Herein,antibacterial silver‑doped fluorescent carbon dots(Ag‑CDs)were synthesized through a stepwise hydrothermal method,with polyethyleneimine(PEI),citric acid(CA),and silver nitrate(AgNO3)serving as precursors.The a...Herein,antibacterial silver‑doped fluorescent carbon dots(Ag‑CDs)were synthesized through a stepwise hydrothermal method,with polyethyleneimine(PEI),citric acid(CA),and silver nitrate(AgNO3)serving as precursors.The applicability and antimicrobial efficacy of these nanomaterials were systematically investigated for metal ion sensing.Experimental evidence demonstrated that the Ag‑CDs exhibited a pronounced fluorescence quenching response toward ferric ions(Fe^(3+)),enabling their quantitative determination via a linear concentration‑dependent relationship.These Ag‑CDs exhibited significant inhibitory effects on biofilm growth and disruption for both Escherichia coli and Staphylococcus aureus.Mechanism investigations indicate that Ag‑CDs induced the death of Escherichia coli and Pseudomonas aeruginosa by disrupting their bacterial morphology and structure,triggering the generation of intracellular reactive oxygen species(ROS),and impairing their antioxidant defense system.展开更多
Developing catalysts with excellent stability while significantly reducing the overpotential of the oxygen evolution reaction(OER) is crucial for advancing overall water splitting(OWS) systems.In this study,we synthes...Developing catalysts with excellent stability while significantly reducing the overpotential of the oxygen evolution reaction(OER) is crucial for advancing overall water splitting(OWS) systems.In this study,we synthesized the electrode material Ce-NiCo-LDHs@SnO_(2)/NF through a two-step hydrothermal reaction,where Ce-doped NiCo-LDHs are grown on nickel foam modified by a SnO_(2) layer.Ce doping adjusts the internal electronic distribution of Ni Co-LDHs,while the introduction of the SnO_(2) layer enhances electron transfer capability.Together,these factors contribute to the reduction of the OER energy barrier and experimental evidence confirms that the reaction proceeds via the lattice oxygen evolution mechanism(LOM).Consequently,Ce-NiCo-LDHs@SnO_(2)/NF exhibits high level electrochemical performance in OER,requiring only 234 m V overpotential to achieve a current density of 10 m A/cm^(2),with a Tafel slope of just 27.39 m V/dec.When paired with Pt/C/NF,an external potential of only 1.54 V is needed to drive OWS to attain a current density amounting to 10 m A/cm^(2).Furthermore,the catalyst demonstrates stability for 100 h during the OWS stability test.This study underscores the feasibility of enhancing the OER performance through Ce doping and the introduction of a conductive SnO_(2) layer.展开更多
β-Ga_(2)O_(3)is a promising candidate for solarblind ultraviolet photodetection owing to its suitable bandgap of approximately 4.9 eV,excellent photoresponse characteristics,and high stability.However,the lack of a s...β-Ga_(2)O_(3)is a promising candidate for solarblind ultraviolet photodetection owing to its suitable bandgap of approximately 4.9 eV,excellent photoresponse characteristics,and high stability.However,the lack of a sufficient driving force within the material leads to extensive bulk charge recombination,limiting its photocurrent and thus posing significant challenges in designing high-performance Ga_(2)O_(3)-based photodetection.In this study,we propose a gradient doping strategy to achieve a Sn-doping concentration gradient along theβ-Ga_(2)O_(3)film thickness.By combining sol-gel synthesis with rapid thermal annealing,a spatially graded band structure with a full-space built-in electric field is constructed,which increases the width of band bending over a large region and is crucial for significantly enhancing carrier separation and transport in the bulk.The resulting gradient Sn-dopedβ-Ga_(2)O_(3)enables exceptional photoelectric performance without an external bias under 254 nm irradiation,including a superior responsivity of 66.88 mA W^(-1),a high detectivity of 8.12×10^(11)Jones,and a fast rise/decay time of 79/65 ms,outstanding most existing similar reported photoelectrochemical(PEC)type optoelectronic devices.Additionally,the device exhibits excellent long-term stability and enables high-resolution underwater ultraviolet imaging.This study demonstrates that the gradient doping strategy provides a feasible approach for enhancing the PEC performance ofβ-Ga_(2)O_(3)photoelectrodes.展开更多
