Transition metal dichalcogenides(TMDs)are a promising class of layered materials in the post-graphene era,with extensive research attention due to their diverse alternative elements and fascinating semiconductor behav...Transition metal dichalcogenides(TMDs)are a promising class of layered materials in the post-graphene era,with extensive research attention due to their diverse alternative elements and fascinating semiconductor behavior.Binary MX2 layers with different metal and/or chalcogen elements have similar structural parameters but varied optoelectronic properties,providing opportunities for atomically substitutional engineering via partial alteration of metal or/and chalcogenide atoms to produce ternary or quaternary TMDs.The resulting multinary TMD layers still maintain structural integrity and homogeneity while achieving tunable(opto)electronic properties across a full range of composition with arbitrary ratios of introduced metal or chalcogen to original counterparts(0–100%).Atomic substitution in TMD layers offers new adjustable degrees of freedom for tailoring crystal phase,band alignment/structure,carrier density,and surface reactive activity,enabling novel and promising applications.This review comprehensively elaborates on atomically substitutional engineering in TMD layers,including theoretical foundations,synthetic strategies,tailored properties,and superior applications.The emerging type of ternary TMDs,Janus TMDs,is presented specifically to highlight their typical compounds,fabrication methods,and potential applications.Finally,opportunities and challenges for further development of multinary TMDs are envisioned to expedite the evolution of this pivotal field.展开更多
Long-term optical data storage(ODS)technology is essential to break the bottleneck of high energy consumption for information storage in the current era of big data.Here,ODS with an ultralong lifetime of 2×10^(7)...Long-term optical data storage(ODS)technology is essential to break the bottleneck of high energy consumption for information storage in the current era of big data.Here,ODS with an ultralong lifetime of 2×10^(7)years is attained with single ultrafast laser pulse induced reduction of Eu^(3+)ions and tailoring of optical properties inside the Eu-doped aluminosilicate glasses.We demonstrate that the induced local modifications in the glass can stand against the temperature of up to 970 K and strong ultraviolet light irradiation with the power density of 100 kW/cm^(2).Furthermore,the active ions of Eu^(2+)exhibit strong and broadband emission with the full width at half maximum reaching 190 nm,and the photoluminescence(PL)is flexibly tunable in the whole visible region by regulating the alkaline earth metal ions in the glasses.The developed technology and materials will be of great significance in photonic applications such as long-term ODS.展开更多
Defect engineering presents great promise in addressing lower specific capacity,sluggish diffusion kinetics and poor cycling life issues in energy storage devices.Herein,multidimensional(0D/2D/3D) structural defects a...Defect engineering presents great promise in addressing lower specific capacity,sluggish diffusion kinetics and poor cycling life issues in energy storage devices.Herein,multidimensional(0D/2D/3D) structural defects are constructed in WO_(3)/MoO_(2) simultaneously via competing for and sharing with O atoms during simple hydrothermal process.OD and 2D defects tailor local electron,activating more sites and generating built-in electric fields to yield ion reservoir,meanwhile,3D defect owning lower anisotropic property tailors Mg^(2+) diffusion channels to fully exploit Mg^(2+) adsorbed sites induced by OD and 2D defects,enhance the kinetics and maintain structural stability.Benefitted from synergistic effect of 0D/2D/3D structural defects,the designed WO_(3)/MoO_(2) shows the higher specific capacity(112.8 mA h g^(-1) at 50 mA g^(-1) with average attenuation rate per cycle of 0.068%),superior rate capability and excellent cycling stability(specific capacity retention of 80% after 1500 cycles at 1000 mA g^(-1)).This strategy provides design ideas of introducing multidimensional structural defects for tailoring local electron and microstructure to improve energy storage property.展开更多
