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
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
Rapid developments in lithium-ion battery(LIB)technology have been fueled by the expanding market for electric vehicles and increased demands for energy storage.Recently,thick electrode fabrication by solvent-free met...Rapid developments in lithium-ion battery(LIB)technology have been fueled by the expanding market for electric vehicles and increased demands for energy storage.Recently,thick electrode fabrication by solvent-free methods has emerged as a promising strategy for enhancing the energy density of LIBs.However,as electrode thickness increases,the tortuosity of lithium-ion transport also increases,resulting in severe polarization and poor electrochemical performance.Here,we investigate the effect of conductive agent morphology on the structural and electrochemical properties of 250μm thick lithium iron phosphate(LFP)/conductive agent/polytetrafluoroethylene(PTFE)-based electrodes.Three commercially available conductive additives,namely 0D Super P,1D multi-walled carbon nanotubes(MWCNTs),and 2D graphene nanoplatelets(GNPs),were incorporated into LFP-based electrodes.The MWCNT-incorporated electrode with a high loading mass(42 mg cm^(-2))exhibited a high porosity(ε=51%)and low tortuosity(τ=4.02)owing to its highly interconnected fibrous network of MWCNTs.Due to the fast lithium-ion transport kinetics in the MWCNT-incorporated electrode,the electrochemical performances exhibited a high specific capacity of 157 mAh g^(-1)at 0.1 C and an areal capacity of 7.16 mAh cm_(-2)at 0.1 C with a high-rate capability and excellent cycling stability over 300 cycles at 0.1 C.This study provides a guidance for utilizing conductive agents to apply in the low tortuous thick electrode fabricated by a solvent-free process.Additionally,this work paves the way to achieve scalable and sustainable dry processing techniques for developing next-generation energy storage technologies.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
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
This paper described an organic solvent-free, rapid, simple, and space-saving method of sample preparation followed by HPLC coupled photo-diode array (PDA) detector for simultaneous quantification of cyromazine (CYR) ...This paper described an organic solvent-free, rapid, simple, and space-saving method of sample preparation followed by HPLC coupled photo-diode array (PDA) detector for simultaneous quantification of cyromazine (CYR) and its decy-cropropylated metabolite, melamine (MEL), in milk. The HPLC-PDA was performed on an Inertsil? HILIC column with an isocratic aqueous mobile phase. Analytes were extracted from the sample using water, and purified by Mono-Spin?-C18, a centrifugal monolithic silica spin mini-columns, and quantified within 20 min. The method, performed under 100% aqueous conditions, obtained average recoveries for CYR and MEL in the range of 93.2% - 99.1% with relative standard deviations ≤ 2.8%. The quantitation limits were 8.5 ng/mL for CYR and 10 ng/mL for MEL, respectively. No organic solvents were used at any stage of the analysis.展开更多
In this paper,we consider the maximal positive definite solution of the nonlinear matrix equation.By using the idea of Algorithm 2.1 in ZHANG(2013),a new inversion-free method with a stepsize parameter is proposed to ...In this paper,we consider the maximal positive definite solution of the nonlinear matrix equation.By using the idea of Algorithm 2.1 in ZHANG(2013),a new inversion-free method with a stepsize parameter is proposed to obtain the maximal positive definite solution of nonlinear matrix equation X+A^(*)X|^(-α)A=Q with the case 0<α≤1.Based on this method,a new iterative algorithm is developed,and its convergence proof is given.Finally,two numerical examples are provided to show the effectiveness of the proposed method.展开更多
Convex feasibility problems are widely used in image reconstruction,sparse signal recovery,and other areas.This paper is devoted to considering a class of convex feasibility problem arising from sparse signal recovery...Convex feasibility problems are widely used in image reconstruction,sparse signal recovery,and other areas.This paper is devoted to considering a class of convex feasibility problem arising from sparse signal recovery.We rst derive the projection formulas for a vector onto the feasible sets.The centralized circumcentered-reection method is designed to solve the convex feasibility problem.Some numerical experiments demonstrate the feasibility and e ectiveness of the proposed algorithm,showing superior performance compared to conventional alternating projection methods.展开更多
