MgH_(2) is considered one of the most promising hydrogen storage materials because of its safety,high efficiency,high hydrogen storage quantity and low cost characteristics.But some shortcomings are still existed:high...MgH_(2) is considered one of the most promising hydrogen storage materials because of its safety,high efficiency,high hydrogen storage quantity and low cost characteristics.But some shortcomings are still existed:high operating temperature and poor hydrogen absorption dynamics,which limit its application.Porous Ni_(3)ZnC_(0.7)/Ni loaded carbon nanotubes microspheres(NZC/Ni@CNT)is prepared by facile filtration and calcination method.Then the different amount of NZC/Ni@CNT(2.5,5.0 and 7.5 wt%)is added to the MgH_(2) by ball milling.Among the three samples with different amount of NZC/Ni@CNT(2.5,5.0 and 7.5 wt%),the MgH_(2)-5 wt%NZC/Ni@CNT composite exhibits the best hydrogen storage performances.After testing,the MgH_(2)-5 wt%NZC/Ni@CNT begins to release hydrogen at around 110℃ and hydrogen absorption capacity reaches 2.34 wt%H_(2) at 80℃ within 60 min.Moreover,the composite can release about 5.36 wt%H_(2) at 300℃.In addition,hydrogen absorption and desorption activation energies of the MgH_(2)-5 wt%NZC/Ni@CNT composite are reduced to 37.28 and 84.22 KJ/mol H_(2),respectively.The in situ generated Mg_(2)NiH_(4)/Mg_(2)Ni can serve as a"hydrogen pump"that plays the main role in providing more activation sites and hydrogen diffusion channels which promotes H_(2) dissociation during hydrogen absorption process.In addition,the evenly dispersed Zn and MgZn2 in Mg and MgH_(2) could provide sites for Mg/MgH_(2) nucleation and hydrogen diffusion channel.This attempt clearly proved that the bimetallic carbide Ni_(3)ZnC_(0.7) is a effective additive for the hydrogen storage performances modification of MgH_(2),and the facile synthesis of the Ni_(3)ZnC_(0.7)/Ni@CNT can provide directions of better designing high performance carbide catalysts for improving MgH_(2).展开更多
Hydrogen is an ideal clean energy because of its high calorific value and abundance of sources.However,storing hydrogen in a compact,inexpensive,and safe manner is the main restriction on the extensive utilization of ...Hydrogen is an ideal clean energy because of its high calorific value and abundance of sources.However,storing hydrogen in a compact,inexpensive,and safe manner is the main restriction on the extensive utilization of hydrogen energy.Magnesium(Mg)-based hydrogen storage material is considered a reliable solid hydrogen storage material with the advantages of high hydrogen storage capacity(7.6wt%),good performance,and low cost.However,the high thermodynamic stability and slow kinetics of Mg-based hydrogen storage materials have to be overcome.In this paper,we will review the recent advances in the nanoconfinement of Mg-related hydrogen storage materials by loading Mg particles on different supporting materials,including carbons,metal-organic frameworks,and other materials.Perspectives are also provided for designing high-performance Mg-based materials using nanoconfinement.展开更多
Both macroscopic composition and microstructure should be considered for reasonable microwave ab-sorbent designing.In this study,Co_(3)O_(4)@reduced graphene oxide(rGO)/Celery stalks derived carbon(CDC)was prepared by...Both macroscopic composition and microstructure should be considered for reasonable microwave ab-sorbent designing.In this study,Co_(3)O_(4)@reduced graphene oxide(rGO)/Celery stalks derived carbon(CDC)was prepared by loading Co_(3)O_(4) particles into rGO and biomass-derived carbon mixture through oxidation precipitation.By changing the mass ratio of rGO to CDC,the dielectric and impedance matching proper-ties of the composites can be easily regulated.The RL min value of Co_(3)O_(4)@rGO/CDC_(13) composite(weight ratio for rGO:CDC is 1:3)reaches-84.3 dB with a thickness of 4.6 mm,and the widest effective band-width can be obtained at 4.5 GHz with a matching thickness of 2.8 mm.The Co_(3)O_(4)@rGO/CDC_(13) compos-ite with multiple components(Co_(3)O_(4),CDC,rGO)and 3D net structure produces magnetic/dielectric loss combinations,interfacial polarization,and multiple reflections and scattering,and the CDC with half tube and half sheet structure is conducive to the optimization of impedance matching.The strategy of co-regulating dielectric properties of materials with double carbon provides a novel pathway for the prepa-ration of lightweight,low-cost,and high-performance absorbers.展开更多
