Objectives:Philadelphia chromosome-positive B-cell acute lymphoblastic leukemia and Philadelphia-like B-cell acute lymphoblastic leukemia(Ph+/Ph-like ALL)constitute the majority of relapsed/refractory B-ALL(R/R B-ALL)...Objectives:Philadelphia chromosome-positive B-cell acute lymphoblastic leukemia and Philadelphia-like B-cell acute lymphoblastic leukemia(Ph+/Ph-like ALL)constitute the majority of relapsed/refractory B-ALL(R/R B-ALL)cases,highlighting an urgent need to discover new therapeutic targets.This study aims to elucidate the mechanisms underlying poor prognosis in Ph+/Ph-like ALL through transcriptome sequencing and functional cytological assays,with the goal of informing new clinical treatment strategies.Results:Transcriptomic analysis of Ph+/Ph-like ALL patients revealed that low expression of P2X Purinoceptor 1(P2RX1)was associated with unfavorable outcomes.Specifically,patients with poor prognosis and low P2RX1 expression exhibited downregulation of genes involved in energy and calcium metabolism pathways,along with upregulation of genes governing key cellular processes such as cell proliferation(e.g.,MYC),cell cycle progression(e.g.,CCND2),and apoptosis inhibition(e.g.,DASP6).Cellular experiments demonstrated that SUP-B15 cells overexpressing P2RX1 displayed elevated intracellular levels of ATP,calcium,and glucose,together with enhanced glycolytic capacity,compared to empty vector controls.Treatment of SUP-B15 cells with dexamethasone(Dex),Imatinib,or their combination significantly suppressed proliferation and promoted apoptosis,which was accompanied by increases in intracellular ATP,calcium,and glucose.Moreover,exogenous ATP administration(a P2RX1 agonist)enhanced apoptosis and inhibited proliferation in control cells.Conversely,treatment with NF449(a P2RX1 inhibitor)increased proliferation in both P2RX1-overexpressing and control SUP-B15 cells.Conclusion:Our findings indicate that P2RX1 may exert this function through modulating energy metabolism and calcium homeostasis,resulting in elevated intracellular calcium levels.Sustained elevation of calcium promotes apoptosis,whereas exogenous ATP activates P2RX1,enhances calcium influx,and attenuates the suppression of apoptosis associated with P2RX1 underexpression,ultimately correlating with improved treatment response.展开更多
Given the considerable global interest in the preparation of Ti and TiC,a novel reduction method for TiO_(2) in a CH_(4)-H_(2) atmosphere was proposed,and the reduction thermodynamic behavior,phase equilibrium,and ene...Given the considerable global interest in the preparation of Ti and TiC,a novel reduction method for TiO_(2) in a CH_(4)-H_(2) atmosphere was proposed,and the reduction thermodynamic behavior,phase equilibrium,and energy consumption of TiO_(2) during its reaction with a CH_(4)-H_(2) gas mixture were investigated.The results indicate that the reaction proceeds via a stepwise reduction pathway from TiO_(2) to Ti(C,O),with the Magnéli phase(TinO_(2n-1))and Ti_(3)O_(5) serving as intermediate phases.Notably,the reduction of TiO_(2) by H_(2) is more challenging than that by CH_(4),which may be attributed to the inhibitory effect of H_(2) on the surface carbon precipitation.For the complete carbonization of 1 mol TiO_(2),the total energy required at 1000,1100,and 1200℃is 1159,925,and 977 kJ/mol,respectively,which may be related to the shift of gas-phase equilibrium and the increase in side reactions at high temperatures.展开更多
Dry reforming of methane(DRM)has gained significant attention as a promising route to convert two major greenhouse gases(CO_(2) and CH4)to syngas.The development of efficient catalysts is critical for the engineering ...Dry reforming of methane(DRM)has gained significant attention as a promising route to convert two major greenhouse gases(CO_(2) and CH4)to syngas.The development of efficient catalysts is critical for the engineering applications.In this study,the Ce_(x)Zr_(1-x)O_(2)/ZSM-5 composites with different oxygen vacancy concentrations were synthesized by tuning the Ce/Zr ratio,followed by the deposition of metal Ni to island-like Ce_(x)Zr_(1-x)O_(2)on ZSM-5,forming a variety of Ni-Ce_(x)Zr_(1-x)O_(2)/ZSM-5 catalysts,which were applied for the DRM reaction under 750◦C.Combined with various characterizations,it was found that the oxygen vacancy concentration illustrated the volcanic tendency with the decreased Ce/Zr ratio,and the interaction between metal Ni and Ce_(x)Zr_(1-x)O_(2)exhibited a positive relationship with oxygen vacancy concentration.The enhanced between Ni and Ce_(x)Zr_(1-x)O_(2)interaction could improve the strength and amount of Ni-O-M(M=Ce/Zr)species,making the d-band centers of catalysts closer to the Fermi energy level,which was beneficial to the CH4 and CO_(2) activation,along with the improved capacity to resist sintering and coking.Especially,the C1Z3(Ni-Ce0.25Zr0.75O_(2)/ZSM-5)catalyst with the Ce/Zr ratio of 1/3 demonstrated the optimal catalytic performance with 91.9%CH4 and 93.8%CO_(2) conversions within 50 h,accompanied by the best structural and catalytic stability after 100 h.In-situ DRIFTS was employed to study the reaction path and mechanism,discovering that significant amounts of strengthened Ni-O-M species were conducive to activating adsorbed CH4 and CO_(2),and desorbing the linear CO species.展开更多
