A novel compound, (4,4'-Hbpy)3[NaMo8O26](4,4'-bpy)2(H2O)4 1 (bpy=bipydine), was synthesized by the hydrothermal method. Single-crystal X-ray diffraction shows that compound 1 belongs to the monoclinic system...A novel compound, (4,4'-Hbpy)3[NaMo8O26](4,4'-bpy)2(H2O)4 1 (bpy=bipydine), was synthesized by the hydrothermal method. Single-crystal X-ray diffraction shows that compound 1 belongs to the monoclinic system, space group C2/m with a=19.1921(5), b=18.6931(6), c=9.3821(3) A° β=104.8020(11)°, V=3254.22(17)A°^3 C50H51Mo8N10NaO30, Mr=2062.52, Z=2, F(000)=2016, μ=1.591 mm^-1 and Dc=2.105 g/cm^3. The final R=0.0283 and wR=0.0912 for 3118 observed reflections (I〉20(I)). Compound 1 contains the β-[Mo8O26]^4-anion, sodium ion, 4,4'-bpy and lattice crystalline water molecules. The β-[MosO26] units link the sodium ion to form a chain structure. The infinitechains of [Na(Mo8O26)]^3- blocks are surrounded by protonized 4,4'-bpy cations, 4,4'-bpy and lattice crystalline water molecules. The 2D-IR correlation spectroscopy study indicates that the stretching vibrations of Mo=O occur more preferentially due to the thermal effect. The TGA analysis shows that compound 1 has high thermal stability.展开更多
A number of useful techniques associated with two-dimensional correlation spectroscopy(2DCOS)to improve its performance and utility have been developed in the last 30years.Evolution of these 2DCOS techniques,including...A number of useful techniques associated with two-dimensional correlation spectroscopy(2DCOS)to improve its performance and utility have been developed in the last 30years.Evolution of these 2DCOS techniques,including some of the very recent developments,is reviewed with examples.Topics include merged or modified asynchronous 2Dcorrelation spectrum,two-dimensional codistribution spectroscopy(2DCDS),Pareto scaling,and null-space projection treatment of spectral dataset.展开更多
Ultrathin van der Waals(vdW)magnets provide a possibility to access magnetic ordering in the two-dimensional(2D)limit,which are expected to be applied in the spintronic devices.Raman spectroscopy is a powerful charact...Ultrathin van der Waals(vdW)magnets provide a possibility to access magnetic ordering in the two-dimensional(2D)limit,which are expected to be applied in the spintronic devices.Raman spectroscopy is a powerful characterization method to investigate the spin-related properties in 2D vdW magnets,including magnon and spin–lattice interaction,which are hardly accessible by other optical methods.In this paper,the recent progress of various magnetic properties in 2D vdW magnets studied by Raman spectroscopy is reviewed,including the magnetic transition,spin-wave,spin–lattice interaction,symmetry tuning induced by spin ordering,and nonreciprocal magneto-phonon Raman scattering.展开更多
The generalized two-dimensional correlation analysis based on time-resolved light scattering patterns (2D TRLS) has been employed to study the phase separation process of an epoxy-amine-polyethersulfone blend in whi...The generalized two-dimensional correlation analysis based on time-resolved light scattering patterns (2D TRLS) has been employed to study the phase separation process of an epoxy-amine-polyethersulfone blend in which the secondary phase separation takes place. The results of the 2D TRLS provided more detailed information that was not readily observed in the 1D TRLS patterns. (i) During the first process of phase separation, the sequential order of coarsening in size of the domains among the larger and smaller ones has been reversed between the diffusion regime and the hydrodynamic regime. (ii) The change of the larger domains in size, due to the hydrodynamic flow in the late stage of the first phase separation process, keeps on taking place earlier than that of the new domains appeared in the secondary phase separation process. (iii) During the secondary phase separation process the size growth of the smaller domains takes place earlier than that of the larger ones, probably due to the assumption that the coarsening mode could decrease the interface tension more quickly.展开更多
During the development of ultrathin two-dimensional(2D)materials,the appearance of ripples has been widely observed.However,the formation mechanisms and their influences are still rarely investigated,especially their ...During the development of ultrathin two-dimensional(2D)materials,the appearance of ripples has been widely observed.However,the formation mechanisms and their influences are still rarely investigated,especially their contributions to the electronic structures and optical properties.To compensate for the knowledge gap,we have carried out comprehensive theoretical studies on the monolayer WSe_(2) with a series of ripple structures from 0 to 12Åin different lattice sizes.The sensitivity of the formation energy,band structures,electronic structures,and optical properties to the ripple structures have been performed systematically for the first time.The formation of ripples in Armchair and zigzag simultaneously are more energetically favorable,leading to more flexible optimizations of the optoelectronic properties.The improved charge-locking effect and extension of absorption ranges indicate the significant role of ripple structures.The spontaneous formation of ripples is associated with orbital rearrangements and structural distortions.This leads to the unique charge carrier correlate inversion between W-5d and Se-4p orbitals,resulting in the pinning of the Fermi level.This work has supplied significant references to understand ultrathin 2D structures and benefit their future developments and applications in high-performance optoelectronic devices.展开更多