ZrW_(2)O_(8)is a typical isotropic negative thermal expansion material with cubic structure.However,quenching preparation,pressure phase transition and metastable structure influence its practical applications.Adoptin...ZrW_(2)O_(8)is a typical isotropic negative thermal expansion material with cubic structure.However,quenching preparation,pressure phase transition and metastable structure influence its practical applications.Adopting P to part-substitute W for ZrW_(2-x)P_(x)O_(8-0.5x)has decreased the sintering temperature and avoided the quenching process.When x=0.1,ZrW_(1.9)P_(0.1)O_(7.95)with a stable cubic structure can be obtained at 1150℃.The thermal expansion coefficient is tailored with the P content,and phase transition temperature is lowered.When x=0.5,thermal expansion coefficient attains-13.6×10^(-6)℃^(-1),ZrW_(1.5)P_(0.5)O_(7.75)exhibits enhance negative thermal expansion property.The difference of electronegativity leads to the decrease of phase transition temperature with the increase of P content.The different radii of ions lead to new structure of materials when P substitutes more.The results suggest that the P atom plays the stabilization role in the crystal structure of ZrW_(2-x)P_(x)O_(8-0.5x).展开更多
Background Physical activity(PA)can improve the physical and psychological health of prostate and colorectal cancer survivors,but PA behavior change maintenance is necessary for long-term health benefits.OncoActive is...Background Physical activity(PA)can improve the physical and psychological health of prostate and colorectal cancer survivors,but PA behavior change maintenance is necessary for long-term health benefits.OncoActive is a print-and web-based intervention in which prostate and colorectal cancer patients and survivors receive automatically generated,personalized feedback aimed at integrating PA into daily life to increase and maintain PA.We evaluated the long-term outcomes of OncoActive by examining the 12-month follow-up differences between OncoActive and a control group,and we explored whether PA was maintained during a 6-month non-intervention follow-up period.Methods Prostate or colorectal cancer patients were randomly assigned to an OncoActive(n=249)or a usual care waitlist control group(n=229).OncoActive participants received PA advice and a pedometer.PA outcomes(i.e.,ActiGraph and self-report moderate-to-vigorous intensity PA(MVPA)min/week and days with≥30 min PA)and health-related outcomes(i.e.,fatigue,depression,physical functioning)were assessed at baseline,6 months,and 12 months.Differences between groups and changes over time were assessed with multilevel linear regressions for the primary outcome(ActiGraph MVPA min/week)and all additional outcomes.Results At 12 months,OncoActive participants did not perform better than control group participants at ActiGraph MVPA min/week,self-report MVPA min/week,or ActiGraph days with PA.Only self-report days with PA were significantly higher in OncoActive compared to the control group.For health-related outcomes only long-term fatigue was significantly lower in OncoActive.When exploratively examining PA within OncoActive,the previously found PA effects at the end of the intervention(6 months follow-up)were maintained at 12 months.Furthermore,all PA outcomes improved significantly from baseline to 12 months.The control group showed small but non-significant improvements from 6 months to 12 months(and from baseline to 12 months),resulting in a decline of differences between groups.Conclusion The majority of previously reported significant between-group differences at 6 months follow-up were no longer present at long-term follow-up,possibly because of natural improvement in the control group.At long-term follow-up,fatigue was significantly lower in OncoActive compared to control group participants.Computer-tailored PA advice may give participants an early start toward recovery and potentially contributes to improving long-term health.展开更多
Development of electrodes with high electrocatalytic activity and stability is essential for solving problems that still restrict the extensive application of vanadium redox flow batteries(VRFBs).Here,we designed a no...Development of electrodes with high electrocatalytic activity and stability is essential for solving problems that still restrict the extensive application of vanadium redox flow batteries(VRFBs).Here,we designed a novel negative electrode with superior electrocatalytic activity by tailoring nitrogen functional groups,such as newly formed nitro and pyridinic-N transformed to pyridonic-N,from the prenitrogen-doped electrode.It was experimentally confirmed that an electrode with pyridonic-N and nitro fuctional groups(tailored nitrogen-doped graphite felt,TNGF) has superior electrocatalytic acivity with enhanced electron and mass transfer.Density functional theory calulations demonstrated the pyridonic-N and nitro functional groups