Solid-state batteries(SSBs) with high safety are promising for the energy fields,but the development has long been limited by machinability and interfacial problems.Hence,self-supporting,flexible Nano LLZO CSEs are pr...Solid-state batteries(SSBs) with high safety are promising for the energy fields,but the development has long been limited by machinability and interfacial problems.Hence,self-supporting,flexible Nano LLZO CSEs are prepared with a solvent-free method at 25℃.The 99.8 wt% contents of Nano LLZO particles enable the Nano LLZO CSEs to maintain good thermal stability while exhibiting a wide electrochemical window of 5.0 V and a high Li~+ transfer number of 0.8.The mean modulus reaches 4376 MPa.Benefiting from the interfacial modulation,the Li|Li symmetric batteries based on the Nano LLZO CSEs show benign stability with lithium at the current densities of 0.1 mA cm^(-2),0.2 mA cm^(-2),and 0.5 mA cm^(-2).In addition,the Li|LiFePO_(4)(LFP) SSBs achieve favorable cycling performance:the specific capacity reaches128.1 mAh g^(-1) at 0.5 C rate,with a capacity retention of about 80% after 600 cycles.In the further tests of the LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811) cathodes with higher energy density,the Nano LLZO CSEs also demonstrate good compatibility:the specific capacities of NCM811-based SSBs reach 177.9 mAh g^(-1) at 0.5 C rate,while the capacity retention is over 96% after 150 cycles.Furthermore,the Li|LFP soft-pack SSBs verify the safety characteristics and the potential for application,which have a desirable prospect.展开更多
Mordenite with different Si/Al ratios were synthesized by solvent-free method and used for dimethyl ether(DME)carbonylation reaction.The influence of Si/Al ratio in the feedstock on the structure,porosity and acid sit...Mordenite with different Si/Al ratios were synthesized by solvent-free method and used for dimethyl ether(DME)carbonylation reaction.The influence of Si/Al ratio in the feedstock on the structure,porosity and acid sites were systematically investigated.The characterization results showed that with the increase of Si/Al ratio in the feedstock,part of silicon species fail to enter the skeleton and the specific surface area and pore volume of the samples decreased.The amount of weak acid and medium strong acid decreased alongside with the increasing Si/Al ratio,and the amount of strong acid slightly increased.The Al atoms preferentially enter the strong acid sites in the 8 member ring(MR)channel during the crystallization process.The high Si/Al ratio sample had more acid sites located in the 8 MR channel,leading to more active sites for carbonylation reaction and higher catalytic performance.Appropriately increasing the Si/Al ratio was beneficial for the improvement of carbonylation reaction activity over the mordenite(MOR)catalyst.展开更多
A facile procedure for the synthesis, of quinoxalines is being reported starting from benzil and 1,2-diaminobenzene. The reactions were carried out catalyst-free, solvent-free and under microwave irradiation condition...A facile procedure for the synthesis, of quinoxalines is being reported starting from benzil and 1,2-diaminobenzene. The reactions were carried out catalyst-free, solvent-free and under microwave irradiation conditions in high yield （84-98%） with short time （3-6 min） and environmental benign, as well as convenient operation. The structures of all the compounds have been confirmed on the basis of their IR, 1H NMR, and/or 13C NMR, mass spectral data.展开更多
Designing efficient adsorbents for the deep removal of refractory dibenzothiophene(DBT)from fuel oil is vital for addressing environmental issues such as acid rain.Herein,zinc gluconate and urea-derived porous carbons...Designing efficient adsorbents for the deep removal of refractory dibenzothiophene(DBT)from fuel oil is vital for addressing environmental issues such as acid rain.Herein,zinc gluconate and urea-derived porous carbons SF-ZnNC-T(T represents the carbonization temperature)were synthesized without solvents.Through a temperature-controlled process of“melting the zinc gluconate and urea mixture,forming H-bonded polymers,and carbonizing the polymers,”the optimal carbon,SF-ZnNC-900,was obtained with a large surface area(2280 m^(2)g^(-1),highly dispersed Zn sites,and hierarchical pore structures.Consequently,SF-ZnNC-900 demonstrated significantly higher DBT adsorption capacity of43.2 mg S g^(-1),compared to just 4.3 mg S g^(-1)for the precursor.It also demonstrated good reusability,fast adsorption rate,and the ability for ultra-deep desulfurization.The superior DBT adsorption performance resulted from the evaporation of residual zinc species,which generated abundant mesopores that facilitated DBT transformation,as well as the formation of Zn-N_(x) sites that strengthened the host-vip interaction(ΔE=-1.466 e V).The solvent-free synthesized highly dispersed Zn-doped carbon shows great potential for producing sulfur-free fuel oil and for designing metal-loaded carbon adsorbents.展开更多
Bioinspired active pillar structures,known for their large surface area,mechanical compliance,and diverse deformation modes,have garnered extensive research interest.Among various active pillar structures,liquid cryst...Bioinspired active pillar structures,known for their large surface area,mechanical compliance,and diverse deformation modes,have garnered extensive research interest.Among various active pillar structures,liquid crystal elastomer(LCE)pillar arrays are capable of exhibiting significant and reversible anisotropic deformation under cyclic heating and cooling,showing great potential in tunable adhesion,soft robots,and biomedical devices.However,scaling up LCE pillar manufacturing remains challenging,limiting its practical applications.In this work,a solventfree LCE resin is developed with unique features including simple operating procedure,short fabrication time,and tunable responsive temperature,enabling rapid and large-scale production of LCE pillar arrays.The LCE resin allows for the preparation of complex 3D shapes in addition to film or specimen.The fabrication time can be as short as 4 h,without the need to evaporate solvent.Moreover,the LCE resins can be adjusted with a variable phase transition temperature range from 49.4℃ to 97.7℃ by incorporating non-liquid crystal acrylate chains.The resulting active pillar array structure can undertake sequential actuation upon heating with the tunable actuation temperature.Finally,the application of these pillar arrays in multi-level information encryption is demonstrated.The LCE pillar structure introduced here offers a new strategy for constructing advanced active LCE structures with tunable responsive behavior.展开更多