Marine thin plates are susceptible to welding deformation owing to their low structural stiffness.Therefore,the efficient and accurate prediction of welding deformation is essential for improving welding quality.The t...Marine thin plates are susceptible to welding deformation owing to their low structural stiffness.Therefore,the efficient and accurate prediction of welding deformation is essential for improving welding quality.The traditional thermal elastic-plastic finite element method(TEP-FEM)can accurately predict welding deformation.However,its efficiency is low because of the complex nonlinear transient computation,making it difficult to meet the needs of rapid engineering evaluation.To address this challenge,this study proposes an efficient prediction method for welding deformation in marine thin plate butt welds.This method is based on the coupled temperature gradient-thermal strain method(TG-TSM)that integrates inherent strain theory with a shell element finite element model.The proposed method first extracts the distribution pattern and characteristic value of welding-induced inherent strain through TEP-FEM analysis.This strain is then converted into the equivalent thermal load applied to the shell element model for rapid computation.The proposed method-particularly,the gradual temperature gradient-thermal strain method(GTG-TSM)-achieved improved computational efficiency and consistent precision.Furthermore,the proposed method required much less computation time than the traditional TEP-FEM.Thus,this study lays the foundation for future prediction of welding deformation in more complex marine thin plates.展开更多
Exploring a simple,rapid,solvent-free synthetic method for mass production of cheap,broadband mi-crowave absorbers remains the main challenge.Here,a mild solvent-free procedure is reported to syn-thesize zinc oxide na...Exploring a simple,rapid,solvent-free synthetic method for mass production of cheap,broadband mi-crowave absorbers remains the main challenge.Here,a mild solvent-free procedure is reported to syn-thesize zinc oxide nanoparticles(ZnO NPs)embedded in porous carbon derived from mixing sucrose and zinc nitrate hexahydrate.The characteristic morphology and the ZnO NPs distribution in these compos-ites were tuned using the different raw materials proportions.The mesoporous structure of porous car-bon benefits the compositional advantages between carbon foam and ZnO NPs.The optimal synthesized ZnO/C-2 carbon material demonstrates the strongest absorption of-41.7 dB with a frequency of 14.5 GHz at a thin thickness of 2 mm,and its widest effective absorption is close to 6 GHz(12.2-17.8 GHz).This work produces a feasible route for the sensible design of other effective microwave absorbers for large-scale production.展开更多
γ-MnO2 nanorobs and Au/γ-MnO2 catalysts were synthesized and characterized by the X-ray powder diffraction XRD the scanning electron microscope SEM and transmission electron microscope TEM . The characterizations sh...γ-MnO2 nanorobs and Au/γ-MnO2 catalysts were synthesized and characterized by the X-ray powder diffraction XRD the scanning electron microscope SEM and transmission electron microscope TEM . The characterizations show that Au particles are well dispersed on the surface of γ-MnO2 nanorobs with a particle size of about 10 nm.The catalytic performance is evaluated in solvent-free toluene oxidation with oxygen. The influences of several process parameters such as reaction time reaction temperature initial oxygen pressure and catalyst amounts on the catalytic performance are studied.Catalytic results reveal that Au/γ-MnO2 catalyst has a unique selectivity to benzaldehyde and all these factors greatly influence the conversion of toluene and selectivity of bezaldehyde benzoic acid and benzyl benzoate.However these factors have slight influence on the selectivity of benzyl alcohol.展开更多
The effects of calcination temperature on the physicochemical properties of manganese oxide catalysts prepared by a precipitation method were assessed by X-ray diffraction,N2 adsorption-desorption,X-ray photoelectron ...The effects of calcination temperature on the physicochemical properties of manganese oxide catalysts prepared by a precipitation method were assessed by X-ray diffraction,N2 adsorption-desorption,X-ray photoelectron spectroscopy,H2 temperature-programmed reduction,O2 temperature-programmed desorption,and thermogravimetry-differential analysis.The catalytic performance of each of these materials during the selective oxidation of cyclohexane with oxygen in a solvent-free system was subsequently examined.It was found that the MnOx-500 catalyst,calcined at 500 °C,consisted of a Mn2O3 phase in addition to Mn5O8 and Mn3O4 phases and possessed a low surface area.Unlike MnOx-500,the MnOx-400 catalyst prepared at 400 °C was composed solely of Mn3O4 and Mn5O8 and had a higher surface area.The pronounced catalytic activity of this latter material for the oxidation of cyclohexene was determined to result from numerous factors,including a higher concentration of surface adsorbed oxygen,greater