An in-built N^(+)pocket electrically doped tunnel field-effect transistor(ED-TFET)-based biosensor has been reported for the first time.The proposed device begins with a PN junction structure with a control gate(CG)an...An in-built N^(+)pocket electrically doped tunnel field-effect transistor(ED-TFET)-based biosensor has been reported for the first time.The proposed device begins with a PN junction structure with a control gate(CG)and two polarity gates(PG1 and PG2).Utilizing the polarity bias concept,a narrow N^(+)pocket is formed between the source and channel without the need for additional doping steps,achieved through biasing PG1 and PG2 at-1.2 V and 1.2 V,respectively.This method not only addresses issues related to doping control but also eliminates constraints associated with thermal budgets and simplifies the fabrication process compared to traditional TFETs.To facilitate biomolecule sensing within the device,a nanogap cavity is formed in the gate dielectric by selectively etching a section of the polarity gate dielectric layer toward the source side.The investigation into the presence of neutral and charged molecules within the cavities has been conducted by examining variations in the electrical properties of the proposed biosensor.Key characteristics assessed include drain current,energy band,and electric field distribution.The performance of the biosensor is measured using various metrics such as drain current(I_(DS)),subthreshold swing(SS),threshold voltage(V_(TH)),drain current ratio(I_(ON)/I_(OFF)).The proposed in-built N^(+)pocket ED-TFET-based biosensor reaches a peak sensitivity of 1.08×10~(13)for a neutral biomolecule in a completely filled nanogap with a dielectric constant of 12.Additionally,the effects of cavity geometry and different fill factors(FFs)on sensitivity are studied.展开更多
The outstanding performance of O3-type NaNi_(1/3)Fe_(1/3)Mn_(1/3)O_(2)(NFM111)at both high and low temperatures coupled with its impressive specific capacity makes it an excellent cathode material for sodium-ion batte...The outstanding performance of O3-type NaNi_(1/3)Fe_(1/3)Mn_(1/3)O_(2)(NFM111)at both high and low temperatures coupled with its impressive specific capacity makes it an excellent cathode material for sodium-ion batteries.However,its poor cycling,owing to highpressure phase transitions,is one of its disadvantages.In this study,Cu/Ti was introduced into NFM111 cathode material using a solidphase method.Through both theoretically and experimentally,this study found that Cu doping provides a higher redox potential in NFM111,improving its reversible capacity and charge compensation process.The introduction of Ti would enhance the cycling stability of the material,smooth its charge and discharge curves,and suppress its high-voltage phase transitions.Accordingly,the NaNi_(0.27)Fe_(0.28)Mn_(0.33)Cu_(0.05)Ti_(0.06)O_(2)sample used in the study exhibited a remarkable rate performance of 142.97 mAh·g^(-1)at 0.1 C(2.0-4.2 V)and an excellent capacity retention of 72.81%after 300 cycles at 1C(1C=150 mA·g^(-1)).展开更多
Precise heterometal doping or substitution of specific metal sites in isostructural metal clusters remains a formidable synthetic challenge,despite its transformative potential for modulating excited-state characteris...Precise heterometal doping or substitution of specific metal sites in isostructural metal clusters remains a formidable synthetic challenge,despite its transformative potential for modulating excited-state characteristics and customizing optical properties.In this work,we achieved the precise synthesis of isostructural alloy clusters R/S-Ag_(3)Cu([Ag_(3)Cu(tppm)(R/S-IPTT)]ClO_(4),R/S-IPTT=R/S-4-isopropylthiazolidine-2-thiolate,tppm=tris(diphenylphosphino)methane)in high yield(89%-91%)through selective doping of a Cu(Ⅰ)atom into chiral homometallic cluster enantiomers R/S-Ag_(4)([Ag_(4)(tppm)(R/S-IPTT)]ClO_(4)).In stark contrast to R/S-Ag_(4)(Φ_(em)<0.5%)that displays weak circularly polarized luminescence(CPL)with phosphorescence characteristic,R/S-Ag_(3)Cu(Φ_(em)≈70%)demonstrates strong CPL properties featured with thermally activated delay fluorescence(TADF)at ambient temperature.The