A series of TiO2/Bi2O3 heterojunction microfibers have been fabricated using cotton fibers as bio-templates, and characterized by XRD, SEM and UV-Vis techniques. Results reveal that Bi2O3 in the TiO2/Bi2O3 sample is a...A series of TiO2/Bi2O3 heterojunction microfibers have been fabricated using cotton fibers as bio-templates, and characterized by XRD, SEM and UV-Vis techniques. Results reveal that Bi2O3 in the TiO2/Bi2O3 sample is assigned to monoclinic and tetragonal mix-crystal phase. Fibers lengths can reach several micrometers and diameters range from 0.5 μm to 3 μm. Compared with pure TiO2 and Bi2O3, TiO2/Bi2O3 samples display better absorption in visible light region. Photocatalytic activity was evaluated by degradation of MB under visible light irradiation. TiO2/Bi2O3 microfibers exhibite much higher activity than pure TiO2 and Bi2O3, and 22.84%TiO2/Bi2O3 can achieve the decomposition of about 95%MB, which is attributed to synergistic effects of the strong visible-light absorption of TiO2/Bi2O3 microfibers and the heterojunction formed between TiO2 and Bi2O3.展开更多
Enhanced oil recovery(EOR)operations increasingly depend on emulsion-based formulations that exhibit long-term stability under reservoir conditions while minimizing surfactant dosage.In this context,hybrid systems com...Enhanced oil recovery(EOR)operations increasingly depend on emulsion-based formulations that exhibit long-term stability under reservoir conditions while minimizing surfactant dosage.In this context,hybrid systems combining nanoparticles and surfactants offer a promising route to achieving both interfacial stability and formulation efficiency.Among potential nanoparticle candidates,Ti3C2TxMXene exhibits high surface area and interfacial activity.However,its application in diesel-in-water Pickering emulsions under EOR-relevant conditions has not been explored.Challenges such as high hydrophilicity and strong electrostatic repulsion have limited the use of unmodified MXene as a standalone stabilizer in colloidal systems.To address this limitation,diesel-in-water Pickering emulsions were formulated using DL-Ti3C2TxMXene combined with Tween 40(0.5 wt%)and antifoam(0.15 wt%),aiming to investigate their synergistic stabilization behavior across MXene concentrations ranging from 0.1 to 1.5 wt%.The MXene-only system exhibited complete and immediate phase separation,whereas the hybrid emulsions demonstrated markedly enhanced stability,with no phase separation observed at 0.1 and 0.5 wt%after 24 h.A concentration-dependent trend was evident.At lower MXene contents,interfacial adsorption improved,and droplet sizes remained small and uniform.At higher concentrations(≥1.0 wt%),aggregation increased,and demulsification became more pronounced.Interfacial tension decreased steadily with increasing MXene content,reaching 0.86 mN/m at1.5 wt%,while zeta potential remained strongly negative(-47.7 mV at 0.5 wt%),indicating sufficient electrostatic repulsion.Rheological analysis revealed a transition to shear-thinning behavior at higher MXene contents,confirming the formation of internal network structures.Compared to other reported systems based on silica(SiO2),zinc oxide(ZnO),or functionalized MXenes,the MXene-Tween 40formulation achieved superior short-and long-term emulsion stability without requiring surface modification or external stimuli.To the best of our knowledge,this is the first study to report the successful stabilization of diesel-in-water Pickering emulsions using unmodified Ti3C2TxMXene.These findings highlight the synergistic interaction between MXene and Tween 40 and present a robust,surfactant-lean formulation suitable for oilfield applications.展开更多
