N-doped carbons as one of the most prominent anode materials to replace standard graphite exhibit outstanding Li+storage performance.However,N-doped carbon anodes still suffer from low N-doping levels and low initial ...N-doped carbons as one of the most prominent anode materials to replace standard graphite exhibit outstanding Li+storage performance.However,N-doped carbon anodes still suffer from low N-doping levels and low initial Coulombic efficiency(ICE).In this study,high N-doped and low graphitic-N carbons(LGNCs)with enhanced ICE were synthesized by taking advantage of a denitrification strategy for graphitic carbon nitride(g-C_(3)N_(4)).In brief,more than 14.5 at%of N from g-C_(3)N_(4)(55.1 at%N)was retained by reacting graphitic-N with lithium,which was subsequently removed.As graphitic-N is largely responsible for the irreversible capacity,the anode's performance was significantly increased.Compared to general N-doped carbons with high graphitic-N proportion(>50%)and low N content(<15 at%),LGNCs delivered a low proportion of 10.8%-17.2% within the high N-doping content of 14.5-42.7 at%,leading to an enhanced specific capacity of 1499.9mAh g^(-1) at an ICE of 93.7% for the optimal sample of LGNC(4:1).This study provides a facile strategy to control the N content and speciation,achieving both high Li+storage capacity and high ICE,and thus promoting research and application of N-doped carbon materials.展开更多
Hydrogels offer tissue-like softness,stretchability,fracture toughness,ionic conductivity,and compatibility with biological tissues,which make them promising candidates for fabricating flexible bioelectronics.A soft h...Hydrogels offer tissue-like softness,stretchability,fracture toughness,ionic conductivity,and compatibility with biological tissues,which make them promising candidates for fabricating flexible bioelectronics.A soft hydrogel film offers an ideal interface to directly bridge thin-film electronics with the soft tissues.However,it remains difficult to fabricate a soft hydrogel film with an ultrathin configuration and excellent mechanical strength.Here we report a biological tissue-inspired ultrasoft microfiber composite ultrathin(<5μm)hydrogel film,which is currently the thinnest hydrogel film as far as we know.The embedded microfibers endow the composite hydrogel with prominent mechanical strength(tensile stress~6 MPa)and anti-tearing property.Moreover,our microfiber composite hydrogel offers the capability of tunable mechanical properties in a broad range,allowing for matching the modulus of most biological tissues and organs.The incorporation of glycerol and salt ions imparts the microfiber composite hydrogel with high ionic conductivity and prominent anti-dehydration behavior.Such microfiber composite hydrogels are promising for constructing attaching-type flexible bioelectronics to monitor biosignals.展开更多
P2-type layered oxides with the general Na-deficient composition Na_(x)TMO_(2)(x<1,TM:transition metal)are a promising class of cathode materials for sodium-ion batteries.The open Na+transport pathways present in t...P2-type layered oxides with the general Na-deficient composition Na_(x)TMO_(2)(x<1,TM:transition metal)are a promising class of cathode materials for sodium-ion batteries.The open Na+transport pathways present in the structure lead to low diffusion barriers and enable high charge/discharge rates.However,a phase transition from P2 to O2 structure occurring above 4.2 V and metal dissolution at low potentials upon discharge results in rapid capacity degradation.In this work,we demonstrate the positive effect of configurational entropy on the stability of the crystal structure during battery operation.Three different compositions of layered P2-type oxides were synthesized by solid-state chemistry,Na_(0.67)(Mn_(0.55)Ni_(0.21)Co_(0.24))O_(2),Na_(0.67)(Mn_(0.45)Ni_(0.18)Co_(0.24)Ti_(0.1)Mg_(0.03))O_(2) and Na_(0.67)(Mn_(0.45)Ni_(0.18)Co_(0.18)Ti_(0.1)Mg_(0.03)Al_(0.04)Fe_(0.02))O_(2) with low,medium and high configurational entropy,respectively.The high-entropy cathode material shows lower structural transformation and Mn dissolution upon cycling in a wide voltage range from 1.5 to 4.6 V.Advanced operando techniques and post-mortem analysis were used to probe the underlying reaction mechanism thoroughly.Overall,the high-entropy strategy is a promising route for improving the electrochemical performance of P2 layered oxide cathodes for advanced sodium-ion battery applications.展开更多
基金National Natural Science Foundation of China,Grant/Award Number:51777138Deutsche Forschungsgemeinschaft(DFG,German Research Foundation),Grant/Award Number:491183248Open Access Publishing Fund of the University of Bayreuth。
文摘N-doped carbons as one of the most prominent anode materials to replace standard graphite exhibit outstanding Li+storage performance.However,N-doped carbon anodes still suffer from low N-doping levels and low initial Coulombic efficiency(ICE).In this study,high N-doped and low graphitic-N carbons(LGNCs)with enhanced ICE were synthesized by taking advantage of a denitrification strategy for graphitic carbon nitride(g-C_(3)N_(4)).In brief,more than 14.5 at%of N from g-C_(3)N_(4)(55.1 at%N)was retained by reacting graphitic-N with lithium,which was subsequently removed.As graphitic-N is largely responsible for the irreversible capacity,the anode's performance was significantly increased.Compared to general N-doped carbons with high graphitic-N proportion(>50%)and low N content(<15 at%),LGNCs delivered a low proportion of 10.8%-17.2% within the high N-doping content of 14.5-42.7 at%,leading to an enhanced specific capacity of 1499.9mAh g^(-1) at an ICE of 93.7% for the optimal sample of LGNC(4:1).This study provides a facile strategy to control the N content and speciation,achieving both high Li+storage capacity and high ICE,and thus promoting research and application of N-doped carbon materials.
