanium isopropoxide.The light yellow crystal of cluster solid solutions Eu_(2)Ti_(4-x)Cd_(x),containing a mixture of Eu_(2)Ti_4 and Eu_(2)Ti_(3)Cd,was obtained by in situ doping Cd^(2+) and S^(2–).Eu_(2)Ti_(3.92)Cd_(0.08) displays efficient photocatalytic hydrogen evolution activity without a co-catalyst,which is up to 2.6 times that of Eu_(2)Ti_4.Femtosecond time-resolved transient absorption spectroscopy and spin-polarized density functional calculations showed that the enhanced photocatalytic performance of Eu_(2)Ti_(4-x)Cd_(x) can be attributed to the narrower HOMO-LUMO gap and lower LUMO position than that of Eu_(2)Ti_4.This studyprovides an in situ doping method to realize the simple preparation of cluster solid solution.展开更多
Subject Code:B01 Photocatalytic hydrogen evolution by water-splitting has been recognized as one of the most promising solutions to the global energy and environment crisis,owing to its renewable solar energy source a...Subject Code:B01 Photocatalytic hydrogen evolution by water-splitting has been recognized as one of the most promising solutions to the global energy and environment crisis,owing to its renewable solar energy source and clean chemical fuel product.Cadmium sulfide(CdS)and TiO2(or related polyoxo-titanium clusters)are two展开更多
Perovskite and organic solar cells usually require electron-transport interlayers to efficiently transport electrons from the photoactive layer to the metal electrode.In general,pure organic or inorganic materials are...Perovskite and organic solar cells usually require electron-transport interlayers to efficiently transport electrons from the photoactive layer to the metal electrode.In general,pure organic or inorganic materials are applied into the interlayers,but organic–inorganic hybrid materials have been rarely reported for this application.In this work,we report using the first titanium-oxo cluster-based organic–inorganic hybrid as the interlayer material by introducing largeπ-conjugated benzo[ghi]perylenetriimides as an organic part via a simple ligand-exchange reaction.This new hybrid material showed excellent solubility,well-aligned energy levels,and excellent electron mobilities,enabling its great potential application as an interlayer in solar cells such as perovskite and organic solar cells,providing high power conversion efficiencies of>20%and 16%,respectively.Therefore,we claim that our present work introduces a new class of cluster-based organic–inorganic hybrid interlayer materials that exhibit promising application in organic electronics.展开更多
Multi-view clustering is a critical research area in computer science aimed at effectively extracting meaningful patterns from complex,high-dimensional data that single-view methods cannot capture.Traditional fuzzy cl...Multi-view clustering is a critical research area in computer science aimed at effectively extracting meaningful patterns from complex,high-dimensional data that single-view methods cannot capture.Traditional fuzzy clustering techniques,such as Fuzzy C-Means(FCM),face significant challenges in handling uncertainty and the dependencies between different views.To overcome these limitations,we introduce a new multi-view fuzzy clustering approach that integrates picture fuzzy sets with a dual-anchor graph method for multi-view data,aiming to enhance clustering accuracy and robustness,termed Multi-view Picture Fuzzy Clustering(MPFC).In particular,the picture fuzzy set theory extends the capability to represent uncertainty by modeling three membership levels:membership degrees,neutral degrees,and refusal degrees.This allows for a more flexible representation of uncertain and conflicting data than traditional fuzzy models.Meanwhile,dual-anchor graphs exploit the similarity relationships between data points and integrate information across views.This combination improves stability,scalability,and robustness when handling noisy and heterogeneous data.Experimental results on several benchmark datasets demonstrate significant improvements in clustering accuracy and efficiency,outperforming traditional methods.Specifically,the MPFC algorithm demonstrates outstanding clustering performance on a variety of datasets,attaining a Purity(PUR)score of 0.6440 and an Accuracy(ACC)score of 0.6213 for the 3 Sources dataset,underscoring its robustness and efficiency.The proposed approach significantly contributes to fields such as pattern recognition,multi-view relational data analysis,and large-scale clustering problems.Future work will focus on extending the method for semi-supervised multi-view clustering,aiming to enhance adaptability,scalability,and performance in real-world applications.展开更多
Federated learning is a machine learning framework designed to protect privacy by keeping training data on clients’devices without sharing private data.It trains a global model through collaboration between clients a...Federated learning is a machine learning framework designed to protect privacy by keeping training data on clients’devices without sharing private data.It trains a global model through collaboration between clients and the server.However,the presence of data heterogeneity can lead to inefficient model training and even reduce the final model’s accuracy and generalization capability.Meanwhile,data scarcity can result in suboptimal cluster distributions for few-shot clients in centralized clustering tasks,and standalone personalization tasks may cause severe overfitting issues.To address these limitations,we introduce a federated learning dual optimization model based on clustering and personalization strategy(FedCPS).FedCPS adopts a decentralized approach,where clients identify their cluster membership locally without relying on a centralized clustering algorithm.Building on this,FedCPS introduces personalized training tasks locally,adding a regularization term to control deviations between local and cluster models.This improves the generalization ability of the final model while mitigating overfitting.The use of weight-sharing techniques also reduces the computational cost of central machines.Experimental results on MNIST,FMNIST,CIFAR10,and CIFAR100 datasets demonstrate that our method achieves better personalization effects compared to other personalized federated learning methods,with an average test accuracy improvement of 0.81%–2.96%.Meanwhile,we adjusted the proportion of few-shot clients to evaluate the impact on accuracy across different methods.The experiments show that FedCPS reduces accuracy by only 0.2%–3.7%,compared to 2.1%–10%for existing methods.Our method demonstrates its advantages across diverse data environments.展开更多
