A new sol-gel process is applied to fabricate the BST (BaxSr1-xTiO3) sol and nano-powder of La-Mn-Al co-doping with Ba/Sr ratio 65/35, and the BST thick film is prepared in the Pt/Ti/SiO2/Si substrate. The powder an...A new sol-gel process is applied to fabricate the BST (BaxSr1-xTiO3) sol and nano-powder of La-Mn-Al co-doping with Ba/Sr ratio 65/35, and the BST thick film is prepared in the Pt/Ti/SiO2/Si substrate. The powder and thick film are characterized by X-ray diffraction and transmission electron microscope. The influence of La-Mn-Al co-doping on the dielectric properties and micro-structure of BST thick film is analyzed. The results show that the La, Mn, and Al ions can take an obvious restraint on the growth of BaSrTiO3 grains. The polycrystalline particles come into being during the crystallization of thick film, which may improve the uniformity and compactness of thick film. The influence of unequal-valence and doping amount on the leakage current, dielectric loss, and dielectric property are mainly discussed. The dielectric constant and dielectric loss of thick film are 1200 and 0.03, respectively, in the case of 1mol% La doping, 2mol% Mn doping, and 1mol% Al doping.展开更多
S and Co co-doped carbon catalysts were prepared via pyrolysis of MOF-71 and thiourea mixtures at 800℃at a mass ratio of MOF-71 to thiourea of 1:0.1 to effectively activate peroxymonosulfate(PMS)for methylene blue(MB...S and Co co-doped carbon catalysts were prepared via pyrolysis of MOF-71 and thiourea mixtures at 800℃at a mass ratio of MOF-71 to thiourea of 1:0.1 to effectively activate peroxymonosulfate(PMS)for methylene blue(MB)degradation.The effects of two different mixing routes were identified on the MB degradation performance.Particularly,the catalyst obtained by the alcohol solvent evaporation(MOF-AEP)mixing route could degrade 95.60%MB(50 mg/L)within 4 min(degradation rate:K=0.78 min^(-1)),which was faster than that derived from the direct grinding method(MOF-DGP,80.97%,K=0.39 min^(-1)).X-ray photoelectron spectroscopy revealed that the Co-S content of MOF-AEP(43.39at%)was less than that of MOF-DGP(54.73at%),and the proportion of C-S-C in MOF-AEP(13.56at%)was higher than that of MOF-DGP(10.67at%).Density functional theory calculations revealed that the adsorption energy of Co for PMS was -2.94 eV when sulfur was doped as C-S-C on the carbon skeleton,which was higher than that when sulfur was doped next to cobalt in the form of Co-S bond(-2.86 eV).Thus,the C-S-C sites might provide more contributions to activate PMS compared with Co-S.Furthermore,the degradation parameters,including pH and MOF-AEP dosage,were investigated.Finally,radical quenching experiments and electron paramagnetic resonance(EPR)measurements revealed that ^(1)O_(2)might be the primary catalytic species,whereas·O~(2-)might be the secondary one in degrading MB.展开更多
Ni-rich layered oxide cathodes have shown promise for high-energy lithium-ion batteries(LIBs)but are usually limited to mild environments because of their rapid performance degradation under extreme temperature condit...Ni-rich layered oxide cathodes have shown promise for high-energy lithium-ion batteries(LIBs)but are usually limited to mild environments because of their rapid performance degradation under extreme temperature conditions(below0°C and above 50 °C).Here,we report the design of F/Mo co-doped LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(FMNCM)cathode for high-performance LIBs from-20 to 60°C.F^(-) doping with high electronegativity into the cathode surface is found to enhance the stability of surface lattice structure and protect the interface from side reactions with the electrolyte by generating a LiF-rich surface layer.Concurrently,the Mo^(6+) doping suppresses phase transition,which blocks Li^(+)/Ni^(2+) mixing,and stabilizes lithium-ion diffusion pathway.Remarkably,the FMNCM cathode demonstrates excellent cycling stability at a high cutoff voltage of 4.4 V,even at 60°C,maintaining 90.6%capacity retention at 3 C after 150 cycles.Additionally,at temperatures as low as-20°C,it retains 77.1%of its room temperature capacity,achieving an impressive 97.5%capacity retention after 500 cycles.Such stable operation under wide temperatures has been further validated in practical Ah-level pouch-cells.This study sheds light on both fundamental mechanisms and practical implications for the design of advanced cathode materials for wide-temperature LIBs,presenting a promising path towards high-energy and long-cycling LIBs with temperatureadaptability.展开更多
Atomic-scale doping strategies and structure design play pivotal roles in tailoring the electronic structure and physicochemical property of electromagnetic wave absorption(EMWA)materials.However,the relationship betw...Atomic-scale doping strategies and structure design play pivotal roles in tailoring the electronic structure and physicochemical property of electromagnetic wave absorption(EMWA)materials.However,the relationship between configuration and electromagnetic(EM)loss mechanism has remained elusive.Herein,drawing inspiration from the DNA transcription process,we report the successful synthesis of novel in situ Mn/N co-doped helical carbon nanotubes with ultrabroad EMWA capability.Theoretical calculation and EM simulation confirm that the orbital coupling and spin polarization of the Mn–N4–C configuration,along with cross polarization generated by the helical structure,endow the helical converters with enhanced EM loss.As a result,HMC-8 demonstrates outstanding EMWA performance,achieving a minimum reflection loss of−63.13 dB at an ultralow thickness of 1.29 mm.Through precise tuning of the graphite domain size,HMC-7 achieves an effective absorption bandwidth(EAB)of 6.08 GHz at 2.02 mm thickness.Furthermore,constructing macroscale gradient metamaterials enables an ultrabroadband EAB of 12.16 GHz at a thickness of only 5.00 mm,with the maximum radar cross section reduction value reaching 36.4 dB m2.This innovative approach not only advances the understanding of metal–nonmetal co-doping but also realizes broadband EMWA,thus contributing to the development of EMWA mechanisms and applications.展开更多