The imperative pursuit of elevated energy density in lithium primary coin cells(LPCCs)necessitates strategic architectural optimization to align with evolving market demands.A predominant approach involves the systema...The imperative pursuit of elevated energy density in lithium primary coin cells(LPCCs)necessitates strategic architectural optimization to align with evolving market demands.A predominant approach involves the systematic replacement of metallic structural support components(MSSCs)to minimize non-active constituent ratios,contingent upon maintaining robust interfacial contact integrity among electrodes,separators,and battery shells.Herein,we present a novel LPCC configuration employing solvent-free processed ultra-thick fluorinated carbon cathode(UCFxC)to achieve complete MSSCs elimination.The engineered UCFxC demonstrates exceptional areal capacity metrics(249.45 mg cm^(-2),215.77 m Ah cm^(-2)),enabling a 27.8% mass reduction compared with conventional laboratoryassembled coin cell while achieving 941.5% energy density enhancement through optimized electrode conductivity.Notably,single-walled carbon nanotube(SWCNT)-modified UCFxC architectures exhibited superior performance with energy exceeding 1.0 Wh at 50℃.This architectural paradigm provides valuable insights for developing next-generation high-energy-density LPCC systems,with practical implications for advancing miniaturized power source technologies.展开更多
Slurry casting has been used to fabricate lithium-ion battery electrodes for decades,which involves toxic and expensive organic solvents followed by high-cost vacuum drying and electrode calendering.This work presents...Slurry casting has been used to fabricate lithium-ion battery electrodes for decades,which involves toxic and expensive organic solvents followed by high-cost vacuum drying and electrode calendering.This work presents a new manufacturing method using a nonthermal plasma to create inter-particle binding without using any polymeric binding materials,enabling solvent-free manufacturing electrodes with any electrochemistry of choice.The cold-plasma-coating technique enables fabricating electrodes with thickness(>200 pm),high mass loading(>30 mg cm^(-2)),high peel strength,and the ability to print lithium-ion batteries in an arbitrary geometry.This crosscutting,chemistry agnostic,platform technology would increase energy density,eliminate the use of solvents,vacuum drying,and calendering processes during production,and reduce manufacturing cost for current and future cell designs.Here,lithium iron phosphate and lithium cobalt oxide were used as examples to demonstrate the efficacy of the cold-plasma-coating technique.It is found that the mechanical peel strength of cold-plasma-coating-manufactured lithium iron phosphate is over an order of magnitude higher than that of slurry-casted lithium iron phosphate electrodes.Full cells assembled with a graphite anode and the cold-plasma-coating-lithium iron phosphate cathode offer highly reversible cycling performance with a capacity retention of 81.6%over 500 cycles.For the highly conductive cathode material lithium cobalt oxide,an areal capacity of 4.2 mAh cm^(-2)at 0.2 C is attained.We anticipate that this new,highly scalable manufacturing technique will redefine global lithium-ion battery manufacturing providing significantly reduced plant footprints and material costs.展开更多
The rheological properties and limited flow velocities of solvent-free nanofluids are crucial for their technologically significant applications.In particular,the flow in a solvent-free nanofluid system is steady only...The rheological properties and limited flow velocities of solvent-free nanofluids are crucial for their technologically significant applications.In particular,the flow in a solvent-free nanofluid system is steady only when the flow velocity is lower than a critical value.In this paper,we establish a rigid-flexible dynamic model to investigate the existence of the upper bound on the steady flow velocities for three solvent-free nanofluid systems.Then,the effects of the structural parameters on the upper bound on the steady flow velocities are examined with the proposed structure-preserving method.It is found that each of these solvent-free nanofluid systems has an upper bound on the steady flow velocity,which exhibits distinct dependence on their structural parameters,such as the graft density of branch chains and the size of the cores.In addition,among the three types of solvent-free nanofluids,the magnetic solvent-free nanofluid poses the largest upper bound on the steady flow velocity,demonstrating that it is a better choice when a large flow velocity is required in real applications.展开更多
Full-color emissive carbon dots(CDs)hold a great promise for various applications,especially in light emitting diodes(LEDs).However,the existing synthetic routes for CDs are carried out in solutions,which suffer from ...Full-color emissive carbon dots(CDs)hold a great promise for various applications,especially in light emitting diodes(LEDs).However,the existing synthetic routes for CDs are carried out in solutions,which suffer from low yields,high pressures,various byproducts,large amounts of waste solvents,and complicated photoluminescence(PL)origins.Therefore,it is necessary to explore large scale synthesis of CDs with high quantum yield(QY)across the entire visible range from a single carbon source by a solvent-free method.In this work,a series of CDs with tunable PL emission from 442 to 621 nm,QY of 23%-56%,and production yield within 34%-72%,are obtained by heating o-phenylenediamine with the catalysis of KCl.Detailed characterizations identify that,the differences between these CDs with respect to the graphitization degree,graphitic nitrogen content,and oxygen-containing functional groups,are responsible for their distinct optical properties,which can be modulated by controlling the deamination and dehydrogenation processes during reactions.Blue,green,yellow,red emissive films,and LEDs are prepared by dispersing the corresponding CDs into polyvinyl alcohol(PVA).All types of white LEDs(WLEDs)with high colorrendering-index(CRI),including warm WLEDs,standard WLEDs,and cool WLEDs,are also fabricated by mixing the red,green,and blue emissive CDs into PVA matrix by the appropriate ratios.展开更多
Generating hollow structure inside titanium silicalite-1(TS-1)is a widely used method to improve its liquid-phase oxidation catalytic performance in industry.However,traditional dissolution-recrystallization method us...Generating hollow structure inside titanium silicalite-1(TS-1)is a widely used method to improve its liquid-phase oxidation catalytic performance in industry.However,traditional dissolution-recrystallization method usually required a large amount of aqueous solution of organic template,leading to unfavorable polluted waste,low production efficiency,and high manufacture cost.Here,a facile and environmental friendly strategy was proposed for the post-synthesis of hollow TS-1 zeolite with a solventfree method utilizing NH4HCO3 and tetrapropylammounium bromide as selective etching agents,which reduced the usage of organic template and avoided the liquid waste.The high crystallinity,the microporous structure,and the active Ti sites were preserved at a high product yield(>93%).The formation mechanism of hollow structure was also investigated by exploring effects of different reactants and experimental parameters.Meanwhile,the obtained hollow TS-1 showed an outstanding performance in the epoxidation of 1-hexene in comparison to the parent zeolite.展开更多
