The increase in anthropogenic carbon dioxide(CO_(2))emissions has exacerbated the deterioration of the global environment,which should be controlled to achieve carbon neutrality.Central to the core goal of achieving c...The increase in anthropogenic carbon dioxide(CO_(2))emissions has exacerbated the deterioration of the global environment,which should be controlled to achieve carbon neutrality.Central to the core goal of achieving carbon neutrality is the utilization of CO_(2) under economic and sustainable conditions.Recently,the strong need for carbon neutrality has led to a proliferation of studies on the direct conversion of CO_(2) into carboxylic acids,which can effectively alleviate CO_(2) emissions and create high-value chemicals.The purpose of this review is to present the application prospects of carboxylic acids and the basic principles of CO_(2) conversion into carboxylic acids through photo-,electric-,and thermal catalysis.Special attention is focused on the regulation strategy of the activity of abundant catalysts at the molecular level,inspiring the preparation of high-performance catalysts.In addition,theoretical calculations,advanced technologies,and numerous typical examples are introduced to elaborate on the corresponding process and influencing factors of catalytic activity.Finally,challenges and prospects are provided for the future development of this field.It is hoped that this review will contribute to a deeper understanding of the conversion of CO_(2) into carboxylic acids and inspire more innovative breakthroughs.展开更多
Distraction spinal cord injury is caused by some degree of distraction or longitudinal tension on the spinal cord and commonly occurs in patients who undergo corrective operation for severe spinal deformity.With the i...Distraction spinal cord injury is caused by some degree of distraction or longitudinal tension on the spinal cord and commonly occurs in patients who undergo corrective operation for severe spinal deformity.With the increased degree and duration of distraction,spinal cord injuries become more serious in terms of their neurophysiology,histology,and behavior.Very few studies have been published on the specific characteristics of distraction spinal cord injury.In this study,we systematically review 22 related studies involving animal models of distraction spinal cord injury,focusing particularly on the neurophysiological,histological,and behavioral characteristics of this disease.In addition,we summarize the mechanisms underlying primary and secondary injuries caused by distraction spinal cord injury and clarify the effects of different degrees and durations of distraction on the primary injuries associated with spinal cord injury.We provide new concepts for the establishment of a model of distraction spinal cord injury and related basic research,and provide reference guidelines for the clinical diagnosis and treatment of this disease.展开更多
Chilled chicken is inevitably contaminated by microorganisms during slaughtering and processing,resulting in spoilage.Cutting parts of chilled chicken,especially wings,feet,and other skin-on products,are abundant in c...Chilled chicken is inevitably contaminated by microorganisms during slaughtering and processing,resulting in spoilage.Cutting parts of chilled chicken,especially wings,feet,and other skin-on products,are abundant in collagen,which may be the primary target for degradation by spoilage microorganisms.In this work,a total of 17 isolates of spoilage bacteria that could secrete both collagenase and lipase were determined by raw-chicken juice agar(RJA)method,and the results showed that 7 strains of Serratia,Aeromonas,and Pseudomonas could significantly decompose the collagen ingredients.The gelatin zymography showed that Serratia liquefaciens(F5)and(G7)had apparent degradation bands around 50 kDa,and Aeromonas veronii(G8)and Aeromonas salmonicida(H8)had a band around.65 and 95 kDa,respectively.The lipase and collagenase activities were detected isolate-by-isolate,with F5 showing the highest collagenase activity.For spoilage ability on meat in situ,F5 performed strongest in spoilage ability,indicated by the total viable counts,total volatile basic nitrogen content,sensory scores,lipase,and collagenase activity.This study provides a theoretical basis for spoilage heterogeneity of strains with high-producing collagenase in meat.展开更多
Pre-polymerized vinyl trimethoxy silane(PVTMS)@MWCNT nano-aerogel system was constructed via radical polymerization,sol-gel transition and supercritical CO_(2)drying.The fabricated organic-inorganic hybrid PVTMS@MWCNT...Pre-polymerized vinyl trimethoxy silane(PVTMS)@MWCNT nano-aerogel system was constructed via radical polymerization,sol-gel transition and supercritical CO_(2)drying.The fabricated organic-inorganic hybrid PVTMS@MWCNT aerogel structure shows nano-pore size(30-40 nm),high specific surface area(559 m^(2)g^(−1)),high void fraction(91.7%)and enhanced mechanical property:(1)the nano-pore size is beneficial for efficiently blocking thermal conduction and thermal convection via Knudsen effect(beneficial for infrared(IR)stealth);(2)the heterogeneous interface was beneficial for IR reflection(beneficial for IR stealth)and MWCNT polarization loss(beneficial for electromagnetic wave(EMW)attenuation);(3)the high void fraction was beneficial for enhancing thermal insulation(beneficial for IR stealth)and EMW impedance match(beneficial for EMW attenuation).Guided by the above theoretical design strategy,PVTMS@MWCNT nano-aerogel shows superior EMW absorption property(cover all Ku-band)and thermal IR stealth property(ΔT reached 60.7℃).Followed by a facial combination of the above nano-aerogel with graphene film of high electrical conductivity,an extremely high electromagnetic interference shielding material(66.5 dB,2.06 mm thickness)with superior absorption performance of an average absorption-to-reflection(A/R)coefficient ratio of 25.4 and a low reflection bandwidth of 4.1 GHz(A/R ratio more than 10)was experimentally obtained in this work.展开更多
Zinc(Zn)is considered a promising biodegradable metal for implant applications due to its appropriate degradability and favorable osteogenesis properties.In this work,laser powder bed fusion(LPBF)additive manufacturin...Zinc(Zn)is considered a promising biodegradable metal for implant applications due to its appropriate degradability and favorable osteogenesis properties.In this work,laser powder bed fusion(LPBF)additive manufacturing was employed to fabricate pure Zn with a heterogeneous microstructure and exceptional strength-ductility synergy.An optimized processing window of LPBF was established for printing Zn samples with relative densities greater than 99%using a laser power range of 80∼90 W and a scanning speed of 900 mm s−1.The Zn sample printed with a power of 80 W at a speed of 900 mm s−1 exhibited a hierarchical heterogeneous microstructure consisting of millimeter-scale molten pool boundaries,micrometer-scale bimodal grains,and nanometer-scale pre-existing dislocations,due to rapid cooling rates and significant thermal gradients formed in the molten pools.The printed sample exhibited the highest ductility of∼12.1%among all reported LPBF-printed pure Zn to date with appreciable ultimate tensile strength(∼128.7 MPa).Such superior strength-ductility synergy can be attributed to the presence of multiple deformation mechanisms that are primarily governed by heterogeneous deformation-induced hardening resulting from the alternative arrangement of bimodal Zn grains with pre-existing dislocations.Additionally,continuous strain hardening was facilitated through the interactions between deformation twins,grains and dislocations as strain accumulated,further contributing to the superior strength-ductility synergy.These findings provide valuable insights into the deformation behavior and mechanisms underlying exceptional mechanical properties of LPBF-printed Zn and its alloys for implant applications.展开更多
