A novel green nanophosphor CaHPO4：Tb3＋ was synthesized via a room-temperatureco-precipitation route driven by ethanol solvent. X-ray powder diffraction （XRD）, scanningelectron microscopy （SEM） and photoluminesce...A novel green nanophosphor CaHPO4：Tb3＋ was synthesized via a room-temperatureco-precipitation route driven by ethanol solvent. X-ray powder diffraction （XRD）, scanningelectron microscopy （SEM） and photoluminescence spectroscopy （PL） techniques were utilizedto characterize the structure, morphology and fluorescence performance of the obtained powders.The results demonstrated that the prepared samples were well crystallized with triclinic phaseCaHPO4 structure and particle-like morphology. Photoluminescence measurements indicated thatCaHPOa：Tb3＋ had a strong absorption peak at 370 nm and exhibited characteristic emissions withseveral sharp peaks corresponding to the transitions 5D4-7FJ （jr = 6-3） of Tb3＋. Moreover, theluminescence optimum concentration for CaHPO4：Tb3＋ was determined to be 11 mol%, whichmight be a promising green-emitting ohosohor for display applications.展开更多
A Fe-containing mesoporous silica has been synthesized at room temperature using alkylamine as templating surfactant; XRD, IR, ESR and Si-29 MAS NMR spectra provided evidence of the presence of framework and non-frame...A Fe-containing mesoporous silica has been synthesized at room temperature using alkylamine as templating surfactant; XRD, IR, ESR and Si-29 MAS NMR spectra provided evidence of the presence of framework and non-framework iron(III) in Fe-HMS material.展开更多
The convenient synthesis of the composite electrode with high supercapacitance performance plays an important role in practical application but is challenging.Herein,the carbon nanotubes(CNTs)coupled with lowcrystalli...The convenient synthesis of the composite electrode with high supercapacitance performance plays an important role in practical application but is challenging.Herein,the carbon nanotubes(CNTs)coupled with lowcrystalline sulfur and nitrogen co-doped Ni Co-LDH(denoted as SN-Ni Co-LDH)nanosheets array are grown on Ni Co foam(NCF)substrate by two convenient steps of metal induced self-assembly and corrosion engineering,which present the advantages of operating at roomtemperature and low preparation costs.Benefiting from the S–N co-doping and low-crystallinity of Ni Co-LDH,the prepared SN-Ni Co-LDH@CNTs@NCF electrode presents a topping charge capacity of 2470 C·g^(-1)(4.94 C·cm^(-2))at 5 m A·cm^(-2).Furthermore,the fabricated asymmetry supercapacitor(ASC)achieves an extraordinary energy density of 77 Wh·kg^(-1)(0.617 m Wh·cm^(-2))at a power density of 438 W·kg^(-1)(3.5 m W·cm^(-2))and outstanding stability(91%capacity retention after 5000 cycles at20 m A·cm^(-2)).Impressively,the structure evolution of Ni Co-LDH during the charge/discharge processes has been thoroughly elucidated by in-situ Raman spectra.Therefore,this work verifies a powerful strategy and practical value for preparing composite electrodes with high supercapacitance performance,and also provides guidance for the rational design of the smart electrodes.展开更多
Neurons are highly polarized cells with axons reaching over a meter long in adult humans.To survive and maintain their proper function,neurons depend on specific mechanisms that regulate spatiotemporal signaling and m...Neurons are highly polarized cells with axons reaching over a meter long in adult humans.To survive and maintain their proper function,neurons depend on specific mechanisms that regulate spatiotemporal signaling and metabolic events,which need to be carried out at the right place,time,and intensity.Such mechanisms include axonal transport,local synthesis,and liquid-liquid phase separations.Alterations and malfunctions in these processes are correlated to neurodegenerative diseases such as amyotrophic lateral sclerosis(ALS).展开更多
Currently,the carbothermal reduction-nitridation(CRN)process is the predominant method for preparing aluminum nitride(AlN)powder.Although AlN powder prepared by CRN process exhibits high purity and excellent sintering...Currently,the carbothermal reduction-nitridation(CRN)process is the predominant method for preparing aluminum nitride(AlN)powder.Although AlN powder prepared by CRN process exhibits high purity and excellent sintering activity,it also presents challenges such as the necessity for high reaction temperatures and difficulties in achieving uniform mixing of its raw materials.This study presents a comprehensive investigation into preparation process of AlN nanopowders using a combination of hydrothermal synthesis and CRN.In the hydrothermal reaction,a homogeneous composite precursor consisting of carbon and boehmite(γ-AlOOH)is synthesized at 200℃using aluminum nitrate as the aluminum source,sucrose as the carbon source,and urea as the precipitant.During the hydrothermal process,the precursor develops a core-shell structure,with boehmite tightly coated with carbon(γ-AlOOH@C)due to electrostatic attraction.Compared with conventional precursor,the hydrothermal hybrid offers many advantages,such as ultrafine particles,uniform particle size distribution,good dispersion,high reactivity,and environmental friendliness.The carbon shell enhances thermodynamic stability of γ-Al_(2)O_(3) compared to the corundum phase(α-Al_(2)O_(3))by preventing the loss of the surface area in alumina.This stability enables γ-Al_(2)O_(3) to maintain high reactivity during CRN process,which initiates at 1300℃,and concludes at 1400℃.The underlying mechanisms are substantiated through experiments and thermodynamic calculations.This research provides a robust theoretical and experimental foundation for the hydrothermal combined carbothermal preparation of non-oxide ceramic nanopowders.展开更多
The paper researches the effect of temperature on ammonia synthesis. The ammonia synthesis reaction N2(g)+3H2(g)=2NH3(g)is exothermic with a negative entropy change. ΔG0condition is fulfilled at lower temperatures up...The paper researches the effect of temperature on ammonia synthesis. The ammonia synthesis reaction N2(g)+3H2(g)=2NH3(g)is exothermic with a negative entropy change. ΔG0condition is fulfilled at lower temperatures up to 464 K. It is a constant equilibrium of the ammonia synthesis reaction K′p≫1at lower temperatures, which means that the NH3(g)) synthesis reaction is shifted in the direction of NH3(g) formation (higher production of ammonia). The downside of lowering the temperature is that more ammonia is obtained, but the reaction rate slows down. Above 464K, the free enthalpy of the NH3(g) synthesis reaction is greater than zero, so the reaction enters thermodynamically unfavorable conditions. By increasing the reaction temperature, the ammonia yield NH3(g) decreases in the equilibrium mixture. At 400 K, it is 0.5128 kmol/kmol (51.28%) and at 900 K, the synthesis process NH3(g) is practically complete.展开更多
