Potassium-ion hybrid capacitors(KIHCs) have attracted increasing research interest because of the virtues of potassium-ion batteries and supercapacitors.The development of KIHCs is subject to the investigation of appl...Potassium-ion hybrid capacitors(KIHCs) have attracted increasing research interest because of the virtues of potassium-ion batteries and supercapacitors.The development of KIHCs is subject to the investigation of applicable K+storage materials which are able to accommodate the relatively large size and high activity of potassium.Here,we report a cocoon silk chemistry strategy to synthesize a hierarchically porous nitrogen-doped carbon(SHPNC).The as-prepared SHPNC with high surface area and rich N-doping not only offers highly efficient channels for the fast transport of electrons and K ions during cycling,but also provides sufficient void space to relieve volume expansion of electrode and improves its stability.Therefore,KIHCs with SHPNC anode and activated carbon cathode afford high energy of 135 Wh kg-1(calculated based on the total mass of anode and cathode),long lifespan,and ultrafast charge/slow discharge performance.This study defines that the KIHCs show great application prospect in the field of high-performance energy storage devices.展开更多
Lithium metal has gained extensive attention as the most ideal candidate for next-generation battery anode owing to the ultrahigh specific capacity and the lowest electrochemical potential.However,uncontrollable dendr...Lithium metal has gained extensive attention as the most ideal candidate for next-generation battery anode owing to the ultrahigh specific capacity and the lowest electrochemical potential.However,uncontrollable dendrite growth and huge volume variation extremely restrict the future deployment of lithium metal batteries.Herein,we report metal chalcogenide SnSSe with unique nanoplate stacking structure as a robust substrate for stable Li metal anode.During the initial Li plating process,lithiophilic Li_(22)Sn_(5) alloy and Li_(2)S/Li_(2)Se sites are obtained via in-situ electrochemical reaction of Li metal and SnSSe.Density functional theory(DFT)calculation demonstrates that the formed Li_(2)S/Li_(2)Se achieves low Li diffusion energy barrier,ensuring rapid Li~+migration.Li_(22)Sn_(5) alloy provides strong nucleation sites,promoting uniform Li nucleation.Furthermore,in-situ optical microscopy analysis suggests that the synthesized effect fundamentally inhibits lithium dendrite growth.Consequently,SnSSe modified Cu foil delivered an ultralow nucleation overpotential,superior cycling stability with 450 cycles(Coulombic efficiency,>98%),and excellent plating/stripping behavior over 2200 h at 0.5 mA cm^(-2).Moreover,the brilliant reversible cycles and rate capability were also realized in Li@SnSSe//LiFePO_(4)(LFP)full cell,shedding light on the feasibility of SnSSe for stable and dendrite-free lithium metal anode.展开更多
High areal capacity is one of the critically important points for potassium-ion batteries(PIBs)for practical applications,which relies on high areal-massloading electrodes operating at high reversible capacity.However...High areal capacity is one of the critically important points for potassium-ion batteries(PIBs)for practical applications,which relies on high areal-massloading electrodes operating at high reversible capacity.However,it is remarkably restricted by the mechanical instability and sluggish charge transfer induced by the increased mass loading.To overcome such challenge,we report the rationally designed bimetallic selenides CoSe2/SnSe2 heterostructures confined in hierarchical carbon nanofibers(CSSe@CNFs),which enables the electrodes robust mechanical stability,enhanced electron transport,and reduced ion-diffusion energy barrier for facilitating reaction kinetics.Accordingly,an impressive areal mass loading up to 25.3 mg cm^(−2)was achieved,which endowed a high areal capacity of 7.58 mAh cm^(−2)for such a free-standing electrode.This is stateof-the-art among the PIBs,exceeding that of today’s industry standard(∼3 mAh cm^(−2)for LIBs).Furthermore,it delivered long-term stability over 3700 cycles at high current density(∼2 mA cm^(−2),vs 1 mA cm^(−2)in LIBs).Moreover,the as-constructed full battery achieved a high energy density of 172.8 Wh kg-1 at 0.05 A g^(−1)with a satisfied cycle stability over 2000 cycles at 2 A g^(−1)and high reversibility with Coulombic efficiency of 100%;thus,signifying its bright future toward commercial application for advanced PIBs.展开更多
