The development of optoelectronic technologies demands photodetectors with miniaturization,broadband operation,high sensitivity,and low power consumption.Although 2D van der Waals(vd W)heterostructures are promising c...The development of optoelectronic technologies demands photodetectors with miniaturization,broadband operation,high sensitivity,and low power consumption.Although 2D van der Waals(vd W)heterostructures are promising candidates due to their built-in electric fields,ultrafast photocarrier separation,and tunable bandgaps,defect states limit their performance.Therefore,the modulation of the optoelectronic properties in such heterostructures is imperative.Surface charge transfer doping(SCTD)has emerged as a promising strategy for non-destructive modulation of electronic and optoelectronic characteristics in two-dimensional materials.In this work,we demonstrate the construction of high-performance p-i-n vertical heterojunction photodetectors through SCTD of MoTe_(2)/ReS_(2)heterostructure using p-type F_(4)-TCNQ.Systematic characterization reveals that the interfacial doping process effectively amplifies the built-in electric field,enhancing photogenerated carrier separation efficiency.Compared to the pristine heterojunction device,the doped photodetector exhibits remarkable visible to nearinfrared(635-1064 nm)performance.Particularly under 1064 nm illumination at zero bias,the device achieves a responsivity of 2.86 A/W and specific detectivity of 1.41×10^(12)Jones.Notably,the external quantum efficiency reaches an exceptional value of 334%compared to the initial 11.5%,while maintaining ultrafast response characteristics with rise/fall times of 11.6/15.6μs.This work provides new insights into interface engineering through molecular doping for developing high-performance vd W optoelectronic devices.展开更多
Electrochemical CO_(2) reduction reaction(CO_(2)RR) into valuable formate provides a strategy for carbon neutrality.Bismuth(Bi) catalysts,attributed to their appropriate energy barrier of OCHO*intermediate,have demons...Electrochemical CO_(2) reduction reaction(CO_(2)RR) into valuable formate provides a strategy for carbon neutrality.Bismuth(Bi) catalysts,attributed to their appropriate energy barrier of OCHO*intermediate,have demonstrated substantial potential for the advancement of electrocatalytic CO_(2) reduction to formate.However,due to the weak bonding of protons(H^(*)) of Bi,the available protonate of CO_(2) on Bi is insufficient,which limits the formation of OCHO^(*).Prediction by theoretical calculation,chlorine doping can effectively promote the dissociation of H_(2)O and thus achieve effective proton supply.We prepare chlorine-doped Bi(Cl-Bi) via an electrochemical conversion strategy for electroreduction of CO_(2) .An obvious improvement of faradaic efficiency(FE) of formate(96.7% at-0.95 V vs.RHE) can be achieved on Cl-Bi,higher than that of Bi(89.4%).Meanwhile,Cl-Bi has the highest formate production rate of 275 μmol h^(-1)cm^(-2)at-0.95 V vs.RHE,which is 1.2 times higher than that of Bi(224 μmol h^(-1)cm^(-2)).In situ characterizations and kinetic analysis reveal that chlorine doping promotes the activation of H_(2)O and supply sufficient protons to promote the protonation of CO_(2) to OCHO^(*),which is consistent with theoretical calculation.The study presents an effective strategy for rational design of highly efficient electrocatalysts to promote green chemical production.展开更多
LiNiO_(2)(LNO)is one of the most promising cathode materials for lithium-ion batteries.Tungsten element in enhancing the stability of LNO has been researched extensively.However,the understanding of the specific dopin...LiNiO_(2)(LNO)is one of the most promising cathode materials for lithium-ion batteries.Tungsten element in enhancing the stability of LNO has been researched extensively.However,the understanding of the specific doping process and existing form of W are still not perfect.This study proposes a lithium-induced grain boundary phase W doping mechanism.The results demonstrate that the introduced W atomsfirst react with the lithium source to generate a Li–W–O phase at the grain boundary of primary particles.With the increase of lithium ratio,W atoms gradually diffuse from the grain boundary phase to the interior layered structure to achieve W doping.The feasibility of grain boundary phase doping is verified byfirst principles calculation.Furthermore,it is found that the Li2WO4 grain boundary phase is an excellent lithium ion conductor,which can protect the cathode surface and improve the rate performance.The doped W can alleviate the harmful H2↔H3 phase transition,thereby inhibiting the generation of microcracks,and improving the electrochemical performance.Consequently,the 0.3 wt%W-doped sample provides a significant improved capacity retention of 88.5%compared with the pristine LNO(80.7%)after 100 cycles at 2.8–4.3 V under 1C.展开更多