1989 is the beginning of intensive research into the phenomena of cold nuclear fusion, renamed “The Low Energy Nuclear Synthesis Reactions” (LENR). Based on these results and the long-term research of earthquakes an...1989 is the beginning of intensive research into the phenomena of cold nuclear fusion, renamed “The Low Energy Nuclear Synthesis Reactions” (LENR). Based on these results and the long-term research of earthquakes and volcanic activity, the authors of this article put forward a hypothesis about the mainly chemical nature of the energy released at earthquakes and volcanic eruptions with the participation of primordial hydrogen and helium: high mobility of hydrogen and oxidizers provide focusing and accumulation of the latent chemical energy, which is realized suddenly and instantaneously as explosions and initiate the earthquake and/or eruptions. The volcanic eruption is viewed therein as a special type of earthquake whereby the hypocenter rises to the earth’s surface. The authors proposed a new hypothesis that LENRs significant energy to earthquakes and eruptions at the synthesis of elements lighter than iron, thus creating excess energy, which is partially used for the synthesis of heavier elements. The combination of the chemical and nuclear reactions transforms these centers of geophysical activity into giant reactors where the nuclear, chemical, and thermal transformation of mantle materials and the creation of primary deposits of heavy elements such as uranium, thorium, gold, etc. So, all chemical elements heavier than iron are not detected in the solar wind. These elements discovered on our planet could be (and probably were) created on planet Earth and not imported from explosive supernovae or far-off remote stars. To the best of our knowledge, this hypothesis has not been proposed until now.展开更多
Ferromagnetic Fe3O4 nanoparticles were synthesized using water as the solvent through the sol-gel method, which was selected for its cost-effectiveness, simplicity, and eco-friendly nature. The synthesized nanoparticl...Ferromagnetic Fe3O4 nanoparticles were synthesized using water as the solvent through the sol-gel method, which was selected for its cost-effectiveness, simplicity, and eco-friendly nature. The synthesized nanoparticles were characterized using a variety of techniques, including Fourier Transform Infrared (FTIR) spectroscopy, X-ray powder diffraction (XRD), Scanning Electron Microscopy (SEM), Thermogravimetric Analysis (TGA), and Vibrating Sample Magnetometer (VSM). These characterizations confirmed the successful formation of Fe3O4 nanoparticles. The FTIR spectra identified characteristic peaks corresponding to the functional groups present, and XRD analysis, using Scherer’s equation, determined an average crystalline size of 1.2 nm for the Fe3O4 nanoparticles. TGA results demonstrated the thermal stability of the nanoparticles, SEM imaging revealed distinct honeycomb-like structures for the nanoparticles synthesized with water as the solvent, while the VSM analysis was used to determine the magnetic behavior of the nanoparticles.展开更多
Cycloheptatriene is a privileged structural motif present in many bioactive compounds,pharmaceutical agents and natural products,especially in a large number of core structures of sesquiterpenoids.Herein,a mild and ef...Cycloheptatriene is a privileged structural motif present in many bioactive compounds,pharmaceutical agents and natural products,especially in a large number of core structures of sesquiterpenoids.Herein,a mild and efficient synthetic approach was reported for access of a series of C2 or C3-(cycloheptatrienyl)-substituted indoles.A wide range of functional groups can be well tolerated in this transformation,especially including hydroxyl,halo,carboxylic acid and its derivative groups.Based on these results,a rational mechanism via electrophilic substitution of indoles with tropylium tetrafluoroborate is proposed.展开更多
High-pressure synthesis of lutetium hydrides from molecular hydrogen(H_(2))and lutetium(Lu)is systematically investigated using synchrotron X-ray diffraction,Raman spectroscopy,and visual observations.We demonstrate t...High-pressure synthesis of lutetium hydrides from molecular hydrogen(H_(2))and lutetium(Lu)is systematically investigated using synchrotron X-ray diffraction,Raman spectroscopy,and visual observations.We demonstrate that the reaction pathway between H_(2)and Lu invariably follows the sequence Lu→LuH_(2)→LuH_(3)and exhibits a notable time dependence.A comprehensive diagram representing the formation and synthesis of lutetium hydrides as a function of pressure and time is constructed.Our findings indicate that the synthesis can be accelerated by elevated temperature and decelerated by increased pressure.Notably,two critical pressure thresholds at ambient temperature are identified:the synthesis of LuH_(2)from Lu commences at a minimum pressure of~3 GPa,while~28 GPa is the minimum pressure at which LuH_(2)fails to transform into LuH_(3)within a time scale of months.This underscores the significant impact of temporal factors on synthesis,with the reaction completion time increasing sub-linearly with rising pressure.Furthermore,the cubic phase of LuH_(3)can be obtained exclusively through compressing the trigonal LuH_(3)phase at~11.5 GPa.We also demonstrate that the bandgap of LuH_(3)slowly closes under pressure and is noticeably lower than that of LuH_(2).展开更多
