Al-containing MAX phase ceramic has demonstrated great potential in the field of high-performance low-voltage electrical contact material.Elucidating the anti-arc erosion mechanism of the MAX phase is crucial for furt...Al-containing MAX phase ceramic has demonstrated great potential in the field of high-performance low-voltage electrical contact material.Elucidating the anti-arc erosion mechanism of the MAX phase is crucial for further improving performance,but it is not well-understood.In this study,Ag/Ti_(3)AlC_(2) electrical contact material was synthesized by powder metallurgy and examined by nanoindentation techniques such as constant loading rate indentation,creep testing,and continuous stiffness measurements.Our results indicated a gradual degradation in the nano-mechanical properties of the Ti_(3)AlC_(2) reinforcing phase with increasing arc erosion times,although the rate of this degradation appeared to decelerate over arc erosion times.Specifically,continuous stiffness measurements highlighted the uneven mechanical properties within Ti_(3)AlC_(2),attributing this heterogeneity to the phase’s decomposition.During the early(1-100 times)and intermediate(100-1000 times)stages of arc erosion,the decline in the nano-mechanical properties of Ti_(3)AlC_(2) was primarily ascribed to the decomposition of Ti_(3)AlC_(2) and limited surface oxidation.During the later stage of arc erosion(1000-6200 times),the inner region of Ti_(3)AlC_(2) also sustained arc damage,but a thick oxide layer formed on its surface,enhancing the mechanical properties and overall arc erosion resistance of the Ag/Ti_(3)AlC_(2).展开更多
Rapid charge carrier recombination rate and insufficient light harvesting capacity are two dominat-ing drawbacks encountered in zinc indium sulfide(ZnIn_(2)S_(4))for photocatalytic applications.Herein,a chemical reduc...Rapid charge carrier recombination rate and insufficient light harvesting capacity are two dominat-ing drawbacks encountered in zinc indium sulfide(ZnIn_(2)S_(4))for photocatalytic applications.Herein,a chemical reduction method was performed to combine bimetallic Ag-Pd alloy nanoparticles(NPs)with spherical-like ZnIn_(2)S_(4)(ZIS).By optimizing Ag:Pd molar ratio and overall loading amount,the optimal Ag_(0.25)Pd_(0.75)-ZIS sample exhibited a maximum H_(2)evolution rate(125.4μmol/h)under visible light,which was higher than that of ZIS,Ag-ZIS and Pd-ZIS.The loading of Ag NPs contribution to PHE reaction by its plasmonic effect was negligible compared to that of Pd loading(Schottky effect).The apparent quan-tum yield(AQY)values over Ag_(0.25)Pd_(0.75)-ZIS sample could reach up to 18.3%at 400 nm and 15.8%at 420 nm.The enhanced activity for photocatalytic hydrogen evolution(PHE)over Ag_(0.25)Pd_(0.75)-ZIS sample was mainly due to the bimetallic synergistic effect that presented as follows.Firstly,the plasmon hy-bridization by loading Ag-Pd bimetallic alloy can significantly increase light harvesting capacity of ZIS.Secondly,the optimal Schottky barrier height formed between Ag-Pd alloy and ZIS interface was benefi-cial for prolonging electron-hole pair lifetimes,promoting charge carrier separation and thus facilitating PHE efficiency.Density functional theory(DFT)analysis indicated that the adsorption energy of H∗over Pd_(0.75)Ag_(0.25)alloy was very close to zero and thus theoretically possessed the highest activity for H_(2)evo-lution,which is in line with experimental results.Combined theoretical calculation with experimental results,a reasonable photocatalytic mechanism was proposed and verified.展开更多
Semiconductor materials with heterogeneous interfaces and twin structures generally demonstrate a higher concentration of carriers and better electrical stability.A variety of Cu-doped Co_(0.98)Cu_(x)Mn_(2.02−x)O_(4)(...Semiconductor materials with heterogeneous interfaces and twin structures generally demonstrate a higher concentration of carriers and better electrical stability.A variety of Cu-doped Co_(0.98)Cu_(x)Mn_(2.02−x)O_(4)(0≤x≤0.5)negative temperature coefficient(NTC)ceramics with dual phases and twin structures were successfully prepared in this study.Rietveld refinement indicates that the content of a cubic spinel phase increases with increasing Cu content.The addition of Cu can promote grain growth and densification.Atomic-level structural characterization reveals the evolution of twin morphology from large lamellae with internal fine lamellae(LIT lamellae)to large lamellae without internal fine lamellae(L lamellae)and the distribution of twin boundary defects.First-principles calculations reveal that the dual phases and twin structures have lower oxygen-vacancy formation energy than those in the case of the pure tetragonal and cubic spinel,thereby enhancing the transmission of carriers.Additionally,the three-dimensional charge-density difference shows that metal ions at the interface lose electrons and dwell in high valence states,thereby enhancing electrical stability of the NTC ceramics.Furthermore,the additional Cu ions engage in electron-exchange interactions with Mn and Co ions,thereby reducing resistivity.In comparison to previous Cu-containing systems,the Co_(0.98)Cu_(x)Mn_(2.02−x)O_(4)series exhibit superior stability(aging value≤2.84%),tunable room-temperature resistivity(ρ),and material constant(B)value(17.5Ω·cm≤ρ≤7325Ω·cm,2836 K≤B≤4315 K).These discoveries lay a foundation for designing and developing new NTC ceramics with ultra-high performance.展开更多
基金supported by the National Natural Science Foundation of China(52101064,52171033)Jiangsu Planned Projects for Postdoctoral Research Funds(2020Z158)Natural Science Foundation of Jiangsu Province(BK20220627).
