Nitrogen-doped carbon(N-C)materials have demonstrated exceptional performances in activating peroxymonosulfate(PMS)for environmental remediation.However,accommodating higher nitrogen contents remains challenging in N-...Nitrogen-doped carbon(N-C)materials have demonstrated exceptional performances in activating peroxymonosulfate(PMS)for environmental remediation.However,accommodating higher nitrogen contents remains challenging in N-C due to the thermodynamic instability of C-N skeleton.In this study,we proposed an innovative epitaxial growth approach to synthesize two-dimensional N-C nanosheets.Leveraging the abundant amino groups supplied by the polymer dots as growing sites,we successfully attained a high nitrogen level and spontaneously introduced abundant structural defects in the carbon framework.The resulting N-C nanosheets exhibited outstanding catalytic activity for the activation of PMS toward selective oxidation of diethyl 1,4-dihydro-2,6-dimethyl-3,5-pyridinedicarboxylate(1,4-DHP)into diethyl2,6-dimethylpyridine-3,5-dicarboxylate,which serves as a valuable intermediate in the synthesis of various pharmaceutical compounds.Comprehensive experimental and characterization investigations verified that the nitrogen sites and defects are the primary active sites for PMS activation and selective oxidation of 1,4-DHP.This work offered an efficient approach for the fabrication of high-nitrogen-loading carbon materials for catalytic oxidation reactions.展开更多
Cu-based MOFs,i.e.,HKUST-1,etc.,have been pertinently chosen as the pristine materials for CO2 ER due to the unique ability of copper for generation hydrocarbon fuel.However,the limited conductivity and stability b...Cu-based MOFs,i.e.,HKUST-1,etc.,have been pertinently chosen as the pristine materials for CO2 ER due to the unique ability of copper for generation hydrocarbon fuel.However,the limited conductivity and stability become the stumbling-block that prevents the development of it.The exploring of MOFsderived M-C materials starts a new chapter for the MOFs precursors,which provides a remarkable electronic connection between carbon matrix and metals/metal oxides.N-doped M-N-C with extensive M-N sites scattering into the carbon matrix are more popular because of their impressive contribution to catalytic activity and specific product selectivity.Nevertheless,Cu-N-C system remained undeveloped up to now.The lack of ideal precursor,the sensitivity of Cu to be oxidized,and the difficulties in the synthesis of small size Cu nanoparticles are thus known as the main barriers to the development of Cu-N-C electrocatalysts.Herein,a nitrogen-rich Cu-BTT MOF is employed for the derivation of N-doped Cu-N-CT composite electrocatalysts by the pyrolyze method.High-temperature pyrolysis product of Cu-N-C1100exhibits the best catalytic activity for productions of CO(-0.6 V vs.RHE,jCO=0.4 mA/cm2)and HCOOH(-0.9 V vs.RHE,jHCOOH=1.4 mA/cm2).展开更多
Transition metal nitrides have become the focus of research in sodium ion batteries(SIBs)due to their unique metal properties and high theoretical capacity.However,the low actual capacity is still the main bottleneck ...Transition metal nitrides have become the focus of research in sodium ion batteries(SIBs)due to their unique metal properties and high theoretical capacity.However,the low actual capacity is still the main bottleneck for their application.Herein,using Mo-aniline frameworks as precursors,the carbon encapsulated nitrogen-rich MoxN is decorated by few-layered MoSe2 nanosheets(MoSe2@MoxN/C-I)after the facile calcinating,selenizing,and nitriding.The carbon encapsulation can effectively strengthen the structural stability of MoxN.The nitrogen-rich MoxN and decoration of few-layered MoSe2 can create rich heterointerfaces and extra active sites for rapid sodium-ion storage,thus promoting reaction kinetics and improving actual capacity.The MoSe2@MoxN/C-I as an anode achieves a large reversible capacity of 522.8 mAh g-1at 0.1 A g-1,and 254.3 mAh g-1capacity is obtained after 6000 cycles at 5.0 A g-1,showing signally improved sodium-ion storage properties.The storage mechanisms and kinetic behaviors are described systematically via the advanced testing techniques and density functional theory(DFT)calculations.It is found that the nitrogen-rich MoxN as the substrate is the basis of long cycling stability,and the few-layered MoSe2 are the key to improving actual capacity.This work indicates that the decoration of few-layered selenides has a broad application prospect in high-performance metal-ion batteries.展开更多