Novel green ceramic pigments Y_(3)Ga_(3)MgSiO_(12)∶xCr^(3+)(x=0−0.2)were successfully synthesized via the conventional solid-state approach.The properties of the pigments were studied by XRD,FE-SEM,UV-Vis spectroscop...Novel green ceramic pigments Y_(3)Ga_(3)MgSiO_(12)∶xCr^(3+)(x=0−0.2)were successfully synthesized via the conventional solid-state approach.The properties of the pigments were studied by XRD,FE-SEM,UV-Vis spectroscopy,XPS,and chromaticity analysis.The findings reveal that the trivalent chromium ions occupy the[Ga1O6]octahedral sites within the garnet lattice,and the relatively weak crystal field environment provided by the matrix endows the pigments with green characteristics.The samples prepared by calcination at 1400℃exhibit the most excellent performance in terms of phase purity,morphology,and color properties.The chromaticity values for the representative sample Y_(3)Ga_(3)MgSiO_(12)∶0.05Cr^(3+)are L^(*)=81.16,a^(*)=−12.53,and b^(*)=12.71,and the color remains stable after the stability test.Moreover,when glazed with Y_(3)Ga_(3)MgSiO_(12)∶xCr^(3+)(x=0−0.2)pigments,the smooth glaze surfaces exhibit vivid and saturated green tones,demonstrating their remarkable coloring capabilities and promising potential as a practical pigment for medium-temperature applications.This research underscores the vast application prospects of Y_(3)Ga_(3)MgSiO_(12)∶Cr^(3+)as an innovative green ceramic pigment.展开更多
Y_(3)Al_(2)Ga_(3)O_(12):Ce^(3+),Cr^(3+)(YAGG:Ce^(3+),Cr^(3+)),as a persistent luminescent material,has advantages of high initial luminescence intensity and long persistent time,which is promising in persistent lumine...Y_(3)Al_(2)Ga_(3)O_(12):Ce^(3+),Cr^(3+)(YAGG:Ce^(3+),Cr^(3+)),as a persistent luminescent material,has advantages of high initial luminescence intensity and long persistent time,which is promising in persistent luminescent material applications.At present,YAGG:Ce^(3+),Cr^(3+)powders exhibit good persistent performance,but their persistent performance of ceramics still needs to be further improved to meet the new requirements.In this work,(Y_(0.998)Ce_(0.002))_(3)(Al_(1-x)Cr_(x))_(2)Ga_(3)O_(12) ceramics with different Cr^(3+)doping concentrations were prepared by solid-state reaction,including air pre-sintering,hot isostatic pressing(HIP)post-treatment and air annealing,to investigate the effects of Cr^(3+)doping concentration on the microstructure,optical properties and persistent performance of the ceramics.The results showed that as the doping concentration of Cr^(3+)increased from 0.025%to 0.2%(in atom),no significant effect of Cr^(3+)concentration on the morphology of pre-sintered ceramics or HIP post-treatment ceramics was observed,but the in-line transmittance gradually increased while the persistent performance gradually decreased.Among them,YAGG:Ce^(3+),Cr^(3+)ceramics doped with 0.025%Cr^(3+)showed the strongest initial luminescence intensity exceeding 6055 mcd/m^(2) and a persistent time of 1030 min after air pre-sintering combined with HIP post-treatment and air annealing.By optimizing the Cr^(3+)doping concentration and the fabrication process,the persistent luminescence(PersL)performance of the YAGG:Ce^(3+),Cr^(3+)ceramics was obviously improved.展开更多
