A new vanadium（Ⅲ） phosphite,V2（HPO3）3（1）,was synthesized hydrothermally with V2O5,H3PO3 as reactants,1,6-diaminopropane（1,6-HAD） as the structure-directing agent and characterized by single crystal X-ray diff...A new vanadium（Ⅲ） phosphite,V2（HPO3）3（1）,was synthesized hydrothermally with V2O5,H3PO3 as reactants,1,6-diaminopropane（1,6-HAD） as the structure-directing agent and characterized by single crystal X-ray diffraction,powder X-ray diffraction,IR spectroscopy,TGA,ICP-AES and elemental analyses.Single-crystal X-ray diffraction analysis reveals that compound 1 crystallized in the P6（3）/m hexagonal space group with the unit-cell parameters：a=0.80436（10） nm,c=0.73972（2） nm,V=0.41447（13） nm^3,Z=4.The construction of 3D framework structure of compound 1 may be viewed as the assembly of V2O9 dimers and HPO3 pseudo-pyramids which lead to form the one-dimensional 4,12-member ring channels along the [001] direction.展开更多
Lithium-sulfur(Li-S)batteries are promising candidates for next-generation energy storage devices due to their high energy density,low cost,and environmental friendliness.However,their practical application remains li...Lithium-sulfur(Li-S)batteries are promising candidates for next-generation energy storage devices due to their high energy density,low cost,and environmental friendliness.However,their practical application remains limited by the polysulfide shuttle effect,sulfur volume expansion,and poor electronic conductivity of S and Li2S.In this study,titanium carbide(TiC)was grown on Ti foam using chemical vapor deposition(CVD)to construct a binder-free,highly conductive,and porous TiC-Ti three-dimensional(3D)framework sulfur host for enhancing the Li-S battery performance.This 3D framework combines highly porous Ti foam with the polar surface of CVD-synthesized TiC nanoflowers,enabling efficient electron and ion transport,anchoring polysulfides to mitigate the shuttle effect,and accommodating sulfur volume expansion for enhanced cycling stability.Our study demonstrated that Li-S batteries utilizing TiC-Ti 3D framework@S cathodes achieved a high initial discharge capacity of 1506 mAh·g^(−1) at 0.1 C and maintained 93.3%of their capacity after 500 cycles at 1 C,with an exceptionally low average capacity decay of 0.01%per cycle.Additionally,the TiC-Ti 3D framework@S cathodes exhibited reduced charge transfer resistance after cycling,indicating enhanced interfacial reaction kinetics and stability.These findings confirm that the CVD-synthesized TiC-Ti 3D framework can serve as an efficient binder-free sulfur host,which provides a promising material and structural strategy for high-performance Li-S battery design.展开更多
Three-dimensional(3 D)frameworks have received much attention as an effective modification strategy for next-generation high-energy-density lithium metal batteries.However,the top-growth mode of lithium(Li)on the 3 D ...Three-dimensional(3 D)frameworks have received much attention as an effective modification strategy for next-generation high-energy-density lithium metal batteries.However,the top-growth mode of lithium(Li)on the 3 D framework remains a tough challenge.To achieve a uniform bottom-up Li growth,a scheme involving Ag concentration gradient in 3 D PVDF framework(C-Ag/PVDF)is proposed.Ag nanoparticles with a concentration gradient induce an interface activity gradient in the 3 D framework,and this gradient feature is still maintained during the cycle.As a result,the C-Ag/PVDF framework delivers a long lifespan over 1800 h at a current density of 1 mA cm^(-2) with a capacity of 1 mAh cm^(-2),and shows an ultra-long life(>1300 h)even at a high current density of 4 mA cm^(-2) with a capacity of 4 mAh cm^(-2).The advantage of concentration gradient provides further insights into the optimal design of the 3 D framework for stable Li metal anode.展开更多