Single-ion conductors based on covalent organic frameworks(COFs)have garnered attention as a potential alternative to currently prevalent inorganic ion conductors owing to their structural uniqueness and chemical vers...Single-ion conductors based on covalent organic frameworks(COFs)have garnered attention as a potential alternative to currently prevalent inorganic ion conductors owing to their structural uniqueness and chemical versatility.However,the sluggish Li+conduction has hindered their practical applications.Here,we present a class of solvent-free COF single-ion conductors(Li-COF@P)based on weak ion-dipole interaction as opposed to traditional strong ion-ion interaction.The ion(Li+from the COF)-dipole(oxygen from poly(ethylene glycol)diacrylate embedded in the COF pores)interaction in the Li-COF@P promotes ion dissociation and Li+migration via directional ionic channels.Driven by this single-ion transport behavior,the Li-COF@P enables reversible Li plating/stripping on Li-metal electrodes and stable cycling performance(88.3%after 2000 cycles)in organic batteries(Li metal anode||5,5’-dimethyl-2,2’-bis-p-benzoquinone(Me2BBQ)cathode)under ambient operating conditions,highlighting the electrochemical viability of the Li-COF@P for all-solid-state organic batteries.展开更多
To analyze the differences in the transport and distribution of different types of proppants and to address issues such as the short effective support of proppant and poor placement in hydraulically intersecting fract...To analyze the differences in the transport and distribution of different types of proppants and to address issues such as the short effective support of proppant and poor placement in hydraulically intersecting fractures,this study considered the combined impact of geological-engineering factors on conductivity.Using reservoir production parameters and the discrete elementmethod,multispherical proppants were constructed.Additionally,a 3D fracture model,based on the specified conditions of the L block,employed coupled(Computational Fluid Dynamics)CFD-DEM(Discrete ElementMethod)for joint simulations to quantitatively analyze the transport and placement patterns of multispherical proppants in intersecting fractures.Results indicate that turbulent kinetic energy is an intrinsic factor affecting proppant transport.Moreover,the efficiency of placement and migration distance of low-sphericity quartz sand constructed by the DEM in the main fracture are significantly reduced compared to spherical ceramic proppants,with a 27.7%decrease in the volume fraction of the fracture surface,subsequently affecting the placement concentration and damaging fracture conductivity.Compared to small-angle fractures,controlling artificial and natural fractures to expand at angles of 45°to 60°increases the effective support length by approximately 20.6%.During hydraulic fracturing of gas wells,ensuring the fracture support area and post-closure conductivity can be achieved by controlling the sphericity of proppants and adjusting the perforation direction to control the direction of artificial fractures.展开更多
This study investigated the physicochemical properties,enzyme activities,volatile flavor components,microbial communities,and sensory evaluation of high-temperature Daqu(HTD)during the maturation process,and a standar...This study investigated the physicochemical properties,enzyme activities,volatile flavor components,microbial communities,and sensory evaluation of high-temperature Daqu(HTD)during the maturation process,and a standard system was established for comprehensive quality evaluation of HTD.There were obvious changes in the physicochemical properties,enzyme activities,and volatile flavor components at different storage periods,which affected the sensory evaluation of HTD to a certain extent.The results of high-throughput sequencing revealed significant microbial diversity,and showed that the bacterial community changed significantly more than did the fungal community.During the storage process,the dominant bacterial genera were Kroppenstedtia and Thermoascus.The correlation between dominant microorganisms and quality indicators highlighted their role in HTD quality.Lactococcus,Candida,Pichia,Paecilomyces,and protease activity played a crucial role in the formation of isovaleraldehyde.Acidic protease activity had the greatest impact on the microbial community.Moisture promoted isobutyric acid generation.Furthermore,the comprehensive quality evaluation standard system was established by the entropy weight method combined with multi-factor fuzzy mathematics.Consequently,this study provides innovative insights for comprehensive quality evaluation of HTD during storage and establishes a groundwork for scientific and rational storage of HTD and quality control of sauce-flavor Baijiu.展开更多
Due to the heterogeneity of rock masses and the variability of in situ stress,the traditional linear inversion method is insufficiently accurate to achieve high accuracy of the in situ stress field.To address this cha...Due to the heterogeneity of rock masses and the variability of in situ stress,the traditional linear inversion method is insufficiently accurate to achieve high accuracy of the in situ stress field.To address this challenge,nonlinear stress boundaries for a numerical model are determined through regression analysis of a series of nonlinear coefficient matrices,which are derived from the bubbling method.Considering the randomness and flexibility of the bubbling method,a parametric study is conducted to determine recommended ranges for these parameters,including the standard deviation(σb)of bubble radii,the non-uniform coefficient matrix number(λ)for nonlinear stress boundaries,and the number(m)and positions of in situ stress measurement points.A model case study provides a reference for the selection of these parameters.Additionally,when the nonlinear in situ stress inversion method is employed,stress distortion inevitably occurs near model boundaries,aligning with the Saint Venant's principle.Two strategies are proposed accordingly:employing a systematic reduction of nonlinear coefficients to achieve high inversion accuracy while minimizing significant stress distortion,and excluding regions with severe stress distortion near the model edges while utilizing the central part of the model for subsequent simulations.These two strategies have been successfully implemented in the nonlinear in situ stress inversion of the Xincheng Gold Mine and have achieved higher inversion accuracy than the linear method.Specifically,the linear and nonlinear inversion methods yield root mean square errors(RMSE)of 4.15 and 3.2,and inversion relative errors(δAve)of 22.08%and 17.55%,respectively.Therefore,the nonlinear inversion method outperforms the traditional multiple linear regression method,even in the presence of a systematic reduction in the nonlinear stress boundaries.展开更多