Energetic materials,characterized by their capacity to store and release substantial energy,hold pivotal significance in some fields,particularly in defense applications.Microfluidics,with its ability to manipulate fl...Energetic materials,characterized by their capacity to store and release substantial energy,hold pivotal significance in some fields,particularly in defense applications.Microfluidics,with its ability to manipulate fluids and facilitate droplet formation at the microscale,enables precise control of chemical reactions.Recent scholarly endeavors have increasingly harnessed microfluidic reactors in the realm of energetic materials,yielding morphologically controllable particles with enhanced uniformity and explosive efficacy.However,crucial insights into microfluidic-based methodologies are dispersed across various publications,necessitating a systematic compilation.Accordingly,this review addresses this gap by concentrating on the synthesis of energetic materials through microfluidics.Specifically,the methods based on micro-mixing and droplets in the previous papers are summarized and the strategies to control the critical parameters within chemical reactions are discussed in detail.Then,the comparison in terms of advantages and disadvantages is attempted.As demonstrated in the last section regarding perspectives,challenges such as clogging,dead zones,and suboptimal production yields are non-ignoble in the promising fields and they might be addressed by integrating sound,optics,or electrical energy to meet heightened requirements.This comprehensive overview aims to consolidate and analyze the diverse array of microfluidic approaches in energetic material synthesis,offering valuable insights for future research directions.展开更多
Red mud(RM)is a solid waste generated in the aluminum industry after the extraction of alumina oxide;its multiple elements and higher pH value likely pose a severe threat to the environment after treatment.However,RM&...Red mud(RM)is a solid waste generated in the aluminum industry after the extraction of alumina oxide;its multiple elements and higher pH value likely pose a severe threat to the environment after treatment.However,RM's higher concentrations of metal components,particularly Fe_(2)O_(3)and rare earth elements(REEs),render RM promising for catalytic application.Hence,this work showed an efficient high-speed RM to catalyze electrocatalytic nitrate-to-ammonia reduction reaction(NARR).RM calcined at 500℃(RM-500)exhibited excellent catalytic performance.Faradaic efficiency of ammonia(FENH_(3))in an electrolyte solution containing 1 mol·L^(-1)NO_(3)-achieved a maximum value of 92.3%at-0.8 V(vs.RHE).Additionally,24-h cycle testing and post-reaction PXRD and SEM indicated that the RM-500 electrocatalyst is stable during NARR.The RM-500 demonstrated a high FE of NH_(3)-to-NO_(3)-of 89.7%at 1.85 V(vs.RHE),showing great potential in the ammonia fuel cells technology and achieving the nitrogen cycle.展开更多
Among hyperspectral imaging technologies, interferometric spectral imaging is widely used in remote sening due to advantages of large luminous flux and high resolution. However, with complicated mechanism, interferome...Among hyperspectral imaging technologies, interferometric spectral imaging is widely used in remote sening due to advantages of large luminous flux and high resolution. However, with complicated mechanism, interferometric imaging faces the impact of multi-stage degradation. Most exsiting interferometric spectrum reconstruction methods are based on tradition model-based framework with multiple steps, showing poor efficiency and restricted performance. Thus, we propose an interferometric spectrum reconstruction method based on degradation synthesis and deep learning.Firstly, based on imaging mechanism, we proposed an mathematical model of interferometric imaging to analyse the degradation components as noises and trends during imaging. The model consists of three stages, namely instrument degradation, sensing degradation, and signal-independent degradation process. Then, we designed calibration-based method to estimate parameters in the model, of which the results are used for synthesizing realistic dataset for learning-based algorithms.In addition, we proposed a dual-stage interferogram spectrum reconstruction framework, which supports pre-training and integration of denoising DNNs. Experiments exhibits the reliability of our degradation model and synthesized data, and the effectiveness of the proposed reconstruction method.展开更多
Zeolite nanosheets with a short b-axis thickness are highly desirable in lots of catalytic reactions due to their reduced diffusion resistance. Nevertheless, conventional synthesis methods usually require expensive st...Zeolite nanosheets with a short b-axis thickness are highly desirable in lots of catalytic reactions due to their reduced diffusion resistance. Nevertheless, conventional synthesis methods usually require expensive structure-directing agents(SDAs), pricey raw materials, and eco-unfriendly fluorine-containing additives. Here, we contributed a cost-effective and fluoride-free synthesis method for synthesizing high-quality MFI zeolite nanosheets through a Silicalite-1(Sil-1) seed suspension and urea cooperative strategy, only with inexpensive colloidal silica as the Si source. Our approach was effective for synthesizing both Sil-1 and aluminum-containing ZSM-5 nanosheets. By optimizing key synthesis parameters,including seed aging time, seed quantity, and urea concentration, we achieved precise control over the crystal face aspect ratio and b-axis thickness. We also revealed a non-classical oriented nanosheet growth mechanism, where Sil-1 seeds induced the formation of quasi-ordered precursor particles, and the(010)crystal planes of these particles facilitated urea adsorption, thereby promoting c-axis-oriented growth.The obtained ZSM-5 nanosheets exhibited exceptional catalytic performance in the benzene alkylation with ethanol, maintaining stability for over 500 h, which is 5 times longer than traditional ZSM-5 catalysts. Furthermore, large-scale production of ZSM-5 nanosheets was successfully carried out in a 3 L highpressure autoclave, yielding samples consistent with those from laboratory-scale synthesis. This work marks a significant step forward in the sustainable and efficient production of MFI nanosheets using inexpensive and environmentally friendly raw materials, offering the broad applicability in catalysis.展开更多
Vicinal diamines are key motifs widely-found in many pharmaceuticals and biologically active molecules.An appealing approach for synthesizing these molecules is the amination of enamines,but few examples have been exp...Vicinal diamines are key motifs widely-found in many pharmaceuticals and biologically active molecules.An appealing approach for synthesizing these molecules is the amination of enamines,but few examples have been explored.With the utilization of nitrogen-centered radicals(NCRs),here we present the development of a dual bio-/photo-catalytic system for achieving enantioselective hydroamination of enamides,which can give easy access to diverse enantioenriched vicinal diamines.These reactions progress efficiently under green light excitation and exhibit excellent enantioselectivities(up to>99%enantiomeric excess).Mechanistic studies uncovered the synergistic effect of the enzyme and the externally added organophotoredox catalyst Rhodamine B(RhB).This work demonstrates the effectiveness of photobiocatalysis to generate and control high-energy radical intermediates,addressing a long-standing challenge in chemical synthesis.展开更多