quantities of the surface Mn4＋ ions that promote oxygen mobility and the extent of O2 adsorption and reducibility on the catalyst.The effects of various reaction conditions on the activity of the MnOx-400 during the oxidation of cyclohexane were also evaluated,such as the reaction temperature,reaction time,and initial oxygen pressure.Following a 4 h reaction at an initial O2 pressure of 0.5 MPa and 140 °C,an 8.0% cyclohexane conversion and 5.0% yield of cyclohexanol and cyclohexanone were achieved over the MnOx-400 catalyst.In contrast,employing MnOx-500 resulted in a 6.1% conversion of cyclohexane and 75% selectivity for cyclohexanol and cyclohexanone.After being recycled through 10 replicate uses,the catalytic activity of the MnOx-400 catalyst was unchanged,demonstrating its good stability.展开更多
A series of Co-imbedded zeolite-based catalysts were synthesized following a facile solvent-free grinding route.The catalytic performance for direct syngas conversion to gasoline range hydrocarbons was compared with t...A series of Co-imbedded zeolite-based catalysts were synthesized following a facile solvent-free grinding route.The catalytic performance for direct syngas conversion to gasoline range hydrocarbons was compared with their counterpart Co-impregnated zeolite-based catalysts.Successful transformation of solid raw materials to targeted zeolite was confirmed by XRD,SEM,STEM,and N2 physisorption analysis.An in-depth study of acidic strength and acidic site distribution was conducted by NH3-TPD and Py-IR spectroscopy.Acidic strength showed a pivotal role in defining product range.Co@S1,with the weakest acidic strength of silicalite-1 among three types of zeolites,evaded over-cracking of product and exhibited the highest gasoline and isoparaffin selectivity(≈70%and 30.7%,respectively).Moreover,the solvent-free raw material grinding route for zeolite synthesis accompanies several advantages like the elimination of production of wastewater,high product yield within confined crystallization space,and elimination of safety concerns regarding high pressure due to the absence of the solvent.Facileness and easiness of the solvent-free synthesis route together with promising catalytic performance strongly support its application on the industrial scale.展开更多
Carbides/carbon composites are emerging as a new kind of binary dielectric systems with good microwave absorption performance.Herein,we obtain a series of tungsten carbide/carbon composites through a simple solvent-fr...Carbides/carbon composites are emerging as a new kind of binary dielectric systems with good microwave absorption performance.Herein,we obtain a series of tungsten carbide/carbon composites through a simple solvent-free strategy,where the solid mixture of dicyandiamide(DCA)and ammonium metatungstate(AM)is employed as the precursor.Ultrafine cubic WC1-x nanoparticles(3-4 nm)are in situ generated and uniformly dispersed on carbon nanosheets.This configuration overcomes some disadvantages of conventional carbides/carbon composites and is greatly helpful for electromagnetic dissipation.It is found that the weight ratio of DCA to AM can regulate chemical composition of these composites,while less impact on the average size of WC1-x nanoparticles.With the increase in carbon nanosheets,the relative complex permittivity and dielectric loss ability are constantly enhanced through conductive loss and polarization relaxation.The different dielectric properties endow these composites with distinguishable attenuation ability and impedance matching.When DCA/AM weight ratio is 6.0,the optimized composite can produce good microwave absorption performance,whose strongest reflection loss intensity reaches up to-55.6 dB at 17.5 GHz and qualified absorption bandwidth covers 3.6-18.0 GHz by manipulating the thickness from 1.0 to 5.0 mm.Such a performance is superior to many conventional carbides/carbon composites.展开更多
Six new asymmetric thiocarbonohydrazones 3a-3f were synthesized from following steps： firstly hydrazine hydrate reacted with carbon disulfide to form thiocarbonohydrazide （1） under microwave irradiation. Then compo...Six new asymmetric thiocarbonohydrazones 3a-3f were synthesized from following steps： firstly hydrazine hydrate reacted with carbon disulfide to form thiocarbonohydrazide （1） under microwave irradiation. Then compound （1） reacted with ketone and different aldehydes step by step to give 3a-3f with excellent yields under solvent-free conditions using microwave irradiation. Their structures have been determined by elemental analysis, IR, MS and ^1H NMR data. 2009 Qing Han Li. Published by Elsevier B.V. on behalf of Chinese Chemical Society. All rights reserved.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 Materials/Parts Technology Development Programs(RS-2024-00466920,RS-2024-00432627,and RS-2024-00421058)funded by the Ministry of Trade,Industry&Energy(MOTIE,Korea).