Geomechanical assessment using coupled reservoir-geomechanical simulation is becoming increasingly important for analyzing the potential geomechanical risks in subsurface geological developments.However,a robust and e...Geomechanical assessment using coupled reservoir-geomechanical simulation is becoming increasingly important for analyzing the potential geomechanical risks in subsurface geological developments.However,a robust and efficient geomechanical upscaling technique for heterogeneous geological reservoirs is lacking to advance the applications of three-dimensional(3D)reservoir-scale geomechanical simulation considering detailed geological heterogeneities.Here,we develop convolutional neural network(CNN)proxies that reproduce the anisotropic nonlinear geomechanical response caused by lithological heterogeneity,and compute upscaled geomechanical properties from CNN proxies.The CNN proxies are trained using a large dataset of randomly generated spatially correlated sand-shale realizations as inputs and simulation results of their macroscopic geomechanical response as outputs.The trained CNN models can provide the upscaled shear strength(R^(2)>0.949),stress-strain behavior(R^(2)>0.925),and volumetric strain changes(R^(2)>0.958)that highly agree with the numerical simulation results while saving over two orders of magnitude of computational time.This is a major advantage in computing the upscaled geomechanical properties directly from geological realizations without the need to perform local numerical simulations to obtain the geomechanical response.The proposed CNN proxybased upscaling technique has the ability to(1)bridge the gap between the fine-scale geocellular models considering geological uncertainties and computationally efficient geomechanical models used to assess the geomechanical risks of large-scale subsurface development,and(2)improve the efficiency of numerical upscaling techniques that rely on local numerical simulations,leading to significantly increased computational time for uncertainty quantification using numerous geological realizations.展开更多
Reservoir heterogeneities play a crucial role in governing reservoir performance and management.Traditionally,detailed and inter-well heterogeneity analyses are commonly performed by mapping seismic facies change in t...Reservoir heterogeneities play a crucial role in governing reservoir performance and management.Traditionally,detailed and inter-well heterogeneity analyses are commonly performed by mapping seismic facies change in the seismic data,which is a time-intensive task.Many researchers have utilized a robust Grey-level co-occurrence matrix(GLCM)-based texture attributes to map reservoir heterogeneity.However,these attributes take seismic data as input and might not be sensitive to lateral lithology variation.To incorporate the lithology information,we have developed an innovative impedance-based texture approach using GLCM workflow by integrating 3D acoustic impedance volume(a rock propertybased attribute)obtained from a deep convolution network-based impedance inversion.Our proposed workflow is anticipated to be more sensitive toward mapping lateral changes than the conventional amplitude-based texture approach,wherein seismic data is used as input.To evaluate the improvement,we applied the proposed workflow to the full-stack 3D seismic data from the Poseidon field,NW-shelf,Australia.This study demonstrates that a better demarcation of reservoir gas sands with improved lateral continuity is achievable with the presented approach compared to the conventional approach.In addition,we assess the implication of multi-stage faulting on facies distribution for effective reservoir characterization.This study also suggests a well-bounded potential reservoir facies distribution along the parallel fault lines.Thus,the proposed approach provides an efficient strategy by integrating the impedance information with texture attributes to improve the inference on reservoir heterogeneity,which can serve as a promising tool for identifying potential reservoir zones for both production benefits and fluid storage.展开更多
The performance of optical interconnection has improved dramatically in recent years.Silicon-based optoelectronic heterogeneous integration is the key enabler to achieve high performance optical interconnection,which ...The performance of optical interconnection has improved dramatically in recent years.Silicon-based optoelectronic heterogeneous integration is the key enabler to achieve high performance optical interconnection,which not only provides the optical gain which is absent from native Si substrates and enables complete photonic functionalities on chip,but also improves the system performance through advanced heterogeneous integrated packaging.This paper reviews recent progress of silicon-based optoelectronic heterogeneous integration in high performance optical interconnection.The research status,development trend and application of ultra-low loss optical waveguides,high-speed detectors,high-speed modulators,lasers and 2D,2.5D,3D and monolithic integration are focused on.展开更多
The conventional dynamic heterogeneous redundancy(DHR)architecture suffers from the security threats caused by the stability differences and similar vulnerabilities among the executors.To overcome these challenges,we ...The conventional dynamic heterogeneous redundancy(DHR)architecture suffers from the security threats caused by the stability differences and similar vulnerabilities among the executors.To overcome these challenges,we propose an intelligent DHR architecture,which is more feasible by intelligently combining the random distribution based dynamic scheduling algorithm(RD-DS)and information weight and heterogeneity based arbitrament(IWHA)algorithm.In the proposed architecture,the random distribution function and information weight are employed to achieve the optimal selection of executors in the process of RD-DS,which avoids the case that some executors fail to be selected due to their stability difference in the conventional DHR architecture.Then,through introducing the heterogeneity to restrict the information weights in the procedure of the IWHA,the proposed architecture solves the common mode escape issue caused by the existence of multiple identical error output results of similar vulnerabilities.The experimental results characterize that the proposed architecture outperforms in heterogeneity,scheduling times,security,and stability over the conventional DHR architecture under the same conditions.展开更多
Gastric cancer(GC)is a major cause of cancer-related mortality worldwide.GC is determined by multiple(epi)genetic and environmental factors;can occur at distinct anatomic positions of the stomach;and displays high het...Gastric cancer(GC)is a major cause of cancer-related mortality worldwide.GC is determined by multiple(epi)genetic and environmental factors;can occur at distinct anatomic positions of the stomach;and displays high heterogeneity,with different cellular origins and diverse histological and molecular features.This heterogeneity has hindered efforts to fully understand the pathology of GC and develop efficient therapeutics.In the past decade,great progress has been made in the study of GC,particularly in molecular subtyping,investigation of the immune microenvironment,and defining the evolutionary path and dynamics.Preclinical mouse models,particularly immunocompetent models that mimic the cellular and molecular features of human GC,in combination with organoid culture and clinical studies,have provided powerful tools for elucidating the molecular and cellular mechanisms underlying GC pathology and immune evasion,and the development of novel therapeutic strategies.Herein,we first briefly introduce current progress and challenges in GC study and subsequently summarize immunocompetent GC mouse models,emphasizing the potential application of genetically engineered mouse models in antitumor immunity and immunotherapy studies.展开更多
