The design of cost-effective and efficient metal-free carbon-based catalysts for the hydrogen evolution reaction(HER)is of great significance for increasing the production of clean hydrogen by the electrolysis of alka...The design of cost-effective and efficient metal-free carbon-based catalysts for the hydrogen evolution reaction(HER)is of great significance for increasing the production of clean hydrogen by the electrolysis of alkaline water.Precise control of the electronic structure by heteroatom doping has proven to be efficient for increasing catalytic activity.Nevertheless,both the structural characteristics and the underlying mechanism are not well understood,especially for doping with two different atoms,thus limiting the use of these catalysts.We report the production of phosphorus and nitrogen co-doped hollow carbon nanospheres(HCNs)by the copolymerization of pyrrole and aniline at a Triton X-100 micelle-interface,followed by doping with phytic acid and carbonization.The unique pore structure and defect-rich framework of the HCNs expose numerous active sites.Crucially,the combined effect of graphitic nitrogen and phosphorus-carbon bonds modulate the local electronic structure of adjacent C atoms and facilitates electron transfer.As a res-ult,the HCN carbonized at 1100°C exhibited superior HER activity and an outstanding stability(70 h at a current density of 10 mA cm^(−2))in alkaline water,because of the large number of graphitic nitrogen and phosphorus-carbon bonds.展开更多
To realize the application of electromagnetic wave absorption(EWA)devices in humid marine environments,bifunctional EWA materials with better EWA capacities and anticorrosion properties have great exploration signific...To realize the application of electromagnetic wave absorption(EWA)devices in humid marine environments,bifunctional EWA materials with better EWA capacities and anticorrosion properties have great exploration significance and systematic research re-quirements.By utilizing the low-cost and excellent magnetic and stable chemical characteristics of barium ferrite(BaFe_(12)O_(19))and using the high dielectric loss and excellent chemical inertia of nanocarbon clusters,a new type of nanocomposites with carbon nanoclusters en-capsulating BaFe_(12)O_(19)was designed and synthesized by combining an impregnation method and a high-temperature calcination strategy.Furthermore,Ce-Mn ions were introduced into the BaFe_(12)O_(19)lattice to improve the dielectric and magnetic properties of BaFe_(12)O_(19)cores significantly,and the energy band structure of the doped lattice and the orders of Ce replacing Fe sites were calculated.Benefiting from Ce-Mn ion doping and carbon nanocluster encapsulation,the composite material exhibited excellent dual functionality of corrosion resist-ance and EWA.When BaCe_(0.2)Mn_(0.3)Fe_(11.5)O_(19)-C(BCM-C)was calcined at 600°C,the minimum reflection loss of-20.1 dB was achieved at 14.43 GHz.The Ku band’s effective absorption bandwidth of 4.25 GHz was achieved at an absorber thickness of only 1.3 mm.The BCM-C/polydimethylsiloxane coating had excellent corrosion resistance in the simulated marine environment(3.5wt%NaCl solution).The|Z|0.01Hz value of BCM-C remained at 106Ω·cm^(2)after 12 soaking days.The successful preparation of the BaFe_(12)O_(19)composite en-capsulated with carbon nanoclusters provides new insights into the preparation of multifunctional absorbent materials and the fabrication of absorbent devices applied in humid marine environments in the future.展开更多
Herein,an external crosslinker facilitated the hypercrosslinking of ferrocene and a nitrogen heterocyclic compound(either melamine or imidazole)through a direct Friedel-Crafts reaction,which led to the formation of ni...Herein,an external crosslinker facilitated the hypercrosslinking of ferrocene and a nitrogen heterocyclic compound(either melamine or imidazole)through a direct Friedel-Crafts reaction,which led to the formation of nitrogen-containing hypercrosslinked fer-rocene polymer precursors(HCP-FCs).Subsequent carbonization of these precursors results in the production of iron-nitrogen-doped por-ous carbon absorbers(Fe-NPCs).The Fe-NPCs demonstrate a porous structure comprising aggregated nanotubes and nanospheres.The porosity of this structure can be modulated by adjusting the iron and nitrogen contents to optimize impedance matching.The uniform dis-tribution of Fe-N_(x)C,N dipoles,andα-Fe within the carbon matrix can be ensured by using hypercrosslinked ferrocenes in constructing porous carbon,providing the absorber with numerous polarization sites and a conductive network.The electromagnetic wave absorption performance of the specially designed Fe-NPC-M_(2)absorbers is satisfactory,revealing a minimum reflection loss of-55.3 dB at 2.5 mm and an effective absorption bandwidth of 6.00 GHz at 2.0 mm.By utilizing hypercrosslinked polymers(HCPs)as precursors,a novel method for developing highly efficient carbon-based absorbing agents is introduced in this research.展开更多
In recent years,metal phosphosulfides have attracted great attention as the promising anode materials in sodium/potassium batteries because of their incorporation of the advantages of metal phosphides and sulfides.How...In recent years,metal phosphosulfides have attracted great attention as the promising anode materials in sodium/potassium batteries because of their incorporation of the advantages of metal phosphides and sulfides.However,they are also confronted with the problem of unstable battery performance due to the heavy volume expansion and sluggish ion reaction kinetics.Herein,yolk-shell cobalt phosphosulfide nanocrystals encapsulating into multi-heterogeneous atom(N,P,S)-doped carbon framework(Co_(9)S_(8)/CoP@NPSC)were constructed by employing dodecahedral ZIF-67 as precursor and a polymer as carbon sources through simultaneous sulfidation and phosphorization processes.The synergistic effect of Co_(9)S_(8)and CoP component and the yolk-shell structure greatly improve the bettery performance and structural stability.In addition,the multiple hetero-atoms doped carbon frameworks enhance the conductivity of the electrode materials and increase the spacing of carbon layers to supply sufficient active sites and facilitate the Na^(+)/K^(+)transport.The electrochemical results demonstrated that Co_(9)S_(8)/CoP@NPSC exhibited the pleasant reversible capacity(360.47 mAh/g at 1 A/g)after 300 cycles and an unpredictable cycling stability(103.22 mAh/g after 1000 cycles)in the SIBs application.The ex-situ XRD and XPS analyses were further applied to study the sodium ion storage mechanism and the multi-step phase transition reaction of the yolk-shell heterogeneous structure.This work provides new perspectives for the preparation of novel structure metal phosphosulfide and their applications in anode materials for sodium/potassium batteries and other secondary batteries.展开更多
Thermoelectric water spitting to hydrogen systems has great potential in the production of environment-friendly fuel using renewable solar energy in the future.In this work,we prepared porous nanosheet Mo doping Ni_(5...Thermoelectric water spitting to hydrogen systems has great potential in the production of environment-friendly fuel using renewable solar energy in the future.In this work,we prepared porous nanosheet Mo doping Ni_(5)P_(4)catalysts on nickel foam with efficient hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)performance in alkaline media.Density Functional Theory(DFT)calculations and experimental studies have shown that Mo doping deadeneds the interaction between H and O atomic orbitals of transition state water molecules,effectively weakening the activation energy of H_(2)O dissociation.Therefore,Mo doping is favorable for enhancing HER activity with overpotential at 10 mA cm^(-2)of 93 mV and Tafel slope of 40.1 mV dec^(-1)in 1 M KOH.Besides,it exhibits high alkaline OER activity with an ultra-low overpotential of 200 mV at 10 mA cm^(-2).Moreover,this catalyst only needs 1.537 V in a dual-electrode configuration of the electrolytic cell,which is much lower than the commercial Pt/C-RuO_(2)couple(1.614 V).In addition,we have developed and constructed a solar thermoelectric generator(TEG)that is capable of floating on water.This TEG has a continuous power output and an exceptionally long lifespan,providing a stable power supply to the synthesized catalyst electrolyzer.It can produce a maximum power output of over 90 mW,meeting the requirement of converting solar radiation heat into usable electricity.As a result,the system achieves productivity of 0.11 mL min^(-1)H_(2).This solar thermal energy conversion technology shows the possibility of large-scale industrial production of H_(2)and provides a new idea for exploring heat source utilization.展开更多
