TiNb_(2)O_(7)represents an up-and-coming anode material for fast-charging lithium-ion batteries,but its practicalities are severely impeded by slow transfer rates of ionic and electronic especially at the low-temperat...TiNb_(2)O_(7)represents an up-and-coming anode material for fast-charging lithium-ion batteries,but its practicalities are severely impeded by slow transfer rates of ionic and electronic especially at the low-temperature conditions.Herein,we introduce crystallographic engineering to enhance structure stability and promote Li+diffusion kinetics of TiNb_(2)O_(7)(TNO).The density functional theory computation reveals that Ti^(4+)is replaced by Sb^(5+)and Nb^(5+)in crystal lattices,which can reduce the Li+diffusion impediment and improve electronic conductivity.Synchrotron radiation X-ray 3D nano-computed tomography and in situ X-ray diffraction measurement confirm the introduction of Sb/Nb alleviates volume expansion during lithiation and delithiation processes,contributing to enhancing structure stability.Extended X-ray absorption fine structure spectra results verify that crystallographic engineering also increases short Nb-O bond length in TNO-Sb/Nb.Accordingly,the TNO-Sb/Nb anode delivers an outstanding capacity retention rate of 89.8%at 10 C after 700 cycles and excellent rate performance(140.4 mAh g^(−1) at 20 C).Even at−30℃,TNO-Sb/Nb anode delivers a capacity of 102.6 mAh g^(−1) with little capacity degeneration for 500 cycles.This work provides guidance for the design of fast-charging batteries at low-temperature condition.展开更多
Micrometer-sized silicon oxide(SiO)anodes encounter challenges in large-scale applications due to significant volume expansion during the alloy/de-alloy process.Herein,an innovative deep eutectic electrolyte derived f...Micrometer-sized silicon oxide(SiO)anodes encounter challenges in large-scale applications due to significant volume expansion during the alloy/de-alloy process.Herein,an innovative deep eutectic electrolyte derived from succinonitrile is introduced to enhance the cycling stability of SiO anodes.Density functional theory calculations validate a robust ion-dipole interaction between lithium ions(Li^(+))and succinonitrile(SN).The cosolvent fluoroethylene carbonate(FEC)optimizes the Li^(+)solvation structure in the SN-based electrolyte with its weakly solvating ability.Molecular dynamics simulations investigate the regulating mechanism of ion-dipole and cation-anion interaction.The unique Li^(+)solvation structure,enriched with FEC and TFSI^(-),facilitates the formation of an inorganic-organic composite solid electrolyte interphase on SiO anodes.Micro-CT further detects the inhibiting effect on the SiO volume expansion.As a result,the SiO|LiCoO_(2) full cells exhibit excellent electrochemical performance in deep eutectic-based electrolytes.This work presents an effective strategy for extending the cycle life of SiO anodes by designing a new SN-based deep eutectic electrolyte.展开更多
Sodium metal batteries(SMBs)are promising candidates for next-generation energy storage devices owing to their excellent safety performance and natural abunda nce of sodium.However,the insurmountable obstacles of dend...Sodium metal batteries(SMBs)are promising candidates for next-generation energy storage devices owing to their excellent safety performance and natural abunda nce of sodium.However,the insurmountable obstacles of dendrite formation and quick capacity decay are caused by an unstable and inhomogeneous solid electrolyte interphase that resulted from the immediate interactions between the Na metal anode and organic liquid electrolyte.Herein,a customised glass fibre separator coupled with chitosan(CS@GF)was developed to modulate the sodium ion(Na^(+))flux.The CS@GF separator facilitates the Na+homogeneous deposition on the anode side through redistribution at the chitosan polyactive sites and by inhibiting the decomposition of the electrolyte to robust solid electrolyte interphase(SEI)formation.Multiphysics simulations show that chitosan incorporated into SMBs through the separator can make the local electric field around the anode uniform,thus facilitating the transfer of cations.Na|Na symmetric cells utilising a CS@GF separator exhibited an outstanding cycle stability of over 600 h(0.5 mA cm^(-2)).Meanwhile,the Na|Na_(3)V_(5)(PO_(4))_(3)full cell exhibited excellent fast-charging performance(93.47%capacity retention after 1500 cycles at 5C).This study presents a promising strategy for inhibiting dendrite growth and realizes stable Na metal batteries,which significantly boosts the development of high-performance SMBs.展开更多