selective substitution of the apical Ag(Ⅰ)atom in Ag_(4)triangular pyramid with a Cu(Ⅰ)atom not only gives rise to beyond 100-fold boosting of photoluminescence quantum yield(PLQY),but also leads to more pronounced optically chiral activity of alloy clusters in excited states in view of the larger photoluminescence dissymmetry factors(g_(PL))of R/S-Ag_(3)Cu(-3.5×10^(-3)/3.4×10^(-3))than that of R/S-Ag_(4)(-2.7×10^(-3)/2.6×10^(-3)).Furthermore,compared with chiral homometallic clusters R/S-Cu_(4)([Cu_(4)(tppm)(R/S-IPTT)]ClO_(4))with the same TADF characteristic at ambient temperature,R/S-Ag_(3)Cu manifests 1.7-fold PLQY and 6-fold g_(PL)due to faster reverse intersystem crossing(RISC)and more effective coupling of electric and magnetic transition moments in alloy clusters.This work not only presents a typical example of selective heterometal doping to modulate excited-state properties of isostructural metal clusters,but also gets deeper insight into the doping chemistry of dissimilar metals at the molecular level.展开更多
O3-types layered cathode materials in sodium-ion batteries(SIBs)suffer from the obvious lattice distortion induced by the complex phase transitions during Na^(+)intercalation/deintercalation process,leading to severe ...O3-types layered cathode materials in sodium-ion batteries(SIBs)suffer from the obvious lattice distortion induced by the complex phase transitions during Na^(+)intercalation/deintercalation process,leading to severe structural collapse and performance degradation.Herein,a series of high valence tantalum(Ta^(5+))doped Na(Ni_(0.4)Fe_(0.2)Mn_(0.4))_(1−x)Ta_(x)O_(2)(x=0/0.0025/0.005/0.01)secondary spherical particles are firstly developed,where Ta^(5+)doping enables the refined primary grain with a tightly stacked rod-like morphology.Comprehensive structural analysis via Neutron powder diffraction(NPD)and Synchrotron radiation X-ray diffraction(SXRD)reveals an expanded NaO_(2)slab and a reduction in Na site vacancy.The potential charge compensation mechanism is further illustrated by X-ray absorption spectroscopy(XAS)and X-ray photoelectron spectroscopy(XPS),unveiling a partial reduction from Ni^(3+)to Ni^(2+)with Ta^(5+)doping.In situ X-ray diffraction(in situ XRD)suggests that the decorated sample undergoes a volume change as low as 0.8%,in contrast with the pristine one(1.5%).Thus,the optimized sample with x=0.005 retains an enhanced capacity retention up to 70.4%at 1 C after 300 cycles in half-cell and delivers a high energy density of 251 Wh kg^(-1)(0.1 C)and with a good capacity retention of 81.0%at 1 C after 200 cycles in full-cell.Our findings provide new insights into the mechanism of high valence Ta^(5+)doping in stabilizing layered oxides cathode materials for SIBs.展开更多
In recent years,the research on superconductivity in one-dimensional(1D)materials has been attracting increasing attention due to its potential applications in low-dimensional nanodevices.However,the critical temperat...In recent years,the research on superconductivity in one-dimensional(1D)materials has been attracting increasing attention due to its potential applications in low-dimensional nanodevices.However,the critical temperature(T_(c))of 1D superconductors is low.In this work,we theoretically investigate the possible high T_(c) superconductivity of(5,5)carbon nanotube(CNT).The pristine(5,5)CNT is a Dirac semimetal and can be modulated into a semiconductor by full hydrogenation.Interestingly,by further hole doping,it can be regulated into a metallic state with the sp^(3)-hybridized σ electrons metalized,and a giant Kohn anomaly appears in the optical phonons.The two factors together enhance the electron–phonon coupling,and lead to high-T_(c) superconductivity.When the hole doping concentration of hydrogenated-(5,5)CNT is 2.5 hole/cell,the calculated T_(c) is 82.3 K,exceeding the boiling point of liquid nitrogen.Therefore,the predicted hole-doped hydrogenated-(5,5)CNT provides a new platform for 1D high-T_(c) superconductivity and may have potential applications in 1D nanodevices.展开更多