In groundwater hydrology,aquitard heterogeneity is often less considered compared to aquifers,despite its significant impact on groundwater hydraulics and groundwater resources evaluation.A semi-analytical solution is...In groundwater hydrology,aquitard heterogeneity is often less considered compared to aquifers,despite its significant impact on groundwater hydraulics and groundwater resources evaluation.A semi-analytical solution is derived for pumping-induced well hydraulics and groundwater budget with consideration of vertical heterogeneity in aquitard hydraulic conductivity(K)and specific storage(S_(s)).The proposed new solution is innovative in its partitioning of the aquitard into multiple homogeneous sub-layers to enable consideration of various forms of vertically heterogeneous K or S_(s).Two scenarios of analytical investigations are explored:one is the presence of aquitard interlayers with distinct K or S_(s) values,a common field-scale occurrence;another is an exponentially depth-decaying aquitard S_(s),a regional-scale phenomenon supported by statistical analysis.Analytical investigations reveal that a low-K interlayer can significantly increase aquifer drawdown and enhance aquifer/aquitard depletion;a high-S_(s) interlayer can noticeably reduce aquifer drawdown and increase aquitard depletion.Locations of low-K or high-S_(s) interlayers also significantly impact well hydraulics and groundwater budget.In the context of an exponentially depth-decaying aquitard S_(s),a larger decay exponent can enhance aquifer drawdown.When using current models with a vertically homogeneous aquitard,half the sum of the geometric and harmonic means of exponentially depth-decaying aquitard S_(s) should be used to calculate aquitard depletion and unconfined aquifer leakage.展开更多
Selective conversion of fructose to 1,2-propanediol(1,2-PDO)is considered as a sustainable and cost-effective alternative to petroleum-based processes,however,this approach still faces challenges associated with low e...Selective conversion of fructose to 1,2-propanediol(1,2-PDO)is considered as a sustainable and cost-effective alternative to petroleum-based processes,however,this approach still faces challenges associated with low efficiency and harsh reaction conditions.Here,we have successfully synthesized a novel bifunctional Ru-WO_(x)-MgO_(y) catalyst through a facile'one-pot'solvothermal method.Remarkably,this catalyst exhibits exceptional catalytic performances in the conversion of fructose to 1,2-PDO under mild reaction conditions.The yield of 1,2-PDO is up to 56.2%at 140°C for 4 h under an ultra-low hydrogen pressure of only 0.2 MPa,surpassing the reported results in recent literature(below 51%).Comprehensive characterizations and density functional theory(DFT)calculations reveal that the presence of oxygen vacancies in the Ru-WO_(x)-MgO_(y) catalyst,serving as active acidic sites,facilitates the chemoselective cleavage of C-C bonds in fructose,which leads to the generation of active intermediates and ultimately resulted in the high yield of 1,2-PDO.展开更多
To investigate the complex macro-mechanical properties of coal from a micro-mechanical perspective,we have conducted a series of micro-mechanical experiments on coal using a nano-indentation instrument.These experimen...To investigate the complex macro-mechanical properties of coal from a micro-mechanical perspective,we have conducted a series of micro-mechanical experiments on coal using a nano-indentation instrument.These experiments were conducted under both dynamic and static loading conditions,allowing us to gather the micro-mechanical parameters of coal for further analysis of its micro-mechanical heterogeneity using the box counting statistical method and the Weibull model.The research findings indicate that the load–displacement curves of the coal mass under the two different loading modes exhibit noticeable discreteness.This can be attributed to the stress concentration phenomenon caused by variations in the mechanical properties of the micro-units during the loading process of the coal mass.Consequently,there are significant fluctuations in the micro-mechanical parameters of the coal mass.Moreover,the mechanical heterogeneity of the coal at the nanoscale was confirmed based on the calculation results of the standard deviation coefficient and Weibull modulus of the coal body’s micromechanical parameters.These results reveal the influence of microstructural defects and minerals on the uniformity of the stress field distribution within the loaded coal body,as well as on the ductility characteristics of the micro-defect structure.Furthermore,there is a pronounced heterogeneity in the micromechanical parameters.Furthermore,we have established a relationship between the macro and micro elastic modulus of coal by applying the Mori-Tanaka homogenization method.This relationship holds great significance for revealing the micro-mechanical failure mechanism of coal.展开更多
The post-collisional Cenozoic basic volcanic rocks in NE Turkey show temporal variations in whole-rock lithophile element and highly siderophile element(HSE)systematics that are mainly associated with the nature of su...The post-collisional Cenozoic basic volcanic rocks in NE Turkey show temporal variations in whole-rock lithophile element and highly siderophile element(HSE)systematics that are mainly associated with the nature of sub-continental lithospheric mantle(SCLM)sources and parental melt generation.So far,the traditional whole-rock lithophile geochemical data of these basic volcanic rocks have provided important constraints on the nature of SCLM sources.Integrated lithophile element and HSE geochemical data of these basic volcanic rocks also reveal the heterogeneity of the SCLM source,which is principally related to variable metasomatism resulting from previous subduction(s)and post-collisional mantle-crust interactions in an extensional setting.Lithophile element geochemical features suggest that the parental magmas have derived from metasomatized spinel-to garnet-bearing SCLM sources for Eocene and Miocene basic volcanic rocks with subduction signatures whereas originated from spinel-to garnet-bearing SCLM sources for Mio-Pliocene and Plio-Quaternary basaltic volcanic rocks without the subduction signature.Lithophile element and HSE geo-chemistry also reveal that Eocene and Miocene basic vol-canic rocks were affected by more pronounced crustal contamination than the basaltic volcanic rocks of Mio-Pliocene and Quaternary.Furthermore,the integrated lithophile element and HSE compositions of these basic volcanic rocks,together with the regional asymmetric lithospheric delamination model,reveal that the compositional variation(especially due to metasomatism)was significant temporally in the heterogeneity of the SCLM sources from which parental magmas formed during the Cenozoic era.展开更多
Research on discrete memristor-based neural networks has received much attention.However,current research mainly focuses on memristor–based discrete homogeneous neuron networks,while memristor-coupled discrete hetero...Research on discrete memristor-based neural networks has received much attention.However,current research mainly focuses on memristor–based discrete homogeneous neuron networks,while memristor-coupled discrete heterogeneous neuron networks are rarely reported.In this study,a new four-stable discrete locally active memristor is proposed and its nonvolatile and locally active properties are verified by its power-off plot and DC V–I diagram.Based on two-dimensional(2D)discrete Izhikevich neuron and 2D discrete Chialvo neuron,a heterogeneous discrete neuron network is constructed by using the proposed discrete memristor as a coupling synapse connecting the two heterogeneous neurons.Considering the coupling strength as the control parameter,chaotic firing,periodic firing,and hyperchaotic firing patterns are revealed.In particular,multiple coexisting firing patterns are observed,which are induced by different initial values of the memristor.Phase synchronization between the two heterogeneous neurons is discussed and it is found that they can achieve perfect synchronous at large coupling strength.Furthermore,the effect of Gaussian white noise on synchronization behaviors is also explored.We demonstrate that the presence of noise not only leads to the transition of firing patterns,but also achieves the phase synchronization between two heterogeneous neurons under low coupling strength.展开更多