From the standpoint of chemical structures,the organic backbones of energetic materials can be classified into aromatic rings,nonaromatic rings,and open chains.Although the category of aromatic energetic compounds exh...From the standpoint of chemical structures,the organic backbones of energetic materials can be classified into aromatic rings,nonaromatic rings,and open chains.Although the category of aromatic energetic compounds exhibits several advantages in the regulation of energetic properties,the nonaromatic heterocycles,assembling nitramino explosophores with simple alkyl bridges,still have prevailed in benchmark materials.The methylene bridge plays a pivotal role in the constructions of the classic nonaromatic heterocycle-based energetic compounds,e.g.,hexahydro-1,3,5-trinitro-1,3,5-triazine(RDX)and octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine(HMX),whereas ethylene bridge is the core moiety of state-of-the-art explosive 2,4,6,8,10,12-hexanitro-2,4,6,8,10,12-hexaazaisowurtzitane(CL-20).In this context,it is of great interest to employ simple and practical bridges to assemble aromatic and nonaromatic nitrogen-rich heterocycles,thereby expanding the structural diversity of energetic materials,e.g.,bridged and fused nitrogen-rich poly-heterocycles.Furthermore,alkyl-bridged poly-heterocycles highlight the potential for the open chain type of energetic materials.In this review,the development of alkyl bridges in linking nitrogen-rich heterocycles is presented,and the perspective of the newly constructed energetic backbones is summarized for the future design of advanced energetic materials.展开更多
Nitrogen-rich porous carbonaceous materials have shown great potential in energy storage and conversion applications due to their facile fabrication,high electronic conductivity,and improved hydrophilic property.Herei...Nitrogen-rich porous carbonaceous materials have shown great potential in energy storage and conversion applications due to their facile fabrication,high electronic conductivity,and improved hydrophilic property.Herein,three-dimensional porous N-rich carbon foams are fabricated through a one-step carbonization-activation method of the commercial melamine foam,and displaying hierarchically porous structure(macro-,meso-,and micro-pores),large surface area(1686.5 m2 g^-1),high N-containing level(3.3 at%),and excellent compressibility.The as-prepared carbon foams as electrodes for quasi-solid-state supercapacitors exhibit enhanced energy storage ability with 210 F g^-1 and 2.48c at 0.1 A g^-1,and150 F g^-1 and 1.77 F cm^-2 at 1 A g^-1,respectively.Moreover,as an electrode for lithium-based dual-ion capacitor,this distinctive porous carbon also delivers remarkable specific capacitance with 143.6 F g^-1 at0.1 A g^-1 and 116.2 F g^-1 at 1 A g^-1.The simple preparation method and the fascinating electrochemical performance endow the N-rich porous carbon foams great prospects as high-performance electrodes for electrochemical energy storage.展开更多
The combination of a powerful CO2-enriching carrier and robust active component provides a new idea for the construction of efficient catalysts for electrocatalytic CO2reduction.Herein,novel perforated nitrogen-...The combination of a powerful CO2-enriching carrier and robust active component provides a new idea for the construction of efficient catalysts for electrocatalytic CO2reduction.Herein,novel perforated nitrogen-rich graphene-like carbon nanolayers(PNGC)are prepared from biomass derivatives,which promotes the oriented deposition of In-doped Cu2(OH)3(NO3)nanosheet patches.A robust Cu-In/PNGC composite catalyst is then obtained via simple in-situ electrochemical reduction.Unsurprisingly,CuIn/PNGC exhibits a CO Faradaic efficiency(FECO)of 91.3%and a remarkable CO partial current density(jCO)of 136.4 m A cm-2at a moderate overpotential of 0.59 V for electrocatalytic CO2reduction reaction(CO2RR).DFT calculations and experimental studies indicate that the strong carrier effect of PNGC makes PNGC carried Cu-In nanosheets improved the adsorption capacity of CO2gas,reconfigured electronic structure,and reduced free energy of key intermediate formation,thereby the CO2activation and conversion are promoted.展开更多
The nitrogen content of tetrazolo triazines is 68.9%.In this paper,tetrazolotriazines was synthetized.The TG-DSC test indicated its decomposition process in detail.The non-isothermal kinetic parameters were speculated...The nitrogen content of tetrazolo triazines is 68.9%.In this paper,tetrazolotriazines was synthetized.The TG-DSC test indicated its decomposition process in detail.The non-isothermal kinetic parameters were speculated by Kissinger and Ozawa methods.It revealed the mechanism function of thermal decomposition.The impact and friction sensitivity were tested.The detonation pressure and velocity were calculated.It has a wide range of potential applications as a kind of energetic material.展开更多