Several ternary oxides CuCeZrO_(y)(CCZ)were synthesized by a facile grinding method followed by calcination at high temperatures,and used as catalysts for CO oxidation at low temperatures.The influences of calcination...Several ternary oxides CuCeZrO_(y)(CCZ)were synthesized by a facile grinding method followed by calcination at high temperatures,and used as catalysts for CO oxidation at low temperatures.The influences of calcination temperature(400-600℃)on the physicochemical properties of the assynthesized ternary oxides were investigated by thermogravimetric analysis/differential scanning calorimetry(TGA/DSC),X-ray diffraction(XRD),transmission electron microscopy(TEM),Raman,inductively coupled plasma-optical emission spectrometry(ICP-OES),N_(2) adsorption,H_(2)-temperature programmed reduction(H_(2)-TPR),and X-ray photoelectron spectroscopy(XPS)characterizations.The results show that the increase in calcination temperature from 400 to 500℃is conducive to the high dispersion of CuOx on catalyst surface and the incorporation of Cu species into the support to form the Cu-Ce-Zr-O solid solution.Further raising of calcination temperature from 500 to 600℃,however,leads to the segregation of Cu species from the solid solution to aggregate on support surface and growth of highly dispersed CuOx nanoparticles.The highest catalytic activity is acquired over the CCZ calcined at 500℃,which can be ascribed to the largest contents of Cu+species and oxygen vacancies owing to the formation of the maximum amount of Cu-Ce-Zr-O solid solution.展开更多
The separation-of-variable(SOV)methods,such as the improved SOV method,the variational SOV method,and the extended SOV method,have been proposed by the present authors and coworkers to obtain the closed-form analytica...The separation-of-variable(SOV)methods,such as the improved SOV method,the variational SOV method,and the extended SOV method,have been proposed by the present authors and coworkers to obtain the closed-form analytical solutions for free vibration and eigenbuckling of rectangular plates and circular cylindrical shells.By taking the free vibration of rectangular thin plates as an example,this work presents the theoretical framework of the SOV methods in an instructive way,and the bisection–based solution procedures for a group of nonlinear eigenvalue equations.Besides,the explicit equations of nodal lines of the SOV methods are presented,and the relations of nodal line patterns and frequency orders are investigated.It is concluded that the highly accurate SOV methods have the same accuracy for all frequencies,the mode shapes about repeated frequencies can also be precisely captured,and the SOV methods do not have the problem of missing roots as well.展开更多
Soil improvement is one of the most important issues in geotechnical engineering practice.The wide application of traditional improvement techniques(cement/chemical materials)are limited due to damage ecological en-vi...Soil improvement is one of the most important issues in geotechnical engineering practice.The wide application of traditional improvement techniques(cement/chemical materials)are limited due to damage ecological en-vironment and intensify carbon emissions.However,the use of microbially induced calcium carbonate pre-cipitation(MICP)to obtain bio-cement is a novel technique with the potential to induce soil stability,providing a low-carbon,environment-friendly,and sustainable integrated solution for some geotechnical engineering pro-blems in the environment.This paper presents a comprehensive review of the latest progress in soil improvement based on the MICP strategy.It systematically summarizes and overviews the mineralization mechanism,influ-encing factors,improved methods,engineering characteristics,and current field application status of the MICP.Additionally,it also explores the limitations and correspondingly proposes prospective applications via the MICP approach for soil improvement.This review indicates that the utilization of different environmental calcium-based wastes in MICP and combination of materials and MICP are conducive to meeting engineering and market demand.Furthermore,we recommend and encourage global collaborative study and practice with a view to commercializing MICP technique in the future.The current review purports to provide insights for engineers and interdisciplinary researchers,and guidance for future engineering applications.展开更多
A facile procedure for the synthesis of 2,4,5-lriarylimidazoles is being reported starting from benzil, aromatic aldehyde and ammonium acetate. The reactions were carried out with catalyst-free, solvent-free and under...A facile procedure for the synthesis of 2,4,5-lriarylimidazoles is being reported starting from benzil, aromatic aldehyde and ammonium acetate. The reactions were carried out with catalyst-free, solvent-free and under microwave irradiation conditions in high yield （80-99%） with short time （3-5 min） and environmental benign, as well as convenient operation. The structures of the compounds have been confirmed on the basis of their IR, 1H NMR, and/or 13C NMR, MS, and elemental analyzer.展开更多
Bearing is an indispensable key component in mechanical equipment,and its working state is directly related to the stability and safety of the whole equipment.In recent years,with the rapid development of artificial i...Bearing is an indispensable key component in mechanical equipment,and its working state is directly related to the stability and safety of the whole equipment.In recent years,with the rapid development of artificial intelligence technology,especially the breakthrough of deep learning technology,it provides a new idea for bearing fault diagnosis.Deep learning can automatically learn features from a large amount of data,has a strong nonlinear modeling ability,and can effectively solve the problems existing in traditional methods.Aiming at the key problems in bearing fault diagnosis,this paper studies the fault diagnosis method based on deep learning,which not only provides a new solution for bearing fault diagnosis but also provides a reference for the application of deep learning in other mechanical fault diagnosis fields.展开更多
基金supported by Science and Technology Project of China Southern Power Grid (SZKJXM20230049/090000KC23010038)。
文摘Solid-state batteries(SSBs) with high safety are promising for the energy fields,but the development has long been limited by machinability and interfacial problems.Hence,self-supporting,flexible Nano LLZO CSEs are prepared with a solvent-free method at 25℃.The 99.8 wt% contents of Nano LLZO particles enable the Nano LLZO CSEs to maintain good thermal stability while exhibiting a wide electrochemical window of 5.0 V and a high Li~+ transfer number of 0.8.The mean modulus reaches 4376 MPa.Benefiting from the interfacial modulation,the Li|Li symmetric batteries based on the Nano LLZO CSEs show benign stability with lithium at the current densities of 0.1 mA cm^(-2),0.2 mA cm^(-2),and 0.5 mA cm^(-2).In addition,the Li|LiFePO_(4)(LFP) SSBs achieve favorable cycling performance:the specific capacity reaches128.1 mAh g^(-1) at 0.5 C rate,with a capacity retention of about 80% after 600 cycles.In the further tests of the LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811) cathodes with higher energy density,the Nano LLZO CSEs also demonstrate good compatibility:the specific capacities of NCM811-based SSBs reach 177.9 mAh g^(-1) at 0.5 C rate,while the capacity retention is over 96% after 150 cycles.Furthermore,the Li|LFP soft-pack SSBs verify the safety characteristics and the potential for application,which have a desirable prospect.