Bi/Bi2Fe4O9nanocomposites consisting of Bi2Fe4O9nanosheets decorated with Bi nanodots were synthesized by a hydrothermal method.The formation of Bi nanodots on the Bi2Fe4O9nanosheet surfaces...Bi/Bi2Fe4O9nanocomposites consisting of Bi2Fe4O9nanosheets decorated with Bi nanodots were synthesized by a hydrothermal method.The formation of Bi nanodots on the Bi2Fe4O9nanosheet surfaces was attributed to the reducibility of 2-methoxyethanol in the precursor solution.Comparative photocatalytic evaluation reveals that the Bi/Bi2Fe4O9nanocomposites significantly enhance the degradation efficiency(99.0%)of bisphenol A compared with Bi2Fe4O9nanosheets(64.2%)under 120 min simulated solar irradiation.This remarkable enhancement can be attributed to the established Bi/Bi2Fe4O9heterojunction structure,which effectively facilitates the separation of photogenerated electron-hole pairs and accelerates interfacial charge transfer between the metallic Bi nanodots and semiconductor Bi2Fe4O9nanosheets.The synergistic effects arising from this unique architecture ultimately lead to superior photocatalytic performance.展开更多
Developing high-performance near-room-temperature thermoelectric materials is crucial for solid-state cooling and low-grade waste heat recovery.While n-type Mg3(Sb,Bi)2has emerged as a promising candidate,its pe...Developing high-performance near-room-temperature thermoelectric materials is crucial for solid-state cooling and low-grade waste heat recovery.While n-type Mg3(Sb,Bi)2has emerged as a promising candidate,its performance is fundamentally bottlenecked by the strong coupling of charge and heat transport,particularly the restricted carrier mobility originating from highly localized polar covalent bonds.Herein,we propose a synergistic strategy that manipulates chemical bond polarity and constructs multiscale defect architectures via Ni doping to decouple electron and phonon transport.First-principles calculations and structural analyses reveal that substituting Mg with the more electronegative Ni significantly reduces the cation-anion electronegativity difference.This effectively weakens the polarity of the Mg-(Sb,Bi)bonds and drives an antibonding-state-induced electron delocalization,yielding a remarkable~49.5%enhancement in room-temperature carrier mobility(up to 265.69 cm2V-1s-1).Concurrently,exceeding the solid solubility limit of Ni triggers the spontaneous formation of Ni-rich nanoprecipitates.These precipitates,coupled with point defects and local lattice distortions,establish a robust multiscale scattering network that effectively suppresses the lattice thermal conductivity to 0.74 W m-1K-1at 300 K.Consequently,the optimized Mg3.3Sb0.5Bi1.497Te0.003Ni0.01sample achieves an exceptional room-temperature power factor of~31.61μW cm-1K-2,culminating in a high room-temperature ZT of 0.84 and a peak ZT of 1.10 at 423 K.This work not only highlights the potential of n-type Mg3(Sb,Bi)2for near-room-temperature applications but also establishes a universal paradigm for optimizing polar thermoelectric semiconductors through electronegativity-driven bond engineering.展开更多
Magnesium hydride serves as a promising solid-state hydrogen storage material owing to its high potential.However,its practical applications are constrained by the high enthalpy of hydrogen absorption and slow kinetic...Magnesium hydride serves as a promising solid-state hydrogen storage material owing to its high potential.However,its practical applications are constrained by the high enthalpy of hydrogen absorption and slow kinetics.In this study,we prepared a Ni/Ti3O5@graphene oxide(GO)dual-heterojunction composite material via solvent heating,electrostatic adsorption,and calcination to improve the hydrogen storage capabilities of MgH2.Adding Ni/Ti3O5@GO to MgH2 lowered the initial dehydrogenation temperature of MgH2 to 183℃;at a dehydrogenation temperature of 275℃,6.4 wt.