Although CoO is a promising electrode material for supercapacitors due to its high theoretical capacitance,the practical applications still suffering from inferior electrochemical activity owing to its low electrical ...Although CoO is a promising electrode material for supercapacitors due to its high theoretical capacitance,the practical applications still suffering from inferior electrochemical activity owing to its low electrical conductivity,poor structural stability and inefficient nanostructure.Herein,we report a novel Cu0/Cu+co-doped CoO composite with adjustable metallic Cu0 and ion Cu+via a facile strategy.Through interior(Cu+)and exterior(Cu0)decoration of CoO,the electrochemical performance of CoO electrode has been significantly improved due to both the beneficial flower-like nanostructure and the synergetic effect of Cu0/Cu+co-doping,which results in a significantly enhanced specific capacitance(695 F g^(-1) at 1 A g^(-1))and high cyclic stability(93.4%retention over 10,000 cycles)than pristine CoO.Furthermore,this co-doping strategy is also applicable to other transition metal oxide(NiO)with enhanced electrochemical performance.In addition,an asymmetric hybrid supercapacitor was assembled using the Cu0/Cu+co-doped CoO electrode and active carbon,which delivers a remarkable maximal energy density(35 Wh kg^(-1)),exceptional power density(16 kW kg^(-1))and ultralong cycle life(91.5%retention over 10,000 cycles).Theoretical calculations further verify that the co-doping of Cu^(0)/Cu^(+)can tune the electronic structure of CoO and improve the conductivity and electron transport.This study demonstrates a facile and favorable strategy to enhance the electrochemical performance of transition metal oxide electrode materials.展开更多
Layered LiCoO_(2)(LCO)acts as a dominant cathode material for lithium-ion batteries(LIBs)in 3C products because of its high compacted density and volumetric energy density.Although improving the high cutoff voltage is...Layered LiCoO_(2)(LCO)acts as a dominant cathode material for lithium-ion batteries(LIBs)in 3C products because of its high compacted density and volumetric energy density.Although improving the high cutoff voltage is an effective strategy to increase its capacity,such behavior would trigger rapid capacity decay due to the surface or/and structure degradation.Herein,we propose a bi-functional surface strategy involving constructing a robust spinel-like phase coating layer with great integrity and compatibility to LiCoO_(2) and modulating crystal lattice by anion and cation gradient co-doping at the subsurface.As a result,the modified LiCoO_(2)(AFM-LCO)shows a capacity retention of 80.9%after 500 cycles between 3.0and 4.6 V.The Al,F,Mg enriched spinel-like phase coating layer serves as a robust physical barrier to effectively inhibit the undesired side reactions between the electrolyte and the cathode.Meanwhile,the Al,F,Mg gradient co-doping significantly enhances the surficial structure stability,suppresses Co dissolution and oxygen release,providing a stable path for Li-ions mobility all through the long-term cycles.Thus,the surface bi-functional strategy is an effective method to synergistically improve the electrochemical performances of LCO at a high cut-off voltage of 4.6 V.展开更多
Electrochemical reduction of CO_(2)(CERR)to value-added chemicals is an attractive strategy for greenhouse gas mitigation,and carbon recycles utilization.Conventional metal catalysts suffered from low durability and s...Electrochemical reduction of CO_(2)(CERR)to value-added chemicals is an attractive strategy for greenhouse gas mitigation,and carbon recycles utilization.Conventional metal catalysts suffered from low durability and sluggish kinetics impede the practical application.On the other hand,doped carbon materials recently demonstrate superior catalytic performance in CERR,which shows the potential to diminish the problems of metal catalysts to some extent.Herein,we present the design and fabrication of nitrogen(N),phosphorus(P)co-doped metal-free carbon materials as an efficient and stable electrocatalyst for reduction of CO_(2) to CO,which exhibits an excellent performance with a high faradaic efficiency of 92%(-0.55 V vs.RHE)and up to 24 h stability.A series of characterizations including TEM and XPS verified that nitrogen and phosphorous are successfully incorporated into the carbon matrix.Moreover,the comparisons between co-doping and single doping catalysts reveal that co-doping can significantly increase CERR performance.The improved catalytic activity is attributed to the synergetic effects between nitrogen and phosphorous dopants,which effectively modulate properties of the active site.The density functional theory(DFT)calculations were also performed to understand the synergy effects of dopants.It is revealed that the phosphorous doping can significantly lower the Gibbs free energy of COOH^(*)formation.Moreover,the introduction of the second dopants phosphorous can reduce the reaction barrier along the reaction path and cause polarization of density of states at the Fermi level.These changes can greatly enhance the activity of the catalysts.From a combined experimental and computational exploration,current work provides valuable insights into the reaction mechanism of CERR on N,P co-doped carbon catalysts,and the influence from synergy effects between dopants,which paves the way for the rational design of novel metal-free catalysts for CO2 electro-reduction.展开更多
Using the first-principles calculations, we investigate the electronic band structure and the quantum transport properties of metallic carbon nanotubes (MCNTs) with B/N pair co-doping. The results about formation en...Using the first-principles calculations, we investigate the electronic band structure and the quantum transport properties of metallic carbon nanotubes (MCNTs) with B/N pair co-doping. The results about formation energy show that the B/N pair co-doping configuration is a most stable structure. We find that the electronic structure and the transport properties are very sensitive to the doping concentration of the B/N pairs in MCNTs, where the energy gaps increase with doping concentration increasing both along the tube axis and around the tube, because the mirror symmetry of MCNT is broken by doping B/N pairs. In addition, we discuss conductance dips of the transmission spectrum of doped MCNTs. These unconventional doping effects could be used to design novel nanoelectronic devices.展开更多