Photocatalytic nitrogen fixation has emerged as a sustainable alternative for ammonia synthesis,playing a crucial role in alleviating energy shortages and environmental pollution.In this study,PbBiO_(2)Br was applied ...Photocatalytic nitrogen fixation has emerged as a sustainable alternative for ammonia synthesis,playing a crucial role in alleviating energy shortages and environmental pollution.In this study,PbBiO_(2)Br was applied to photocatalytic nitrogen fixation for the first time,and its photocatalytic performance was effectively enhanced through Cu doping.The catalyst was synthesized via a simple reduction method,and its morphology,structure,and physicochemical properties were systematically investigated using various characterization techniques and density functional theory calculations.The results revealed that the incorporation of Cu2+partially replaced Pb2+,inducing lattice distortion in PbBiO_(2)Br,promoting the formation of oxygen vacancies,and modifying its electronic band structure.Specifically,Cu doping led to a slight bandgap narrowing,a reduction in work function,and a significant upward shift in the conduction band position.These changes enhanced light absorption,facilitated charge carrier migration and separation,and improved the reduction ability of photogenerated electrons.Moreover,Cu doping promoted N_(2)adsorption and activation.Consequently,the photocatalytic nitrogen fixation performance of Cu-doped PbBiO_(2)Br was significantly enhanced,achieving an optimal nitrogen fixation rate of 293μmol L^(−1)g^(−1)h^(−1),which is 3.6 times higher than that of pristine PbBiO_(2)Br.Additionally,Cu–PbBiO_(2)Br also showed good activity in the photocatalytic degradation of RhB,with a degradation rate 4.6 times higher than that of PbBiO_(2)Br.This work offers new insights into the application of PbBiO_(2)Br in photocatalytic nitrogen fixation and offers valuable guidance for the development of highly efficient nitrogen fixation materials in the future.展开更多
Mn^(2+)-doped CsPbCl_(3)(Mn^(2+):CsPbCl_(3)) nanocrystals(NCs) have attracted considerable attention due to their unique strong and broad orange-red emission band,presenting promising applications in the field of phot...Mn^(2+)-doped CsPbCl_(3)(Mn^(2+):CsPbCl_(3)) nanocrystals(NCs) have attracted considerable attention due to their unique strong and broad orange-red emission band,presenting promising applications in the field of photoelectric devices.However,pristine Mn^(2+):CsPbCl_(3)NCs commonly suffer from low photoluminescence quantum yield(PL QY) and stability issues.Herein,we introduced europium ions(Eu^(3+))into Mn^(2+):CsPbCl_(3)NCs via the thermal injection synthesis method to obtain high performance Eu^(3+)and Mn^(2+)codoped CsPbCl_(3)(Eu^(3+)/Mn^(2+):CsPbCl_(3)) NCs.The maximum PL QY of the resulting Eu^(3+)/Mn^(2+):CsPbCl_(3)NCs reaches up to 90.92%.It is found that the doping of Eu^(3+)ions significantly reduces the non-radiative recombination caused by high defect states,and improves the energy transfer efficiency from exciton to Mn^(2+),thereby boosting the PL performance.Moreover,doping Eu^(3+)ions notably improves the UV-light and water stability of Mn^(2+):CsPbCl_(3)NCs.We further demonstrate the application versatility of Eu^(3+)/Mn^(2+):CsPbCl_(3)NCs in white light emitting diodes(WLEDs) and optical anticounterfeiting applications.This work provides a valuable perspective for the attainment of high performance Mn^(2+):CsPbCl_(3)NCs and lays a foundation for the codoping of other lanthanide ions to adjust the luminescence properties of Mn^(2+):CsPbCl_(3)NCs.展开更多
文摘Herein,antibacterial silver‑doped fluorescent carbon dots(Ag‑CDs)were synthesized through a stepwise hydrothermal method,with polyethyleneimine(PEI),citric acid(CA),and silver nitrate(AgNO3)serving as precursors.The applicability and antimicrobial efficacy of these nanomaterials were systematically investigated for metal ion sensing.Experimental evidence demonstrated that the Ag‑CDs exhibited a pronounced fluorescence quenching response toward ferric ions(Fe^(3+)),enabling their quantitative determination via a linear concentration‑dependent relationship.These Ag‑CDs exhibited significant inhibitory effects on biofilm growth and disruption for both Escherichia coli and Staphylococcus aureus.Mechanism investigations indicate that Ag‑CDs induced the death of Escherichia coli and Pseudomonas aeruginosa by disrupting their bacterial morphology and structure,triggering the generation of intracellular reactive oxygen species(ROS),and impairing their antioxidant defense system.