Composting as a solution to the increasing generation of municipal solid waste (MSW), also contribute to GHGs emission when not controlled and could lack some basic nutrients, especially nitrogen. This study assessed ...Composting as a solution to the increasing generation of municipal solid waste (MSW), also contribute to GHGs emission when not controlled and could lack some basic nutrients, especially nitrogen. This study assessed the split-additions of nitrogen-rich substrate to composting materials and their effect on GHGs emissions as well as the quality of the composts. Nitrogen-rich substrates formulated from pig and goat manure were co-composted with MSW for a 12-weeks period by split adding at mesophilic (˚C) and thermophilic (>50˚C) stages in five different treatments. Representative samples from the compost were taken from each treatment for physicochemical, heavy metals and bacteriological analysis. In-situ CH4, CO2, N2O gas emissions were also analyzed weekly during composting. It was observed that all the treatments showed significant organic matter decomposition, reaching thermophilic temperatures in the first week of composting. The absence affects the suitable agronomic properties. All nitrogen-rich substrate applied at thermophilic stage (Treatment two) recorded the highest N, P and K concentrations of 1.34%, 0.97% and 2.45%, respectively with highest nitrogen retention. In terms of GHG emissions, CO2 was highest at the thermophilic stage when N-rich substrate was added in all treatment, while CH4 was highest in the mesophilic stage with N-rich substrate addition. N2O showed no specific trend in the treatments. Split addition of the N-rich substrate for co-composting of MSW produced compost which is stable, has less nutrient loss and low GHG emissions. Split addition of a nitrogen-rich substrate could be an option for increasing the fertilizer value of MSW compost.展开更多
Energetic coordination compound with 5-nitro-tetrazole (NT) as ligand has gained more and more attentions due to its extreme explosive properties and ecological friendly pyrolysis productsF1-61 The research results ...Energetic coordination compound with 5-nitro-tetrazole (NT) as ligand has gained more and more attentions due to its extreme explosive properties and ecological friendly pyrolysis productsF1-61 The research results in 1994 proposed from Sandia National Laboratories proves tetrammine-cis-bis (5-nitro-2H-tetrazole-N2 ) cobalt ( Ⅲ ) perchlorate (BNCP) to be a more powerful explosive and undergoes deflagration-to- detonation (DDT)展开更多
Redox-active porous aromatic frameworks(PAFs)have emerged as hopeful candidates for sodium-ion batteries(SIBs)in view of their porous structures,chemical stability and tunable architectures.Herein,we successfully synt...Redox-active porous aromatic frameworks(PAFs)have emerged as hopeful candidates for sodium-ion batteries(SIBs)in view of their porous structures,chemical stability and tunable architectures.Herein,we successfully synthesized two redox-active PAFs(PAF-305 and PAF-306)with different nitrogen-containing motifs,and demonstrated their application as cathode materials for SIBs.Density functional theory(DFT)calculations reveal that nitrogen-rich PAF-305 exhibits a lower lowest unoccupied molecular orbital(LUMO)energy level(-3.35 eV)and a narrower energy gap(Eg)(2.40 eV)compared with nitrogen-poor PAF-306.As expected,PAF-305 displays outstanding electrochemical performance,comprising a high reversible capacity of 145.2 mAh g-1at 0.05 A g-1and satisfactory cycling stability with 92% capacity retention over 1000 cycles at 0.2 A g-1.Remarkably,PAF-305 maintains robust electrochemical properties across a wide temperature range(-20℃ to 50℃).Through a combination of experimental characterizations and theoretical calculations,the sodium-ion storage mechanism of PAF-305 is elucidated.This study not only provides a promising strategy for exploring other redox-active organic units in the design of novel PAFs,but also expands the potential applications of PAFs in energy storage systems.展开更多
