In this work,a new ZnO/CoNiO_(2)/CoO/C metal oxides composite is prepared by cost-effective hydrothermal method coupled with annealing process under N_(2) atmosphere.Notably,the oxidation-defect annealing environment ...In this work,a new ZnO/CoNiO_(2)/CoO/C metal oxides composite is prepared by cost-effective hydrothermal method coupled with annealing process under N_(2) atmosphere.Notably,the oxidation-defect annealing environment is conducive to both morphology and component of the composite,which flower-like ZnO/CoNiO_(2)/CoO/C is obtained.Benefited from good chemical stability of ZnO,high energy capacity of CoNiO_(2) and CoO and good conductivity of C,the as-prepared sample shows promising electrochemical behavior,including the specific capacity of 1435 C·g^(-1) at 1 A·g^(-1),capacity retention of 87.3%at 20 A·g^(-1),and cycling stability of 90.5%for 3000 cycles at 5 A·g^(-1),respectively.Furthermore,the prepared ZnO/CoNiO_(2)/CoO/C/NF//AC aqueous hybrid supercapacitors device delivers the best specific energy of 55.9 W·h·kg^(-1) at 850 W·kg^(-1).The results reflect that the as-prepared ZnO/CoNiO_(2)/CoO/C microflowers are considered as high performance electrode materials for supercapacitor,and the strategy mentioned in this paper is benefit to prepare mixed metal oxides composite for energy conversion and storage.展开更多
Atmospheric pollutants can deteriorate air quality and put human health at risk.There is a growing need for green,economical,and efficient technologies,among which catalytic elimination technology is the most promisin...Atmospheric pollutants can deteriorate air quality and put human health at risk.There is a growing need for green,economical,and efficient technologies,among which catalytic elimination technology is the most promising,to remove atmospheric pollutants.Two-dimensional transition metal oxides(2D TMOs)have recently become attractive catalysts due to their highly exposed active sites,excellent reactant transport properties,and extraordinary catalytic performance.This review systematically summarizes the topdown and bottom-up preparation methods of 2D TMOs and focuses on the specific applications of 2D TMOs in the catalytic elimination of atmospheric inorganic pollutants and volatile organic pollutants.The development of 2D TMOs in the catalytic elimination of atmospheric pollutants is prospected.This review is expected to provide design insights into efficient 2D TMOs to remove atmospheric pollutants.展开更多
The oxygen evolution reaction(OER) with slow kinetics is the rate-limiting step of electrochemical water splitting.A reasonable construction of interface nanostructures is the key to improving the OER efficiency and d...The oxygen evolution reaction(OER) with slow kinetics is the rate-limiting step of electrochemical water splitting.A reasonable construction of interface nanostructures is the key to improving the OER efficiency and durability of non-noble metal electrocatalysts.In this study,a FeOOH/NiCo_(2)S_(4) core-shell nanorod array with abundant heterogeneous interfaces and high density of active sites was successfully prepared by a microwave-as sis ted method.Experimental research and theoretical calculations show that the abundant strong coupling Ni/Co-S-Fe interface helps in adjusting the electronic structure of the material surface,optimizing the adsorption energy of the intermediate,and realizing an efficient catalytic process.The as-synthesized FeOOH/NiCo_(2)S_(4)/NF composite electrode exhibited lower overpotential(198 mV) and Tafel slope(62 mV·dec^(-1)) at a current density of 10 mA·cm^(-2)and excellent stability(approximately 100% retention after100 h) than the NiCo_(2)S_(4)/nickel foam(NF).In conclusion,constructing heterojunctions with complementary active materials is an effective strategy to design efficient and robust OER electrocatalysts.展开更多
Transition metal selenides have been widely studied as anode materials of sodium ion batteries(SIBs),however,the investigation of solid-electrolyte-interface(SEI)on these materials,which is critical to the electrochem...Transition metal selenides have been widely studied as anode materials of sodium ion batteries(SIBs),however,the investigation of solid-electrolyte-interface(SEI)on these materials,which is critical to the electrochemical performance of SIBs,remains at its infancy.Here in this paper,ZnSe@C nanoparticles were prepared from ZIF-8 and the SEI layers on these electrodes with and without reduced graphene oxide(rGO)layers were examined in details by X-ray photoelectron spectroscopies at varied charged/discharged states.It is observed that fast and complicated electrolyte decomposition reactions on ZnSe@C leads to quite thick SEI film and intercalation of solvated sodium ions through such thick SEI film results in slow ion diffusion kinetics and unstable electrode structure.However,the presence of rGO could efficiently suppress the decomposition of electrolyte,thus thin and stable SEI film was formed.ZnSe@C electrodes wrapped by rGO demonstrates enhanced interfacial charge transfer kinetics and high electrochemical performance,a capacity retention of 96.4%,after 1000 cycles at 5 A/g.This study might offer a simple avenue for the designing high performance anode materials through manipulation of SEI film.展开更多