Lithium nickel oxide(Li_(2)NiO_(2)),as a sacrificial cathode prelithiation additive,has been used to compensate for the lithium loss for improving the lifespan of lithium-ion batteries(LIBs).However,high-cost Li_(2)Ni...Lithium nickel oxide(Li_(2)NiO_(2)),as a sacrificial cathode prelithiation additive,has been used to compensate for the lithium loss for improving the lifespan of lithium-ion batteries(LIBs).However,high-cost Li_(2)NiO_(2)suffers from inferior delithiation kinetics during the first cycle.Herein,we investigated the effects of the cost-effective copper substituted Li_(2)Ni_(1-x)Cu_(x)O_(2)(x=0,0.2,0.3,0.5,0.7)synthesized by a high-temperature solid-phase method on the structure,morphology,electrochemical performance of graphite‖LiFePO_(4)battery.The X-ray diffraction(XRD)refinement result demonstrated that Cu substitution strategy could be favorable for eliminating the NiO_(x)impurity phase and weakening Li-O bond.Analysis on density of states(DOS)indicates that Cu substitution is good for enhancing the electronic conductivity,as well as reducing the delithi-ation voltage polarization confirmed by electrochemical characterizations.Therefore,the optimal Li_(2)Ni_(0.7)Cu_(0.3)O_(2)delivered a high delithiation capacity of 437 mAh·g^(-1),around 8%above that of the pristine Li_(2)NiO_(2).Furthermore,a graphite‖LiFePO_(4)pouch cell with a nominal capacity of 3000 mAh demonstrated a notably improved reversible capacity,energy density and cycle life through introducing 2 wt%Li_(2)Ni_(0.7)Cu_(0.3)O_(2)additive,delivering a 6.2 mAh·g^(-1)higher initial discharge capacity and achieving around 5%improvement in capacity retentnion at 0.5P over 1000 cycles.Additionally,the post-mortem analyses testified that the Li_(2)Ni_(0.7)Cu_(0.3)O_(2)additive could suppress solid electrolyte interphase(SEI)decomposition and homogenize the Li distribution,which benefits to stabilizing interface between graphite and electrolyte,and alleviating dendritic Li plating.In conclusion,the Li_(2)Ni_(0.7)Cu_(0.3)O_(2)additive may offer advantages such as lower cost,lower delithiation voltage and higher prelithiation capacity compared with Li_(2)NiO_(2),making it a promising candidate of cathode prelithiation additive for next-generation LIBs.展开更多
The LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)(NCM)cathode materials have emerged as critical components in lithium-ion batteries due to their high energy and power densities.The co-precipitation method is widely used in laborator...The LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)(NCM)cathode materials have emerged as critical components in lithium-ion batteries due to their high energy and power densities.The co-precipitation method is widely used in laboratory and industry settings to optimize the crystallinity,grain morphology,particle size,and sphericity of precursor materials,directly affecting NCM battery performance.This review addresses the nucleation mechanism and the thermodynamic and kinetic reaction processes of co-precipitation.The comprehensive effects of key parameters on precursor physicochemical properties are also systematically interpreted.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
BACKGROUND Diabetes mellitus(DM)is linked to an earlier onset and heightened severity of urinary complications,particularly bladder dysfunction,which profoundly impacts patient quality of life.Overactive bladder(OAB)i...BACKGROUND Diabetes mellitus(DM)is linked to an earlier onset and heightened severity of urinary complications,particularly bladder dysfunction,which profoundly impacts patient quality of life.Overactive bladder(OAB)is a common storage disorder of the lower urinary tract and is characterized by urgency,frequency,and nocturia.Several factors contribute to bladder dysfunction in diabetic individuals,including changes in urothelial signaling,detrusor morphology,and central nervous system regulation.The transient receptor potential vanilloid type 1 channel,expressed by bladder urothelial cells,is upregulated in OAB and plays a crucial role in ATP release during bladder filling.This ATP release subsequently activates purinergic receptor P2X3,further exacerbating OAB symptoms.AIM To clarify the mechanism of Roux-en-Y gastric bypass(RYGB)metabolic surgery to improve OAB in type 2 DM(T2DM).METHODS The model of T2DM was induced by feeding a high-fat diet to mice for 16 weeks.After 16 weeks,sham