文摘Al-containing MAX phase ceramic has demonstrated great potential in the field of high-performance low-voltage electrical contact material.Elucidating the anti-arc erosion mechanism of the MAX phase is crucial for further improving performance,but it is not well-understood.In this study,Ag/Ti_(3)AlC_(2) electrical contact material was synthesized by powder metallurgy and examined by nanoindentation techniques such as constant loading rate indentation,creep testing,and continuous stiffness measurements.Our results indicated a gradual degradation in the nano-mechanical properties of the Ti_(3)AlC_(2) reinforcing phase with increasing arc erosion times,although the rate of this degradation appeared to decelerate over arc erosion times.Specifically,continuous stiffness measurements highlighted the uneven mechanical properties within Ti_(3)AlC_(2),attributing this heterogeneity to the phase’s decomposition.During the early(1-100 times)and intermediate(100-1000 times)stages of arc erosion,the decline in the nano-mechanical properties of Ti_(3)AlC_(2) was primarily ascribed to the decomposition of Ti_(3)AlC_(2) and limited surface oxidation.During the later stage of arc erosion(1000-6200 times),the inner region of Ti_(3)AlC_(2) also sustained arc damage,but a thick oxide layer formed on its surface,enhancing the mechanical properties and overall arc erosion resistance of the Ag/Ti_(3)AlC_(2).
基金financially supported by the National Natural Science Foundation of China (No. 51902282)Qinglan Project of Jiangsu of China, Postgraduate Research & Practice Innovation Program of Yancheng Institute of Technology (No. KYCX21_XZ005)+2 种基金Open Fund of Key Laboratory for Advanced Technology in Environmental Protection of Jiangsu ProvinceNatural Science Foundation of Jiangsu Province (Nos. BK20211361 and BX2021054)College Natural Science Research Project of Jiangsu Province (No. 20KJA430004)
文摘Rapid charge carrier recombination rate and insufficient light harvesting capacity are two dominat-ing drawbacks encountered in zinc indium sulfide(ZnIn_(2)S_(4))for photocatalytic applications.Herein,a chemical reduction method was performed to combine bimetallic Ag-Pd alloy nanoparticles(NPs)with spherical-like ZnIn_(2)S_(4)(ZIS).By optimizing Ag:Pd molar ratio and overall loading amount,the optimal Ag_(0.25)Pd_(0.75)-ZIS sample exhibited a maximum H_(2)evolution rate(125.4μmol/h)under visible light,which was higher than that of ZIS,Ag-ZIS and Pd-ZIS.The loading of Ag NPs contribution to PHE reaction by its plasmonic effect was negligible compared to that of Pd loading(Schottky effect).The apparent quan-tum yield(AQY)values over Ag_(0.25)Pd_(0.75)-ZIS sample could reach up to 18.3%at 400 nm and 15.8%at 420 nm.The enhanced activity for photocatalytic hydrogen evolution(PHE)over Ag_(0.25)Pd_(0.75)-ZIS sample was mainly due to the bimetallic synergistic effect that presented as follows.Firstly,the plasmon hy-bridization by loading Ag-Pd bimetallic alloy can significantly increase light harvesting capacity of ZIS.Secondly,the optimal Schottky barrier height formed between Ag-Pd alloy and ZIS interface was benefi-cial for prolonging electron-hole pair lifetimes,promoting charge carrier separation and thus facilitating PHE efficiency.Density functional theory(DFT)analysis indicated that the adsorption energy of H∗over Pd_(0.75)Ag_(0.25)alloy was very close to zero and thus theoretically possessed the highest activity for H_(2)evo-lution,which is in line with experimental results.Combined theoretical calculation with experimental results,a reasonable photocatalytic mechanism was proposed and verified.
基金supported by the National Natural Science Foundation of China(Grant No.52002347)Natural Science Foundation of the Jiangsu Higher Education Institutions of China(Grant No.19KJB430039).
文摘Semiconductor materials with heterogeneous interfaces and twin structures generally demonstrate a higher concentration of carriers and better electrical stability.A variety of Cu-doped Co_(0.98)Cu_(x)Mn_(2.02−x)O_(4)(0≤x≤0.5)negative temperature coefficient(NTC)ceramics with dual phases and twin structures were successfully prepared in this study.Rietveld refinement indicates that the content of a cubic spinel phase increases with increasing Cu content.The addition of Cu can promote grain growth and densification.Atomic-level structural characterization reveals the evolution of twin morphology from large lamellae with internal fine lamellae(LIT lamellae)to large lamellae without internal fine lamellae(L lamellae)and the distribution of twin boundary defects.First-principles calculations reveal that the dual phases and twin structures have lower oxygen-vacancy formation energy than those in the case of the pure tetragonal and cubic spinel,thereby enhancing the transmission of carriers.Additionally,the three-dimensional charge-density difference shows that metal ions at the interface lose electrons and dwell in high valence states,thereby enhancing electrical stability of the NTC ceramics.Furthermore,the additional Cu ions engage in electron-exchange interactions with Mn and Co ions,thereby reducing resistivity.In comparison to previous Cu-containing systems,the Co_(0.98)Cu_(x)Mn_(2.02−x)O_(4)series exhibit superior stability(aging value≤2.84%),tunable room-temperature resistivity(ρ),and material constant(B)value(17.5Ω·cm≤ρ≤7325Ω·cm,2836 K≤B≤4315 K).These discoveries lay a foundation for designing and developing new NTC ceramics with ultra-high performance.