1T-MoS_(2)nanosheets,with metallic conductivity and high capacity,hold great potential for lithium-ion capacitors(LICs),but suffer from sluggish reaction kinetics due to dense stacking.Herein,1T-MoS_(2)nanosheets with...1T-MoS_(2)nanosheets,with metallic conductivity and high capacity,hold great potential for lithium-ion capacitors(LICs),but suffer from sluggish reaction kinetics due to dense stacking.Herein,1T-MoS_(2)nanosheets with enlarged interlayer spacing,vertically bonded to reduced graphene oxide(rGO)(1T-MoS_(2)/rGO),were designed using a hydrothermal-assisted dispersion and intercalation strategy.The active nitrogen species derived from N,N-dimethylformamide(DMF)not only bridge the rGO and MoS_(2)through strong Mo-N-C bonds to promote the formation of dispersed MoS_(2)nanosheets,but also intercalate into the MoS_(2)structure,further enlarging the interlayer spacing.This unique structure synergistically enhances meso-and microscale mass transfer outside and inside of the few-layered nanosheets,significantly improving electrochemical reaction kinetics and reducing the kinetic mismatch between the anode and cathode.Consequently,the resulting 1T-MoS_(2)/rGO achieves a capacity of 500 mAh g^(-1)after 500 cycles at 5 A g^(-1)and a high rate performance of 587 mAh g^(-1)at a high rate of 10 A g^(-1).Moreover,the assembled 3D vertical 1T-MoS_(2)/rGO//AC LIC delivers a high energy density of 100.3 Wh kg^(-1)at a power density of1.0 kW kg^(-1),and long cycle stability with capacity retention as high as 91.02%after 5000 cycles at 2 A g^(-1).This work provides a generalizable strategy for engineering two-dimensional material-based electrodes,offering new insights into high-performance energy storage systems.展开更多
As a promising cathode material for aqueous zinc-ion batteries,1T-MoS_(2)has been extensively investigated because of its facile two-dimensional ion-diffusion channels and high electrical conductivity.However,the limi...As a promising cathode material for aqueous zinc-ion batteries,1T-MoS_(2)has been extensively investigated because of its facile two-dimensional ion-diffusion channels and high electrical conductivity.However,the limited number of available Zn storage sites,i.e.,limited capacity,hinders its application because the inserted Zn^(2+),which form strong electrostatic interactions with 1T-MoS_(2),preventing subsequent Zn^(2+)insertion.Currently,the approach of enlarging the interlayer distance to reduce electrostatic interactions has been commonly used to enhance the capacity and reduce Zn^(2+)migration barriers.However,an enlarged interlayer spacing can weaken the van der Waals force between 1T-MoS_(2)monolayers,easily disrupting the structural stability.Herein,to address this issue,an effective strategy based on Fe doping is proposed for 1T-MoS_(2)(Fe-1T-MoS_(2)).The theoretical calculations reveal that Fe doping can simultaneously moderate the rate of decrease in the adsorption energy after gradually increasing the number of stored atoms,and enhance the electron delocalization on metal-O bonds.Therefore,the experiment results show that Fe doping can simultaneously activate more Zn storage sites,thus enhancing the capacity,and stabilize the structural stability for improved cycling performance.Consequently,Fe-1T-MoS_(2)exhibits a larger capacity(189 mAh·g^(-1)at 0.1 A·g^(-1))and superior cycling stability(78%capacity retention after 400 cycles at 2 A·g^(-1))than pure 1T-MoS_(2).This work may open up a new avenue for constructing high-performance MoS_(2)-based cathodes.展开更多