Blockchain-enabled cybersecurity system to ensure and strengthen decentralized digital transaction is gradually gaining popularity in the digital era for various areas like finance,transportation,healthcare,education,...Blockchain-enabled cybersecurity system to ensure and strengthen decentralized digital transaction is gradually gaining popularity in the digital era for various areas like finance,transportation,healthcare,education,and supply chain management.Blockchain interactions in the heterogeneous network have fascinated more attention due to the authentication of their digital application exchanges.However,the exponential development of storage space capabilities across the blockchain-based heterogeneous network has become an important issue in preventing blockchain distribution and the extension of blockchain nodes.There is the biggest challenge of data integrity and scalability,including significant computing complexity and inapplicable latency on regional network diversity,operating system diversity,bandwidth diversity,node diversity,etc.,for decision-making of data transactions across blockchain-based heterogeneous networks.Data security and privacy have also become the main concerns across the heterogeneous network to build smart IoT ecosystems.To address these issues,today’s researchers have explored the potential solutions of the capability of heterogeneous network devices to perform data transactions where the system stimulates their integration reliably and securely with blockchain.The key goal of this paper is to conduct a state-of-the-art and comprehensive survey on cybersecurity enhancement using blockchain in the heterogeneous network.This paper proposes a full-fledged taxonomy to identify the main obstacles,research gaps,future research directions,effective solutions,andmost relevant blockchain-enabled cybersecurity systems.In addition,Blockchain based heterogeneous network framework with cybersecurity is proposed in this paper tomeet the goal of maintaining optimal performance data transactions among organizations.Overall,this paper provides an in-depth description based on the critical analysis to overcome the existing work gaps for future research where it presents a potential cybersecurity design with key requirements of blockchain across a heterogeneous network.展开更多
Selective cleavage of Csp^(2)-OCH_(3)bond in lignin without breaking other types of C-O bonds followed by N-functionalization is fascinating for on-purpose valorization of biomass.Here,a Co/Ni-based dual-atom catalyst...Selective cleavage of Csp^(2)-OCH_(3)bond in lignin without breaking other types of C-O bonds followed by N-functionalization is fascinating for on-purpose valorization of biomass.Here,a Co/Ni-based dual-atom catalyst CoNiDA@NC prepared by in-situ evaporation and acid-etching of metal species from tailor-made metal–organic frameworks was efficient for reductive upgrading of various lignin-derived phenols to cyclohexanols(88.5%–99.9%yields),which had ca.4 times higher reaction rate than the single-atom catalyst and was superior to state-of-the-art heterogeneous catalysts.The synergistic catalysis of Co/Ni dual atoms facilitated both hydrogen dissociation and hydrogenolysis steps,and could optimize adsorption configuration of lignin-derived methoxylated phenols to further favor the Csp^(2)-OCH_(3)cleavage,as elaborated by theoretical calculations.Notably,the CoNi_(DA)@NC catalyst was highly recyclable,and exhibited excellent demethoxylation performance(77.1%yield)in real lignin monomer mixtures.Via in-situ cascade conversion processes assisted by dual-atom catalysis,various high-value N-containing chemicals,including caprolactams and cyclohexylamines,could be produced from lignin.展开更多
Developing advanced battery-type materials with abundant active sites,high conductivity,versatile morphologies,and hierarchically porous structures is crucial for realizing high-quality hybrid supercapacitors.Herein,h...Developing advanced battery-type materials with abundant active sites,high conductivity,versatile morphologies,and hierarchically porous structures is crucial for realizing high-quality hybrid supercapacitors.Herein,heterogeneous FeS@NiS is synthesized by cationic Co doping via surface-structure engineering.The density functional theory(DFT)theoretical calculations are firstly performed to predict the advantages of Co dopant by improving the OH^(−)adsorption properties and adjusting electronic structure,benefiting ions/electron transfer.The dynamic surface evolution is further explored which demonstrates that CoFeS@CoNiS could be quickly reconstructed to Ni(Co)Fe_(2)O_(4)during the charging process,while the unstable structure of the amorphous Ni(Co)Fe_(2)O_(4)results in partial conversion to Ni/Co/FeOOH at high potentials,which contributes to the more reactive active site and good structural stability.Thus,the free-standing electrode reveals excellent electrochemical performance with a superior capacity(335.6 mA h g^(−1),2684 F g^(−1))at 3 A g^(−1).Furthermore,the as-fabricated device shows a quality energy density of 78.1 W h kg^(−1)at a power density of 750 W kg^(−1)and excellent cycle life of 92.1%capacitance retention after 5000 cycles.This work offers a facile strategy to construct versatile morphological structures using electrochemical activation and holds promising applications in energy-related fields.展开更多
Poor cycling stability in lithium–sulfur(Li–S)batteries necessitates advanced electrode/electrolyte design and innovative interlayer architectures.Heterogeneous catalysis has emerged as a promising approach,leveragi...Poor cycling stability in lithium–sulfur(Li–S)batteries necessitates advanced electrode/electrolyte design and innovative interlayer architectures.Heterogeneous catalysis has emerged as a promising approach,leveraging the adsorption and catalytic performance on lithium polysulfides(LiPSs)to inhibit LiPSs shuttling and improve redox kinetics.In this study,we report an ultrathin and laminar SnO_(2)@MXene heterostructure interlayer(SnO_(2)@MX),where SnO_(2) quantum dots(QDs)are uniformly distributed across the MXene layer.The combined structure of SnO_(2) QDs and MXene,along with the creation of numerous active boundary sites with coordination electron environments,plays a critical role in manipulating the catalytic kinetics of sulfur species.The Li–S cell with the SnO_(2)@MX-modified separator not only demonstrates superior electrochemical performance compared to cells with a bare separator but also induces homogeneous Li deposition during cycling.As a result,an areal capacity of 7.6 mAh cm^(-2) under a sulfur loading of 7.5 mg cm^(-2) and a high stability over 500 cycles are achieved.Our work demonstrates a feasible strategy of utilizing a laminar separator interlayer for advanced Li–S batteries awaiting commercialization and may shed light on the understanding of heterostructure catalysis with enhanced reaction kinetics.展开更多
Despite having significant effects on social contagions,individual heterogeneity has frequently been overlooked in earlier studies.To better understand the complexity of social contagions,a non-Markovian model incorpo...Despite having significant effects on social contagions,individual heterogeneity has frequently been overlooked in earlier studies.To better understand the complexity of social contagions,a non-Markovian model incorporating heterogeneous social influence and adoption thresholds is introduced.For theoretical analysis,a generalized edge-based compartmental theory which considers the heterogeneities of social influence and adoption thresholds is developed.Focusing on the final adoption size,the critical propagation probability,and the phase transition type,social contagions for adoption thresholds that follow normal distributions with various standard deviations,follow various distributions,and correlate with degrees are investigated.When thresholds follow normal distributions,a larger standard deviation results in a larger final adoption size when the information propagation probability is relatively low.However,when the information propagation probability is relatively high,a larger standard deviation results in a smaller final adoption size.When thresholds follow various distributions,crossover phenomena in phase transition are observed when investigating the relationship of the final adoption size versus the average adoption threshold for some threshold distributions.When thresholds are correlated with degrees,similar crossover phenomena occur when investigating the relationship of the final adoption size versus the degree correlation index.Additionally,we find that increasing the heterogeneity of social influence suppresses the effects of adoption threshold heterogeneity on social contagions in three cases.Our theory predictions agree well with the simulation results.展开更多
基金financial support from the King Abdullah University of Science and Technology(KAUST).