%of H2 escaped from the MgH2 bulk.In addition,the hydrogen storage material absorbed 1.8 wt.%H2 at 30℃ for 30 min.The calculated activation energy of dehydrogenation was 48.221±0.141 kJ·mol-1,which was significantly lower than that of the ball-milled MgH2(112.63±1.44 kJ·mol-1).Mechanistic analysis results revealed that the heterojunction constructed from the multiphase compound system provided a large number of active sites and hydrogen diffusion routes,resulting in a synergistic catalytic effect that enhanced the hydrogen storage capacity of MgH2.In this work,we clarified the compositions of fuzzy interfaces in heterostructured materials by conducting ultraviolet photoelectron spectroscopy tests and identified key composite materials for the formation of heterojunctions.展开更多
Industrial fly ash-derived SiO2aerogel with abundant mesopores has an excellent ability to support active ingredients for constructing efficient and stable catalyst in electrochemical CO2reduction reaction(CO_(2...Industrial fly ash-derived SiO2aerogel with abundant mesopores has an excellent ability to support active ingredients for constructing efficient and stable catalyst in electrochemical CO2reduction reaction(CO2RR).However,how to select and arrange active sites on its surface poses significant challenges due to its non-conductive nature.Here,we subtly designed and synthesized multi-component architectures to achieve the high efficiency of CO2RR to CO.The embedding of active and amorphous nitrogen-doped carbon(NC)nanosheets on the surface and inside of SiO2aerogel ensures the charge transport on the catalyst surface,and Er2O3improves dissociation of H2O,enabling the supply of protons for CO2RR.Simultaneously,Er2O3-induced defects/vacancies,nanoclusters coordinated with N on amorphous NC and single Ni in NC play crucial role in enhancing adsorption and activation of CO2.Consequently,the Ni-Er2O3/NC-SiO2catalyst exhibits the maintenance of FECOhigher than 95%over a wide potential window(-0.22 to-1.12 V vs.RHE)in a flow cell with gas-liquid-solid electrode.This work not only provides an atomistic understanding of nature of active sites in CO2RR but also contributes to the secondary utilization of industrial fly ash for a carbon-neutral future.展开更多
Sodium-ion batteries(SIBs)are regarded as a promising alternative to lithium-ion batteries for grid-scale energy storage owing to their low cost and sustainability;however,their competitiveness is still limited by rel...Sodium-ion batteries(SIBs)are regarded as a promising alternative to lithium-ion batteries for grid-scale energy storage owing to their low cost and sustainability;however,their competitiveness is still limited by relatively low energy density.Here,we report a scalable Mn-Fe-Ni layered oxide with a compositional-structural dual-gradient(DG)architecture synthesized via a three-step co-precipitation method.By exploiting the opposite roles of high-ionic-potential Mn and low-ionic-potential Fe in stabilizing the P2 and O3 frameworks,respectively,a pure compositional Mn/Fe gradient is translated into a structural P2/O3 gradient with precisely guided synthesis conditions.The Fe-deficient surface effectively suppressed Fe4+-induced side reactions,while the stable P2-type shell and the enlarged R value of the O3 core further enhanced cycling stability during structural evolution.The optimized cathode delivered an energy density of 478 Wh kg-1at 4.2 V,with 82%capacity retention after 200 cycles in half cells and 91%retention after 1600 cycles in full cells.This study demonstrates a viable pathway for developing high-energy-density and long-lifetime cathodes for sodium-ion batteries.展开更多