Sunscreen agents derived from plants have been regarded as promising alternatives to artificial compounds.In this work,carbon dots(CDs)were prepared from carrot juice via a continuous microflowbased approach,where the...Sunscreen agents derived from plants have been regarded as promising alternatives to artificial compounds.In this work,carbon dots(CDs)were prepared from carrot juice via a continuous microflowbased approach,where the influence of process parameters was studied and optimized.Complimentary characterization revealed the CDs not only have small size,narrow size distribution,and good water solubility,but also have abundant functional groups as well as excellent UV absorption performance.Relying on these properties,the CDs were used as UV absorbers,suggesting they have strong long-term UV absorption ability over a broad pH range.The UV-absorption properties of the CDs were confirmed by incorporating the CDs in polyvinyl alcohol(PVA)to get C-CDs@PVA films of different thickness,in which significantly enhanced UV absorption performance was observed.Besides,the sun protection performance is also related to the film thickness.Afterwards,the practical application of the CDs was evaluated by adding them in a typical skin cream.With the addition of the CDs,the cream has drastically reduced UV transmittance in both UVA and UVB regions,and exhibits better UV absorption performance than commercial sunscreen agents.The CDs also demonstrated low cytotoxicity and high DPPH radical scavenging activity,making them promising as green sunscreen absorbers.This work is expected to provide a guidance for the development of green and effective natural sunscreen agents via microflowbased method.展开更多
Constructing a framework carrier to stabilize protein conformation,induce high embedding efficiency,and acquire low mass-transfer resistance is an urgent issue in the development of immobilized enzymes.Hydrogen-bonded...Constructing a framework carrier to stabilize protein conformation,induce high embedding efficiency,and acquire low mass-transfer resistance is an urgent issue in the development of immobilized enzymes.Hydrogen-bonded organic frameworks(HOFs)have promising application potential for embedding enzymes.In fact,no metal involvement is required,and HOFs exhibit superior biocompatibility,and free access to substrates in mesoporous channels.Herein,a facile in situ growth approach was proposed for the self-assembly of alcohol dehydrogenase encapsulated in HOF.The micron-scale bio-catalytic composite was rapidly synthesized under mild conditions(aqueous phase and ambient temperature)with a controllable embedding rate.The high crystallinity and periodic arrangement channels of HOF were preserved at a high enzyme encapsulation efficiency of 59%.This bio-composite improved the tolerance of the enzyme to the acid-base environment and retained 81%of its initial activity after five cycles of batch hydrogenation involving NADH coenzyme.Based on this controllably synthesized bio-catalytic material and a common lipase,we further developed a two-stage cascade microchemical system and achieved the continuous production of chiral hydroxybutyric acid(R-3-HBA).展开更多
High molecular weight poly(1,4-butylene 2,5-furandicarboxylate-co-isosorbide 2,5-furandicarboxylate)copolyesters(PBSIF-x)were synthesized via melt-polycondensation of 2,5-furandicarboxylic acid(FDCA),with varying rati...High molecular weight poly(1,4-butylene 2,5-furandicarboxylate-co-isosorbide 2,5-furandicarboxylate)copolyesters(PBSIF-x)were synthesized via melt-polycondensation of 2,5-furandicarboxylic acid(FDCA),with varying ratios of isosorbide(ISB)and 1,4-butylene glycol(BDO)catalyzed by antimony trioxide(Sb_(2)O_(3)).The PBSIF-x structures were investigated using FTIR and~1H NMR,while the GPC analysis exhibited the copolyesters molecular weights with number average molecular mass(M_n)in the range of 11079-15153 g/mol.The DSC results show that PBSIF-x copolyesters have a single glass-transition temperature(T_(g))(77.45-110.96℃),increasing with the increase in ISB content,while TGA analysis demonstrates excellent thermal stability up to 320℃.From the thermal result,properties of PBSIF-x copolyesters are found to be within the interval of their parent homologues poly(butylene 2,5-furandicarboxylate)(PBF)and poly(isosorbide 2,5-furandicarboxylate)(PIF),which confirms the aromatic/aliphatic blending within the polymer matrix for enhanced polymer stability and performance.展开更多
In this paper,an image processing algorithm which is able to synthesize material textures of arbitrary shapes is proposed.The presented approach uses an arbitrary image to construct a structure layer of the material.T...In this paper,an image processing algorithm which is able to synthesize material textures of arbitrary shapes is proposed.The presented approach uses an arbitrary image to construct a structure layer of the material.The resulting structure layer is then used to constrain the material texture synthesis.The field of second-moment matrices is used to represent the structure layer.Many tests with various constraint images are conducted to ensure that the proposed approach accurately reproduces the visual aspects of the input material sample.The results demonstrate that the proposed algorithm is able to accurately synthesize arbitrary-shaped material textures while respecting the local characteristics of the exemplar.This paves the way toward the synthesis of 3D material textures of arbitrary shapes from 2D material samples,which has a wide application range in virtual material design and materials characterization.展开更多