Many fields,such as neuroscience,are experiencing the vast prolife ration of cellular data,underscoring the need fo r organizing and interpreting large datasets.A popular approach partitions data into manageable subse...Many fields,such as neuroscience,are experiencing the vast prolife ration of cellular data,underscoring the need fo r organizing and interpreting large datasets.A popular approach partitions data into manageable subsets via hierarchical clustering,but objective methods to determine the appropriate classification granularity are missing.We recently introduced a technique to systematically identify when to stop subdividing clusters based on the fundamental principle that cells must differ more between than within clusters.Here we present the corresponding protocol to classify cellular datasets by combining datadriven unsupervised hierarchical clustering with statistical testing.These general-purpose functions are applicable to any cellular dataset that can be organized as two-dimensional matrices of numerical values,including molecula r,physiological,and anatomical datasets.We demonstrate the protocol using cellular data from the Janelia MouseLight project to chara cterize morphological aspects of neurons.展开更多
The pursuit of Ag-based alloys with both high strength and toughness has posed a longstanding chal-lenge.In this study,we investigated the cluster strengthening and grain refinement toughening mecha-nisms in fully oxi...The pursuit of Ag-based alloys with both high strength and toughness has posed a longstanding chal-lenge.In this study,we investigated the cluster strengthening and grain refinement toughening mecha-nisms in fully oxidized AgMgNi alloys,which were internally oxidized at 800℃ for 8 h under an oxy-gen atmosphere.We found that Mg-O clusters contributed to the hardening(138 HV)and strengthening(376.9 MPa)of the AgMg alloy through solid solution strengthening effects,albeit at the expense of duc-tility.To address this limitation,we introduced Ni nanoparticles into the AgMg alloy,resulting in signifi-cant grain refinement within its microstructure.Specifically,the grain size decreased from 67.2μm in the oxidized AgMg alloy to below 6.0μm in the oxidized AgMgNi alloy containing 0.3 wt%Ni.Consequently,the toughness increased significantly,rising from toughness value of 2177.9 MJ m^(-3) in the oxidized AgMg alloy to 6186.1 MJ m^(-3) in the oxidized AgMgNi alloy,representing a remarkable 2.8-fold enhancement.Furthermore,the internally oxidized AgMgNi alloy attained a strength of up to 387.6 MPa,comparable to that of the internally oxidized AgMg alloy,thereby demonstrating the successful realization of concurrent strengthening and toughening.These results collectively offer a novel approach for the design of high-performance alloys through the synergistic combination of cluster strengthening and grain refinement toughening.展开更多
Given customizable crystal structure and intriguing optical properties,lanthanide titanium-oxygen clusters(LTOCs)with atomic-level accuracy have gained a lot of interest.In this study,we prepared[Ln_(9)Ti_(2)(μ4-O)(...Given customizable crystal structure and intriguing optical properties,lanthanide titanium-oxygen clusters(LTOCs)with atomic-level accuracy have gained a lot of interest.In this study,we prepared[Ln_(9)Ti_(2)(μ4-O)(μ3-OH)_(14)(acac)_(17)(CH_(3)O)_(2)(CH_(3)OH)_(3)](Ln=Tb_(x)Eu_(9−x)(x=0,4,6,7,8,9),Hacac=acetylacetone),Tb^(3+)and Eu^(3+)co-doped LTOCs,to modify the optical properties for the luminescence thermometer.In detail,the serial LTOCs display dual characteristic emission peaks of ^(5)D_(4)→^(7)F_(5) for Tb^(3+)and^(5)D_(0)→^(7)F_(2) for Eu^(3+)at 548 and 616 nm,respectively,under 330 nm excitation.Effective energy transfer(ET)between Tb^(3+)ions and Eu^(3+)ions was revealed in terms of both emission spectra and luminescence lifetime.The ^(5)D_(0)→^(7)F_(2) emission intensity of Eu^(3+)ions at 616 nm is maximally enhanced(by a factor of 11.2)with a change in the relative molar ratio of Tb^(3+)to Eu^(3+),along with a change in the ET efficiency of Tb^(3+)→Eu^(3+).In addition,the luminescent color changes from red,orange,yellow,to green.This precise control of the ET process between rare-earth ions allows{Tb_(6)Eu_(3)Ti_(2)}to reach a maximum relative sensitivity of 1.241 K^(−1) at 355 K,which is an enhancement of up to 4.6-fold with respect to the previously reported homonuclear emission,holding great potential in the optical thermometers.展开更多
Objectives To identify core symptoms and symptom clusters in patients with neuromyelitis optica spectrum disorder(NMOSD)by network analysis.Methods From October 10 to 30,2023,140 patients with NMOSD were selected to p...Objectives To identify core symptoms and symptom clusters in patients with neuromyelitis optica spectrum disorder(NMOSD)by network analysis.Methods From October 10 to 30,2023,140 patients with NMOSD were selected to participate in this online questionnaire survey.The survey tools included a general information questionnaire and a self-made NMOSD symptoms scale,which included the prevalence,severity,and distress of 29 symptoms.Cluster analysis was used to identify symptom clusters,and network analysis was used to analyze the symptom network and node characteristics and central indicators including strength centrality(r_(s)),closeness centrality(r_(c))and betweeness centrality(r_(b))were used to identify core symptoms and symptom clusters.Results The most common symptom was pain(65.7%),followed by paraesthesia(65.0%),fatigue(65.0%),easy awakening(63.6%).Regarding the burden level of symptoms,pain was the most burdensome symptom,followed by paraesthesia,easy awakening,fatigue,and difficulty falling asleep.Six clusters were identified:somatosensory,motor,visual,and memory symptom clusters,bladder and rectum symptom clusters,sleep symptoms clusters,and neuropsychological symptom clusters.Fatigue(r_(s)=12.39,r_(b)=68.00,r_(c)=0.02)was the most central and prominent bridge symptom,and motor symptom cluster(r_(s)=2.68,r_(c)=0.10)was the most central symptom cluster among the six clusters.Conclusions Our study demonstrated the necessity of symptom management targeting fatigue,pain,and motor symptom cluster in patients with NMOSD.展开更多
