The non-isothermal decomposition reaction of Nd[(C_5H_ 10NS_2)_3(C_ 12H_8N_2)] were carried out by means of TG-DTG and the thermal decomposition mechanism, and the associated kinetics was investigated. The kinetic par...The non-isothermal decomposition reaction of Nd[(C_5H_ 10NS_2)_3(C_ 12H_8N_2)] were carried out by means of TG-DTG and the thermal decomposition mechanism, and the associated kinetics was investigated. The kinetic parameters are obtained from an analysis of the TG-DTG curves at different heating rate by integral and differential methods. The most probable kinetic model function of the decomposition reaction is Maple Power of n=3/2, f(α)=2/3α -1/2 and the apparent activation energy E is 116.67 kJ·mol -1 and the pre-exponential factor lg[A/s -1] is 7.6891.展开更多
Exploring a novel strategy for large-scale production of battery-type Ni(OH)_(2)-based composites,with excellent capacitive performance,is still greatly challenging.Herein,we developed a facile and cost-effective stra...Exploring a novel strategy for large-scale production of battery-type Ni(OH)_(2)-based composites,with excellent capacitive performance,is still greatly challenging.Herein,we developed a facile and cost-effective strategy to in situ grow a layer of Ni(OH)_(2)/Ti_(3)C_(2)T_(x)composite on the nickel foam(NF)collector,where Ti_(3)C_(2)T_(x)is not only a conductive component,but also a catalyst that accelerates the oxidation of NF to Ni(OH)_(2).Detailed analysis reveals that the crystallinity,morphology,and electronic structure of the integrated electrode can be tuned via the electrochemical activation,which is beneficial for improving electrical conductivity and redox activity.As expected,the integrated electrode shows a specific capacity of 1.09 C cm^(-2)at 1 mA cm^(-2)after three custom activation cycles and maintains 92.4%of the initial capacity after 1500 cycles.Moreover,a hybrid supercapacitor composed of Ni(OH)_(2)/Ti_(3)C_(2)T_(x)/NF cathode and activated carbon anode provides an energy density of 0.1 mWh cm^(-2)at a power density of 0.97 mW cm^(-2),and excellent cycling stability with about 110%capacity retention rate after 5000 cycles.This work would afford an economical and convenient method to steer commercial Ni foam into advanced Ni(OH)_(2)-based composite materials as binder-free electrodes for hybrid supercapacitors.展开更多
The rising flexible and intelligent electronics greatly facilitate the noninvasive and timely tracking of physiological information in telemedicine healthcare.Meticulously building bionic-sensitive moieties is vital f...The rising flexible and intelligent electronics greatly facilitate the noninvasive and timely tracking of physiological information in telemedicine healthcare.Meticulously building bionic-sensitive moieties is vital for designing efficient electronic skin with advanced cognitive functionalities to pluralistically capture external stimuli.However,realistic mimesis,both in the skin’s three-dimensional interlocked hierarchical structures and synchronous encoding multistimuli information capacities,remains a challenging yet vital need for simplifying the design of flexible logic circuits.Herein,we construct an artificial epidermal device by in situ growing Cu_(3)(HHTP)_(2) particles onto the hollow spherical Ti_(3)C_(2)T_(x) surface,aiming to concurrently emulate the spinous and granular layers of the skin’s epidermis.The bionic Ti_(3)C_(2)T_(x)@Cu_(3)(HHTP)_(2) exhibits independent NO_(2) and pressure response,as well as novel functionalities such as acoustic signature perception and Morse code-encrypted message communication.Ultimately,a wearable alarming system with a mobile application terminal is self-developed by integrating the bimodular senor into flexible printed circuits.This system can assess risk factors related with asthmatic,such as stimulation of external NO_(2) gas,abnormal expiratory behavior and exertion degrees of fingers,achieving a recognition accuracy of 97.6%as assisted by a machine learning algorithm.Our work provides a feasible routine to develop intelligent multifunctional healthcare equipment for burgeoning transformative telemedicine diagnosis.展开更多