Liquid state methanol and ethanol under different temperatures have been investigated by FT-NIR(Fourier transform nearinfrared) spectroscopy,generalized two-dimensional(2D) correlation spectroscopy,and PCA(principal c...Liquid state methanol and ethanol under different temperatures have been investigated by FT-NIR(Fourier transform nearinfrared) spectroscopy,generalized two-dimensional(2D) correlation spectroscopy,and PCA(principal component analysis) . First,the FT-NIR spectra were measured over a temperature range of 30-64(or 30-71) °C,and then the 2D correlation spectra were computed.Combining near-infrared spectroscopy,generalized 2D correlation spectroscopy,and references,we analyzed the molecular structures(especially the hydrogen bond) of methanol and ethanol,and performed the NIR band assignments. The PCA method was employed to verify the results of the 2D analysis.This study will be helpful to the understanding of these reagents.展开更多
Two dimensional asynchronous spectra were used to characterize coordination between carbonyl group of butanone and metal ions by using an approach proposed in our recent paper.Spectral variation of n-π^*transition b...Two dimensional asynchronous spectra were used to characterize coordination between carbonyl group of butanone and metal ions by using an approach proposed in our recent paper.Spectral variation of n-π^*transition band of carbonyl group is used to probe the coordination even if metal ions does not possess any characteristic peak in spectra.Experimental results indicate that Ca^2+ and Al^3+ show considerable ability to coordinate with the carbonyl group of butanone and bring about spectral variation of the n-π-*transition band,which is manifested by cross peaks in 2D asynchronous spectra.展开更多
This paper reports the pH-induced structural changes in the surface immobilized poly(L-lysine)(PLL)film.Two-dimensional(2D) correlation analysis was applied to the Fourier transform infrared(FTIR)spectra of th...This paper reports the pH-induced structural changes in the surface immobilized poly(L-lysine)(PLL)film.Two-dimensional(2D) correlation analysis was applied to the Fourier transform infrared(FTIR)spectra of the surface-immobilized PLL film to examine the spectral changes induced by the alternations of the protonation state of the amino group in the side chain.Significant spectral changes in the FTIR spectra of the PLL film were observed between pH 7 and 8.The decrease in the protonation state of the amino group in the side chain induced spectral changes in the amino group as well as conformational changes in the alky]group in the side chain.From pH 1-8,the spectral changes in the amino and alkyl groups in the side chain occurred before those of the amide group in the main chain of the surface immobilized PLL film.展开更多
Metal binding of organic ligands can definitely affect its environmental behavior in waters,while information on the binding heterogeneity with different organic ligands is still lacked till now.In this study,the bind...Metal binding of organic ligands can definitely affect its environmental behavior in waters,while information on the binding heterogeneity with different organic ligands is still lacked till now.In this study,the binding of zinc with organic matters associated with cyanobacterial blooms,including dissolved organic matters(DOM) and attached organic matters(AOM),were studied by using fluorescence quenching titration combined with two-dimensional correlation spectroscopy(2D-COS).Metal-induced fluorescent quenching was obviously observed both for DOM and AOM,indicating the formation of metal-ligand complexes.Compared with the one-dimensional spectra,2D-COS revealed the sequences of metal-ligand interaction with the following orders:276 nm 〉 232 ran for DOM and232 nm 〉 276 nm for AOM.Furthermore,the modified Stern-Volmer model showed that the binding constant(logKM) of 276 nm in DOM was higher than that of 232 nm(4.93 vs.4.51),while AOM was characterized with a high binding affinity for 232 nm(log KM:4.83).The ranks of log KM values were consistent with the sequential orders derived from 2D-COS results both for the two samples.Fluorescence quenching titration combined with 2D-COS was an effective method to characterize the metal-ligand interaction.展开更多