Layered lithium-rich manganese-based oxide(LRMO)has the limitation of inevitable evolution of lattice oxygen release and layered structure transformation.Herein,a multilayer reconstruction strategy is applied to LRMO ...Layered lithium-rich manganese-based oxide(LRMO)has the limitation of inevitable evolution of lattice oxygen release and layered structure transformation.Herein,a multilayer reconstruction strategy is applied to LRMO via facile pyrolysis of potassium Prussian blue.The multilayer interface is visually observed using an atomic-resolution scanning transmission electron microscope and a high-resolution transmission electron microscope.Combined with the electrochemical characterization,the redox of lattice oxygen is suppressed during the initial charging.In situ X-ray diffraction and the high-resolution transmission electron microscope demonstrate that the suppressed evolution of lattice oxygen eliminates the variation in the unit cell parameters during initial(de)lithiation,which further prevents lattice distortion during long cycling.As a result,the initial Coulombic efficiency of the modified LRMO is up to 87.31%,and the rate capacity and long-term cycle stability also improved considerably.In this work,a facile surface reconstruction strategy is used to suppress vigorous anionic redox,which is expected to stimulate material design in high-performance lithium ion batteries.展开更多
The electronic structure and magnetism of eskolaite are studied by using first-principles calculations where the on-site Coulomb interaction and the exchange interaction are taken into account and the LSDA＋U method i...The electronic structure and magnetism of eskolaite are studied by using first-principles calculations where the on-site Coulomb interaction and the exchange interaction are taken into account and the LSDA＋U method is used. The calculated energies of magnetic configurations are very well fitted by the Heisenberg Hamiltonian with interactions in five neighbour shells; interaction with two nearest neighbours is found to be dominant. The Neel temperature is calculated in the spin-3/2 pair-cluster approximation. It is found that the measurements are in good agreement with the calculations of lattice parameters, density of states, band gap, local magnetic moment, and the Neel temperature for the values of U and J that are close to those obtained within the constrained occupation method. The band gap is of the Mott-Hubbard type.展开更多
Remarkable phenomena arise at well-defined heterostructures, composed of transition metal oxides, which is absent in the bulk counterpart, providing us a paradigm for exploring the various electron correlation effects...Remarkable phenomena arise at well-defined heterostructures, composed of transition metal oxides, which is absent in the bulk counterpart, providing us a paradigm for exploring the various electron correlation effects. The functional properties of such heterostructures have attracted much attention in the microelectronic and renewable energy fields. Exotic and unexpected states of matter could arise from the reconstruction and coupling among lattice, charge, orbital and spin at the interfaces. Aberration-corrected scanning transmission electron microscopy （STEM） is a powerful tool to visualize the lattice structure and electronic structure at the atomic scale. In the present study some novel phenomena of oxide heterostructures at the atomic scale are summarized and pointed out from the perspective of electron microscopy.展开更多