文摘The increase in anthropogenic carbon dioxide(CO_(2))emissions has exacerbated the deterioration of the global environment,which should be controlled to achieve carbon neutrality.Central to the core goal of achieving carbon neutrality is the utilization of CO_(2) under economic and sustainable conditions.Recently,the strong need for carbon neutrality has led to a proliferation of studies on the direct conversion of CO_(2) into carboxylic acids,which can effectively alleviate CO_(2) emissions and create high-value chemicals.The purpose of this review is to present the application prospects of carboxylic acids and the basic principles of CO_(2) conversion into carboxylic acids through photo-,electric-,and thermal catalysis.Special attention is focused on the regulation strategy of the activity of abundant catalysts at the molecular level,inspiring the preparation of high-performance catalysts.In addition,theoretical calculations,advanced technologies,and numerous typical examples are introduced to elaborate on the corresponding process and influencing factors of catalytic activity.Finally,challenges and prospects are provided for the future development of this field.It is hoped that this review will contribute to a deeper understanding of the conversion of CO_(2) into carboxylic acids and inspire more innovative breakthroughs.
基金supported by the National Natural Science Foundation of China,No.81772421(to YH).
文摘Distraction spinal cord injury is caused by some degree of distraction or longitudinal tension on the spinal cord and commonly occurs in patients who undergo corrective operation for severe spinal deformity.With the increased degree and duration of distraction,spinal cord injuries become more serious in terms of their neurophysiology,histology,and behavior.Very few studies have been published on the specific characteristics of distraction spinal cord injury.In this study,we systematically review 22 related studies involving animal models of distraction spinal cord injury,focusing particularly on the neurophysiological,histological,and behavioral characteristics of this disease.In addition,we summarize the mechanisms underlying primary and secondary injuries caused by distraction spinal cord injury and clarify the effects of different degrees and durations of distraction on the primary injuries associated with spinal cord injury.We provide new concepts for the establishment of a model of distraction spinal cord injury and related basic research,and provide reference guidelines for the clinical diagnosis and treatment of this disease.
基金financed by grants from the Natural Science Foundation of Jiangsu Province in China (BK20221515)the National Natural Science Foundation of China (32172266)。
文摘Chilled chicken is inevitably contaminated by microorganisms during slaughtering and processing,resulting in spoilage.Cutting parts of chilled chicken,especially wings,feet,and other skin-on products,are abundant in collagen,which may be the primary target for degradation by spoilage microorganisms.In this work,a total of 17 isolates of spoilage bacteria that could secrete both collagenase and lipase were determined by raw-chicken juice agar(RJA)method,and the results showed that 7 strains of Serratia,Aeromonas,and Pseudomonas could significantly decompose the collagen ingredients.The gelatin zymography showed that Serratia liquefaciens(F5)and(G7)had apparent degradation bands around 50 kDa,and Aeromonas veronii(G8)and Aeromonas salmonicida(H8)had a band around.65 and 95 kDa,respectively.The lipase and collagenase activities were detected isolate-by-isolate,with F5 showing the highest collagenase activity.For spoilage ability on meat in situ,F5 performed strongest in spoilage ability,indicated by the total viable counts,total volatile basic nitrogen content,sensory scores,lipase,and collagenase activity.This study provides a theoretical basis for spoilage heterogeneity of strains with high-producing collagenase in meat.
基金the National Natural Science Foundation(No.52073187)NSAF Foundation(No.U2230202)for their financial support of this project+3 种基金National Natural Science Foundation(No.51721091)Programme of Introducing Talents of Discipline to Universities(No.B13040)State Key Laboratory of Polymer Materials Engineering(No.sklpme2022-2-03)support of China Scholarship Council
文摘Pre-polymerized vinyl trimethoxy silane(PVTMS)@MWCNT nano-aerogel system was constructed via radical polymerization,sol-gel transition and supercritical CO_(2)drying.The fabricated organic-inorganic hybrid PVTMS@MWCNT aerogel structure shows nano-pore size(30-40 nm),high specific surface area(559 m^(2)g^(−1)),high void fraction(91.7%)and enhanced mechanical property:(1)the nano-pore size is beneficial for efficiently blocking thermal conduction and thermal convection via Knudsen effect(beneficial for infrared(IR)stealth);(2)the heterogeneous interface was beneficial for IR reflection(beneficial for IR stealth)and MWCNT polarization loss(beneficial for electromagnetic wave(EMW)attenuation);(3)the high void fraction was beneficial for enhancing thermal insulation(beneficial for IR stealth)and EMW impedance match(beneficial for EMW attenuation).Guided by the above theoretical design strategy,PVTMS@MWCNT nano-aerogel shows superior EMW absorption property(cover all Ku-band)and thermal IR stealth property(ΔT reached 60.7℃).Followed by a facial combination of the above nano-aerogel with graphene film of high electrical conductivity,an extremely high electromagnetic interference shielding material(66.5 dB,2.06 mm thickness)with superior absorption performance of an average absorption-to-reflection(A/R)coefficient ratio of 25.4 and a low reflection bandwidth of 4.1 GHz(A/R ratio more than 10)was experimentally obtained in this work.
基金National Natural Science Foundation of China (52305358)the Fundamental Research Funds for the Central Universities (2023ZYGXZR061)+3 种基金Guangdong Basic and Applied Basic Research Foundation (2022A1515010304)Science and Technology Program of Guangzhou (202201010362)Young Elite Scientists Sponsorship Program by CAST . (2023QNRC001)Young Talent Support Project of Guangzhou (QT-2023-001)
文摘Zinc(Zn)is considered a promising biodegradable metal for implant applications due to its appropriate degradability and favorable osteogenesis properties.In this work,laser powder bed fusion(LPBF)additive manufacturing was employed to fabricate pure Zn with a heterogeneous microstructure and exceptional strength-ductility synergy.An optimized processing window of LPBF was established for printing Zn samples with relative densities greater than 99%using a laser power range of 80∼90 W and a scanning speed of 900 mm s−1.The Zn sample printed with a power of 80 W at a speed of 900 mm s−1 exhibited a hierarchical heterogeneous microstructure consisting of millimeter-scale molten pool boundaries,micrometer-scale bimodal grains,and nanometer-scale pre-existing dislocations,due to rapid cooling rates and significant thermal gradients formed in the molten pools.The printed sample exhibited the highest ductility of∼12.1%among all reported LPBF-printed pure Zn to date with appreciable ultimate tensile strength(∼128.7 MPa).Such superior strength-ductility synergy can be attributed to the presence of multiple deformation mechanisms that are primarily governed by heterogeneous deformation-induced hardening resulting from the alternative arrangement of bimodal Zn grains with pre-existing dislocations.Additionally,continuous strain hardening was facilitated through the interactions between deformation twins,grains and dislocations as strain accumulated,further contributing to the superior strength-ductility synergy.These findings provide valuable insights into the deformation behavior and mechanisms underlying exceptional mechanical properties of LPBF-printed Zn and its alloys for implant applications.