In speech recognition research,because of the variety of languages,corresponding speech recognition systems need to be constructed for different languages.Especially in a dialect speech recognition system,there are ma...In speech recognition research,because of the variety of languages,corresponding speech recognition systems need to be constructed for different languages.Especially in a dialect speech recognition system,there are many special words and oral language features.In addition,dialect speech data is very scarce.Therefore,constructing a dialect speech recognition system is difficult.This paper constructs a speech recognition system for Sichuan dialect by combining a hidden Markov model(HMM)and a deep long short-term memory(LSTM)network.Using the HMM-LSTM architecture,we created a Sichuan dialect dataset and implemented a speech recognition system for this dataset.Compared with the deep neural network(DNN),the LSTM network can overcome the problem that the DNN only captures the context of a fixed number of information items.Moreover,to identify polyphone and special pronunciation vocabularies in Sichuan dialect accurately,we collect all the characters in the dataset and their common phoneme sequences to form a lexicon.Finally,this system yields a 11.34%character error rate on the Sichuan dialect evaluation dataset.As far as we know,it is the best performance for this corpus at present.展开更多
Potassium-ion batteries(PIBs)are of academic and economic significance,but still limited by the lack of highly active electrode materials for de-/intercalation of large-radius K ions.Herein,an interconnected nitrogen/...Potassium-ion batteries(PIBs)are of academic and economic significance,but still limited by the lack of highly active electrode materials for de-/intercalation of large-radius K ions.Herein,an interconnected nitrogen/sulfur co-doped carbon nanosheep bundle(N/S-CSB)was proposed as the potassium ions storage material.The rich co-doping of nitrogen/sulfur of N/S-CNB with three-dimensional hierarchical bundled array structure yields distensible interlayer spaces to buffer the volume expansion during K+insertion/extraction,offers more electrochemical active sites to obtain a high specific capacity,and provides efficient channels for fast ion/electron transports.Therefore,the N/S-CSB anode achieved high reversible specific capacity of 365 mAh/g obtained at 50 mA/g after 200 cycles with a coulombic efficiency(CE)close to 100%,high rate performance and long cycle stability.Moreover,the in-situ Raman spectra indicated outstanding reaction kinetics of as-prepared N/S-CSB anode.展开更多
钾离子电池(PIBs)面临的一个关键问题是设计具有先进结构的负极材料,以实现快速电荷传输以提高钾的存储性能.采用碳二亚胺铁(FeNCN)作为阳极,由于其含有一定数量的共价键且在分子水平上具有稳定的结构,使得储钾系统能够实现优异的电化...钾离子电池(PIBs)面临的一个关键问题是设计具有先进结构的负极材料,以实现快速电荷传输以提高钾的存储性能.采用碳二亚胺铁(FeNCN)作为阳极,由于其含有一定数量的共价键且在分子水平上具有稳定的结构,使得储钾系统能够实现优异的电化学性能.FeNCN阳极具有高导电性,带隙接近0 eV,并且由于其共价键结构具有良好的结构稳定性.此外,无定形反应产物也为离子扩散提供了多种途径.因此,FeNCN阳极表现出高可逆比容量(在50 mA g^(-1)电流密度下具有600 mA h g^(-1)比容量),显著的倍率性能和长寿命循环(电流密度为500 mA g^(-1)时拥有400 mA h g^(-1)比容量且超过300次循环).通过理论模拟、X射线原位衍射分析和X射线光电子能谱分析揭示了Fe^(2+)和K^(+)之间的转化反应机理.此外,将FeNCN负极与苝-3,4,9,10-四羧酸二酐正极材料匹配,组装成的全电池在198.6 Wkg^(-1)的功率密度下实现了184.7 W h kg^(-1)的超高能量密度,明显高于以往所有铁基负极的PIBs或钾离子混合电容器.展开更多
基金financially supported by the Fundamental Research Funds of the Central Universities(No.531118010112)the Double FirstClass University Initiative of Hunan University(No.531109100004)+1 种基金the Fundamental Research Funds of the Central Universities(No.531107051048)support from the Hunan Key Laboratory of TwoDimensional Materials(No.801200005)。
文摘Potassium-ion hybrid capacitors(KIHCs) have attracted increasing research interest because of the virtues of potassium-ion batteries and supercapacitors.The development of KIHCs is subject to the investigation of applicable K+storage materials which are able to accommodate the relatively large size and high activity of potassium.Here,we report a cocoon silk chemistry strategy to synthesize a hierarchically porous nitrogen-doped carbon(SHPNC).The as-prepared SHPNC with high surface area and rich N-doping not only offers highly efficient channels for the fast transport of electrons and K ions during cycling,but also provides sufficient void space to relieve volume expansion of electrode and improves its stability.Therefore,KIHCs with SHPNC anode and activated carbon cathode afford high energy of 135 Wh kg-1(calculated based on the total mass of anode and cathode),long lifespan,and ultrafast charge/slow discharge performance.This study defines that the KIHCs show great application prospect in the field of high-performance energy storage devices.