operation and RYGB operation were performed.The related indexes of glucose metabolism were also detected to evaluate the therapeutic effect,and the recovery degree of bladder function and micturition behavior of mice was assessed by urodynamics and micturition spot analysis.RESULTS Compared with the normal mice in the sham group,T2DM mice had increased urine spot count,uncontrolled urination behavior,shortened urination interval,and reduced bladder capacity.Immunohistochemistry and immunofluorescence costaining showed that Transient receptor potential vanilloid type 1(TRPV1)and purinergic receptor P2X3 were both expressed in mouse bladder epithelial layer,and they had the same localization.In the bladder of T2DM mice,the mRNA and protein expression of TRPV1 and P2X3 were significantly increased.The ATP content in urine of T2DM mice was significantly higher than that of the sham group.After RYGB operation,the glucose metabolism index of the RYGB group was significantly improved compared with the OAB group.Comparing the results of urine spots,urodynamics,and histology,it was found that the function and morphological structure of the bladder in the RYGB group also recovered obviously.Compared with the OAB group,the expression of TRPV1 and P2X3 in the RYGB group was downregulated,and the level of inflammatory factors was significantly decreased.RYGB significantly decreased the content of ATP in urine and activated AMPK signaling.CONCLUSION RYGB downregulated the expression of TRPV1 by inhibiting inflammatory factors,thus inhibiting the enhancement of P2X3 by TRPV1.RYGB directly inhibited the activity of P2X3 by inhibiting ATP synthesis in the bladder epithelium to improve OAB.展开更多
To satisfy the demands of modern society for high-energy–density sulfide-based all-solid-state lithium batteries(ASSLBs),Ni-rich cathode materials have gained much attention for their high capacity and energy density...To satisfy the demands of modern society for high-energy–density sulfide-based all-solid-state lithium batteries(ASSLBs),Ni-rich cathode materials have gained much attention for their high capacity and energy density.However,their practical deployment is hindered by accelerated interface degradation and capacity decay originating from surface oxygen release and lattice oxygen activation during prolonged cycling.In this study,Ti_(x)NbB_((1−x))C_(2)was successfully coated on the surface of LiNi_(0.94)Co_(0.05)Mn_(0.01)O_(2).Density functional theory(DFT)calculations first elucidate a“point-to-point”anchoring mechanism where each surface oxygen atom coordinates with single species(Ti/Nb/B)offered by Ti_(x)NbB_((1−x))C_(2),which forms robust O–M bonds and sustain a stable interface structure.The electron energy loss spectroscopy(EELS)reveals the segregation of Ti/Nb toward subsurface layers during cycling,creating an optimized lattice oxygen coordination environment and suppressing oxygen activation.The dual oxygen stabilization mechanism dramatically improves the reversibility of phase transition and the structural stability of the Ni-rich cathode materials.Moreover,Ti_(x)NbB_((1−x))C_(2)as the protective layer decreases mechanical strain and suppresses the parasitic reactions.Consequently,the engineered cathode delivers 91%capacity retention after 1000 cycles at 0.3 C,suggesting excellent cycling stability.The research delivers a new design philosophy for the coating layer that can stabilize surface oxygen.Furthermore,the atomistic understanding of the structure–property relationship of the Ni-rich cathode materials provides valuable guidance for the future design of new cathode materials with superior structural stability in ASSLBs.展开更多
The reduction of N2 to NH_(3) is an important reaction for the industrial production of ammonia gas.Here,we theoretically study the thermal synthesis of ammonia catalyzed by Ru1@Mo_(2)CO_(x)single-atom catalyst(SAC),w...The reduction of N2 to NH_(3) is an important reaction for the industrial production of ammonia gas.Here,we theoretically study the thermal synthesis of ammonia catalyzed by Ru1@Mo_(2)CO_(x)single-atom catalyst(SAC),where Ru atoms are anchored on the oxygen vacancy of the defective Mo2COx.The results show that Ru1@Mo_(2)CO_(x)exhibits excellent stability,and can effectively adsorb and activate N2,owing to up to0.87|e|charge transfer from it to N2.The optimal pathway of N2-to-NH_(3) conversion is association pathway I,of which the rate-determining step is*NH_(2)→*NH_(3) with the barrier energy of 1.26 eV.Especially,the Mo_(2)CO_(x)center functions as an electron reservoir,donating electrons to the NxHy species,while the Ru single atom serves as a charge transfer pathway,thereby enhancing the reaction activity.This finding provides a theoretical foundation for the rational design of MXene-based SACs for thermal catalytic NH_(3) synthesis.展开更多