Lanthanum modified materials have been widely used for the removal of hazardous anions.In this study,in situ ATR-FTIR and two-dimensional correlation analysis were employed to investigate the adsorption mechanism of a...Lanthanum modified materials have been widely used for the removal of hazardous anions.In this study,in situ ATR-FTIR and two-dimensional correlation analysis were employed to investigate the adsorption mechanism of arsenate(As(V)) on lanthanum-impregnated activated alumina(LAA).Our results showed that electrostatic interaction attracted As(V) anions to the LAA surface,and then As(V) could form monodentate configuration on the LAA surface at pH 5-9.The result of 2D-COS showed that two coexistent adsorbed As(V) species,H2AsO4^- and HAsO4^2-,were adsorbed on the LAA surface without specific sequence at different pH conditions,indicating a negligible role of the incorporated protons of As(V) on the adsorption affinity to LAA surface.The results of this study reveal insights into LAA surface complexes on the molecular scale and provide theoretical support to new metal oxides design for efficient arsenic removal.展开更多
A polyoxovanadium borate [Na(H2O)]2[Na(H2O)2]2[Cu(en)2][V12B18O54(OH)6]·(H3O)2·(H2O)18 1(en = ethylenediamine) has been hydrothermally synthesized and characterized by IR,two-dimensional infra...A polyoxovanadium borate [Na(H2O)]2[Na(H2O)2]2[Cu(en)2][V12B18O54(OH)6]·(H3O)2·(H2O)18 1(en = ethylenediamine) has been hydrothermally synthesized and characterized by IR,two-dimensional infrared(2D IR) correlation spectroscopy with magnetic and thermal perturba-tion,thermal IR spectroscopy,thermal gravimetric analysis and single-crystal X-ray diffraction.It crystallizes in triclinic,space group P with a = 12.981(3),b = 13.044(3),c = 14.208(3) ,α = 63.98(3),β = 77.17(3),γ = 14.208(3)°,V = 2001.0(8) 3,Z = 1,Mr = 2518.05,Dc = 2.090 g/cm-1,F(000) = 1255.0,Mu(mm-1) = 1.756,λ(MoKα) = 0.71073 ,R = 0.0625 and wR = 0.1952.In 1,the [V12B18O54(OH)6]8- units are connected by [Cu(en)2]2+,binuclear Na(1) and Na(2) to form a three-dimensional porous framework.展开更多
In recent years,few-layer or even monolayer ferromagnetic materials have drawn a great deal of attention due to the promising integration of two-dimensional(2D)magnets into next-generation spintronic devices.The SrRuO...In recent years,few-layer or even monolayer ferromagnetic materials have drawn a great deal of attention due to the promising integration of two-dimensional(2D)magnets into next-generation spintronic devices.The SrRuO_(3)monolayer is a rare example of stable 2D magnetism under ambient conditions,but only weak ferromagnetism or antiferromagnetism has been found.The biatomic layer SrRuO_(3)as another environmentally inert 2D magnetic system has been paid less attention heretofore.Here we study both the bi-atomic layer and monolayer SrRuO_(3)in(SrRuO_(3))n/(SrTiO_(3))m(n=1,2)superlattices in which the SrTiO3 serves as a non-magnetic and insulating space layer.Although the monolayer exhibits arguably weak ferromagnetism,we find that the bi-atomic layer exhibits exceedingly strong ferromagnetism with a Tc of 125 K and a saturation magnetization of 1.2μB/Ru,demonstrated by both superconducting quantum interference device(SQUID)magnetometry and element-specific X-ray circular dichroism.Moreover,in the bi-atomic layer SrRuO_(3),we demonstrate that random fluctuations and orbital reconstructions inevitably occurring in the 2D limit are critical to the electrical transport,but are much less critical to the ferromagnetism.Our study demonstrates that the bi-atomic layer SrRuO_(3)is an exceedingly strong 2D ferromagnetic oxide which has great potentials for applications of ultracompact spintronic devices.展开更多
Two-dimensional(2D)honeycomb-like materials have been widely studied due to their fascinating properties.In particular,2D honeycomb-like transition metal monolayers,which are good 2D ferromagnet candidates,have attrac...Two-dimensional(2D)honeycomb-like materials have been widely studied due to their fascinating properties.In particular,2D honeycomb-like transition metal monolayers,which are good 2D ferromagnet candidates,have attracted intense research interest.The honeycomb-like structure of hafnium,hafnene,has been successfully fabricated on the Ir(111)substrate.However,its electronic structure has not yet been directly elucidated.Here,we report the electronic structure of hafnene grown on the Ir(111)substrate using angle-resolved photoemission spectroscopy(ARPES).Our results indicate that the presence of spin-orbit coupling and Hubbard interaction suppresses the earlier predicted Dirac cones at the K points of the Brillouin zone.The observed band structure of hafnene near the Fermi level is very simple:an electron pocket centered at theΓpoint of the Brillouin zone.This electron pocket shows typical parabolic dispersion,and its estimated electron effective mass and electron density are approximately 1.8_(me)and 7×10^(14)cm^(-2),respectively.Our results demonstrate the existence of 2D electron gas in hafnene grown on the Ir(111)substrate and therefore provide key information for potential hafnene-based device applications.展开更多