基金financially supported by the National Natural Science Foundation of China(52074113,22005091,and 22005092)the Hunan University Outstanding Youth Science Foundation(531118040319)+5 种基金the Science and Technology Innovation Program of Hunan Province(2021RC3055)the Changsha Municipal Natural Science Foundation(kq2014037)the CITIC Metals Ningbo Energy Co.Ltd.(H202191380246)the Chongqing Talents:Exceptional Young Talents Project(CQYC202105015)the Shenzhen Virtual University Park Basic Research Project of Free exploration(2021Szvup036)financially supported by the Graduate Research and Innovation Projects of Hunan Province(QL20210088)。
文摘Lithium metal has gained extensive attention as the most ideal candidate for next-generation battery anode owing to the ultrahigh specific capacity and the lowest electrochemical potential.However,uncontrollable dendrite growth and huge volume variation extremely restrict the future deployment of lithium metal batteries.Herein,we report metal chalcogenide SnSSe with unique nanoplate stacking structure as a robust substrate for stable Li metal anode.During the initial Li plating process,lithiophilic Li_(22)Sn_(5) alloy and Li_(2)S/Li_(2)Se sites are obtained via in-situ electrochemical reaction of Li metal and SnSSe.Density functional theory(DFT)calculation demonstrates that the formed Li_(2)S/Li_(2)Se achieves low Li diffusion energy barrier,ensuring rapid Li~+migration.Li_(22)Sn_(5) alloy provides strong nucleation sites,promoting uniform Li nucleation.Furthermore,in-situ optical microscopy analysis suggests that the synthesized effect fundamentally inhibits lithium dendrite growth.Consequently,SnSSe modified Cu foil delivered an ultralow nucleation overpotential,superior cycling stability with 450 cycles(Coulombic efficiency,>98%),and excellent plating/stripping behavior over 2200 h at 0.5 mA cm^(-2).Moreover,the brilliant reversible cycles and rate capability were also realized in Li@SnSSe//LiFePO_(4)(LFP)full cell,shedding light on the feasibility of SnSSe for stable and dendrite-free lithium metal anode.
基金supported by the National Natural Science Foundation of China(grant nos.52074113,22005091,and 22005092)the Hunan University Outstanding Youth Science Foundation(grant no.531118040319).
文摘High areal capacity is one of the critically important points for potassium-ion batteries(PIBs)for practical applications,which relies on high areal-massloading electrodes operating at high reversible capacity.However,it is remarkably restricted by the mechanical instability and sluggish charge transfer induced by the increased mass loading.To overcome such challenge,we report the rationally designed bimetallic selenides CoSe2/SnSe2 heterostructures confined in hierarchical carbon nanofibers(CSSe@CNFs),which enables the electrodes robust mechanical stability,enhanced electron transport,and reduced ion-diffusion energy barrier for facilitating reaction kinetics.Accordingly,an impressive areal mass loading up to 25.3 mg cm^(−2)was achieved,which endowed a high areal capacity of 7.58 mAh cm^(−2)for such a free-standing electrode.This is stateof-the-art among the PIBs,exceeding that of today’s industry standard(∼3 mAh cm^(−2)for LIBs).Furthermore,it delivered long-term stability over 3700 cycles at high current density(∼2 mA cm^(−2),vs 1 mA cm^(−2)in LIBs).Moreover,the as-constructed full battery achieved a high energy density of 172.8 Wh kg-1 at 0.05 A g^(−1)with a satisfied cycle stability over 2000 cycles at 2 A g^(−1)and high reversibility with Coulombic efficiency of 100%;thus,signifying its bright future toward commercial application for advanced PIBs.