Ultrahigh-Ni layered oxide cathodes suffer from high surface reactivity and severe strain propagation in sulfide all-solid-state batteries.Herein,we propose an in situ transformation strategy employing indium oxide to...Ultrahigh-Ni layered oxide cathodes suffer from high surface reactivity and severe strain propagation in sulfide all-solid-state batteries.Herein,we propose an in situ transformation strategy employing indium oxide to“capture”residual lithium impurities on the ultrahigh-Ni LiNi_(0.9)Co_(0.05)Mn_(0.05)O_(2)(NCM90)cathode.Simultaneously,the near-surface structure is reconstructed and forms a conformal epitaxial layer via residual alkali“welding”.The reconstructed layer effectively suppresses spontaneous side reactions at the cathode-electrolyte interface and then prevents the structural fatigue in the bulk phase.The sulfide all-solid-state lithium batteries(ASSLBs)deliver a high reversible capacity of∼2 mAh cm^(–2)(>190 mAh g^(–1),0.069 mA cm^(–2)),long cycling stability,and a good rate capability with a cathode loading of 9 mg cm^(–2).Coupling synchrotron X-ray tomography(micro-/nano-CT)and X-ray absorption near-edge structure(XANES),the multi-scale observations from the particle level to the electrode levels reveal greatly alleviated interfacial instability and chemo-mechanical disintegration.We highlight the importance of surface engineering in stabilizing Ni-rich layered cathodes toward high-energy sulfide ASSLBs.展开更多
Research on biometrics for high security applica- tions has not attracted as much attention as civilian or foren- sic applications. Limited research and deficient analysis so far has led to a lack of general solutions...Research on biometrics for high security applica- tions has not attracted as much attention as civilian or foren- sic applications. Limited research and deficient analysis so far has led to a lack of general solutions and leaves this as a challenging issue. This work provides a systematic analy- sis and identification of the problems to be solved in order to meet the performance requirements for high security applica- tions, a double low problem. A hybrid ensemble framework is proposed to solve this problem. Setting an adequately high threshold for each matcher can guarantee a zero false accep- tance rate （FAR） and then use the hybrid ensemble framework makes the false reject rate （FRR） as low as possible. Three ex- periments are performed to verify the effectiveness and gener- alization of the framework. First, two fingerprint verification algorithms are fused. In this test only 10.55% of fingerprints are falsely rejected with zero false acceptance rate, this is sig- nificantly lower than other state of the art methods. Second, in face verification, the framework also results in a large re- duction in incorrect classification. Finally, assessing the per- formance of the framework on a combination of face and gait verification using a heterogeneous database show this frame- work can achieve both 0% false rejection and 0% false accep- tance simultaneously.展开更多
基金supported by the National Natural Science Foundation of China(22279026,2247090373)the Natural Science Foundation of Chongqing(CSTB2022NSCQ-MSX1401)+2 种基金the China Postdoctoral Science Foundation(2024M764198)the National Natural Science Foundation of China(22509044)the Fundamental Research Funds for the Central Universities(grant no.HIT.OCEF.2022017).
文摘TiNb_(2)O_(7)represents an up-and-coming anode material for fast-charging lithium-ion batteries,but its practicalities are severely impeded by slow transfer rates of ionic and electronic especially at the low-temperature conditions.Herein,we introduce crystallographic engineering to enhance structure stability and promote Li+diffusion kinetics of TiNb_(2)O_(7)(TNO).The density functional theory computation reveals that Ti^(4+)is replaced by Sb^(5+)and Nb^(5+)in crystal lattices,which can reduce the Li+diffusion impediment and improve electronic conductivity.Synchrotron radiation X-ray 3D nano-computed tomography and in situ X-ray diffraction measurement confirm the introduction of Sb/Nb alleviates volume expansion during lithiation and delithiation processes,contributing to enhancing structure stability.Extended X-ray absorption fine structure spectra results verify that crystallographic engineering also increases short Nb-O bond length in TNO-Sb/Nb.Accordingly,the TNO-Sb/Nb anode delivers an outstanding capacity retention rate of 89.8%at 10 C after 700 cycles and excellent rate performance(140.4 mAh g^(−1) at 20 C).Even at−30℃,TNO-Sb/Nb anode delivers a capacity of 102.6 mAh g^(−1) with little capacity degeneration for 500 cycles.This work provides guidance for the design of fast-charging batteries at low-temperature condition.
基金supported by the National Natural Science Foundation of China(22279026)the National Key Research and Development Program of China(2022YFE0138900)+2 种基金the Young Elite Scientist sponsorship program by CAST(no.20200148)the Natural Science Funds of Heilongjiang Province(YQ2021B003)the Fundamental Research Funds for the Central Universities(grant no.HIT.OCEF.2022017).
