Ingenious design and fabrication of advanced carbon-based sulfur cathodes are extremely important to the development of high-energy lithium-sulfur batteries,which hold promise as the next-generation power source.Herei...Ingenious design and fabrication of advanced carbon-based sulfur cathodes are extremely important to the development of high-energy lithium-sulfur batteries,which hold promise as the next-generation power source.Herein,for the first time,we report a novel versatile hyphae-mediated biological assembly technology to achieve scale production of hyphae carbon fibers(HCFs)derivatives,in which different components including carbon,metal compounds,and semiconductors can be homogeneously assembled with HCFs to form composite networks.The mechanism of biological adsorption assembly is also proposed.As a representative,reduced graphene oxides(rGOs)decorated with hollow carbon spheres(HCSs)successfully co-assemble with HCFs to form HCSs@rGOs/HCFs hosts for sulfur cathodes.In this unique architecture,not only large accommodation space for sulfur but also restrained volume expansion and fast charge transport paths are realized.Meanwhile,multiscale physical barriers plus chemisorption sites are simultaneously established to anchor soluble lithium polysulfides.Accordingly,the designed HCSs@rGOs/HCFs-S cathodes deliver a high capacity(1189 mA h g^(-1)at 0.1 C)and good high-rate capability(686 mA h g^(-1)at 5 C).Our work provides a new approach for the preparation of high-performance carbon-based electrodes for energy storage devices.展开更多
The development of anode materials with high rate capability and long charge-discharge plateau is the key to improve per-formance of lithium-ion capacitors(LICs).Herein,the porous graphitic carbon(PGC-1300)derived fro...The development of anode materials with high rate capability and long charge-discharge plateau is the key to improve per-formance of lithium-ion capacitors(LICs).Herein,the porous graphitic carbon(PGC-1300)derived from a new triply interpenetrated co-balt metal-organic framework(Co-MOF)was prepared through the facile and robust carbonization at 1300°C and washing by HCl solu-tion.The as-prepared PGC-1300 featured an optimized graphitization degree and porous framework,which not only contributes to high plateau capacity(105.0 mAh·g^(−1)below 0.2 V at 0.05 A·g^(−1)),but also supplies more convenient pathways for ions and increases the rate capability(128.5 mAh·g^(−1)at 3.2 A·g^(−1)).According to the kinetics analyses,it can be found that diffusion regulated surface induced capa-citive process and Li-ions intercalation process are coexisted for lithium-ion storage.Additionally,LIC PGC-1300//AC constructed with pre-lithiated PGC-1300 anode and activated carbon(AC)cathode exhibited an increased energy density of 102.8 Wh·kg^(−1),a power dens-ity of 6017.1 W·kg^(−1),together with the excellent cyclic stability(91.6%retention after 10000 cycles at 1.0 A·g^(−1)).展开更多
The mechanical properties and microstructure were investigated under different Zn content and heat treatment conditions in a Mg-Zn-YGd cast alloy.A part of the long period stacking order(LPSO)phases transformed to W-M...The mechanical properties and microstructure were investigated under different Zn content and heat treatment conditions in a Mg-Zn-YGd cast alloy.A part of the long period stacking order(LPSO)phases transformed to W-M^ZnaRE?phases with an increase in Zn content from 0.9 at.%to 1.8 at.%,and the ultimate tensile strength(UTS)increased from 229 MPa to 248 MPa.With solution treatment at 480°C,the content of the LPSO phase and strength sharply decreased in the Mg-1.8Zn-0.8Y-0.8Gd alloy,whereas this change was not significantly observed in the Mg-0.9Zn-O.8Y-O.8Gd alloy.After solution treatment,the elongation significantly improved and the UTS sharply decreased in both alloys.The lamellar and filminess LPSO phases were observed with aging treatment at 200℃.Moreover,the strengthening efficiency of lamellar and filminess LPSO phases was lower than that of the block LPSO phases.Therefore,the UTS of the T6 state was lower than that of the as-cast alloy.展开更多
Magnesium matrix composites (MMC) reinforced with 5wt% tricalcium phosphate (TCP) particles were prepared by powder metallurgy. Pure magnesium (CP-Mg) was fabricated by the same procedure for comparison. Scannin...Magnesium matrix composites (MMC) reinforced with 5wt% tricalcium phosphate (TCP) particles were prepared by powder metallurgy. Pure magnesium (CP-Mg) was fabricated by the same procedure for comparison. Scanning electron microscopy and en- ergy-dispersive X-ray spectroscopy analyses revealed that TCP particles were distributed homogeneously in the MMC. In order to investi- gate the corrosion properties, MMC samples were immersed in a simulated body fluid (SBF) at 310~0.5 K for 72 h. The mass loss of the samples in SBF and the pH values of the SBF were evaluated. Moreover, electrochemical measurements were conducted in the SBF. It was shown that the corrosion rate of the MMC decreased with the addition of TCP compared with CP-Mg. Hydroxyapatite was formed on the surface of MMC samples after immersion in the SBF for 72 h but not on the surface of CP-Mg.展开更多
The influence of Ultrafine Full-Vulcanized Acrylate Powdered Rubber(UFAPR) on the isothermal crystallization kinetics and nonisothermal crystallization behavior of PA6 has been studied by means of DSC. The results sho...The influence of Ultrafine Full-Vulcanized Acrylate Powdered Rubber(UFAPR) on the isothermal crystallization kinetics and nonisothermal crystallization behavior of PA6 has been studied by means of DSC. The results show that with the introduction of a small amount of UFAPR, the crystallization rate of PA6 can be increased obviously, and the crystallization temperature range can be augmented and the crystallite size distribution of the crystal can be narrowed down. The change of free energy perpendicular to the crystal nucleus, which has been calculated according to the Hoffman theory, is consistent with the result of Avrami′s equation. The unit surface free energy of the radial-developing crystal spherulite decreases while the crystallization rate of PA6 increases with the introduction of UFAPR. Meanwhile, it is shown by means of the polarizing microscope(PLM) that the crystal size drops down and the number of the crystal grains augments with the addition of UFAPR, which shows that UFAPR can function as a nucleating agent.展开更多