基金supported by China National Natural Science Foundation(22008260,21908123)。
文摘Mordenite with different Si/Al ratios were synthesized by solvent-free method and used for dimethyl ether(DME)carbonylation reaction.The influence of Si/Al ratio in the feedstock on the structure,porosity and acid sites were systematically investigated.The characterization results showed that with the increase of Si/Al ratio in the feedstock,part of silicon species fail to enter the skeleton and the specific surface area and pore volume of the samples decreased.The amount of weak acid and medium strong acid decreased alongside with the increasing Si/Al ratio,and the amount of strong acid slightly increased.The Al atoms preferentially enter the strong acid sites in the 8 member ring(MR)channel during the crystallization process.The high Si/Al ratio sample had more acid sites located in the 8 MR channel,leading to more active sites for carbonylation reaction and higher catalytic performance.Appropriately increasing the Si/Al ratio was beneficial for the improvement of carbonylation reaction activity over the mordenite(MOR)catalyst.
基金Jiangsu Key Laboratory for Chemistry of Low-Dimensional Materials for financial support(No.JSKC07041)
文摘A facile procedure for the synthesis, of quinoxalines is being reported starting from benzil and 1,2-diaminobenzene. The reactions were carried out catalyst-free, solvent-free and under microwave irradiation conditions in high yield （84-98%） with short time （3-6 min） and environmental benign, as well as convenient operation. The structures of all the compounds have been confirmed on the basis of their IR, 1H NMR, and/or 13C NMR, mass spectral data.
基金supported by the National Natural Science Foundation of China(Grant No.22378065,22278077,22278076)。
文摘Designing efficient adsorbents for the deep removal of refractory dibenzothiophene(DBT)from fuel oil is vital for addressing environmental issues such as acid rain.Herein,zinc gluconate and urea-derived porous carbons SF-ZnNC-T(T represents the carbonization temperature)were synthesized without solvents.Through a temperature-controlled process of“melting the zinc gluconate and urea mixture,forming H-bonded polymers,and carbonizing the polymers,”the optimal carbon,SF-ZnNC-900,was obtained with a large surface area(2280 m^(2)g^(-1),highly dispersed Zn sites,and hierarchical pore structures.Consequently,SF-ZnNC-900 demonstrated significantly higher DBT adsorption capacity of43.2 mg S g^(-1),compared to just 4.3 mg S g^(-1)for the precursor.It also demonstrated good reusability,fast adsorption rate,and the ability for ultra-deep desulfurization.The superior DBT adsorption performance resulted from the evaporation of residual zinc species,which generated abundant mesopores that facilitated DBT transformation,as well as the formation of Zn-N_(x) sites that strengthened the host-vip interaction(ΔE=-1.466 e V).The solvent-free synthesized highly dispersed Zn-doped carbon shows great potential for producing sulfur-free fuel oil and for designing metal-loaded carbon adsorbents.
基金financially supported by the National Key Research and Development Program of China(No.2023YFB3812500)the National Natural Science Foundation of China(No.52105003)the Beijing Municipal Natural Science Foundation(No.2222058)。
文摘Bioinspired active pillar structures,known for their large surface area,mechanical compliance,and diverse deformation modes,have garnered extensive research interest.Among various active pillar structures,liquid crystal elastomer(LCE)pillar arrays are capable of exhibiting significant and reversible anisotropic deformation under cyclic heating and cooling,showing great potential in tunable adhesion,soft robots,and biomedical devices.However,scaling up LCE pillar manufacturing remains challenging,limiting its practical applications.In this work,a solventfree LCE resin is developed with unique features including simple operating procedure,short fabrication time,and tunable responsive temperature,enabling rapid and large-scale production of LCE pillar arrays.The LCE resin allows for the preparation of complex 3D shapes in addition to film or specimen.The fabrication time can be as short as 4 h,without the need to evaporate solvent.Moreover,the LCE resins can be adjusted with a variable phase transition temperature range from 49.4℃ to 97.7℃ by incorporating non-liquid crystal acrylate chains.The resulting active pillar array structure can undertake sequential actuation upon heating with the tunable actuation temperature.Finally,the application of these pillar arrays in multi-level information encryption is demonstrated.The LCE pillar structure introduced here offers a new strategy for constructing advanced active LCE structures with tunable responsive behavior.