Three-dimensional holey nitrogen-doped carbon matrixes decorated with molybdenum dioxide(MoO_(2))nanoparticles have been successfully synthesized via a NaCl-assisted template strategy.The obtained MoO_(2)/C composites...Three-dimensional holey nitrogen-doped carbon matrixes decorated with molybdenum dioxide(MoO_(2))nanoparticles have been successfully synthesized via a NaCl-assisted template strategy.The obtained MoO_(2)/C composites offered multi-advantages,including higher specific surface area,more active sites,more ions/electrons transmission channels,and shorter transmission path due to the synergistic effect of the uniformly distributed MoO_(2) nanoparticles and porous carbon structure.Especially,the oxygen vacancies were introduced into the prepared composites and enhanced the Li^(+)intercalation/deintercalation process during electrochemical cycling by the Coulomb force.The existence of the local built-in electric field was proved by experimental data,differential charge density distribution,and density of states calculation.The uniquely designed structure and introduced oxygen vacancy defects endowed the MoO_(2)/C composites with excellent electrochemical properties.In view of the synergistic effect of the uniquely designed morphology and introduced oxygen vacancy defects,the MoO_(2)/C composites exhibited superior electrochemical performance of a high capacity of 918.2 mAh g^(-1) at 0.1 A g^(-1) after 130 cycles,562.1 mAh g^(-1) at 1.0 A g^(-1) after 1000 cycles,and a capacity of 181.25 mAh g^(-1) even at 20.0 A g^(-1).This strategy highlights the path to promote the commercial application of MoO_(2)-based and other transition metal oxide electrodes for energy storage devices.展开更多
The microscopic morphology of electromagnetic wave absorbers influences the multiple reflections of electromagnetic waves and impedance matching,determining the absorption properties.Herein,the urchin-shaped bimetalli...The microscopic morphology of electromagnetic wave absorbers influences the multiple reflections of electromagnetic waves and impedance matching,determining the absorption properties.Herein,the urchin-shaped bimetallic nickel-cobalt oxide/carbon(NiCo_(2)O_(4)/C)composites are prepared via a hy-drothermal route,whose absorption properties are investigated by different morphologies regulated by changing calcination temperature.A minimum reflection loss(RL_(min))of-75.26 dB is achieved at a match-ing thickness of 1.5 mm,and the effective absorption bandwidth(EAB)of 8.96 GHz is achieved at 2 mm.Multi-advantages of the synthesized NiCo_(2)O_(4)/C composites contribute to satisfactory absorption proper-ties.First,the interweaving of the needle-like structures increases the opportunities for scattering and multiple reflections of incident electromagnetic waves,and builds up a conductive network to facilitate the enhancement of conductive losses.Second,the carbon component in the NiCo_(2)O_(4)/C composites en-hances the interfacial polarization and reduces the density of the absorber.Besides,generous oxygen va-cancy defects are introduced into the NiCo_(2)O_(4)/C composites,which induces defect polarization and dipole polarization.In summary,the ternary coordination of components,defects and morphology led to out-standing electromagnetic wave absorption,which lightened the path for improving the electromagnetic wave absorption property and enriching the family of NiCo_(2)O_(4) absorbers with excellent performance.展开更多
Herein,the core-shell structured N-doped carbon coated Fe7S8 nano-aggregates(Fe7S8@NC)were controllably prepared via a simple three-step synthesis strategy.The appropriate thickness of N-doped carbon layer outside Fe7...Herein,the core-shell structured N-doped carbon coated Fe7S8 nano-aggregates(Fe7S8@NC)were controllably prepared via a simple three-step synthesis strategy.The appropriate thickness of N-doped carbon layer outside Fe7S8 nano-aggregates can not only inhibit the particle pulverization induced by the big volume changes of Fe7S8,but can increase the electron transfer efficiency.The hierarchical Fe7S8 nano-aggregates composed of some primary nanoparticles can accelerate the lithium or sodium diffusion kinetics.As anode materials for Li-ion batteries(LIBs),the well-designed Fe7S8@NC nanocomposites exhibit outstanding lithium storage performance,which is better than that of pure Fe7S8,Fe3O4@NC and Fe7S8@C.Among these nanocomposites,the N-doped carbon coated Fe7S8 with carbon content of 26.87 wt.