Due to the increasing demand for modified polylactide(PLA)meeting“double green”criteria,the research on sustainable plasticizers for PLA has attracted broad attentions.This study reported an open-ring polymerization...Due to the increasing demand for modified polylactide(PLA)meeting“double green”criteria,the research on sustainable plasticizers for PLA has attracted broad attentions.This study reported an open-ring polymerization method to fabricate cellulose(MCC)-g-PCL(poly(ε-caprolactone))copolymers with a fully sustainable and biodegradable component.MCC-g-PCL copolymers were synthesized,characterized,and used as green plasticizers for the PLA toughening.The results indicated that the MCC-g-PCL derivatives play an important role in the compatibility,crystallization,and toughening of the PLA/MCC-g-PCL composites.The mechanical properties of the fully bio-based PLA/MCC-g-PCL composites were optimized by adding 15 wt%MCC-g-PCL,that is,the elongation at break was 22.6%(~376%higher than that of neat PLA),the tensile strength was 47.3 MPa(comparable to that of neat PLA),and the impact strength was 26 J/m(~130%higher than that of neat PLA).DSC results indicated that MCC-g-PCL reduced the Tg of the PLA blend.When the addition amount was 15 wt%,the Tg of the blend was 58.4°C.Compared with MCC,MCC-g-PCL polyester plasticizer has better thermal stability,T5%(°C)can still be maintained above 300°C.The rheological results showed that MCC-g-PCL acted as a plasticizer,the introduction of PCL flexible chain increased the mobility of PLA molecular chain,and decreased the complex viscosity,storage modulus and loss modulus of PLA blends.The MCC-g-PCL derivatives,as a new green plastic additive,have shown an interesting prospect to prepare fully bio-based composites.展开更多
Mg-8Zn-0.5Zr-0.5Gd alloy was prepared by high pressure solidification. Effect of high pressure on microstructure, micro-hardness and corrosion behavior in Hank's solution of the Mg-8Zn-0.5Zr-0.5Gd alloy were investig...Mg-8Zn-0.5Zr-0.5Gd alloy was prepared by high pressure solidification. Effect of high pressure on microstructure, micro-hardness and corrosion behavior in Hank's solution of the Mg-8Zn-0.5Zr-0.5Gd alloy were investigated by means of optical microscopy (OM), scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), and X-ray diffractometer (XRD). The results showed that, compared with the conventional solidification, high pressure solidification obviously refined the grain size of Mg-8Zn-0.5Zr-0.5Gd alloy. The grain size was refined from 200-300 pm to 100-200 pm and the secondary dendrite arm spacing reduced from 30- 50 pm to 10-30 pro. Moreover, the solubility of Zn in the alloy increased and the amount and size of Mg-Zn-Gd phases significantly decreased. The micro-hardness of the alloy solidified under high pressure was improved significantly from 56.17 HV to 63.14 HV. The polarization resistance (Rp) of the alloy had a substantial increase in simulated body fluid, thus the corrosion rate was significantly reduced from 4.0 to 2.7 mm.year-1.展开更多
Waterborne polymers are vital for coating industry to reduce carbon emissions.However,formation of robust and self-healable films at ambient temperature remains a challenge owing to high energy cost of film formation ...Waterborne polymers are vital for coating industry to reduce carbon emissions.However,formation of robust and self-healable films at ambient temperature remains a challenge owing to high energy cost of film formation process.This work reports a solar-driven film formation of waterborne polyurethanes(WPUs)containing disulfide bonds via in-situ incorporation of 2D titanium carbide(MXene)with ability to convert light to heat.Instead of directly mixed with WPUs,MXene is added to join the reaction with isocyanate-terminated pre-polymer before emulsification process.This approach not only prevents aggregation of MXene in water but stabilizes MXene against thermal degradation which is the key hurdle for mass production of MXene/WPU composites.More importantly,our results show that mechanical performance of WPU films under visible light(100 mW/cm^(2))is overwhelmingly competitive with that processed in oven.Furthermore,the existence of disulfide bonds in PU chains enables fast self-healing of micro-cracks under natural visible light which could vanish completely within 40 min.The fractured specimens were repaired under natural visible light for 2 h,and the self-healing efficiency of tensile strength and elongation at break reached over 94.00%.展开更多
Constructing robust surface and bulk structure is the prerequisite for realizing high performance high voltage LiCoO_(2)(LCO).Herein,we manage to synthesize a surface Mg-doping and bulk Al-doping coreshell structured ...Constructing robust surface and bulk structure is the prerequisite for realizing high performance high voltage LiCoO_(2)(LCO).Herein,we manage to synthesize a surface Mg-doping and bulk Al-doping coreshell structured LCO,which demonstrates excellent cycling performance.Half-cell shows 94.2%capacity retention after 100 cycles at 3.0-4.6 V(vs.Li/Li^(+))cycling,and no capacity decay after 300 cycles for fullcell test(3.0-4.55 V).Based on comprehensive microanalysis and theoretical calculations,the degradation mechanisms and doping effects are systematically revealed.For the undoped LCO,high voltage cycling induces severe interfacial and bulk degradations,where cracks,stripe defects,fatigue H2 phase,and spinel phase are identified in grain bulk.For the doped LCO,Mg-doped surface shell can suppress the interfacial degradations,which not only stabilizes the surface structure by forming a thin rock-salt layer but also significantly improves the electronic conductivity,thus enabling superior rate performance.Bulk Al-doping can suppress the lattice"breathing"effect and the detrimental H3 to H1-3 phase transition,which minimizes the internal strain and defects growth,maintaining the layered structure after prolonged cycling.Combining theoretical calculations,this work deepens our understanding of the doping effects of Mg and Al,which is valuable in guiding the future material design of high voltage LCO.展开更多
The high porosity and tunable chemical functionality of metal-organic frameworks(MOFs)make it a promising catalyst design platform.High-throughput screening of catalytic performance is feasible since the large MOF str...The high porosity and tunable chemical functionality of metal-organic frameworks(MOFs)make it a promising catalyst design platform.High-throughput screening of catalytic performance is feasible since the large MOF structure database is available.In this study,we report a machine learning model for high-throughput screening of MOF catalysts for the CO_(2) cycloaddition reaction.The descriptors for model training were judiciously chosen according to the reaction mechanism,which leads to high accuracy up to 97%for the 75%quantile of the training set as the classification criterion.The feature contribution was further evaluated with SHAP and PDP analysis to provide a certain physical understanding.12,415 hypothetical MOF structures and 100 reported MOFs were evaluated under 100℃ and 1 bar within one day using the model,and 239 potentially efficient catalysts were discovered.Among them,MOF-76(Y)achieved the top performance experimentally among reported MOFs,in good agreement with the prediction.展开更多