Coaxial fiber-shaped supercapacitors are a promising class of energy storage devices requiring high performance for flexible and miniature electronic devices.Yet,they are still struggling from inferior energy density,...Coaxial fiber-shaped supercapacitors are a promising class of energy storage devices requiring high performance for flexible and miniature electronic devices.Yet,they are still struggling from inferior energy density,which comes from the limited choices in materials and structure used.Here,Zn-doped CuO nanowires were designed as 3D framework for aligned distributing high mass loading of MnO2 nanosheets.Zn could be introduced into the CuO crystal lattice to tune the covalency character and thus improve charge transport.The Zn–CuO@MnO2 as positive electrode obtained superior performance without sacrificing its areal and gravimetric capacitances with the increasing of mass loading of MnO2 due to 3D Zn–CuO framework enabling efficient electron transport.A novel category of free-standing asymmetric coaxial fiber-shaped supercapacitor based on Zn0.11CuO@MnO2 core electrode possesses superior specific capacitance and enhanced cell potential window.This asymmetric coaxial structure provides superior performance including higher capacity and better stability under deformation because of sufficient contact between the electrodes and electrolyte.Based on these advantages,the as-prepared asymmetric coaxial fiber-shaped supercapacitor exhibits a high specific capacitance of 296.6 mF cm^−2 and energy density of 133.47μWh cm^−2.In addition,its capacitance retention reaches 76.57%after bending 10,000 times,which demonstrates as-prepared device’s excellent flexibility and long-term cycling stability.展开更多
Carbon-based electric double layer capacitors(EDLCs)hold tremendous potentials due to their high-power performance and excellent cycle stability.However,the practical use of EDLCs is limited by the low energy density ...Carbon-based electric double layer capacitors(EDLCs)hold tremendous potentials due to their high-power performance and excellent cycle stability.However,the practical use of EDLCs is limited by the low energy density in aqueous electrolyte and sluggish diffusion kinetics in organic or/and ionic liquids electrolyte.Herein,3D carbon frameworks(3DCFs)constructed by interconnected nanocages(10-20 nm)with an ultrathin wall of ca.2 nm have been fabricated,which possess high specific surface area,hierarchical porosity and good conductive network.After deoxidization,the deoxidized 3DCF(3DCFDO)exhibits a record low IR drop of 0.064 V at 100 A g^−1 and ultrafast charge/discharge rate up to 10 V s^−1.The related device can be charged up to 77.4%of its maximum capacitance in 0.65 s at 100 A g^−1 in 6 M KOH.It has been found that the 3DCF-DO has a great affinity to EMIMBF4,resulting in a high specific capacitance of 174 F g^−1 at 1 A g^−1,and a high energy density of 34 Wh kg^−1 at an ultrahigh power density of 150 kW kg^−1 at 4 V after a fast charge in 1.11 s.This work provides a facile fabrication of novel 3D carbon frameworks for supercapacitors with ultrafast charge/discharge rate and high energy-power density.展开更多
The global trend towards new energy storage systems has stimulated the development of electrochemical energy storage technologies.Among these technologies,rechargeable aqueous zinc-ion batteries(AZIBs)have attracted c...The global trend towards new energy storage systems has stimulated the development of electrochemical energy storage technologies.Among these technologies,rechargeable aqueous zinc-ion batteries(AZIBs)have attracted considerable interest as a potential alternative to lithium-ion batteries(LIBs)due to their affordable cost,environmental compatibility and high safety standards.In this study,a high-quality electrode for AZIBs has been successfully developed using a dehydrated mixed-valence polyoxometalate-based three-dimensional(3D)inorganic framework material known as[H_6Mn_(3)V^Ⅳ_(15)V-^Ⅴ_(4O)_(46)(H_2O)_(12)](3D-MnVO).This innovative 3D-MnVO material is built from the alternate connections of{V_(19)O_(46)}"sphere-shaped"clusters andμ_(2)-{Mn(H_(2)O)_(4)}bridges,where each{V_(19)O_(46)}cluster is surrounded by three pairs of vertically distributed{Mn(H_(2)O)_(4)}units,thus resulting in the 3D interpenetrating grid-like network from the infinite[-{V_(19)O_(46)}-μ_(2)-Mn(H_(2)O)_(4)-{V_(19)O_(46)}]_∞chains in three mutually perpendicular directions.The 3D framework structure of 3D-MnVO possesses abundant oxygen vacancies,spacious and multi-level interconnected channels for ion transport,which facilitates the efficient