文摘Rapid developments in lithium-ion battery(LIB)technology have been fueled by the expanding market for electric vehicles and increased demands for energy storage.Recently,thick electrode fabrication by solvent-free methods has emerged as a promising strategy for enhancing the energy density of LIBs.However,as electrode thickness increases,the tortuosity of lithium-ion transport also increases,resulting in severe polarization and poor electrochemical performance.Here,we investigate the effect of conductive agent morphology on the structural and electrochemical properties of 250μm thick lithium iron phosphate(LFP)/conductive agent/polytetrafluoroethylene(PTFE)-based electrodes.Three commercially available conductive additives,namely 0D Super P,1D multi-walled carbon nanotubes(MWCNTs),and 2D graphene nanoplatelets(GNPs),were incorporated into LFP-based electrodes.The MWCNT-incorporated electrode with a high loading mass(42 mg cm^(-2))exhibited a high porosity(ε=51%)and low tortuosity(τ=4.02)owing to its highly interconnected fibrous network of MWCNTs.Due to the fast lithium-ion transport kinetics in the MWCNT-incorporated electrode,the electrochemical performances exhibited a high specific capacity of 157 mAh g^(-1)at 0.1 C and an areal capacity of 7.16 mAh cm_(-2)at 0.1 C with a high-rate capability and excellent cycling stability over 300 cycles at 0.1 C.This study provides a guidance for utilizing conductive agents to apply in the low tortuous thick electrode fabricated by a solvent-free process.Additionally,this work paves the way to achieve scalable and sustainable dry processing techniques for developing next-generation energy storage technologies.
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 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This paper described an organic solvent-free, rapid, simple, and space-saving method of sample preparation followed by HPLC coupled photo-diode array (PDA) detector for simultaneous quantification of cyromazine (CYR) and its decy-cropropylated metabolite, melamine (MEL), in milk. The HPLC-PDA was performed on an Inertsil? HILIC column with an isocratic aqueous mobile phase. Analytes were extracted from the sample using water, and purified by Mono-Spin?-C18, a centrifugal monolithic silica spin mini-columns, and quantified within 20 min. The method, performed under 100% aqueous conditions, obtained average recoveries for CYR and MEL in the range of 93.2% - 99.1% with relative standard deviations ≤ 2.8%. The quantitation limits were 8.5 ng/mL for CYR and 10 ng/mL for MEL, respectively. No organic solvents were used at any stage of the analysis.
基金Supported in part by Natural Science Foundation of Guangxi(2023GXNSFAA026246)in part by the Central Government's Guide to Local Science and Technology Development Fund(GuikeZY23055044)in part by the National Natural Science Foundation of China(62363003)。
文摘In this paper,we consider the maximal positive definite solution of the nonlinear matrix equation.By using the idea of Algorithm 2.1 in ZHANG(2013),a new inversion-free method with a stepsize parameter is proposed to obtain the maximal positive definite solution of nonlinear matrix equation X+A^(*)X|^(-α)A=Q with the case 0<α≤1.Based on this method,a new iterative algorithm is developed,and its convergence proof is given.Finally,two numerical examples are provided to show the effectiveness of the proposed method.
基金Supported by the Natural Science Foundation of Guangxi Province(Grant Nos.2023GXNSFAA026067,2024GXN SFAA010521)the National Natural Science Foundation of China(Nos.12361079,12201149,12261026).
文摘Convex feasibility problems are widely used in image reconstruction,sparse signal recovery,and other areas.This paper is devoted to considering a class of convex feasibility problem arising from sparse signal recovery.We rst derive the projection formulas for a vector onto the feasible sets.The centralized circumcentered-reection method is designed to solve the convex feasibility problem.Some numerical experiments demonstrate the feasibility and e ectiveness of the proposed algorithm,showing superior performance compared to conventional alternating projection methods.