The development of low-bandgap nonfullerene acceptors and wide-bandgap polymer donors speeds up the advance of organic solar cells(OSCs)[1-17]. Wide-bandgap copolymers based on fused-ring acceptor units are ideal dono...The development of low-bandgap nonfullerene acceptors and wide-bandgap polymer donors speeds up the advance of organic solar cells(OSCs)[1-17]. Wide-bandgap copolymers based on fused-ring acceptor units are ideal donor materials due to their low-lying HOMO levels, high hole mobilities and complementary light absorption to nonfullerene acceptors[18-25]. Currently, high-performance donors with 18%power conversion efficiencies(PCEs) belong to this type.展开更多
To investigate the role of pre-twins in Mg alloy sheets during warm planar deformation,the stretch forming is conducted at 200℃.Results suggest the formability of the pre-twinned AZ31 Mg alloy sheet is enhanced to 11...To investigate the role of pre-twins in Mg alloy sheets during warm planar deformation,the stretch forming is conducted at 200℃.Results suggest the formability of the pre-twinned AZ31 Mg alloy sheet is enhanced to 11.30 mm.The mechanisms for the improved formability and the deformation behaviors during the planar stretch forming are systematically investigated based on the planar stress states.The Schmid factor for deformation mechanisms are calculated,the results reveal that planar stress states extremely affect the Schmid factor for{10-12}twinning.The detwinning is activated and the prismatic slip is enhanced in the pre-twinned sheet,especially under the planar extension stress state in the outer region.Consequently,the thickness-direction strain is accommodated better.The dynamic recrystallization(DRX)type is continuous DRX(CDRX)regardless of the planar stress state.However,the CDRX degree is greater under the planar extension stress state.Some twin lattices deviate from the perfect{10-12}twinning relation due to the planar compression stress state and the CDRX.The basal texture is weakened when the planar stress state tends to change the texture components.展开更多
It remains as a challenge for realizing efficient photo-responsive catalysts towards largescale degradation of organic pollutants under natural sunlight.This work reports a new pore engineering strategy for creating u...It remains as a challenge for realizing efficient photo-responsive catalysts towards largescale degradation of organic pollutants under natural sunlight.This work reports a new pore engineering strategy for creating ultra-porous g-C_(3)N_(4) micro-tubes with an unprecedentedly high specific surface area of 152.96 m^(2)/g.This is mainly associated with releasing internal vapor pressure in the autoclave where the hydrothermal treatment of the urea/melamine mixture is processed.Supported by microscopic observation,porosity measurement and spectroscopic characterization,it is found that releasing the pressure at halfway of hydrothermal process is vital for forming exfoliated rod-like precursors and the de-aggregation of these rods presents substantial benefits on the production of mesopores on g-C_(3)N_(4) microtubes during the calcination of precursors.This offers a large number of reactive sites required by photocatalytic reaction.Coupling these micro-tubes with Ti_(3)C_(2)T_(X) nanosheets via electrostatic interaction yields a 1D/2D heterojunction with a close interfacial contact.The addition of metallically conductive Ti_(3)C_(2)T_(X) nanosheets accelerates the separation between electrons and holes,and also enhances the light absorption.All these merits of structural design lead to forming a group of highly efficient catalysts demonstrating an excellent photocatalytic degradation rate of k=0.0560 min^(-1)for RhB dyes under 100 mW/cm~2 visible light radiation that micks sunlight outdoors.This laboratory valuation is further supported by an outdoor test that shows a fast degradation rate of 0.0744 min^(-1)under natural sunlight.展开更多
A practical method for the construction of difluoromethylene-containing 1,4-thiazine moieties using readily available diethyl bromodifluoromethanephosphonate(BrCF_(2)PO(OEt)_(2))as difluorocarbene precusor has been de...A practical method for the construction of difluoromethylene-containing 1,4-thiazine moieties using readily available diethyl bromodifluoromethanephosphonate(BrCF_(2)PO(OEt)_(2))as difluorocarbene precusor has been developed.This transformation features the efficient capture of difluorocarbene by pyridinium 1,4-zwitterionic thiolates.A series of structurally novel and functionalized difluoromethylene-containing 1,4-thiazine derivatives were thus synthesized in good yields.展开更多
MXenes have aroused intensive enthusiasm because of their exotic properties and promising applications.However,to date,they are usually synthesized by etching technologies.Developing synthetic technologies provides mo...MXenes have aroused intensive enthusiasm because of their exotic properties and promising applications.However,to date,they are usually synthesized by etching technologies.Developing synthetic technologies provides more opportunities for innovation and may extend unexplored applications.Here,we report a bottom-up gas-phase synthesis of Cl-terminated MXene(Ti_(2)CCl_(2)).The gas-phase synthesis endows Ti_(2)CCl_(2) with unique surface chemistry,high phase purity,and excellent metallic conductivity,which can be used to accelerate polysulfide conversion kinetics and dramatically prolong the cyclability of Li-S batteries.In-depth mechanistic analysis deciphers the origin of the formation of Ti_(2)CCl_(2) and offers a paradigm for tuning MXene chemical vapor deposition.In brief,the gas-phase synthesis transforms the synthesis of MXenes and unlocks the hardly achieved potentials of MXenes.展开更多
In the slightly deformed Al-Mg-Si alloys,dislocation-induced precipitates are frequently observed,and they usually line up,forming sophisticated precipitation microstructures.Using atomic-resolution electron microscop...In the slightly deformed Al-Mg-Si alloys,dislocation-induced precipitates are frequently observed,and they usually line up,forming sophisticated precipitation microstructures.Using atomic-resolution electron microscopy in association with hardness measurements,we systematically investigated these precipitates in relation to the age-hardening responses of the alloys.Our study reveals that the majority of dislocation-induced complex precipitates are actually short-range ordered while long-range disordered polycrystalline precipitates and multiphase composite precipitates,including polycrystalline U2 precipitates,B’/U2,B’-2/U2,B’/B’-2/U2 and’/U2 composite precipitates.It is suggested that the formation of these complex precipitates is mainly owing to a high nucleation rate and rapid growth of different precipitate phases parallel to the associated dislocation lines.Since dislocation-induced precipitates consume more Mg than Si from the matrix and have a high formation kinetics,they will have different impacts on the matrix precipitation in different types of Al-Mg-Si alloys.Our results further demonstrate that for the"normally-β"-hardened"alloy,their formation leads to a coarser precipitate microstructure in the matrix,whereas for the"normally-β’-hardened"alloy,their formation reverses the precipitation pathway in the matrix,resulting in a reduced age-hardening potential of the former alloy and an improved age-hardening potential of the latter alloy.展开更多