Synthetic biology(SynBio)is an emerging field of study with great potential in designing,engineering,and constructing new microbial synthetic cells that do not pre-exist in nature or re-engineering existing cells to a...Synthetic biology(SynBio)is an emerging field of study with great potential in designing,engineering,and constructing new microbial synthetic cells that do not pre-exist in nature or re-engineering existing cells to accomplish industrial purposes.Systems biology seeks to understand biology at multiple dimensions,beginning with the molecular and cellular level and progressing to the tissues and organismal level and characterizes cells as complex information-processing systems.SynBio,on the other hand,toggles further and strives to develop and create its systems from scratch.SynBio is now applied in the development of novel therapeutic drugs for the prevention of human diseases,scale up industrial processes,and accomplish previously unfeasible industrial outcomes.This is made possible through significant breakthroughs in DNA sequencing and synthesis technology,as well as insights gained from synthetic chemistry and systems biology.SynBio technologies have allowed for the introduction of improved and synthetic metabolic functionalities in microorganisms to enable the synthesis of a range of pharmacologically-relevant compounds for pharmaceutical exploration.SynBio applications range from finding new ways to making industrial chemical synthesis processes more sustainable as well as the microbial synthesis of improved therapeutic modalities.Hence,this study underpins several innovations,auspicious potentials,and future directions afforded by SynBio that proposes improved industrial microbial synthesis for pharmaceutical exploration.展开更多
基金supported by the National Natural Science Foundation of China(21663021)China Postdoctoral Science Foundation(2015M571977)+1 种基金the Natural Science Foundation of Jiangxi Province(20161BAB213058)the Natural Science Key Project of Jiangxi Province(2017ACB20040)
文摘A novel green nanophosphor CaHPO4：Tb3＋ was synthesized via a room-temperatureco-precipitation route driven by ethanol solvent. X-ray powder diffraction （XRD）, scanningelectron microscopy （SEM） and photoluminescence spectroscopy （PL） techniques were utilizedto characterize the structure, morphology and fluorescence performance of the obtained powders.The results demonstrated that the prepared samples were well crystallized with triclinic phaseCaHPO4 structure and particle-like morphology. Photoluminescence measurements indicated thatCaHPOa：Tb3＋ had a strong absorption peak at 370 nm and exhibited characteristic emissions withseveral sharp peaks corresponding to the transitions 5D4-7FJ （jr = 6-3） of Tb3＋. Moreover, theluminescence optimum concentration for CaHPO4：Tb3＋ was determined to be 11 mol%, whichmight be a promising green-emitting ohosohor for display applications.
文摘A Fe-containing mesoporous silica has been synthesized at room temperature using alkylamine as templating surfactant; XRD, IR, ESR and Si-29 MAS NMR spectra provided evidence of the presence of framework and non-framework iron(III) in Fe-HMS material.
基金supported by the National Natural Science Foundation of China(Nos.21978111,22278175 and 22108094)Zhejiang Provincial Natural Science Foundation of China(Nos.LZ24B060001 and LY22E020016)+1 种基金Jiaxing Key Research Project(No.2022BZ10001)the“Innovation Jiaxing·Excellent Talent Support Plan”Top Talent for Innovation and Entrepreneurship。
文摘The convenient synthesis of the composite electrode with high supercapacitance performance plays an important role in practical application but is challenging.Herein,the carbon nanotubes(CNTs)coupled with lowcrystalline sulfur and nitrogen co-doped Ni Co-LDH(denoted as SN-Ni Co-LDH)nanosheets array are grown on Ni Co foam(NCF)substrate by two convenient steps of metal induced self-assembly and corrosion engineering,which present the advantages of operating at roomtemperature and low preparation costs.Benefiting from the S–N co-doping and low-crystallinity of Ni Co-LDH,the prepared SN-Ni Co-LDH@CNTs@NCF electrode presents a topping charge capacity of 2470 C·g^(-1)(4.94 C·cm^(-2))at 5 m A·cm^(-2).Furthermore,the fabricated asymmetry supercapacitor(ASC)achieves an extraordinary energy density of 77 Wh·kg^(-1)(0.617 m Wh·cm^(-2))at a power density of 438 W·kg^(-1)(3.5 m W·cm^(-2))and outstanding stability(91%capacity retention after 5000 cycles at20 m A·cm^(-2)).Impressively,the structure evolution of Ni Co-LDH during the charge/discharge processes has been thoroughly elucidated by in-situ Raman spectra.Therefore,this work verifies a powerful strategy and practical value for preparing composite electrodes with high supercapacitance performance,and also provides guidance for the rational design of the smart electrodes.
文摘Neurons are highly polarized cells with axons reaching over a meter long in adult humans.To survive and maintain their proper function,neurons depend on specific mechanisms that regulate spatiotemporal signaling and metabolic events,which need to be carried out at the right place,time,and intensity.Such mechanisms include axonal transport,local synthesis,and liquid-liquid phase separations.Alterations and malfunctions in these processes are correlated to neurodegenerative diseases such as amyotrophic lateral sclerosis(ALS).
基金National Key Research and Development Program of China(2022YFB3708500,2023YFB3611000)Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China(2020ZZ109)。
文摘Currently,the carbothermal reduction-nitridation(CRN)process is the predominant method for preparing aluminum nitride(AlN)powder.Although AlN powder prepared by CRN process exhibits high purity and excellent sintering activity,it also presents challenges such as the necessity for high reaction temperatures and difficulties in achieving uniform mixing of its raw materials.This study presents a comprehensive investigation into preparation process of AlN nanopowders using a combination of hydrothermal synthesis and CRN.In the hydrothermal reaction,a homogeneous composite precursor consisting of carbon and boehmite(γ-AlOOH)is synthesized at 200℃using aluminum nitrate as the aluminum source,sucrose as the carbon source,and urea as the precipitant.During the hydrothermal process,the precursor develops a core-shell structure,with boehmite tightly coated with carbon(γ-AlOOH@C)due to electrostatic attraction.Compared with conventional precursor,the hydrothermal hybrid offers many advantages,such as ultrafine particles,uniform particle size distribution,good dispersion,high reactivity,and environmental friendliness.The carbon shell enhances thermodynamic stability of γ-Al_(2)O_(3) compared to the corundum phase(α-Al_(2)O_(3))by preventing the loss of the surface area in alumina.This stability enables γ-Al_(2)O_(3) to maintain high reactivity during CRN process,which initiates at 1300℃,and concludes at 1400℃.The underlying mechanisms are substantiated through experiments and thermodynamic calculations.This research provides a robust theoretical and experimental foundation for the hydrothermal combined carbothermal preparation of non-oxide ceramic nanopowders.