promoted the adsorption,charge transfer,and bond formation with the vanadium species,which is consistent with expermental results.In addition,the V2+/V3+redox reaction mechanism on pyridonic-N and nitro functional groups was estabilised based on density functional theory(DFT) results.When TNGF was applied to a VRFB,it enabled enhanced-electrolyte utilization and energy efficiencies(EE) of 57.9% and 64.6%,respectively,at a current density of 250 mA cm^(-2).These results are 18.6% and 8.9% higher than those of VRFB with electrode containing graphitic-N and pyridinicN groups.Interestingly,TNGF-based VRFB still operated with an EE of 59% at a high current density of300 mA cm^(-2).The TNGF-based VRFB exhibited stable cycling performance without noticeable decay of EE over 450 charge-discharge cycles at a current density of 250 mA cm^(-2).The results of this study suggest that introducing pyridonic-N and nitro groups on the electrode is effective for improving the electrochemical performance of VRFBs.展开更多
3C-SiC又称β-SiC,有着优异的耐高温、耐腐蚀、耐辐照性能,是反应堆这类复杂环境中的理想材料。近年来,一维碳化硅纳米线材料成为碳化硅材料研究领域的热门研究方向,同时也面临加工手段匮乏、加工难度大的问题。我们通过化学气相沉积法...3C-SiC又称β-SiC,有着优异的耐高温、耐腐蚀、耐辐照性能,是反应堆这类复杂环境中的理想材料。近年来,一维碳化硅纳米线材料成为碳化硅材料研究领域的热门研究方向,同时也面临加工手段匮乏、加工难度大的问题。我们通过化学气相沉积法成功制备了含有高密度堆叠层错的3C-SiC纳米线,并采用扫描电子显微镜(Scanning Electron Microscope,SEM)、透射电子显微镜(Transmission Electron Microscope,TEM)、X射线衍射(X-Ray Diffraction,XRD)以及拉曼光谱(Raman spectrum)等多种手段对制备出来的碳化硅纳米线进行了微观结构表征,揭示了其独特的微观形态和晶体结构特征;进一步研究了超声裁剪碳化硅纳米线,利用“气泡-射流”模型结合碳化硅纳米线的形态解释了碳化硅纳米线的超声裁剪过程,探索了碳化硅纳米线的直径、强度、缺陷等对其在超声过程中断裂行为的影响。本研究为碳化硅纳米线的超声裁剪加工和纳米线的强度研究提供了新的视角,对于未来碳化硅纳米线在核能领域的应用具有重要的意义。展开更多
基金This work was supported by National Key R&D Program of China(2021YFF1200200)Peiyang Talents Project of Tianjin University.
文摘Transition metal dichalcogenides(TMDs)are a promising class of layered materials in the post-graphene era,with extensive research attention due to their diverse alternative elements and fascinating semiconductor behavior.Binary MX2 layers with different metal and/or chalcogen elements have similar structural parameters but varied optoelectronic properties,providing opportunities for atomically substitutional engineering via partial alteration of metal or/and chalcogenide atoms to produce ternary or quaternary TMDs.The resulting multinary TMD layers still maintain structural integrity and homogeneity while achieving tunable(opto)electronic properties across a full range of composition with arbitrary ratios of introduced metal or chalcogen to original counterparts(0–100%).Atomic substitution in TMD layers offers new adjustable degrees of freedom for tailoring crystal phase,band alignment/structure,carrier density,and surface reactive activity,enabling novel and promising applications.This review comprehensively elaborates on atomically substitutional engineering in TMD layers,including theoretical foundations,synthetic strategies,tailored properties,and superior applications.The emerging type of ternary TMDs,Janus TMDs,is presented specifically to highlight their typical compounds,fabrication methods,and potential applications.Finally,opportunities and challenges for further development of multinary TMDs are envisioned to expedite the evolution of this pivotal field.
基金supports from the National Key R&D Program of China (No. 2021YFB2802000 and 2021YFB2800500)the National Natural Science Foundation of China (Grant Nos. U20A20211, 51902286, 61775192, 61905215, and 62005164)+2 种基金Key Research Project of Zhejiang Labthe State Key Laboratory of High Field Laser Physics (Shanghai Institute of Optics and Fine Mechanics, Chinese Academy of Sciences)China Postdoctoral Science Foundation (2021M702799)。
文摘Long-term optical data storage(ODS)technology is essential to break the bottleneck of high energy consumption for information storage in the current era of big data.Here,ODS with an ultralong lifetime of 2×10^(7)years is attained with single ultrafast laser pulse induced reduction of Eu^(3+)ions and tailoring of optical properties inside the Eu-doped aluminosilicate glasses.We demonstrate that the induced local modifications in the glass can stand against the temperature of up to 970 K and strong ultraviolet light irradiation with the power density of 100 kW/cm^(2).Furthermore,the active ions of Eu^(2+)exhibit strong and broadband emission with the full width at half maximum reaching 190 nm,and the photoluminescence(PL)is flexibly tunable in the whole visible region by regulating the alkaline earth metal ions in the glasses.The developed technology and materials will be of great significance in photonic applications such as long-term ODS.