An improved neural network model was developed for prediction of mechanical properties in the de-sign and development of new types of magnesium alloys by refining the types of input variables and using a more reasonab...An improved neural network model was developed for prediction of mechanical properties in the de-sign and development of new types of magnesium alloys by refining the types of input variables and using a more reasonable algorithm. The results showed that the improved model apparently decreased the prediction errors, and raised the accuracy of the prediction results. Better preprocessing parame-ters were found to be [0.15, 0.90] for the tensile strength, [0.1, 0.9] for the yield strength, and [0.15, 0.90] for the elongation. When the above parameters were used, the relativity for predicition of strength was bigger than 0.95. By using improved ANN analysis, more reasonable process parameters and compo- sition could be obtained in some magnesium alloys without addition of strontoum.展开更多
Abrasive wear is a common failure phenomenon that often limits the service life of sealing elements. Evaluation and comparison of the abrasion resistance of polytetrafluoroethylene (PTFE) were conducted using Al2O3par...Abrasive wear is a common failure phenomenon that often limits the service life of sealing elements. Evaluation and comparison of the abrasion resistance of polytetrafluoroethylene (PTFE) were conducted using Al2O3particleswithsizesintherange5to200 μmonapin-on-flattribo-testerunderdryreciprocatingsliding conditions at room temperature. Based on the examined worn surface characteristics of both PTFE and 316L stainless steel (as a counterpart) and the analyzed coefficient of friction (COF) evolutions, the wear mechanism and particle size effect have been explored in detail. The results demonstrate that the abrasive size is the main contributing factor, which can drastically impact the wear mechanism and tribological properties of tribo-pairs. The COF exhibits different evolution characteristics (trends) for different abrasive sizes. For moderate particle sizes, the COF trends become more complicated and the most evident wear of the metallic counterpart is evident. The activity behaviors of abrasives are dominated by the particle size. Particles can becomes embedded in one of the tribo-pair materials to plough-cut the counterpart, thus causing two-body abrasive wear. The abrasives can also behave as free rolling bodies, which play the role of third body to realize three-body "PTFE-abrasive-316L"abrasion. When abrasives are involved in the wear process, both the wear rate and COF of the metallic counterpart increase, but the material removal rate of the PTFE is reduced. The results obtained can offer guidelines regarding the design and protection of seals.展开更多
Pyrolyzed Fe/N/C catalyst has been considered as the most promising candidate to replace Pt for oxygen reduction reaction(ORR) in fuel cells.However,poor stability of Fe/N/C catalyst,mainly attributed to the oxidation...Pyrolyzed Fe/N/C catalyst has been considered as the most promising candidate to replace Pt for oxygen reduction reaction(ORR) in fuel cells.However,poor stability of Fe/N/C catalyst,mainly attributed to the oxidation corrosion by aggressive ·OH radical,severely hampers its applications.However,the exact mechanism for generation of ·OH is unclear yet.Herein,we developed a fluorescent method to effectively detect ·OH generated from ORR on Fe/N/C catalyst by using coumarin as a fluorescent probe.A great difference in potential dependence between ·OH and H2O2 generated from the ORR was observed,which suggests that ·OH is not generated from the decomposition of H2O2 as traditional viewpoint.展开更多
Adding alloying elements to improve the performances or the manufacturing processes of Al-Mg-Si alloys has long been a serious issue in developing advanced automotive aluminum materials.The Zn element,among those prom...Adding alloying elements to improve the performances or the manufacturing processes of Al-Mg-Si alloys has long been a serious issue in developing advanced automotive aluminum materials.The Zn element,among those promising ones,has demonstrated positive alloying effects on Al-Mg-Si alloys.However,the atomic-scale roles of Zn in an age-hardened Al-Mg-Si-Zn alloy have not been adequately understood.Using atomic-resolution electron microscopy,here we report the precise locations of Zn elements in all hardening precipitates involved and their alloying mechanism at the atomic scale when alloying the alloy.Our results show that Zn atoms enter all the major hardening phases to occupy specific featured atomic sites of the original elements,e.g.the Si1 and Mg2 sites in theβ’-2 phase,and modify their crystal structures,interfacial structures and morphologies in characteristic manners.It is revealed that for theβ’-phase,Zn atoms occupy unique atomic sites,whereas for other phases,they demonstrate similar behaviors as other additive alloying elements such as Ag and Cu do.展开更多
基金Natural Science Foundation for Distinguished Young Scholars of Zhejiang Province,Grant/Award Number:LR20E020001Foundation of State Key Laboratory of Coal Conversion,Grant/Award Number:J20-21-909+4 种基金Science and Technology Department of Zhejiang Province,Grant/Award Number:2023C01231National Natural Science Foundation of China,Grant/Award Numbers:52372235,52073252,52002052,22379020,U20A20253,21972127,22279116Open Project Program of the State Key Laboratory of Photocatalysis on Energy and Environment,Grant/Award Number:SKLPEE-KF202206Key Research and Development Project of Science and Technology Department of Sichuan Province,Grant/Award Number:2022YFSY0004Ministry of Education,Grant/Award Number:KFM 202202。
文摘Ingenious design and fabrication of advanced carbon-based sulfur cathodes are extremely important to the development of high-energy lithium-sulfur batteries,which hold promise as the next-generation power source.Herein,for the first time,we report a novel versatile hyphae-mediated biological assembly technology to achieve scale production of hyphae carbon fibers(HCFs)derivatives,in which different components including carbon,metal compounds,and semiconductors can be homogeneously assembled with HCFs to form composite networks.The mechanism of biological adsorption assembly is also proposed.As a representative,reduced graphene oxides(rGOs)decorated with hollow carbon spheres(HCSs)successfully co-assemble with HCFs to form HCSs@rGOs/HCFs hosts for sulfur cathodes.In this unique architecture,not only large accommodation space for sulfur but also restrained volume expansion and fast charge transport paths are realized.Meanwhile,multiscale physical barriers plus chemisorption sites are simultaneously established to anchor soluble lithium polysulfides.Accordingly,the designed HCSs@rGOs/HCFs-S cathodes deliver a high capacity(1189 mA h g^(-1)at 0.1 C)and good high-rate capability(686 mA h g^(-1)at 5 C).Our work provides a new approach for the preparation of high-performance carbon-based electrodes for energy storage devices.