Two-dimensional(2D)noble transition-metal dichalcogenide materials(NTMDs)have garnered remarkable attention due to their intriguing properties exhibiting potential applications in nanoelectronics,optoelectronics,and p...Two-dimensional(2D)noble transition-metal dichalcogenide materials(NTMDs)have garnered remarkable attention due to their intriguing properties exhibiting potential applications in nanoelectronics,optoelectronics,and photonics.The electronic structure and physical properties of 2D NTMDs can be effectively modulated using alloy engineering strategy.Nevertheless,the precise growth of wafer-scale 2D NTMDs alloys remains a significant challenge.In this work,we have achieved the controllable preparation of wafer-scale(2-inch)2D PdS_(2x)Se_(2(1-x)) nanofilms(NFs)with fully tunable compositions on various substrates using pre-deposited Pd NFs assisted chemical vapor deposition technique.High-performance photodetectors based on the PdS_(2x)Se_(2(1-x))NFs were fabricated,which exhibit broadband photodetection performance from visible to near-infrared(NIR)wavelength range at room temperature.Significantly,the PdS0.9Se1.1-based photodetectors display a responsivity up to 0.192 A W^(-1) and a large specific detectivity of 5.5×1011 Jones for 850 nm light,enabling an excellent high-resolution NIR single-pixel imaging(SPI)without an additional filtering circuit.Our work paves a new route for the controlled synthesis of wafer-scale and high-quality 2D NTMDs alloy NFs,which is essential for designing advanced optoelectronic devices.展开更多
目的探究纤维蛋白原样蛋白1(fibrinogen-like protein 1,FGL1)和膜联蛋白A11(annexin A11,ANXA11)对肺癌手术患者效用评估价值及与预后的相关性。方法将本院2020年1月至2023年12月接诊的98例肺癌患者纳入肺癌组,另选取98例健康人作为对...目的探究纤维蛋白原样蛋白1(fibrinogen-like protein 1,FGL1)和膜联蛋白A11(annexin A11,ANXA11)对肺癌手术患者效用评估价值及与预后的相关性。方法将本院2020年1月至2023年12月接诊的98例肺癌患者纳入肺癌组,另选取98例健康人作为对照组。受试者入院后分别于空腹状态下采取6 mL肘静脉血,采用ELISA法检测血清ANXA11水平,采用实时荧光定量PCR技术检测ANXA11表达水平。根据术后1个月肿瘤标志物变化、影像学表现和免疫功能指标变化情况分为治疗有效组(n=68)和无效组(n=30)。患者出院后均行12~36个月的随访,根据患者预后情况分为预后良好组(n=63)和预后不良组(n=35)。对比对照组和肺癌组/有效组和无效组/预后FGL1、ANXA11表达差异;ROC分析FGL1、ANXA11单一及联合检测对肺癌手术患者临床效用评估价值;Spearman分析FGL1、ANXA11表达与预后的关系。结果肺癌组FGL1和ANXA11表达水平明显高于对照组(均P<0.05);无效组FGL1和ANXA11表达水平明显高于有效组(均P<0.05);ROC结果显示FGL1、ANXA11单独及联合检测对肺癌手术患者效用评估的曲线线下面积分别为0.928,并且联合检测具有较高的特异性(95.59%)以及敏感度(90.00%),诊断价值显著高于单独检测ROC曲线线下面积(均P<0.05);预后不良组FGL1和ANXA11表达水平明显高于预后良好组(均P<0.05);Spearman相关性结果显示FGL1、ANXA11与肺癌手术患者预后呈显著正相关(r=0.771、0.793,均P<0.05)。结论肺癌患者的FGL1与ANXA11表达水平高于健康人,治疗无效者高于有效者,预后不良者高于良好者,二者单独及联合检测对患者手术治疗效用评估均有价值,且其与预后相关性显著。展开更多
基金the financial support from the National Natural Science Foundation of China(No.52225208 and 51802131)the Training Program for academic and technical leaders in major disciplines of Jiangxi Province-Young Talents(No.20212BCJ23021)the Natural Science Foundation of Jiangxi Province,China(No.20232BAB204020).
文摘1T-MoS_(2)nanosheets,with metallic conductivity and high capacity,hold great potential for lithium-ion capacitors(LICs),but suffer from sluggish reaction kinetics due to dense stacking.Herein,1T-MoS_(2)nanosheets with enlarged interlayer spacing,vertically bonded to reduced graphene oxide(rGO)(1T-MoS_(2)/rGO),were designed using a hydrothermal-assisted dispersion and intercalation strategy.The active nitrogen species derived from N,N-dimethylformamide(DMF)not only bridge the rGO and MoS_(2)through strong Mo-N-C bonds to promote the formation of dispersed MoS_(2)nanosheets,but also intercalate into the MoS_(2)structure,further enlarging the interlayer spacing.This unique structure synergistically enhances meso-and microscale mass transfer outside and inside of the few-layered nanosheets,significantly improving electrochemical reaction kinetics and reducing the kinetic mismatch between the anode and cathode.Consequently,the resulting 1T-MoS_(2)/rGO achieves a capacity of 500 mAh g^(-1)after 500 cycles at 5 A g^(-1)and a high rate performance of 587 mAh g^(-1)at a high rate of 10 A g^(-1).Moreover,the assembled 3D vertical 1T-MoS_(2)/rGO//AC LIC delivers a high energy density of 100.3 Wh kg^(-1)at a power density of1.0 kW kg^(-1),and long cycle stability with capacity retention as high as 91.02%after 5000 cycles at 2 A g^(-1).This work provides a generalizable strategy for engineering two-dimensional material-based electrodes,offering new insights into high-performance energy storage systems.
基金supported by the National Natural Science Foundation of China(No.52102318)the Fellowship of China Postdoctoral Science Foundation(Nos.2021TQ0287 and 2022M722855)Xingdian Talent Support Foundation of Yunnan Province(2020).