Nickel-rich cathode materials have received widespread attention due to their high energy density.However,the poor rate capability and inferior cycle stability seriously hinder their large-scale application.The tradit...Nickel-rich cathode materials have received widespread attention due to their high energy density.However,the poor rate capability and inferior cycle stability seriously hinder their large-scale application.The traditional co-precipitation method for preparing them has a long process and easily arises agglomeration leading to inhomogeneous element distribution.Here,a novel precursor containing Li element was prepared by ultrafast spray pyrolysis(SP)in 3–5 s.Then the precursor was used to synthesize pristine LiNi_(0.9)Co_(0.05)Mn_(0.05)O_(2)(NCM90)and 1%Mg modified LiNi_(0.9)Co_(0.05)Mn_(0.05)O_(2)(NCM90-Mg1).This method gets rid of mixing Li/Mg source and the precursor prepared by common co-precipitation,thus could achieve homogeneous lithiation and Mg2+doping.The cell parameter c is expanded,and the cation disorder is reduced after Mg2+doping.Furthermore,the harmful H2-H3 phase transition in NCM90-Mg1 is also well suppressed.As a result,the obtained NCM90-Mg1 shows better electrochemical performance than NCM90.Within 2.8–4.3 V(25℃),the specific discharge capacity of NCM90-Mg1 at 5 C is as high as 169.1m Ah/g,and an outstanding capacity retention of 70.0%(10.0%higher than NCM90)can be obtained after400 cycles at 0.5 C.At 45℃,a capacity retention of 81.9%after 100 cycles at 1 C is recorded for NCM90-Mg1.Moreover,the NCM90-Mg1 also exhibits superior cycle stability when cycled at high cut-off voltage(4.5 V,25℃),possessing the capacity retention of 79.2%after 200 cycles at 1 C.Therefore,SP can be proposed as a powerful method for the preparation of multi-element materials for next-generation high energy density LIBs.展开更多
A novel method for preparing Ta-doped Ti02 via using Ta2 05 as the doping source is proposed. The preparation process combines the hydrothernlal fluorination of Ta2O5 and the subsequent formation of Ta-doped TiO2 sol....A novel method for preparing Ta-doped Ti02 via using Ta2 05 as the doping source is proposed. The preparation process combines the hydrothernlal fluorination of Ta2O5 and the subsequent formation of Ta-doped TiO2 sol. The results show that the doped sample annealed at 393 K generates an unstable intermediate NH4 TiOF3, which converts into anatase TiO2 with the increase of temperature. After annealing at ≥673K, the Ta-doped TiO2 nanocrystals with the grain size 〈20nm are obtained. Both the XRD and TG-DSC results confirm that Ta doping prevents the anatase-rutile crystal transition of TiO2. The band gap values of the doped samples, as obtained by UV-vis diffuse reflectance spectra, are smaller than that of pure anatase TiO2. The first-principle pseudopotential method calculations indicate that Ta5＋ lies in the TiO2 lattice at the interstitial position.展开更多
The catalytic direct synthesis of dimethyl carbonate(DMC)from CO_(2)and methanol is a crucial approach to utilizing CO_(2)and producing high-value chemicals.However,the high stability of the CO_(2)molecule imposes the...The catalytic direct synthesis of dimethyl carbonate(DMC)from CO_(2)and methanol is a crucial approach to utilizing CO_(2)and producing high-value chemicals.However,the high stability of the CO_(2)molecule imposes thermodynamic limitations on this reaction pathway,along with challenges related to insufficient catalyst activity and stability.Currently,solutions primarily focus on developing efficient catalyst.Herein,La-doped CeO_(2)nanoflower catalysts(La_(x)CeO_(2))were synthesized via hydrothermal method.Characterization reveals that La doping optimizes the pore structure and enriched oxygen vacancies,thereby enhancing catalytic performance.Notably,La_(0.1)CeO_(2)exhibits the largest pore size and highest oxygen vacancy content,achieving a remarkable DMC productivity of 9.42 mmol/g under 140℃,4 MPa of CO_(2),and 3 h of reactio n,surpassing pure CeO_(2)nano flowers.Based on experimental findings and in-situ diffuse infrared Fourier transform analysis,a plausible reaction pathway was proposed.This work underscores the potential of La_(x)CeO_(2)nano flowers as efficient catalysts for sustainable CO_(2)conversion to DMC.展开更多
Reducing the cost of RuO_(2)/TiO_(2)catalysts is still one of the urgent challenges in catalytic HCl oxidation.In the present work,a Ce-doped TiO_(2)supported RuO_(2)catalyst with a low Ru loading was developed,showin...Reducing the cost of RuO_(2)/TiO_(2)catalysts is still one of the urgent challenges in catalytic HCl oxidation.In the present work,a Ce-doped TiO_(2)supported RuO_(2)catalyst with a low Ru loading was developed,showing a high activity in the catalytic oxidation of HCl to Cl_(2).The results on some extensive characterizations of both Ce-doped TiO_(2)carriers and their supported RuO_(2)catalysts show that the doping of Ce into TiO_(2)can effectively change the lattice parameters of TiO_(2)to improve the dispersion of the active RuO_(2)species on the carrier,which facilitates the production of surface Ru species to expose more active sites for boosting the catalytic performance even under some harsh reaction conditions.This work provides some scientific basis and technical support for chlorine recycling.展开更多
