针对光固化Al2O3陶瓷在脱脂烧结后易形成孔洞、力学性能差的问题,系统研究了石墨烯添加对陶瓷浆料流变性、沉降性、固化行为及烧结体力学性能的影响。采用γ-缩水甘油醚氧丙基三甲氧基硅烷(KH560)对Al2O3粉体进行表面改性,并加入不同含...针对光固化Al2O3陶瓷在脱脂烧结后易形成孔洞、力学性能差的问题,系统研究了石墨烯添加对陶瓷浆料流变性、沉降性、固化行为及烧结体力学性能的影响。采用γ-缩水甘油醚氧丙基三甲氧基硅烷(KH560)对Al2O3粉体进行表面改性,并加入不同含量的石墨烯,制备高固相、低粘度的光固化浆料。通过傅里叶红外光谱、旋转流变仪、沉降试验及Beer-Lambert模型分析,优化了浆料配方与光固化工艺参数。结果表明:当KH560含量为2.5wt%、石墨烯含量为0.01wt%时,浆料粘度最低、沉降分层最少;在曝光时间4 s条件下,添加0.01wt%石墨烯的浆料透射深度为382μm,临界曝光能量为44.3 m J/cm2。经1750℃烧结后,陶瓷零件致密度达99.7%,弯曲强度为27.61 MPa,维氏硬度为13.45GPa。石墨烯通过位阻效应及裂纹偏转机制有效促进了烧结致密化并改善了力学性能。本研究为光固化增材制造高致密、高性能氧化铝陶瓷提供了试验依据。展开更多
Magnesium hydride serves as a promising solid-state hydrogen storage material owing to its high potential.However,its practical applications are constrained by the high enthalpy of hydrogen absorption and slow kinetic...Magnesium hydride serves as a promising solid-state hydrogen storage material owing to its high potential.However,its practical applications are constrained by the high enthalpy of hydrogen absorption and slow kinetics.In this study,we prepared a Ni/Ti3O5@graphene oxide(GO)dual-heterojunction composite material via solvent heating,electrostatic adsorption,and calcination to improve the hydrogen storage capabilities of MgH2.Adding Ni/Ti3O5@GO to MgH2 lowered the initial dehydrogenation temperature of MgH2 to 183℃;at a dehydrogenation temperature of 275℃,6.4 wt.%of H2 escaped from the MgH2 bulk.In addition,the hydrogen storage material absorbed 1.8 wt.%H2 at 30℃ for 30 min.The calculated activation energy of dehydrogenation was 48.221±0.141 kJ·mol-1,which was significantly lower than that of the ball-milled MgH2(112.63±1.44 kJ·mol-1).Mechanistic analysis results revealed that the heterojunction constructed from the multiphase compound system provided a large number of active sites and hydrogen diffusion routes,resulting in a synergistic catalytic effect that enhanced the hydrogen storage capacity of MgH2.In this work,we clarified the compositions of fuzzy interfaces in heterostructured materials by conducting ultraviolet photoelectron spectroscopy tests and identified key composite materials for the formation of heterojunctions.展开更多
Ni/Al_2O_3-SiO_2 catalysts were synthesized via one-step method employing SiO_2 as an additive for the selective hydrogenation of butyne-1,4-diol(B_3D) to butane-1,4-diol(B1D). The prepared catalysts were evaluated by...Ni/Al_2O_3-SiO_2 catalysts were synthesized via one-step method employing SiO_2 as an additive for the selective hydrogenation of butyne-1,4-diol(B_3D) to butane-1,4-diol(B1D). The prepared catalysts were evaluated by a series of characterization techniques including BET, XRD, SEM, EDX-mapping, TEM, H_2-TPR, XPS, NH_3-TPD and Py-FTIR. Compared to Ni/Al_2O_3 catalyst, the SiO_2-doped samples exhibited better B_3D conversion. SiO_2 could help to form a strong interaction between NiO with the support, which inhibited Ni agglomeration at high temperature, improved the Ni dispersion, and enhanced the hydrogenation activity. B_1D selectivity was mainly influenced by the quantity of Lewis acid sites in addition to the Ni dispersion. The catalyst with a silica loading of 6.4% demonstrated an excellent selectivity of 75.18%(by 13% higher than the contrastive Ni/Al_2O_3 catalyst), which was attributed to the larger amount of Lewis acid sites and the moderate interaction between NiO with the support, which could facilitate the nickel dispersion on a preferable surface area of 176.3 m^2/g of support.展开更多