As an emerging crystalline porous material,hydrogen bonded organic frameworks(HOFs)have enormous potential in photocatalytic field.However,poor stability and rapid recombination of photogenerated charges hinder their ...As an emerging crystalline porous material,hydrogen bonded organic frameworks(HOFs)have enormous potential in photocatalytic field.However,poor stability and rapid recombination of photogenerated charges hinder their practical application in photocatalytic H2O2production.To address the above challenges,this work employs a wet chemical method to grow In2S3nanosheets in situ on the surface of highly stable HOF nanorods(PFC-1),resulting in a novel inorganic/organic In2S3/PFC-1(IP)S-scheme heterojunction.The optimal IP composite achieves a significantly improved photocatalytic H2O2evolution rate of 3.78 mmol g-1h-1,which is 2.9-and 3.7-fold than that of In2S3and PFC-1,respectively.The elevated visible-light absorption,abundant active sites,and effective charge separation of IP S-scheme heterojunction result in the improvement in photocatalytic performance.Additionally,photocatalytic H2O2production of IP goes through a two-electron O2 reduction reaction pathway.This work offers a novel strategy for the fabrication of efficient HOF-based S-scheme heterostructures and their application in photocatalytic field.展开更多
In this work,the TiO2/Sb2S3 nanorod arrays(NRAs)were synthesized through a two-stage hydrothermal route for photoelectrochemical(PEC)water splitting.The effect of annealing treatment in Ar ambience on the PEC...In this work,the TiO2/Sb2S3 nanorod arrays(NRAs)were synthesized through a two-stage hydrothermal route for photoelectrochemical(PEC)water splitting.The effect of annealing treatment in Ar ambience on the PEC activity of TiO2/Sb2S3 composite sample was investigated by electrochemical impedance analysis,including Nyquist and Mott-Schottky(M-S)plots.It was demonstrated that vacuum annealing could crystallize Sb2S3 component and change its color from red to black,leading to an increment of photocurrent density from 1.9 A/m2 to 4.25 A/m2 at 0 V versus saturated calomel electrode(VSCE).The enhanced PEC performance was mainly attributed to the improved visible light absorption.Moreover,annealing treatment facilitated retarding the electron-hole recombination occurred at the solid/liquid interfaces.Our work might provide a novel strategy for enhancing the PEC performance of a semiconductor electrode.展开更多
针对光固化Al2O3陶瓷在脱脂烧结后易形成孔洞、力学性能差的问题,系统研究了石墨烯添加对陶瓷浆料流变性、沉降性、固化行为及烧结体力学性能的影响。采用γ-缩水甘油醚氧丙基三甲氧基硅烷(KH560)对Al2O3粉体进行表面改性,并加入不同含...针对光固化Al2O3陶瓷在脱脂烧结后易形成孔洞、力学性能差的问题,系统研究了石墨烯添加对陶瓷浆料流变性、沉降性、固化行为及烧结体力学性能的影响。采用γ-缩水甘油醚氧丙基三甲氧基硅烷(KH560)对Al2O3粉体进行表面改性,并加入不同含量的石墨烯,制备高固相、低粘度的光固化浆料。通过傅里叶红外光谱、旋转流变仪、沉降试验及Beer-Lambert模型分析,优化了浆料配方与光固化工艺参数。结果表明:当KH560含量为2.5wt%、石墨烯含量为0.01wt%时,浆料粘度最低、沉降分层最少;在曝光时间4 s条件下,添加0.01wt%石墨烯的浆料透射深度为382μm,临界曝光能量为44.3 m J/cm2。经1750℃烧结后,陶瓷零件致密度达99.7%,弯曲强度为27.61 MPa,维氏硬度为13.45GPa。石墨烯通过位阻效应及裂纹偏转机制有效促进了烧结致密化并改善了力学性能。本研究为光固化增材制造高致密、高性能氧化铝陶瓷提供了试验依据。展开更多
P2型层状过渡金属氧化物(P2-NaxTMO2)因其优异的循环稳定性和倍率性能,成为钠离子电池正极材料的有力候选者。然而,其在高电压下的不可逆相变和固有低理论容量问题,阻碍了实际应用。本研究工作提出高熵策略与双相结构的协同设计...P2型层状过渡金属氧化物(P2-NaxTMO2)因其优异的循环稳定性和倍率性能,成为钠离子电池正极材料的有力候选者。然而,其在高电压下的不可逆相变和固有低理论容量问题,阻碍了实际应用。本研究工作提出高熵策略与双相结构的协同设计来克服这些挑战。通过在P2相高熵基体中引入O3相,构建新型P2/O3双相高熵层状氧化物Na0.70Ni0.25Mn0.35Co0.15Fe0.05Ti0.20O2(简称Na0.70NMCFT)。其中,高熵设计通过构型熵稳定效应有效抑制P2相的不可逆相变,而O3相则通过协同作用弥补容量不足并提升循环稳定性。此外,双相组分之间的相互作用进一步促进P2-O3与P2-P3相变的高度可逆性。Na0.70NMCFT在1C倍率下的初始放电容量为102.08 mAhg-1,200次循环后容量保持率达88.15%,表明具有优异的循环稳定性。更重要的是,即使在10C的高倍率下,Na0.70NMCFT仍能提供85.67 mAh g-1的初始放电比容量,并在1000次循环后容量保持率达70%。本工作证实双相高熵设计在提升钠离子电池正极性能中的关键作用,为开发先进钠离子电池正极材料提供了新思路。展开更多
基金V. ACKNOWLEDGEMENTS This work was supported by the Scientific Research Program Funded by Shaanxi Provincial Education Department (No.2013JK0690), and the Shaanxi Province Natural Science Foundation (No.2013JM2013), the National Natural Science Foundation of China (No.21203160), and the Special Research Fund of Xianyang Normal University (No. 11XSYK204).