Solid oxide electrolysis cells(SOECs)can effectively convert CO_(2)into high value-added CO fuel.In this paper,Sc-doped Sr_(2)Fe_(1.5)Mo_(0.3)Sc_(0.2)O_(6−δ)(SFMSc)perovskite oxide material is synthesized via solid-p...Solid oxide electrolysis cells(SOECs)can effectively convert CO_(2)into high value-added CO fuel.In this paper,Sc-doped Sr_(2)Fe_(1.5)Mo_(0.3)Sc_(0.2)O_(6−δ)(SFMSc)perovskite oxide material is synthesized via solid-phase method as the cathode for CO_(2)electrolysis by SOECs.XRD confirms that SFMSc exhibits a stable cubic phase crystal structure.The experimental results of TPD,TG,EPR,CO_(2)-TPD further demonstrate that Sc-doping increases the concentration of oxygen vacancy in the material and the chemical adsorption capacity of CO_(2)molecules.Electrochemical tests reveal that SFMSc single cell achieves a current density of 2.26 A/cm^(2) and a lower polarization impedance of 0.32Ω·cm^(2) at 800°C under the applied voltage of 1.8 V.And no significant performance attenuation or carbon deposition is observed after 80 h continuous long-term stability test.This study provides a favorable support for the development of SOEC cathode materials with good electro-catalytic performance and stability.展开更多
In this paper, we have demonstrated an Er-doped ultrafast laser with a single mode fiber-gradient index multimode fiber-single mode fiber(SMF-GIMF-SMF, SMS) structure as saturable absorber(SA), which can generate not ...In this paper, we have demonstrated an Er-doped ultrafast laser with a single mode fiber-gradient index multimode fiber-single mode fiber(SMF-GIMF-SMF, SMS) structure as saturable absorber(SA), which can generate not only stable single-pulse state, but also special mode-locked pulses with the characteristics of high energy and noisy behaviors at proper pump power and cavity polarization state. In addition, we have deeply investigated the real-time spectral evolutions of the mode-locked pulses through the dispersive Fourier transformation(DFT) technique. It can be found that the pulse regime can actually consist of a lot of small noise pulses with randomly varying intensities. We believe that these results will further enrich the nonlinear dynamical processes in the ultrafast lasers.展开更多
Nitrogen doping in chemical vapor deposition-derived ultrananocrystalline diamond(UNCD)films in-creases the electronic conductivity,yet its microstructural effects on electron transport are insufficiently understood.W...Nitrogen doping in chemical vapor deposition-derived ultrananocrystalline diamond(UNCD)films in-creases the electronic conductivity,yet its microstructural effects on electron transport are insufficiently understood.We investigated the formation of nitrogen-induced diaph-ite structures(hybrid diamond-graphite phases)and their role in changing the conductivity.Nitrogen doping in a hy-drogen-rich plasma environment promotes the emergence of unique sp^(3)-sp^(2)bonding interfaces,where diamond grains are covalently integrated with graphitic domains,facilitating a structure-driven electronic transition.High-resolution transmis-sion electron microscopy and selected area electron diffraction reveal five-fold,six-fold and twelve-fold symmetries,along with an atypical{200}crystallographic reflection,confirming diaphite formation in 5%and 10%N-doped UNCD films,while high-er doping levels(15%and 20%)result in extensive graphitization.Raman spectroscopy tracks the evolution of sp^(2)bonding with increasing nitrogen content,while atomic force microscopy and X-ray diffraction indicate a consistent diamond grain size of~8 nm.Cryogenic electronic transport measurements reveal a conductivity increase from 8.72 to 708 S/cm as the nitrogen dop-ing level increases from 5%to 20%,which is attributed to defect-mediated carrier transport and 3D weak localization.The res-ulting conductivity is three orders of magnitude higher than previously reported.These findings establish a direct correlation between diaphite structural polymorphism and tunable electronic properties in nitrogen-doped UNCD films,offering new ways for defect-engineering diamond-based electronic materials.展开更多
We used the natural product chamomile as a carbon source to synthesize praseodymium(Pr) and nitrogen(N) co-doped biomass carbon dots(Pr/N-BCDs) with remarkable luminescence properties by one-step hydrothermal method.C...We used the natural product chamomile as a carbon source to synthesize praseodymium(Pr) and nitrogen(N) co-doped biomass carbon dots(Pr/N-BCDs) with remarkable luminescence properties by one-step hydrothermal method.Compared with single N-doped BCDs(N-BCDs) and Pr-doped BCDs(Pr-BCDs),Pr/N-BCDs not only showed better fluorescence properties and stability but also achieved a significant increase in quantum yield of 12%.More importantly,under certain conditions,Pr/N-BCDs and 2,4-dinitrophenylhydrazide(2,4-DNPH) had significant fluorescence internal filtration effect(IFE) and dynamic quenching effect,and in the concentration range of0.50-20 μmol·L^(-1),the concentration of 2,4-DNPH had a good linear relationship with the fluorescence quenching signal,and the detection limit was as low as 2.1 nmol·L^(-1).展开更多
The accepted doping ion in Ti^(4+)-site of PbZr_(y)Ti_(1–y)O_(3)(PZT)-based piezoelectric ceramics is a well-known method to increase mechanical quality factor(Q_(m)),since the acceptor coupled by oxygen vacancy beco...The accepted doping ion in Ti^(4+)-site of PbZr_(y)Ti_(1–y)O_(3)(PZT)-based piezoelectric ceramics is a well-known method to increase mechanical quality factor(Q_(m)),since the acceptor coupled by oxygen vacancy becomes defect dipole,which prevents the domain rotation.In this field,a serious problem is that generally,Qm decreases as the temperature(T)increases,since the oxygen vacancies are decoupled from the defect dipoles.In this work,Q_(m) of Pb_(0.95)Sr_(0.05)(Zr_(0.53)Ti_(0.47))O_(3)(PSZT)ceramics doped by 0.40%Fe_(2)O_(3)(in mole)abnormally increases as T increases,of which the Qm and piezoelectric coefficient(d_(33))at room temperature and Curie temperature(TC)are 507,292 pC/N,and 345℃,respectively.The maximum Qm of 824 was achieved in the range of 120–160℃,which is 62.52%higher than that at room temperature,while the dynamic piezoelectric constant(d_(31))was just slightly decreased by 3.85%.X-ray diffraction(XRD)and piezoresponse force microscopy results show that the interplanar spacing and the fine domains form as temperature increases,and the thermally stimulated depolarization current shows that the defect dipoles are stable even the temperature up to 240℃.It can be deduced that the aggregation of oxygen vacancies near the fine domains and defect dipole can be stable up to 240℃,which pins domain rotation,resulting in the enhanced Q_(m) with the increasing temperature.These results give a potential path to design high Q_(m) at high temperature.展开更多