The mechanical,thermodynamic properties and electrical conductivities of L1_(2)-Al_(3)X(X=Zr,Sc,Er,Yb,Hf)structural phases in aluminum conductors were investigated through a first-principles study.The results demonstr...The mechanical,thermodynamic properties and electrical conductivities of L1_(2)-Al_(3)X(X=Zr,Sc,Er,Yb,Hf)structural phases in aluminum conductors were investigated through a first-principles study.The results demonstrate that all structural phases have good alloy-forming ability and structural stability,where Al_(3)Zr is the most superior.Al_(3)Zr,Al_(3)Hf and Al_(3)Sc have enhanced shear and deformation resistance in comparison to other phases.Within the temperature range of 200−600 K,Al_(3)Er and Al_(3)Yb possess the greatest thermodynamic stability,followed by Al_(3)Hf,Al_(3)Zr and Al_(3)Sc.Al_(3)Er and Al_(3)Yb have higher thermodynamic stability than Al_(3)Hf,Al_(3)Zr and Al_(3)Sc.All structural phases exhibit substantial metallic properties,indicating their good electrical conductivity.The electrical conductivities of Al_(3)Hf and Al_(3)Zr are higher than those of Al_(3)Er,Al_(3)Yb and Al_(3)Sc.The covalent bond properties in Al_(3)Sc,Al_(3)Er and Al_(3)Yb enhance the hardness,brittleness and thermodynamic stability of the structural phase.The thermodynamic stability of Al_(3)Sc is significantly reduced by ionic bonds.展开更多
Most studies have shown that oxygen vacancies on Ce_(x)Zr_(1-x)O_(2) solid solution are important for enhancing the catalytic oxidation performance.However,a handful of studies investigated the different roles of surf...Most studies have shown that oxygen vacancies on Ce_(x)Zr_(1-x)O_(2) solid solution are important for enhancing the catalytic oxidation performance.However,a handful of studies investigated the different roles of surface and subsurface oxygen vacancies on the performance and mechanisms of catalysts.Herein,a series of zirconium doping on CeO_(2) samples(CeO_(2),Ce_(0.95)Zr_(0.05)O_(2),and Ce_(0.8)5Zr_(0.15)O_(2))with various surface-to-subsurface oxygen vacancies ratios have been synthesized and applied in toluene catalytic oxidation.The obtained Ce_(0.95)Zr_(0.05)O_(2) exhibits an excellent catalytic performance with a 90%toluene conversion at 295℃,which is 68℃lower than that of CeO_(2).Additionally,the obtained Ce_(0.95)Zr_(0.05)O_(2)catalyst also exhibited good catalytic stability and water resistance.The XRD and HRTEM results show that Zr ions are incorporated into CeO_(2) lattice,forming Ce_(x)Zr_(1-x)O_(2) solid solution.Temperature-programmed experiments reveal that Ce_(0.95)Zr_(0.05)O_(2) shows excellent lowtemperature reducibility and abundant surface oxygen species.In-situ DRIFTS tests were used to probe the reaction mechanism,and the function of Zr doping in promoting the activation of oxygen was further determined.Density functional theory(DFT)calculations indicate that the vacancy formation energy and O_(2) adsorption energy are both lower on Ce_(0.95)Zr_(0.05)O_(2),confirming the reason for its superior catalytic performance.展开更多
The low-dose X-ray induced long afterglow near infrared(NIR)luminescence from Cr^(3+)doped Zn_(1-x)Cd_(x)Ga_(2)O_(4)spinel solid solutions was investigated.The structure analysis shows the good formation of Zn_(1-x)Cd...The low-dose X-ray induced long afterglow near infrared(NIR)luminescence from Cr^(3+)doped Zn_(1-x)Cd_(x)Ga_(2)O_(4)spinel solid solutions was investigated.The structure analysis shows the good formation of Zn_(1-x)Cd_(x)Ga_(2)O_(4)spinel solid solutions,which possesses a cubic spinel structure with Fd3m space group.The formation of Zn_(1-x)Cd_(x)Ga_(2)O_(4)spinel solid solutions induces the obvious increase of long afterglow near infrared luminescence excited by low-dose X-ray,When the content of doped Cd^(2+)reaches 0.1,the low-dose X-ray induced long afterglow NIR luminescence is the maximum.More importantly,only 5 s Xray irradiation can induce more than 6 h NIR afterglow emission,of which the afterglow luminescent intensity is still 5 times stronger than the background intensity after 6 h.The thermoluminescent results show that under the 5 s exposure of X-ray,the trap density of Zn_(0.9)Cd_(0.1)Ga_(2)O_(4):Cr^(3+)is much higher than that of ZnGa_(2)O_(4):Cr^(3+).The replacement of Cd^(2+)ions with large radius at Zn^(2+)sites causes the increase of de fects and dislocations,which results in the obvious increase of trap co ncentrations.And the addition of high-z number elements Cd^(2+)would enhance the X-ray absorption of the solid solutions,which thus can be easily excited by low-dose X-ray.Zn_(0.9)Cd_(0.1)Ga_(2)O_(4):1%Cr^(3+)solid solution is a potential candidate of lowdose X-ray induced long afterglow luminescent materials.展开更多
基金supported by Guangdong Province Basic and Applied Basic Research Fund Project(2023A1515220104)Open Fund of Key Laboratory of Hepatoaplenic Surgery,Ministry of Education(Award Number:GPKF202407).