基金supported by the National Natural Science Foundation of China (No.52274304)。
文摘Developing catalysts with excellent stability while significantly reducing the overpotential of the oxygen evolution reaction(OER) is crucial for advancing overall water splitting(OWS) systems.In this study,we synthesized the electrode material Ce-NiCo-LDHs@SnO_(2)/NF through a two-step hydrothermal reaction,where Ce-doped NiCo-LDHs are grown on nickel foam modified by a SnO_(2) layer.Ce doping adjusts the internal electronic distribution of Ni Co-LDHs,while the introduction of the SnO_(2) layer enhances electron transfer capability.Together,these factors contribute to the reduction of the OER energy barrier and experimental evidence confirms that the reaction proceeds via the lattice oxygen evolution mechanism(LOM).Consequently,Ce-NiCo-LDHs@SnO_(2)/NF exhibits high level electrochemical performance in OER,requiring only 234 m V overpotential to achieve a current density of 10 m A/cm^(2),with a Tafel slope of just 27.39 m V/dec.When paired with Pt/C/NF,an external potential of only 1.54 V is needed to drive OWS to attain a current density amounting to 10 m A/cm^(2).Furthermore,the catalyst demonstrates stability for 100 h during the OWS stability test.This study underscores the feasibility of enhancing the OER performance through Ce doping and the introduction of a conductive SnO_(2) layer.
基金supported by the National Natural Science Foundation of China(12304102,62574029)Natural Science Foundation of Chongqing(CSTB2023NSCQ-MSX0479)+1 种基金Science and Technology Research Project of Chongqing Education Committee(KJQN202400558)Doctoral Scientific Research Fund of Chongqing Normal University(23XLB029)。
文摘β-Ga_(2)O_(3)is a promising candidate for solarblind ultraviolet photodetection owing to its suitable bandgap of approximately 4.9 eV,excellent photoresponse characteristics,and high stability.However,the lack of a sufficient driving force within the material leads to extensive bulk charge recombination,limiting its photocurrent and thus posing significant challenges in designing high-performance Ga_(2)O_(3)-based photodetection.In this study,we propose a gradient doping strategy to achieve a Sn-doping concentration gradient along theβ-Ga_(2)O_(3)film thickness.By combining sol-gel synthesis with rapid thermal annealing,a spatially graded band structure with a full-space built-in electric field is constructed,which increases the width of band bending over a large region and is crucial for significantly enhancing carrier separation and transport in the bulk.The resulting gradient Sn-dopedβ-Ga_(2)O_(3)enables exceptional photoelectric performance without an external bias under 254 nm irradiation,including a superior responsivity of 66.88 mA W^(-1),a high detectivity of 8.12×10^(11)Jones,and a fast rise/decay time of 79/65 ms,outstanding most existing similar reported photoelectrochemical(PEC)type optoelectronic devices.Additionally,the device exhibits excellent long-term stability and enables high-resolution underwater ultraviolet imaging.This study demonstrates that the gradient doping strategy provides a feasible approach for enhancing the PEC performance ofβ-Ga_(2)O_(3)photoelectrodes.