Diamond with silicon vacancies has an important role as a promising single-photon source applicable in the quantum information field.However,in a microwave plasma chemical vapor deposition(MPCVD)system,due to the pres...Diamond with silicon vacancies has an important role as a promising single-photon source applicable in the quantum information field.However,in a microwave plasma chemical vapor deposition(MPCVD)system,due to the presence of unintentional silicon doping sources such as quartz windows,the behavior of silicon vacancy formation in silicon-doped diamond is complex.In this work,the underlying mechanism of formation of silicon vacancies by unintentional silicon doping in diamond is investigated from the perspective of growing surface kinetics in a two-gas-flow MPCVD system.This system is equipped with a novel susceptor geometry designed to deliver an additional gas flow directly onto the substrate surface.Increasing the concentration of growth doping substances on the substrate surface thereby enhances the efficiency of silicon vacancy formation in diamond.At the same time,by changing the substrate deposition angle the distribution of gas and plasma on the substrate surface is changed,thereby regulating the concentration and distribution of silicon vacancies formed by unintentional silicon doping.Experimental and computational results demonstrate that the difference in silicon vacancies formed by unintentional silicon doping in diamond depends on the substances present on the substrate surface and the distribution of plasma.展开更多
Perovskite barium titanate(BaTiO3)demonstrates exceptional dielectric properties as a promising microwave-absorbing(MA)material.Leveraging structural flexibility of perovskites,magnetic components can be incorporated ...Perovskite barium titanate(BaTiO3)demonstrates exceptional dielectric properties as a promising microwave-absorbing(MA)material.Leveraging structural flexibility of perovskites,magnetic components can be incorporated at A/B-sites to enhance MA performance,yet the fundamental disparity in MA mechanisms between A/B-site magnetic doping remains elusive.Herein,nickel-doped BaTiO3 perovskites were systematically synthesized through precise adjustment of the Ba/Ti molar ratio to achieve both A-site(Ni_(x)Ba_(1−x)TiO_(3),N_(x)BTO)and B-site(BaTi_(1−x)Ni_(x)O_(3),BTN^(x)O)substitutions(0≤x≤0.1)via a simple one-step hydrothermal method.Notably,A-site Ni^(2+)substitution in N_(x)BTO induced superior magnetic loss(tanδμ=0.39)attributed to eddy-current dissipation,while B-site doping in BTN^(x)O achieved higher dielectric loss(tanδε=0.49).The N0.1BTO sample exhibited optimal MA performance with a remarkable minimum reflection loss(RLmin)of−44.39 dB and broad effective absorption bandwidth(EAB=8.66 GHz)covering the Ku-band and 67%X-band.Multimodal analysis revealed synergistic interactions among multiple reflection and scattering,multi-polarization relaxation,natural resonance,and eddy currents.In contrast,BTN0.01O demonstrated deeper RLmin(−50.88 dB)but narrower EAB(3.33 GHz)governed by dielectric mechanisms.Structural characterization indicated A-site doping induced lattice distortion,reduced unit-cell volume,and optimized oxygen vacancy distribution,synergistically balancing magneto-dielectric parameters.Conversely,B-site substitution increased oxygen vacancy concentration and carrier mobility while amplifying dielectric fluctuations.The spatial occupation preference of A/B dopants(A-site and B-site)governs lattice symmetry breaking,consequently establishing structure-property relationships and underpinning the material’s tunable dielectric behavior and magnetic phenomena.This work proposes a site-selective doping strategy for designing high-performance perovskite MA materials through magneto-dielectric equilibrium optimization.展开更多
In a high heat flux ablative environment,the surface temperature of aircraft rises rapidly,leading to traditional high thermal conductivity materials being ineffective at protecting internal metal components.In this s...In a high heat flux ablative environment,the surface temperature of aircraft rises rapidly,leading to traditional high thermal conductivity materials being ineffective at protecting internal metal components.In this study,continuous carbon fiber reinforced Li_(2)O-Al_(2)O_(3)-SiO_(2)(C_(f)/LAS)glass ceramic composites doped with SiC particles(SiC_(p))were prepared by slurry immersion winding and hot pressing sintering.Effect of matrix crystallinity on ablative properties of the composites under ultra-high heat flux was investigated.By utilizing heat absorption and low thermal conductivity characteristics associated with SiO_(2)gasification within composite materials,both surface and internal temperatures of these materials are effectively reduced,thereby ensuring the safe operation of aircraft and electronic devices.Results indicate that the average linear ablation rate of composites doped with 10%(in mass)of SiC_(p)significantly decreases at a heat flux of 20 MW/m^(2).Transmission electron microscope observation reveals that the doped glass matrix exhibits increased crystallinity,reduced internal stress,and minimized lattice distortion,thereby enhancing the composites’high-temperature performance.However,excessive SiC_(p)doping leads to reduced crystallinity and deteriorated ablation performance.Ultimately,the average linear ablation rate of C_(f)/LAS composites with 10%(in mass)SiC_(p)at 20 MW/m^(2)heat flux is comparable to that of commercial carbon/carbon composites,accompanied by providing lower thermal conductivity and higher bending strength.This novel high-performance C_(f)/LAS composite is cost-effective,short-cycled,and suitable for mass production,offering promising potential for widespread application in ablation-resistant components of hypersonic vehicles.展开更多
The development of high-performance,reproducible carbon(C)-based supercapacitors remains a significant challenge because of limited specific capacitance.Herein,we present a novel strategy for fabricating LaCoO_(x) and...The development of high-performance,reproducible carbon(C)-based supercapacitors remains a significant challenge because of limited specific capacitance.Herein,we present a novel strategy for fabricating LaCoO_(x) and cobalt(Co)-doped nanoporous C(LaCoO_(x)/Co@ZNC)through the carbonization of Co/Zn-zeolitic imidazolate framework(ZIF)crystals derived from a PVP-Co/Zn/La precursor.The unique ZIF structure effectively disrupted the graphitic C framework,preserved the Co active sites,and enhanced the electrical conductivity.The synergistic interaction between pyridinic nitrogen and Co ions further promoted redox reactions.In addition,the formation of a hierarchical pore structure through zinc sublimation facili-tated electrolyte diffusion.The resulting LaCoO_(x)/Co@ZNC exhibited exceptional electrochemical performance,delivering a remarkable specific capacitance of 2,789 F/g at 1 A/g and outstanding cycling stability with 92%capacitance retention after 3,750 cycles.Our findings provide the basis for a promising approach to advancing C-based energy storage technologies.展开更多
We investigate the interplay between the pseudogap state and d-wave superconductivity in the two-dimensional doped Hubbard model by employing an eight-site cluster dynamical mean-field theory method.By tuning electron...We investigate the interplay between the pseudogap state and d-wave superconductivity in the two-dimensional doped Hubbard model by employing an eight-site cluster dynamical mean-field theory method.By tuning electron hopping parameters,the strong-coupling pseudogap in the two-dimensional Hubbard model can be either enhanced or suppressed in the doped Mott insulator regime.We find that in underdoped cases,the closing of pseudogap leads to a significant enhancement of superconductivity,indicating competition between the two in the underdoped regime.In contrast,at large dopings,suppressing the pseudogap is accompanied by a concurrent decrease in the superconducting transition temperature Tc,which can be attributed to a reduction in antiferromagnetic correlations behind both the pseudogap and superconductivity.We elucidate this evolving relationship between pseudogap and superconductivity across different doping regimes.展开更多