基金the financial support from the National Natural Science Foundation of China,Grant Nos.52307249the Natural Science Foundation of Shanghai Province,Nos.23ZR1465900+2 种基金the Chenguang Program of Shanghai Education Development Foundation and Shanghai Municipal Education Commission,Nos.23CGA25the Fundamental Research Funds for the Central Universities at Tongji University,Nos.PA2022000668/22120220426the Nanchang Automotive Institute of Intelligence&New Energy of Tongji University,Nos.TPD-TC202211-02。
文摘The imperative pursuit of elevated energy density in lithium primary coin cells(LPCCs)necessitates strategic architectural optimization to align with evolving market demands.A predominant approach involves the systematic replacement of metallic structural support components(MSSCs)to minimize non-active constituent ratios,contingent upon maintaining robust interfacial contact integrity among electrodes,separators,and battery shells.Herein,we present a novel LPCC configuration employing solvent-free processed ultra-thick fluorinated carbon cathode(UCFxC)to achieve complete MSSCs elimination.The engineered UCFxC demonstrates exceptional areal capacity metrics(249.45 mg cm^(-2),215.77 m Ah cm^(-2)),enabling a 27.8% mass reduction compared with conventional laboratoryassembled coin cell while achieving 941.5% energy density enhancement through optimized electrode conductivity.Notably,single-walled carbon nanotube(SWCNT)-modified UCFxC architectures exhibited superior performance with energy exceeding 1.0 Wh at 50℃.This architectural paradigm provides valuable insights for developing next-generation high-energy-density LPCC systems,with practical implications for advancing miniaturized power source technologies.
基金the financial support from Intecells Inc.via an award number AWD_19-08-0127the support from Paul M.Rady Mechanical Engineering Department at University of Colorado Boulder
文摘Slurry casting has been used to fabricate lithium-ion battery electrodes for decades,which involves toxic and expensive organic solvents followed by high-cost vacuum drying and electrode calendering.This work presents a new manufacturing method using a nonthermal plasma to create inter-particle binding without using any polymeric binding materials,enabling solvent-free manufacturing electrodes with any electrochemistry of choice.The cold-plasma-coating technique enables fabricating electrodes with thickness(>200 pm),high mass loading(>30 mg cm^(-2)),high peel strength,and the ability to print lithium-ion batteries in an arbitrary geometry.This crosscutting,chemistry agnostic,platform technology would increase energy density,eliminate the use of solvents,vacuum drying,and calendering processes during production,and reduce manufacturing cost for current and future cell designs.Here,lithium iron phosphate and lithium cobalt oxide were used as examples to demonstrate the efficacy of the cold-plasma-coating technique.It is found that the mechanical peel strength of cold-plasma-coating-manufactured lithium iron phosphate is over an order of magnitude higher than that of slurry-casted lithium iron phosphate electrodes.Full cells assembled with a graphite anode and the cold-plasma-coating-lithium iron phosphate cathode offer highly reversible cycling performance with a capacity retention of 81.6%over 500 cycles.For the highly conductive cathode material lithium cobalt oxide,an areal capacity of 4.2 mAh cm^(-2)at 0.2 C is attained.We anticipate that this new,highly scalable manufacturing technique will redefine global lithium-ion battery manufacturing providing significantly reduced plant footprints and material costs.
基金Project supported by the National Natural Science Foundation of China(No.12172281)the Fund of the Science and Technology Innovation Team of Shaanxi Province of China(No.2022TD-61)+2 种基金the Open Project of State Key Laboratory of Performance Monitoring and Protecting of Rail Transit InfrastructureEast China Jiaotong University(No.HJGZ2023102)the Shaanxi Province Key Research and Development Project(No.2024SFYBXM-531)。
文摘The rheological properties and limited flow velocities of solvent-free nanofluids are crucial for their technologically significant applications.In particular,the flow in a solvent-free nanofluid system is steady only when the flow velocity is lower than a critical value.In this paper,we establish a rigid-flexible dynamic model to investigate the existence of the upper bound on the steady flow velocities for three solvent-free nanofluid systems.Then,the effects of the structural parameters on the upper bound on the steady flow velocities are examined with the proposed structure-preserving method.It is found that each of these solvent-free nanofluid systems has an upper bound on the steady flow velocity,which exhibits distinct dependence on their structural parameters,such as the graft density of branch chains and the size of the cores.In addition,among the three types of solvent-free nanofluids,the magnetic solvent-free nanofluid poses the largest upper bound on the steady flow velocity,demonstrating that it is a better choice when a large flow velocity is required in real applications.
基金This work was financially supported by the National Natural Science Foundation of China(Nos.51803233,21771039,and 21975048)China Postdoctoral Science Foundation(No.2019M651999).
文摘Full-color emissive carbon dots(CDs)hold a great promise for various applications,especially in light emitting diodes(LEDs).However,the existing synthetic routes for CDs are carried out in solutions,which suffer from low yields,high pressures,various byproducts,large amounts of waste solvents,and complicated photoluminescence(PL)origins.Therefore,it is necessary to explore large scale synthesis of CDs with high quantum yield(QY)across the entire visible range from a single carbon source by a solvent-free method.In this work,a series of CDs with tunable PL emission from 442 to 621 nm,QY of 23%-56%,and production yield within 34%-72%,are obtained by heating o-phenylenediamine with the catalysis of KCl.Detailed characterizations identify that,the differences between these CDs with respect to the graphitization degree,graphitic nitrogen content,and oxygen-containing functional groups,are responsible for their distinct optical properties,which can be modulated by controlling the deamination and dehydrogenation processes during reactions.Blue,green,yellow,red emissive films,and LEDs are prepared by dispersing the corresponding CDs into polyvinyl alcohol(PVA).All types of white LEDs(WLEDs)with high colorrendering-index(CRI),including warm WLEDs,standard WLEDs,and cool WLEDs,are also fabricated by mixing the red,green,and blue emissive CDs into PVA matrix by the appropriate ratios.