文摘Objectives:Philadelphia chromosome-positive B-cell acute lymphoblastic leukemia and Philadelphia-like B-cell acute lymphoblastic leukemia(Ph+/Ph-like ALL)constitute the majority of relapsed/refractory B-ALL(R/R B-ALL)cases,highlighting an urgent need to discover new therapeutic targets.This study aims to elucidate the mechanisms underlying poor prognosis in Ph+/Ph-like ALL through transcriptome sequencing and functional cytological assays,with the goal of informing new clinical treatment strategies.Results:Transcriptomic analysis of Ph+/Ph-like ALL patients revealed that low expression of P2X Purinoceptor 1(P2RX1)was associated with unfavorable outcomes.Specifically,patients with poor prognosis and low P2RX1 expression exhibited downregulation of genes involved in energy and calcium metabolism pathways,along with upregulation of genes governing key cellular processes such as cell proliferation(e.g.,MYC),cell cycle progression(e.g.,CCND2),and apoptosis inhibition(e.g.,DASP6).Cellular experiments demonstrated that SUP-B15 cells overexpressing P2RX1 displayed elevated intracellular levels of ATP,calcium,and glucose,together with enhanced glycolytic capacity,compared to empty vector controls.Treatment of SUP-B15 cells with dexamethasone(Dex),Imatinib,or their combination significantly suppressed proliferation and promoted apoptosis,which was accompanied by increases in intracellular ATP,calcium,and glucose.Moreover,exogenous ATP administration(a P2RX1 agonist)enhanced apoptosis and inhibited proliferation in control cells.Conversely,treatment with NF449(a P2RX1 inhibitor)increased proliferation in both P2RX1-overexpressing and control SUP-B15 cells.Conclusion:Our findings indicate that P2RX1 may exert this function through modulating energy metabolism and calcium homeostasis,resulting in elevated intracellular calcium levels.Sustained elevation of calcium promotes apoptosis,whereas exogenous ATP activates P2RX1,enhances calcium influx,and attenuates the suppression of apoptosis associated with P2RX1 underexpression,ultimately correlating with improved treatment response.
文摘Given the considerable global interest in the preparation of Ti and TiC,a novel reduction method for TiO_(2) in a CH_(4)-H_(2) atmosphere was proposed,and the reduction thermodynamic behavior,phase equilibrium,and energy consumption of TiO_(2) during its reaction with a CH_(4)-H_(2) gas mixture were investigated.The results indicate that the reaction proceeds via a stepwise reduction pathway from TiO_(2) to Ti(C,O),with the Magnéli phase(TinO_(2n-1))and Ti_(3)O_(5) serving as intermediate phases.Notably,the reduction of TiO_(2) by H_(2) is more challenging than that by CH_(4),which may be attributed to the inhibitory effect of H_(2) on the surface carbon precipitation.For the complete carbonization of 1 mol TiO_(2),the total energy required at 1000,1100,and 1200℃is 1159,925,and 977 kJ/mol,respectively,which may be related to the shift of gas-phase equilibrium and the increase in side reactions at high temperatures.
基金the following financial supports:National Natural Science Foundation of China(22075225 and 22038011)Innovative Scientific Program of CNNC,State Key Laboratory of Clean and Efficient Coal Utilization,Taiyuan University of Technology(MJNYSKL202401,MJNYSKL202404).
文摘Dry reforming of methane(DRM)has gained significant attention as a promising route to convert two major greenhouse gases(CO_(2) and CH4)to syngas.The development of efficient catalysts is critical for the engineering applications.In this study,the Ce_(x)Zr_(1-x)O_(2)/ZSM-5 composites with different oxygen vacancy concentrations were synthesized by tuning the Ce/Zr ratio,followed by the deposition of metal Ni to island-like Ce_(x)Zr_(1-x)O_(2)on ZSM-5,forming a variety of Ni-Ce_(x)Zr_(1-x)O_(2)/ZSM-5 catalysts,which were applied for the DRM reaction under 750◦C.Combined with various characterizations,it was found that the oxygen vacancy concentration illustrated the volcanic tendency with the decreased Ce/Zr ratio,and the interaction between metal Ni and Ce_(x)Zr_(1-x)O_(2)exhibited a positive relationship with oxygen vacancy concentration.The enhanced between Ni and Ce_(x)Zr_(1-x)O_(2)interaction could improve the strength and amount of Ni-O-M(M=Ce/Zr)species,making the d-band centers of catalysts closer to the Fermi energy level,which was beneficial to the CH4 and CO_(2) activation,along with the improved capacity to resist sintering and coking.Especially,the C1Z3(Ni-Ce0.25Zr0.75O_(2)/ZSM-5)catalyst with the Ce/Zr ratio of 1/3 demonstrated the optimal catalytic performance with 91.9%CH4 and 93.8%CO_(2) conversions within 50 h,accompanied by the best structural and catalytic stability after 100 h.In-situ DRIFTS was employed to study the reaction path and mechanism,discovering that significant amounts of strengthened Ni-O-M species were conducive to activating adsorbed CH4 and CO_(2),and desorbing the linear CO species.