Catalytic oxidation of NO at room temperature was carried out over nitrogen(N)-doped sludge char(SC)prepared from pyrolysis ofmunicipal sewage sludge,and urea was adopted as nitrogen source.The effects of different N-...Catalytic oxidation of NO at room temperature was carried out over nitrogen(N)-doped sludge char(SC)prepared from pyrolysis ofmunicipal sewage sludge,and urea was adopted as nitrogen source.The effects of different N-doping methods(one-step and two-step method),dried sludge(DS)/urea mass ratios(5:1,4:1,3:1,2:1,and 1:1),SC preparation procedures(pyrolysis only,pyrolysis with acid washing,and pyrolysis with KOH activation and acid washing),and different pyrolysis temperatures(500,600,700,and 800°C)on the catalytic oxidation of NO were compared to optimize the procedure for SC preparation.The results indicated that N-doping could obviously promote the catalytic performance of SC.The one-step method with simultaneous sludge pyrolysis(at 700°C),KOH activation,and N-doping(DS/urea of 3:1)was the optimal procedure for preparing the N-doped SC with the NO conversion rate of 54.7%,whereas the optimal NO conversion rate of SC without N-doping was only 47.3%.Urea worked both as carbon and nitrogen source,which could increase about 2.9%-16.5%of carbon and 24.8%-42.7%of nitrogen content in SC pyrolyzed at 700°C.N-doping significantly promoted microporosity of SC.The optimal N-doped SC showed specific surface areas of 571.38 m^(2)/g,much higher than 374.34 m^(2)/g of the optimal SC without N-doping.In addition,N-doping also increased amorphousness and surface basicity of SC through the formation of N-containing groups.Finally,three reaction paths,i.e.microporous reactor,active sites,and basic site control path,were proposed to explain the mechanism of N-doping on promoting the catalytic performance of NO.展开更多
Garnet Li_(7)La_(3)Zr_(2)O_(12)(LLZO)electrolytes have been recognized as a promising candidate to replace liquid/molten-state electrolytes in battery applications due to their exceptional performance,particularly Ga-...Garnet Li_(7)La_(3)Zr_(2)O_(12)(LLZO)electrolytes have been recognized as a promising candidate to replace liquid/molten-state electrolytes in battery applications due to their exceptional performance,particularly Ga-doped LLZO(LLZGO),which exhibits high ionic conductivity.However,the limited size of the Liþtransport bottleneck restricts its high-current discharging performance.The present study focuses on the synthesis of Ga^(3+)þand Ba^(2+)þco-doped LLZO(LLZGBO)and investigates the influence of doping contents on the morphology,crystal structure,Liþtransport bottleneck size,and ionic conductivity.In particular,Ga_(0.32)Ba_(0.15)exhibits the highest ionic conductivity(6.11E-2 S cm^(-1) at 550 C)in comparison with other compositions,which can be attributed to its higher-energy morphology,larger bottleneck and unique Liþtransport channel.In addition to Ba^(2+),Sr^(2+)þand Ca^(2+)have been co-doped with Ga3þinto LLZO,respectively,to study the effect of doping ion radius on crystal structures and the properties of electrolytes.The characterization results demonstrate that the easier Liþtransport and higher ionic conductivity can be obtained when the electrolyte is doped with larger-radius ions.As a result,the assembled thermal battery with Ga_(0.32)Ba_(0.15)-LLZO electrolyte exhibits a remarkable voltage platform of 1.81 V and a high specific capacity of 455.65 mA h g^(-1) at an elevated temperature of 525℃.The discharge specific capacity of the thermal cell at 500 mA amounts to 63%of that at 100 mA,showcasing exceptional high-current discharging performance.When assembled as prototypes with fourteen single cells connected in series,the thermal batteries deliver an activation time of 38 ms and a discharge time of 32 s with the current density of 100 mA cm^(-2).These findings suggest that Ga,Ba co-doped LLZO solid-state electrolytes with high ionic conductivities holds great potential for high-capacity,quick-initiating and high-current discharging thermal batteries.展开更多
Luminescent materials for application in temperature sensing have caught a lot of interest in recent years.Particularly erbium(Er^(3+))-doped fluoride-based materials(EFM),which are readily accessible by near-infrared...Luminescent materials for application in temperature sensing have caught a lot of interest in recent years.Particularly erbium(Er^(3+))-doped fluoride-based materials(EFM),which are readily accessible by near-infrared(NIR)excitation to produce efficient photon conversion.It has been established that ytterbium(Yb^(3+))may improve the performance of EFMs in both bulk and nanostructured forms by energy transfer channels among rare-earth ions in interstitial clusters.In this work,a comprehensive analysis of the Er^(3+):Yb^(3+):CaF_(2)crystalline structure,photoluminescence,and energy transfer from Yb^(3+)to Er^(3+)is presented for powders prepared by combustion synthesis.The Er^(3+):Yb^(3+):CaF_(2)powders display exceptional photon down-shift and up-conversion when exposed to NIR light(λ=975 nm).The luminescence spectral change of the NIR emission around 1.5μm,which corresponds to the Er^(3+)electronic transition ^(4)I_(13/2)→^(4)I_(15/2),was investigated in a temperature range of 298-423 K for application in temperature sensing of biological systems exploring the third biological window.The luminescence intensity ratio technique was applied to the thermally coupled Stark sublevels of states^(4)I_(13/2)and^(4)I_(15/2)with the highest estimated temperature relative sensitivity being around 0.4%/K at 298 K.展开更多
Bismuth-doped antimony tungstate(Bi-doped Sb_(2)WO_(6))microspheres were synthesized via a novel hydrothermal synthesis approach.These microspheres were then used as active layers in gas sensors for the detection of c...Bismuth-doped antimony tungstate(Bi-doped Sb_(2)WO_(6))microspheres were synthesized via a novel hydrothermal synthesis approach.These microspheres were then used as active layers in gas sensors for the detection of carbon dioxide(CO_(2)),a significant greenhouse gas and a critical parameter for evaluating air quality.The incorporation of bismuth significantly enhances the gas-sensing performance of the Sb_(2)WO_(6)microspheres,with the 4%Bidoped sensing active layer achieving a remarkable response value of 15 when exposed to 200 ppm of CO_(2),outperforming the undoped Sb_(2)WO_(6).Furthermore,the selectivity of the 4%Bi-Sb_(2)WO_(6)sensor toward CO_(2)gas was enhanced relative to the Sb_(2)WO_(6)sensor.The fundamental mechanisms of gas sensing and the factors contributing to the improved CO_(2)response of 4%Bi-Sb_(2)WO_(6)micro spheres were investigated using density functional theory.Bi-doped Sb_(2)WO_(6)materials exhibit significant advantages in gas-sensing applications,including improved conductivity,enhanced gas adsorption capacity,increased reaction rates,good chemical stability,excellent selectivity,and the ability to adjust electron density.These characteristics enable Bi-doped Sb_(2)WO_(6)to demonstrate higher sensitivity and rapid response capabilities in gas sensors,making it suitable for practical applications.展开更多
基金financially supported by the project of the National Natural Science Foundation of China(52322203)the Key Research and Development Program of Shaanxi Province(2024GHZDXM-21)。
文摘The design of cost-effective and efficient metal-free carbon-based catalysts for the hydrogen evolution reaction(HER)is of great significance for increasing the production of clean hydrogen by the electrolysis of alkaline water.Precise control of the electronic structure by heteroatom doping has proven to be efficient for increasing catalytic activity.Nevertheless,both the structural characteristics and the underlying mechanism are not well understood,especially for doping with two different atoms,thus limiting the use of these catalysts.We report the production of phosphorus and nitrogen co-doped hollow carbon nanospheres(HCNs)by the copolymerization of pyrrole and aniline at a Triton X-100 micelle-interface,followed by doping with phytic acid and carbonization.The unique pore structure and defect-rich framework of the HCNs expose numerous active sites.Crucially,the combined effect of graphitic nitrogen and phosphorus-carbon bonds modulate the local electronic structure of adjacent C atoms and facilitates electron transfer.As a res-ult,the HCN carbonized at 1100°C exhibited superior HER activity and an outstanding stability(70 h at a current density of 10 mA cm^(−2))in alkaline water,because of the large number of graphitic nitrogen and phosphorus-carbon bonds.