基金the National Natural Science Foundation of China(No.52004179)the Natural Nat-ural Science Foundation of Guangxi Province,China(No.2020GXNSFAA159015)Shanxi Water and Wood New Carbon Materials Technology Co.,Ltd.,China,and Shanxi Wote Haimer New Materials Technology Co.,Ltd,China.
文摘The development of anode materials with high rate capability and long charge-discharge plateau is the key to improve per-formance of lithium-ion capacitors(LICs).Herein,the porous graphitic carbon(PGC-1300)derived from a new triply interpenetrated co-balt metal-organic framework(Co-MOF)was prepared through the facile and robust carbonization at 1300°C and washing by HCl solu-tion.The as-prepared PGC-1300 featured an optimized graphitization degree and porous framework,which not only contributes to high plateau capacity(105.0 mAh·g^(−1)below 0.2 V at 0.05 A·g^(−1)),but also supplies more convenient pathways for ions and increases the rate capability(128.5 mAh·g^(−1)at 3.2 A·g^(−1)).According to the kinetics analyses,it can be found that diffusion regulated surface induced capa-citive process and Li-ions intercalation process are coexisted for lithium-ion storage.Additionally,LIC PGC-1300//AC constructed with pre-lithiated PGC-1300 anode and activated carbon(AC)cathode exhibited an increased energy density of 102.8 Wh·kg^(−1),a power dens-ity of 6017.1 W·kg^(−1),together with the excellent cyclic stability(91.6%retention after 10000 cycles at 1.0 A·g^(−1)).
文摘The mechanical properties and microstructure were investigated under different Zn content and heat treatment conditions in a Mg-Zn-YGd cast alloy.A part of the long period stacking order(LPSO)phases transformed to W-M^ZnaRE?phases with an increase in Zn content from 0.9 at.%to 1.8 at.%,and the ultimate tensile strength(UTS)increased from 229 MPa to 248 MPa.With solution treatment at 480°C,the content of the LPSO phase and strength sharply decreased in the Mg-1.8Zn-0.8Y-0.8Gd alloy,whereas this change was not significantly observed in the Mg-0.9Zn-O.8Y-O.8Gd alloy.After solution treatment,the elongation significantly improved and the UTS sharply decreased in both alloys.The lamellar and filminess LPSO phases were observed with aging treatment at 200℃.Moreover,the strengthening efficiency of lamellar and filminess LPSO phases was lower than that of the block LPSO phases.Therefore,the UTS of the T6 state was lower than that of the as-cast alloy.
基金the National Key Technologies R&D Program(No.2011BAE22B04)Chong qing Science and Technology Commission(No.2008BB4055)
文摘Magnesium matrix composites (MMC) reinforced with 5wt% tricalcium phosphate (TCP) particles were prepared by powder metallurgy. Pure magnesium (CP-Mg) was fabricated by the same procedure for comparison. Scanning electron microscopy and en- ergy-dispersive X-ray spectroscopy analyses revealed that TCP particles were distributed homogeneously in the MMC. In order to investi- gate the corrosion properties, MMC samples were immersed in a simulated body fluid (SBF) at 310~0.5 K for 72 h. The mass loss of the samples in SBF and the pH values of the SBF were evaluated. Moreover, electrochemical measurements were conducted in the SBF. It was shown that the corrosion rate of the MMC decreased with the addition of TCP compared with CP-Mg. Hydroxyapatite was formed on the surface of MMC samples after immersion in the SBF for 72 h but not on the surface of CP-Mg.
基金Supported by the National Natural Science Foundation of China( No.5 99730 0 3)
文摘The influence of Ultrafine Full-Vulcanized Acrylate Powdered Rubber(UFAPR) on the isothermal crystallization kinetics and nonisothermal crystallization behavior of PA6 has been studied by means of DSC. The results show that with the introduction of a small amount of UFAPR, the crystallization rate of PA6 can be increased obviously, and the crystallization temperature range can be augmented and the crystallite size distribution of the crystal can be narrowed down. The change of free energy perpendicular to the crystal nucleus, which has been calculated according to the Hoffman theory, is consistent with the result of Avrami′s equation. The unit surface free energy of the radial-developing crystal spherulite decreases while the crystallization rate of PA6 increases with the introduction of UFAPR. Meanwhile, it is shown by means of the polarizing microscope(PLM) that the crystal size drops down and the number of the crystal grains augments with the addition of UFAPR, which shows that UFAPR can function as a nucleating agent.
基金supported by the National Natural Science Foundation of China(21574030,52063007,51863004)Guizhou Province High-Level Innovative Talents Fund([2020]6024)+1 种基金Guizhou Provincial Science and Technology Projects(Grant No.[2022]024)and the Science and Technology Project of Baiyun District,Guiyang City(Grant No.[2020]26)the authors gratefully acknowledge the financial support from the National Engineering Research Center for Compounding and Modification of Polymeric Materials(Guizhou Material Industrial Technology Institute).