By systematically reviewing the development status of global carbon dioxide capture,utilization and storage(CCUS)cluster,and comparing domestic and international CCUS industrial models and successful experiences,this ...By systematically reviewing the development status of global carbon dioxide capture,utilization and storage(CCUS)cluster,and comparing domestic and international CCUS industrial models and successful experiences,this study explores the challenges and strategies for the scaled development of the CCUS industry of China.Globally,the CCUS industry has entered a phase of scaled and clustered development.North America has established a system of key technologies in large-scale CO_(2) capture,long-distance pipeline transmission,pipeline network optimization,and large-scale CO_(2) flooding for enhanced oil recovery(CO_(2)-EOR),with relatively mature cluster development and a gradual shift in industrial model from CO_(2)-EOR to geological storage.The CCUS industry of China has developed rapidly across all segments but remains in the early stage of cluster development,facing challenges such as absent business model,insufficient policy support,and technological gaps in core areas.China needs to improve the policy support system to boost enterprises participation across the entire industrial chain,strengthen top-level design and medium-to long-term planning to accelerate demonstration projects construction for whole-process CCUS clusters,advance for a full-chain technological system,including low-cost capture,pipeline optimization and EOR/storage integration technologies,and strengthen personnel training,strengthen discipline construction and university-enterprise research cooperation.展开更多
Thermally activated delayed fluorescence(TADF)materials driven by a through-space charge transfer(TSCT)mechanism have garnered wide interest.However,access of TSCT-TADF molecules with longwavelength emission remains a...Thermally activated delayed fluorescence(TADF)materials driven by a through-space charge transfer(TSCT)mechanism have garnered wide interest.However,access of TSCT-TADF molecules with longwavelength emission remains a formidable challenge.In this study,we introduce a novel V-type DA-D-A’emitter,Trz-mCzCbCz,by using a carborane scaffold.This design strategically incorporates carbazole(Cz)and 2,4,6-triphenyl-1,3,5-triazine(Trz)as donor and acceptor moieties,respectively.Theoretical calculations alongside experimental validations affirm the typical TSCT-TADF characteristics of this luminogen.Owing to the unique structural and electronic attributes of carboranes,Trz-mCzCbCz exhibits an orange-red emission,markedly diverging from the traditional blue-to-green emissions observed in classical Cz and Trz-based TADF molecules.Moreover,bright emission in aggregates was observed for Trz-mCzCbCz with absolute photoluminescence quantum yield(PLQY)of up to 88.8%.As such,we have successfully fabricated five organic light-emitting diodes(OLEDs)by utilizing Trz-mCzCbCz as the emitting layer.It is important to note that both the reverse intersystem crossing process and the TADF properties are profoundly influenced by host materials.The fabricated OLED devices reached a maximum external quantum efficiency(EQE)of 12.7%,with an emission peak at 592 nm.This represents the highest recorded efficiency for TSCT-TADF OLEDs employing carborane derivatives as emitting layers.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.21901037,21901038 and 92161111)the Program for Professor of Special Appointment(Eastern Scholar)at Shanghai Institutions of Higher Learning+1 种基金the Fundamental Research Funds for the Central Universities(No.2232019G-07)the International Cooperation Fund of Science and Technology Commission of Shanghai Municipality(No.21130750100)。
文摘N-doping has significant influence in manipulating the properties of TiO_(2),and this has stimulated the development of N-donor-functionalized titanium-oxo clusters(TOCs)as molecular models to study the structure-property relationship.However,the structural type and photoresponsive application are still limited for such TOCs,especially regarding the high-nuclearity TOCs that contain structure unit of TiO_(2)for photocatalysis.Herein,we showed the synthesis of a series of high-nuclearity TOCs 1-3 compounds usingπ-conjugated 1,10-phenanthroline(phen)as chromophore and N-donor functional ligand.Compound 1 features cocrystal structure composed of one[Ti_(26)]~(2+)and half[Ti_(22)]~(2+),which renders it as the first cocrystallized TOC containing two positively charged species and phen-functionalized TOC showing the highest nuclearity up to 37 Ti centers.By adjusting the synthetic conditions,the individual{Ti_(22)}and{Ti_(26)}clusters can also be isolated as Compounds 2 and 3,respectively.The core structure of{Ti_(22)}is mainly constructed from four lacunary{Ti_(4)}derived from pentagonal{Ti(Ti)_5}unit,while{Ti_(26)}is built from four complete{Ti(Ti)_5}unit.Notably,a{Ti_8O_(14)}structure unit of anatase TiO_(2)can be identified in{Ti_(26)}.Based on the unique structural features and proper photophysical and photochemical properties of Compounds 1-3,they are applied for photocatalytic sulfoxidation.Owing to the presence of anatase structure unit in{Ti_(26)}and the synergistic effect from{Ti_(22)}and{Ti_(26)},the catalytic performance presents in the order of Compound 1>Compound 3>Compound 2.This work provides excellent models to understand the structureproperty relationship from the perspective of cocrystallization and Ti-O binding model and will further promote the application of TOCs as functional catalysts for organic transformation.