基金supported by the National Natural Science Foundation of China under Grant No. 52072196, 52002199, 52002200, 52102106Major Basic Research Program of Natural Science Foundation of Shandong Province under Grant No. ZR2020ZD09+5 种基金the Natural Science Foundation of Shandong Province under Grant No. ZR2019BEM042, ZR2020QE063the Innovation and Technology Program of Shandong Province under Grant No. 2020KJA004the Taishan Scholars Program of Shandong Province under No. ts201511034Postdoctoral Program in Qingdao under No. QDBSH20220202019the innovation Capability Improvement Project of Small and Medium-sized Technological Enterprises in Shandong Province under No. 2021TSGC1156the Financial Support From the Qingdao West Coast New Area Science and Technology Project under No. 2020-104。
文摘Defect engineering presents great promise in addressing lower specific capacity,sluggish diffusion kinetics and poor cycling life issues in energy storage devices.Herein,multidimensional(0D/2D/3D) structural defects are constructed in WO_(3)/MoO_(2) simultaneously via competing for and sharing with O atoms during simple hydrothermal process.OD and 2D defects tailor local electron,activating more sites and generating built-in electric fields to yield ion reservoir,meanwhile,3D defect owning lower anisotropic property tailors Mg^(2+) diffusion channels to fully exploit Mg^(2+) adsorbed sites induced by OD and 2D defects,enhance the kinetics and maintain structural stability.Benefitted from synergistic effect of 0D/2D/3D structural defects,the designed WO_(3)/MoO_(2) shows the higher specific capacity(112.8 mA h g^(-1) at 50 mA g^(-1) with average attenuation rate per cycle of 0.068%),superior rate capability and excellent cycling stability(specific capacity retention of 80% after 1500 cycles at 1000 mA g^(-1)).This strategy provides design ideas of introducing multidimensional structural defects for tailoring local electron and microstructure to improve energy storage property.
基金Project supported by the Key Scientific and Technological Research Projects of Henan Province,China(Grant Nos.222102220021 and 222102220056)。
文摘ZrW_(2)O_(8)is a typical isotropic negative thermal expansion material with cubic structure.However,quenching preparation,pressure phase transition and metastable structure influence its practical applications.Adopting P to part-substitute W for ZrW_(2-x)P_(x)O_(8-0.5x)has decreased the sintering temperature and avoided the quenching process.When x=0.1,ZrW_(1.9)P_(0.1)O_(7.95)with a stable cubic structure can be obtained at 1150℃.The thermal expansion coefficient is tailored with the P content,and phase transition temperature is lowered.When x=0.5,thermal expansion coefficient attains-13.6×10^(-6)℃^(-1),ZrW_(1.5)P_(0.5)O_(7.75)exhibits enhance negative thermal expansion property.The difference of electronegativity leads to the decrease of phase transition temperature with the increase of P content.The different radii of ions lead to new structure of materials when P substitutes more.The results suggest that the P atom plays the stabilization role in the crystal structure of ZrW_(2-x)P_(x)O_(8-0.5x).
基金funded by the Dutch Cancer Society (Koningin Wilhelmina Kankerfonds Kankerbestrijding,Grant No.NOU2012-5585).
文摘Background Physical activity(PA)can improve the physical and psychological health of prostate and colorectal cancer survivors,but PA behavior change maintenance is necessary for long-term health benefits.OncoActive is a print-and web-based intervention in which prostate and colorectal cancer patients and survivors receive automatically generated,personalized feedback aimed at integrating PA into daily life to increase and maintain PA.We evaluated the long-term outcomes of OncoActive by examining the 12-month follow-up differences between OncoActive and a control group,and we explored whether PA was maintained during a 6-month non-intervention follow-up period.Methods Prostate or colorectal cancer patients were randomly assigned to an OncoActive(n=249)or a usual care waitlist control group(n=229).OncoActive participants received PA advice and a pedometer.PA outcomes(i.e.,ActiGraph and self-report moderate-to-vigorous intensity PA(MVPA)min/week and days with≥30 min PA)and health-related outcomes(i.e.,fatigue,depression,physical functioning)were assessed at baseline,6 months,and 12 months.Differences between groups and changes over time were assessed with multilevel linear regressions for the primary outcome(ActiGraph MVPA min/week)and all additional outcomes.Results At 12 months,OncoActive participants did not perform better than control group participants at ActiGraph MVPA min/week,self-report MVPA min/week,or ActiGraph days with PA.Only self-report days with PA were significantly higher in OncoActive compared to the control group.For health-related outcomes only long-term fatigue was significantly lower in OncoActive.When exploratively examining PA within OncoActive,the previously found PA effects at the end of the intervention(6 months follow-up)were maintained at 12 months.Furthermore,all PA outcomes improved significantly from baseline to 12 months.The control group showed small but non-significant improvements from 6 months to 12 months(and from baseline to 12 months),resulting in a decline of differences between groups.Conclusion The majority of previously reported significant between-group differences at 6 months follow-up were no longer present at long-term follow-up,possibly because of natural improvement in the control group.At long-term follow-up,fatigue was significantly lower in OncoActive compared to control group participants.Computer-tailored PA advice may give participants an early start toward recovery and potentially contributes to improving long-term health.