摘要A series of TiO2/Bi2O3 heterojunction microfibers have been fabricated using cotton fibers as bio-templates, and characterized by XRD, SEM and UV-Vis techniques. Results reveal that Bi2O3 in the TiO2/Bi2O3 sample is assigned to monoclinic and tetragonal mix-crystal phase. Fibers lengths can reach several micrometers and diameters range from 0.5 μm to 3 μm. Compared with pure TiO2 and Bi2O3, TiO2/Bi2O3 samples display better absorption in visible light region. Photocatalytic activity was evaluated by degradation of MB under visible light irradiation. TiO2/Bi2O3 microfibers exhibite much higher activity than pure TiO2 and Bi2O3, and 22.84%TiO2/Bi2O3 can achieve the decomposition of about 95%MB, which is attributed to synergistic effects of the strong visible-light absorption of TiO2/Bi2O3 microfibers and the heterojunction formed between TiO2 and Bi2O3.
基金support of the Qatar National Research Fund(QNRF),grant reference number GSRA9-L-2-0511-22005。
摘要Enhanced oil recovery(EOR)operations increasingly depend on emulsion-based formulations that exhibit long-term stability under reservoir conditions while minimizing surfactant dosage.In this context,hybrid systems combining nanoparticles and surfactants offer a promising route to achieving both interfacial stability and formulation efficiency.Among potential nanoparticle candidates,Ti3C2TxMXene exhibits high surface area and interfacial activity.However,its application in diesel-in-water Pickering emulsions under EOR-relevant conditions has not been explored.Challenges such as high hydrophilicity and strong electrostatic repulsion have limited the use of unmodified MXene as a standalone stabilizer in colloidal systems.To address this limitation,diesel-in-water Pickering emulsions were formulated using DL-Ti3C2TxMXene combined with Tween 40(0.5 wt%)and antifoam(0.15 wt%),aiming to investigate their synergistic stabilization behavior across MXene concentrations ranging from 0.1 to 1.5 wt%.The MXene-only system exhibited complete and immediate phase separation,whereas the hybrid emulsions demonstrated markedly enhanced stability,with no phase separation observed at 0.1 and 0.5 wt%after 24 h.A concentration-dependent trend was evident.At lower MXene contents,interfacial adsorption improved,and droplet sizes remained small and uniform.At higher concentrations(≥1.0 wt%),aggregation increased,and demulsification became more pronounced.Interfacial tension decreased steadily with increasing MXene content,reaching 0.86 mN/m at1.5 wt%,while zeta potential remained strongly negative(-47.7 mV at 0.5 wt%),indicating sufficient electrostatic repulsion.Rheological analysis revealed a transition to shear-thinning behavior at higher MXene contents,confirming the formation of internal network structures.Compared to other reported systems based on silica(SiO2),zinc oxide(ZnO),or functionalized MXenes,the MXene-Tween 40formulation achieved superior short-and long-term emulsion stability without requiring surface modification or external stimuli.To the best of our knowledge,this is the first study to report the successful stabilization of diesel-in-water Pickering emulsions using unmodified Ti3C2TxMXene.These findings highlight the synergistic interaction between MXene and Tween 40 and present a robust,surfactant-lean formulation suitable for oilfield applications.