Covalent organic frameworks(COFs)are promising candidates for the rapid purification of toxic pollutants and mitigation of radioactive iodine leakage in nuclear accidents.In particular,COFs constructed from meta-posit...Covalent organic frameworks(COFs)are promising candidates for the rapid purification of toxic pollutants and mitigation of radioactive iodine leakage in nuclear accidents.In particular,COFs constructed from meta-position monomers can form clover-like morphology,increasing the specific surface area and providing multidimensional diffusion pathways for iodine.Herein,two nitrogen-rich COFs(DFPT-COF and DFPB-COF)featuring well-defined cloverlike nanochannels were successfully fabricated,demonstrating exceptional iodine capture performance.Compared to DFPB-COF,DFPT-COF exhibits better iodine capture performance(5.58 g g−1for I2vapor)due to its large specific surface area and rich nitrogen adsorption sites.Moreover,the adsorption dynamics of DFPT-COF for liquid iodine follow a pseudosecond-order kinetic model and the adsorption isotherm model complies with the Langmuir model.Notably,DFPT-COF exhibited excellent renewable adsorption performance,suggesting its potential as a sustainable and efficient green adsorbent for iodine in nuclear waste management.展开更多
The pursuit of heat-resistant energetic materials(HREMs)with thermal stability beyond 450℃ presents a significant challenge that has yet to be achieved.In this work,we develop an innovative electronic delocalization ...The pursuit of heat-resistant energetic materials(HREMs)with thermal stability beyond 450℃ presents a significant challenge that has yet to be achieved.In this work,we develop an innovative electronic delocalization strategy to design and synthesize a planar dizwitterionic diamino-bistriazolotetrazine,designated as TYX-1.The unique structural feature of TYX-1,including a nitrogen-rich fused ring system,planar conformation,and dizwitterionic configuration,combined with its hydrogen-bonded organic framework(HOF)structure,confer exceptional thermal stability(The onset temperature is 428℃,and the peak temperature is 473℃),high density(1.84 g/cm3),and remarkable detonation performance(detonation velocity:8616 m/s).Furthermore,TYX-1 exhibits an impressive insensitivity(impact sensitivity>40 J;friction sensitivity>360 N),surpassing all previously reported HREMs.Theoretical calculations and single-crystal clearly indicate that the delocalizedπelectrons within the dizwitterionic bistriazolotetrazine rings and the HOF structure of TYX-1 are pivotal in ensuring its high thermal stability and high energy density.The discovery of TYX-1 marks a significant advancement in the field of HREMs and is anticipated to catalyze substantial progress in various high-temperature applications reliant on energetic materials.展开更多
An imine-based nitrogen-rich covalent-organic framework(COF)was successfully synthesized using two tri-angular building units under solvothermal reaction condition.The gas adsorption properties of the obtained micro-p...An imine-based nitrogen-rich covalent-organic framework(COF)was successfully synthesized using two tri-angular building units under solvothermal reaction condition.The gas adsorption properties of the obtained micro-porous nitrogen-rich COF were investigated.The results indicated that the activated COF material presented good up take capabilities of CO2 and CH4 at 61.2 and 43.4 cm3·g−1at 1 atm and 273 K,respectively,showing its applica-tion potential in selective gas capture and separation.展开更多
Eliminating the usage of metal current collectors and binders in traditional battery electrode configuration is an effective strategy to significantly improve the capacities of lithium ion batteries (LIBs). Herein, we...Eliminating the usage of metal current collectors and binders in traditional battery electrode configuration is an effective strategy to significantly improve the capacities of lithium ion batteries (LIBs). Herein, we demonstrate the construction of porous vanadium nitride (VN) nanosheet network in situ grown on nitrogen-rich (N-rich) carbon textile (N-C@P-VN) as lightweight and binder-free anode for LIBs. The N-rich carbon textile is used both as the current collector and host to store Li+, thus improving the specific capacities of binder-free VN anode and meanwhile reducing the inert mass of the whole cell. Moreover, the open spaces in carbon textile and vertically aligned pores in VN nanosheet network can not only provide an expressway for Li+ and e− transport, but also afford more active sites. As a result, the binder-free N-C@P-VN anode maintains a specific capacity of 1,040 mAh·g−1 (or an areal capacity of 2.6 mAh·cm−2) after 100 cycles at 0.1 mA·cm−2 in half cell. Moreover, in an assembled N-C@P-VN//LiFePO4 full cell, it exhibits an areal capacity of 1.7 mAh·cm−2 after 300 cycles at 0.1 C. The synergistic strategy of N-C substrate and porous VN network could be applied to guide rational design of similar N-C@nitride or sulfide hybrid systems with corresponding sulfur-doped carbon textile as the substrate.展开更多