文摘As a promising cathode material for aqueous zinc-ion batteries,1T-MoS_(2)has been extensively investigated because of its facile two-dimensional ion-diffusion channels and high electrical conductivity.However,the limited number of available Zn storage sites,i.e.,limited capacity,hinders its application because the inserted Zn^(2+),which form strong electrostatic interactions with 1T-MoS_(2),preventing subsequent Zn^(2+)insertion.Currently,the approach of enlarging the interlayer distance to reduce electrostatic interactions has been commonly used to enhance the capacity and reduce Zn^(2+)migration barriers.However,an enlarged interlayer spacing can weaken the van der Waals force between 1T-MoS_(2)monolayers,easily disrupting the structural stability.Herein,to address this issue,an effective strategy based on Fe doping is proposed for 1T-MoS_(2)(Fe-1T-MoS_(2)).The theoretical calculations reveal that Fe doping can simultaneously moderate the rate of decrease in the adsorption energy after gradually increasing the number of stored atoms,and enhance the electron delocalization on metal-O bonds.Therefore,the experiment results show that Fe doping can simultaneously activate more Zn storage sites,thus enhancing the capacity,and stabilize the structural stability for improved cycling performance.Consequently,Fe-1T-MoS_(2)exhibits a larger capacity(189 mAh·g^(-1)at 0.1 A·g^(-1))and superior cycling stability(78%capacity retention after 400 cycles at 2 A·g^(-1))than pure 1T-MoS_(2).This work may open up a new avenue for constructing high-performance MoS_(2)-based cathodes.
基金supported by Open Research Fund of Songshan Lake Materials Laboratory(No.2023SLABFK08)Key Research and Development Program of Hunan Province(No.2022GK2007)+2 种基金Key Project from Department Education of Hunan Province(No.22A0123)National Natural Science Foundation of China(No.11974301)Graduate Student Research Innovation of Xi-angtan University(No.XDCX2024Y198).
文摘Two-dimensional(2D)noble transition-metal dichalcogenide materials(NTMDs)have garnered remarkable attention due to their intriguing properties exhibiting potential applications in nanoelectronics,optoelectronics,and photonics.The electronic structure and physical properties of 2D NTMDs can be effectively modulated using alloy engineering strategy.Nevertheless,the precise growth of wafer-scale 2D NTMDs alloys remains a significant challenge.In this work,we have achieved the controllable preparation of wafer-scale(2-inch)2D PdS_(2x)Se_(2(1-x)) nanofilms(NFs)with fully tunable compositions on various substrates using pre-deposited Pd NFs assisted chemical vapor deposition technique.High-performance photodetectors based on the PdS_(2x)Se_(2(1-x))NFs were fabricated,which exhibit broadband photodetection performance from visible to near-infrared(NIR)wavelength range at room temperature.Significantly,the PdS0.9Se1.1-based photodetectors display a responsivity up to 0.192 A W^(-1) and a large specific detectivity of 5.5×1011 Jones for 850 nm light,enabling an excellent high-resolution NIR single-pixel imaging(SPI)without an additional filtering circuit.Our work paves a new route for the controlled synthesis of wafer-scale and high-quality 2D NTMDs alloy NFs,which is essential for designing advanced optoelectronic devices.
文摘目的探究纤维蛋白原样蛋白1(fibrinogen-like protein 1,FGL1)和膜联蛋白A11(annexin A11,ANXA11)对肺癌手术患者效用评估价值及与预后的相关性。方法将本院2020年1月至2023年12月接诊的98例肺癌患者纳入肺癌组,另选取98例健康人作为对照组。受试者入院后分别于空腹状态下采取6 mL肘静脉血,采用ELISA法检测血清ANXA11水平,采用实时荧光定量PCR技术检测ANXA11表达水平。根据术后1个月肿瘤标志物变化、影像学表现和免疫功能指标变化情况分为治疗有效组(n=68)和无效组(n=30)。患者出院后均行12~36个月的随访,根据患者预后情况分为预后良好组(n=63)和预后不良组(n=35)。对比对照组和肺癌组/有效组和无效组/预后FGL1、ANXA11表达差异;ROC分析FGL1、ANXA11单一及联合检测对肺癌手术患者临床效用评估价值;Spearman分析FGL1、ANXA11表达与预后的关系。结果肺癌组FGL1和ANXA11表达水平明显高于对照组(均P<0.05);无效组FGL1和ANXA11表达水平明显高于有效组(均P<0.05);ROC结果显示FGL1、ANXA11单独及联合检测对肺癌手术患者效用评估的曲线线下面积分别为0.928,并且联合检测具有较高的特异性(95.59%)以及敏感度(90.00%),诊断价值显著高于单独检测ROC曲线线下面积(均P<0.05);预后不良组FGL1和ANXA11表达水平明显高于预后良好组(均P<0.05);Spearman相关性结果显示FGL1、ANXA11与肺癌手术患者预后呈显著正相关(r=0.771、0.793,均P<0.05)。结论肺癌患者的FGL1与ANXA11表达水平高于健康人,治疗无效者高于有效者,预后不良者高于良好者,二者单独及联合检测对患者手术治疗效用评估均有价值,且其与预后相关性显著。