基金National Natural Science Foundation of China(Nos.92161111,21901037 and 21901038)。
文摘Photoactive functionalized titanium-oxo clusters(TOCs)are regarded as an important model compound for dye-sensitized titanium dioxide solar cells.However,the dyes used for sensitizing TOCs are still limited.Herein,two cyclic TOCs are reported,namely,[Ti_(6)(μ_(3)-O)_(2)(Oi-Pr)_(8))(LA)_(2)]·i-PrOH(S1)and[Ti_(6)(μ_(3)-O)2(Oi-Pr)_(8))(LV)_(2)]·i-PrOH(S2),which are functionalized by photoactive naphthalene diimide(NDI)chromophores.Their molecular structures and photophysical and photochemical properties were systematically studied.As shown by ultraviolet-visible(UV-vis)spectra and photocurrent study results,the band gap and the photocurrent response of S1 and S2 were derived from NDI ligands which extend the absorption edge of S1 and S2 approaching 500 nm and afford high photocurrent densities of 2.12μA/cm^(2)and 1.95μA/cm^(2)for S1 and S2,respectively,demonstrating the significance of the photoactive ligand in modulating photoresponse of TOCs.This work is expected to enrich the structural library of photoactive TOCs and provide insights into understanding the structure-property relationships of sensitized clusters.
基金supported by the National Natural Science Foundation of China (NSFC,No.21922111)the Strategic Priority Research Program of the Chinese Academy of Sciences (No.XDB20000000)。
文摘Supramolecular transformations of coordination cage or capsule have received much attention recently,which help elucidate this natural self-assembly behavior in biological systems.The current study describes the first supramolecular transformation of titanium-o rganic coordination capsule triggered by phenol(and H_(3) PO_(3)).The structural alterations are accompanied by the reconstruction of 5-coordinated Ti centers to 6-coordinated ones.Meanwhile,different amounts of encapsulated phenol vip molecules can be identified,dependent on the sizes of the obtained cavities.In addition,they display much better visible light absorption and air stability than the isopropanol stabilized ones.
基金financially supported by the National Natural Science Foundation of China(Grant Nos.22325105,22201159,22171164,91961105,92361301,and 52261135637)the Natural Science Foundation of Shandong Province(Nos.ZR2021QB077 and ZR2024MB120)the Doctoral Program of Liaocheng University(No.318051944).
文摘The synthesis of titanium oxo clusters(TOCs)with both chirality and photoactivity is urgently needed to expand their applications.However,this remains a significant challenge due to synthetic difficulties and limitations in chiral ligand selection.In this work,we have isolated two pairs of enantiomeric TOCs,[Ti_(3)(μ_(3)-O)(R/S-L1)_(2)(^(i)PrO)_(6)](R/S-Ti_(3);^(i)PrOH=isopropanol,R/S-L1=R/S-2'-hydroxy-[1,1'-binaphthalen]-2-yl isopropyl hydrogenphosphate)and[Ti_(4)(μ_(2)-O)(μ_(4)-O)(R/S-L2)_(2)(EtO)_(8)](R/S-Ti4;EtOH=ethanol,R/S-L2=R/S-2'-hydroxy-[1,1'-binaphthalen]-2-yl ethyl hydrogenphosphate),via an in situ ligand transformation approach.The R/S-L1 and R/S-L2 ligands were obtained by alcoholysis of R/S-L(R/S-1,1'-binaphthyl-2,2'-diyl hydrogenphosphate)in different reaction solvents.These ligands,with additional coordination sites,facilitated the formation of novel TOCs and improved their stability.Importantly,these clusters exhibited exceptional stability in solid state and maintained appreciable stability in solution.Furthermore,the introduction of chiral ligands not only imparts a homochiral nature to R/S-Ti3 and R/S-Ti4 but also confers upon them superior photoelectric properties due to ligand-to-metal charge transfer(LMCT)phenomena,as confirmed by theoretical calculations.This study offers a valuable synthetic strategy for preparing photoactive chiral TOCs,and we anticipate it will inspire new discoveries in the field of chiral metal nanoclusters.
基金supported by the National Key R&D Program of China(Nos.2022YFA1502903 and 2021YFA1501502)the National Natural Science Foundation of China(Nos.22275179 and 92477116).