%shows a high reversible specific capacity of 833 mAh·g^−1 after 1,000 cycles at a high current density of 2 A·g^−1.The above electrode also shows excellent high rate sodium storage performance.The experimental and theoretical analyses indicate that the outstanding electrochemical performance could be attributed to the synergistic effect of hierarchical Fe7S8 nanostructure and conductive N-doped carbon layer.The quantitative kinetic analysis indicates that the charge storage of Fe7S8@NC electrode is a combination of diffusion-controlled battery behavior and surface-induced capacitance behavior.展开更多
Confined metal clusters as sub-nanometer reactors for electrocatalytic N_(2) reduction reaction(eNRR)have received increasing attention due to the unique metal-metal interaction and higher activity than singleatom cat...Confined metal clusters as sub-nanometer reactors for electrocatalytic N_(2) reduction reaction(eNRR)have received increasing attention due to the unique metal-metal interaction and higher activity than singleatom catalysts.Herein,the inspiration of the superior capacitance and unique microenvironment with regular surface cavities of the porous boron nitride(p-BN)nanosheets,we systematically studied the catalytic activity for NRR of transition-metal single-clusters in the triplet form(V_(3),Fe_(3),Mo_(3) and W_(3))confined in the surface cavities of the p-BN sheets by spin-polarized density functional theory(DFT)calculations.After a two-step screening strategy,Mo_(3)@p-BN was found to have high catalytic activity and selectivity with a rather low limiting potential(-0.34 V)for the NRR.The anchored Mo_(3) singlecluster can be stably embedded on the surface cavities of the substrate preventing the diffusion of the active Mo atoms.More importantly,the Mo atoms in the Mo_(3) single-cluster would act as“cache”to accelerate electron transfer between active metal centers and nitrogen-containing intermediates via the intimate Mo-Mo interactions.The cooperation of Mo atoms can also provide a large number of occupied and unoccupied d orbitals to make the"donation-backdonation"mechanism more effective.This work not only provides a quite promising electrocatalyst for NRR,but also brings new insights into the rational design of triple-atom NRR catalysts.展开更多
基金supported by research programs of National Natural Science Foundation of China(52101274,51731002)Natural Science Foundation of Shandong Province(No.ZR2020QE011)Youth Top Talent Foundation of Yantai University(2219008).
文摘MgH_(2) is considered one of the most promising hydrogen storage materials because of its safety,high efficiency,high hydrogen storage quantity and low cost characteristics.But some shortcomings are still existed:high operating temperature and poor hydrogen absorption dynamics,which limit its application.Porous Ni_(3)ZnC_(0.7)/Ni loaded carbon nanotubes microspheres(NZC/Ni@CNT)is prepared by facile filtration and calcination method.Then the different amount of NZC/Ni@CNT(2.5,5.0 and 7.5 wt%)is added to the MgH_(2) by ball milling.Among the three samples with different amount of NZC/Ni@CNT(2.5,5.0 and 7.5 wt%),the MgH_(2)-5 wt%NZC/Ni@CNT composite exhibits the best hydrogen storage performances.After testing,the MgH_(2)-5 wt%NZC/Ni@CNT begins to release hydrogen at around 110℃ and hydrogen absorption capacity reaches 2.34 wt%H_(2) at 80℃ within 60 min.Moreover,the composite can release about 5.36 wt%H_(2) at 300℃.In addition,hydrogen absorption and desorption activation energies of the MgH_(2)-5 wt%NZC/Ni@CNT composite are reduced to 37.28 and 84.22 KJ/mol H_(2),respectively.The in situ generated Mg_(2)NiH_(4)/Mg_(2)Ni can serve as a"hydrogen pump"that plays the main role in providing more activation sites and hydrogen diffusion channels which promotes H_(2) dissociation during hydrogen absorption process.In addition,the evenly dispersed Zn and MgZn2 in Mg and MgH_(2) could provide sites for Mg/MgH_(2) nucleation and hydrogen diffusion channel.This attempt clearly proved that the bimetallic carbide Ni_(3)ZnC_(0.7) is a effective additive for the hydrogen storage performances modification of MgH_(2),and the facile synthesis of the Ni_(3)ZnC_(0.7)/Ni@CNT can provide directions of better designing high performance carbide catalysts for improving MgH_(2).