The Ni-ultrahigh cathode material is one of the best choices for further increasing energy-density of lithium-ion batteries(LIBs),but they generally suffer from the poor structure stability and rapid capacity fade.Her...The Ni-ultrahigh cathode material is one of the best choices for further increasing energy-density of lithium-ion batteries(LIBs),but they generally suffer from the poor structure stability and rapid capacity fade.Herein,the tungsten and phosphate polyanion co-doped LiNi_(0.9)Co_(0.1)O_(2)cathode materials are successfully fabricated in terms of Li(Ni_(0.9)Co_(0.7))_(1-x)W_(x)O_(2-4y)(PO_(4))_(y) by the precursor modification and subsequent annealing.The higher bonding energy of W—O(672 kJ·mol^(-1))can extremely stabilize the lattice oxygen of Ni-rich oxides compared with Ni—O(391.6 kJ·mol^(-1))and Co—O(368 kJ·mol^(-1)).Meanwhile,the stronger bonding of Ni—(PO_(4)^(3-))vs.Ni—O could fix Ni cations in the transition metal layer,and hence suppressing the Li/Ni disorder during the charge/discharge process.Therefore,the optimized Li(Ni_(0.9)Co_(0.1))_(0.99)W_(0.01)O_(1.96)(PO_4)_(0.01)delivers a remarkably extended cycling life with 95.1%retention of its initial capacity of 207.4 mA·h·g^(-1)at 0.2 C after 200 cycles.Meantime,the heteroatoms doping does not sacrifice the specific capacity even at different rates.展开更多
Brain plasticity-A universal tool with many variations:The study of brain plasticity has been gaining interest since almost a century and has now reached a huge amount of information(>80,000 results in PubMed).Over...Brain plasticity-A universal tool with many variations:The study of brain plasticity has been gaining interest since almost a century and has now reached a huge amount of information(>80,000 results in PubMed).Overall,different types of plasticity,including stem cell-driven genesis of new neurons(adult neurogenesis),cells in arrested maturation(dormant neurons),neuro-glial and synaptic plasticity,can coexist and contribute to grant plastic changes in the brain,from a cellular to system level(Benedetti and Couillard-Despres,2022;Bonfanti et al.,2023).展开更多
The p-type doping efficiency of 4 H silicon carbide(4 H-SiC)is rather low due to the large ionization energies of p-type dopants.Such an issue impedes the exploration of the full advantage of 4 H-SiC for semiconductor...The p-type doping efficiency of 4 H silicon carbide(4 H-SiC)is rather low due to the large ionization energies of p-type dopants.Such an issue impedes the exploration of the full advantage of 4 H-SiC for semiconductor devices.In this study,we show that co-doping group-IVB elements effectively decreases the ionization energy of the most widely used p-type dopant,i.e.,aluminum(Al),through the defect-level repulsion between the energy levels of group-IVB elements and that of Al in 4 H-SiC.Among group-IVB elements Ti has the most prominent effectiveness.Ti decreases the ionization energy of Al by nearly 50%,leading to a value as low as~0.13 eV.As a result,the ionization rate of Al with Ti co-doping is up to~5 times larger than that without co-doping at room temperature when the doping concentration is up to 10^(18)cm^(-3).This work may encourage the experimental co-doping of group-IVB elements such as Ti and Al to significantly improve the p-type doping efficiency of 4 H-SiC.展开更多
Lithium (Li) metal batteries have attracted much attention owing to its ultra-high energy density.However,as important part of Li metal batteries,Li anodes still face many challenges,mainly including uncontrolled dend...Lithium (Li) metal batteries have attracted much attention owing to its ultra-high energy density.However,as important part of Li metal batteries,Li anodes still face many challenges,mainly including uncontrolled dendritic Li formation,dramatical volume variation and serious pulverization.Herein,manganese dioxide (MnO_(2)) nanosheet modified nitrogen (N),phosphorus (P) co-doping carbon nanofibers(NPC) on carbon cloth (CC)(MnO_(2)@NPC-CC) is successfully fabricated through electrodeposition approach and further treated with Li by the molten-infusion method to prepare Li based Mn@NPC-CC(Li-Mn@NPC-CC) electrode.The synergy of MnO_(2) and NPC obviously increases the reaction rate between MnO_(2)@NPC-CC and Li and guides even Li distribution over infusion process.Additionally,theoretical calculation,simulation and experimental results further indicate that N,P,Mn multi-doping effectively improves the superior lithiophilicity of Li-Mn@NPC-CC,which induces uniform Li deposition/dissolution to suppress dendrite growth over cycles.Moreover,conductive and porous NPC matrix not only effectively improves the stability of Li-Mn@NPC-CC,but also provides abundant spaces to accelerate the transfer of ion/electron and buffer electrode dimension variation during cycling.Hence,Li-Mn@NPC-CC-based symmetric cells exhibit extra-long cycling life (over 2200 h) with small hysteresis of 20 mV.When the LiMn@NPC-CC anode couples with air,Li iron phosphate (LiFePO_(4)),or hard carbon (C) cathode,the assembled full cells exhibit outstanding performance with low hysteresis and stable cycling properties.Especially,the corresponding pouch-typed Li–air cells also exhibit good performance at different bending angles and even power a series of electronic devices.展开更多
Developing effective and long-term treatment strategies for rare and complex neurodegenerative diseases is challenging. One of the major roadblocks is the extensive heterogeneity among patients. This hinders understan...Developing effective and long-term treatment strategies for rare and complex neurodegenerative diseases is challenging. One of the major roadblocks is the extensive heterogeneity among patients. This hinders understanding the underlying disease-causing mechanisms and building solutions that have implications for a broad spectrum of patients. One potential solution is to develop personalized medicine approaches based on strategies that target the most prevalent cellular events that are perturbed in patients. Especially in patients with a known genetic mutation, it may be possible to understand how these mutations contribute to problems that lead to neurodegeneration. Protein–protein interaction analyses offer great advantages for revealing how proteins interact, which cellular events are primarily involved in these interactions, and how they become affected when key genes are mutated in patients. This line of investigation also suggests novel druggable targets for patients with different mutations. Here, we focus on alsin and spastin, two proteins that are identified as “causative” for amyotrophic lateral sclerosis and hereditary spastic paraplegia, respectively, when mutated. Our review analyzes the protein interactome for alsin and spastin, the canonical pathways that are primarily important for each protein domain, as well as compounds that are either Food and Drug Administration–approved or are in active clinical trials concerning the affected cellular pathways. This line of research begins to pave the way for personalized medicine approaches that are desperately needed for rare neurodegenerative diseases that are complex and heterogeneous.展开更多