BNp/Al2O3-SiO2 system ceramic matrix composites with different volume fractions (10%-60%) of hexagonal BN particulates (BNp) were prepared by hot-press sintering technique. Phase components, microstructure, mechan...BNp/Al2O3-SiO2 system ceramic matrix composites with different volume fractions (10%-60%) of hexagonal BN particulates (BNp) were prepared by hot-press sintering technique. Phase components, microstructure, mechanical properties and plasma erosion resistance were also investigated. With the increase of h-BNp content, relative density and Vickers' hardness of the composite ceramics decrease, while the flexural strength, elastic modulus and fracture toughness increase and then decrease. The plasma erosion resistance linearly deteriorated with the increase of BNp content which is mainly determined by the density, crystal structure and atomic number of the elements.展开更多
This article reports the production of COx free hydrogen and carbon nanofibers by the catalytic decomposition of methane over Ni-Al2O3-SiO2 catalysts. The influence of reaction temperature, pretreatment temperature, a...This article reports the production of COx free hydrogen and carbon nanofibers by the catalytic decomposition of methane over Ni-Al2O3-SiO2 catalysts. The influence of reaction temperature, pretreatment temperature, and effect of reductive pretreatment on the decomposition of methane activity is investigated. The physico-chemical characteristics of fresh and deactivated samples were characterized using BET-SA, XRD, TPR, SEM/TEM, CHNS analyses and correlated with the methane decomposition results obtained. The Ni-Al-Si (4 : 0.5 : 1.5) catalyst reduced with hydrazine hydrate produced better H2 yields of ca. 1815 mol H2/mol Ni than the catalyst reduced with 5% H2/N2.展开更多
According to the design principle of the central composite experimental,the method of response surface analysis with three factors and three levels was adopted based on one factor test.A second-order quadratic equatio...According to the design principle of the central composite experimental,the method of response surface analysis with three factors and three levels was adopted based on one factor test.A second-order quadratic equation for photocatalysis of Procion Red MX-5B was built.Response surface and contour were graphed with the decoloration rate of Procion Red MX-5B as the response value.Based on the analysis of the response surface plots and their corresponding contour plots,effects of pH value,irradiation time and catalyst loading were explored.By using this new method,the optimum decoloration condition was obtained as follows:pH value,1.3;irradiation time,49.9 min;catalyst loading,0.57 g/L.In the optimization,R-Squared and Adj R-Squared correlation coefficients for quadratic model were evaluated quite satisfactorily as 0.9310 and 0.8620,respectively.Under the optimum conditions established,the performance of 99.47% for color removal was experimentally reached.It was found that all factors considered have an important effect on the decolorization efficiency of Procion Red MX-5B.By the ANOVA analysis and model confirmation the optimal solution obtained using RSM was experimentally validated and credible with preferable instructional ability for experiments.展开更多
Through measuring the coefficient of linear expansion, the structure and properties of the Li2O-Al2O3-SiO2 low expansion glass ceramics containing B2O3 are studied by JR and XRD. It is shoutn that the IR method is eff...Through measuring the coefficient of linear expansion, the structure and properties of the Li2O-Al2O3-SiO2 low expansion glass ceramics containing B2O3 are studied by JR and XRD. It is shoutn that the IR method is efficient in the study of the glass-ceramics structure. There is a " Boron abnormality" in the system which has an important influence on the properties of the glass-ceramics.展开更多