基金supported by the National Key R&D Program of China(Nos.2022YFB3504804 and 2023YFF0718303)the National Natural Science Foundation of China(Nos.51871219,52071324,52031014,and 52401255)+1 种基金Science and Technology Project of Shenyang City(No.22-101-0-27)Liaoning Institute of Science and Technology Doctoral Initiation Fund Project(No.2307B19).
文摘To realize the application of electromagnetic wave absorption(EWA)devices in humid marine environments,bifunctional EWA materials with better EWA capacities and anticorrosion properties have great exploration significance and systematic research re-quirements.By utilizing the low-cost and excellent magnetic and stable chemical characteristics of barium ferrite(BaFe_(12)O_(19))and using the high dielectric loss and excellent chemical inertia of nanocarbon clusters,a new type of nanocomposites with carbon nanoclusters en-capsulating BaFe_(12)O_(19)was designed and synthesized by combining an impregnation method and a high-temperature calcination strategy.Furthermore,Ce-Mn ions were introduced into the BaFe_(12)O_(19)lattice to improve the dielectric and magnetic properties of BaFe_(12)O_(19)cores significantly,and the energy band structure of the doped lattice and the orders of Ce replacing Fe sites were calculated.Benefiting from Ce-Mn ion doping and carbon nanocluster encapsulation,the composite material exhibited excellent dual functionality of corrosion resist-ance and EWA.When BaCe_(0.2)Mn_(0.3)Fe_(11.5)O_(19)-C(BCM-C)was calcined at 600°C,the minimum reflection loss of-20.1 dB was achieved at 14.43 GHz.The Ku band’s effective absorption bandwidth of 4.25 GHz was achieved at an absorber thickness of only 1.3 mm.The BCM-C/polydimethylsiloxane coating had excellent corrosion resistance in the simulated marine environment(3.5wt%NaCl solution).The|Z|0.01Hz value of BCM-C remained at 106Ω·cm^(2)after 12 soaking days.The successful preparation of the BaFe_(12)O_(19)composite en-capsulated with carbon nanoclusters provides new insights into the preparation of multifunctional absorbent materials and the fabrication of absorbent devices applied in humid marine environments in the future.
基金supported by the National Natural Science Foundation of China(No.51803041)the University and Local Integration Development Project of Yantai,China(No.2022 XDRHXMXK08).
文摘Herein,an external crosslinker facilitated the hypercrosslinking of ferrocene and a nitrogen heterocyclic compound(either melamine or imidazole)through a direct Friedel-Crafts reaction,which led to the formation of nitrogen-containing hypercrosslinked fer-rocene polymer precursors(HCP-FCs).Subsequent carbonization of these precursors results in the production of iron-nitrogen-doped por-ous carbon absorbers(Fe-NPCs).The Fe-NPCs demonstrate a porous structure comprising aggregated nanotubes and nanospheres.The porosity of this structure can be modulated by adjusting the iron and nitrogen contents to optimize impedance matching.The uniform dis-tribution of Fe-N_(x)C,N dipoles,andα-Fe within the carbon matrix can be ensured by using hypercrosslinked ferrocenes in constructing porous carbon,providing the absorber with numerous polarization sites and a conductive network.The electromagnetic wave absorption performance of the specially designed Fe-NPC-M_(2)absorbers is satisfactory,revealing a minimum reflection loss of-55.3 dB at 2.5 mm and an effective absorption bandwidth of 6.00 GHz at 2.0 mm.By utilizing hypercrosslinked polymers(HCPs)as precursors,a novel method for developing highly efficient carbon-based absorbing agents is introduced in this research.
基金supported by National Natural Science Foundation of China(Nos.52472194,52101243)Natural Science Foundation of Guangdong Province,China(No.2023A1515012619)the Science and Technology Planning Project of Guangzhou(No.202201010565)。
文摘In recent years,metal phosphosulfides have attracted great attention as the promising anode materials in sodium/potassium batteries because of their incorporation of the advantages of metal phosphides and sulfides.However,they are also confronted with the problem of unstable battery performance due to the heavy volume expansion and sluggish ion reaction kinetics.Herein,yolk-shell cobalt phosphosulfide nanocrystals encapsulating into multi-heterogeneous atom(N,P,S)-doped carbon framework(Co_(9)S_(8)/CoP@NPSC)were constructed by employing dodecahedral ZIF-67 as precursor and a polymer as carbon sources through simultaneous sulfidation and phosphorization processes.The synergistic effect of Co_(9)S_(8)and CoP component and the yolk-shell structure greatly improve the bettery performance and structural stability.In addition,the multiple hetero-atoms doped carbon frameworks enhance the conductivity of the electrode materials and increase the spacing of carbon layers to supply sufficient active sites and facilitate the Na^(+)/K^(+)transport.The electrochemical results demonstrated that Co_(9)S_(8)/CoP@NPSC exhibited the pleasant reversible capacity(360.47 mAh/g at 1 A/g)after 300 cycles and an unpredictable cycling stability(103.22 mAh/g after 1000 cycles)in the SIBs application.The ex-situ XRD and XPS analyses were further applied to study the sodium ion storage mechanism and the multi-step phase transition reaction of the yolk-shell heterogeneous structure.This work provides new perspectives for the preparation of novel structure metal phosphosulfide and their applications in anode materials for sodium/potassium batteries and other secondary batteries.
基金supported by the Hainan Provincial Natural Science Foundation of China(Nos.522MS038 and 522QN282)the National Natural Science Foundation of China(Nos.52172086 and 52301268)the Start-up Research Foundation of Hainan University(No.KYQD(ZR)-22019).