基金the National Key R&D Program of China(2016YFC0801800)General Program of the National Natural Science Foundation of China(Grant No.61772353)+1 种基金the Key Program of the National Natural Science Foundation of China(Grant No.61332002)and Fok Ying Tung Education Foundation(151068).
文摘In speech recognition research,because of the variety of languages,corresponding speech recognition systems need to be constructed for different languages.Especially in a dialect speech recognition system,there are many special words and oral language features.In addition,dialect speech data is very scarce.Therefore,constructing a dialect speech recognition system is difficult.This paper constructs a speech recognition system for Sichuan dialect by combining a hidden Markov model(HMM)and a deep long short-term memory(LSTM)network.Using the HMM-LSTM architecture,we created a Sichuan dialect dataset and implemented a speech recognition system for this dataset.Compared with the deep neural network(DNN),the LSTM network can overcome the problem that the DNN only captures the context of a fixed number of information items.Moreover,to identify polyphone and special pronunciation vocabularies in Sichuan dialect accurately,we collect all the characters in the dataset and their common phoneme sequences to form a lexicon.Finally,this system yields a 11.34%character error rate on the Sichuan dialect evaluation dataset.As far as we know,it is the best performance for this corpus at present.
基金the National Natural Science Foundation of China(Nos.52074113 and 22005091)the Fundamental Research Funds of the Central Universities(No.531107051048)+2 种基金Xidong Duan acknowledges support by the National Natural Science Foundation of China(No.51872086)the Hunan Key Laboratory of Two-Dimensional Materials(No.2018TP1010)the Innovative Research Groups of Hunan Province(No.2020JJ1001)。
文摘Potassium-ion batteries(PIBs)are of academic and economic significance,but still limited by the lack of highly active electrode materials for de-/intercalation of large-radius K ions.Herein,an interconnected nitrogen/sulfur co-doped carbon nanosheep bundle(N/S-CSB)was proposed as the potassium ions storage material.The rich co-doping of nitrogen/sulfur of N/S-CNB with three-dimensional hierarchical bundled array structure yields distensible interlayer spaces to buffer the volume expansion during K+insertion/extraction,offers more electrochemical active sites to obtain a high specific capacity,and provides efficient channels for fast ion/electron transports.Therefore,the N/S-CSB anode achieved high reversible specific capacity of 365 mAh/g obtained at 50 mA/g after 200 cycles with a coulombic efficiency(CE)close to 100%,high rate performance and long cycle stability.Moreover,the in-situ Raman spectra indicated outstanding reaction kinetics of as-prepared N/S-CSB anode.
基金financially supported by the National Natural Science Foundation of China(52074113,22005091 and 22005092)Hunan University Outstanding Youth Science Foundation(531118040319)+4 种基金the Science and Technology Innovation Program of Hunan Province(2021RC3055)Changsha Municipal Natural Science Foundation(43184)the CITIC Metals Ningbo Energy Co.,Ltd.(H202191380246)Chongqing Talents:Exceptional Young Talents Project(CQYC202105015)Shenzhen Virtual University Park Basic Research Project of Free exploration(2021Szvup036)。
文摘钾离子电池(PIBs)面临的一个关键问题是设计具有先进结构的负极材料,以实现快速电荷传输以提高钾的存储性能.采用碳二亚胺铁(FeNCN)作为阳极,由于其含有一定数量的共价键且在分子水平上具有稳定的结构,使得储钾系统能够实现优异的电化学性能.FeNCN阳极具有高导电性,带隙接近0 eV,并且由于其共价键结构具有良好的结构稳定性.此外,无定形反应产物也为离子扩散提供了多种途径.因此,FeNCN阳极表现出高可逆比容量(在50 mA g^(-1)电流密度下具有600 mA h g^(-1)比容量),显著的倍率性能和长寿命循环(电流密度为500 mA g^(-1)时拥有400 mA h g^(-1)比容量且超过300次循环).通过理论模拟、X射线原位衍射分析和X射线光电子能谱分析揭示了Fe^(2+)和K^(+)之间的转化反应机理.此外,将FeNCN负极与苝-3,4,9,10-四羧酸二酐正极材料匹配,组装成的全电池在198.6 Wkg^(-1)的功率密度下实现了184.7 W h kg^(-1)的超高能量密度,明显高于以往所有铁基负极的PIBs或钾离子混合电容器.