基金the financial support from Australian Research Council under DECRA Scheme(No.DE210100253)merit SXR beamline from Australian Nuclear Science and Technology Organization(ANSTO,No.AS231/SXR/19680)。
摘要Nitrogen-doped carbon(N-C)materials have demonstrated exceptional performances in activating peroxymonosulfate(PMS)for environmental remediation.However,accommodating higher nitrogen contents remains challenging in N-C due to the thermodynamic instability of C-N skeleton.In this study,we proposed an innovative epitaxial growth approach to synthesize two-dimensional N-C nanosheets.Leveraging the abundant amino groups supplied by the polymer dots as growing sites,we successfully attained a high nitrogen level and spontaneously introduced abundant structural defects in the carbon framework.The resulting N-C nanosheets exhibited outstanding catalytic activity for the activation of PMS toward selective oxidation of diethyl 1,4-dihydro-2,6-dimethyl-3,5-pyridinedicarboxylate(1,4-DHP)into diethyl2,6-dimethylpyridine-3,5-dicarboxylate,which serves as a valuable intermediate in the synthesis of various pharmaceutical compounds.Comprehensive experimental and characterization investigations verified that the nitrogen sites and defects are the primary active sites for PMS activation and selective oxidation of 1,4-DHP.This work offered an efficient approach for the fabrication of high-nitrogen-loading carbon materials for catalytic oxidation reactions.
基金supported by the National Natural Science Foundation of China(20171169)Six Talent Peaks Project in Jiangsu Province(No.2017-XNY-043)+1 种基金the projects funded by the High-Level Personnel Support Program of Yang-Zhou Universitythe Priority Academic Program Development of Jiangsu Higher Education Institutions。
摘要Cu-based MOFs,i.e.,HKUST-1,etc.,have been pertinently chosen as the pristine materials for CO2 ER due to the unique ability of copper for generation hydrocarbon fuel.However,the limited conductivity and stability become the stumbling-block that prevents the development of it.The exploring of MOFsderived M-C materials starts a new chapter for the MOFs precursors,which provides a remarkable electronic connection between carbon matrix and metals/metal oxides.N-doped M-N-C with extensive M-N sites scattering into the carbon matrix are more popular because of their impressive contribution to catalytic activity and specific product selectivity.Nevertheless,Cu-N-C system remained undeveloped up to now.The lack of ideal precursor,the sensitivity of Cu to be oxidized,and the difficulties in the synthesis of small size Cu nanoparticles are thus known as the main barriers to the development of Cu-N-C electrocatalysts.Herein,a nitrogen-rich Cu-BTT MOF is employed for the derivation of N-doped Cu-N-CT composite electrocatalysts by the pyrolyze method.High-temperature pyrolysis product of Cu-N-C1100exhibits the best catalytic activity for productions of CO(-0.6 V vs.RHE,jCO=0.4 mA/cm2)and HCOOH(-0.9 V vs.RHE,jHCOOH=1.4 mA/cm2).
基金supported by the National Natural Science Foundation of China(52171207,51762021)the Natural Science Foundation of Jiangxi province(20212BAB204031,20192ACB21009)。
摘要Transition metal nitrides have become the focus of research in sodium ion batteries(SIBs)due to their unique metal properties and high theoretical capacity.However,the low actual capacity is still the main bottleneck for their application.Herein,using Mo-aniline frameworks as precursors,the carbon encapsulated nitrogen-rich MoxN is decorated by few-layered MoSe2 nanosheets(MoSe2@MoxN/C-I)after the facile calcinating,selenizing,and nitriding.The carbon encapsulation can effectively strengthen the structural stability of MoxN.The nitrogen-rich MoxN and decoration of few-layered MoSe2 can create rich heterointerfaces and extra active sites for rapid sodium-ion storage,thus promoting reaction kinetics and improving actual capacity.The MoSe2@MoxN/C-I as an anode achieves a large reversible capacity of 522.8 mAh g-1at 0.1 A g-1,and 254.3 mAh g-1capacity is obtained after 6000 cycles at 5.0 A g-1,showing signally improved sodium-ion storage properties.The storage mechanisms and kinetic behaviors are described systematically via the advanced testing techniques and density functional theory(DFT)calculations.It is found that the nitrogen-rich MoxN as the substrate is the basis of long cycling stability,and the few-layered MoSe2 are the key to improving actual capacity.This work indicates that the decoration of few-layered selenides has a broad application prospect in high-performance metal-ion batteries.