Controlling the spatial distribution of functional groups on two-dimensional(2D)materials on a micrometer scale and below represents a fascinating opportunity to achieve anisotropic(opto)electronic properties of these...Controlling the spatial distribution of functional groups on two-dimensional(2D)materials on a micrometer scale and below represents a fascinating opportunity to achieve anisotropic(opto)electronic properties of these materials.Periodic patterns of covalent functionalization can lead to pericxJic potentials in the monolayer;however,creating such superstructures is very challenging.Here,we describe an original approach to the periodic functionalization of graphene induced by substrate patterning using a pulsed laser.Laser-induced periodic surface structures(LIPSS)are produced on silicon wafers with thermally-grown oxide layers.The irradiation conditions for the formation of UPSS confined at the SiO2/Si interface have been unravelled.LIPSS imprint their periodicity to the reactivity of the monolayer graphene placed on the substrate via modulation of its local doping level.This method is clean,straightforward and scalable with high spatial resolution.展开更多
A Keggin-type polyoxomolybdate[H2biim]{Ni(biim)3(SiMO12O40)}[biim =1H,1'H-[2,2']biimidazolyl]has been synthesized under hydrothermal condition and characterized by XRD,temperature-dependent IR,TG,temperature-ind...A Keggin-type polyoxomolybdate[H2biim]{Ni(biim)3(SiMO12O40)}[biim =1H,1'H-[2,2']biimidazolyl]has been synthesized under hydrothermal condition and characterized by XRD,temperature-dependent IR,TG,temperature-induced and magnetism-induced 2D infrared correlation spectroscopy(2D-IR COS)and UV-vis DRS in order to explore the relationship between structure and properties.Temperatureinduced 2D-IR COS spectroscopy indicates that the terminal Mo-Oμ/υbonds are more sensitive than the bridging Mo=Ot,bands to temperature variation,which is in agreement with the conclusion of temperature-dependent IR.Magnetism-dependent 2D-IR COS spectroscopy reveals the stretching vibration of the Mo=Ot,occurs prior to the stretching vibration of the Mo-Oμ/υ,which is due to the coordination environment and the valence of the Si atom.The stability of compound 1 is investigated via TG and temperature-dependent IR.In RhB degradation,compound 1 shows good photocatalytic abilities.展开更多
Emerging single-cell technologies create new opportunities for unraveling tumor heterogeneity.However,the development of high-content phenotyping platform is still at its infancy.Here,we develop a microfluidic chip fo...Emerging single-cell technologies create new opportunities for unraveling tumor heterogeneity.However,the development of high-content phenotyping platform is still at its infancy.Here,we develop a microfluidic chip for two-dimensional(2D)profiling of tumor chemotactic and molecular features at single cell resolution.Individual cells were captured by the triangular micropillar arrays in the cell-loading channel,facilitating downstream single-cell analysis.For 2D phenotyping,the chemotactic properties of tumor cells were visualized through cellular migratory behavior in microchannels,while their protein expression was profiled with multiplex surface enhanced Raman scattering(SERS)nanovectors,in which Raman reporter-embedded gold@silver core-shell nanoparticles(Au@Ag REPs)were modified with DNA aptamers targeting cellular surface proteins.As a proof of concept,breast cancer cells with diverse phenotypes were tested on the chip,demonstrating the capability of this platform for simultaneous chemotactic and molecular analysis.The chip is expected to provide a powerful tool for investigating tumor heterogeneity and promoting clinical precision medicine.展开更多
基金This work was supported by the Foundation of Education Committee of Fujian Province (K02028, JB04049), the State Key Laboratory of Structural Chemistry, and Science and Technology Foundation of Fuzhou University
文摘A novel compound, (4,4'-Hbpy)3[NaMo8O26](4,4'-bpy)2(H2O)4 1 (bpy=bipydine), was synthesized by the hydrothermal method. Single-crystal X-ray diffraction shows that compound 1 belongs to the monoclinic system, space group C2/m with a=19.1921(5), b=18.6931(6), c=9.3821(3) A° β=104.8020(11)°, V=3254.22(17)A°^3 C50H51Mo8N10NaO30, Mr=2062.52, Z=2, F(000)=2016, μ=1.591 mm^-1 and Dc=2.105 g/cm^3. The final R=0.0283 and wR=0.0912 for 3118 observed reflections (I〉20(I)). Compound 1 contains the β-[Mo8O26]^4-anion, sodium ion, 4,4'-bpy and lattice crystalline water molecules. The β-[MosO26] units link the sodium ion to form a chain structure. The infinitechains of [Na(Mo8O26)]^3- blocks are surrounded by protonized 4,4'-bpy cations, 4,4'-bpy and lattice crystalline water molecules. The 2D-IR correlation spectroscopy study indicates that the stretching vibrations of Mo=O occur more preferentially due to the thermal effect. The TGA analysis shows that compound 1 has high thermal stability.