As a potential application of titanium-oxide nanoparticles, it is extremely important to investigate a detailed picture of the surface and interior structural properties of nanocrystalline materials, such as rutile an...As a potential application of titanium-oxide nanoparticles, it is extremely important to investigate a detailed picture of the surface and interior structural properties of nanocrystalline materials, such as rutile and anatase with diameters 7.0 and 4.5nm, respectively. X-ray absorption spectroscopy has been used to identify the local Ti environment and related electronic structure. We combine the experimental results at the Ti edge in both bulk and nano-crystals to determine the lattice distortion in terms of differently characteristic preedge features and the variation in the multiple-scattering region of X-ray absorption near-edge structure (XANES) spectra. The relationship between the transition peaks and the surface-to volume ratio is also discussed.展开更多
Li-rich layered oxide(LRLO)cathodes have been regarded as promising candidates for next-generation Li-ion batteries due to their exceptionally high energy density,which combines cationic and anionic redox activities.H...Li-rich layered oxide(LRLO)cathodes have been regarded as promising candidates for next-generation Li-ion batteries due to their exceptionally high energy density,which combines cationic and anionic redox activities.However,continuous voltage decay during cycling remains the primary obstacle for practical applications,which has yet to be fundamentally addressed.It is widely acknowledged that voltage decay originates from the irreversible migration of transition metal ions,which usually further exacerbates structural evolution and aggravates the irreversible oxygen redox reactions.Recently,constructing O2-type structure has been considered one of the most promising approaches for inhibiting voltage decay.In this review,the relationship between voltage decay and structural evolution is systematically elucidated.Strategies to suppress voltage decay are systematically summarized.Additionally,the design of O2-type structure and the corresponding mechanism of suppressing voltage decay are comprehensively discussed.Unfortunately,the reported O2-type LRLO cathodes still exhibit partially disordered structure with extended cycles.Herein,the factors that may cause the irreversible transition metal migrations in O2-type LRLO materials are also explored,while the perspectives and challenges for designing high-performance O2-type LRLO cathodes without voltage decay are proposed.展开更多
基金supported by the National Natural Science Foundation of China(22078215)Research Project by Shanxi Scholarship Council of China(2021-055)。
文摘In this work,a new ZnO/CoNiO_(2)/CoO/C metal oxides composite is prepared by cost-effective hydrothermal method coupled with annealing process under N_(2) atmosphere.Notably,the oxidation-defect annealing environment is conducive to both morphology and component of the composite,which flower-like ZnO/CoNiO_(2)/CoO/C is obtained.Benefited from good chemical stability of ZnO,high energy capacity of CoNiO_(2) and CoO and good conductivity of C,the as-prepared sample shows promising electrochemical behavior,including the specific capacity of 1435 C·g^(-1) at 1 A·g^(-1),capacity retention of 87.3%at 20 A·g^(-1),and cycling stability of 90.5%for 3000 cycles at 5 A·g^(-1),respectively.Furthermore,the prepared ZnO/CoNiO_(2)/CoO/C/NF//AC aqueous hybrid supercapacitors device delivers the best specific energy of 55.9 W·h·kg^(-1) at 850 W·kg^(-1).The results reflect that the as-prepared ZnO/CoNiO_(2)/CoO/C microflowers are considered as high performance electrode materials for supercapacitor,and the strategy mentioned in this paper is benefit to prepare mixed metal oxides composite for energy conversion and storage.
基金supported by the Strategic Priority Research Program of the Chinese Academy of Sciences,China(Nos.XDA23010300 and XDA23010000)National Natural Science Foundation of China(Nos.51878644 and 41573138)+1 种基金the National Key Research and Development Program of China(No.2016YFA0203000)the Plan for"National Youth Talents"of the Organization Department of the Central Committee。
文摘Atmospheric pollutants can deteriorate air quality and put human health at risk.There is a growing need for green,economical,and efficient technologies,among which catalytic elimination technology is the most promising,to remove atmospheric pollutants.Two-dimensional transition metal oxides(2D TMOs)have recently become attractive catalysts due to their highly exposed active sites,excellent reactant transport properties,and extraordinary catalytic performance.This review systematically summarizes the topdown and bottom-up preparation methods of 2D TMOs and focuses on the specific applications of 2D TMOs in the catalytic elimination of atmospheric inorganic pollutants and volatile organic pollutants.The development of 2D TMOs in the catalytic elimination of atmospheric pollutants is prospected.This review is expected to provide design insights into efficient 2D TMOs to remove atmospheric pollutants.