Nitrogen dioxide(NO_(2))is a significant air pollutant with harmful effects on human health and the environment.Timely and accurate monitoring of NO_(2)concentrations is crucial for improving air quality and protectin...Nitrogen dioxide(NO_(2))is a significant air pollutant with harmful effects on human health and the environment.Timely and accurate monitoring of NO_(2)concentrations is crucial for improving air quality and protecting public health.However,quantifying NO_(2)in the presence of other gases remains challenging.Herein,we integrate Ru onto the MoS_(2)surface to form Ru-S-Mo active sites,thereby tuning the electronic structure of MoS_(2)for enhanced NO_(2)detection.This sensor shows excellent sensitivity(29.7%at 100×10^(-6)NO_(2)and 25℃),with a linear response to NO_(2)ranging from 0.5 to 200×10^(-6),and a significantly reduced response/recovery time from 160/3636 s for pure MoS_(2)to 58/427 s for Ru@MoS_(2)at 100×10^(-6)NO_(2).Additionally,the sensor is highly selective for NO_(2),exhibiting a response 14 times higher than for other gases,and possesses strong anti-interference capabilities,accurately quantifying NO_(2)in the presence of varying H_(2)concentrations(10×10^(-6)-200×10^(-6))with a low RSD of 5.34%.A portable wireless NO_(2)monitoring system was successfully constructed using Ru@MoS_(2),enabling real-time gas leak detection(10×10^(-6)-50×10^(-6))with hazard warnings and maintaining a stable response to NO_(2)over a 4-week period.This work extends the gas sensing applications of MoS_(2)and provides a portable,wireless,and high-selectivity NO_(2)sensing method for environmental monitoring and safety assurance.展开更多
The poor corrosion resistance of magnesium(Mg)and its alloys limits their application in various fields.Micro arc oxidation(MAO)coatings can improve the corrosion resistance,but the pore defects and low surface hardne...The poor corrosion resistance of magnesium(Mg)and its alloys limits their application in various fields.Micro arc oxidation(MAO)coatings can improve the corrosion resistance,but the pore defects and low surface hardness make them susceptible to wear and accelerated corrosion during usage.In this study,a ZrO_(2)nanoparticles doped-MAO coating is prepared on the ZK61 Mg alloy by utilizing an MgF_(2)passivation layer to prevent ablation.The ZrO_(2)nanoparticles re-melt and precipitate due to local discharging,which produces evenly dispersed nanocrystals in the MAO coating.As a result,the hardness of the MAO coating with the appropriate ZrO_(2)concentration increases by over 10 times,while the wear rate decreases and corrosion resistance increases.With increasing ZrO_(2)concentrations,the corrosion potentials increase from−1.528 V of the bare ZK61 Mg alloy to−1.184 V,the corrosion current density decreases from 1.065×10^(–4)A cm^(–2)to 3.960×10^(–8)A cm^(–2),and the charge transfer resistance increases from 3.41×10^(2)Ωcm^(2)to 6.782×10^(5)Ωcm^(2).Immersion tests conducted in a salt solution for 28 d reveal minimal corrosion in contrast to severe corrosion on the untreated ZK61 Mg alloy.ZrO_(2)nanoparticles improve the corrosion resistance of MAO coatings by sealing pores and secondary strengthening of the corrosion product layer.展开更多
基金financial support from 2024 Domestic Visiting Scholar Program for Teachers'Professional Development in Universities(Grant No.FX2024022)National Natural Science Foundation of China(Grant No.61904043)。