P2-type nickel-manganese-based layered oxides are promising cathode materials for sodium-ion batteries(SIBs),but their application is limited by initial specific capacity and anion redox instability.Herein,a P2/O3 bip...P2-type nickel-manganese-based layered oxides are promising cathode materials for sodium-ion batteries(SIBs),but their application is limited by initial specific capacity and anion redox instability.Herein,a P2/O3 biphasic Na0.67Ni0.33Mn0.6Cu0.05Mg0.07Ti0.01O2(Ni33Mn60)was prepared by adjusting the Ni/Mn ratio with as Na0.67Ni0.23Mn0.65Cu0.05Mg0.07Ti0.01O2(Ni23Mn65)matrix and is reported to exhibit high initial discharge capacity,cyclability and rate capability.The density functional theory(DFT)calculation and experimental data prove the enhancement of the Mn3+/Mn4+redox process to improve the specific discharge capacity and the P2/O3biphasic structure to optimize the anion kinetics.The synthesized oxide Ni33Mn60 delivers a high initial discharge specific capacity of 140.21 mAh g-1,a crucial discharge capacity of 76.07 mAh g-1at 10C,a preferable capacity retention rate of 78.97%after 200 cycles at 5C and cycle stability at high voltages above 4.3V.In situ X-ray diffraction(XRD)and galvanostatic intermittent titration technique(GITT)tests show that Ni33Mn60 has reversible structure evolution and fast Na+diffusion kinetics due to the ion effect and unique P2/O3 biphasic structure,respectively.This work provides a new thought about adjusting matrix ratio for the preparation of P2/O3 biphasic cathode materials for advanced SIBs.展开更多
The ineluctable introduction of lithium salt to polymer solid-state electrolytes incurs a compromise between strength,ionic conductivity,and thickness.Here,we propose Al2O3-coated polyimide(AO/PI)porous film as ...The ineluctable introduction of lithium salt to polymer solid-state electrolytes incurs a compromise between strength,ionic conductivity,and thickness.Here,we propose Al2O3-coated polyimide(AO/PI)porous film as a high-strength substrate to support fast-ion-conducting polymer-in-salt(PIS)solid-state electrolytes,aiming to suppress lithium dendrite growth and improve full-cell performance.The Al2O3coating layer not only refines the wettability of polyimide porous film to PIS,but also performs as a high modulus protective layer to suppress the growth of lithium dendrites.The resulting PI/AO@PIS exhibits a small thickness of only 35μm with an outstanding tensile strength of 11.3 MPa and Young's modulus of 537.6 MPa.In addition,the PI/AO@PIS delivers a high ionic conductivity of 0.1 m S/cm at 25°C.As a result,the PI/AO@PIS enables symmetric Li cells to achieve exceptional cyclability for over 1000 h at 0.1 m A/cm2without noticeable lithium dendrite formation.Moreover,the PI/AO@PIS-based LiFePO4||Li full cells demonstrate outstanding rate performance(125.7 m Ah/g at 5 C)and impressive cycling stability(96.1%capacity retention at 1 C after 200 cycles).This work highlights the efficacy of enhancing the mechanical properties of polymer matrices and extending cell performance through the incorporation of a dense inorganic interface layer.展开更多
An In2O3 supported nickel catalyst has been prepared by wet chemical reduction with sodium borohydride(NaBH4) as a reducing agent for selective hydrogenation of carbon dioxide to methanol. Highly dispersed Ni species ...An In2O3 supported nickel catalyst has been prepared by wet chemical reduction with sodium borohydride(NaBH4) as a reducing agent for selective hydrogenation of carbon dioxide to methanol. Highly dispersed Ni species with intense Ni-In2O3 interaction and enhanced oxygen vacancies have been achieved.The highly dispersed Ni species serve as the active sites for hydrogen activation and hydrogen spillover.Abundant H adatoms are thereby generated for the oxygen vacancy creation on the In2O3 surface. The enhanced surface oxygen vacancies further lead to improved CO2 conversion. As a result, an effective synergy between the active Ni sites