文摘Thermoelectric water spitting to hydrogen systems has great potential in the production of environment-friendly fuel using renewable solar energy in the future.In this work,we prepared porous nanosheet Mo doping Ni_(5)P_(4)catalysts on nickel foam with efficient hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)performance in alkaline media.Density Functional Theory(DFT)calculations and experimental studies have shown that Mo doping deadeneds the interaction between H and O atomic orbitals of transition state water molecules,effectively weakening the activation energy of H_(2)O dissociation.Therefore,Mo doping is favorable for enhancing HER activity with overpotential at 10 mA cm^(-2)of 93 mV and Tafel slope of 40.1 mV dec^(-1)in 1 M KOH.Besides,it exhibits high alkaline OER activity with an ultra-low overpotential of 200 mV at 10 mA cm^(-2).Moreover,this catalyst only needs 1.537 V in a dual-electrode configuration of the electrolytic cell,which is much lower than the commercial Pt/C-RuO_(2)couple(1.614 V).In addition,we have developed and constructed a solar thermoelectric generator(TEG)that is capable of floating on water.This TEG has a continuous power output and an exceptionally long lifespan,providing a stable power supply to the synthesized catalyst electrolyzer.It can produce a maximum power output of over 90 mW,meeting the requirement of converting solar radiation heat into usable electricity.As a result,the system achieves productivity of 0.11 mL min^(-1)H_(2).This solar thermal energy conversion technology shows the possibility of large-scale industrial production of H_(2)and provides a new idea for exploring heat source utilization.
基金supported by National Key R&D Program of China(2021YFB4001401)National Natural Science Foundation of China(52272190,22178023).
文摘Solid oxide electrolysis cells(SOECs)can effectively convert CO_(2)into high value-added CO fuel.In this paper,Sc-doped Sr_(2)Fe_(1.5)Mo_(0.3)Sc_(0.2)O_(6−δ)(SFMSc)perovskite oxide material is synthesized via solid-phase method as the cathode for CO_(2)electrolysis by SOECs.XRD confirms that SFMSc exhibits a stable cubic phase crystal structure.The experimental results of TPD,TG,EPR,CO_(2)-TPD further demonstrate that Sc-doping increases the concentration of oxygen vacancy in the material and the chemical adsorption capacity of CO_(2)molecules.Electrochemical tests reveal that SFMSc single cell achieves a current density of 2.26 A/cm^(2) and a lower polarization impedance of 0.32Ω·cm^(2) at 800°C under the applied voltage of 1.8 V.And no significant performance attenuation or carbon deposition is observed after 80 h continuous long-term stability test.This study provides a favorable support for the development of SOEC cathode materials with good electro-catalytic performance and stability.
基金supported by the Guangdong Basic and Applied Basic Research Foundation (No.2023A1515010093)the Shenzhen Fundamental Research Program (Stable Support Plan Program)(Nos.JCYJ20220809170611004, 20231121110828001 and 20231121113641002)the National Taipei University of Technology-Shenzhen University Joint Research Program (No.2024001)。
文摘In this paper, we have demonstrated an Er-doped ultrafast laser with a single mode fiber-gradient index multimode fiber-single mode fiber(SMF-GIMF-SMF, SMS) structure as saturable absorber(SA), which can generate not only stable single-pulse state, but also special mode-locked pulses with the characteristics of high energy and noisy behaviors at proper pump power and cavity polarization state. In addition, we have deeply investigated the real-time spectral evolutions of the mode-locked pulses through the dispersive Fourier transformation(DFT) technique. It can be found that the pulse regime can actually consist of a lot of small noise pulses with randomly varying intensities. We believe that these results will further enrich the nonlinear dynamical processes in the ultrafast lasers.
文摘Nitrogen doping in chemical vapor deposition-derived ultrananocrystalline diamond(UNCD)films in-creases the electronic conductivity,yet its microstructural effects on electron transport are insufficiently understood.We investigated the formation of nitrogen-induced diaph-ite structures(hybrid diamond-graphite phases)and their role in changing the conductivity.Nitrogen doping in a hy-drogen-rich plasma environment promotes the emergence of unique sp^(3)-sp^(2)bonding interfaces,where diamond grains are covalently integrated with graphitic domains,facilitating a structure-driven electronic transition.High-resolution transmis-sion electron microscopy and selected area electron diffraction reveal five-fold,six-fold and twelve-fold symmetries,along with an atypical{200}crystallographic reflection,confirming diaphite formation in 5%and 10%N-doped UNCD films,while high-er doping levels(15%and 20%)result in extensive graphitization.Raman spectroscopy tracks the evolution of sp^(2)bonding with increasing nitrogen content,while atomic force microscopy and X-ray diffraction indicate a consistent diamond grain size of~8 nm.Cryogenic electronic transport measurements reveal a conductivity increase from 8.72 to 708 S/cm as the nitrogen dop-ing level increases from 5%to 20%,which is attributed to defect-mediated carrier transport and 3D weak localization.The res-ulting conductivity is three orders of magnitude higher than previously reported.These findings establish a direct correlation between diaphite structural polymorphism and tunable electronic properties in nitrogen-doped UNCD films,offering new ways for defect-engineering diamond-based electronic materials.
基金supported by the National Natural Science Foundation of China (Grant No.22063010)the Natural Science Foundation of Shaanxi Province (Grant No.2022QFY07-05)Yan'an Science and Technology Plan Project (Grants No.2022SLJBZ-002, 2023-CYL-193)。
文摘We used the natural product chamomile as a carbon source to synthesize praseodymium(Pr) and nitrogen(N) co-doped biomass carbon dots(Pr/N-BCDs) with remarkable luminescence properties by one-step hydrothermal method.Compared with single N-doped BCDs(N-BCDs) and Pr-doped BCDs(Pr-BCDs),Pr/N-BCDs not only showed better fluorescence properties and stability but also achieved a significant increase in quantum yield of 12%.More importantly,under certain conditions,Pr/N-BCDs and 2,4-dinitrophenylhydrazide(2,4-DNPH) had significant fluorescence internal filtration effect(IFE) and dynamic quenching effect,and in the concentration range of0.50-20 μmol·L^(-1),the concentration of 2,4-DNPH had a good linear relationship with the fluorescence quenching signal,and the detection limit was as low as 2.1 nmol·L^(-1).
基金National Natural Science Foundation of China(U2241242)National Key R&D Program of China(2023YFB3812000,2021YFA0716502)。
文摘The accepted doping ion in Ti^(4+)-site of PbZr_(y)Ti_(1–y)O_(3)(PZT)-based piezoelectric ceramics is a well-known method to increase mechanical quality factor(Q_(m)),since the acceptor coupled by oxygen vacancy becomes defect dipole,which prevents the domain rotation.In this field,a serious problem is that generally,Qm decreases as the temperature(T)increases,since the oxygen vacancies are decoupled from the defect dipoles.In this work,Q_(m) of Pb_(0.95)Sr_(0.05)(Zr_(0.53)Ti_(0.47))O_(3)(PSZT)ceramics doped by 0.40%Fe_(2)O_(3)(in mole)abnormally increases as T increases,of which the Qm and piezoelectric coefficient(d_(33))at room temperature and Curie temperature(TC)are 507,292 pC/N,and 345℃,respectively.The maximum Qm of 824 was achieved in the range of 120–160℃,which is 62.52%higher than that at room temperature,while the dynamic piezoelectric constant(d_(31))was just slightly decreased by 3.85%.X-ray diffraction(XRD)and piezoresponse force microscopy results show that the interplanar spacing and the fine domains form as temperature increases,and the thermally stimulated depolarization current shows that the defect dipoles are stable even the temperature up to 240℃.It can be deduced that the aggregation of oxygen vacancies near the fine domains and defect dipole can be stable up to 240℃,which pins domain rotation,resulting in the enhanced Q_(m) with the increasing temperature.These results give a potential path to design high Q_(m) at high temperature.
基金supported by the National Natural Science Foundation of China(Grant No.62274084)the Fundamental Research Funds for the Central Universities(Grant No.0210-14380193).