(C_(6)H_(14)N_(2))[Na(ClO_(4))_(3)]是新型含能钙钛矿化合物的典型代表,需明确其热分解行为、热分解机制及感度特性,以推动其在配方中的应用。以差示扫描量热-热重分析方法实现了分解放热量、分解温度等参数的获取;以动力学模拟计算...(C_(6)H_(14)N_(2))[Na(ClO_(4))_(3)]是新型含能钙钛矿化合物的典型代表,需明确其热分解行为、热分解机制及感度特性,以推动其在配方中的应用。以差示扫描量热-热重分析方法实现了分解放热量、分解温度等参数的获取;以动力学模拟计算解析了相关分解机理;以同步热分析-红外-质谱联用技术结合原位红外技术探索了(C_(6)H_(14)N_(2))[Na(ClO_(4))_(3)]的分解产物及分解历程;以国军标法获得了热感度、摩擦感度与撞击感度参数。结果表明:在10℃·min^(-1)的升温速率下,(C_(6)H_(14)N_(2))[Na(ClO_(4))_(3)]分解放热量为4227 J·g^(-1),分解温度则达到345℃,高于黑索今(RDX)、奥克托今(HMX)、六硝基六氮杂异伍兹烷(CL-20)等多数现役含能材料,显示了优异的热稳定性;分解产物研究表明其立方笼状骨架有效稳定了内部结合的有机物分子,使其热稳定性较高。此外,(C_(6)H_(14)N_(2))[Na(ClO_(4))_(3)]在100℃下加热48 h的放气量约0.04 m L·g^(-1),撞击感度与机械感度分别为32%和80%,优于RDX和HMX。展开更多
Structural properties of the organic-inorganic hybrid(C_(2)H_(5)NH_(3))_(2)CuCl_(4) have been investigated by means of x-ray powder diffraction and Rietveld analysis. A structural phase transition from Pbca to Aba2 oc...Structural properties of the organic-inorganic hybrid(C_(2)H_(5)NH_(3))_(2)CuCl_(4) have been investigated by means of x-ray powder diffraction and Rietveld analysis. A structural phase transition from Pbca to Aba2 occurs at T_(4)= 240 K, which results in a paraelectric–ferroelectric phase transition. The release of the Jahn–Teller distortion with increasing temperature toward T_(4) is revealed by the structural analysis.展开更多
Rationally manipulating surface reconstruction of catalysts for water oxidation,inducing formation and dynamic accumulation of catalytically active centers still face numerous challenges.Herein,the introduction of[Cr(...Rationally manipulating surface reconstruction of catalysts for water oxidation,inducing formation and dynamic accumulation of catalytically active centers still face numerous challenges.Herein,the introduction of[Cr(C_(2)O_(4))_(3)]^(3-)into NiFe LDHs by intercalation engineering to promote surface reconstruction achieves an advanced oxygen evolution reaction(OER)activity.In view of the weak electronegativity of Cr^(3+) in[Cr(C_(2)O_(4))_(3)]^(3-),the intercalation of[Cr(C_(2)O_(4))_(3)]^(3-)is expected to result in an electron-rich structure of Fe sites in NiFe LDHs,and higher valence state of Ni can be formed with the charge transfer between Fe and Ni.The optimized electronic structure of NiFe-[Cr(C_(2)O_(4))_(3)]^(3-)-LDHs with more active Ni^(3+) species and the expedited dynamic generation of Ni^(3+) (Fe)OOH phase during the OER process contributed to its excellent catalytic property,revealed by in situ X-ray absorption spectroscopy,Raman spectroscopy,and quasi-in situ X-ray photoelectron spectroscopy.With the modulated electronic structure of metal sites,NiFe-[Cr(C_(2)O_(4))_(3)]^(3-)-LDHs exhibited promoted OER property with a lower overpotential of 236 mV at the current density of 10 mA cm^(-2).This work illustrates the intercalation of conjugated anion to dynamically construct desired Ni^(3+) sites with the optimal electronic environment for improved OER electrocatalysis.展开更多