and surface oxygen vacancies on In2O3 causes a superior catalytic performance for CO2 hydrogenation with high methanol selectivity. Carbon monoxide is the only by product detected. The formation of methane can be ignored. When the reaction temperature is lower than 225 ℃,the selectivity of methanol is 100%. It is higher than 64% at the temperature range between 225 ℃ and 275 ℃. The methanol selectivity is still higher than 54% at 300 ℃ with a CO2 conversion of 18.47% and a methanol yield of 0.55 gMeOHg-1cath-1(at 5 MPa). The activity of Ni/In2O3 is higher than most of the reported In2O3-based catalysts.展开更多
摘要针对光固化Al2O3陶瓷在脱脂烧结后易形成孔洞、力学性能差的问题,系统研究了石墨烯添加对陶瓷浆料流变性、沉降性、固化行为及烧结体力学性能的影响。采用γ-缩水甘油醚氧丙基三甲氧基硅烷(KH560)对Al2O3粉体进行表面改性,并加入不同含量的石墨烯,制备高固相、低粘度的光固化浆料。通过傅里叶红外光谱、旋转流变仪、沉降试验及Beer-Lambert模型分析,优化了浆料配方与光固化工艺参数。结果表明:当KH560含量为2.5wt%、石墨烯含量为0.01wt%时,浆料粘度最低、沉降分层最少;在曝光时间4 s条件下,添加0.01wt%石墨烯的浆料透射深度为382μm,临界曝光能量为44.3 m J/cm2。经1750℃烧结后,陶瓷零件致密度达99.7%,弯曲强度为27.61 MPa,维氏硬度为13.45GPa。石墨烯通过位阻效应及裂纹偏转机制有效促进了烧结致密化并改善了力学性能。本研究为光固化增材制造高致密、高性能氧化铝陶瓷提供了试验依据。
基金supported by the National Natural Science Foundation of China[grant number U24A2044]Science and Technology Major Program of Guangxi Province[grant number GUIKEAA24206007].
摘要Magnesium hydride serves as a promising solid-state hydrogen storage material owing to its high potential.However,its practical applications are constrained by the high enthalpy of hydrogen absorption and slow kinetics.In this study,we prepared a Ni/Ti3O5@graphene oxide(GO)dual-heterojunction composite material via solvent heating,electrostatic adsorption,and calcination to improve the hydrogen storage capabilities of MgH2.Adding Ni/Ti3O5@GO to MgH2 lowered the initial dehydrogenation temperature of MgH2 to 183℃;at a dehydrogenation temperature of 275℃,6.4 wt.%of H2 escaped from the MgH2 bulk.In addition,the hydrogen storage material absorbed 1.8 wt.%H2 at 30℃ for 30 min.The calculated activation energy of dehydrogenation was 48.221±0.141 kJ·mol-1,which was significantly lower than that of the ball-milled MgH2(112.63±1.44 kJ·mol-1).Mechanistic analysis results revealed that the heterojunction constructed from the multiphase compound system provided a large number of active sites and hydrogen diffusion routes,resulting in a synergistic catalytic effect that enhanced the hydrogen storage capacity of MgH2.In this work,we clarified the compositions of fuzzy interfaces in heterostructured materials by conducting ultraviolet photoelectron spectroscopy tests and identified key composite materials for the formation of heterojunctions.
基金Financial support from the National Natural Science Foundation of China (21163019) is gratefully acknowledged
摘要Ni/Al_2O_3-SiO_2 catalysts were synthesized via one-step method employing SiO_2 as an additive for the selective hydrogenation of butyne-1,4-diol(B_3D) to butane-1,4-diol(B1D). The prepared catalysts were evaluated by a series of characterization techniques including BET, XRD, SEM, EDX-mapping, TEM, H_2-TPR, XPS, NH_3-TPD and Py-FTIR. Compared to Ni/Al_2O_3 catalyst, the SiO_2-doped samples exhibited better B_3D conversion. SiO_2 could help to form a strong interaction between NiO with the support, which inhibited Ni agglomeration at high temperature, improved the Ni dispersion, and enhanced the hydrogenation activity. B_1D selectivity was mainly influenced by the quantity of Lewis acid sites in addition to the Ni dispersion. The catalyst with a silica loading of 6.4% demonstrated an excellent selectivity of 75.18%(by 13% higher than the contrastive Ni/Al_2O_3 catalyst), which was attributed to the larger amount of Lewis acid sites and the moderate interaction between NiO with the support, which could facilitate the nickel dispersion on a preferable surface area of 176.3 m^2/g of support.