文摘Titanium-based materials have emerged as promising candidates for photo-Fenton-like catalysis,whereas their structural complexities impede precise understanding of the relevant structure–activity relationships.Owing to their well-defined and tunable structures,titaniumoxo clusters appear to be facile models for looking into the photophysical and photochemical processes in Ti-H_(2)O_(2) systems.Using PTC-3 as a prototype,we interrogated the relationship between Ti-site coordination environments and photo-Fenton-like behaviors.Through integrated in-situ/exsitu spectroscopic analyses and theoretical simulations,we elucidated light-driven H_(2)O_(2) activation on hexa-coordinated and penta-coordinated Ti sites in PTC-3.The superiority of penta-coordinated Ti site was identified,where extended visible-light absorption and promoted electron transfer could synergistically boost the activation of H_(2)O_(2) into superoxide radicals.This work brightens the role of Ti-site coordination geometry in photo-Fenton-like processes and paves the way for pursuing titanium-based advanced oxidation.
文摘Under hydrothermal and solvothermal conditions,two novel cobalt-based complexes,{[Co_(2)(CIA)(OH)(1,4-dtb)]·3.2H_(2)O}n(HU23)and{[Co_(2)(CIA)(OH)(1,4-dib)]·3.5H2O·DMF}n(HU24),were successfully constructed by coordinatively assembling the semi-rigid multidentate ligand 5-(1-carboxyethoxy)isophthalic acid(H₃CIA)with the Nheterocyclic ligands 1,4-di(4H-1,2,4-triazol-4-yl)benzene(1,4-dtb)and 1,4-di(1H-imidazol-1-yl)benzene(1,4-dib),respectively,around Co^(2+)ions.Single-crystal X-ray diffraction analysis revealed that in both complexes HU23 and HU24,the CIA^(3-)anions adopt aκ^(7)-coordination mode,bridging six Co^(2+)ions via their five carboxylate oxygen atoms and one ether oxygen atom.This linkage forms tetranuclear[Co4(μ3-OH)2]^(6+)units.These Co-oxo cluster units were interconnected by CIA^(3-)anions to assemble into 2D kgd-type structures featuring a 3,6-connected topology.The 2D layers were further connected by 1,4-dtb and 1,4-dib,resulting in 3D pillar-layered frameworks for HU23 and HU24.Notably,despite the similar configurations of 1,4-dtb and 1,4-dib,differences in their coordination spatial orientations lead to topological divergence in the 3D frameworks of HU23 and HU24.Topological analysis indicates that the frameworks of HU23 and HU24 can be simplified into a 3,10-connected net(point symbol:(4^(10).6^(3).8^(2))(4^(3))_(2))and a 3,8-connected tfz-d net(point symbol:(4^(3))_(2)((4^(6).6^(18).8^(4)))),respectively.This structural differentiation confirms the precise regulatory role of ligands on the topology of metal-organic frameworks.Moreover,the ultraviolet-visible absorption spectra confirmed that HU23 and HU24 have strong absorption capabilities for ultraviolet and visible light.According to the Kubelka-Munk method,their bandwidths were 2.15 and 2.08 eV,respectively,which are consistent with those of typical semiconductor materials.Variable-temperature magnetic susceptibility measurements(2-300 K)revealed significant antiferromagnetic coupling in both complexes,with their effective magnetic moments decreasing markedly as the temperature lowered.CCDC:2457554,HU23;2457553,HU24.
基金supported by the Research Project of China Southern Power Grid(No.056200KK52222031).
文摘This paper proposes an equivalent modeling method for photovoltaic(PV)power stations via a particle swarm optimization(PSO)K-means clustering(KMC)algorithm with passive filter parameter clustering to address the complexities,simulation time cost and convergence problems of detailed PV power station models.First,the amplitude–frequency curves of different filter parameters are analyzed.Based on the results,a grouping parameter set for characterizing the external filter characteristics is established.These parameters are further defined as clustering parameters.A single PV inverter model is then established as a prerequisite foundation.The proposed equivalent method combines the global search capability of PSO with the rapid convergence of KMC,effectively overcoming the tendency of KMC to become trapped in local optima.This approach enhances both clustering accuracy and numerical stability when determining equivalence for PV inverter units.Using the proposed clustering method,both a detailed PV power station model and an equivalent model are developed and compared.Simulation and hardwarein-loop(HIL)results based on the equivalent model verify that the equivalent method accurately represents the dynamic characteristics of PVpower stations and adapts well to different operating conditions.The proposed equivalent modeling method provides an effective analysis tool for future renewable energy integration research.
基金National Natural Science Foundation of China,Grant/Award Numbers:U23A2095,22371278,92061104Science Fund for Distinguished Young Scholars of Fujian Province,Grant/Award Number:2021J06035+1 种基金Funding of Fujian Provincial Chemistry Discipline Alliance,Grant/Award Number:50025401Youth Innovation Promotion Association of the Chinese Academy of Sciences,Grant/Award Number:Y2021081。
文摘Compared with nanoparticle-aspect relatives titanium dioxide(TiO2),titanium-oxo clusters(TOCs)are atomically structural-determined and can be further precisely modified through coordination and supramolecular chemistry.Another parallel research direction is titanium-based metal-organic frameworks,and those based on TOC have attracted particular attention because of their high optical performances resulting from the cluster aggregation effect.Though challenging,assembling macro-materials from specific clusters helps establish the assembly chemistry of clusters and incorporates porous andflexible characteristics into a single bulk material.Although separate reviews are reported in these two branches,no com-prehensive review is available to highlight the bridges between them.Herein,we review and summarize the development and progress of new aggregation of TOCs,from intramolecular unique cluster aggregation to hierarchical intermolecular aggre-gation via covalent forces,coordination bonds,and non-covalent forces using the specific clusters as precursors.We hope this reviewfills the gap in the methodology of assembling particular-aggregated TOCs and their derived frameworks,providing general guidance to researchers interested in this area.