基金Funded by the National Natural Science Foundation of China(No.50902108)。
摘要Bi/Bi2Fe4O9nanocomposites consisting of Bi2Fe4O9nanosheets decorated with Bi nanodots were synthesized by a hydrothermal method.The formation of Bi nanodots on the Bi2Fe4O9nanosheet surfaces was attributed to the reducibility of 2-methoxyethanol in the precursor solution.Comparative photocatalytic evaluation reveals that the Bi/Bi2Fe4O9nanocomposites significantly enhance the degradation efficiency(99.0%)of bisphenol A compared with Bi2Fe4O9nanosheets(64.2%)under 120 min simulated solar irradiation.This remarkable enhancement can be attributed to the established Bi/Bi2Fe4O9heterojunction structure,which effectively facilitates the separation of photogenerated electron-hole pairs and accelerates interfacial charge transfer between the metallic Bi nanodots and semiconductor Bi2Fe4O9nanosheets.The synergistic effects arising from this unique architecture ultimately lead to superior photocatalytic performance.
基金supported by the National Natural Science Foundation of China(Grant No.52471247)the Guangdong Innovative and Entrepreneurial Research Team Program(Grant No.2021ZT09L227)the Open Research Fund of Guangdong Provincial Key Laboratory of New Energy Materials Service Safety(Grant No.NEMSS202404)。
摘要Developing high-performance near-room-temperature thermoelectric materials is crucial for solid-state cooling and low-grade waste heat recovery.While n-type Mg3(Sb,Bi)2has emerged as a promising candidate,its performance is fundamentally bottlenecked by the strong coupling of charge and heat transport,particularly the restricted carrier mobility originating from highly localized polar covalent bonds.Herein,we propose a synergistic strategy that manipulates chemical bond polarity and constructs multiscale defect architectures via Ni doping to decouple electron and phonon transport.First-principles calculations and structural analyses reveal that substituting Mg with the more electronegative Ni significantly reduces the cation-anion electronegativity difference.This effectively weakens the polarity of the Mg-(Sb,Bi)bonds and drives an antibonding-state-induced electron delocalization,yielding a remarkable~49.5%enhancement in room-temperature carrier mobility(up to 265.69 cm2V-1s-1).Concurrently,exceeding the solid solubility limit of Ni triggers the spontaneous formation of Ni-rich nanoprecipitates.These precipitates,coupled with point defects and local lattice distortions,establish a robust multiscale scattering network that effectively suppresses the lattice thermal conductivity to 0.74 W m-1K-1at 300 K.Consequently,the optimized Mg3.3Sb0.5Bi1.497Te0.003Ni0.01sample achieves an exceptional room-temperature power factor of~31.61μW cm-1K-2,culminating in a high room-temperature ZT of 0.84 and a peak ZT of 1.10 at 423 K.This work not only highlights the potential of n-type Mg3(Sb,Bi)2for near-room-temperature applications but also establishes a universal paradigm for optimizing polar thermoelectric semiconductors through electronegativity-driven bond engineering.
基金supported by the National Natural Science Foundation of China[grant number U24A2044]Science and Technology Major Program of Guangxi Province[grant number GUIKEAA24206007].
摘要Magnesium hydride serves as a promising solid-state hydrogen storage material owing to its high potential.However,its practical applications are constrained by the high enthalpy of hydrogen absorption and slow kinetics.In this study,we prepared a Ni/Ti3O5@graphene oxide(GO)dual-heterojunction composite material via solvent heating,electrostatic adsorption,and calcination to improve the hydrogen storage capabilities of MgH2.Adding Ni/Ti3O5@GO to MgH2 lowered the initial dehydrogenation temperature of MgH2 to 183℃;at a dehydrogenation temperature of 275℃,6.4 wt.%of H2 escaped from the MgH2 bulk.In addition,the hydrogen storage material absorbed 1.8 wt.%H2 at 30℃ for 30 min.The calculated activation energy of dehydrogenation was 48.221±0.141 kJ·mol-1,which was significantly lower than that of the ball-milled MgH2(112.63±1.44 kJ·mol-1).Mechanistic analysis results revealed that the heterojunction constructed from the multiphase compound system provided a large number of active sites and hydrogen diffusion routes,resulting in a synergistic catalytic effect that enhanced the hydrogen storage capacity of MgH2.In this work,we clarified the compositions of fuzzy interfaces in heterostructured materials by conducting ultraviolet photoelectron spectroscopy tests and identified key composite materials for the formation of heterojunctions.