基金Project(HIT.NSRIF.2010112)supported by the Fundamental Research Fund for the Central Universities,ChinaProjects(50902030,51021002)supported by the National Natural Science Foundation of China
摘要BNp/Al2O3-SiO2 system ceramic matrix composites with different volume fractions (10%-60%) of hexagonal BN particulates (BNp) were prepared by hot-press sintering technique. Phase components, microstructure, mechanical properties and plasma erosion resistance were also investigated. With the increase of h-BNp content, relative density and Vickers' hardness of the composite ceramics decrease, while the flexural strength, elastic modulus and fracture toughness increase and then decrease. The plasma erosion resistance linearly deteriorated with the increase of BNp content which is mainly determined by the density, crystal structure and atomic number of the elements.
摘要This article reports the production of COx free hydrogen and carbon nanofibers by the catalytic decomposition of methane over Ni-Al2O3-SiO2 catalysts. The influence of reaction temperature, pretreatment temperature, and effect of reductive pretreatment on the decomposition of methane activity is investigated. The physico-chemical characteristics of fresh and deactivated samples were characterized using BET-SA, XRD, TPR, SEM/TEM, CHNS analyses and correlated with the methane decomposition results obtained. The Ni-Al-Si (4 : 0.5 : 1.5) catalyst reduced with hydrazine hydrate produced better H2 yields of ca. 1815 mol H2/mol Ni than the catalyst reduced with 5% H2/N2.
基金Sponsored by the National Natural Science Foundation of China (Grant No. 51078100)the National Creative Research Groups granted by NSFC(Grant No. 50821002)+1 种基金Excellent Youth Foundation of Heilongjiang Scientific Committee(Grant No. JC2010-03)State Key Laboratory of Urban Water Resource and Environment(Grant No. 2010DX11)
摘要According to the design principle of the central composite experimental,the method of response surface analysis with three factors and three levels was adopted based on one factor test.A second-order quadratic equation for photocatalysis of Procion Red MX-5B was built.Response surface and contour were graphed with the decoloration rate of Procion Red MX-5B as the response value.Based on the analysis of the response surface plots and their corresponding contour plots,effects of pH value,irradiation time and catalyst loading were explored.By using this new method,the optimum decoloration condition was obtained as follows:pH value,1.3;irradiation time,49.9 min;catalyst loading,0.57 g/L.In the optimization,R-Squared and Adj R-Squared correlation coefficients for quadratic model were evaluated quite satisfactorily as 0.9310 and 0.8620,respectively.Under the optimum conditions established,the performance of 99.47% for color removal was experimentally reached.It was found that all factors considered have an important effect on the decolorization efficiency of Procion Red MX-5B.By the ANOVA analysis and model confirmation the optimal solution obtained using RSM was experimentally validated and credible with preferable instructional ability for experiments.
摘要Through measuring the coefficient of linear expansion, the structure and properties of the Li2O-Al2O3-SiO2 low expansion glass ceramics containing B2O3 are studied by JR and XRD. It is shoutn that the IR method is efficient in the study of the glass-ceramics structure. There is a " Boron abnormality" in the system which has an important influence on the properties of the glass-ceramics.