文摘The development of optoelectronic technologies demands photodetectors with miniaturization,broadband operation,high sensitivity,and low power consumption.Although 2D van der Waals(vd W)heterostructures are promising candidates due to their built-in electric fields,ultrafast photocarrier separation,and tunable bandgaps,defect states limit their performance.Therefore,the modulation of the optoelectronic properties in such heterostructures is imperative.Surface charge transfer doping(SCTD)has emerged as a promising strategy for non-destructive modulation of electronic and optoelectronic characteristics in two-dimensional materials.In this work,we demonstrate the construction of high-performance p-i-n vertical heterojunction photodetectors through SCTD of MoTe_(2)/ReS_(2)heterostructure using p-type F_(4)-TCNQ.Systematic characterization reveals that the interfacial doping process effectively amplifies the built-in electric field,enhancing photogenerated carrier separation efficiency.Compared to the pristine heterojunction device,the doped photodetector exhibits remarkable visible to nearinfrared(635-1064 nm)performance.Particularly under 1064 nm illumination at zero bias,the device achieves a responsivity of 2.86 A/W and specific detectivity of 1.41×10^(12)Jones.Notably,the external quantum efficiency reaches an exceptional value of 334%compared to the initial 11.5%,while maintaining ultrafast response characteristics with rise/fall times of 11.6/15.6μs.This work provides new insights into interface engineering through molecular doping for developing high-performance vd W optoelectronic devices.
基金financially supported by the Natural Science Foundation of Shandong Province (No.ZR2022QE076)the National Natural Science Foundation of China (No.52202092)the Science and Technology Support Plan for Youth Innovation of Colleges and Universities of Shandong Province of China (No.2023KJ104)。
文摘Electrochemical CO_(2) reduction reaction(CO_(2)RR) into valuable formate provides a strategy for carbon neutrality.Bismuth(Bi) catalysts,attributed to their appropriate energy barrier of OCHO*intermediate,have demonstrated substantial potential for the advancement of electrocatalytic CO_(2) reduction to formate.However,due to the weak bonding of protons(H^(*)) of Bi,the available protonate of CO_(2) on Bi is insufficient,which limits the formation of OCHO^(*).Prediction by theoretical calculation,chlorine doping can effectively promote the dissociation of H_(2)O and thus achieve effective proton supply.We prepare chlorine-doped Bi(Cl-Bi) via an electrochemical conversion strategy for electroreduction of CO_(2) .An obvious improvement of faradaic efficiency(FE) of formate(96.7% at-0.95 V vs.RHE) can be achieved on Cl-Bi,higher than that of Bi(89.4%).Meanwhile,Cl-Bi has the highest formate production rate of 275 μmol h^(-1)cm^(-2)at-0.95 V vs.RHE,which is 1.2 times higher than that of Bi(224 μmol h^(-1)cm^(-2)).In situ characterizations and kinetic analysis reveal that chlorine doping promotes the activation of H_(2)O and supply sufficient protons to promote the protonation of CO_(2) to OCHO^(*),which is consistent with theoretical calculation.The study presents an effective strategy for rational design of highly efficient electrocatalysts to promote green chemical production.
基金supported by the National Natural Science Foundation of China(No.52122407,No.52174285,52404317)the Science and Technology Innovation Program of Hunan Province(No.2022RC3048).
文摘LiNiO_(2)(LNO)is one of the most promising cathode materials for lithium-ion batteries.Tungsten element in enhancing the stability of LNO has been researched extensively.However,the understanding of the specific doping process and existing form of W are still not perfect.This study proposes a lithium-induced grain boundary phase W doping mechanism.The results demonstrate that the introduced W atomsfirst react with the lithium source to generate a Li–W–O phase at the grain boundary of primary particles.With the increase of lithium ratio,W atoms gradually diffuse from the grain boundary phase to the interior layered structure to achieve W doping.The feasibility of grain boundary phase doping is verified byfirst principles calculation.Furthermore,it is found that the Li2WO4 grain boundary phase is an excellent lithium ion conductor,which can protect the cathode surface and improve the rate performance.The doped W can alleviate the harmful H2↔H3 phase transition,thereby inhibiting the generation of microcracks,and improving the electrochemical performance.Consequently,the 0.3 wt%W-doped sample provides a significant improved capacity retention of 88.5%compared with the pristine LNO(80.7%)after 100 cycles at 2.8–4.3 V under 1C.