文摘Diamond with silicon vacancies has an important role as a promising single-photon source applicable in the quantum information field.However,in a microwave plasma chemical vapor deposition(MPCVD)system,due to the presence of unintentional silicon doping sources such as quartz windows,the behavior of silicon vacancy formation in silicon-doped diamond is complex.In this work,the underlying mechanism of formation of silicon vacancies by unintentional silicon doping in diamond is investigated from the perspective of growing surface kinetics in a two-gas-flow MPCVD system.This system is equipped with a novel susceptor geometry designed to deliver an additional gas flow directly onto the substrate surface.Increasing the concentration of growth doping substances on the substrate surface thereby enhances the efficiency of silicon vacancy formation in diamond.At the same time,by changing the substrate deposition angle the distribution of gas and plasma on the substrate surface is changed,thereby regulating the concentration and distribution of silicon vacancies formed by unintentional silicon doping.Experimental and computational results demonstrate that the difference in silicon vacancies formed by unintentional silicon doping in diamond depends on the substances present on the substrate surface and the distribution of plasma.
基金the Central Universities(Nos.SWU-KF25028 and SWU-XDJH202314)Natural Science Foundation Project of Chongqing(No.cstc2024ycjh-bgzxm0005)the Opening Project of State Key Laboratory of Solid Lubrication(No.LSL2416)for financial support.We also thank Analytical&Testing Center in Southwest University for SEM test.
文摘Perovskite barium titanate(BaTiO3)demonstrates exceptional dielectric properties as a promising microwave-absorbing(MA)material.Leveraging structural flexibility of perovskites,magnetic components can be incorporated at A/B-sites to enhance MA performance,yet the fundamental disparity in MA mechanisms between A/B-site magnetic doping remains elusive.Herein,nickel-doped BaTiO3 perovskites were systematically synthesized through precise adjustment of the Ba/Ti molar ratio to achieve both A-site(Ni_(x)Ba_(1−x)TiO_(3),N_(x)BTO)and B-site(BaTi_(1−x)Ni_(x)O_(3),BTN^(x)O)substitutions(0≤x≤0.1)via a simple one-step hydrothermal method.Notably,A-site Ni^(2+)substitution in N_(x)BTO induced superior magnetic loss(tanδμ=0.39)attributed to eddy-current dissipation,while B-site doping in BTN^(x)O achieved higher dielectric loss(tanδε=0.49).The N0.1BTO sample exhibited optimal MA performance with a remarkable minimum reflection loss(RLmin)of−44.39 dB and broad effective absorption bandwidth(EAB=8.66 GHz)covering the Ku-band and 67%X-band.Multimodal analysis revealed synergistic interactions among multiple reflection and scattering,multi-polarization relaxation,natural resonance,and eddy currents.In contrast,BTN0.01O demonstrated deeper RLmin(−50.88 dB)but narrower EAB(3.33 GHz)governed by dielectric mechanisms.Structural characterization indicated A-site doping induced lattice distortion,reduced unit-cell volume,and optimized oxygen vacancy distribution,synergistically balancing magneto-dielectric parameters.Conversely,B-site substitution increased oxygen vacancy concentration and carrier mobility while amplifying dielectric fluctuations.The spatial occupation preference of A/B dopants(A-site and B-site)governs lattice symmetry breaking,consequently establishing structure-property relationships and underpinning the material’s tunable dielectric behavior and magnetic phenomena.This work proposes a site-selective doping strategy for designing high-performance perovskite MA materials through magneto-dielectric equilibrium optimization.
基金National Natural Science Foundation of China(U23A6014,52103357)。
文摘In a high heat flux ablative environment,the surface temperature of aircraft rises rapidly,leading to traditional high thermal conductivity materials being ineffective at protecting internal metal components.In this study,continuous carbon fiber reinforced Li_(2)O-Al_(2)O_(3)-SiO_(2)(C_(f)/LAS)glass ceramic composites doped with SiC particles(SiC_(p))were prepared by slurry immersion winding and hot pressing sintering.Effect of matrix crystallinity on ablative properties of the composites under ultra-high heat flux was investigated.By utilizing heat absorption and low thermal conductivity characteristics associated with SiO_(2)gasification within composite materials,both surface and internal temperatures of these materials are effectively reduced,thereby ensuring the safe operation of aircraft and electronic devices.Results indicate that the average linear ablation rate of composites doped with 10%(in mass)of SiC_(p)significantly decreases at a heat flux of 20 MW/m^(2).Transmission electron microscope observation reveals that the doped glass matrix exhibits increased crystallinity,reduced internal stress,and minimized lattice distortion,thereby enhancing the composites’high-temperature performance.However,excessive SiC_(p)doping leads to reduced crystallinity and deteriorated ablation performance.Ultimately,the average linear ablation rate of C_(f)/LAS composites with 10%(in mass)SiC_(p)at 20 MW/m^(2)heat flux is comparable to that of commercial carbon/carbon composites,accompanied by providing lower thermal conductivity and higher bending strength.This novel high-performance C_(f)/LAS composite is cost-effective,short-cycled,and suitable for mass production,offering promising potential for widespread application in ablation-resistant components of hypersonic vehicles.
基金supported financially by National Natural Science Foundation of China(NSFC)(Nos.22478115,22075083)the Programme of Introducing Talents of Discipline to Universities(No.B16017).
文摘The development of high-performance,reproducible carbon(C)-based supercapacitors remains a significant challenge because of limited specific capacitance.Herein,we present a novel strategy for fabricating LaCoO_(x) and cobalt(Co)-doped nanoporous C(LaCoO_(x)/Co@ZNC)through the carbonization of Co/Zn-zeolitic imidazolate framework(ZIF)crystals derived from a PVP-Co/Zn/La precursor.The unique ZIF structure effectively disrupted the graphitic C framework,preserved the Co active sites,and enhanced the electrical conductivity.The synergistic interaction between pyridinic nitrogen and Co ions further promoted redox reactions.In addition,the formation of a hierarchical pore structure through zinc sublimation facili-tated electrolyte diffusion.The resulting LaCoO_(x)/Co@ZNC exhibited exceptional electrochemical performance,delivering a remarkable specific capacitance of 2,789 F/g at 1 A/g and outstanding cycling stability with 92%capacitance retention after 3,750 cycles.Our findings provide the basis for a promising approach to advancing C-based energy storage technologies.
基金supported by the National Natural Science Foundation of China(Grant Nos.12274472,12494594,12494591,and 92165204)National Key Research and Development Program of China(Grant No.2022YFA1402802)+2 种基金Guangdong Provincial Key Laboratory of Magnetoelectric Physics and Devices(Grant No.2022B1212010008)Guangdong Fundamental Research Center for Magnetoelectric Physics(Grant No.2024B0303390001)Guangdong Provincial Quantum Science Strategic Initiative(Grant No.GDZX2401010)。
文摘We investigate the interplay between the pseudogap state and d-wave superconductivity in the two-dimensional doped Hubbard model by employing an eight-site cluster dynamical mean-field theory method.By tuning electron hopping parameters,the strong-coupling pseudogap in the two-dimensional Hubbard model can be either enhanced or suppressed in the doped Mott insulator regime.We find that in underdoped cases,the closing of pseudogap leads to a significant enhancement of superconductivity,indicating competition between the two in the underdoped regime.In contrast,at large dopings,suppressing the pseudogap is accompanied by a concurrent decrease in the superconducting transition temperature Tc,which can be attributed to a reduction in antiferromagnetic correlations behind both the pseudogap and superconductivity.We elucidate this evolving relationship between pseudogap and superconductivity across different doping regimes.