intercalation/deintercalation of hydrated Zn^(2+)into the pores of the primary structure via the intercalation capacitance mechanism.As a result,the 3D-MnVO electrode exhibits excellent diffusion rates and minimal interfacial resistance.At a current density of 0.1 A·g^(-1),the 3D-MnVO cathode delivers a commendable discharge capacity of170.5 mAh·g^(-1)with 81.6%capacity retention after100 charge/discharge cycles.Furthermore,even at a high current density of 1.0 A·g^(-1),the 3D-MnVO electrode delivers a remarkable reversible capacity of198.9 mAh·g^(-1).Our research results provide valuable insights into the development of advanced polyoxometalate-based 3D inorganic framework electrode materials for high-performance rechargeable AZIBs.展开更多
Constructing three dimensional(3D)covalent organic frameworks(COFs)through the entanglement of two dimensional(2D)nets is a promising but underdeveloped strategy.Herein,we report the design and synthesis of a fluorine...Constructing three dimensional(3D)covalent organic frameworks(COFs)through the entanglement of two dimensional(2D)nets is a promising but underdeveloped strategy.Herein,we report the design and synthesis of a fluorine functionalized 3DCOF(3D-An-COF-F)formed by entangled 2D sql nets.The structure of 3D-An-COF-F was determined by the combination of continuous rotation electron diffraction technique and modelling based on the chemical information from real space.Interestingly,compared to the isostructural 3D-An-COF without F atom s,3DAn-COF-F showed an improved CO_(2)sorption ability and higher CO_(2)/N_(2)selectivity.Our study not only demonstrated the generality of constructing 3D COFs with entangled 2D nets by introducing bulky groups vertically in planar building blocks,but also will expand the diversity of 3D COFs for various applications.展开更多
Developing high-performance non-precious metal electrocatalysts for oxygen reduction reaction(ORR)is crucial for the commercialization of fuel cells and metal-air batteries.However,doped carbon-based materials only sh...Developing high-performance non-precious metal electrocatalysts for oxygen reduction reaction(ORR)is crucial for the commercialization of fuel cells and metal-air batteries.However,doped carbon-based materials only show good ORR activity in alkaline medium,and become less effective in acidic environment.We believe that an appropriate combination of both ionic and electronic transport path,and well dopant distribution of doped carbon-based materials would help to realize high ORR performance un-der both acidic and alkaline cond让ions.Accordingly,a nitrogen and sulfur co-doped carbon framework with hierarchical through-hole structure is fabricated by morphology-controlled solid-state pyrolysis of poly(aniline-co-2-ami no thiophenol)foam.The uniform high concentrations of nitrogen and sulfur,high intrinsic conductivity,and integrated three dimensional ionic and electronic transfer passageways of the 3D porous structure lead to synergistic effects in catalyzing ORR.As a result,the limiting current density of the carbonized poly(aniline-co-2-aminothiophenol)foam is equivalent to commercial Pt/C in acidic environment,and twice the latter in alkaline medium.展开更多
A new 3D Ag（I） coordination polymer {[Ag（AZDB）（0.5）（bpe）（0.5）]·H2O}n（1） has been papared by azobenzene-3,3？-dicarboxylicate（H2AZDB）, 1,2-bis（4-pyridyl）ethylene（bpe） and silver salts via hydroth...A new 3D Ag（I） coordination polymer {[Ag（AZDB）（0.5）（bpe）（0.5）]·H2O}n（1） has been papared by azobenzene-3,3？-dicarboxylicate（H2AZDB）, 1,2-bis（4-pyridyl）ethylene（bpe） and silver salts via hydrothermal method. The compound was fully characterized by single-crystal X-ray diffraction, elemental analyses, infrared spectrum（IR）, powder X-ray diffraction（PXRD） and thermogravimetric analysis（TGA）. The strucrural analysis indicate that compound 1 shows a 3D pillared-layer framework constructed from a unique 1D Ag2O2 ribbon and pyridyl/carboxylicate mixed system, which features a 2-nodal（4, 6）-connected fsc net with a（4^4·6^10·8）（4^4·6^2） topology.Moreover, the photoluminescent properties have also been discussed.展开更多