文摘The paper researches the effect of temperature on ammonia synthesis. The ammonia synthesis reaction N2(g)+3H2(g)=2NH3(g)is exothermic with a negative entropy change. ΔG0condition is fulfilled at lower temperatures up to 464 K. It is a constant equilibrium of the ammonia synthesis reaction K′p≫1at lower temperatures, which means that the NH3(g)) synthesis reaction is shifted in the direction of NH3(g) formation (higher production of ammonia). The downside of lowering the temperature is that more ammonia is obtained, but the reaction rate slows down. Above 464K, the free enthalpy of the NH3(g) synthesis reaction is greater than zero, so the reaction enters thermodynamically unfavorable conditions. By increasing the reaction temperature, the ammonia yield NH3(g) decreases in the equilibrium mixture. At 400 K, it is 0.5128 kmol/kmol (51.28%) and at 900 K, the synthesis process NH3(g) is practically complete.
文摘1989 is the beginning of intensive research into the phenomena of cold nuclear fusion, renamed “The Low Energy Nuclear Synthesis Reactions” (LENR). Based on these results and the long-term research of earthquakes and volcanic activity, the authors of this article put forward a hypothesis about the mainly chemical nature of the energy released at earthquakes and volcanic eruptions with the participation of primordial hydrogen and helium: high mobility of hydrogen and oxidizers provide focusing and accumulation of the latent chemical energy, which is realized suddenly and instantaneously as explosions and initiate the earthquake and/or eruptions. The volcanic eruption is viewed therein as a special type of earthquake whereby the hypocenter rises to the earth’s surface. The authors proposed a new hypothesis that LENRs significant energy to earthquakes and eruptions at the synthesis of elements lighter than iron, thus creating excess energy, which is partially used for the synthesis of heavier elements. The combination of the chemical and nuclear reactions transforms these centers of geophysical activity into giant reactors where the nuclear, chemical, and thermal transformation of mantle materials and the creation of primary deposits of heavy elements such as uranium, thorium, gold, etc. So, all chemical elements heavier than iron are not detected in the solar wind. These elements discovered on our planet could be (and probably were) created on planet Earth and not imported from explosive supernovae or far-off remote stars. To the best of our knowledge, this hypothesis has not been proposed until now.
文摘Ferromagnetic Fe3O4 nanoparticles were synthesized using water as the solvent through the sol-gel method, which was selected for its cost-effectiveness, simplicity, and eco-friendly nature. The synthesized nanoparticles were characterized using a variety of techniques, including Fourier Transform Infrared (FTIR) spectroscopy, X-ray powder diffraction (XRD), Scanning Electron Microscopy (SEM), Thermogravimetric Analysis (TGA), and Vibrating Sample Magnetometer (VSM). These characterizations confirmed the successful formation of Fe3O4 nanoparticles. The FTIR spectra identified characteristic peaks corresponding to the functional groups present, and XRD analysis, using Scherer’s equation, determined an average crystalline size of 1.2 nm for the Fe3O4 nanoparticles. TGA results demonstrated the thermal stability of the nanoparticles, SEM imaging revealed distinct honeycomb-like structures for the nanoparticles synthesized with water as the solvent, while the VSM analysis was used to determine the magnetic behavior of the nanoparticles.
文摘Cycloheptatriene is a privileged structural motif present in many bioactive compounds,pharmaceutical agents and natural products,especially in a large number of core structures of sesquiterpenoids.Herein,a mild and efficient synthetic approach was reported for access of a series of C2 or C3-(cycloheptatrienyl)-substituted indoles.A wide range of functional groups can be well tolerated in this transformation,especially including hydroxyl,halo,carboxylic acid and its derivative groups.Based on these results,a rational mechanism via electrophilic substitution of indoles with tropylium tetrafluoroborate is proposed.
基金supported by research grants of the Youth Innovation Promotion Association of CAS(Grant No.2021446)the National Science Foundation of China(Grant Nos.12204484,51672279,12174398 and 11874361)+1 种基金the Anhui Key Research and Development Program(Grant No.2022h11020007)the HFIPS Director’s Fund of the Chinese Academy of Sciences(Grant Nos.BJPY2022B02,YZJJ202102,YZJJ-GGZX-2022-01,and 2021YZGH03).
文摘High-pressure synthesis of lutetium hydrides from molecular hydrogen(H_(2))and lutetium(Lu)is systematically investigated using synchrotron X-ray diffraction,Raman spectroscopy,and visual observations.We demonstrate that the reaction pathway between H_(2)and Lu invariably follows the sequence Lu→LuH_(2)→LuH_(3)and exhibits a notable time dependence.A comprehensive diagram representing the formation and synthesis of lutetium hydrides as a function of pressure and time is constructed.Our findings indicate that the synthesis can be accelerated by elevated temperature and decelerated by increased pressure.Notably,two critical pressure thresholds at ambient temperature are identified:the synthesis of LuH_(2)from Lu commences at a minimum pressure of~3 GPa,while~28 GPa is the minimum pressure at which LuH_(2)fails to transform into LuH_(3)within a time scale of months.This underscores the significant impact of temporal factors on synthesis,with the reaction completion time increasing sub-linearly with rising pressure.Furthermore,the cubic phase of LuH_(3)can be obtained exclusively through compressing the trigonal LuH_(3)phase at~11.5 GPa.We also demonstrate that the bandgap of LuH_(3)slowly closes under pressure and is noticeably lower than that of LuH_(2).