基金National Natural Science Foundation of China(22468034,22162019,22261040)Key Research and Development Project of Ordos(YF20240062)Science and Technology Projects of Inner Mongolia Autonomous Region(2021GG0195)。
摘要Industrial fly ash-derived SiO2aerogel with abundant mesopores has an excellent ability to support active ingredients for constructing efficient and stable catalyst in electrochemical CO2reduction reaction(CO2RR).However,how to select and arrange active sites on its surface poses significant challenges due to its non-conductive nature.Here,we subtly designed and synthesized multi-component architectures to achieve the high efficiency of CO2RR to CO.The embedding of active and amorphous nitrogen-doped carbon(NC)nanosheets on the surface and inside of SiO2aerogel ensures the charge transport on the catalyst surface,and Er2O3improves dissociation of H2O,enabling the supply of protons for CO2RR.Simultaneously,Er2O3-induced defects/vacancies,nanoclusters coordinated with N on amorphous NC and single Ni in NC play crucial role in enhancing adsorption and activation of CO2.Consequently,the Ni-Er2O3/NC-SiO2catalyst exhibits the maintenance of FECOhigher than 95%over a wide potential window(-0.22 to-1.12 V vs.RHE)in a flow cell with gas-liquid-solid electrode.This work not only provides an atomistic understanding of nature of active sites in CO2RR but also contributes to the secondary utilization of industrial fly ash for a carbon-neutral future.
基金National Natural Science Foundation(NNSF)of China(No.52572267)Guangdong Basic and Applied Basic Research Foundation(2023A1515140126)+1 种基金Ministry of Science and Technology of Guangdong Province(2023B0909020001)Guangdong High-level Innovation Institute Project(2021B0909050001)。
摘要Sodium-ion batteries(SIBs)are regarded as a promising alternative to lithium-ion batteries for grid-scale energy storage owing to their low cost and sustainability;however,their competitiveness is still limited by relatively low energy density.Here,we report a scalable Mn-Fe-Ni layered oxide with a compositional-structural dual-gradient(DG)architecture synthesized via a three-step co-precipitation method.By exploiting the opposite roles of high-ionic-potential Mn and low-ionic-potential Fe in stabilizing the P2 and O3 frameworks,respectively,a pure compositional Mn/Fe gradient is translated into a structural P2/O3 gradient with precisely guided synthesis conditions.The Fe-deficient surface effectively suppressed Fe4+-induced side reactions,while the stable P2-type shell and the enlarged R value of the O3 core further enhanced cycling stability during structural evolution.The optimized cathode delivered an energy density of 478 Wh kg-1at 4.2 V,with 82%capacity retention after 200 cycles in half cells and 91%retention after 1600 cycles in full cells.This study demonstrates a viable pathway for developing high-energy-density and long-lifetime cathodes for sodium-ion batteries.
摘要As an emerging crystalline porous material,hydrogen bonded organic frameworks(HOFs)have enormous potential in photocatalytic field.However,poor stability and rapid recombination of photogenerated charges hinder their practical application in photocatalytic H2O2production.To address the above challenges,this work employs a wet chemical method to grow In2S3nanosheets in situ on the surface of highly stable HOF nanorods(PFC-1),resulting in a novel inorganic/organic In2S3/PFC-1(IP)S-scheme heterojunction.The optimal IP composite achieves a significantly improved photocatalytic H2O2evolution rate of 3.78 mmol g-1h-1,which is 2.9-and 3.7-fold than that of In2S3and PFC-1,respectively.The elevated visible-light absorption,abundant active sites,and effective charge separation of IP S-scheme heterojunction result in the improvement in photocatalytic performance.Additionally,photocatalytic H2O2production of IP goes through a two-electron O2 reduction reaction pathway.This work offers a novel strategy for the fabrication of efficient HOF-based S-scheme heterostructures and their application in photocatalytic field.