基金This work was supported by the National Natural Science Foundation of China(Nos.21875140,21835002,21522105,and 51861145313)the Shanghai Science and Technology Plan(No.21DZ2260400)+4 种基金the China Ministry of Science and Technology(No.2021YFA1501401)The authors thank the support from Analytical Instrumentation Center(No.SPSTAIC10112914)SPST,ShanghaiTech UniversityThe authors also thank Prof.Osamu Terasaki and CħEM SPST,ShanghaiTech University(No.EM02161943)for scientific and characterization support.Y.F.thanks Junyan Li(Jilin University)for his assistance in 3D tomographic data collection.
文摘Generating hollow structure inside titanium silicalite-1(TS-1)is a widely used method to improve its liquid-phase oxidation catalytic performance in industry.However,traditional dissolution-recrystallization method usually required a large amount of aqueous solution of organic template,leading to unfavorable polluted waste,low production efficiency,and high manufacture cost.Here,a facile and environmental friendly strategy was proposed for the post-synthesis of hollow TS-1 zeolite with a solventfree method utilizing NH4HCO3 and tetrapropylammounium bromide as selective etching agents,which reduced the usage of organic template and avoided the liquid waste.The high crystallinity,the microporous structure,and the active Ti sites were preserved at a high product yield(>93%).The formation mechanism of hollow structure was also investigated by exploring effects of different reactants and experimental parameters.Meanwhile,the obtained hollow TS-1 showed an outstanding performance in the epoxidation of 1-hexene in comparison to the parent zeolite.
基金supported by the Basic Science Research Program (No.RS-2024-00344021) through the National Research Foundation of Korea (NRF) funded by the Ministry of Science, ICT and future Planningthe financial support from the National Natural Science Foundation of China (52103277)+2 种基金the Program for Science & Technology Innovation Talents in Universities of Henan Province (23HASTIT015)Natural Science Foundation of Henan Province (242300421073)supported by the Technology Innovation Program (20010960) funded by the Ministry of Trade, Industry & Energy (MOTIE, Korea)
文摘Single-ion conductors based on covalent organic frameworks(COFs)have garnered attention as a potential alternative to currently prevalent inorganic ion conductors owing to their structural uniqueness and chemical versatility.However,the sluggish Li+conduction has hindered their practical applications.Here,we present a class of solvent-free COF single-ion conductors(Li-COF@P)based on weak ion-dipole interaction as opposed to traditional strong ion-ion interaction.The ion(Li+from the COF)-dipole(oxygen from poly(ethylene glycol)diacrylate embedded in the COF pores)interaction in the Li-COF@P promotes ion dissociation and Li+migration via directional ionic channels.Driven by this single-ion transport behavior,the Li-COF@P enables reversible Li plating/stripping on Li-metal electrodes and stable cycling performance(88.3%after 2000 cycles)in organic batteries(Li metal anode||5,5’-dimethyl-2,2’-bis-p-benzoquinone(Me2BBQ)cathode)under ambient operating conditions,highlighting the electrochemical viability of the Li-COF@P for all-solid-state organic batteries.
基金funded by the project of the Major Scientific and Technological Projects of CNOOC in the 14th Five-Year Plan(No.KJGG2022-0701)the CNOOC Research Institute(No.2020PFS-03).
文摘To analyze the differences in the transport and distribution of different types of proppants and to address issues such as the short effective support of proppant and poor placement in hydraulically intersecting fractures,this study considered the combined impact of geological-engineering factors on conductivity.Using reservoir production parameters and the discrete elementmethod,multispherical proppants were constructed.Additionally,a 3D fracture model,based on the specified conditions of the L block,employed coupled(Computational Fluid Dynamics)CFD-DEM(Discrete ElementMethod)for joint simulations to quantitatively analyze the transport and placement patterns of multispherical proppants in intersecting fractures.Results indicate that turbulent kinetic energy is an intrinsic factor affecting proppant transport.Moreover,the efficiency of placement and migration distance of low-sphericity quartz sand constructed by the DEM in the main fracture are significantly reduced compared to spherical ceramic proppants,with a 27.7%decrease in the volume fraction of the fracture surface,subsequently affecting the placement concentration and damaging fracture conductivity.Compared to small-angle fractures,controlling artificial and natural fractures to expand at angles of 45°to 60°increases the effective support length by approximately 20.6%.During hydraulic fracturing of gas wells,ensuring the fracture support area and post-closure conductivity can be achieved by controlling the sphericity of proppants and adjusting the perforation direction to control the direction of artificial fractures.
文摘This study investigated the physicochemical properties,enzyme activities,volatile flavor components,microbial communities,and sensory evaluation of high-temperature Daqu(HTD)during the maturation process,and a standard system was established for comprehensive quality evaluation of HTD.There were obvious changes in the physicochemical properties,enzyme activities,and volatile flavor components at different storage periods,which affected the sensory evaluation of HTD to a certain extent.The results of high-throughput sequencing revealed significant microbial diversity,and showed that the bacterial community changed significantly more than did the fungal community.During the storage process,the dominant bacterial genera were Kroppenstedtia and Thermoascus.The correlation between dominant microorganisms and quality indicators highlighted their role in HTD quality.Lactococcus,Candida,Pichia,Paecilomyces,and protease activity played a crucial role in the formation of isovaleraldehyde.Acidic protease activity had the greatest impact on the microbial community.Moisture promoted isobutyric acid generation.Furthermore,the comprehensive quality evaluation standard system was established by the entropy weight method combined with multi-factor fuzzy mathematics.Consequently,this study provides innovative insights for comprehensive quality evaluation of HTD during storage and establishes a groundwork for scientific and rational storage of HTD and quality control of sauce-flavor Baijiu.
基金funded by the National Key R&D Program of China(Grant No.2022YFC2903904)the National Natural Science Foundation of China(Grant Nos.51904057 and U1906208).