基金financially supported by Hainan Province Clinical Medical Center,the National Natural Science Foundation of China (Nos.81860373,51862006,81902154 and 82060386)Hainan Province Science and Technology Special Fund (Nos.ZDKJ2021029 and ZDYF2021SHFZ068)。
文摘The oxygen evolution reaction(OER) with slow kinetics is the rate-limiting step of electrochemical water splitting.A reasonable construction of interface nanostructures is the key to improving the OER efficiency and durability of non-noble metal electrocatalysts.In this study,a FeOOH/NiCo_(2)S_(4) core-shell nanorod array with abundant heterogeneous interfaces and high density of active sites was successfully prepared by a microwave-as sis ted method.Experimental research and theoretical calculations show that the abundant strong coupling Ni/Co-S-Fe interface helps in adjusting the electronic structure of the material surface,optimizing the adsorption energy of the intermediate,and realizing an efficient catalytic process.The as-synthesized FeOOH/NiCo_(2)S_(4)/NF composite electrode exhibited lower overpotential(198 mV) and Tafel slope(62 mV·dec^(-1)) at a current density of 10 mA·cm^(-2)and excellent stability(approximately 100% retention after100 h) than the NiCo_(2)S_(4)/nickel foam(NF).In conclusion,constructing heterojunctions with complementary active materials is an effective strategy to design efficient and robust OER electrocatalysts.
基金supported by the Fundamental Research Funds for Central Universities(SCUT Grant No.2019ZD22)the Guangdong Innovative and Entrepreneurial Research Team Program(No.2016ZT06N569)。
文摘Transition metal selenides have been widely studied as anode materials of sodium ion batteries(SIBs),however,the investigation of solid-electrolyte-interface(SEI)on these materials,which is critical to the electrochemical performance of SIBs,remains at its infancy.Here in this paper,ZnSe@C nanoparticles were prepared from ZIF-8 and the SEI layers on these electrodes with and without reduced graphene oxide(rGO)layers were examined in details by X-ray photoelectron spectroscopies at varied charged/discharged states.It is observed that fast and complicated electrolyte decomposition reactions on ZnSe@C leads to quite thick SEI film and intercalation of solvated sodium ions through such thick SEI film results in slow ion diffusion kinetics and unstable electrode structure.However,the presence of rGO could efficiently suppress the decomposition of electrolyte,thus thin and stable SEI film was formed.ZnSe@C electrodes wrapped by rGO demonstrates enhanced interfacial charge transfer kinetics and high electrochemical performance,a capacity retention of 96.4%,after 1000 cycles at 5 A/g.This study might offer a simple avenue for the designing high performance anode materials through manipulation of SEI film.
基金This work was financially supported by the High‐level Talents'Discipline Construction Fund of Shandong University(31370089963078)the Shandong Provincial Science and Technology Major Project(2018JM RH0211 and 2017CXGC1010)+3 种基金the Research Funds of Shandong University(10000089395121)the Natural Science Foundation of Shandong Province(ZR2019MEM052 and ZR2017MEM002)The National Natural Science Foundation of China(grant no.52002287)the Start‐up Funding of Wenzhou University are acknowledged.
文摘Layered lithium-rich manganese-based oxide(LRMO)has the limitation of inevitable evolution of lattice oxygen release and layered structure transformation.Herein,a multilayer reconstruction strategy is applied to LRMO via facile pyrolysis of potassium Prussian blue.The multilayer interface is visually observed using an atomic-resolution scanning transmission electron microscope and a high-resolution transmission electron microscope.Combined with the electrochemical characterization,the redox of lattice oxygen is suppressed during the initial charging.In situ X-ray diffraction and the high-resolution transmission electron microscope demonstrate that the suppressed evolution of lattice oxygen eliminates the variation in the unit cell parameters during initial(de)lithiation,which further prevents lattice distortion during long cycling.As a result,the initial Coulombic efficiency of the modified LRMO is up to 87.31%,and the rate capacity and long-term cycle stability also improved considerably.In this work,a facile surface reconstruction strategy is used to suppress vigorous anionic redox,which is expected to stimulate material design in high-performance lithium ion batteries.