基金supported by the Significant Science and Technology Project in Xiamen(Future Industry Field)(Grant No.3502Z20231057).
文摘Lithium nickel oxide(Li_(2)NiO_(2)),as a sacrificial cathode prelithiation additive,has been used to compensate for the lithium loss for improving the lifespan of lithium-ion batteries(LIBs).However,high-cost Li_(2)NiO_(2)suffers from inferior delithiation kinetics during the first cycle.Herein,we investigated the effects of the cost-effective copper substituted Li_(2)Ni_(1-x)Cu_(x)O_(2)(x=0,0.2,0.3,0.5,0.7)synthesized by a high-temperature solid-phase method on the structure,morphology,electrochemical performance of graphite‖LiFePO_(4)battery.The X-ray diffraction(XRD)refinement result demonstrated that Cu substitution strategy could be favorable for eliminating the NiO_(x)impurity phase and weakening Li-O bond.Analysis on density of states(DOS)indicates that Cu substitution is good for enhancing the electronic conductivity,as well as reducing the delithi-ation voltage polarization confirmed by electrochemical characterizations.Therefore,the optimal Li_(2)Ni_(0.7)Cu_(0.3)O_(2)delivered a high delithiation capacity of 437 mAh·g^(-1),around 8%above that of the pristine Li_(2)NiO_(2).Furthermore,a graphite‖LiFePO_(4)pouch cell with a nominal capacity of 3000 mAh demonstrated a notably improved reversible capacity,energy density and cycle life through introducing 2 wt%Li_(2)Ni_(0.7)Cu_(0.3)O_(2)additive,delivering a 6.2 mAh·g^(-1)higher initial discharge capacity and achieving around 5%improvement in capacity retentnion at 0.5P over 1000 cycles.Additionally,the post-mortem analyses testified that the Li_(2)Ni_(0.7)Cu_(0.3)O_(2)additive could suppress solid electrolyte interphase(SEI)decomposition and homogenize the Li distribution,which benefits to stabilizing interface between graphite and electrolyte,and alleviating dendritic Li plating.In conclusion,the Li_(2)Ni_(0.7)Cu_(0.3)O_(2)additive may offer advantages such as lower cost,lower delithiation voltage and higher prelithiation capacity compared with Li_(2)NiO_(2),making it a promising candidate of cathode prelithiation additive for next-generation LIBs.
基金supported by the Major Science and Technology Project of Shenzhen’s Innovation and Entrepreneurship Program(Grant No.KJZD20231023100301004)Foshan Science and Technology Innovation Team Project(1920001004098)the Hydrometal urgy and Battery Materials Laboratory at PT.QMB New Energy Materials(Indonesia)under GEM Co.,Ltd.(China)as a company group。
文摘The LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)(NCM)cathode materials have emerged as critical components in lithium-ion batteries due to their high energy and power densities.The co-precipitation method is widely used in laboratory and industry settings to optimize the crystallinity,grain morphology,particle size,and sphericity of precursor materials,directly affecting NCM battery performance.This review addresses the nucleation mechanism and the thermodynamic and kinetic reaction processes of co-precipitation.The comprehensive effects of key parameters on precursor physicochemical properties are also systematically interpreted.
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.
基金Supported by National Natural Science Foundation of China,No.81860268 and No.82201000Ningxia Natural Science Foundation,No.2021AAC02025+3 种基金Ningxia Science and Technology Innovation Leading Talent Training ProjectNo.2020GKLRLX06 and No.2020GKLRLX11Ningxia Medical University Research Project,No.XJKF240315Ningxia Key Research and Development Project,No.2023BEG03021 and No.2021BEB04034.