基金financial support provided by the Future Energy System at University of Alberta and NSERC Discovery Grant RGPIN-2023-04084。
文摘Geomechanical assessment using coupled reservoir-geomechanical simulation is becoming increasingly important for analyzing the potential geomechanical risks in subsurface geological developments.However,a robust and efficient geomechanical upscaling technique for heterogeneous geological reservoirs is lacking to advance the applications of three-dimensional(3D)reservoir-scale geomechanical simulation considering detailed geological heterogeneities.Here,we develop convolutional neural network(CNN)proxies that reproduce the anisotropic nonlinear geomechanical response caused by lithological heterogeneity,and compute upscaled geomechanical properties from CNN proxies.The CNN proxies are trained using a large dataset of randomly generated spatially correlated sand-shale realizations as inputs and simulation results of their macroscopic geomechanical response as outputs.The trained CNN models can provide the upscaled shear strength(R^(2)>0.949),stress-strain behavior(R^(2)>0.925),and volumetric strain changes(R^(2)>0.958)that highly agree with the numerical simulation results while saving over two orders of magnitude of computational time.This is a major advantage in computing the upscaled geomechanical properties directly from geological realizations without the need to perform local numerical simulations to obtain the geomechanical response.The proposed CNN proxybased upscaling technique has the ability to(1)bridge the gap between the fine-scale geocellular models considering geological uncertainties and computationally efficient geomechanical models used to assess the geomechanical risks of large-scale subsurface development,and(2)improve the efficiency of numerical upscaling techniques that rely on local numerical simulations,leading to significantly increased computational time for uncertainty quantification using numerous geological realizations.
文摘Reservoir heterogeneities play a crucial role in governing reservoir performance and management.Traditionally,detailed and inter-well heterogeneity analyses are commonly performed by mapping seismic facies change in the seismic data,which is a time-intensive task.Many researchers have utilized a robust Grey-level co-occurrence matrix(GLCM)-based texture attributes to map reservoir heterogeneity.However,these attributes take seismic data as input and might not be sensitive to lateral lithology variation.To incorporate the lithology information,we have developed an innovative impedance-based texture approach using GLCM workflow by integrating 3D acoustic impedance volume(a rock propertybased attribute)obtained from a deep convolution network-based impedance inversion.Our proposed workflow is anticipated to be more sensitive toward mapping lateral changes than the conventional amplitude-based texture approach,wherein seismic data is used as input.To evaluate the improvement,we applied the proposed workflow to the full-stack 3D seismic data from the Poseidon field,NW-shelf,Australia.This study demonstrates that a better demarcation of reservoir gas sands with improved lateral continuity is achievable with the presented approach compared to the conventional approach.In addition,we assess the implication of multi-stage faulting on facies distribution for effective reservoir characterization.This study also suggests a well-bounded potential reservoir facies distribution along the parallel fault lines.Thus,the proposed approach provides an efficient strategy by integrating the impedance information with texture attributes to improve the inference on reservoir heterogeneity,which can serve as a promising tool for identifying potential reservoir zones for both production benefits and fluid storage.
基金Project supported in part by the National Key Research and Development Program of China(Grant No.2021YFB2206504)the National Natural Science Foundation of China(Grant No.62235017)the China Postdoctoral Science Foundation(Grant No.2021M703125).
文摘The performance of optical interconnection has improved dramatically in recent years.Silicon-based optoelectronic heterogeneous integration is the key enabler to achieve high performance optical interconnection,which not only provides the optical gain which is absent from native Si substrates and enables complete photonic functionalities on chip,but also improves the system performance through advanced heterogeneous integrated packaging.This paper reviews recent progress of silicon-based optoelectronic heterogeneous integration in high performance optical interconnection.The research status,development trend and application of ultra-low loss optical waveguides,high-speed detectors,high-speed modulators,lasers and 2D,2.5D,3D and monolithic integration are focused on.
基金supported by the National Key Research and Development Program of China(2020YFE0200600)the National Natural Science Foundation of China(U22B2026)。
文摘The conventional dynamic heterogeneous redundancy(DHR)architecture suffers from the security threats caused by the stability differences and similar vulnerabilities among the executors.To overcome these challenges,we propose an intelligent DHR architecture,which is more feasible by intelligently combining the random distribution based dynamic scheduling algorithm(RD-DS)and information weight and heterogeneity based arbitrament(IWHA)algorithm.In the proposed architecture,the random distribution function and information weight are employed to achieve the optimal selection of executors in the process of RD-DS,which avoids the case that some executors fail to be selected due to their stability difference in the conventional DHR architecture.Then,through introducing the heterogeneity to restrict the information weights in the procedure of the IWHA,the proposed architecture solves the common mode escape issue caused by the existence of multiple identical error output results of similar vulnerabilities.The experimental results characterize that the proposed architecture outperforms in heterogeneity,scheduling times,security,and stability over the conventional DHR architecture under the same conditions.
基金supported by the National Key R&D Program of China(Grant No.2020YFA0803200 and 2023YFC2505903)National Natural Science Foundation of China(Grant Nos.82003014,31930026,81972876,82150112,92168116,81725014,81822035,and 82222052)+1 种基金China Postdoctoral Science Foundation(Grant No.2020M671231)Fundamental Research Funds for the Central Universities(Grant No.22120240327)。
文摘Gastric cancer(GC)is a major cause of cancer-related mortality worldwide.GC is determined by multiple(epi)genetic and environmental factors;can occur at distinct anatomic positions of the stomach;and displays high heterogeneity,with different cellular origins and diverse histological and molecular features.This heterogeneity has hindered efforts to fully understand the pathology of GC and develop efficient therapeutics.In the past decade,great progress has been made in the study of GC,particularly in molecular subtyping,investigation of the immune microenvironment,and defining the evolutionary path and dynamics.Preclinical mouse models,particularly immunocompetent models that mimic the cellular and molecular features of human GC,in combination with organoid culture and clinical studies,have provided powerful tools for elucidating the molecular and cellular mechanisms underlying GC pathology and immune evasion,and the development of novel therapeutic strategies.Herein,we first briefly introduce current progress and challenges in GC study and subsequently summarize immunocompetent GC mouse models,emphasizing the potential application of genetically engineered mouse models in antitumor immunity and immunotherapy studies.
基金financially supported by the National Key Research and Development Program of China(Grant No.2019YFC1804301)the National Science Fourdation of China(Grant No.42272279,41902244)partial support from a Discovery Grant awarded by the Natural Sciences and Engineering Research Council of Canada(NSERC)。
文摘In groundwater hydrology,aquitard heterogeneity is often less considered compared to aquifers,despite its significant impact on groundwater hydraulics and groundwater resources evaluation.A semi-analytical solution is derived for pumping-induced well hydraulics and groundwater budget with consideration of vertical heterogeneity in aquitard hydraulic conductivity(K)and specific storage(S_(s)).The proposed new solution is innovative in its partitioning of the aquitard into multiple homogeneous sub-layers to enable consideration of various forms of vertically heterogeneous K or S_(s).Two scenarios of analytical investigations are explored:one is the presence of aquitard interlayers with distinct K or S_(s) values,a common field-scale occurrence;another is an exponentially depth-decaying aquitard S_(s),a regional-scale phenomenon supported by statistical analysis.Analytical investigations reveal that a low-K interlayer can significantly increase aquifer drawdown and enhance aquifer/aquitard depletion;a high-S_(s) interlayer can noticeably reduce aquifer drawdown and increase aquitard depletion.Locations of low-K or high-S_(s) interlayers also significantly impact well hydraulics and groundwater budget.In the context of an exponentially depth-decaying aquitard S_(s),a larger decay exponent can enhance aquifer drawdown.When using current models with a vertically homogeneous aquitard,half the sum of the geometric and harmonic means of exponentially depth-decaying aquitard S_(s) should be used to calculate aquitard depletion and unconfined aquifer leakage.