基金financially supported by the Research Program from Korea Institute of Industrial Technology(EM220011)the Technology Innovation Program(20020229,Development of technology for manufacturing catalysts and electrode parts by use of low contents precious metals of rare metals) funded by the Ministry of Trade,Industry&Energy(MOTIE,Korea)+2 种基金the National Research Foundation of Korea(NRF) grant funded by the Korea government(MSIT)(2022R1F1A1072569)supported by the Basic Science Research Program through the National Research Foundation of Korea(NRF) funded by the Ministry of Science,ICT & Future Planning(NRF2020R1C1C1010493)“Regional Innovation Strategy(RIS)” through the National Research Foundation of Korea(NRF) funded by the Ministry of Education(MOE)(2021RIS-004)。
文摘Development of electrodes with high electrocatalytic activity and stability is essential for solving problems that still restrict the extensive application of vanadium redox flow batteries(VRFBs).Here,we designed a novel negative electrode with superior electrocatalytic activity by tailoring nitrogen functional groups,such as newly formed nitro and pyridinic-N transformed to pyridonic-N,from the prenitrogen-doped electrode.It was experimentally confirmed that an electrode with pyridonic-N and nitro fuctional groups(tailored nitrogen-doped graphite felt,TNGF) has superior electrocatalytic acivity with enhanced electron and mass transfer.Density functional theory calulations demonstrated the pyridonic-N and nitro functional groups promoted the adsorption,charge transfer,and bond formation with the vanadium species,which is consistent with expermental results.In addition,the V2+/V3+redox reaction mechanism on pyridonic-N and nitro functional groups was estabilised based on density functional theory(DFT) results.When TNGF was applied to a VRFB,it enabled enhanced-electrolyte utilization and energy efficiencies(EE) of 57.9% and 64.6%,respectively,at a current density of 250 mA cm^(-2).These results are 18.6% and 8.9% higher than those of VRFB with electrode containing graphitic-N and pyridinicN groups.Interestingly,TNGF-based VRFB still operated with an EE of 59% at a high current density of300 mA cm^(-2).The TNGF-based VRFB exhibited stable cycling performance without noticeable decay of EE over 450 charge-discharge cycles at a current density of 250 mA cm^(-2).The results of this study suggest that introducing pyridonic-N and nitro groups on the electrode is effective for improving the electrochemical performance of VRFBs.
文摘3C-SiC又称β-SiC,有着优异的耐高温、耐腐蚀、耐辐照性能,是反应堆这类复杂环境中的理想材料。近年来,一维碳化硅纳米线材料成为碳化硅材料研究领域的热门研究方向,同时也面临加工手段匮乏、加工难度大的问题。我们通过化学气相沉积法成功制备了含有高密度堆叠层错的3C-SiC纳米线,并采用扫描电子显微镜(Scanning Electron Microscope,SEM)、透射电子显微镜(Transmission Electron Microscope,TEM)、X射线衍射(X-Ray Diffraction,XRD)以及拉曼光谱(Raman spectrum)等多种手段对制备出来的碳化硅纳米线进行了微观结构表征,揭示了其独特的微观形态和晶体结构特征;进一步研究了超声裁剪碳化硅纳米线,利用“气泡-射流”模型结合碳化硅纳米线的形态解释了碳化硅纳米线的超声裁剪过程,探索了碳化硅纳米线的直径、强度、缺陷等对其在超声过程中断裂行为的影响。本研究为碳化硅纳米线的超声裁剪加工和纳米线的强度研究提供了新的视角,对于未来碳化硅纳米线在核能领域的应用具有重要的意义。