文摘BACKGROUND Diabetes mellitus(DM)is linked to an earlier onset and heightened severity of urinary complications,particularly bladder dysfunction,which profoundly impacts patient quality of life.Overactive bladder(OAB)is a common storage disorder of the lower urinary tract and is characterized by urgency,frequency,and nocturia.Several factors contribute to bladder dysfunction in diabetic individuals,including changes in urothelial signaling,detrusor morphology,and central nervous system regulation.The transient receptor potential vanilloid type 1 channel,expressed by bladder urothelial cells,is upregulated in OAB and plays a crucial role in ATP release during bladder filling.This ATP release subsequently activates purinergic receptor P2X3,further exacerbating OAB symptoms.AIM To clarify the mechanism of Roux-en-Y gastric bypass(RYGB)metabolic surgery to improve OAB in type 2 DM(T2DM).METHODS The model of T2DM was induced by feeding a high-fat diet to mice for 16 weeks.After 16 weeks,sham operation and RYGB operation were performed.The related indexes of glucose metabolism were also detected to evaluate the therapeutic effect,and the recovery degree of bladder function and micturition behavior of mice was assessed by urodynamics and micturition spot analysis.RESULTS Compared with the normal mice in the sham group,T2DM mice had increased urine spot count,uncontrolled urination behavior,shortened urination interval,and reduced bladder capacity.Immunohistochemistry and immunofluorescence costaining showed that Transient receptor potential vanilloid type 1(TRPV1)and purinergic receptor P2X3 were both expressed in mouse bladder epithelial layer,and they had the same localization.In the bladder of T2DM mice,the mRNA and protein expression of TRPV1 and P2X3 were significantly increased.The ATP content in urine of T2DM mice was significantly higher than that of the sham group.After RYGB operation,the glucose metabolism index of the RYGB group was significantly improved compared with the OAB group.Comparing the results of urine spots,urodynamics,and histology,it was found that the function and morphological structure of the bladder in the RYGB group also recovered obviously.Compared with the OAB group,the expression of TRPV1 and P2X3 in the RYGB group was downregulated,and the level of inflammatory factors was significantly decreased.RYGB significantly decreased the content of ATP in urine and activated AMPK signaling.CONCLUSION RYGB downregulated the expression of TRPV1 by inhibiting inflammatory factors,thus inhibiting the enhancement of P2X3 by TRPV1.RYGB directly inhibited the activity of P2X3 by inhibiting ATP synthesis in the bladder epithelium to improve OAB.
基金supported by the National Natural Science Foundation of China(21203008,21975025,12274025,22372008,and 22179007)Hainan Province Science and Technology Special Fund(ZDYF2021SHFZ232 and ZDYF2023GXJS022)Hainan Province Postdoctoral Science Foundation(300333)。
文摘To satisfy the demands of modern society for high-energy–density sulfide-based all-solid-state lithium batteries(ASSLBs),Ni-rich cathode materials have gained much attention for their high capacity and energy density.However,their practical deployment is hindered by accelerated interface degradation and capacity decay originating from surface oxygen release and lattice oxygen activation during prolonged cycling.In this study,Ti_(x)NbB_((1−x))C_(2)was successfully coated on the surface of LiNi_(0.94)Co_(0.05)Mn_(0.01)O_(2).Density functional theory(DFT)calculations first elucidate a“point-to-point”anchoring mechanism where each surface oxygen atom coordinates with single species(Ti/Nb/B)offered by Ti_(x)NbB_((1−x))C_(2),which forms robust O–M bonds and sustain a stable interface structure.The electron energy loss spectroscopy(EELS)reveals the segregation of Ti/Nb toward subsurface layers during cycling,creating an optimized lattice oxygen coordination environment and suppressing oxygen activation.The dual oxygen stabilization mechanism dramatically improves the reversibility of phase transition and the structural stability of the Ni-rich cathode materials.Moreover,Ti_(x)NbB_((1−x))C_(2)as the protective layer decreases mechanical strain and suppresses the parasitic reactions.Consequently,the engineered cathode delivers 91%capacity retention after 1000 cycles at 0.3 C,suggesting excellent cycling stability.The research delivers a new design philosophy for the coating layer that can stabilize surface oxygen.Furthermore,the atomistic understanding of the structure–property relationship of the Ni-rich cathode materials provides valuable guidance for the future design of new cathode materials with superior structural stability in ASSLBs.
基金the financial support from National Natural Science Foundation of China(22479032,22363001 and 22250710677)the NSFC Center for Single-Atom Catalysis(22388102)+2 种基金the National Key R&D Project(2022YFA1503900)the Natural Science Special Foundation of Guizhou University(No.202140)Guizhou Provincial Key Laboratory Platform Project(ZSYS[2025]008).
文摘The reduction of N2 to NH_(3) is an important reaction for the industrial production of ammonia gas.Here,we theoretically study the thermal synthesis of ammonia catalyzed by Ru1@Mo_(2)CO_(x)single-atom catalyst(SAC),where Ru atoms are anchored on the oxygen vacancy of the defective Mo2COx.The results show that Ru1@Mo_(2)CO_(x)exhibits excellent stability,and can effectively adsorb and activate N2,owing to up to0.87|e|charge transfer from it to N2.The optimal pathway of N2-to-NH_(3) conversion is association pathway I,of which the rate-determining step is*NH_(2)→*NH_(3) with the barrier energy of 1.26 eV.Especially,the Mo_(2)CO_(x)center functions as an electron reservoir,donating electrons to the NxHy species,while the Ru single atom serves as a charge transfer pathway,thereby enhancing the reaction activity.This finding provides a theoretical foundation for the rational design of MXene-based SACs for thermal catalytic NH_(3) synthesis.