基金National Natural Science Foundation of China(Grant Nos.22075023,22205022,and 22235003)to provide fund for conducting experiments。
摘要From the standpoint of chemical structures,the organic backbones of energetic materials can be classified into aromatic rings,nonaromatic rings,and open chains.Although the category of aromatic energetic compounds exhibits several advantages in the regulation of energetic properties,the nonaromatic heterocycles,assembling nitramino explosophores with simple alkyl bridges,still have prevailed in benchmark materials.The methylene bridge plays a pivotal role in the constructions of the classic nonaromatic heterocycle-based energetic compounds,e.g.,hexahydro-1,3,5-trinitro-1,3,5-triazine(RDX)and octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine(HMX),whereas ethylene bridge is the core moiety of state-of-the-art explosive 2,4,6,8,10,12-hexanitro-2,4,6,8,10,12-hexaazaisowurtzitane(CL-20).In this context,it is of great interest to employ simple and practical bridges to assemble aromatic and nonaromatic nitrogen-rich heterocycles,thereby expanding the structural diversity of energetic materials,e.g.,bridged and fused nitrogen-rich poly-heterocycles.Furthermore,alkyl-bridged poly-heterocycles highlight the potential for the open chain type of energetic materials.In this review,the development of alkyl bridges in linking nitrogen-rich heterocycles is presented,and the perspective of the newly constructed energetic backbones is summarized for the future design of advanced energetic materials.
基金Financial supports from the National Natural Science Foundation of China(51872027)Beijing Natural Science Foundation(L172023)。
摘要Nitrogen-rich porous carbonaceous materials have shown great potential in energy storage and conversion applications due to their facile fabrication,high electronic conductivity,and improved hydrophilic property.Herein,three-dimensional porous N-rich carbon foams are fabricated through a one-step carbonization-activation method of the commercial melamine foam,and displaying hierarchically porous structure(macro-,meso-,and micro-pores),large surface area(1686.5 m2 g^-1),high N-containing level(3.3 at%),and excellent compressibility.The as-prepared carbon foams as electrodes for quasi-solid-state supercapacitors exhibit enhanced energy storage ability with 210 F g^-1 and 2.48c at 0.1 A g^-1,and150 F g^-1 and 1.77 F cm^-2 at 1 A g^-1,respectively.Moreover,as an electrode for lithium-based dual-ion capacitor,this distinctive porous carbon also delivers remarkable specific capacitance with 143.6 F g^-1 at0.1 A g^-1 and 116.2 F g^-1 at 1 A g^-1.The simple preparation method and the fascinating electrochemical performance endow the N-rich porous carbon foams great prospects as high-performance electrodes for electrochemical energy storage.
基金supported by the National Natural Science Foundation of China(U21B2099)。
摘要The combination of a powerful CO2-enriching carrier and robust active component provides a new idea for the construction of efficient catalysts for electrocatalytic CO2reduction.Herein,novel perforated nitrogen-rich graphene-like carbon nanolayers(PNGC)are prepared from biomass derivatives,which promotes the oriented deposition of In-doped Cu2(OH)3(NO3)nanosheet patches.A robust Cu-In/PNGC composite catalyst is then obtained via simple in-situ electrochemical reduction.Unsurprisingly,CuIn/PNGC exhibits a CO Faradaic efficiency(FECO)of 91.3%and a remarkable CO partial current density(jCO)of 136.4 m A cm-2at a moderate overpotential of 0.59 V for electrocatalytic CO2reduction reaction(CO2RR).DFT calculations and experimental studies indicate that the strong carrier effect of PNGC makes PNGC carried Cu-In nanosheets improved the adsorption capacity of CO2gas,reconfigured electronic structure,and reduced free energy of key intermediate formation,thereby the CO2activation and conversion are promoted.