基金supported by the Fundamental Research Funds for the Central Universities(No.2019ZDPY04).
摘要In this work,the TiO2/Sb2S3 nanorod arrays(NRAs)were synthesized through a two-stage hydrothermal route for photoelectrochemical(PEC)water splitting.The effect of annealing treatment in Ar ambience on the PEC activity of TiO2/Sb2S3 composite sample was investigated by electrochemical impedance analysis,including Nyquist and Mott-Schottky(M-S)plots.It was demonstrated that vacuum annealing could crystallize Sb2S3 component and change its color from red to black,leading to an increment of photocurrent density from 1.9 A/m2 to 4.25 A/m2 at 0 V versus saturated calomel electrode(VSCE).The enhanced PEC performance was mainly attributed to the improved visible light absorption.Moreover,annealing treatment facilitated retarding the electron-hole recombination occurred at the solid/liquid interfaces.Our work might provide a novel strategy for enhancing the PEC performance of a semiconductor electrode.
摘要针对光固化Al2O3陶瓷在脱脂烧结后易形成孔洞、力学性能差的问题,系统研究了石墨烯添加对陶瓷浆料流变性、沉降性、固化行为及烧结体力学性能的影响。采用γ-缩水甘油醚氧丙基三甲氧基硅烷(KH560)对Al2O3粉体进行表面改性,并加入不同含量的石墨烯,制备高固相、低粘度的光固化浆料。通过傅里叶红外光谱、旋转流变仪、沉降试验及Beer-Lambert模型分析,优化了浆料配方与光固化工艺参数。结果表明:当KH560含量为2.5wt%、石墨烯含量为0.01wt%时,浆料粘度最低、沉降分层最少;在曝光时间4 s条件下,添加0.01wt%石墨烯的浆料透射深度为382μm,临界曝光能量为44.3 m J/cm2。经1750℃烧结后,陶瓷零件致密度达99.7%,弯曲强度为27.61 MPa,维氏硬度为13.45GPa。石墨烯通过位阻效应及裂纹偏转机制有效促进了烧结致密化并改善了力学性能。本研究为光固化增材制造高致密、高性能氧化铝陶瓷提供了试验依据。
摘要P2型层状过渡金属氧化物(P2-NaxTMO2)因其优异的循环稳定性和倍率性能,成为钠离子电池正极材料的有力候选者。然而,其在高电压下的不可逆相变和固有低理论容量问题,阻碍了实际应用。本研究工作提出高熵策略与双相结构的协同设计来克服这些挑战。通过在P2相高熵基体中引入O3相,构建新型P2/O3双相高熵层状氧化物Na0.70Ni0.25Mn0.35Co0.15Fe0.05Ti0.20O2(简称Na0.70NMCFT)。其中,高熵设计通过构型熵稳定效应有效抑制P2相的不可逆相变,而O3相则通过协同作用弥补容量不足并提升循环稳定性。此外,双相组分之间的相互作用进一步促进P2-O3与P2-P3相变的高度可逆性。Na0.70NMCFT在1C倍率下的初始放电容量为102.08 mAhg-1,200次循环后容量保持率达88.15%,表明具有优异的循环稳定性。更重要的是,即使在10C的高倍率下,Na0.70NMCFT仍能提供85.67 mAh g-1的初始放电比容量,并在1000次循环后容量保持率达70%。本工作证实双相高熵设计在提升钠离子电池正极性能中的关键作用,为开发先进钠离子电池正极材料提供了新思路。