基金Supported by the National Natural Science Foundation of China under Grant No.51975138the High-Tech Ship Scientific Research Project from the Ministry of Industry and Information Technology under Grant No.CJ05N20the National Defense Basic Research Project under Grant No.JCKY2023604C006.
文摘Marine thin plates are susceptible to welding deformation owing to their low structural stiffness.Therefore,the efficient and accurate prediction of welding deformation is essential for improving welding quality.The traditional thermal elastic-plastic finite element method(TEP-FEM)can accurately predict welding deformation.However,its efficiency is low because of the complex nonlinear transient computation,making it difficult to meet the needs of rapid engineering evaluation.To address this challenge,this study proposes an efficient prediction method for welding deformation in marine thin plate butt welds.This method is based on the coupled temperature gradient-thermal strain method(TG-TSM)that integrates inherent strain theory with a shell element finite element model.The proposed method first extracts the distribution pattern and characteristic value of welding-induced inherent strain through TEP-FEM analysis.This strain is then converted into the equivalent thermal load applied to the shell element model for rapid computation.The proposed method-particularly,the gradual temperature gradient-thermal strain method(GTG-TSM)-achieved improved computational efficiency and consistent precision.Furthermore,the proposed method required much less computation time than the traditional TEP-FEM.Thus,this study lays the foundation for future prediction of welding deformation in more complex marine thin plates.
基金the State Key Lab of Advanced Technology for Materials Synthesis and Processing(Wuhan Univer-sity of Technology)for financial support.
文摘Exploring a simple,rapid,solvent-free synthetic method for mass production of cheap,broadband mi-crowave absorbers remains the main challenge.Here,a mild solvent-free procedure is reported to syn-thesize zinc oxide nanoparticles(ZnO NPs)embedded in porous carbon derived from mixing sucrose and zinc nitrate hexahydrate.The characteristic morphology and the ZnO NPs distribution in these compos-ites were tuned using the different raw materials proportions.The mesoporous structure of porous car-bon benefits the compositional advantages between carbon foam and ZnO NPs.The optimal synthesized ZnO/C-2 carbon material demonstrates the strongest absorption of-41.7 dB with a frequency of 14.5 GHz at a thin thickness of 2 mm,and its widest effective absorption is close to 6 GHz(12.2-17.8 GHz).This work produces a feasible route for the sensible design of other effective microwave absorbers for large-scale production.
基金The National Natural Science Foundation of China(No.21276050)the Scientific Research Foundation of Graduate School of Southeast University(No.YBJJ1341)
文摘γ-MnO2 nanorobs and Au/γ-MnO2 catalysts were synthesized and characterized by the X-ray powder diffraction XRD the scanning electron microscope SEM and transmission electron microscope TEM . The characterizations show that Au particles are well dispersed on the surface of γ-MnO2 nanorobs with a particle size of about 10 nm.The catalytic performance is evaluated in solvent-free toluene oxidation with oxygen. The influences of several process parameters such as reaction time reaction temperature initial oxygen pressure and catalyst amounts on the catalytic performance are studied.Catalytic results reveal that Au/γ-MnO2 catalyst has a unique selectivity to benzaldehyde and all these factors greatly influence the conversion of toluene and selectivity of bezaldehyde benzoic acid and benzyl benzoate.However these factors have slight influence on the selectivity of benzyl alcohol.