A novel 3D polymer 1 （C26H22CoN4O4, Mr = 513.41） constructed from H2C4BIm （2,2＇-（1,4-butanediyl）bis（1H-benzimidazole）], 1,3-bdc （1,3-benzenedicarboxylate） and Co（II） has been successfully synthesized under...A novel 3D polymer 1 （C26H22CoN4O4, Mr = 513.41） constructed from H2C4BIm （2,2＇-（1,4-butanediyl）bis（1H-benzimidazole）], 1,3-bdc （1,3-benzenedicarboxylate） and Co（II） has been successfully synthesized under hydrothermal conditions and characterized by single-crystal X-ray diffraction analysis. The crystal belongs to the tetragonal system, space group I-42d with a = 24.315（5）, b = 24.315（5）, c = 8.343（2）, V = 4933（2）3, Z = 8, Dc = 1.383 g/cm3, μ（MoKα） = 0.735 mm-1, F（000） = 2120, S = 1.156, the final R = 0.0596 and wR = 0.1346 for 1529 reflections with I 2σ（I）. Complex 1 contains 1D chains which are connected by extensive hydrogen-bonding interactions to form the 2D folded layer and 3D framework, which also stabilize the structure.展开更多
Stable solid-electrolyte interphase(SEI)is crucial for advanced development of lithium metal batteries.However,the continuous collapse and reconstruction of SEI will deplete fresh Li and electrolytes upon cycling,lead...Stable solid-electrolyte interphase(SEI)is crucial for advanced development of lithium metal batteries.However,the continuous collapse and reconstruction of SEI will deplete fresh Li and electrolytes upon cycling,leading to irreversible capacity loss.Herein,we addressed this issue by pre-formation of artificial robust hybrid interphase on a 3D layered graphene/lithium metal framework,in which is constructed by LiF associated with Li2TiF 6generated by the in-situ reaction between the surfacial lithium and titanium fluoride contained electrolytes.The as-obtained interphase can maintain the structure integrality and avoid continuous consumption of the fresh Li and electrolytes.As a consequence,the Li symmetric cells achieve high-efficiency Li deposition and stable cycling over 3600 h.When paired with LiFePO_(4)cathodes,the coin cells exhibit long lifespan(>800 cycles)with almost 88.3%retention of the initial capacity.展开更多
文摘A new vanadium（Ⅲ） phosphite,V2（HPO3）3（1）,was synthesized hydrothermally with V2O5,H3PO3 as reactants,1,6-diaminopropane（1,6-HAD） as the structure-directing agent and characterized by single crystal X-ray diffraction,powder X-ray diffraction,IR spectroscopy,TGA,ICP-AES and elemental analyses.Single-crystal X-ray diffraction analysis reveals that compound 1 crystallized in the P6（3）/m hexagonal space group with the unit-cell parameters：a=0.80436（10） nm,c=0.73972（2） nm,V=0.41447（13） nm^3,Z=4.The construction of 3D framework structure of compound 1 may be viewed as the assembly of V2O9 dimers and HPO3 pseudo-pyramids which lead to form the one-dimensional 4,12-member ring channels along the [001] direction.
文摘Lithium-sulfur(Li-S)batteries are promising candidates for next-generation energy storage devices due to their high energy density,low cost,and environmental friendliness.However,their practical application remains limited by the polysulfide shuttle effect,sulfur volume expansion,and poor electronic conductivity of S and Li2S.In this study,titanium carbide(TiC)was grown on Ti foam using chemical vapor deposition(CVD)to construct a binder-free,highly conductive,and porous TiC-Ti three-dimensional(3D)framework sulfur host for enhancing the Li-S battery performance.This 3D framework combines highly porous Ti foam with the polar surface of CVD-synthesized TiC nanoflowers,enabling efficient electron and ion transport,anchoring polysulfides to mitigate the shuttle effect,and accommodating sulfur volume expansion for enhanced cycling stability.Our study demonstrated that Li-S batteries utilizing TiC-Ti 3D framework@S cathodes achieved a high initial discharge capacity of 1506 mAh·g^(−1) at 0.1 C and maintained 93.3%of their capacity after 500 cycles at 1 C,with an exceptionally low average capacity decay of 0.01%per cycle.Additionally,the TiC-Ti 3D framework@S cathodes exhibited reduced charge transfer resistance after cycling,indicating enhanced interfacial reaction kinetics and stability.These findings confirm that the CVD-synthesized TiC-Ti 3D framework can serve as an efficient binder-free sulfur host,which provides a promising material and structural strategy for high-performance Li-S battery design.