基金supported by the National Natural Science Foundation of China (21871224,92161104,92161203,21721001)。
文摘Molecular solid solutions of metal clusters containing different metal centers with well-defined structures can accurately regulate the HOMO-LUMO gap,but are rarely available.Herein,a series of colorless lanthanide-titanium-oxo clusters Ln_(2)Ti_4(μ_(2)-O)_(2)(μ_(3)-O)_4(Piv)_(10)(THF)_(2)(Ln_(2)Ti_4,Ln = Eu,Gd,Tb,and Ce,HPiv = pivalic acid) were synthesized by the reaction of pivalic acid with Ln(Ac)_(3) and titanium isopropoxide.The light yellow crystal of cluster solid solutions Eu_(2)Ti_(4-x)Cd_(x),containing a mixture of Eu_(2)Ti_4 and Eu_(2)Ti_(3)Cd,was obtained by in situ doping Cd^(2+) and S^(2–).Eu_(2)Ti_(3.92)Cd_(0.08) displays efficient photocatalytic hydrogen evolution activity without a co-catalyst,which is up to 2.6 times that of Eu_(2)Ti_4.Femtosecond time-resolved transient absorption spectroscopy and spin-polarized density functional calculations showed that the enhanced photocatalytic performance of Eu_(2)Ti_(4-x)Cd_(x) can be attributed to the narrower HOMO-LUMO gap and lower LUMO position than that of Eu_(2)Ti_4.This studyprovides an in situ doping method to realize the simple preparation of cluster solid solution.
文摘Subject Code:B01 Photocatalytic hydrogen evolution by water-splitting has been recognized as one of the most promising solutions to the global energy and environment crisis,owing to its renewable solar energy source and clean chemical fuel product.Cadmium sulfide(CdS)and TiO2(or related polyoxo-titanium clusters)are two
基金supported by MOST(nos.2018YFA0208504 and 2017YFA0204702)NSFC(51773207,52073016,5197030531,and 21801213)of China+2 种基金The Fundamental Research Funds for the Central Universities further supported this work(no.XK1802-2)Open Project of State Key Laboratory of Supramolecular Structure and Materials(no.sklssm202043)Jiangxi Provincial Department of Science and Technology(nos.20192ACB20009,20192BBEL50026,20202ACBL213004,and 20203BBE53062).
文摘Perovskite and organic solar cells usually require electron-transport interlayers to efficiently transport electrons from the photoactive layer to the metal electrode.In general,pure organic or inorganic materials are applied into the interlayers,but organic–inorganic hybrid materials have been rarely reported for this application.In this work,we report using the first titanium-oxo cluster-based organic–inorganic hybrid as the interlayer material by introducing largeπ-conjugated benzo[ghi]perylenetriimides as an organic part via a simple ligand-exchange reaction.This new hybrid material showed excellent solubility,well-aligned energy levels,and excellent electron mobilities,enabling its great potential application as an interlayer in solar cells such as perovskite and organic solar cells,providing high power conversion efficiencies of>20%and 16%,respectively.Therefore,we claim that our present work introduces a new class of cluster-based organic–inorganic hybrid interlayer materials that exhibit promising application in organic electronics.
基金funded by the Research Project:THTETN.05/24-25,VietnamAcademy of Science and Technology.
文摘Multi-view clustering is a critical research area in computer science aimed at effectively extracting meaningful patterns from complex,high-dimensional data that single-view methods cannot capture.Traditional fuzzy clustering techniques,such as Fuzzy C-Means(FCM),face significant challenges in handling uncertainty and the dependencies between different views.To overcome these limitations,we introduce a new multi-view fuzzy clustering approach that integrates picture fuzzy sets with a dual-anchor graph method for multi-view data,aiming to enhance clustering accuracy and robustness,termed Multi-view Picture Fuzzy Clustering(MPFC).In particular,the picture fuzzy set theory extends the capability to represent uncertainty by modeling three membership levels:membership degrees,neutral degrees,and refusal degrees.This allows for a more flexible representation of uncertain and conflicting data than traditional fuzzy models.Meanwhile,dual-anchor graphs exploit the similarity relationships between data points and integrate information across views.This combination improves stability,scalability,and robustness when handling noisy and heterogeneous data.Experimental results on several benchmark datasets demonstrate significant improvements in clustering accuracy and efficiency,outperforming traditional methods.Specifically,the MPFC algorithm demonstrates outstanding clustering performance on a variety of datasets,attaining a Purity(PUR)score of 0.6440 and an Accuracy(ACC)score of 0.6213 for the 3 Sources dataset,underscoring its robustness and efficiency.The proposed approach significantly contributes to fields such as pattern recognition,multi-view relational data analysis,and large-scale clustering problems.Future work will focus on extending the method for semi-supervised multi-view clustering,aiming to enhance adaptability,scalability,and performance in real-world applications.
基金supported by the Foundation of President of Hebei University(XZJJ202303).