文摘A number of useful techniques associated with two-dimensional correlation spectroscopy(2DCOS)to improve its performance and utility have been developed in the last 30years.Evolution of these 2DCOS techniques,including some of the very recent developments,is reviewed with examples.Topics include merged or modified asynchronous 2Dcorrelation spectrum,two-dimensional codistribution spectroscopy(2DCDS),Pareto scaling,and null-space projection treatment of spectral dataset.
基金Project supported by Beijing Natural Science Foundation,China(Grant No.JQ18014)the National Natural Science Foundation of China(Grant No.12074371)Strategic Priority Research Program of Chinese Academy of Sciences(Grant No.XDB28000000),and CAS Interdisciplinary Innovation Team.
文摘Ultrathin van der Waals(vdW)magnets provide a possibility to access magnetic ordering in the two-dimensional(2D)limit,which are expected to be applied in the spintronic devices.Raman spectroscopy is a powerful characterization method to investigate the spin-related properties in 2D vdW magnets,including magnon and spin–lattice interaction,which are hardly accessible by other optical methods.In this paper,the recent progress of various magnetic properties in 2D vdW magnets studied by Raman spectroscopy is reviewed,including the magnetic transition,spin-wave,spin–lattice interaction,symmetry tuning induced by spin ordering,and nonreciprocal magneto-phonon Raman scattering.
基金supported by the National Natural Science of Foundation of China(NSFC)(Nos.20674014, 20425415,20274010,50103003,20221402)
文摘The generalized two-dimensional correlation analysis based on time-resolved light scattering patterns (2D TRLS) has been employed to study the phase separation process of an epoxy-amine-polyethersulfone blend in which the secondary phase separation takes place. The results of the 2D TRLS provided more detailed information that was not readily observed in the 1D TRLS patterns. (i) During the first process of phase separation, the sequential order of coarsening in size of the domains among the larger and smaller ones has been reversed between the diffusion regime and the hydrodynamic regime. (ii) The change of the larger domains in size, due to the hydrodynamic flow in the late stage of the first phase separation process, keeps on taking place earlier than that of the new domains appeared in the secondary phase separation process. (iii) During the secondary phase separation process the size growth of the smaller domains takes place earlier than that of the larger ones, probably due to the assumption that the coarsening mode could decrease the interface tension more quickly.
基金support from the National Key R&D Program of China(No.2021YFA1501101)the National Natural Science Foundation of China/Research Grant Council of Hong Kong Joint Research Scheme(No.N_PolyU502/21)+3 种基金the funding for Projects of Strategic Importance of The Hong Kong Polytechnic University(Project Code:1-ZE2V)the Shenzhen Fundamental Research Scheme-General Program(No.JCYJ20220531090807017)the Natural Science Foundation of Guangdong Province(No.2023A1515012219)the Departmental General Research Fund(Project Code:ZVUL)from The Hong Kong Polytechnic University.
文摘During the development of ultrathin two-dimensional(2D)materials,the appearance of ripples has been widely observed.However,the formation mechanisms and their influences are still rarely investigated,especially their contributions to the electronic structures and optical properties.To compensate for the knowledge gap,we have carried out comprehensive theoretical studies on the monolayer WSe_(2) with a series of ripple structures from 0 to 12Åin different lattice sizes.The sensitivity of the formation energy,band structures,electronic structures,and optical properties to the ripple structures have been performed systematically for the first time.The formation of ripples in Armchair and zigzag simultaneously are more energetically favorable,leading to more flexible optimizations of the optoelectronic properties.The improved charge-locking effect and extension of absorption ranges indicate the significant role of ripple structures.The spontaneous formation of ripples is associated with orbital rearrangements and structural distortions.This leads to the unique charge carrier correlate inversion between W-5d and Se-4p orbitals,resulting in the pinning of the Fermi level.This work has supplied significant references to understand ultrathin 2D structures and benefit their future developments and applications in high-performance optoelectronic devices.