Amyotrophic lateral sclerosis(ALS)is a neuromuscular condition resulting from the progressive degeneration of motor neurons in the cortex,brainstem,and spinal cord.While the typical clinical phenotype of ALS involves ...Amyotrophic lateral sclerosis(ALS)is a neuromuscular condition resulting from the progressive degeneration of motor neurons in the cortex,brainstem,and spinal cord.While the typical clinical phenotype of ALS involves both upper and lower motor neurons,human and animal studies over the years have highlighted the potential spread to other motor and non-motor regions,expanding the phenotype of ALS.Although superoxide dismutase 1(SOD1)mutations represent a minority of ALS cases,the SOD1 gene remains a milestone in ALS research as it represents the first genetic target for personalized therapies.Despite numerous single case reports or case series exhibiting extramotor symptoms in patients with ALS mutations in SOD1(SOD1-ALS),no studies have comprehensively explored the full spectrum of extramotor neurological manifestations in this subpopulation.In this narrative review,we analyze and discuss the available literature on extrapyramidal and non-motor features during SOD1-ALS.The multifaceted expression of SOD1 could deepen our understanding of the pathogenic mechanisms,pointing towards a multidisciplinary approach for affected patients in light of new therapeutic strategies for SOD1-ALS.展开更多
A series of photocatalysts of un-doped, single-doped and co-doped nanometer titanium diox- ide (TiO2) have been successfully prepared by template method using Fe(NO3)3.9H2O, La(NO3)3.6H2O, and tetrabutyl titanat...A series of photocatalysts of un-doped, single-doped and co-doped nanometer titanium diox- ide (TiO2) have been successfully prepared by template method using Fe(NO3)3.9H2O, La(NO3)3.6H2O, and tetrabutyl titanate as precursors and glucan as template. Scanning electron microscopy, X-ray diffraction, and N2 adsorption-desorption measurement were employed to characterize the morphology, crystal structure and surface structure of the samples. The photo-absorbance of the obtained catalysts was measured by UV-Vis absorption spectroscopy, and the photocatalytic activities of the prepared samples under UV and visible light were estimated by measuring the degradation rate of methyl orange in an aqueous solution. The characterizations indicated that the prepared photocatalysts consisted of anatase phase and possessed high surface area of ca. 163-176 m2/g. It was shown that the Fe and La co-doped nano-TiO2 could be activated by visible light and could thus be used as an effective catalyst in photo-oxidation reactions. The synergistic effect of Fe and La co-doping played an important role in improving the photocatalytic activity. In addition, the possibility of cyclic usage of co-doped nano-TiO2 was also confirmed, the photocatalytic activity of codoped nano-TiO2 remained above 89.6% of the fresh sample after being used four times.展开更多
In order to improve the photocatalytic performance of mesoporous titania under visible light, a series of photocatalysts of S and Ag co-doped mesoporous titania have been successfully prepared by template method using...In order to improve the photocatalytic performance of mesoporous titania under visible light, a series of photocatalysts of S and Ag co-doped mesoporous titania have been successfully prepared by template method using thiourea, AgNO3 and tetrabutyl titanate as precursors and Pluronic P123 (EO20PO70EO20) as template. Scanning electron microscopy (SEM), X-ray diffraction (XRD), nitrogen adsorption-desorption measurements, and UV-visible spectroscopy (UV-Vis) were employed to characterize the morphology, crystal structure, surface structure, and optical absorption properties of the samples. The microcrystal of the photocatalysts consisted of anatase phase and was approximately present in the form of spherical particle. The photocatalytic performance was studied by photodegradation methyl orange (MO) in water under UV and visible light irradiation. The calcination temperature and the doping content influenced the photoactivity. In addition, the possibility of cyclic usage of co-doped mesoporous titania was also confirmed, the photocatalytic activity of mesoporous titania remained above 89% of that of the fresh sample after being used four times. It was shown that the co-doped mesoporous titania could be activated by visible light and could thus be potentially applied for the treatment of water contaminated by organic pollutants. The synergistic effect of sulfur and silver co-doping played an important role in improving the photocatalytic activity.展开更多
基金supported by the National High Technology Research and Development Program of China under Grant No2007AA032120the National Natural Science Foundation of China under Grant No 60777043
文摘A new sol-gel process is applied to fabricate the BST (BaxSr1-xTiO3) sol and nano-powder of La-Mn-Al co-doping with Ba/Sr ratio 65/35, and the BST thick film is prepared in the Pt/Ti/SiO2/Si substrate. The powder and thick film are characterized by X-ray diffraction and transmission electron microscope. The influence of La-Mn-Al co-doping on the dielectric properties and micro-structure of BST thick film is analyzed. The results show that the La, Mn, and Al ions can take an obvious restraint on the growth of BaSrTiO3 grains. The polycrystalline particles come into being during the crystallization of thick film, which may improve the uniformity and compactness of thick film. The influence of unequal-valence and doping amount on the leakage current, dielectric loss, and dielectric property are mainly discussed. The dielectric constant and dielectric loss of thick film are 1200 and 0.03, respectively, in the case of 1mol% La doping, 2mol% Mn doping, and 1mol% Al doping.