基金financially supported by the research programs of the National Natural Science Foundation of China (No. 52101274)the Natural Science Foundation of Shandong Province, China (No. ZR2020QE011)the Youth Top Talent Foundation of Yantai University, China (No. 2219008)
文摘Hydrogen is an ideal clean energy because of its high calorific value and abundance of sources.However,storing hydrogen in a compact,inexpensive,and safe manner is the main restriction on the extensive utilization of hydrogen energy.Magnesium(Mg)-based hydrogen storage material is considered a reliable solid hydrogen storage material with the advantages of high hydrogen storage capacity(7.6wt%),good performance,and low cost.However,the high thermodynamic stability and slow kinetics of Mg-based hydrogen storage materials have to be overcome.In this paper,we will review the recent advances in the nanoconfinement of Mg-related hydrogen storage materials by loading Mg particles on different supporting materials,including carbons,metal-organic frameworks,and other materials.Perspectives are also provided for designing high-performance Mg-based materials using nanoconfinement.
基金supported by the National Natural Science Foundation of China(No.52101274)the Natural Science Foundation of Shandong Province(No.ZR2020QE011)the Youth Top Talent Foundation of Yantai University(No.2219008).
文摘Both macroscopic composition and microstructure should be considered for reasonable microwave ab-sorbent designing.In this study,Co_(3)O_(4)@reduced graphene oxide(rGO)/Celery stalks derived carbon(CDC)was prepared by loading Co_(3)O_(4) particles into rGO and biomass-derived carbon mixture through oxidation precipitation.By changing the mass ratio of rGO to CDC,the dielectric and impedance matching proper-ties of the composites can be easily regulated.The RL min value of Co_(3)O_(4)@rGO/CDC_(13) composite(weight ratio for rGO:CDC is 1:3)reaches-84.3 dB with a thickness of 4.6 mm,and the widest effective band-width can be obtained at 4.5 GHz with a matching thickness of 2.8 mm.The Co_(3)O_(4)@rGO/CDC_(13) compos-ite with multiple components(Co_(3)O_(4),CDC,rGO)and 3D net structure produces magnetic/dielectric loss combinations,interfacial polarization,and multiple reflections and scattering,and the CDC with half tube and half sheet structure is conducive to the optimization of impedance matching.The strategy of co-regulating dielectric properties of materials with double carbon provides a novel pathway for the prepa-ration of lightweight,low-cost,and high-performance absorbers.
基金financially supported by the National Natural Science Foundation of China(No.52207249)the research program of Top Talent Project of Yantai University(No.1115/2220001)+1 种基金the Yantai Basic Research Project(No.2022JCYJ04)the Science Fund of Shandong Laboratory of Advanced Materials and Green Manufacturing(No.AMGM2021F11).
文摘Three-dimensional holey nitrogen-doped carbon matrixes decorated with molybdenum dioxide(MoO_(2))nanoparticles have been successfully synthesized via a NaCl-assisted template strategy.The obtained MoO_(2)/C composites offered multi-advantages,including higher specific surface area,more active sites,more ions/electrons transmission channels,and shorter transmission path due to the synergistic effect of the uniformly distributed MoO_(2) nanoparticles and porous carbon structure.Especially,the oxygen vacancies were introduced into the prepared composites and enhanced the Li^(+)intercalation/deintercalation process during electrochemical cycling by the Coulomb force.The existence of the local built-in electric field was proved by experimental data,differential charge density distribution,and density of states calculation.The uniquely designed structure and introduced oxygen vacancy defects endowed the MoO_(2)/C composites with excellent electrochemical properties.In view of the synergistic effect of the uniquely designed morphology and introduced oxygen vacancy defects,the MoO_(2)/C composites exhibited superior electrochemical performance of a high capacity of 918.2 mAh g^(-1) at 0.1 A g^(-1) after 130 cycles,562.1 mAh g^(-1) at 1.0 A g^(-1) after 1000 cycles,and a capacity of 181.25 mAh g^(-1) even at 20.0 A g^(-1).This strategy highlights the path to promote the commercial application of MoO_(2)-based and other transition metal oxide electrodes for energy storage devices.
基金financially supported by the National Natu-ral Science Foundation of China(No.52207249)the Natural Sci-ence Foundation of Shandong Province(No.ZR2022ME089)+2 种基金the research program of Top Talent Project of Yantai University(No.1115/2220001)the Yantai Basic Research Project(No.2022JCYJ04)the Science Fund of Shandong Laboratory of Advanced Ma-terials and Green Manufacturing(No.AMGM2021F11).The au-thors would like to thank the Deanship of Scientific Research at Umm Al-Qura University for supporting this work by Grant Code:22UQU4320141DSR72.