基金supported by Shanghai Pujiang Program(No.22PJD001)the Fundamental Research Funds for the Central Universities(No.2232021G-11).
文摘Catalytic oxidation of NO at room temperature was carried out over nitrogen(N)-doped sludge char(SC)prepared from pyrolysis ofmunicipal sewage sludge,and urea was adopted as nitrogen source.The effects of different N-doping methods(one-step and two-step method),dried sludge(DS)/urea mass ratios(5:1,4:1,3:1,2:1,and 1:1),SC preparation procedures(pyrolysis only,pyrolysis with acid washing,and pyrolysis with KOH activation and acid washing),and different pyrolysis temperatures(500,600,700,and 800°C)on the catalytic oxidation of NO were compared to optimize the procedure for SC preparation.The results indicated that N-doping could obviously promote the catalytic performance of SC.The one-step method with simultaneous sludge pyrolysis(at 700°C),KOH activation,and N-doping(DS/urea of 3:1)was the optimal procedure for preparing the N-doped SC with the NO conversion rate of 54.7%,whereas the optimal NO conversion rate of SC without N-doping was only 47.3%.Urea worked both as carbon and nitrogen source,which could increase about 2.9%-16.5%of carbon and 24.8%-42.7%of nitrogen content in SC pyrolyzed at 700°C.N-doping significantly promoted microporosity of SC.The optimal N-doped SC showed specific surface areas of 571.38 m^(2)/g,much higher than 374.34 m^(2)/g of the optimal SC without N-doping.In addition,N-doping also increased amorphousness and surface basicity of SC through the formation of N-containing groups.Finally,three reaction paths,i.e.microporous reactor,active sites,and basic site control path,were proposed to explain the mechanism of N-doping on promoting the catalytic performance of NO.
基金the National Key R&D Program of China(No.2023YFC3009501)the National Natural Science Foundation of China(No.52374298)+1 种基金the project of State Key Laboratory of Explosion Science and Safety Protection(Beijing Institute of Technology,No.QNKT23-17)Aeronautical Science Foundation of China(No.20174072003).
文摘Garnet Li_(7)La_(3)Zr_(2)O_(12)(LLZO)electrolytes have been recognized as a promising candidate to replace liquid/molten-state electrolytes in battery applications due to their exceptional performance,particularly Ga-doped LLZO(LLZGO),which exhibits high ionic conductivity.However,the limited size of the Liþtransport bottleneck restricts its high-current discharging performance.The present study focuses on the synthesis of Ga^(3+)þand Ba^(2+)þco-doped LLZO(LLZGBO)and investigates the influence of doping contents on the morphology,crystal structure,Liþtransport bottleneck size,and ionic conductivity.In particular,Ga_(0.32)Ba_(0.15)exhibits the highest ionic conductivity(6.11E-2 S cm^(-1) at 550 C)in comparison with other compositions,which can be attributed to its higher-energy morphology,larger bottleneck and unique Liþtransport channel.In addition to Ba^(2+),Sr^(2+)þand Ca^(2+)have been co-doped with Ga3þinto LLZO,respectively,to study the effect of doping ion radius on crystal structures and the properties of electrolytes.The characterization results demonstrate that the easier Liþtransport and higher ionic conductivity can be obtained when the electrolyte is doped with larger-radius ions.As a result,the assembled thermal battery with Ga_(0.32)Ba_(0.15)-LLZO electrolyte exhibits a remarkable voltage platform of 1.81 V and a high specific capacity of 455.65 mA h g^(-1) at an elevated temperature of 525℃.The discharge specific capacity of the thermal cell at 500 mA amounts to 63%of that at 100 mA,showcasing exceptional high-current discharging performance.When assembled as prototypes with fourteen single cells connected in series,the thermal batteries deliver an activation time of 38 ms and a discharge time of 32 s with the current density of 100 mA cm^(-2).These findings suggest that Ga,Ba co-doped LLZO solid-state electrolytes with high ionic conductivities holds great potential for high-capacity,quick-initiating and high-current discharging thermal batteries.
基金Project supported in part by the Brazilian Agency Conselho Nacional de Desenvolvimento Científico e Tecnológico(CNPq)。
文摘Luminescent materials for application in temperature sensing have caught a lot of interest in recent years.Particularly erbium(Er^(3+))-doped fluoride-based materials(EFM),which are readily accessible by near-infrared(NIR)excitation to produce efficient photon conversion.It has been established that ytterbium(Yb^(3+))may improve the performance of EFMs in both bulk and nanostructured forms by energy transfer channels among rare-earth ions in interstitial clusters.In this work,a comprehensive analysis of the Er^(3+):Yb^(3+):CaF_(2)crystalline structure,photoluminescence,and energy transfer from Yb^(3+)to Er^(3+)is presented for powders prepared by combustion synthesis.The Er^(3+):Yb^(3+):CaF_(2)powders display exceptional photon down-shift and up-conversion when exposed to NIR light(λ=975 nm).The luminescence spectral change of the NIR emission around 1.5μm,which corresponds to the Er^(3+)electronic transition ^(4)I_(13/2)→^(4)I_(15/2),was investigated in a temperature range of 298-423 K for application in temperature sensing of biological systems exploring the third biological window.The luminescence intensity ratio technique was applied to the thermally coupled Stark sublevels of states^(4)I_(13/2)and^(4)I_(15/2)with the highest estimated temperature relative sensitivity being around 0.4%/K at 298 K.
基金financially supported by the Outstanding Youth Foundation of Jiangsu Province of China(No.BK20211548)Yangzhou Science and Technology Plan Project(No.YZ2023246)+1 种基金China Scholarship Council(No.202308320445)the Postgraduate Research and Practice Innovation Program of Jiangsu Province of China(No.KYCX23_3551)
文摘Bismuth-doped antimony tungstate(Bi-doped Sb_(2)WO_(6))microspheres were synthesized via a novel hydrothermal synthesis approach.These microspheres were then used as active layers in gas sensors for the detection of carbon dioxide(CO_(2)),a significant greenhouse gas and a critical parameter for evaluating air quality.The incorporation of bismuth significantly enhances the gas-sensing performance of the Sb_(2)WO_(6)microspheres,with the 4%Bidoped sensing active layer achieving a remarkable response value of 15 when exposed to 200 ppm of CO_(2),outperforming the undoped Sb_(2)WO_(6).Furthermore,the selectivity of the 4%Bi-Sb_(2)WO_(6)sensor toward CO_(2)gas was enhanced relative to the Sb_(2)WO_(6)sensor.The fundamental mechanisms of gas sensing and the factors contributing to the improved CO_(2)response of 4%Bi-Sb_(2)WO_(6)micro spheres were investigated using density functional theory.Bi-doped Sb_(2)WO_(6)materials exhibit significant advantages in gas-sensing applications,including improved conductivity,enhanced gas adsorption capacity,increased reaction rates,good chemical stability,excellent selectivity,and the ability to adjust electron density.These characteristics enable Bi-doped Sb_(2)WO_(6)to demonstrate higher sensitivity and rapid response capabilities in gas sensors,making it suitable for practical applications.