基金Project supported by the Ministry of Education’s Supply and Demand Matching Employment and Education Project(Grant No.2024110776329)。
文摘An in-built N^(+)pocket electrically doped tunnel field-effect transistor(ED-TFET)-based biosensor has been reported for the first time.The proposed device begins with a PN junction structure with a control gate(CG)and two polarity gates(PG1 and PG2).Utilizing the polarity bias concept,a narrow N^(+)pocket is formed between the source and channel without the need for additional doping steps,achieved through biasing PG1 and PG2 at-1.2 V and 1.2 V,respectively.This method not only addresses issues related to doping control but also eliminates constraints associated with thermal budgets and simplifies the fabrication process compared to traditional TFETs.To facilitate biomolecule sensing within the device,a nanogap cavity is formed in the gate dielectric by selectively etching a section of the polarity gate dielectric layer toward the source side.The investigation into the presence of neutral and charged molecules within the cavities has been conducted by examining variations in the electrical properties of the proposed biosensor.Key characteristics assessed include drain current,energy band,and electric field distribution.The performance of the biosensor is measured using various metrics such as drain current(I_(DS)),subthreshold swing(SS),threshold voltage(V_(TH)),drain current ratio(I_(ON)/I_(OFF)).The proposed in-built N^(+)pocket ED-TFET-based biosensor reaches a peak sensitivity of 1.08×10~(13)for a neutral biomolecule in a completely filled nanogap with a dielectric constant of 12.Additionally,the effects of cavity geometry and different fill factors(FFs)on sensitivity are studied.
基金supported by the Low-Cost Long-Life Batteries program,China(No.WL-24-08-01)the National Natural Science Foundation of China(No.22279007)。
文摘The outstanding performance of O3-type NaNi_(1/3)Fe_(1/3)Mn_(1/3)O_(2)(NFM111)at both high and low temperatures coupled with its impressive specific capacity makes it an excellent cathode material for sodium-ion batteries.However,its poor cycling,owing to highpressure phase transitions,is one of its disadvantages.In this study,Cu/Ti was introduced into NFM111 cathode material using a solidphase method.Through both theoretically and experimentally,this study found that Cu doping provides a higher redox potential in NFM111,improving its reversible capacity and charge compensation process.The introduction of Ti would enhance the cycling stability of the material,smooth its charge and discharge curves,and suppress its high-voltage phase transitions.Accordingly,the NaNi_(0.27)Fe_(0.28)Mn_(0.33)Cu_(0.05)Ti_(0.06)O_(2)sample used in the study exhibited a remarkable rate performance of 142.97 mAh·g^(-1)at 0.1 C(2.0-4.2 V)and an excellent capacity retention of 72.81%after 300 cycles at 1C(1C=150 mA·g^(-1)).
基金supported by the National Natural Science Foundation of China(92061202,21531008,22175181)the Fujian Province Science and Technology Project Program(2022H0041)the Self-deployment Project Research Program of Haixi Institute,Chinese Academy of Sciences(CXZX-2022-GH11)。
文摘Precise heterometal doping or substitution of specific metal sites in isostructural metal clusters remains a formidable synthetic challenge,despite its transformative potential for modulating excited-state characteristics and customizing optical properties.In this work,we achieved the precise synthesis of isostructural alloy clusters R/S-Ag_(3)Cu([Ag_(3)Cu(tppm)(R/S-IPTT)]ClO_(4),R/S-IPTT=R/S-4-isopropylthiazolidine-2-thiolate,tppm=tris(diphenylphosphino)methane)in high yield(89%-91%)through selective doping of a Cu(Ⅰ)atom into chiral homometallic cluster enantiomers R/S-Ag_(4)([Ag_(4)(tppm)(R/S-IPTT)]ClO_(4)).In stark contrast to R/S-Ag_(4)(Φ_(em)<0.5%)that displays weak circularly polarized luminescence(CPL)with phosphorescence characteristic,R/S-Ag_(3)Cu(Φ_(em)≈70%)demonstrates strong CPL properties featured with thermally activated delay fluorescence(TADF)at ambient temperature.The selective substitution of the apical Ag(Ⅰ)atom in Ag_(4)triangular pyramid with a Cu(Ⅰ)atom not only gives rise to beyond 100-fold boosting of photoluminescence quantum yield(PLQY),but also leads to more pronounced optically chiral activity of alloy clusters in excited states in view of the larger photoluminescence dissymmetry factors(g_(PL))of R/S-Ag_(3)Cu(-3.5×10^(-3)/3.4×10^(-3))than that of R/S-Ag_(4)(-2.7×10^(-3)/2.6×10^(-3)).Furthermore,compared with chiral homometallic clusters R/S-Cu_(4)([Cu_(4)(tppm)(R/S-IPTT)]ClO_(4))with the same TADF characteristic at ambient temperature,R/S-Ag_(3)Cu manifests 1.7-fold PLQY and 6-fold g_(PL)due to faster reverse intersystem crossing(RISC)and more effective coupling of electric and magnetic transition moments in alloy clusters.This work not only presents a typical example of selective heterometal doping to modulate excited-state properties of isostructural metal clusters,but also gets deeper insight into the doping chemistry of dissimilar metals at the molecular level.