文摘The microscopic morphology of electromagnetic wave absorbers influences the multiple reflections of electromagnetic waves and impedance matching,determining the absorption properties.Herein,the urchin-shaped bimetallic nickel-cobalt oxide/carbon(NiCo_(2)O_(4)/C)composites are prepared via a hy-drothermal route,whose absorption properties are investigated by different morphologies regulated by changing calcination temperature.A minimum reflection loss(RL_(min))of-75.26 dB is achieved at a match-ing thickness of 1.5 mm,and the effective absorption bandwidth(EAB)of 8.96 GHz is achieved at 2 mm.Multi-advantages of the synthesized NiCo_(2)O_(4)/C composites contribute to satisfactory absorption proper-ties.First,the interweaving of the needle-like structures increases the opportunities for scattering and multiple reflections of incident electromagnetic waves,and builds up a conductive network to facilitate the enhancement of conductive losses.Second,the carbon component in the NiCo_(2)O_(4)/C composites en-hances the interfacial polarization and reduces the density of the absorber.Besides,generous oxygen va-cancy defects are introduced into the NiCo_(2)O_(4)/C composites,which induces defect polarization and dipole polarization.In summary,the ternary coordination of components,defects and morphology led to out-standing electromagnetic wave absorption,which lightened the path for improving the electromagnetic wave absorption property and enriching the family of NiCo_(2)O_(4) absorbers with excellent performance.
基金The authors thank the National Natural Science Foundation of China(No.51772257)the Major Basic Research Project of Shandong Natural Science Foundation(No.ZR2018ZC1459)Doctor Foundation of Shandong Province(No.ZR2017BB081)for financial support.
文摘Herein,the core-shell structured N-doped carbon coated Fe7S8 nano-aggregates(Fe7S8@NC)were controllably prepared via a simple three-step synthesis strategy.The appropriate thickness of N-doped carbon layer outside Fe7S8 nano-aggregates can not only inhibit the particle pulverization induced by the big volume changes of Fe7S8,but can increase the electron transfer efficiency.The hierarchical Fe7S8 nano-aggregates composed of some primary nanoparticles can accelerate the lithium or sodium diffusion kinetics.As anode materials for Li-ion batteries(LIBs),the well-designed Fe7S8@NC nanocomposites exhibit outstanding lithium storage performance,which is better than that of pure Fe7S8,Fe3O4@NC and Fe7S8@C.Among these nanocomposites,the N-doped carbon coated Fe7S8 with carbon content of 26.87 wt.%shows a high reversible specific capacity of 833 mAh·g^−1 after 1,000 cycles at a high current density of 2 A·g^−1.The above electrode also shows excellent high rate sodium storage performance.The experimental and theoretical analyses indicate that the outstanding electrochemical performance could be attributed to the synergistic effect of hierarchical Fe7S8 nanostructure and conductive N-doped carbon layer.The quantitative kinetic analysis indicates that the charge storage of Fe7S8@NC electrode is a combination of diffusion-controlled battery behavior and surface-induced capacitance behavior.
基金financially supported by the National Natural Science Foundation of China(Nos.21771182,21501177 and 21673240)the Guangdong Innovation Research Team for Higher Education(No.2017KCXTD030)+1 种基金the High-level Talents Project of Dongguan University of Technology(No.KCYKYQD2017017)the Open Project Program of the State Key Laboratory of Structural Chemistry,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences(No.20200006)。
文摘Confined metal clusters as sub-nanometer reactors for electrocatalytic N_(2) reduction reaction(eNRR)have received increasing attention due to the unique metal-metal interaction and higher activity than singleatom catalysts.Herein,the inspiration of the superior capacitance and unique microenvironment with regular surface cavities of the porous boron nitride(p-BN)nanosheets,we systematically studied the catalytic activity for NRR of transition-metal single-clusters in the triplet form(V_(3),Fe_(3),Mo_(3) and W_(3))confined in the surface cavities of the p-BN sheets by spin-polarized density functional theory(DFT)calculations.After a two-step screening strategy,Mo_(3)@p-BN was found to have high catalytic activity and selectivity with a rather low limiting potential(-0.34 V)for the NRR.The anchored Mo_(3) singlecluster can be stably embedded on the surface cavities of the substrate preventing the diffusion of the active Mo atoms.More importantly,the Mo atoms in the Mo_(3) single-cluster would act as“cache”to accelerate electron transfer between active metal centers and nitrogen-containing intermediates via the intimate Mo-Mo interactions.The cooperation of Mo atoms can also provide a large number of occupied and unoccupied d orbitals to make the"donation-backdonation"mechanism more effective.This work not only provides a quite promising electrocatalyst for NRR,but also brings new insights into the rational design of triple-atom NRR catalysts.