基金Supported by the State Key Laboratory of Explosion Science and Technology(Beijing Institute of Technology)(YBKT16-09,QNKT16-03)
摘要The nitrogen content of tetrazolo triazines is 68.9%.In this paper,tetrazolotriazines was synthetized.The TG-DSC test indicated its decomposition process in detail.The non-isothermal kinetic parameters were speculated by Kissinger and Ozawa methods.It revealed the mechanism function of thermal decomposition.The impact and friction sensitivity were tested.The detonation pressure and velocity were calculated.It has a wide range of potential applications as a kind of energetic material.
摘要Composting as a solution to the increasing generation of municipal solid waste (MSW), also contribute to GHGs emission when not controlled and could lack some basic nutrients, especially nitrogen. This study assessed the split-additions of nitrogen-rich substrate to composting materials and their effect on GHGs emissions as well as the quality of the composts. Nitrogen-rich substrates formulated from pig and goat manure were co-composted with MSW for a 12-weeks period by split adding at mesophilic (˚C) and thermophilic (>50˚C) stages in five different treatments. Representative samples from the compost were taken from each treatment for physicochemical, heavy metals and bacteriological analysis. In-situ CH4, CO2, N2O gas emissions were also analyzed weekly during composting. It was observed that all the treatments showed significant organic matter decomposition, reaching thermophilic temperatures in the first week of composting. The absence affects the suitable agronomic properties. All nitrogen-rich substrate applied at thermophilic stage (Treatment two) recorded the highest N, P and K concentrations of 1.34%, 0.97% and 2.45%, respectively with highest nitrogen retention. In terms of GHG emissions, CO2 was highest at the thermophilic stage when N-rich substrate was added in all treatment, while CH4 was highest in the mesophilic stage with N-rich substrate addition. N2O showed no specific trend in the treatments. Split addition of the N-rich substrate for co-composting of MSW produced compost which is stable, has less nutrient loss and low GHG emissions. Split addition of a nitrogen-rich substrate could be an option for increasing the fertilizer value of MSW compost.
摘要Energetic coordination compound with 5-nitro-tetrazole (NT) as ligand has gained more and more attentions due to its extreme explosive properties and ecological friendly pyrolysis productsF1-61 The research results in 1994 proposed from Sandia National Laboratories proves tetrammine-cis-bis (5-nitro-2H-tetrazole-N2 ) cobalt ( Ⅲ ) perchlorate (BNCP) to be a more powerful explosive and undergoes deflagration-to- detonation (DDT)
基金supported by the Science&Technology Department of Jilin Province(20230508057RC)。
摘要Redox-active porous aromatic frameworks(PAFs)have emerged as hopeful candidates for sodium-ion batteries(SIBs)in view of their porous structures,chemical stability and tunable architectures.Herein,we successfully synthesized two redox-active PAFs(PAF-305 and PAF-306)with different nitrogen-containing motifs,and demonstrated their application as cathode materials for SIBs.Density functional theory(DFT)calculations reveal that nitrogen-rich PAF-305 exhibits a lower lowest unoccupied molecular orbital(LUMO)energy level(-3.35 eV)and a narrower energy gap(Eg)(2.40 eV)compared with nitrogen-poor PAF-306.As expected,PAF-305 displays outstanding electrochemical performance,comprising a high reversible capacity of 145.2 mAh g-1at 0.05 A g-1and satisfactory cycling stability with 92% capacity retention over 1000 cycles at 0.2 A g-1.Remarkably,PAF-305 maintains robust electrochemical properties across a wide temperature range(-20℃ to 50℃).Through a combination of experimental characterizations and theoretical calculations,the sodium-ion storage mechanism of PAF-305 is elucidated.This study not only provides a promising strategy for exploring other redox-active organic units in the design of novel PAFs,but also expands the potential applications of PAFs in energy storage systems.
基金supported financially by the Jiangxi Provincial Natural Science Foundation(20232BAB203009)the National Natural Science Foundation of China(22506017,22376024).
摘要Covalent organic frameworks(COFs)are promising candidates for the rapid purification of toxic pollutants and mitigation of radioactive iodine leakage in nuclear accidents.In particular,COFs constructed from meta-position monomers can form clover-like morphology,increasing the specific surface area and providing multidimensional diffusion pathways for iodine.Herein,two nitrogen-rich COFs(DFPT-COF and DFPB-COF)featuring well-defined cloverlike nanochannels were successfully fabricated,demonstrating exceptional iodine capture performance.Compared to DFPB-COF,DFPT-COF exhibits better iodine capture performance(5.58 g g−1for I2vapor)due to its large specific surface area and rich nitrogen adsorption sites.Moreover,the adsorption dynamics of DFPT-COF for liquid iodine follow a pseudosecond-order kinetic model and the adsorption isotherm model complies with the Langmuir model.Notably,DFPT-COF exhibited excellent renewable adsorption performance,suggesting its potential as a sustainable and efficient green adsorbent for iodine in nuclear waste management.