基金National Natural Science Foundation of China (No. 52274403)。
文摘The mechanical,thermodynamic properties and electrical conductivities of L1_(2)-Al_(3)X(X=Zr,Sc,Er,Yb,Hf)structural phases in aluminum conductors were investigated through a first-principles study.The results demonstrate that all structural phases have good alloy-forming ability and structural stability,where Al_(3)Zr is the most superior.Al_(3)Zr,Al_(3)Hf and Al_(3)Sc have enhanced shear and deformation resistance in comparison to other phases.Within the temperature range of 200−600 K,Al_(3)Er and Al_(3)Yb possess the greatest thermodynamic stability,followed by Al_(3)Hf,Al_(3)Zr and Al_(3)Sc.Al_(3)Er and Al_(3)Yb have higher thermodynamic stability than Al_(3)Hf,Al_(3)Zr and Al_(3)Sc.All structural phases exhibit substantial metallic properties,indicating their good electrical conductivity.The electrical conductivities of Al_(3)Hf and Al_(3)Zr are higher than those of Al_(3)Er,Al_(3)Yb and Al_(3)Sc.The covalent bond properties in Al_(3)Sc,Al_(3)Er and Al_(3)Yb enhance the hardness,brittleness and thermodynamic stability of the structural phase.The thermodynamic stability of Al_(3)Sc is significantly reduced by ionic bonds.
基金supported by the National Natural Science Foundation(No.51678291)the Basic Science(Natural Science)Research in Higher Education in Jiangsu Province(No.23KJA610003)the High-level Scientific Research Foundation for the introduction of talent in Nanjing Institute of Technology(No.YKJ201999)。
文摘Most studies have shown that oxygen vacancies on Ce_(x)Zr_(1-x)O_(2) solid solution are important for enhancing the catalytic oxidation performance.However,a handful of studies investigated the different roles of surface and subsurface oxygen vacancies on the performance and mechanisms of catalysts.Herein,a series of zirconium doping on CeO_(2) samples(CeO_(2),Ce_(0.95)Zr_(0.05)O_(2),and Ce_(0.8)5Zr_(0.15)O_(2))with various surface-to-subsurface oxygen vacancies ratios have been synthesized and applied in toluene catalytic oxidation.The obtained Ce_(0.95)Zr_(0.05)O_(2) exhibits an excellent catalytic performance with a 90%toluene conversion at 295℃,which is 68℃lower than that of CeO_(2).Additionally,the obtained Ce_(0.95)Zr_(0.05)O_(2)catalyst also exhibited good catalytic stability and water resistance.The XRD and HRTEM results show that Zr ions are incorporated into CeO_(2) lattice,forming Ce_(x)Zr_(1-x)O_(2) solid solution.Temperature-programmed experiments reveal that Ce_(0.95)Zr_(0.05)O_(2) shows excellent lowtemperature reducibility and abundant surface oxygen species.In-situ DRIFTS tests were used to probe the reaction mechanism,and the function of Zr doping in promoting the activation of oxygen was further determined.Density functional theory(DFT)calculations indicate that the vacancy formation energy and O_(2) adsorption energy are both lower on Ce_(0.95)Zr_(0.05)O_(2),confirming the reason for its superior catalytic performance.
基金Project supported by the State Key Research Project of Shandong Natural Science Foundation(ZR2020KB019)the fund of"Two-Hundred Talent"Plan of Yantai City+1 种基金the National Natural Science Foundation of China(11974013)the Natural Science Foundation of Fujian Province(2022J011270)。
文摘The low-dose X-ray induced long afterglow near infrared(NIR)luminescence from Cr^(3+)doped Zn_(1-x)Cd_(x)Ga_(2)O_(4)spinel solid solutions was investigated.The structure analysis shows the good formation of Zn_(1-x)Cd_(x)Ga_(2)O_(4)spinel solid solutions,which possesses a cubic spinel structure with Fd3m space group.The formation of Zn_(1-x)Cd_(x)Ga_(2)O_(4)spinel solid solutions induces the obvious increase of long afterglow near infrared luminescence excited by low-dose X-ray,When the content of doped Cd^(2+)reaches 0.1,the low-dose X-ray induced long afterglow NIR luminescence is the maximum.More importantly,only 5 s Xray irradiation can induce more than 6 h NIR afterglow emission,of which the afterglow luminescent intensity is still 5 times stronger than the background intensity after 6 h.The thermoluminescent results show that under the 5 s exposure of X-ray,the trap density of Zn_(0.9)Cd_(0.1)Ga_(2)O_(4):Cr^(3+)is much higher than that of ZnGa_(2)O_(4):Cr^(3+).The replacement of Cd^(2+)ions with large radius at Zn^(2+)sites causes the increase of de fects and dislocations,which results in the obvious increase of trap co ncentrations.And the addition of high-z number elements Cd^(2+)would enhance the X-ray absorption of the solid solutions,which thus can be easily excited by low-dose X-ray.Zn_(0.9)Cd_(0.1)Ga_(2)O_(4):1%Cr^(3+)solid solution is a potential candidate of lowdose X-ray induced long afterglow luminescent materials.