基金financially supported by the National Natural Science Foundation of China(Nos.51602018 and 51902018)the Natural Science Foundation of Beijing Municipality(No.2154052)+3 种基金the China Postdoctoral Science Foundation(No.2014M560044)the Fundamental Research Funds for the Central Universities(No.FRF-MP-20-22)USTB Research Center for International People-to-people Exchange in Science,Technology and Civilization(No.2022KFYB007)Education and Teaching Reform Foundation at University of Science and Technology Beijing(Nos.2023JGC027,KC2022QYW06,and KC2022TS09)。
文摘S and Co co-doped carbon catalysts were prepared via pyrolysis of MOF-71 and thiourea mixtures at 800℃at a mass ratio of MOF-71 to thiourea of 1:0.1 to effectively activate peroxymonosulfate(PMS)for methylene blue(MB)degradation.The effects of two different mixing routes were identified on the MB degradation performance.Particularly,the catalyst obtained by the alcohol solvent evaporation(MOF-AEP)mixing route could degrade 95.60%MB(50 mg/L)within 4 min(degradation rate:K=0.78 min^(-1)),which was faster than that derived from the direct grinding method(MOF-DGP,80.97%,K=0.39 min^(-1)).X-ray photoelectron spectroscopy revealed that the Co-S content of MOF-AEP(43.39at%)was less than that of MOF-DGP(54.73at%),and the proportion of C-S-C in MOF-AEP(13.56at%)was higher than that of MOF-DGP(10.67at%).Density functional theory calculations revealed that the adsorption energy of Co for PMS was -2.94 eV when sulfur was doped as C-S-C on the carbon skeleton,which was higher than that when sulfur was doped next to cobalt in the form of Co-S bond(-2.86 eV).Thus,the C-S-C sites might provide more contributions to activate PMS compared with Co-S.Furthermore,the degradation parameters,including pH and MOF-AEP dosage,were investigated.Finally,radical quenching experiments and electron paramagnetic resonance(EPR)measurements revealed that ^(1)O_(2)might be the primary catalytic species,whereas·O~(2-)might be the secondary one in degrading MB.
基金the financial support from the National Natural Science Foundation of China(51972156,52072378,52102054 and 51927803)the National Key R&D Program of China(2022YFB3803400,2021YFB3800301)+2 种基金the Shenyang Science and Technology Program(22-322-3-19)the Youth Fund of the Education Department of Liaoning Province(LJKQZ20222324)the Outstanding Youth Fund of University of Science and Technology Liaoning(2023YQ11).
文摘Ni-rich layered oxide cathodes have shown promise for high-energy lithium-ion batteries(LIBs)but are usually limited to mild environments because of their rapid performance degradation under extreme temperature conditions(below0°C and above 50 °C).Here,we report the design of F/Mo co-doped LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(FMNCM)cathode for high-performance LIBs from-20 to 60°C.F^(-) doping with high electronegativity into the cathode surface is found to enhance the stability of surface lattice structure and protect the interface from side reactions with the electrolyte by generating a LiF-rich surface layer.Concurrently,the Mo^(6+) doping suppresses phase transition,which blocks Li^(+)/Ni^(2+) mixing,and stabilizes lithium-ion diffusion pathway.Remarkably,the FMNCM cathode demonstrates excellent cycling stability at a high cutoff voltage of 4.4 V,even at 60°C,maintaining 90.6%capacity retention at 3 C after 150 cycles.Additionally,at temperatures as low as-20°C,it retains 77.1%of its room temperature capacity,achieving an impressive 97.5%capacity retention after 500 cycles.Such stable operation under wide temperatures has been further validated in practical Ah-level pouch-cells.This study sheds light on both fundamental mechanisms and practical implications for the design of advanced cathode materials for wide-temperature LIBs,presenting a promising path towards high-energy and long-cycling LIBs with temperatureadaptability.
基金supported by the National Natural Science Foundation of China(22265021)the Aeronautical Science Foundation of China(2020Z056056003)Jiangxi Provincial Natural Science Foundation(20232BAB212004).
文摘Atomic-scale doping strategies and structure design play pivotal roles in tailoring the electronic structure and physicochemical property of electromagnetic wave absorption(EMWA)materials.However,the relationship between configuration and electromagnetic(EM)loss mechanism has remained elusive.Herein,drawing inspiration from the DNA transcription process,we report the successful synthesis of novel in situ Mn/N co-doped helical carbon nanotubes with ultrabroad EMWA capability.Theoretical calculation and EM simulation confirm that the orbital coupling and spin polarization of the Mn–N4–C configuration,along with cross polarization generated by the helical structure,endow the helical converters with enhanced EM loss.As a result,HMC-8 demonstrates outstanding EMWA performance,achieving a minimum reflection loss of−63.13 dB at an ultralow thickness of 1.29 mm.Through precise tuning of the graphite domain size,HMC-7 achieves an effective absorption bandwidth(EAB)of 6.08 GHz at 2.02 mm thickness.Furthermore,constructing macroscale gradient metamaterials enables an ultrabroadband EAB of 12.16 GHz at a thickness of only 5.00 mm,with the maximum radar cross section reduction value reaching 36.4 dB m2.This innovative approach not only advances the understanding of metal–nonmetal co-doping but also realizes broadband EMWA,thus contributing to the development of EMWA mechanisms and applications.