基金Project supported by the Qianjiang Talent Project of Zhejiang Province, China (Grant No 2007R10028)the National Natural Science Foundation of China (Grant No 50802089)+2 种基金the Opening Project of State Key Laboratory of High Performance Ceramicsand Superfine Microstructure, China (Grant No SKL200805SIC)the Scientific Research Foundation for the Returned Overseas Chinese Scholars,Ministry of Education of China (Grant No [2008] 890)Natural Science Foundation of Zhejiang Province,China (Grant No Y407188)
文摘The electronic structure and magnetism of eskolaite are studied by using first-principles calculations where the on-site Coulomb interaction and the exchange interaction are taken into account and the LSDA＋U method is used. The calculated energies of magnetic configurations are very well fitted by the Heisenberg Hamiltonian with interactions in five neighbour shells; interaction with two nearest neighbours is found to be dominant. The Neel temperature is calculated in the spin-3/2 pair-cluster approximation. It is found that the measurements are in good agreement with the calculations of lattice parameters, density of states, band gap, local magnetic moment, and the Neel temperature for the values of U and J that are close to those obtained within the constrained occupation method. The band gap is of the Mott-Hubbard type.
基金supported by the National Key Basic Research Program of China(Grant No.2014CB921002)the Strategic Priority Research Program of Chinese Academy of Sciences(Grant No.XDB07030200)the National Natural Science Foundation of China(Grant Nos.51522212 and51421002)
文摘Remarkable phenomena arise at well-defined heterostructures, composed of transition metal oxides, which is absent in the bulk counterpart, providing us a paradigm for exploring the various electron correlation effects. The functional properties of such heterostructures have attracted much attention in the microelectronic and renewable energy fields. Exotic and unexpected states of matter could arise from the reconstruction and coupling among lattice, charge, orbital and spin at the interfaces. Aberration-corrected scanning transmission electron microscopy （STEM） is a powerful tool to visualize the lattice structure and electronic structure at the atomic scale. In the present study some novel phenomena of oxide heterostructures at the atomic scale are summarized and pointed out from the perspective of electron microscopy.
基金One of us (Z.Y. Wu) was supported by 100-Talent Research Program of The Chinese Academy of Sciences. One of the authors (K. Ibrahim) is grateful to the National Natural Science Foundation of China (NSFC) for financial support (Grant No. 10074063) The
文摘As a potential application of titanium-oxide nanoparticles, it is extremely important to investigate a detailed picture of the surface and interior structural properties of nanocrystalline materials, such as rutile and anatase with diameters 7.0 and 4.5nm, respectively. X-ray absorption spectroscopy has been used to identify the local Ti environment and related electronic structure. We combine the experimental results at the Ti edge in both bulk and nano-crystals to determine the lattice distortion in terms of differently characteristic preedge features and the variation in the multiple-scattering region of X-ray absorption near-edge structure (XANES) spectra. The relationship between the transition peaks and the surface-to volume ratio is also discussed.
基金funded by the National Natural Science Foundation of China(Grant Nos.22279092 and 5202780089).
文摘Li-rich layered oxide(LRLO)cathodes have been regarded as promising candidates for next-generation Li-ion batteries due to their exceptionally high energy density,which combines cationic and anionic redox activities.However,continuous voltage decay during cycling remains the primary obstacle for practical applications,which has yet to be fundamentally addressed.It is widely acknowledged that voltage decay originates from the irreversible migration of transition metal ions,which usually further exacerbates structural evolution and aggravates the irreversible oxygen redox reactions.Recently,constructing O2-type structure has been considered one of the most promising approaches for inhibiting voltage decay.In this review,the relationship between voltage decay and structural evolution is systematically elucidated.Strategies to suppress voltage decay are systematically summarized.Additionally,the design of O2-type structure and the corresponding mechanism of suppressing voltage decay are comprehensively discussed.Unfortunately,the reported O2-type LRLO cathodes still exhibit partially disordered structure with extended cycles.Herein,the factors that may cause the irreversible transition metal migrations in O2-type LRLO materials are also explored,while the perspectives and challenges for designing high-performance O2-type LRLO cathodes without voltage decay are proposed.
基金financially supported by the National Natural Science Foundation of China (No. 52102201, No. 52102200)the Basic and Applied Basic Research Foundation of Guangdong Province (No. 2021B1515130002)。