基金the financial support from the Natural Science Foundation of Chongqing(CSTB2022NSCQ-MSX0458)the State Key Laboratory of Coal Mine Disaster Dynamics and Control(2011DA105287-MS202203)+4 种基金the Joint Fund for Innovation and Development of Chongqing(CSTB2022NSCQ-LZX0030)the financial support from the National Natural Science Foundation of China(22168027 and 22308169)the financial support from the Natural Science Foundation of Chongqing(cstc2021jcyj-msxmX0741)the financial support from the National Natural Science Foundation of China(22105028)the Natural Science Foundation of Chongqing(cstc2021jcyj-msxmX0572)。
文摘Selective conversion of fructose to 1,2-propanediol(1,2-PDO)is considered as a sustainable and cost-effective alternative to petroleum-based processes,however,this approach still faces challenges associated with low efficiency and harsh reaction conditions.Here,we have successfully synthesized a novel bifunctional Ru-WO_(x)-MgO_(y) catalyst through a facile'one-pot'solvothermal method.Remarkably,this catalyst exhibits exceptional catalytic performances in the conversion of fructose to 1,2-PDO under mild reaction conditions.The yield of 1,2-PDO is up to 56.2%at 140°C for 4 h under an ultra-low hydrogen pressure of only 0.2 MPa,surpassing the reported results in recent literature(below 51%).Comprehensive characterizations and density functional theory(DFT)calculations reveal that the presence of oxygen vacancies in the Ru-WO_(x)-MgO_(y) catalyst,serving as active acidic sites,facilitates the chemoselective cleavage of C-C bonds in fructose,which leads to the generation of active intermediates and ultimately resulted in the high yield of 1,2-PDO.
基金Projects(U23B2093,52274245)supported by the National Natural Science Foundation of ChinaProject(KFJJ22-15M)supported by the Opening Project of State Key Laboratory of Explosion Science and Technology,China。
文摘To investigate the complex macro-mechanical properties of coal from a micro-mechanical perspective,we have conducted a series of micro-mechanical experiments on coal using a nano-indentation instrument.These experiments were conducted under both dynamic and static loading conditions,allowing us to gather the micro-mechanical parameters of coal for further analysis of its micro-mechanical heterogeneity using the box counting statistical method and the Weibull model.The research findings indicate that the load–displacement curves of the coal mass under the two different loading modes exhibit noticeable discreteness.This can be attributed to the stress concentration phenomenon caused by variations in the mechanical properties of the micro-units during the loading process of the coal mass.Consequently,there are significant fluctuations in the micro-mechanical parameters of the coal mass.Moreover,the mechanical heterogeneity of the coal at the nanoscale was confirmed based on the calculation results of the standard deviation coefficient and Weibull modulus of the coal body’s micromechanical parameters.These results reveal the influence of microstructural defects and minerals on the uniformity of the stress field distribution within the loaded coal body,as well as on the ductility characteristics of the micro-defect structure.Furthermore,there is a pronounced heterogeneity in the micromechanical parameters.Furthermore,we have established a relationship between the macro and micro elastic modulus of coal by applying the Mori-Tanaka homogenization method.This relationship holds great significance for revealing the micro-mechanical failure mechanism of coal.
文摘The post-collisional Cenozoic basic volcanic rocks in NE Turkey show temporal variations in whole-rock lithophile element and highly siderophile element(HSE)systematics that are mainly associated with the nature of sub-continental lithospheric mantle(SCLM)sources and parental melt generation.So far,the traditional whole-rock lithophile geochemical data of these basic volcanic rocks have provided important constraints on the nature of SCLM sources.Integrated lithophile element and HSE geochemical data of these basic volcanic rocks also reveal the heterogeneity of the SCLM source,which is principally related to variable metasomatism resulting from previous subduction(s)and post-collisional mantle-crust interactions in an extensional setting.Lithophile element geochemical features suggest that the parental magmas have derived from metasomatized spinel-to garnet-bearing SCLM sources for Eocene and Miocene basic volcanic rocks with subduction signatures whereas originated from spinel-to garnet-bearing SCLM sources for Mio-Pliocene and Plio-Quaternary basaltic volcanic rocks without the subduction signature.Lithophile element and HSE geo-chemistry also reveal that Eocene and Miocene basic vol-canic rocks were affected by more pronounced crustal contamination than the basaltic volcanic rocks of Mio-Pliocene and Quaternary.Furthermore,the integrated lithophile element and HSE compositions of these basic volcanic rocks,together with the regional asymmetric lithospheric delamination model,reveal that the compositional variation(especially due to metasomatism)was significant temporally in the heterogeneity of the SCLM sources from which parental magmas formed during the Cenozoic era.
基金Project supported by the National Natural Science Foundations of China(Grant Nos.62171401 and 62071411).
文摘Research on discrete memristor-based neural networks has received much attention.However,current research mainly focuses on memristor–based discrete homogeneous neuron networks,while memristor-coupled discrete heterogeneous neuron networks are rarely reported.In this study,a new four-stable discrete locally active memristor is proposed and its nonvolatile and locally active properties are verified by its power-off plot and DC V–I diagram.Based on two-dimensional(2D)discrete Izhikevich neuron and 2D discrete Chialvo neuron,a heterogeneous discrete neuron network is constructed by using the proposed discrete memristor as a coupling synapse connecting the two heterogeneous neurons.Considering the coupling strength as the control parameter,chaotic firing,periodic firing,and hyperchaotic firing patterns are revealed.In particular,multiple coexisting firing patterns are observed,which are induced by different initial values of the memristor.Phase synchronization between the two heterogeneous neurons is discussed and it is found that they can achieve perfect synchronous at large coupling strength.Furthermore,the effect of Gaussian white noise on synchronization behaviors is also explored.We demonstrate that the presence of noise not only leads to the transition of firing patterns,but also achieves the phase synchronization between two heterogeneous neurons under low coupling strength.
基金The authors would like to acknowledge the Institute for Big Data Analytics and Artificial Intelligence(IBDAAI),Universiti TeknologiMARA and the Ministry of Higher Education,Malaysia for the financial support through Fundamental Research Grant Scheme(FRGS)Grant No.FRGS/1/2021/ICT11/UITM/01/1.
文摘Blockchain-enabled cybersecurity system to ensure and strengthen decentralized digital transaction is gradually gaining popularity in the digital era for various areas like finance,transportation,healthcare,education,and supply chain management.Blockchain interactions in the heterogeneous network have fascinated more attention due to the authentication of their digital application exchanges.However,the exponential development of storage space capabilities across the blockchain-based heterogeneous network has become an important issue in preventing blockchain distribution and the extension of blockchain nodes.There is the biggest challenge of data integrity and scalability,including significant computing complexity and inapplicable latency on regional network diversity,operating system diversity,bandwidth diversity,node diversity,etc.,for decision-making of data transactions across blockchain-based heterogeneous networks.Data security and privacy have also become the main concerns across the heterogeneous network to build smart IoT ecosystems.To address these issues,today’s researchers have explored the potential solutions of the capability of heterogeneous network devices to perform data transactions where the system stimulates their integration reliably and securely with blockchain.The key goal of this paper is to conduct a state-of-the-art and comprehensive survey on cybersecurity enhancement using blockchain in the heterogeneous network.This paper proposes a full-fledged taxonomy to identify the main obstacles,research gaps,future research directions,effective solutions,andmost relevant blockchain-enabled cybersecurity systems.In addition,Blockchain based heterogeneous network framework with cybersecurity is proposed in this paper tomeet the goal of maintaining optimal performance data transactions among organizations.Overall,this paper provides an in-depth description based on the critical analysis to overcome the existing work gaps for future research where it presents a potential cybersecurity design with key requirements of blockchain across a heterogeneous network.