基金financially supported by Science and Technology on Applied Physical Chemistry Laboratory,China(Grant No.61426022220303)supported by the Young Scientists Fund of the National Natural Science Foundation of China(Grant No.52305617)。
文摘Energetic materials,characterized by their capacity to store and release substantial energy,hold pivotal significance in some fields,particularly in defense applications.Microfluidics,with its ability to manipulate fluids and facilitate droplet formation at the microscale,enables precise control of chemical reactions.Recent scholarly endeavors have increasingly harnessed microfluidic reactors in the realm of energetic materials,yielding morphologically controllable particles with enhanced uniformity and explosive efficacy.However,crucial insights into microfluidic-based methodologies are dispersed across various publications,necessitating a systematic compilation.Accordingly,this review addresses this gap by concentrating on the synthesis of energetic materials through microfluidics.Specifically,the methods based on micro-mixing and droplets in the previous papers are summarized and the strategies to control the critical parameters within chemical reactions are discussed in detail.Then,the comparison in terms of advantages and disadvantages is attempted.As demonstrated in the last section regarding perspectives,challenges such as clogging,dead zones,and suboptimal production yields are non-ignoble in the promising fields and they might be addressed by integrating sound,optics,or electrical energy to meet heightened requirements.This comprehensive overview aims to consolidate and analyze the diverse array of microfluidic approaches in energetic material synthesis,offering valuable insights for future research directions.
基金supported by grants from the National Natural Science Foundation of China(22178339)2023 Innovation-driven Development Special Foundation of Guangxi Province(AA23023021)the Hundred Talents Program(A)of the Chinese Academy of Sciences.
文摘Red mud(RM)is a solid waste generated in the aluminum industry after the extraction of alumina oxide;its multiple elements and higher pH value likely pose a severe threat to the environment after treatment.However,RM's higher concentrations of metal components,particularly Fe_(2)O_(3)and rare earth elements(REEs),render RM promising for catalytic application.Hence,this work showed an efficient high-speed RM to catalyze electrocatalytic nitrate-to-ammonia reduction reaction(NARR).RM calcined at 500℃(RM-500)exhibited excellent catalytic performance.Faradaic efficiency of ammonia(FENH_(3))in an electrolyte solution containing 1 mol·L^(-1)NO_(3)-achieved a maximum value of 92.3%at-0.8 V(vs.RHE).Additionally,24-h cycle testing and post-reaction PXRD and SEM indicated that the RM-500 electrocatalyst is stable during NARR.The RM-500 demonstrated a high FE of NH_(3)-to-NO_(3)-of 89.7%at 1.85 V(vs.RHE),showing great potential in the ammonia fuel cells technology and achieving the nitrogen cycle.
文摘Among hyperspectral imaging technologies, interferometric spectral imaging is widely used in remote sening due to advantages of large luminous flux and high resolution. However, with complicated mechanism, interferometric imaging faces the impact of multi-stage degradation. Most exsiting interferometric spectrum reconstruction methods are based on tradition model-based framework with multiple steps, showing poor efficiency and restricted performance. Thus, we propose an interferometric spectrum reconstruction method based on degradation synthesis and deep learning.Firstly, based on imaging mechanism, we proposed an mathematical model of interferometric imaging to analyse the degradation components as noises and trends during imaging. The model consists of three stages, namely instrument degradation, sensing degradation, and signal-independent degradation process. Then, we designed calibration-based method to estimate parameters in the model, of which the results are used for synthesizing realistic dataset for learning-based algorithms.In addition, we proposed a dual-stage interferogram spectrum reconstruction framework, which supports pre-training and integration of denoising DNNs. Experiments exhibits the reliability of our degradation model and synthesized data, and the effectiveness of the proposed reconstruction method.
基金Joint Project of Dalian University of Technology-Dalian Institute of Chemical Physics (HX20230236)。
文摘Zeolite nanosheets with a short b-axis thickness are highly desirable in lots of catalytic reactions due to their reduced diffusion resistance. Nevertheless, conventional synthesis methods usually require expensive structure-directing agents(SDAs), pricey raw materials, and eco-unfriendly fluorine-containing additives. Here, we contributed a cost-effective and fluoride-free synthesis method for synthesizing high-quality MFI zeolite nanosheets through a Silicalite-1(Sil-1) seed suspension and urea cooperative strategy, only with inexpensive colloidal silica as the Si source. Our approach was effective for synthesizing both Sil-1 and aluminum-containing ZSM-5 nanosheets. By optimizing key synthesis parameters,including seed aging time, seed quantity, and urea concentration, we achieved precise control over the crystal face aspect ratio and b-axis thickness. We also revealed a non-classical oriented nanosheet growth mechanism, where Sil-1 seeds induced the formation of quasi-ordered precursor particles, and the(010)crystal planes of these particles facilitated urea adsorption, thereby promoting c-axis-oriented growth.The obtained ZSM-5 nanosheets exhibited exceptional catalytic performance in the benzene alkylation with ethanol, maintaining stability for over 500 h, which is 5 times longer than traditional ZSM-5 catalysts. Furthermore, large-scale production of ZSM-5 nanosheets was successfully carried out in a 3 L highpressure autoclave, yielding samples consistent with those from laboratory-scale synthesis. This work marks a significant step forward in the sustainable and efficient production of MFI nanosheets using inexpensive and environmentally friendly raw materials, offering the broad applicability in catalysis.
文摘Vicinal diamines are key motifs widely-found in many pharmaceuticals and biologically active molecules.An appealing approach for synthesizing these molecules is the amination of enamines,but few examples have been explored.With the utilization of nitrogen-centered radicals(NCRs),here we present the development of a dual bio-/photo-catalytic system for achieving enantioselective hydroamination of enamides,which can give easy access to diverse enantioenriched vicinal diamines.These reactions progress efficiently under green light excitation and exhibit excellent enantioselectivities(up to>99%enantiomeric excess).Mechanistic studies uncovered the synergistic effect of the enzyme and the externally added organophotoredox catalyst Rhodamine B(RhB).This work demonstrates the effectiveness of photobiocatalysis to generate and control high-energy radical intermediates,addressing a long-standing challenge in chemical synthesis.