文摘Due to the increasing demand for modified polylactide(PLA)meeting“double green”criteria,the research on sustainable plasticizers for PLA has attracted broad attentions.This study reported an open-ring polymerization method to fabricate cellulose(MCC)-g-PCL(poly(ε-caprolactone))copolymers with a fully sustainable and biodegradable component.MCC-g-PCL copolymers were synthesized,characterized,and used as green plasticizers for the PLA toughening.The results indicated that the MCC-g-PCL derivatives play an important role in the compatibility,crystallization,and toughening of the PLA/MCC-g-PCL composites.The mechanical properties of the fully bio-based PLA/MCC-g-PCL composites were optimized by adding 15 wt%MCC-g-PCL,that is,the elongation at break was 22.6%(~376%higher than that of neat PLA),the tensile strength was 47.3 MPa(comparable to that of neat PLA),and the impact strength was 26 J/m(~130%higher than that of neat PLA).DSC results indicated that MCC-g-PCL reduced the Tg of the PLA blend.When the addition amount was 15 wt%,the Tg of the blend was 58.4°C.Compared with MCC,MCC-g-PCL polyester plasticizer has better thermal stability,T5%(°C)can still be maintained above 300°C.The rheological results showed that MCC-g-PCL acted as a plasticizer,the introduction of PCL flexible chain increased the mobility of PLA molecular chain,and decreased the complex viscosity,storage modulus and loss modulus of PLA blends.The MCC-g-PCL derivatives,as a new green plastic additive,have shown an interesting prospect to prepare fully bio-based composites.
基金financially supported by National Natural Science Foundations of China(Grant No.51201062)Natural Science Foundation of Heilongjiang Province(Grant No.2015038)
文摘Mg-8Zn-0.5Zr-0.5Gd alloy was prepared by high pressure solidification. Effect of high pressure on microstructure, micro-hardness and corrosion behavior in Hank's solution of the Mg-8Zn-0.5Zr-0.5Gd alloy were investigated by means of optical microscopy (OM), scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), and X-ray diffractometer (XRD). The results showed that, compared with the conventional solidification, high pressure solidification obviously refined the grain size of Mg-8Zn-0.5Zr-0.5Gd alloy. The grain size was refined from 200-300 pm to 100-200 pm and the secondary dendrite arm spacing reduced from 30- 50 pm to 10-30 pro. Moreover, the solubility of Zn in the alloy increased and the amount and size of Mg-Zn-Gd phases significantly decreased. The micro-hardness of the alloy solidified under high pressure was improved significantly from 56.17 HV to 63.14 HV. The polarization resistance (Rp) of the alloy had a substantial increase in simulated body fluid, thus the corrosion rate was significantly reduced from 4.0 to 2.7 mm.year-1.
基金National Natural Science Foundation of China(Grant No.21503110)for supporting this work.
文摘Waterborne polymers are vital for coating industry to reduce carbon emissions.However,formation of robust and self-healable films at ambient temperature remains a challenge owing to high energy cost of film formation process.This work reports a solar-driven film formation of waterborne polyurethanes(WPUs)containing disulfide bonds via in-situ incorporation of 2D titanium carbide(MXene)with ability to convert light to heat.Instead of directly mixed with WPUs,MXene is added to join the reaction with isocyanate-terminated pre-polymer before emulsification process.This approach not only prevents aggregation of MXene in water but stabilizes MXene against thermal degradation which is the key hurdle for mass production of MXene/WPU composites.More importantly,our results show that mechanical performance of WPU films under visible light(100 mW/cm^(2))is overwhelmingly competitive with that processed in oven.Furthermore,the existence of disulfide bonds in PU chains enables fast self-healing of micro-cracks under natural visible light which could vanish completely within 40 min.The fractured specimens were repaired under natural visible light for 2 h,and the self-healing efficiency of tensile strength and elongation at break reached over 94.00%.
基金the National Natural Science Foundation of China(12174015)the Natural Science Foundation of Beijing,China(2212003)+1 种基金the China National Petroleum Corporation Innovation Found(2021DQ02-1004)the National Natural Science Foundation of China(12102053)。
文摘Constructing robust surface and bulk structure is the prerequisite for realizing high performance high voltage LiCoO_(2)(LCO).Herein,we manage to synthesize a surface Mg-doping and bulk Al-doping coreshell structured LCO,which demonstrates excellent cycling performance.Half-cell shows 94.2%capacity retention after 100 cycles at 3.0-4.6 V(vs.Li/Li^(+))cycling,and no capacity decay after 300 cycles for fullcell test(3.0-4.55 V).Based on comprehensive microanalysis and theoretical calculations,the degradation mechanisms and doping effects are systematically revealed.For the undoped LCO,high voltage cycling induces severe interfacial and bulk degradations,where cracks,stripe defects,fatigue H2 phase,and spinel phase are identified in grain bulk.For the doped LCO,Mg-doped surface shell can suppress the interfacial degradations,which not only stabilizes the surface structure by forming a thin rock-salt layer but also significantly improves the electronic conductivity,thus enabling superior rate performance.Bulk Al-doping can suppress the lattice"breathing"effect and the detrimental H3 to H1-3 phase transition,which minimizes the internal strain and defects growth,maintaining the layered structure after prolonged cycling.Combining theoretical calculations,this work deepens our understanding of the doping effects of Mg and Al,which is valuable in guiding the future material design of high voltage LCO.
基金financial support from the National Key Research and Development Program of China(2021YFB 3501501)the National Natural Science Foundation of China(No.22225803,22038001,22108007 and 22278011)+1 种基金Beijing Natural Science Foundation(No.Z230023)Beijing Science and Technology Commission(No.Z211100004321001).