基金financially supported by the National Science Foundation of China(Grant No.11804106)。
文摘Although CoO is a promising electrode material for supercapacitors due to its high theoretical capacitance,the practical applications still suffering from inferior electrochemical activity owing to its low electrical conductivity,poor structural stability and inefficient nanostructure.Herein,we report a novel Cu0/Cu+co-doped CoO composite with adjustable metallic Cu0 and ion Cu+via a facile strategy.Through interior(Cu+)and exterior(Cu0)decoration of CoO,the electrochemical performance of CoO electrode has been significantly improved due to both the beneficial flower-like nanostructure and the synergetic effect of Cu0/Cu+co-doping,which results in a significantly enhanced specific capacitance(695 F g^(-1) at 1 A g^(-1))and high cyclic stability(93.4%retention over 10,000 cycles)than pristine CoO.Furthermore,this co-doping strategy is also applicable to other transition metal oxide(NiO)with enhanced electrochemical performance.In addition,an asymmetric hybrid supercapacitor was assembled using the Cu0/Cu+co-doped CoO electrode and active carbon,which delivers a remarkable maximal energy density(35 Wh kg^(-1)),exceptional power density(16 kW kg^(-1))and ultralong cycle life(91.5%retention over 10,000 cycles).Theoretical calculations further verify that the co-doping of Cu^(0)/Cu^(+)can tune the electronic structure of CoO and improve the conductivity and electron transport.This study demonstrates a facile and favorable strategy to enhance the electrochemical performance of transition metal oxide electrode materials.
基金supported by the National Natural Science Foundation of China(22075170,52072233)the Beijing National Laboratory for Condensed Matter Physics。
文摘Layered LiCoO_(2)(LCO)acts as a dominant cathode material for lithium-ion batteries(LIBs)in 3C products because of its high compacted density and volumetric energy density.Although improving the high cutoff voltage is an effective strategy to increase its capacity,such behavior would trigger rapid capacity decay due to the surface or/and structure degradation.Herein,we propose a bi-functional surface strategy involving constructing a robust spinel-like phase coating layer with great integrity and compatibility to LiCoO_(2) and modulating crystal lattice by anion and cation gradient co-doping at the subsurface.As a result,the modified LiCoO_(2)(AFM-LCO)shows a capacity retention of 80.9%after 500 cycles between 3.0and 4.6 V.The Al,F,Mg enriched spinel-like phase coating layer serves as a robust physical barrier to effectively inhibit the undesired side reactions between the electrolyte and the cathode.Meanwhile,the Al,F,Mg gradient co-doping significantly enhances the surficial structure stability,suppresses Co dissolution and oxygen release,providing a stable path for Li-ions mobility all through the long-term cycles.Thus,the surface bi-functional strategy is an effective method to synergistically improve the electrochemical performances of LCO at a high cut-off voltage of 4.6 V.
基金supported by the National Natural Science Foundation of China(21573255,21573062)Natural Science Foundation of Liao Ning Province(20180510014)+1 种基金supported by Joint Research Fund Liaoning-Shenyang National Laboratory for Materials Science and the State Key Laboratory of Catalytic Materials and Reaction Engineering(RIPP,SINOPEC)supported by the Special Program for Applied Research on Super Computation of the NSFC Guangdong Joint Fund(the second phase)under Grant No.U1501501。
文摘Electrochemical reduction of CO_(2)(CERR)to value-added chemicals is an attractive strategy for greenhouse gas mitigation,and carbon recycles utilization.Conventional metal catalysts suffered from low durability and sluggish kinetics impede the practical application.On the other hand,doped carbon materials recently demonstrate superior catalytic performance in CERR,which shows the potential to diminish the problems of metal catalysts to some extent.Herein,we present the design and fabrication of nitrogen(N),phosphorus(P)co-doped metal-free carbon materials as an efficient and stable electrocatalyst for reduction of CO_(2) to CO,which exhibits an excellent performance with a high faradaic efficiency of 92%(-0.55 V vs.RHE)and up to 24 h stability.A series of characterizations including TEM and XPS verified that nitrogen and phosphorous are successfully incorporated into the carbon matrix.Moreover,the comparisons between co-doping and single doping catalysts reveal that co-doping can significantly increase CERR performance.The improved catalytic activity is attributed to the synergetic effects between nitrogen and phosphorous dopants,which effectively modulate properties of the active site.The density functional theory(DFT)calculations were also performed to understand the synergy effects of dopants.It is revealed that the phosphorous doping can significantly lower the Gibbs free energy of COOH^(*)formation.Moreover,the introduction of the second dopants phosphorous can reduce the reaction barrier along the reaction path and cause polarization of density of states at the Fermi level.These changes can greatly enhance the activity of the catalysts.From a combined experimental and computational exploration,current work provides valuable insights into the reaction mechanism of CERR on N,P co-doped carbon catalysts,and the influence from synergy effects between dopants,which paves the way for the rational design of novel metal-free catalysts for CO2 electro-reduction.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.10325415 and 50504017)the Natural Science Foundation of Hunan Province,China(Grant No.07JJ3102)+1 种基金the Scientific Research Fund of Hunan Provincial Education Department,China(Grant No.10C1171)the Science Development Foundation of Central South University,China(Grant Nos.08SDF02 and 09SDF09)
文摘Using the first-principles calculations, we investigate the electronic band structure and the quantum transport properties of metallic carbon nanotubes (MCNTs) with B/N pair co-doping. The results about formation energy show that the B/N pair co-doping configuration is a most stable structure. We find that the electronic structure and the transport properties are very sensitive to the doping concentration of the B/N pairs in MCNTs, where the energy gaps increase with doping concentration increasing both along the tube axis and around the tube, because the mirror symmetry of MCNT is broken by doping B/N pairs. In addition, we discuss conductance dips of the transmission spectrum of doped MCNTs. These unconventional doping effects could be used to design novel nanoelectronic devices.