基金supported by the Medical Scientific Research Foundation of Guangdong Province,China(B2009043)
文摘Liquid state methanol and ethanol under different temperatures have been investigated by FT-NIR(Fourier transform nearinfrared) spectroscopy,generalized two-dimensional(2D) correlation spectroscopy,and PCA(principal component analysis) . First,the FT-NIR spectra were measured over a temperature range of 30-64(or 30-71) °C,and then the 2D correlation spectra were computed.Combining near-infrared spectroscopy,generalized 2D correlation spectroscopy,and references,we analyzed the molecular structures(especially the hydrogen bond) of methanol and ethanol,and performed the NIR band assignments. The PCA method was employed to verify the results of the 2D analysis.This study will be helpful to the understanding of these reagents.
基金financially supported by the National Natural Science Foundation of China(No.51373003)Beijing Natural Science Foundation(No.2122059)
文摘Two dimensional asynchronous spectra were used to characterize coordination between carbonyl group of butanone and metal ions by using an approach proposed in our recent paper.Spectral variation of n-π^*transition band of carbonyl group is used to probe the coordination even if metal ions does not possess any characteristic peak in spectra.Experimental results indicate that Ca^2+ and Al^3+ show considerable ability to coordinate with the carbonyl group of butanone and bring about spectral variation of the n-π-*transition band,which is manifested by cross peaks in 2D asynchronous spectra.
基金supported by Yeungnam University Research Grants in 2013a Human Resources Development Program of Korea Institute of Energy Technology Evaluation and Planning (KETEP) grant(No.20104010100580) funded by the Korean Ministry of Knowledge Economy
文摘This paper reports the pH-induced structural changes in the surface immobilized poly(L-lysine)(PLL)film.Two-dimensional(2D) correlation analysis was applied to the Fourier transform infrared(FTIR)spectra of the surface-immobilized PLL film to examine the spectral changes induced by the alternations of the protonation state of the amino group in the side chain.Significant spectral changes in the FTIR spectra of the PLL film were observed between pH 7 and 8.The decrease in the protonation state of the amino group in the side chain induced spectral changes in the amino group as well as conformational changes in the alky]group in the side chain.From pH 1-8,the spectral changes in the amino and alkyl groups in the side chain occurred before those of the amide group in the main chain of the surface immobilized PLL film.
基金funded by the National Natural Science Foundation of China(Nos.51479187,51209192)the China Postdoctoral Science Foundation(Nos.2014T70505+1 种基金2013M 540438)the PAPD,and the State Key Laboratory of Pollution Control and Resource Reuse Foundation(No.PCRRF13011)
文摘Metal binding of organic ligands can definitely affect its environmental behavior in waters,while information on the binding heterogeneity with different organic ligands is still lacked till now.In this study,the binding of zinc with organic matters associated with cyanobacterial blooms,including dissolved organic matters(DOM) and attached organic matters(AOM),were studied by using fluorescence quenching titration combined with two-dimensional correlation spectroscopy(2D-COS).Metal-induced fluorescent quenching was obviously observed both for DOM and AOM,indicating the formation of metal-ligand complexes.Compared with the one-dimensional spectra,2D-COS revealed the sequences of metal-ligand interaction with the following orders:276 nm 〉 232 ran for DOM and232 nm 〉 276 nm for AOM.Furthermore,the modified Stern-Volmer model showed that the binding constant(logKM) of 276 nm in DOM was higher than that of 232 nm(4.93 vs.4.51),while AOM was characterized with a high binding affinity for 232 nm(log KM:4.83).The ranks of log KM values were consistent with the sequential orders derived from 2D-COS results both for the two samples.Fluorescence quenching titration combined with 2D-COS was an effective method to characterize the metal-ligand interaction.
基金supported by the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB14020201)the National Basic Research Program of China(No. 2014CB441102)+1 种基金the National Natural Science Foundation of China(No.21477144)the Young Scientists Fund of RCEES, RCEES-QN-20130017F
文摘Lanthanum modified materials have been widely used for the removal of hazardous anions.In this study,in situ ATR-FTIR and two-dimensional correlation analysis were employed to investigate the adsorption mechanism of arsenate(As(V)) on lanthanum-impregnated activated alumina(LAA).Our results showed that electrostatic interaction attracted As(V) anions to the LAA surface,and then As(V) could form monodentate configuration on the LAA surface at pH 5-9.The result of 2D-COS showed that two coexistent adsorbed As(V) species,H2AsO4^- and HAsO4^2-,were adsorbed on the LAA surface without specific sequence at different pH conditions,indicating a negligible role of the incorporated protons of As(V) on the adsorption affinity to LAA surface.The results of this study reveal insights into LAA surface complexes on the molecular scale and provide theoretical support to new metal oxides design for efficient arsenic removal.