文摘Novel green ceramic pigments Y_(3)Ga_(3)MgSiO_(12)∶xCr^(3+)(x=0−0.2)were successfully synthesized via the conventional solid-state approach.The properties of the pigments were studied by XRD,FE-SEM,UV-Vis spectroscopy,XPS,and chromaticity analysis.The findings reveal that the trivalent chromium ions occupy the[Ga1O6]octahedral sites within the garnet lattice,and the relatively weak crystal field environment provided by the matrix endows the pigments with green characteristics.The samples prepared by calcination at 1400℃exhibit the most excellent performance in terms of phase purity,morphology,and color properties.The chromaticity values for the representative sample Y_(3)Ga_(3)MgSiO_(12)∶0.05Cr^(3+)are L^(*)=81.16,a^(*)=−12.53,and b^(*)=12.71,and the color remains stable after the stability test.Moreover,when glazed with Y_(3)Ga_(3)MgSiO_(12)∶xCr^(3+)(x=0−0.2)pigments,the smooth glaze surfaces exhibit vivid and saturated green tones,demonstrating their remarkable coloring capabilities and promising potential as a practical pigment for medium-temperature applications.This research underscores the vast application prospects of Y_(3)Ga_(3)MgSiO_(12)∶Cr^(3+)as an innovative green ceramic pigment.
基金National Key R&D Program of China(2023YFB3506600)。
文摘Y_(3)Al_(2)Ga_(3)O_(12):Ce^(3+),Cr^(3+)(YAGG:Ce^(3+),Cr^(3+)),as a persistent luminescent material,has advantages of high initial luminescence intensity and long persistent time,which is promising in persistent luminescent material applications.At present,YAGG:Ce^(3+),Cr^(3+)powders exhibit good persistent performance,but their persistent performance of ceramics still needs to be further improved to meet the new requirements.In this work,(Y_(0.998)Ce_(0.002))_(3)(Al_(1-x)Cr_(x))_(2)Ga_(3)O_(12) ceramics with different Cr^(3+)doping concentrations were prepared by solid-state reaction,including air pre-sintering,hot isostatic pressing(HIP)post-treatment and air annealing,to investigate the effects of Cr^(3+)doping concentration on the microstructure,optical properties and persistent performance of the ceramics.The results showed that as the doping concentration of Cr^(3+)increased from 0.025%to 0.2%(in atom),no significant effect of Cr^(3+)concentration on the morphology of pre-sintered ceramics or HIP post-treatment ceramics was observed,but the in-line transmittance gradually increased while the persistent performance gradually decreased.Among them,YAGG:Ce^(3+),Cr^(3+)ceramics doped with 0.025%Cr^(3+)showed the strongest initial luminescence intensity exceeding 6055 mcd/m^(2) and a persistent time of 1030 min after air pre-sintering combined with HIP post-treatment and air annealing.By optimizing the Cr^(3+)doping concentration and the fabrication process,the persistent luminescence(PersL)performance of the YAGG:Ce^(3+),Cr^(3+)ceramics was obviously improved.