文摘Due to the heterogeneity of rock masses and the variability of in situ stress,the traditional linear inversion method is insufficiently accurate to achieve high accuracy of the in situ stress field.To address this challenge,nonlinear stress boundaries for a numerical model are determined through regression analysis of a series of nonlinear coefficient matrices,which are derived from the bubbling method.Considering the randomness and flexibility of the bubbling method,a parametric study is conducted to determine recommended ranges for these parameters,including the standard deviation(σb)of bubble radii,the non-uniform coefficient matrix number(λ)for nonlinear stress boundaries,and the number(m)and positions of in situ stress measurement points.A model case study provides a reference for the selection of these parameters.Additionally,when the nonlinear in situ stress inversion method is employed,stress distortion inevitably occurs near model boundaries,aligning with the Saint Venant's principle.Two strategies are proposed accordingly:employing a systematic reduction of nonlinear coefficients to achieve high inversion accuracy while minimizing significant stress distortion,and excluding regions with severe stress distortion near the model edges while utilizing the central part of the model for subsequent simulations.These two strategies have been successfully implemented in the nonlinear in situ stress inversion of the Xincheng Gold Mine and have achieved higher inversion accuracy than the linear method.Specifically,the linear and nonlinear inversion methods yield root mean square errors(RMSE)of 4.15 and 3.2,and inversion relative errors(δAve)of 22.08%and 17.55%,respectively.Therefore,the nonlinear inversion method outperforms the traditional multiple linear regression method,even in the presence of a systematic reduction in the nonlinear stress boundaries.
基金Project supported by the National Natural Science Foundation of China(21273150)。
文摘Several ternary oxides CuCeZrO_(y)(CCZ)were synthesized by a facile grinding method followed by calcination at high temperatures,and used as catalysts for CO oxidation at low temperatures.The influences of calcination temperature(400-600℃)on the physicochemical properties of the assynthesized ternary oxides were investigated by thermogravimetric analysis/differential scanning calorimetry(TGA/DSC),X-ray diffraction(XRD),transmission electron microscopy(TEM),Raman,inductively coupled plasma-optical emission spectrometry(ICP-OES),N_(2) adsorption,H_(2)-temperature programmed reduction(H_(2)-TPR),and X-ray photoelectron spectroscopy(XPS)characterizations.The results show that the increase in calcination temperature from 400 to 500℃is conducive to the high dispersion of CuOx on catalyst surface and the incorporation of Cu species into the support to form the Cu-Ce-Zr-O solid solution.Further raising of calcination temperature from 500 to 600℃,however,leads to the segregation of Cu species from the solid solution to aggregate on support surface and growth of highly dispersed CuOx nanoparticles.The highest catalytic activity is acquired over the CCZ calcined at 500℃,which can be ascribed to the largest contents of Cu+species and oxygen vacancies owing to the formation of the maximum amount of Cu-Ce-Zr-O solid solution.
基金supported by the National Natural Science Foundation of China(12172023).
文摘The separation-of-variable(SOV)methods,such as the improved SOV method,the variational SOV method,and the extended SOV method,have been proposed by the present authors and coworkers to obtain the closed-form analytical solutions for free vibration and eigenbuckling of rectangular plates and circular cylindrical shells.By taking the free vibration of rectangular thin plates as an example,this work presents the theoretical framework of the SOV methods in an instructive way,and the bisection–based solution procedures for a group of nonlinear eigenvalue equations.Besides,the explicit equations of nodal lines of the SOV methods are presented,and the relations of nodal line patterns and frequency orders are investigated.It is concluded that the highly accurate SOV methods have the same accuracy for all frequencies,the mode shapes about repeated frequencies can also be precisely captured,and the SOV methods do not have the problem of missing roots as well.
基金funded by the National Natural Science Foundation of China(No.41962016)the Natural Science Foundation of NingXia(Nos.2023AAC02023,2023A1218,and 2021AAC02006).
文摘Soil improvement is one of the most important issues in geotechnical engineering practice.The wide application of traditional improvement techniques(cement/chemical materials)are limited due to damage ecological en-vironment and intensify carbon emissions.However,the use of microbially induced calcium carbonate pre-cipitation(MICP)to obtain bio-cement is a novel technique with the potential to induce soil stability,providing a low-carbon,environment-friendly,and sustainable integrated solution for some geotechnical engineering pro-blems in the environment.This paper presents a comprehensive review of the latest progress in soil improvement based on the MICP strategy.It systematically summarizes and overviews the mineralization mechanism,influ-encing factors,improved methods,engineering characteristics,and current field application status of the MICP.Additionally,it also explores the limitations and correspondingly proposes prospective applications via the MICP approach for soil improvement.This review indicates that the utilization of different environmental calcium-based wastes in MICP and combination of materials and MICP are conducive to meeting engineering and market demand.Furthermore,we recommend and encourage global collaborative study and practice with a view to commercializing MICP technique in the future.The current review purports to provide insights for engineers and interdisciplinary researchers,and guidance for future engineering applications.
基金the Jiangsu Key Laboratory for Chemistry of Low-Dimensional Materials for financial support(No. JSKC07041)
文摘A facile procedure for the synthesis of 2,4,5-lriarylimidazoles is being reported starting from benzil, aromatic aldehyde and ammonium acetate. The reactions were carried out with catalyst-free, solvent-free and under microwave irradiation conditions in high yield （80-99%） with short time （3-5 min） and environmental benign, as well as convenient operation. The structures of the compounds have been confirmed on the basis of their IR, 1H NMR, and/or 13C NMR, MS, and elemental analyzer.
文摘Bearing is an indispensable key component in mechanical equipment,and its working state is directly related to the stability and safety of the whole equipment.In recent years,with the rapid development of artificial intelligence technology,especially the breakthrough of deep learning technology,it provides a new idea for bearing fault diagnosis.Deep learning can automatically learn features from a large amount of data,has a strong nonlinear modeling ability,and can effectively solve the problems existing in traditional methods.Aiming at the key problems in bearing fault diagnosis,this paper studies the fault diagnosis method based on deep learning,which not only provides a new solution for bearing fault diagnosis but also provides a reference for the application of deep learning in other mechanical fault diagnosis fields.