基金National Natural Science Foundation of China(22078125)Postdoctoral Science Foundation of China(2023M741472)Fundamental Research Funds for the Central Universities(JUSRP622038).
文摘Sunscreen agents derived from plants have been regarded as promising alternatives to artificial compounds.In this work,carbon dots(CDs)were prepared from carrot juice via a continuous microflowbased approach,where the influence of process parameters was studied and optimized.Complimentary characterization revealed the CDs not only have small size,narrow size distribution,and good water solubility,but also have abundant functional groups as well as excellent UV absorption performance.Relying on these properties,the CDs were used as UV absorbers,suggesting they have strong long-term UV absorption ability over a broad pH range.The UV-absorption properties of the CDs were confirmed by incorporating the CDs in polyvinyl alcohol(PVA)to get C-CDs@PVA films of different thickness,in which significantly enhanced UV absorption performance was observed.Besides,the sun protection performance is also related to the film thickness.Afterwards,the practical application of the CDs was evaluated by adding them in a typical skin cream.With the addition of the CDs,the cream has drastically reduced UV transmittance in both UVA and UVB regions,and exhibits better UV absorption performance than commercial sunscreen agents.The CDs also demonstrated low cytotoxicity and high DPPH radical scavenging activity,making them promising as green sunscreen absorbers.This work is expected to provide a guidance for the development of green and effective natural sunscreen agents via microflowbased method.
基金supported by the National Key Research and Development Program of China(2019YFA0905100)the National Natural Science Foundation of China(21991102,22378227).
文摘Constructing a framework carrier to stabilize protein conformation,induce high embedding efficiency,and acquire low mass-transfer resistance is an urgent issue in the development of immobilized enzymes.Hydrogen-bonded organic frameworks(HOFs)have promising application potential for embedding enzymes.In fact,no metal involvement is required,and HOFs exhibit superior biocompatibility,and free access to substrates in mesoporous channels.Herein,a facile in situ growth approach was proposed for the self-assembly of alcohol dehydrogenase encapsulated in HOF.The micron-scale bio-catalytic composite was rapidly synthesized under mild conditions(aqueous phase and ambient temperature)with a controllable embedding rate.The high crystallinity and periodic arrangement channels of HOF were preserved at a high enzyme encapsulation efficiency of 59%.This bio-composite improved the tolerance of the enzyme to the acid-base environment and retained 81%of its initial activity after five cycles of batch hydrogenation involving NADH coenzyme.Based on this controllably synthesized bio-catalytic material and a common lipase,we further developed a two-stage cascade microchemical system and achieved the continuous production of chiral hydroxybutyric acid(R-3-HBA).
基金Funded by the Program(BG2021)of High-end Foreign Experts of The State Administration of Foreign Experts Affairs(SAFEA)the Young Talent Project of Hubei Provincial Department of Education,China(No.Q20201108)。
文摘High molecular weight poly(1,4-butylene 2,5-furandicarboxylate-co-isosorbide 2,5-furandicarboxylate)copolyesters(PBSIF-x)were synthesized via melt-polycondensation of 2,5-furandicarboxylic acid(FDCA),with varying ratios of isosorbide(ISB)and 1,4-butylene glycol(BDO)catalyzed by antimony trioxide(Sb_(2)O_(3)).The PBSIF-x structures were investigated using FTIR and~1H NMR,while the GPC analysis exhibited the copolyesters molecular weights with number average molecular mass(M_n)in the range of 11079-15153 g/mol.The DSC results show that PBSIF-x copolyesters have a single glass-transition temperature(T_(g))(77.45-110.96℃),increasing with the increase in ISB content,while TGA analysis demonstrates excellent thermal stability up to 320℃.From the thermal result,properties of PBSIF-x copolyesters are found to be within the interval of their parent homologues poly(butylene 2,5-furandicarboxylate)(PBF)and poly(isosorbide 2,5-furandicarboxylate)(PIF),which confirms the aromatic/aliphatic blending within the polymer matrix for enhanced polymer stability and performance.
文摘In this paper,an image processing algorithm which is able to synthesize material textures of arbitrary shapes is proposed.The presented approach uses an arbitrary image to construct a structure layer of the material.The resulting structure layer is then used to constrain the material texture synthesis.The field of second-moment matrices is used to represent the structure layer.Many tests with various constraint images are conducted to ensure that the proposed approach accurately reproduces the visual aspects of the input material sample.The results demonstrate that the proposed algorithm is able to accurately synthesize arbitrary-shaped material textures while respecting the local characteristics of the exemplar.This paves the way toward the synthesis of 3D material textures of arbitrary shapes from 2D material samples,which has a wide application range in virtual material design and materials characterization.
文摘Synthetic biology(SynBio)is an emerging field of study with great potential in designing,engineering,and constructing new microbial synthetic cells that do not pre-exist in nature or re-engineering existing cells to accomplish industrial purposes.Systems biology seeks to understand biology at multiple dimensions,beginning with the molecular and cellular level and progressing to the tissues and organismal level and characterizes cells as complex information-processing systems.SynBio,on the other hand,toggles further and strives to develop and create its systems from scratch.SynBio is now applied in the development of novel therapeutic drugs for the prevention of human diseases,scale up industrial processes,and accomplish previously unfeasible industrial outcomes.This is made possible through significant breakthroughs in DNA sequencing and synthesis technology,as well as insights gained from synthetic chemistry and systems biology.SynBio technologies have allowed for the introduction of improved and synthetic metabolic functionalities in microorganisms to enable the synthesis of a range of pharmacologically-relevant compounds for pharmaceutical exploration.SynBio applications range from finding new ways to making industrial chemical synthesis processes more sustainable as well as the microbial synthesis of improved therapeutic modalities.Hence,this study underpins several innovations,auspicious potentials,and future directions afforded by SynBio that proposes improved industrial microbial synthesis for pharmaceutical exploration.