基金supported by the National Natural Science Foundation of China(Grant Nos.22105156,22175139,22505195,22171136,22405207 and 22302156)the China National Science Fund for Distinguished Young Scholars(Grant No.22325504)。
摘要The pursuit of heat-resistant energetic materials(HREMs)with thermal stability beyond 450℃ presents a significant challenge that has yet to be achieved.In this work,we develop an innovative electronic delocalization strategy to design and synthesize a planar dizwitterionic diamino-bistriazolotetrazine,designated as TYX-1.The unique structural feature of TYX-1,including a nitrogen-rich fused ring system,planar conformation,and dizwitterionic configuration,combined with its hydrogen-bonded organic framework(HOF)structure,confer exceptional thermal stability(The onset temperature is 428℃,and the peak temperature is 473℃),high density(1.84 g/cm3),and remarkable detonation performance(detonation velocity:8616 m/s).Furthermore,TYX-1 exhibits an impressive insensitivity(impact sensitivity>40 J;friction sensitivity>360 N),surpassing all previously reported HREMs.Theoretical calculations and single-crystal clearly indicate that the delocalizedπelectrons within the dizwitterionic bistriazolotetrazine rings and the HOF structure of TYX-1 are pivotal in ensuring its high thermal stability and high energy density.The discovery of TYX-1 marks a significant advancement in the field of HREMs and is anticipated to catalyze substantial progress in various high-temperature applications reliant on energetic materials.
基金supported by the National Research Foundation (NRF),Prime Minister’s Office,Singapore under its NRF Fellowship (NRF2009NRF-RF001-015)Campus for Research Excellence and Technological Enterprise (CREATE)Programme-Singapore Peking University Research Centre for a Sustainable Low-Carbon Futurethe NTU-A*Star Centre of Excellence for Silicon Technologies (A*Star SERC No.:1123510003).
摘要An imine-based nitrogen-rich covalent-organic framework(COF)was successfully synthesized using two tri-angular building units under solvothermal reaction condition.The gas adsorption properties of the obtained micro-porous nitrogen-rich COF were investigated.The results indicated that the activated COF material presented good up take capabilities of CO2 and CH4 at 61.2 and 43.4 cm3·g−1at 1 atm and 273 K,respectively,showing its applica-tion potential in selective gas capture and separation.
基金This work was supported by the National Natural Science Foundation of China(No.21872008)the Natural Science Foundation of Beijing,China(No.2212019)Beijing Institute of Technology Research Fund Program for Young Scholars(Nos.3100011182019 and 3100011182128).We would also thank the Analysis&Testing Center of Beijing Institute of Technology measurements.
摘要Eliminating the usage of metal current collectors and binders in traditional battery electrode configuration is an effective strategy to significantly improve the capacities of lithium ion batteries (LIBs). Herein, we demonstrate the construction of porous vanadium nitride (VN) nanosheet network in situ grown on nitrogen-rich (N-rich) carbon textile (N-C@P-VN) as lightweight and binder-free anode for LIBs. The N-rich carbon textile is used both as the current collector and host to store Li+, thus improving the specific capacities of binder-free VN anode and meanwhile reducing the inert mass of the whole cell. Moreover, the open spaces in carbon textile and vertically aligned pores in VN nanosheet network can not only provide an expressway for Li+ and e− transport, but also afford more active sites. As a result, the binder-free N-C@P-VN anode maintains a specific capacity of 1,040 mAh·g−1 (or an areal capacity of 2.6 mAh·cm−2) after 100 cycles at 0.1 mA·cm−2 in half cell. Moreover, in an assembled N-C@P-VN//LiFePO4 full cell, it exhibits an areal capacity of 1.7 mAh·cm−2 after 300 cycles at 0.1 C. The synergistic strategy of N-C substrate and porous VN network could be applied to guide rational design of similar N-C@nitride or sulfide hybrid systems with corresponding sulfur-doped carbon textile as the substrate.