文摘The high porosity and tunable chemical functionality of metal-organic frameworks(MOFs)make it a promising catalyst design platform.High-throughput screening of catalytic performance is feasible since the large MOF structure database is available.In this study,we report a machine learning model for high-throughput screening of MOF catalysts for the CO_(2) cycloaddition reaction.The descriptors for model training were judiciously chosen according to the reaction mechanism,which leads to high accuracy up to 97%for the 75%quantile of the training set as the classification criterion.The feature contribution was further evaluated with SHAP and PDP analysis to provide a certain physical understanding.12,415 hypothetical MOF structures and 100 reported MOFs were evaluated under 100℃ and 1 bar within one day using the model,and 239 potentially efficient catalysts were discovered.Among them,MOF-76(Y)achieved the top performance experimentally among reported MOFs,in good agreement with the prediction.
基金the open research fund of Songshan Lake Materials Laboratory(2021SLABFK02)the National Key Research and Development Program of China(2017YFA0206600)the National Natural Science Foundation of China(51773045,21772030,51922032 and 21961160720)。
文摘The development of low-bandgap nonfullerene acceptors and wide-bandgap polymer donors speeds up the advance of organic solar cells(OSCs)[1-17]. Wide-bandgap copolymers based on fused-ring acceptor units are ideal donor materials due to their low-lying HOMO levels, high hole mobilities and complementary light absorption to nonfullerene acceptors[18-25]. Currently, high-performance donors with 18%power conversion efficiencies(PCEs) belong to this type.
基金the Central Government Guided Local Science and Technology Development Projects(YDZJSX2021A010)China Postdoctoral Science Foundation(No.2022M710541)+5 种基金the National Natural Science Foundation of China(51704209,52274397,U1810208)the Projects of International Cooperation in Shanxi(201803D421086)Shanxi Province Patent Promotion Implementation Fund(20200718)Research Project Supported by Shanxi Scholarship Council of China(2022-038)Science and Technology Major Project of Shanxi Province(20191102008,20191102007,20181101008)Taishan Scholars Project Special Fund(2021)。
文摘To investigate the role of pre-twins in Mg alloy sheets during warm planar deformation,the stretch forming is conducted at 200℃.Results suggest the formability of the pre-twinned AZ31 Mg alloy sheet is enhanced to 11.30 mm.The mechanisms for the improved formability and the deformation behaviors during the planar stretch forming are systematically investigated based on the planar stress states.The Schmid factor for deformation mechanisms are calculated,the results reveal that planar stress states extremely affect the Schmid factor for{10-12}twinning.The detwinning is activated and the prismatic slip is enhanced in the pre-twinned sheet,especially under the planar extension stress state in the outer region.Consequently,the thickness-direction strain is accommodated better.The dynamic recrystallization(DRX)type is continuous DRX(CDRX)regardless of the planar stress state.However,the CDRX degree is greater under the planar extension stress state.Some twin lattices deviate from the perfect{10-12}twinning relation due to the planar compression stress state and the CDRX.The basal texture is weakened when the planar stress state tends to change the texture components.
基金supported by the National Natural Science Foundation of China (No.21503110)the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)。
文摘It remains as a challenge for realizing efficient photo-responsive catalysts towards largescale degradation of organic pollutants under natural sunlight.This work reports a new pore engineering strategy for creating ultra-porous g-C_(3)N_(4) micro-tubes with an unprecedentedly high specific surface area of 152.96 m^(2)/g.This is mainly associated with releasing internal vapor pressure in the autoclave where the hydrothermal treatment of the urea/melamine mixture is processed.Supported by microscopic observation,porosity measurement and spectroscopic characterization,it is found that releasing the pressure at halfway of hydrothermal process is vital for forming exfoliated rod-like precursors and the de-aggregation of these rods presents substantial benefits on the production of mesopores on g-C_(3)N_(4) microtubes during the calcination of precursors.This offers a large number of reactive sites required by photocatalytic reaction.Coupling these micro-tubes with Ti_(3)C_(2)T_(X) nanosheets via electrostatic interaction yields a 1D/2D heterojunction with a close interfacial contact.The addition of metallically conductive Ti_(3)C_(2)T_(X) nanosheets accelerates the separation between electrons and holes,and also enhances the light absorption.All these merits of structural design lead to forming a group of highly efficient catalysts demonstrating an excellent photocatalytic degradation rate of k=0.0560 min^(-1)for RhB dyes under 100 mW/cm~2 visible light radiation that micks sunlight outdoors.This laboratory valuation is further supported by an outdoor test that shows a fast degradation rate of 0.0744 min^(-1)under natural sunlight.
基金Financial support from National Natural Science Foundation of China(Nos.21931013 and 22271105)Natural Science Foundation of Fujian Province(No.2022J02009)+2 种基金Open Research Fund of School of Chemistry and Chemical Engineering,Henan Normal Universitythe Instrumental Analysis Center of Huaqiao University for analysis supportthe Subsidized Project for Cultivating Postgraduates’Innovative Ability in Scientific Research of Huaqiao University。
文摘A practical method for the construction of difluoromethylene-containing 1,4-thiazine moieties using readily available diethyl bromodifluoromethanephosphonate(BrCF_(2)PO(OEt)_(2))as difluorocarbene precusor has been developed.This transformation features the efficient capture of difluorocarbene by pyridinium 1,4-zwitterionic thiolates.A series of structurally novel and functionalized difluoromethylene-containing 1,4-thiazine derivatives were thus synthesized in good yields.
基金This work was supported by Basic Frontier Scientific Research of the Chinese Academy of Sciences(ZDBS-LY-JSC041)the National Natural Science Foundation of China(22178348)+1 种基金the open research fund of the State Key Laboratory of Mesoscience and Engineering(MESO-23-D06)the Youth Innovation Promotion Association CAS(292021000085).We also thank Wenchang Wang at Shimadzu(China)for help with the XPS analysis.
文摘MXenes have aroused intensive enthusiasm because of their exotic properties and promising applications.However,to date,they are usually synthesized by etching technologies.Developing synthetic technologies provides more opportunities for innovation and may extend unexplored applications.Here,we report a bottom-up gas-phase synthesis of Cl-terminated MXene(Ti_(2)CCl_(2)).The gas-phase synthesis endows Ti_(2)CCl_(2) with unique surface chemistry,high phase purity,and excellent metallic conductivity,which can be used to accelerate polysulfide conversion kinetics and dramatically prolong the cyclability of Li-S batteries.In-depth mechanistic analysis deciphers the origin of the formation of Ti_(2)CCl_(2) and offers a paradigm for tuning MXene chemical vapor deposition.In brief,the gas-phase synthesis transforms the synthesis of MXenes and unlocks the hardly achieved potentials of MXenes.