基金the National Natural Science Foundation of China(22368014)the Guizhou Provincial S&T Project(ZK[2022]011,GCC[2023]011)+2 种基金the Natural Science Foundation of Guangxi Zhuang Autonomous Region(2023JJA120098)the Guangxi Key Laboratory of Green Chemical Materials and Safety Technology,the Beibu Gulf University(2022SYSZZ02,2022ZZKT04)the Guizhou Provincial Higher Education Institution Program(Qianjiaoji[2023]082)。
文摘Selective cleavage of Csp^(2)-OCH_(3)bond in lignin without breaking other types of C-O bonds followed by N-functionalization is fascinating for on-purpose valorization of biomass.Here,a Co/Ni-based dual-atom catalyst CoNiDA@NC prepared by in-situ evaporation and acid-etching of metal species from tailor-made metal–organic frameworks was efficient for reductive upgrading of various lignin-derived phenols to cyclohexanols(88.5%–99.9%yields),which had ca.4 times higher reaction rate than the single-atom catalyst and was superior to state-of-the-art heterogeneous catalysts.The synergistic catalysis of Co/Ni dual atoms facilitated both hydrogen dissociation and hydrogenolysis steps,and could optimize adsorption configuration of lignin-derived methoxylated phenols to further favor the Csp^(2)-OCH_(3)cleavage,as elaborated by theoretical calculations.Notably,the CoNi_(DA)@NC catalyst was highly recyclable,and exhibited excellent demethoxylation performance(77.1%yield)in real lignin monomer mixtures.Via in-situ cascade conversion processes assisted by dual-atom catalysis,various high-value N-containing chemicals,including caprolactams and cyclohexylamines,could be produced from lignin.
基金financial support from the Chang Jiang Scholars Program (51073047)the National Natural Science Foundation of China (51773049)+5 种基金the China Aerospace Science and Technology Corporation-Harbin Institute of Technology Joint Center for Technology Innovation Fund (HIT15-1A01)the Harbin City Science and Technology Projects (2013DB4BP031 and RC2014QN017035)the Natural Science Foundation of Shandong Province of China (ZR2023QE071)the College Students’ Innovation and Entrepreneurship Training Program Projects of Shandong Province (S202211065048)the Scientific Research Foundation of Qingdao University (DC1900009425)the China Postdoctoral Science Foundation (2022TQ0282)
文摘Developing advanced battery-type materials with abundant active sites,high conductivity,versatile morphologies,and hierarchically porous structures is crucial for realizing high-quality hybrid supercapacitors.Herein,heterogeneous FeS@NiS is synthesized by cationic Co doping via surface-structure engineering.The density functional theory(DFT)theoretical calculations are firstly performed to predict the advantages of Co dopant by improving the OH^(−)adsorption properties and adjusting electronic structure,benefiting ions/electron transfer.The dynamic surface evolution is further explored which demonstrates that CoFeS@CoNiS could be quickly reconstructed to Ni(Co)Fe_(2)O_(4)during the charging process,while the unstable structure of the amorphous Ni(Co)Fe_(2)O_(4)results in partial conversion to Ni/Co/FeOOH at high potentials,which contributes to the more reactive active site and good structural stability.Thus,the free-standing electrode reveals excellent electrochemical performance with a superior capacity(335.6 mA h g^(−1),2684 F g^(−1))at 3 A g^(−1).Furthermore,the as-fabricated device shows a quality energy density of 78.1 W h kg^(−1)at a power density of 750 W kg^(−1)and excellent cycle life of 92.1%capacitance retention after 5000 cycles.This work offers a facile strategy to construct versatile morphological structures using electrochemical activation and holds promising applications in energy-related fields.
基金financial support from the Swiss National Science Foundation via the Southeast Asia–Europe Joint Funding Scheme 2020(Grant No.IZJFZ2_202476)funding from the National Natural Science Foundation of China(Grant Nos.22209118 and 00301054A1073)the Fundamental Research Funds for the Central Universities(Grant Nos.1082204112A26,20826044D3083,and 20822041G4080)。
文摘Poor cycling stability in lithium–sulfur(Li–S)batteries necessitates advanced electrode/electrolyte design and innovative interlayer architectures.Heterogeneous catalysis has emerged as a promising approach,leveraging the adsorption and catalytic performance on lithium polysulfides(LiPSs)to inhibit LiPSs shuttling and improve redox kinetics.In this study,we report an ultrathin and laminar SnO_(2)@MXene heterostructure interlayer(SnO_(2)@MX),where SnO_(2) quantum dots(QDs)are uniformly distributed across the MXene layer.The combined structure of SnO_(2) QDs and MXene,along with the creation of numerous active boundary sites with coordination electron environments,plays a critical role in manipulating the catalytic kinetics of sulfur species.The Li–S cell with the SnO_(2)@MX-modified separator not only demonstrates superior electrochemical performance compared to cells with a bare separator but also induces homogeneous Li deposition during cycling.As a result,an areal capacity of 7.6 mAh cm^(-2) under a sulfur loading of 7.5 mg cm^(-2) and a high stability over 500 cycles are achieved.Our work demonstrates a feasible strategy of utilizing a laminar separator interlayer for advanced Li–S batteries awaiting commercialization and may shed light on the understanding of heterostructure catalysis with enhanced reaction kinetics.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.62266030 and 61863025)。
文摘Despite having significant effects on social contagions,individual heterogeneity has frequently been overlooked in earlier studies.To better understand the complexity of social contagions,a non-Markovian model incorporating heterogeneous social influence and adoption thresholds is introduced.For theoretical analysis,a generalized edge-based compartmental theory which considers the heterogeneities of social influence and adoption thresholds is developed.Focusing on the final adoption size,the critical propagation probability,and the phase transition type,social contagions for adoption thresholds that follow normal distributions with various standard deviations,follow various distributions,and correlate with degrees are investigated.When thresholds follow normal distributions,a larger standard deviation results in a larger final adoption size when the information propagation probability is relatively low.However,when the information propagation probability is relatively high,a larger standard deviation results in a smaller final adoption size.When thresholds follow various distributions,crossover phenomena in phase transition are observed when investigating the relationship of the final adoption size versus the average adoption threshold for some threshold distributions.When thresholds are correlated with degrees,similar crossover phenomena occur when investigating the relationship of the final adoption size versus the degree correlation index.Additionally,we find that increasing the heterogeneity of social influence suppresses the effects of adoption threshold heterogeneity on social contagions in three cases.Our theory predictions agree well with the simulation results.