基金supported by the National Natural Science Foundation of China (20873021,21003020)Doctoral Fund of Ministry of Education of China (20093514120002)New Century Excellent Talent Supported Plan of Fujian Province (SXSJRC2007-21)
文摘A polyoxovanadium borate [Na(H2O)]2[Na(H2O)2]2[Cu(en)2][V12B18O54(OH)6]·(H3O)2·(H2O)18 1(en = ethylenediamine) has been hydrothermally synthesized and characterized by IR,two-dimensional infrared(2D IR) correlation spectroscopy with magnetic and thermal perturba-tion,thermal IR spectroscopy,thermal gravimetric analysis and single-crystal X-ray diffraction.It crystallizes in triclinic,space group P with a = 12.981(3),b = 13.044(3),c = 14.208(3) ,α = 63.98(3),β = 77.17(3),γ = 14.208(3)°,V = 2001.0(8) 3,Z = 1,Mr = 2518.05,Dc = 2.090 g/cm-1,F(000) = 1255.0,Mu(mm-1) = 1.756,λ(MoKα) = 0.71073 ,R = 0.0625 and wR = 0.1952.In 1,the [V12B18O54(OH)6]8- units are connected by [Cu(en)2]2+,binuclear Na(1) and Na(2) to form a three-dimensional porous framework.
基金the National Natural Science Foundation of China(Nos.52072244 and 12104305)the Science and Technology Commission of Shanghai Municipality(No.21JC1405000)+1 种基金the ShanghaiTech Startup Fund.This research used resources of the Advanced Photon Source,a U.S.Department of Energy(DOE)Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract(No.DE-AC02-06CH11357)the Advanced Light Source,a U.S.DOE Office of Science User Facility under Contract(No.DE-AC02-05CH11231).
文摘In recent years,few-layer or even monolayer ferromagnetic materials have drawn a great deal of attention due to the promising integration of two-dimensional(2D)magnets into next-generation spintronic devices.The SrRuO_(3)monolayer is a rare example of stable 2D magnetism under ambient conditions,but only weak ferromagnetism or antiferromagnetism has been found.The biatomic layer SrRuO_(3)as another environmentally inert 2D magnetic system has been paid less attention heretofore.Here we study both the bi-atomic layer and monolayer SrRuO_(3)in(SrRuO_(3))n/(SrTiO_(3))m(n=1,2)superlattices in which the SrTiO3 serves as a non-magnetic and insulating space layer.Although the monolayer exhibits arguably weak ferromagnetism,we find that the bi-atomic layer exhibits exceedingly strong ferromagnetism with a Tc of 125 K and a saturation magnetization of 1.2μB/Ru,demonstrated by both superconducting quantum interference device(SQUID)magnetometry and element-specific X-ray circular dichroism.Moreover,in the bi-atomic layer SrRuO_(3),we demonstrate that random fluctuations and orbital reconstructions inevitably occurring in the 2D limit are critical to the electrical transport,but are much less critical to the ferromagnetism.Our study demonstrates that the bi-atomic layer SrRuO_(3)is an exceedingly strong 2D ferromagnetic oxide which has great potentials for applications of ultracompact spintronic devices.
基金This work is supported by the National Key Research and Development Program of China(Nos.2017YFA0303600 and 2020YFA0308800)the National Natural Science Foundation of China(Nos.11974364,11674367,U2032207,92163206,11974045,and 61725107)+2 种基金the Natural Science Foundation of Zhejiang,China(No.LZ18A040002)the Ningbo Science and Technology Bureau(No.2018B10060)S.L.H.would like also to acknowledge the Ningbo 3315 program.
文摘Two-dimensional(2D)honeycomb-like materials have been widely studied due to their fascinating properties.In particular,2D honeycomb-like transition metal monolayers,which are good 2D ferromagnet candidates,have attracted intense research interest.The honeycomb-like structure of hafnium,hafnene,has been successfully fabricated on the Ir(111)substrate.However,its electronic structure has not yet been directly elucidated.Here,we report the electronic structure of hafnene grown on the Ir(111)substrate using angle-resolved photoemission spectroscopy(ARPES).Our results indicate that the presence of spin-orbit coupling and Hubbard interaction suppresses the earlier predicted Dirac cones at the K points of the Brillouin zone.The observed band structure of hafnene near the Fermi level is very simple:an electron pocket centered at theΓpoint of the Brillouin zone.This electron pocket shows typical parabolic dispersion,and its estimated electron effective mass and electron density are approximately 1.8_(me)and 7×10^(14)cm^(-2),respectively.Our results demonstrate the existence of 2D electron gas in hafnene grown on the Ir(111)substrate and therefore provide key information for potential hafnene-based device applications.