基金supported by the Fundamental Research Funds for the Central Universities,China(ZYGX2019Z008)the National Natural Science Foundation of China(52072061)the Open Fund of the Key Laboratory for Renewable Energy,Chinese Academy of Sciences,Beijing Key Laboratory for New Energy Materials and Devices。
文摘Three-dimensional(3 D)frameworks have received much attention as an effective modification strategy for next-generation high-energy-density lithium metal batteries.However,the top-growth mode of lithium(Li)on the 3 D framework remains a tough challenge.To achieve a uniform bottom-up Li growth,a scheme involving Ag concentration gradient in 3 D PVDF framework(C-Ag/PVDF)is proposed.Ag nanoparticles with a concentration gradient induce an interface activity gradient in the 3 D framework,and this gradient feature is still maintained during the cycle.As a result,the C-Ag/PVDF framework delivers a long lifespan over 1800 h at a current density of 1 mA cm^(-2) with a capacity of 1 mAh cm^(-2),and shows an ultra-long life(>1300 h)even at a high current density of 4 mA cm^(-2) with a capacity of 4 mAh cm^(-2).The advantage of concentration gradient provides further insights into the optimal design of the 3 D framework for stable Li metal anode.
基金the National Natural Science Foundation of China(Nos.21975281,21773293,21603264)CAS Pioneer Hundred Talents Program,the National Key Research and Development Program of China(2016YFA0203301)+1 种基金Jiangsu Planned Projects for Postdoctoral Research Funds(2019K048)Suzhou Science and Technology Plan Project(SYG201926).
文摘Coaxial fiber-shaped supercapacitors are a promising class of energy storage devices requiring high performance for flexible and miniature electronic devices.Yet,they are still struggling from inferior energy density,which comes from the limited choices in materials and structure used.Here,Zn-doped CuO nanowires were designed as 3D framework for aligned distributing high mass loading of MnO2 nanosheets.Zn could be introduced into the CuO crystal lattice to tune the covalency character and thus improve charge transport.The Zn–CuO@MnO2 as positive electrode obtained superior performance without sacrificing its areal and gravimetric capacitances with the increasing of mass loading of MnO2 due to 3D Zn–CuO framework enabling efficient electron transport.A novel category of free-standing asymmetric coaxial fiber-shaped supercapacitor based on Zn0.11CuO@MnO2 core electrode possesses superior specific capacitance and enhanced cell potential window.This asymmetric coaxial structure provides superior performance including higher capacity and better stability under deformation because of sufficient contact between the electrodes and electrolyte.Based on these advantages,the as-prepared asymmetric coaxial fiber-shaped supercapacitor exhibits a high specific capacitance of 296.6 mF cm^−2 and energy density of 133.47μWh cm^−2.In addition,its capacitance retention reaches 76.57%after bending 10,000 times,which demonstrates as-prepared device’s excellent flexibility and long-term cycling stability.
基金the financial support from the National Natural Science Foundation of China(51672033,U1610255,U1703251).
文摘Carbon-based electric double layer capacitors(EDLCs)hold tremendous potentials due to their high-power performance and excellent cycle stability.However,the practical use of EDLCs is limited by the low energy density in aqueous electrolyte and sluggish diffusion kinetics in organic or/and ionic liquids electrolyte.Herein,3D carbon frameworks(3DCFs)constructed by interconnected nanocages(10-20 nm)with an ultrathin wall of ca.2 nm have been fabricated,which possess high specific surface area,hierarchical porosity and good conductive network.After deoxidization,the deoxidized 3DCF(3DCFDO)exhibits a record low IR drop of 0.064 V at 100 A g^−1 and ultrafast charge/discharge rate up to 10 V s^−1.The related device can be charged up to 77.4%of its maximum capacitance in 0.65 s at 100 A g^−1 in 6 M KOH.It has been found that the 3DCF-DO has a great affinity to EMIMBF4,resulting in a high specific capacitance of 174 F g^−1 at 1 A g^−1,and a high energy density of 34 Wh kg^−1 at an ultrahigh power density of 150 kW kg^−1 at 4 V after a fast charge in 1.11 s.This work provides a facile fabrication of novel 3D carbon frameworks for supercapacitors with ultrafast charge/discharge rate and high energy-power density.