文摘Micrometer-sized silicon oxide(SiO)anodes encounter challenges in large-scale applications due to significant volume expansion during the alloy/de-alloy process.Herein,an innovative deep eutectic electrolyte derived from succinonitrile is introduced to enhance the cycling stability of SiO anodes.Density functional theory calculations validate a robust ion-dipole interaction between lithium ions(Li^(+))and succinonitrile(SN).The cosolvent fluoroethylene carbonate(FEC)optimizes the Li^(+)solvation structure in the SN-based electrolyte with its weakly solvating ability.Molecular dynamics simulations investigate the regulating mechanism of ion-dipole and cation-anion interaction.The unique Li^(+)solvation structure,enriched with FEC and TFSI^(-),facilitates the formation of an inorganic-organic composite solid electrolyte interphase on SiO anodes.Micro-CT further detects the inhibiting effect on the SiO volume expansion.As a result,the SiO|LiCoO_(2) full cells exhibit excellent electrochemical performance in deep eutectic-based electrolytes.This work presents an effective strategy for extending the cycle life of SiO anodes by designing a new SN-based deep eutectic electrolyte.
基金funded by the Key Research and Development Program of Shandong Province(2023CXPT069)Opening Funds of the State Key Laboratory of Building Safety and Built Environment(BSBE2022-EET-06)Innovation Project of Guangwei Group Academician Workstation(GWYS-2022-04)。
文摘Sodium metal batteries(SMBs)are promising candidates for next-generation energy storage devices owing to their excellent safety performance and natural abunda nce of sodium.However,the insurmountable obstacles of dendrite formation and quick capacity decay are caused by an unstable and inhomogeneous solid electrolyte interphase that resulted from the immediate interactions between the Na metal anode and organic liquid electrolyte.Herein,a customised glass fibre separator coupled with chitosan(CS@GF)was developed to modulate the sodium ion(Na^(+))flux.The CS@GF separator facilitates the Na+homogeneous deposition on the anode side through redistribution at the chitosan polyactive sites and by inhibiting the decomposition of the electrolyte to robust solid electrolyte interphase(SEI)formation.Multiphysics simulations show that chitosan incorporated into SMBs through the separator can make the local electric field around the anode uniform,thus facilitating the transfer of cations.Na|Na symmetric cells utilising a CS@GF separator exhibited an outstanding cycle stability of over 600 h(0.5 mA cm^(-2)).Meanwhile,the Na|Na_(3)V_(5)(PO_(4))_(3)full cell exhibited excellent fast-charging performance(93.47%capacity retention after 1500 cycles at 5C).This study presents a promising strategy for inhibiting dendrite growth and realizes stable Na metal batteries,which significantly boosts the development of high-performance SMBs.
基金supported by the National Natural Science Foundation of China(22279026 and 22479036)the Major Science and Technology Projects for Independent Innovation of China FAW Group Co.,Ltd.(20240301002ZD)the Fundamental Research Funds for the Central Universities(XNJKKGYDJ2024015).
文摘Ultrahigh-Ni layered oxide cathodes suffer from high surface reactivity and severe strain propagation in sulfide all-solid-state batteries.Herein,we propose an in situ transformation strategy employing indium oxide to“capture”residual lithium impurities on the ultrahigh-Ni LiNi_(0.9)Co_(0.05)Mn_(0.05)O_(2)(NCM90)cathode.Simultaneously,the near-surface structure is reconstructed and forms a conformal epitaxial layer via residual alkali“welding”.The reconstructed layer effectively suppresses spontaneous side reactions at the cathode-electrolyte interface and then prevents the structural fatigue in the bulk phase.The sulfide all-solid-state lithium batteries(ASSLBs)deliver a high reversible capacity of∼2 mAh cm^(–2)(>190 mAh g^(–1),0.069 mA cm^(–2)),long cycling stability,and a good rate capability with a cathode loading of 9 mg cm^(–2).Coupling synchrotron X-ray tomography(micro-/nano-CT)and X-ray absorption near-edge structure(XANES),the multi-scale observations from the particle level to the electrode levels reveal greatly alleviated interfacial instability and chemo-mechanical disintegration.We highlight the importance of surface engineering in stabilizing Ni-rich layered cathodes toward high-energy sulfide ASSLBs.
文摘Research on biometrics for high security applica- tions has not attracted as much attention as civilian or foren- sic applications. Limited research and deficient analysis so far has led to a lack of general solutions and leaves this as a challenging issue. This work provides a systematic analy- sis and identification of the problems to be solved in order to meet the performance requirements for high security applica- tions, a double low problem. A hybrid ensemble framework is proposed to solve this problem. Setting an adequately high threshold for each matcher can guarantee a zero false accep- tance rate （FAR） and then use the hybrid ensemble framework makes the false reject rate （FRR） as low as possible. Three ex- periments are performed to verify the effectiveness and gener- alization of the framework. First, two fingerprint verification algorithms are fused. In this test only 10.55% of fingerprints are falsely rejected with zero false acceptance rate, this is sig- nificantly lower than other state of the art methods. Second, in face verification, the framework also results in a large re- duction in incorrect classification. Finally, assessing the per- formance of the framework on a combination of face and gait verification using a heterogeneous database show this frame- work can achieve both 0% false rejection and 0% false accep- tance simultaneously.