基金The work was supported by project No.18-09055Y and 20-08633X awarded by Czech Science FoundationThe research of I.M.,J.S.,T.J.-Y.D.,and N.M.B.is financed by the European Regional Development Fund and the state budget of the Czech Republic(project BIATRI,No.CZ.02.1.01/0.0/0.0/15_003/0000445,project HiLASE CoE,No.CZ.02.1.01/0.0/0.0/15_006/0000674,programme NPU I,project No.LO1602)+3 种基金The work was further supported by European Regional Development Fund,OP RDE,Project:“Carbon allotropes with rationalized nanointerfaces and nanolinks for environmental and biomedical applications”(No.CZ.02.1.01/0.0/0.0/16_026/0008382)The authors also acknowledge the assistance provided by the Research Infrastructures NanoEnviCz(No.LM2015073)supported by the Ministry of EducationYouth and Sports of the Czech Republic and the project Pro-NanoEnviCz(No.CZ.02.1.01/0.0/0.0/16_013/0001821)supported by the Ministry of EducationYouth and Sports of the Czech Republic and the European Union-European Structural and Investments Funds in the frame of Operational Programme Research Development and Education.
文摘Controlling the spatial distribution of functional groups on two-dimensional(2D)materials on a micrometer scale and below represents a fascinating opportunity to achieve anisotropic(opto)electronic properties of these materials.Periodic patterns of covalent functionalization can lead to pericxJic potentials in the monolayer;however,creating such superstructures is very challenging.Here,we describe an original approach to the periodic functionalization of graphene induced by substrate patterning using a pulsed laser.Laser-induced periodic surface structures(LIPSS)are produced on silicon wafers with thermally-grown oxide layers.The irradiation conditions for the formation of UPSS confined at the SiO2/Si interface have been unravelled.LIPSS imprint their periodicity to the reactivity of the monolayer graphene placed on the substrate via modulation of its local doping level.This method is clean,straightforward and scalable with high spatial resolution.
基金financially supported by the National Natural Science Foundation of China(No.51373003)Beijing Natural Science Foundation(No.2122059)Open Fund of State Key Laboratory of Structural Chemistry(No.20130015) and Science
文摘A Keggin-type polyoxomolybdate[H2biim]{Ni(biim)3(SiMO12O40)}[biim =1H,1'H-[2,2']biimidazolyl]has been synthesized under hydrothermal condition and characterized by XRD,temperature-dependent IR,TG,temperature-induced and magnetism-induced 2D infrared correlation spectroscopy(2D-IR COS)and UV-vis DRS in order to explore the relationship between structure and properties.Temperatureinduced 2D-IR COS spectroscopy indicates that the terminal Mo-Oμ/υbonds are more sensitive than the bridging Mo=Ot,bands to temperature variation,which is in agreement with the conclusion of temperature-dependent IR.Magnetism-dependent 2D-IR COS spectroscopy reveals the stretching vibration of the Mo=Ot,occurs prior to the stretching vibration of the Mo-Oμ/υ,which is due to the coordination environment and the valence of the Si atom.The stability of compound 1 is investigated via TG and temperature-dependent IR.In RhB degradation,compound 1 shows good photocatalytic abilities.
基金This study was supported by the National Science Fund for Excellent Young Scholars(No.61822503)the National Natural Science Foundation of China(Nos.62175030 and 62175027)+3 种基金China Postdoctoral Science Foundation(No.2021TQ0147)Jiangsu Innovation and Entrepreneurship Program(No.JSSCBS20210126)Nanjing Science and Technology Innovation Project for Returned Overseas Chinese Scholars(No.1106000308)the Fundamental Research Funds for the Central Universities(Nos.3206002104D and 3206002108A1).
文摘Emerging single-cell technologies create new opportunities for unraveling tumor heterogeneity.However,the development of high-content phenotyping platform is still at its infancy.Here,we develop a microfluidic chip for two-dimensional(2D)profiling of tumor chemotactic and molecular features at single cell resolution.Individual cells were captured by the triangular micropillar arrays in the cell-loading channel,facilitating downstream single-cell analysis.For 2D phenotyping,the chemotactic properties of tumor cells were visualized through cellular migratory behavior in microchannels,while their protein expression was profiled with multiplex surface enhanced Raman scattering(SERS)nanovectors,in which Raman reporter-embedded gold@silver core-shell nanoparticles(Au@Ag REPs)were modified with DNA aptamers targeting cellular surface proteins.As a proof of concept,breast cancer cells with diverse phenotypes were tested on the chip,demonstrating the capability of this platform for simultaneous chemotactic and molecular analysis.The chip is expected to provide a powerful tool for investigating tumor heterogeneity and promoting clinical precision medicine.