基金financially supported by the National Natural Science Foundation of China(Nos.52071132,52261135632 and U21A20284)Zhongyuan Thousand People PlanThe Zhongyuan Youth Talent Support Program(in Science and Technology),China(No.ZYQR201810139)+5 种基金the Natural Science Foundation of Henan,China(Nos.232300421080 and 222300420138)the Science and Technology Project of Henan Province,China(Nos.232102241038 and 232102241004)the Key Scientific Research Programs in Universities of Henan Province,China-Special Projects for Basic Research(No.23ZX008)the Innovative Funds Plan of Henan University of Technology,China(No.2020ZKCJ04)the Ph.D.Programs Foundation of HenanUniversity of Technology,China(No.2021BS0027)the Doctoral Education Fund of Henan University of Engineering,China(No.DKJ2019004)。
文摘The global trend towards new energy storage systems has stimulated the development of electrochemical energy storage technologies.Among these technologies,rechargeable aqueous zinc-ion batteries(AZIBs)have attracted considerable interest as a potential alternative to lithium-ion batteries(LIBs)due to their affordable cost,environmental compatibility and high safety standards.In this study,a high-quality electrode for AZIBs has been successfully developed using a dehydrated mixed-valence polyoxometalate-based three-dimensional(3D)inorganic framework material known as[H_6Mn_(3)V^Ⅳ_(15)V-^Ⅴ_(4O)_(46)(H_2O)_(12)](3D-MnVO).This innovative 3D-MnVO material is built from the alternate connections of{V_(19)O_(46)}"sphere-shaped"clusters andμ_(2)-{Mn(H_(2)O)_(4)}bridges,where each{V_(19)O_(46)}cluster is surrounded by three pairs of vertically distributed{Mn(H_(2)O)_(4)}units,thus resulting in the 3D interpenetrating grid-like network from the infinite[-{V_(19)O_(46)}-μ_(2)-Mn(H_(2)O)_(4)-{V_(19)O_(46)}]_∞chains in three mutually perpendicular directions.The 3D framework structure of 3D-MnVO possesses abundant oxygen vacancies,spacious and multi-level interconnected channels for ion transport,which facilitates the efficient intercalation/deintercalation of hydrated Zn^(2+)into the pores of the primary structure via the intercalation capacitance mechanism.As a result,the 3D-MnVO electrode exhibits excellent diffusion rates and minimal interfacial resistance.At a current density of 0.1 A·g^(-1),the 3D-MnVO cathode delivers a commendable discharge capacity of170.5 mAh·g^(-1)with 81.6%capacity retention after100 charge/discharge cycles.Furthermore,even at a high current density of 1.0 A·g^(-1),the 3D-MnVO electrode delivers a remarkable reversible capacity of198.9 mAh·g^(-1).Our research results provide valuable insights into the development of advanced polyoxometalate-based 3D inorganic framework electrode materials for high-performance rechargeable AZIBs.
基金financially supported by the National Natural Science Foundation of China(Nos.22225503,U21A20285 and 22375153)the Hubei Provincial Natural Science Foundation of China(No.2023AFA011)the Fundamental Research Funds for Central Universities(No.2042023kf0127)。
文摘Constructing three dimensional(3D)covalent organic frameworks(COFs)through the entanglement of two dimensional(2D)nets is a promising but underdeveloped strategy.Herein,we report the design and synthesis of a fluorine functionalized 3DCOF(3D-An-COF-F)formed by entangled 2D sql nets.The structure of 3D-An-COF-F was determined by the combination of continuous rotation electron diffraction technique and modelling based on the chemical information from real space.Interestingly,compared to the isostructural 3D-An-COF without F atom s,3DAn-COF-F showed an improved CO_(2)sorption ability and higher CO_(2)/N_(2)selectivity.Our study not only demonstrated the generality of constructing 3D COFs with entangled 2D nets by introducing bulky groups vertically in planar building blocks,but also will expand the diversity of 3D COFs for various applications.