基金supported by the National Natural Science Foundation of China (52402298, 52172224, 52202228, 22479112)the Science and Technology Correspondent Project of Tianjin(24YDTPJC00240)+3 种基金Science Research Project of Hebei Education Department (BJK2022011)Central Funds Guiding the Local Science and Technology Development of Hebei Province (236Z4404G)the Beijing Tianjin Hebei Basic Research Cooperation Special Project(E2024202273)Tianjin Sci.&Tech. Program (22YFYSHZ00220)
文摘O3-types layered cathode materials in sodium-ion batteries(SIBs)suffer from the obvious lattice distortion induced by the complex phase transitions during Na^(+)intercalation/deintercalation process,leading to severe structural collapse and performance degradation.Herein,a series of high valence tantalum(Ta^(5+))doped Na(Ni_(0.4)Fe_(0.2)Mn_(0.4))_(1−x)Ta_(x)O_(2)(x=0/0.0025/0.005/0.01)secondary spherical particles are firstly developed,where Ta^(5+)doping enables the refined primary grain with a tightly stacked rod-like morphology.Comprehensive structural analysis via Neutron powder diffraction(NPD)and Synchrotron radiation X-ray diffraction(SXRD)reveals an expanded NaO_(2)slab and a reduction in Na site vacancy.The potential charge compensation mechanism is further illustrated by X-ray absorption spectroscopy(XAS)and X-ray photoelectron spectroscopy(XPS),unveiling a partial reduction from Ni^(3+)to Ni^(2+)with Ta^(5+)doping.In situ X-ray diffraction(in situ XRD)suggests that the decorated sample undergoes a volume change as low as 0.8%,in contrast with the pristine one(1.5%).Thus,the optimized sample with x=0.005 retains an enhanced capacity retention up to 70.4%at 1 C after 300 cycles in half-cell and delivers a high energy density of 251 Wh kg^(-1)(0.1 C)and with a good capacity retention of 81.0%at 1 C after 200 cycles in full-cell.Our findings provide new insights into the mechanism of high valence Ta^(5+)doping in stabilizing layered oxides cathode materials for SIBs.
基金supported by the National Natural Science Foundation of China (Grant Nos.12074213 and 11574108)the Major Basic Program of Natural Science Foundation of Shandong Province (Grant No.ZR2021ZD01)the Natural Science Foundation of Shandong Province (Grant No.ZR2023MA082)。
文摘In recent years,the research on superconductivity in one-dimensional(1D)materials has been attracting increasing attention due to its potential applications in low-dimensional nanodevices.However,the critical temperature(T_(c))of 1D superconductors is low.In this work,we theoretically investigate the possible high T_(c) superconductivity of(5,5)carbon nanotube(CNT).The pristine(5,5)CNT is a Dirac semimetal and can be modulated into a semiconductor by full hydrogenation.Interestingly,by further hole doping,it can be regulated into a metallic state with the sp^(3)-hybridized σ electrons metalized,and a giant Kohn anomaly appears in the optical phonons.The two factors together enhance the electron–phonon coupling,and lead to high-T_(c) superconductivity.When the hole doping concentration of hydrogenated-(5,5)CNT is 2.5 hole/cell,the calculated T_(c) is 82.3 K,exceeding the boiling point of liquid nitrogen.Therefore,the predicted hole-doped hydrogenated-(5,5)CNT provides a new platform for 1D high-T_(c) superconductivity and may have potential applications in 1D nanodevices.