基金supported by the National Key Research and Development Program of China(No.2016YFB0300801)the National Natural Science Foundation of China(Nos.51831004,11427806,51671082,51471067).
文摘In the slightly deformed Al-Mg-Si alloys,dislocation-induced precipitates are frequently observed,and they usually line up,forming sophisticated precipitation microstructures.Using atomic-resolution electron microscopy in association with hardness measurements,we systematically investigated these precipitates in relation to the age-hardening responses of the alloys.Our study reveals that the majority of dislocation-induced complex precipitates are actually short-range ordered while long-range disordered polycrystalline precipitates and multiphase composite precipitates,including polycrystalline U2 precipitates,B’/U2,B’-2/U2,B’/B’-2/U2 and’/U2 composite precipitates.It is suggested that the formation of these complex precipitates is mainly owing to a high nucleation rate and rapid growth of different precipitate phases parallel to the associated dislocation lines.Since dislocation-induced precipitates consume more Mg than Si from the matrix and have a high formation kinetics,they will have different impacts on the matrix precipitation in different types of Al-Mg-Si alloys.Our results further demonstrate that for the"normally-β"-hardened"alloy,their formation leads to a coarser precipitate microstructure in the matrix,whereas for the"normally-β’-hardened"alloy,their formation reverses the precipitation pathway in the matrix,resulting in a reduced age-hardening potential of the former alloy and an improved age-hardening potential of the latter alloy.
基金Supported by the National Natural Science Foundation of China (Grant No. 50725413)the National Basic Research Program of China ("973" Project) (Grant No. 2007CB613704)the National Key Technologies R&D Program of China (Grant No. 2006BAE04B09-7)
文摘An improved neural network model was developed for prediction of mechanical properties in the de-sign and development of new types of magnesium alloys by refining the types of input variables and using a more reasonable algorithm. The results showed that the improved model apparently decreased the prediction errors, and raised the accuracy of the prediction results. Better preprocessing parame-ters were found to be [0.15, 0.90] for the tensile strength, [0.1, 0.9] for the yield strength, and [0.15, 0.90] for the elongation. When the above parameters were used, the relativity for predicition of strength was bigger than 0.95. By using improved ANN analysis, more reasonable process parameters and compo- sition could be obtained in some magnesium alloys without addition of strontoum.
基金This work was supported by the National Natural Science Foundation of China(Nos.51775503 and 51875343)the Natural Science Foundation of Zhejiang Province(No.LY17E050020)+1 种基金the China Postdoctoral ScienceFoundation(Nos.2017M620152and 2018T110392)Jiangxi Natural Science Foundation of China(20171BCD40009).
文摘Abrasive wear is a common failure phenomenon that often limits the service life of sealing elements. Evaluation and comparison of the abrasion resistance of polytetrafluoroethylene (PTFE) were conducted using Al2O3particleswithsizesintherange5to200 μmonapin-on-flattribo-testerunderdryreciprocatingsliding conditions at room temperature. Based on the examined worn surface characteristics of both PTFE and 316L stainless steel (as a counterpart) and the analyzed coefficient of friction (COF) evolutions, the wear mechanism and particle size effect have been explored in detail. The results demonstrate that the abrasive size is the main contributing factor, which can drastically impact the wear mechanism and tribological properties of tribo-pairs. The COF exhibits different evolution characteristics (trends) for different abrasive sizes. For moderate particle sizes, the COF trends become more complicated and the most evident wear of the metallic counterpart is evident. The activity behaviors of abrasives are dominated by the particle size. Particles can becomes embedded in one of the tribo-pair materials to plough-cut the counterpart, thus causing two-body abrasive wear. The abrasives can also behave as free rolling bodies, which play the role of third body to realize three-body "PTFE-abrasive-316L"abrasion. When abrasives are involved in the wear process, both the wear rate and COF of the metallic counterpart increase, but the material removal rate of the PTFE is reduced. The results obtained can offer guidelines regarding the design and protection of seals.
基金supported by the National Key Research and Development Program of China(2017YFA0206500)the National Natural Science Foundation of China(21603103,21875194,21902125,91645121)
文摘Pyrolyzed Fe/N/C catalyst has been considered as the most promising candidate to replace Pt for oxygen reduction reaction(ORR) in fuel cells.However,poor stability of Fe/N/C catalyst,mainly attributed to the oxidation corrosion by aggressive ·OH radical,severely hampers its applications.However,the exact mechanism for generation of ·OH is unclear yet.Herein,we developed a fluorescent method to effectively detect ·OH generated from ORR on Fe/N/C catalyst by using coumarin as a fluorescent probe.A great difference in potential dependence between ·OH and H2O2 generated from the ORR was observed,which suggests that ·OH is not generated from the decomposition of H2O2 as traditional viewpoint.
基金financially supported by the National Key Research and Development Program of China(No.2016YFB0300801)the National Natural Science Foundation of China(Nos.51831004,11427806,51671082,51471067)。
文摘Adding alloying elements to improve the performances or the manufacturing processes of Al-Mg-Si alloys has long been a serious issue in developing advanced automotive aluminum materials.The Zn element,among those promising ones,has demonstrated positive alloying effects on Al-Mg-Si alloys.However,the atomic-scale roles of Zn in an age-hardened Al-Mg-Si-Zn alloy have not been adequately understood.Using atomic-resolution electron microscopy,here we report the precise locations of Zn elements in all hardening precipitates involved and their alloying mechanism at the atomic scale when alloying the alloy.Our results show that Zn atoms enter all the major hardening phases to occupy specific featured atomic sites of the original elements,e.g.the Si1 and Mg2 sites in theβ’-2 phase,and modify their crystal structures,interfacial structures and morphologies in characteristic manners.It is revealed that for theβ’-phase,Zn atoms occupy unique atomic sites,whereas for other phases,they demonstrate similar behaviors as other additive alloying elements such as Ag and Cu do.