基金financial support by the National Natural Science Foundation of China (Grant: 51333008)Young Teacher Training Program of Sun Yat-sen University (Grant: 17lgpy86)
文摘Developing high-performance non-precious metal electrocatalysts for oxygen reduction reaction(ORR)is crucial for the commercialization of fuel cells and metal-air batteries.However,doped carbon-based materials only show good ORR activity in alkaline medium,and become less effective in acidic environment.We believe that an appropriate combination of both ionic and electronic transport path,and well dopant distribution of doped carbon-based materials would help to realize high ORR performance un-der both acidic and alkaline cond让ions.Accordingly,a nitrogen and sulfur co-doped carbon framework with hierarchical through-hole structure is fabricated by morphology-controlled solid-state pyrolysis of poly(aniline-co-2-ami no thiophenol)foam.The uniform high concentrations of nitrogen and sulfur,high intrinsic conductivity,and integrated three dimensional ionic and electronic transfer passageways of the 3D porous structure lead to synergistic effects in catalyzing ORR.As a result,the limiting current density of the carbonized poly(aniline-co-2-aminothiophenol)foam is equivalent to commercial Pt/C in acidic environment,and twice the latter in alkaline medium.
基金supported by the NSF of Hubei Province(No.2014CFB277)the Open Foundation of Ministry of Education Key Laboratory of Synthetic and Natural Functional Molecular Chemistry(No.338080057)
文摘A new 3D Ag（I） coordination polymer {[Ag（AZDB）（0.5）（bpe）（0.5）]·H2O}n（1） has been papared by azobenzene-3,3？-dicarboxylicate（H2AZDB）, 1,2-bis（4-pyridyl）ethylene（bpe） and silver salts via hydrothermal method. The compound was fully characterized by single-crystal X-ray diffraction, elemental analyses, infrared spectrum（IR）, powder X-ray diffraction（PXRD） and thermogravimetric analysis（TGA）. The strucrural analysis indicate that compound 1 shows a 3D pillared-layer framework constructed from a unique 1D Ag2O2 ribbon and pyridyl/carboxylicate mixed system, which features a 2-nodal（4, 6）-connected fsc net with a（4^4·6^10·8）（4^4·6^2） topology.Moreover, the photoluminescent properties have also been discussed.
基金supported by the research grant of Phytochemistry Key Laboratory of Shaanxi Province (No. 09JS066)
文摘A novel 3D polymer 1 （C26H22CoN4O4, Mr = 513.41） constructed from H2C4BIm （2,2＇-（1,4-butanediyl）bis（1H-benzimidazole）], 1,3-bdc （1,3-benzenedicarboxylate） and Co（II） has been successfully synthesized under hydrothermal conditions and characterized by single-crystal X-ray diffraction analysis. The crystal belongs to the tetragonal system, space group I-42d with a = 24.315（5）, b = 24.315（5）, c = 8.343（2）, V = 4933（2）3, Z = 8, Dc = 1.383 g/cm3, μ（MoKα） = 0.735 mm-1, F（000） = 2120, S = 1.156, the final R = 0.0596 and wR = 0.1346 for 1529 reflections with I 2σ（I）. Complex 1 contains 1D chains which are connected by extensive hydrogen-bonding interactions to form the 2D folded layer and 3D framework, which also stabilize the structure.
基金supported by the National Key Research and Development Program of China(No.2018YFA0209600)Science and Technology Key Project of Guangdong Province,China(No.2020B010188002)+4 种基金Guangdong Innovative and Entrepreneurial Research Team Program(No.2019ZT08L075)Foshan Innovative and Entrepreneurial Research Team Program(No.2018IT100031)Guangdong Pearl River Talent Program(No.2019QN01L054)National Natural Science Foundation of China(No.22176063)the Fundamental Research Funds for the Central Universities(No.2020ZYGXZR061)。
文摘Stable solid-electrolyte interphase(SEI)is crucial for advanced development of lithium metal batteries.However,the continuous collapse and reconstruction of SEI will deplete fresh Li and electrolytes upon cycling,leading to irreversible capacity loss.Herein,we addressed this issue by pre-formation of artificial robust hybrid interphase on a 3D layered graphene/lithium metal framework,in which is constructed by LiF associated with Li2TiF 6generated by the in-situ reaction between the surfacial lithium and titanium fluoride contained electrolytes.The as-obtained interphase can maintain the structure integrality and avoid continuous consumption of the fresh Li and electrolytes.As a consequence,the Li symmetric cells achieve high-efficiency Li deposition and stable cycling over 3600 h.When paired with LiFePO_(4)cathodes,the coin cells exhibit long lifespan(>800 cycles)with almost 88.3%retention of the initial capacity.