基金supported by the National Basic Research Program of China(973 Program,2010CB732300)the National Natural Science Foundation of China(21103048)~~
文摘The effects of calcination temperature on the physicochemical properties of manganese oxide catalysts prepared by a precipitation method were assessed by X-ray diffraction,N2 adsorption-desorption,X-ray photoelectron spectroscopy,H2 temperature-programmed reduction,O2 temperature-programmed desorption,and thermogravimetry-differential analysis.The catalytic performance of each of these materials during the selective oxidation of cyclohexane with oxygen in a solvent-free system was subsequently examined.It was found that the MnOx-500 catalyst,calcined at 500 °C,consisted of a Mn2O3 phase in addition to Mn5O8 and Mn3O4 phases and possessed a low surface area.Unlike MnOx-500,the MnOx-400 catalyst prepared at 400 °C was composed solely of Mn3O4 and Mn5O8 and had a higher surface area.The pronounced catalytic activity of this latter material for the oxidation of cyclohexene was determined to result from numerous factors,including a higher concentration of surface adsorbed oxygen,greater quantities of the surface Mn4＋ ions that promote oxygen mobility and the extent of O2 adsorption and reducibility on the catalyst.The effects of various reaction conditions on the activity of the MnOx-400 during the oxidation of cyclohexane were also evaluated,such as the reaction temperature,reaction time,and initial oxygen pressure.Following a 4 h reaction at an initial O2 pressure of 0.5 MPa and 140 °C,an 8.0% cyclohexane conversion and 5.0% yield of cyclohexanol and cyclohexanone were achieved over the MnOx-400 catalyst.In contrast,employing MnOx-500 resulted in a 6.1% conversion of cyclohexane and 75% selectivity for cyclohexanol and cyclohexanone.After being recycled through 10 replicate uses,the catalytic activity of the MnOx-400 catalyst was unchanged,demonstrating its good stability.
基金the financial support from the Zhejiang Province Natural Science Foundation(LY19B060001)the Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering(2018-K25)the Foundation of Zhejiang University of Science and Technology(2019QN18,2019QN23)~~
文摘A series of Co-imbedded zeolite-based catalysts were synthesized following a facile solvent-free grinding route.The catalytic performance for direct syngas conversion to gasoline range hydrocarbons was compared with their counterpart Co-impregnated zeolite-based catalysts.Successful transformation of solid raw materials to targeted zeolite was confirmed by XRD,SEM,STEM,and N2 physisorption analysis.An in-depth study of acidic strength and acidic site distribution was conducted by NH3-TPD and Py-IR spectroscopy.Acidic strength showed a pivotal role in defining product range.Co@S1,with the weakest acidic strength of silicalite-1 among three types of zeolites,evaded over-cracking of product and exhibited the highest gasoline and isoparaffin selectivity(≈70%and 30.7%,respectively).Moreover,the solvent-free raw material grinding route for zeolite synthesis accompanies several advantages like the elimination of production of wastewater,high product yield within confined crystallization space,and elimination of safety concerns regarding high pressure due to the absence of the solvent.Facileness and easiness of the solvent-free synthesis route together with promising catalytic performance strongly support its application on the industrial scale.
基金supported by National Natural Science Foundation of China(21676065 and 21776053)。
文摘Carbides/carbon composites are emerging as a new kind of binary dielectric systems with good microwave absorption performance.Herein,we obtain a series of tungsten carbide/carbon composites through a simple solvent-free strategy,where the solid mixture of dicyandiamide(DCA)and ammonium metatungstate(AM)is employed as the precursor.Ultrafine cubic WC1-x nanoparticles(3-4 nm)are in situ generated and uniformly dispersed on carbon nanosheets.This configuration overcomes some disadvantages of conventional carbides/carbon composites and is greatly helpful for electromagnetic dissipation.It is found that the weight ratio of DCA to AM can regulate chemical composition of these composites,while less impact on the average size of WC1-x nanoparticles.With the increase in carbon nanosheets,the relative complex permittivity and dielectric loss ability are constantly enhanced through conductive loss and polarization relaxation.The different dielectric properties endow these composites with distinguishable attenuation ability and impedance matching.When DCA/AM weight ratio is 6.0,the optimized composite can produce good microwave absorption performance,whose strongest reflection loss intensity reaches up to-55.6 dB at 17.5 GHz and qualified absorption bandwidth covers 3.6-18.0 GHz by manipulating the thickness from 1.0 to 5.0 mm.Such a performance is superior to many conventional carbides/carbon composites.
基金the Natural Science Foundation of Southwest University for Nationalities (No.08NQZ002) for financial support.
文摘Six new asymmetric thiocarbonohydrazones 3a-3f were synthesized from following steps： firstly hydrazine hydrate reacted with carbon disulfide to form thiocarbonohydrazide （1） under microwave irradiation. Then compound （1） reacted with ketone and different aldehydes step by step to give 3a-3f with excellent yields under solvent-free conditions using microwave irradiation. Their structures have been determined by elemental analysis, IR, MS and ^1H NMR data. 2009 Qing Han Li. Published by Elsevier B.V. on behalf of Chinese Chemical Society. All rights reserved.