基金supported by the National Natural Science Foundation of China(91834301)the Innovation Program of Shanghai Municipal Education Commission+1 种基金the Shanghai Scientific and Technological Innovation Project(18JC1410500)the Fundamental Research Funds for the Central Universities(222201718002)。
文摘The Ni-ultrahigh cathode material is one of the best choices for further increasing energy-density of lithium-ion batteries(LIBs),but they generally suffer from the poor structure stability and rapid capacity fade.Herein,the tungsten and phosphate polyanion co-doped LiNi_(0.9)Co_(0.1)O_(2)cathode materials are successfully fabricated in terms of Li(Ni_(0.9)Co_(0.7))_(1-x)W_(x)O_(2-4y)(PO_(4))_(y) by the precursor modification and subsequent annealing.The higher bonding energy of W—O(672 kJ·mol^(-1))can extremely stabilize the lattice oxygen of Ni-rich oxides compared with Ni—O(391.6 kJ·mol^(-1))and Co—O(368 kJ·mol^(-1)).Meanwhile,the stronger bonding of Ni—(PO_(4)^(3-))vs.Ni—O could fix Ni cations in the transition metal layer,and hence suppressing the Li/Ni disorder during the charge/discharge process.Therefore,the optimized Li(Ni_(0.9)Co_(0.1))_(0.99)W_(0.01)O_(1.96)(PO_4)_(0.01)delivers a remarkably extended cycling life with 95.1%retention of its initial capacity of 207.4 mA·h·g^(-1)at 0.2 C after 200 cycles.Meantime,the heteroatoms doping does not sacrifice the specific capacity even at different rates.
基金supported by Progetto Trapezio,Compagnia di San Paolo(67935-2021.2174)to LB,Fondazione CRT(Cassa di Risparmio di Torino,RF=2022.0618)to LB。
文摘Brain plasticity-A universal tool with many variations:The study of brain plasticity has been gaining interest since almost a century and has now reached a huge amount of information(>80,000 results in PubMed).Overall,different types of plasticity,including stem cell-driven genesis of new neurons(adult neurogenesis),cells in arrested maturation(dormant neurons),neuro-glial and synaptic plasticity,can coexist and contribute to grant plastic changes in the brain,from a cellular to system level(Benedetti and Couillard-Despres,2022;Bonfanti et al.,2023).
基金Project supported by the National Key Research and Development Program of China(Grant Nos.2017YFA0205704 and 2018YFB2200101)the National Natural Science Foundation of China(Grant Nos.91964107 and 61774133)+2 种基金Fundamental Research Funds for the Central Universities,China(Grant No.2018XZZX003-02)the National Natural Science Foundation of China for Innovative Research Groups(Grant No.61721005)Zhejiang University Education Foundation Global Partnership Fund。
文摘The p-type doping efficiency of 4 H silicon carbide(4 H-SiC)is rather low due to the large ionization energies of p-type dopants.Such an issue impedes the exploration of the full advantage of 4 H-SiC for semiconductor devices.In this study,we show that co-doping group-IVB elements effectively decreases the ionization energy of the most widely used p-type dopant,i.e.,aluminum(Al),through the defect-level repulsion between the energy levels of group-IVB elements and that of Al in 4 H-SiC.Among group-IVB elements Ti has the most prominent effectiveness.Ti decreases the ionization energy of Al by nearly 50%,leading to a value as low as~0.13 eV.As a result,the ionization rate of Al with Ti co-doping is up to~5 times larger than that without co-doping at room temperature when the doping concentration is up to 10^(18)cm^(-3).This work may encourage the experimental co-doping of group-IVB elements such as Ti and Al to significantly improve the p-type doping efficiency of 4 H-SiC.
基金funding support from the National Natural Science Foundation of China (21905151 and 51772162)the Youth Innovation and Technology Foundation of Shandong Higher Education Institutions, China (2019KJC004)+1 种基金the Outstanding Youth Foundation of Shandong Province, China (ZR2019JQ14)the Taishan Scholar Young Talent Program, Major Scientific and Technological Innovation Project (2019JZZY020405)。
文摘Lithium (Li) metal batteries have attracted much attention owing to its ultra-high energy density.However,as important part of Li metal batteries,Li anodes still face many challenges,mainly including uncontrolled dendritic Li formation,dramatical volume variation and serious pulverization.Herein,manganese dioxide (MnO_(2)) nanosheet modified nitrogen (N),phosphorus (P) co-doping carbon nanofibers(NPC) on carbon cloth (CC)(MnO_(2)@NPC-CC) is successfully fabricated through electrodeposition approach and further treated with Li by the molten-infusion method to prepare Li based Mn@NPC-CC(Li-Mn@NPC-CC) electrode.The synergy of MnO_(2) and NPC obviously increases the reaction rate between MnO_(2)@NPC-CC and Li and guides even Li distribution over infusion process.Additionally,theoretical calculation,simulation and experimental results further indicate that N,P,Mn multi-doping effectively improves the superior lithiophilicity of Li-Mn@NPC-CC,which induces uniform Li deposition/dissolution to suppress dendrite growth over cycles.Moreover,conductive and porous NPC matrix not only effectively improves the stability of Li-Mn@NPC-CC,but also provides abundant spaces to accelerate the transfer of ion/electron and buffer electrode dimension variation during cycling.Hence,Li-Mn@NPC-CC-based symmetric cells exhibit extra-long cycling life (over 2200 h) with small hysteresis of 20 mV.When the LiMn@NPC-CC anode couples with air,Li iron phosphate (LiFePO_(4)),or hard carbon (C) cathode,the assembled full cells exhibit outstanding performance with low hysteresis and stable cycling properties.Especially,the corresponding pouch-typed Li–air cells also exhibit good performance at different bending angles and even power a series of electronic devices.