文摘Federated learning is a machine learning framework designed to protect privacy by keeping training data on clients’devices without sharing private data.It trains a global model through collaboration between clients and the server.However,the presence of data heterogeneity can lead to inefficient model training and even reduce the final model’s accuracy and generalization capability.Meanwhile,data scarcity can result in suboptimal cluster distributions for few-shot clients in centralized clustering tasks,and standalone personalization tasks may cause severe overfitting issues.To address these limitations,we introduce a federated learning dual optimization model based on clustering and personalization strategy(FedCPS).FedCPS adopts a decentralized approach,where clients identify their cluster membership locally without relying on a centralized clustering algorithm.Building on this,FedCPS introduces personalized training tasks locally,adding a regularization term to control deviations between local and cluster models.This improves the generalization ability of the final model while mitigating overfitting.The use of weight-sharing techniques also reduces the computational cost of central machines.Experimental results on MNIST,FMNIST,CIFAR10,and CIFAR100 datasets demonstrate that our method achieves better personalization effects compared to other personalized federated learning methods,with an average test accuracy improvement of 0.81%–2.96%.Meanwhile,we adjusted the proportion of few-shot clients to evaluate the impact on accuracy across different methods.The experiments show that FedCPS reduces accuracy by only 0.2%–3.7%,compared to 2.1%–10%for existing methods.Our method demonstrates its advantages across diverse data environments.
基金supported in part by NIH grants R01NS39600,U01MH114829RF1MH128693(to GAA)。
文摘Many fields,such as neuroscience,are experiencing the vast prolife ration of cellular data,underscoring the need fo r organizing and interpreting large datasets.A popular approach partitions data into manageable subsets via hierarchical clustering,but objective methods to determine the appropriate classification granularity are missing.We recently introduced a technique to systematically identify when to stop subdividing clusters based on the fundamental principle that cells must differ more between than within clusters.Here we present the corresponding protocol to classify cellular datasets by combining datadriven unsupervised hierarchical clustering with statistical testing.These general-purpose functions are applicable to any cellular dataset that can be organized as two-dimensional matrices of numerical values,including molecula r,physiological,and anatomical datasets.We demonstrate the protocol using cellular data from the Janelia MouseLight project to chara cterize morphological aspects of neurons.
基金supported by the National Natural Science Foundation of China(Nos.51977027 and 51967008)the Scientific and Technological Project of Yunnan Precious Metals Lab-oratory(Nos.YPML-2023050250 and YPML-2022050206).
文摘The pursuit of Ag-based alloys with both high strength and toughness has posed a longstanding chal-lenge.In this study,we investigated the cluster strengthening and grain refinement toughening mecha-nisms in fully oxidized AgMgNi alloys,which were internally oxidized at 800℃ for 8 h under an oxy-gen atmosphere.We found that Mg-O clusters contributed to the hardening(138 HV)and strengthening(376.9 MPa)of the AgMg alloy through solid solution strengthening effects,albeit at the expense of duc-tility.To address this limitation,we introduced Ni nanoparticles into the AgMg alloy,resulting in signifi-cant grain refinement within its microstructure.Specifically,the grain size decreased from 67.2μm in the oxidized AgMg alloy to below 6.0μm in the oxidized AgMgNi alloy containing 0.3 wt%Ni.Consequently,the toughness increased significantly,rising from toughness value of 2177.9 MJ m^(-3) in the oxidized AgMg alloy to 6186.1 MJ m^(-3) in the oxidized AgMgNi alloy,representing a remarkable 2.8-fold enhancement.Furthermore,the internally oxidized AgMgNi alloy attained a strength of up to 387.6 MPa,comparable to that of the internally oxidized AgMg alloy,thereby demonstrating the successful realization of concurrent strengthening and toughening.These results collectively offer a novel approach for the design of high-performance alloys through the synergistic combination of cluster strengthening and grain refinement toughening.
基金supported by the National Natural Science Foundation of China(Nos.12174151 and 12304448)the Specific Research Fund of the Innovation Platform for Academicians of Hainan Province(No.YSPTZX202208)+3 种基金Hainan Province Clinical Medical Center(No.QWYH_(2)022341)the Key Laboratory of New Energy and Rare Earth Resource Utilization of the State People’s Committee of China(No.NERE202206)the Department of Science and Technology of Jilin Province(No.20220101059JC)the Key Laboratory of the Ministry of Education for First Aid and Trauma Research(No.KLET-202218).
文摘Given customizable crystal structure and intriguing optical properties,lanthanide titanium-oxygen clusters(LTOCs)with atomic-level accuracy have gained a lot of interest.In this study,we prepared[Ln_(9)Ti_(2)(μ4-O)(μ3-OH)_(14)(acac)_(17)(CH_(3)O)_(2)(CH_(3)OH)_(3)](Ln=Tb_(x)Eu_(9−x)(x=0,4,6,7,8,9),Hacac=acetylacetone),Tb^(3+)and Eu^(3+)co-doped LTOCs,to modify the optical properties for the luminescence thermometer.In detail,the serial LTOCs display dual characteristic emission peaks of ^(5)D_(4)→^(7)F_(5) for Tb^(3+)and^(5)D_(0)→^(7)F_(2) for Eu^(3+)at 548 and 616 nm,respectively,under 330 nm excitation.Effective energy transfer(ET)between Tb^(3+)ions and Eu^(3+)ions was revealed in terms of both emission spectra and luminescence lifetime.The ^(5)D_(0)→^(7)F_(2) emission intensity of Eu^(3+)ions at 616 nm is maximally enhanced(by a factor of 11.2)with a change in the relative molar ratio of Tb^(3+)to Eu^(3+),along with a change in the ET efficiency of Tb^(3+)→Eu^(3+).In addition,the luminescent color changes from red,orange,yellow,to green.This precise control of the ET process between rare-earth ions allows{Tb_(6)Eu_(3)Ti_(2)}to reach a maximum relative sensitivity of 1.241 K^(−1) at 355 K,which is an enhancement of up to 4.6-fold with respect to the previously reported homonuclear emission,holding great potential in the optical thermometers.