基金the funding support from the fellowship of the China Postdoctoral Science Foundation (2022M722329, 2021M700097)the National Natural Science Foundation for Distinguished Young Scholars of China (62125112)+2 种基金the National Natural Science Foundation of China (62071462, 62071463, 62271479, 22109173)the Jiangxi Provincial Natural Science Foundation (20224ACB212001)the support from Nano-X Vacuum Interconnected Workstation&Key Laboratory of Multifunctional Nanomaterials and Smart Systems of Suzhou Institute of Nano-Tech and Nano-Bionics (SINANO),Chinese Academy of Sciences (CAS)
文摘Hydrogels offer tissue-like softness,stretchability,fracture toughness,ionic conductivity,and compatibility with biological tissues,which make them promising candidates for fabricating flexible bioelectronics.A soft hydrogel film offers an ideal interface to directly bridge thin-film electronics with the soft tissues.However,it remains difficult to fabricate a soft hydrogel film with an ultrathin configuration and excellent mechanical strength.Here we report a biological tissue-inspired ultrasoft microfiber composite ultrathin(<5μm)hydrogel film,which is currently the thinnest hydrogel film as far as we know.The embedded microfibers endow the composite hydrogel with prominent mechanical strength(tensile stress~6 MPa)and anti-tearing property.Moreover,our microfiber composite hydrogel offers the capability of tunable mechanical properties in a broad range,allowing for matching the modulus of most biological tissues and organs.The incorporation of glycerol and salt ions imparts the microfiber composite hydrogel with high ionic conductivity and prominent anti-dehydration behavior.Such microfiber composite hydrogels are promising for constructing attaching-type flexible bioelectronics to monitor biosignals.
基金financial support from the China Scholarship Council(CSC)financial support by Deutsche Forschungsgemeinschaft(DFG,German Research Foundation)under Germany’s Excellence Strategy,EXC 2154,project number 390874152+8 种基金financial support from the Federal Ministry of Education and Research(Bundesministerium für Bildung und Forschung,BMBF)under the project‘KaSiLi’(03XP0254D)in the competence cluster‘Excell-BattMat’financial support from the Helmholtz Association(DigiBat project)support by the German Research Foundation(to H H,Grant No.HA 1344/43-1)is gratefully acknowledgedsupport from EnABLES and EPISTORE,projects funded by the European Union’s Horizon 2020 research and innovation program under Grant Agreement No.730957 and 101017709,respectivelyfunding from the Kera-Solar project(Carl Zeiss Foundation)support at beamline P65 of the PETRA Ⅲ synchrotron(Deutsches Elektronen-Synchrotron DESY,Hamburg,Germany)is gratefully acknowledgedEduard Arzt(INM)for his continuing supportAndrea Jung(INM)for her support on ICP-OES measurementsthe support from the Karlsruhe Nano Micro Facility(KNMF,www.knmf.kit.edu),a Helmholtz research infrastructure at Karlsruhe Institute of Technology(KIT,www.kit.du).
文摘P2-type layered oxides with the general Na-deficient composition Na_(x)TMO_(2)(x<1,TM:transition metal)are a promising class of cathode materials for sodium-ion batteries.The open Na+transport pathways present in the structure lead to low diffusion barriers and enable high charge/discharge rates.However,a phase transition from P2 to O2 structure occurring above 4.2 V and metal dissolution at low potentials upon discharge results in rapid capacity degradation.In this work,we demonstrate the positive effect of configurational entropy on the stability of the crystal structure during battery operation.Three different compositions of layered P2-type oxides were synthesized by solid-state chemistry,Na_(0.67)(Mn_(0.55)Ni_(0.21)Co_(0.24))O_(2),Na_(0.67)(Mn_(0.45)Ni_(0.18)Co_(0.24)Ti_(0.1)Mg_(0.03))O_(2) and Na_(0.67)(Mn_(0.45)Ni_(0.18)Co_(0.18)Ti_(0.1)Mg_(0.03)Al_(0.04)Fe_(0.02))O_(2) with low,medium and high configurational entropy,respectively.The high-entropy cathode material shows lower structural transformation and Mn dissolution upon cycling in a wide voltage range from 1.5 to 4.6 V.Advanced operando techniques and post-mortem analysis were used to probe the underlying reaction mechanism thoroughly.Overall,the high-entropy strategy is a promising route for improving the electrochemical performance of P2 layered oxide cathodes for advanced sodium-ion battery applications.