基金supported by the National Natural Science Foundation of China(No.52122407)the Science and Technology Innovation Program of Hunan Province(No.2022RC3048)。
文摘Nickel-rich cathode materials have received widespread attention due to their high energy density.However,the poor rate capability and inferior cycle stability seriously hinder their large-scale application.The traditional co-precipitation method for preparing them has a long process and easily arises agglomeration leading to inhomogeneous element distribution.Here,a novel precursor containing Li element was prepared by ultrafast spray pyrolysis(SP)in 3–5 s.Then the precursor was used to synthesize pristine LiNi_(0.9)Co_(0.05)Mn_(0.05)O_(2)(NCM90)and 1%Mg modified LiNi_(0.9)Co_(0.05)Mn_(0.05)O_(2)(NCM90-Mg1).This method gets rid of mixing Li/Mg source and the precursor prepared by common co-precipitation,thus could achieve homogeneous lithiation and Mg2+doping.The cell parameter c is expanded,and the cation disorder is reduced after Mg2+doping.Furthermore,the harmful H2-H3 phase transition in NCM90-Mg1 is also well suppressed.As a result,the obtained NCM90-Mg1 shows better electrochemical performance than NCM90.Within 2.8–4.3 V(25℃),the specific discharge capacity of NCM90-Mg1 at 5 C is as high as 169.1m Ah/g,and an outstanding capacity retention of 70.0%(10.0%higher than NCM90)can be obtained after400 cycles at 0.5 C.At 45℃,a capacity retention of 81.9%after 100 cycles at 1 C is recorded for NCM90-Mg1.Moreover,the NCM90-Mg1 also exhibits superior cycle stability when cycled at high cut-off voltage(4.5 V,25℃),possessing the capacity retention of 79.2%after 200 cycles at 1 C.Therefore,SP can be proposed as a powerful method for the preparation of multi-element materials for next-generation high energy density LIBs.
基金Supported by the Fundamental Research Funds for the Central Universities under Grant No 2012QNA03
文摘A novel method for preparing Ta-doped Ti02 via using Ta2 05 as the doping source is proposed. The preparation process combines the hydrothernlal fluorination of Ta2O5 and the subsequent formation of Ta-doped TiO2 sol. The results show that the doped sample annealed at 393 K generates an unstable intermediate NH4 TiOF3, which converts into anatase TiO2 with the increase of temperature. After annealing at ≥673K, the Ta-doped TiO2 nanocrystals with the grain size 〈20nm are obtained. Both the XRD and TG-DSC results confirm that Ta doping prevents the anatase-rutile crystal transition of TiO2. The band gap values of the doped samples, as obtained by UV-vis diffuse reflectance spectra, are smaller than that of pure anatase TiO2. The first-principle pseudopotential method calculations indicate that Ta5＋ lies in the TiO2 lattice at the interstitial position.
基金supported by Jiangsu Province Science and Technology Plan Special Fund(BZ2022053)National Natural Science Foundation of China(42476239)+1 种基金Natural Science Research Projects of Universities in Jiangsu Province(24KJD530004)the Dean/Opening Project of Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology(2021K008)。
文摘The catalytic direct synthesis of dimethyl carbonate(DMC)from CO_(2)and methanol is a crucial approach to utilizing CO_(2)and producing high-value chemicals.However,the high stability of the CO_(2)molecule imposes thermodynamic limitations on this reaction pathway,along with challenges related to insufficient catalyst activity and stability.Currently,solutions primarily focus on developing efficient catalyst.Herein,La-doped CeO_(2)nanoflower catalysts(La_(x)CeO_(2))were synthesized via hydrothermal method.Characterization reveals that La doping optimizes the pore structure and enriched oxygen vacancies,thereby enhancing catalytic performance.Notably,La_(0.1)CeO_(2)exhibits the largest pore size and highest oxygen vacancy content,achieving a remarkable DMC productivity of 9.42 mmol/g under 140℃,4 MPa of CO_(2),and 3 h of reactio n,surpassing pure CeO_(2)nano flowers.Based on experimental findings and in-situ diffuse infrared Fourier transform analysis,a plausible reaction pathway was proposed.This work underscores the potential of La_(x)CeO_(2)nano flowers as efficient catalysts for sustainable CO_(2)conversion to DMC.
基金supported by Zhejiang Provincial Key R&D Project(No.2021C01056)the Programme of Introducing Talents of Discipline to Universities(No.D17008).
文摘Reducing the cost of RuO_(2)/TiO_(2)catalysts is still one of the urgent challenges in catalytic HCl oxidation.In the present work,a Ce-doped TiO_(2)supported RuO_(2)catalyst with a low Ru loading was developed,showing a high activity in the catalytic oxidation of HCl to Cl_(2).The results on some extensive characterizations of both Ce-doped TiO_(2)carriers and their supported RuO_(2)catalysts show that the doping of Ce into TiO_(2)can effectively change the lattice parameters of TiO_(2)to improve the dispersion of the active RuO_(2)species on the carrier,which facilitates the production of surface Ru species to expose more active sites for boosting the catalytic performance even under some harsh reaction conditions.This work provides some scientific basis and technical support for chlorine recycling.