基金funded by NIH-NIA R01AG061708 (to PHO)Patrick Grange Memorial Foundation (to PHO)+1 种基金A Long Swim (to PHO)CureSPG4 Foundation (to PHO)。
文摘Developing effective and long-term treatment strategies for rare and complex neurodegenerative diseases is challenging. One of the major roadblocks is the extensive heterogeneity among patients. This hinders understanding the underlying disease-causing mechanisms and building solutions that have implications for a broad spectrum of patients. One potential solution is to develop personalized medicine approaches based on strategies that target the most prevalent cellular events that are perturbed in patients. Especially in patients with a known genetic mutation, it may be possible to understand how these mutations contribute to problems that lead to neurodegeneration. Protein–protein interaction analyses offer great advantages for revealing how proteins interact, which cellular events are primarily involved in these interactions, and how they become affected when key genes are mutated in patients. This line of investigation also suggests novel druggable targets for patients with different mutations. Here, we focus on alsin and spastin, two proteins that are identified as “causative” for amyotrophic lateral sclerosis and hereditary spastic paraplegia, respectively, when mutated. Our review analyzes the protein interactome for alsin and spastin, the canonical pathways that are primarily important for each protein domain, as well as compounds that are either Food and Drug Administration–approved or are in active clinical trials concerning the affected cellular pathways. This line of research begins to pave the way for personalized medicine approaches that are desperately needed for rare neurodegenerative diseases that are complex and heterogeneous.
文摘Amyotrophic lateral sclerosis(ALS)is a neuromuscular condition resulting from the progressive degeneration of motor neurons in the cortex,brainstem,and spinal cord.While the typical clinical phenotype of ALS involves both upper and lower motor neurons,human and animal studies over the years have highlighted the potential spread to other motor and non-motor regions,expanding the phenotype of ALS.Although superoxide dismutase 1(SOD1)mutations represent a minority of ALS cases,the SOD1 gene remains a milestone in ALS research as it represents the first genetic target for personalized therapies.Despite numerous single case reports or case series exhibiting extramotor symptoms in patients with ALS mutations in SOD1(SOD1-ALS),no studies have comprehensively explored the full spectrum of extramotor neurological manifestations in this subpopulation.In this narrative review,we analyze and discuss the available literature on extrapyramidal and non-motor features during SOD1-ALS.The multifaceted expression of SOD1 could deepen our understanding of the pathogenic mechanisms,pointing towards a multidisciplinary approach for affected patients in light of new therapeutic strategies for SOD1-ALS.
文摘A series of photocatalysts of un-doped, single-doped and co-doped nanometer titanium diox- ide (TiO2) have been successfully prepared by template method using Fe(NO3)3.9H2O, La(NO3)3.6H2O, and tetrabutyl titanate as precursors and glucan as template. Scanning electron microscopy, X-ray diffraction, and N2 adsorption-desorption measurement were employed to characterize the morphology, crystal structure and surface structure of the samples. The photo-absorbance of the obtained catalysts was measured by UV-Vis absorption spectroscopy, and the photocatalytic activities of the prepared samples under UV and visible light were estimated by measuring the degradation rate of methyl orange in an aqueous solution. The characterizations indicated that the prepared photocatalysts consisted of anatase phase and possessed high surface area of ca. 163-176 m2/g. It was shown that the Fe and La co-doped nano-TiO2 could be activated by visible light and could thus be used as an effective catalyst in photo-oxidation reactions. The synergistic effect of Fe and La co-doping played an important role in improving the photocatalytic activity. In addition, the possibility of cyclic usage of co-doped nano-TiO2 was also confirmed, the photocatalytic activity of codoped nano-TiO2 remained above 89.6% of the fresh sample after being used four times.
基金This work was supported by the National Natural Sci- ence Foundation of China (No.41373127) and the Liaoning Provincial Natural Science Foundation of China (No.2013020121).
文摘In order to improve the photocatalytic performance of mesoporous titania under visible light, a series of photocatalysts of S and Ag co-doped mesoporous titania have been successfully prepared by template method using thiourea, AgNO3 and tetrabutyl titanate as precursors and Pluronic P123 (EO20PO70EO20) as template. Scanning electron microscopy (SEM), X-ray diffraction (XRD), nitrogen adsorption-desorption measurements, and UV-visible spectroscopy (UV-Vis) were employed to characterize the morphology, crystal structure, surface structure, and optical absorption properties of the samples. The microcrystal of the photocatalysts consisted of anatase phase and was approximately present in the form of spherical particle. The photocatalytic performance was studied by photodegradation methyl orange (MO) in water under UV and visible light irradiation. The calcination temperature and the doping content influenced the photoactivity. In addition, the possibility of cyclic usage of co-doped mesoporous titania was also confirmed, the photocatalytic activity of mesoporous titania remained above 89% of that of the fresh sample after being used four times. It was shown that the co-doped mesoporous titania could be activated by visible light and could thus be potentially applied for the treatment of water contaminated by organic pollutants. The synergistic effect of sulfur and silver co-doping played an important role in improving the photocatalytic activity.