基金financially supported by the Natural Science Foundation of Jiangsu Province(No.BK20201049)China Postdoctoral Science Foundation(No,2022M711724)+2 种基金the Swedish Energy Agency(Nos.P2022-00055 and P2023-00603)STandUP for EnergyMAX IV Laboratory for time on Balder beamline(No.20240704)
摘要P2-type nickel-manganese-based layered oxides are promising cathode materials for sodium-ion batteries(SIBs),but their application is limited by initial specific capacity and anion redox instability.Herein,a P2/O3 biphasic Na0.67Ni0.33Mn0.6Cu0.05Mg0.07Ti0.01O2(Ni33Mn60)was prepared by adjusting the Ni/Mn ratio with as Na0.67Ni0.23Mn0.65Cu0.05Mg0.07Ti0.01O2(Ni23Mn65)matrix and is reported to exhibit high initial discharge capacity,cyclability and rate capability.The density functional theory(DFT)calculation and experimental data prove the enhancement of the Mn3+/Mn4+redox process to improve the specific discharge capacity and the P2/O3biphasic structure to optimize the anion kinetics.The synthesized oxide Ni33Mn60 delivers a high initial discharge specific capacity of 140.21 mAh g-1,a crucial discharge capacity of 76.07 mAh g-1at 10C,a preferable capacity retention rate of 78.97%after 200 cycles at 5C and cycle stability at high voltages above 4.3V.In situ X-ray diffraction(XRD)and galvanostatic intermittent titration technique(GITT)tests show that Ni33Mn60 has reversible structure evolution and fast Na+diffusion kinetics due to the ion effect and unique P2/O3 biphasic structure,respectively.This work provides a new thought about adjusting matrix ratio for the preparation of P2/O3 biphasic cathode materials for advanced SIBs.
基金the financial support from the 261Project of MIIT and Natural Science Foundation of Jiangsu Province(No.BK20240179)。
摘要The ineluctable introduction of lithium salt to polymer solid-state electrolytes incurs a compromise between strength,ionic conductivity,and thickness.Here,we propose Al2O3-coated polyimide(AO/PI)porous film as a high-strength substrate to support fast-ion-conducting polymer-in-salt(PIS)solid-state electrolytes,aiming to suppress lithium dendrite growth and improve full-cell performance.The Al2O3coating layer not only refines the wettability of polyimide porous film to PIS,but also performs as a high modulus protective layer to suppress the growth of lithium dendrites.The resulting PI/AO@PIS exhibits a small thickness of only 35μm with an outstanding tensile strength of 11.3 MPa and Young's modulus of 537.6 MPa.In addition,the PI/AO@PIS delivers a high ionic conductivity of 0.1 m S/cm at 25°C.As a result,the PI/AO@PIS enables symmetric Li cells to achieve exceptional cyclability for over 1000 h at 0.1 m A/cm2without noticeable lithium dendrite formation.Moreover,the PI/AO@PIS-based LiFePO4||Li full cells demonstrate outstanding rate performance(125.7 m Ah/g at 5 C)and impressive cycling stability(96.1%capacity retention at 1 C after 200 cycles).This work highlights the efficacy of enhancing the mechanical properties of polymer matrices and extending cell performance through the incorporation of a dense inorganic interface layer.
基金the National Natural Science Foundation of China(No.21536008 and 21621004)。
摘要An In2O3 supported nickel catalyst has been prepared by wet chemical reduction with sodium borohydride(NaBH4) as a reducing agent for selective hydrogenation of carbon dioxide to methanol. Highly dispersed Ni species with intense Ni-In2O3 interaction and enhanced oxygen vacancies have been achieved.The highly dispersed Ni species serve as the active sites for hydrogen activation and hydrogen spillover.Abundant H adatoms are thereby generated for the oxygen vacancy creation on the In2O3 surface. The enhanced surface oxygen vacancies further lead to improved CO2 conversion. As a result, an effective synergy between the active Ni sites and surface oxygen vacancies on In2O3 causes a superior catalytic performance for CO2 hydrogenation with high methanol selectivity. Carbon monoxide is the only by product detected. The formation of methane can be ignored. When the reaction temperature is lower than 225 ℃,the selectivity of methanol is 100%. It is higher than 64% at the temperature range between 225 ℃ and 275 ℃. The methanol selectivity is still higher than 54% at 300 ℃ with a CO2 conversion of 18.47% and a methanol yield of 0.55 gMeOHg-1cath-1(at 5 MPa). The activity of Ni/In2O3 is higher than most of the reported In2O3-based catalysts.