基金supported by the Natural Science Foundation of Henan Province,China(No.242300421226)the scientific research program of innovation platform in State Tobacco Monopoly Administration.
文摘Nitrogen dioxide(NO_(2))is a significant air pollutant with harmful effects on human health and the environment.Timely and accurate monitoring of NO_(2)concentrations is crucial for improving air quality and protecting public health.However,quantifying NO_(2)in the presence of other gases remains challenging.Herein,we integrate Ru onto the MoS_(2)surface to form Ru-S-Mo active sites,thereby tuning the electronic structure of MoS_(2)for enhanced NO_(2)detection.This sensor shows excellent sensitivity(29.7%at 100×10^(-6)NO_(2)and 25℃),with a linear response to NO_(2)ranging from 0.5 to 200×10^(-6),and a significantly reduced response/recovery time from 160/3636 s for pure MoS_(2)to 58/427 s for Ru@MoS_(2)at 100×10^(-6)NO_(2).Additionally,the sensor is highly selective for NO_(2),exhibiting a response 14 times higher than for other gases,and possesses strong anti-interference capabilities,accurately quantifying NO_(2)in the presence of varying H_(2)concentrations(10×10^(-6)-200×10^(-6))with a low RSD of 5.34%.A portable wireless NO_(2)monitoring system was successfully constructed using Ru@MoS_(2),enabling real-time gas leak detection(10×10^(-6)-50×10^(-6))with hazard warnings and maintaining a stable response to NO_(2)over a 4-week period.This work extends the gas sensing applications of MoS_(2)and provides a portable,wireless,and high-selectivity NO_(2)sensing method for environmental monitoring and safety assurance.
基金supported by the Postdoctoral Fellowship Program of CPSF(No.GZC20231545)the China Postdoctoral Science Foundation(Nos.2024T170557 and 2023M742224)+6 种基金the Shanghai Post-doctoral Excellence Program(No.2023440)the National Natural Science Foundation of China(Nos.52127801,52401101,and 22205012)the Shenzhen Basic Research Project(Nos.JCYJ20210324120001003,JCYJ20200109144608205)the Guangdong Basic and Applied Basic Research Foundation(Nos.2020A1515011301 and 2021A1515012246)the IER Foundation(Nos.IERF202201 andIERF202202),the City University of Hong Kong Donation Research(No.DON-RMG 9229021)the Hong Kong PDFS-RGC Postdoctoral Fellowship Scheme(Nos.PDFS2122–1S08 and CityU 9061014)the Hong Kong HMRF(Health and Medical Research Fund)(Nos.2120972 and CityU 9211320).
文摘The poor corrosion resistance of magnesium(Mg)and its alloys limits their application in various fields.Micro arc oxidation(MAO)coatings can improve the corrosion resistance,but the pore defects and low surface hardness make them susceptible to wear and accelerated corrosion during usage.In this study,a ZrO_(2)nanoparticles doped-MAO coating is prepared on the ZK61 Mg alloy by utilizing an MgF_(2)passivation layer to prevent ablation.The ZrO_(2)nanoparticles re-melt and precipitate due to local discharging,which produces evenly dispersed nanocrystals in the MAO coating.As a result,the hardness of the MAO coating with the appropriate ZrO_(2)concentration increases by over 10 times,while the wear rate decreases and corrosion resistance increases.With increasing ZrO_(2)concentrations,the corrosion potentials increase from−1.528 V of the bare ZK61 Mg alloy to−1.184 V,the corrosion current density decreases from 1.065×10^(–4)A cm^(–2)to 3.960×10^(–8)A cm^(–2),and the charge transfer resistance increases from 3.41×10^(2)Ωcm^(2)to 6.782×10^(5)Ωcm^(2).Immersion tests conducted in a salt solution for 28 d reveal minimal corrosion in contrast to severe corrosion on the untreated ZK61 Mg alloy.ZrO_(2)nanoparticles improve the corrosion resistance of MAO coatings by sealing pores and secondary strengthening of the corrosion product layer.