基金supported by the Specific Research Fund for Top-notch Talents of Guangdong Provincial Hospital of Chinese Medicine(No.2022KT1188).
文摘Objectives To identify core symptoms and symptom clusters in patients with neuromyelitis optica spectrum disorder(NMOSD)by network analysis.Methods From October 10 to 30,2023,140 patients with NMOSD were selected to participate in this online questionnaire survey.The survey tools included a general information questionnaire and a self-made NMOSD symptoms scale,which included the prevalence,severity,and distress of 29 symptoms.Cluster analysis was used to identify symptom clusters,and network analysis was used to analyze the symptom network and node characteristics and central indicators including strength centrality(r_(s)),closeness centrality(r_(c))and betweeness centrality(r_(b))were used to identify core symptoms and symptom clusters.Results The most common symptom was pain(65.7%),followed by paraesthesia(65.0%),fatigue(65.0%),easy awakening(63.6%).Regarding the burden level of symptoms,pain was the most burdensome symptom,followed by paraesthesia,easy awakening,fatigue,and difficulty falling asleep.Six clusters were identified:somatosensory,motor,visual,and memory symptom clusters,bladder and rectum symptom clusters,sleep symptoms clusters,and neuropsychological symptom clusters.Fatigue(r_(s)=12.39,r_(b)=68.00,r_(c)=0.02)was the most central and prominent bridge symptom,and motor symptom cluster(r_(s)=2.68,r_(c)=0.10)was the most central symptom cluster among the six clusters.Conclusions Our study demonstrated the necessity of symptom management targeting fatigue,pain,and motor symptom cluster in patients with NMOSD.
基金Supported by the PetroChina Science and Technology Major Project(2021ZZ01-05)Hainan Merit-based Recruitment Project(ZDYF2024SHFZ147)National Natural Science Foundation of China(NNSC)Project(52474033)。
文摘By systematically reviewing the development status of global carbon dioxide capture,utilization and storage(CCUS)cluster,and comparing domestic and international CCUS industrial models and successful experiences,this study explores the challenges and strategies for the scaled development of the CCUS industry of China.Globally,the CCUS industry has entered a phase of scaled and clustered development.North America has established a system of key technologies in large-scale CO_(2) capture,long-distance pipeline transmission,pipeline network optimization,and large-scale CO_(2) flooding for enhanced oil recovery(CO_(2)-EOR),with relatively mature cluster development and a gradual shift in industrial model from CO_(2)-EOR to geological storage.The CCUS industry of China has developed rapidly across all segments but remains in the early stage of cluster development,facing challenges such as absent business model,insufficient policy support,and technological gaps in core areas.China needs to improve the policy support system to boost enterprises participation across the entire industrial chain,strengthen top-level design and medium-to long-term planning to accelerate demonstration projects construction for whole-process CCUS clusters,advance for a full-chain technological system,including low-cost capture,pipeline optimization and EOR/storage integration technologies,and strengthen personnel training,strengthen discipline construction and university-enterprise research cooperation.
基金supported by the Natural Science Foundation of Jiangsu Province(No.BZ2022007)the National Natural Science Foundation of China(No.92261202)+1 种基金the Ministry of Science and Technology of the People’s Republic of China(No.2021YFE0114800)the Ministry of Science and Higher Education of the Russian Federation(No.075-15-2021-1027).
文摘Thermally activated delayed fluorescence(TADF)materials driven by a through-space charge transfer(TSCT)mechanism have garnered wide interest.However,access of TSCT-TADF molecules with longwavelength emission remains a formidable challenge.In this study,we introduce a novel V-type DA-D-A’emitter,Trz-mCzCbCz,by using a carborane scaffold.This design strategically incorporates carbazole(Cz)and 2,4,6-triphenyl-1,3,5-triazine(Trz)as donor and acceptor moieties,respectively.Theoretical calculations alongside experimental validations affirm the typical TSCT-TADF characteristics of this luminogen.Owing to the unique structural and electronic attributes of carboranes,Trz-mCzCbCz exhibits an orange-red emission,markedly diverging from the traditional blue-to-green emissions observed in classical Cz and Trz-based TADF molecules.Moreover,bright emission in aggregates was observed for Trz-mCzCbCz with absolute photoluminescence quantum yield(PLQY)of up to 88.8%.As such,we have successfully fabricated five organic light-emitting diodes(OLEDs)by utilizing Trz-mCzCbCz as the emitting layer.It is important to note that both the reverse intersystem crossing process and the TADF properties are profoundly influenced by host materials.The fabricated OLED devices reached a maximum external quantum efficiency(EQE)of 12.7%,with an emission peak at 592 nm.This represents the highest recorded efficiency for TSCT-TADF OLEDs employing carborane derivatives as emitting layers.