基金financially supported by the National Natural Science Foundation of China(No.22172144 and 22272151)Key Research and Development Program of Zhejiang Province(2023C03148).
文摘Photocatalytic nitrogen fixation has emerged as a sustainable alternative for ammonia synthesis,playing a crucial role in alleviating energy shortages and environmental pollution.In this study,PbBiO_(2)Br was applied to photocatalytic nitrogen fixation for the first time,and its photocatalytic performance was effectively enhanced through Cu doping.The catalyst was synthesized via a simple reduction method,and its morphology,structure,and physicochemical properties were systematically investigated using various characterization techniques and density functional theory calculations.The results revealed that the incorporation of Cu2+partially replaced Pb2+,inducing lattice distortion in PbBiO_(2)Br,promoting the formation of oxygen vacancies,and modifying its electronic band structure.Specifically,Cu doping led to a slight bandgap narrowing,a reduction in work function,and a significant upward shift in the conduction band position.These changes enhanced light absorption,facilitated charge carrier migration and separation,and improved the reduction ability of photogenerated electrons.Moreover,Cu doping promoted N_(2)adsorption and activation.Consequently,the photocatalytic nitrogen fixation performance of Cu-doped PbBiO_(2)Br was significantly enhanced,achieving an optimal nitrogen fixation rate of 293μmol L^(−1)g^(−1)h^(−1),which is 3.6 times higher than that of pristine PbBiO_(2)Br.Additionally,Cu–PbBiO_(2)Br also showed good activity in the photocatalytic degradation of RhB,with a degradation rate 4.6 times higher than that of PbBiO_(2)Br.This work offers new insights into the application of PbBiO_(2)Br in photocatalytic nitrogen fixation and offers valuable guidance for the development of highly efficient nitrogen fixation materials in the future.
基金Project supported by the National Natural Science Foundation of China (12174075)the Scientific and Technological Bases and Talents of Guangxi (Guike AD21220016)+1 种基金Guangxi Science and Technology Major Project(AA23073018)the special fund for Guangxi Bagui Scholars。
文摘Mn^(2+)-doped CsPbCl_(3)(Mn^(2+):CsPbCl_(3)) nanocrystals(NCs) have attracted considerable attention due to their unique strong and broad orange-red emission band,presenting promising applications in the field of photoelectric devices.However,pristine Mn^(2+):CsPbCl_(3)NCs commonly suffer from low photoluminescence quantum yield(PL QY) and stability issues.Herein,we introduced europium ions(Eu^(3+))into Mn^(2+):CsPbCl_(3)NCs via the thermal injection synthesis method to obtain high performance Eu^(3+)and Mn^(2+)codoped CsPbCl_(3)(Eu^(3+)/Mn^(2+):CsPbCl_(3)) NCs.The maximum PL QY of the resulting Eu^(3+)/Mn^(2+):CsPbCl_(3)NCs reaches up to 90.92%.It is found that the doping of Eu^(3+)ions significantly reduces the non-radiative recombination caused by high defect states,and improves the energy transfer efficiency from exciton to Mn^(2+),thereby boosting the PL performance.Moreover,doping Eu^(3+)ions notably improves the UV-light and water stability of Mn^(2+):CsPbCl_(3)NCs.We further demonstrate the application versatility of Eu^(3+)/Mn^(2+):CsPbCl_(3)NCs in white light emitting diodes(WLEDs) and optical anticounterfeiting applications.This work provides a valuable perspective for the attainment of high performance Mn^(2+):CsPbCl_(3)NCs and lays a foundation for the codoping of other lanthanide ions to adjust the luminescence properties of Mn^(2+):CsPbCl_(3)NCs.