P-xylene(p-C_(8)H_(10))is extremely harmful and dangerous to human health due to high toxicity and strong carcinogenicity.Exploring sensitive material to effectively detect p-xylene is of importance.In this paper,pero...P-xylene(p-C_(8)H_(10))is extremely harmful and dangerous to human health due to high toxicity and strong carcinogenicity.Exploring sensitive material to effectively detect p-xylene is of importance.In this paper,perovskite single crystal(C_(4)H_(9)NH_(3))_(2)PbI_(4) has been successfully synthesized via solution method.The obtained product was analyzed by single crystal X-ray diffraction.With the space group Pbca,orthorhombic(C_(4)H_(9)NH_(3))_(2)PbI_(4) layered perovskite structure consists of an extended two-dimensional network of corner-sharing PbI_(6) octahedron.Single layer perovskite sheets of distorted PbI_(6) octahedron alternated with protonated n-butylammonium cation bilayers,which offers many advantages and provides the possibility of forming a gas sensor device based on the change of resistances.Density functional theory(DFT)simulations regarding the adsorption energy revealed that this organicinorganic hybrid perovskite compound has excellent selectivity toward p-xylene compared with other gases including C_(2)H_(5)OH,C_(6)H_(6),CH_(2)Cl_(2),HCHO,CH_(3)COCH_(3) and C_(7)H_(8).The calculation of electron density,density of states and electron density difference showed the sensing mechanism of p-C_(8)H_(10) is mainly derived from physical adsorption-desorption in view of electron transfer.展开更多
KTi_(2)(PO_(4))_(3)is a promising anode material for potassium storage,but suffers from low conductivity and difficult balance between high capacity and good structural stability.Herein,the Ti_(3)C_(2)T_(x)MXene is us...KTi_(2)(PO_(4))_(3)is a promising anode material for potassium storage,but suffers from low conductivity and difficult balance between high capacity and good structural stability.Herein,the Ti_(3)C_(2)T_(x)MXene is used as a multifunctional binder to fabricate the KTi_(2)(PO_(4))_(3)electrode by the traditional homogenizing-coating method.The MXene nanosheets,together with the conductive agent super P nanoparticles,construct a multiple conductive network for fast electron/ion transfer and high electrochemical kinet-ics.Moreover,the network ensures the structural stability of the KTi_(2)(PO_(4))_(3)electrode during the de-intercalation/intercalation of 4 K^(+)ions,which is beneficial for simultaneously achieving high capacity and good cycle performance.Therefore,the MXene-bonded KTi_(2)(PO_(4))_(3)electrode delivers a reversible capacity of 255.2 mAh/g at 50 mA/g,outstanding rate capability with 132.3 mAh/g at 2 A/g,and ex-cellent cycle performance with 151.6 mAh/g at 1 A/g after 2000 cycles.This work not only suggests a high-performance anode material for potassium-ion batteries,but also demonstrates that the MXene is a promising binder material for constructing conductive electrodes in rechargeable batteries.展开更多
文摘The non-isothermal decomposition reaction of Nd[(C_5H_ 10NS_2)_3(C_ 12H_8N_2)] were carried out by means of TG-DTG and the thermal decomposition mechanism, and the associated kinetics was investigated. The kinetic parameters are obtained from an analysis of the TG-DTG curves at different heating rate by integral and differential methods. The most probable kinetic model function of the decomposition reaction is Maple Power of n=3/2, f(α)=2/3α -1/2 and the apparent activation energy E is 116.67 kJ·mol -1 and the pre-exponential factor lg[A/s -1] is 7.6891.
基金supported by the NSF of China(Nos.21971143,21805165,22209098)the 111 Project(D20015)+1 种基金the major research and development project of Hubei Three Gorges Laboratory(2022-3)the Natural Science Foundation of Hubei Province(2022CFB326)
文摘Exploring a novel strategy for large-scale production of battery-type Ni(OH)_(2)-based composites,with excellent capacitive performance,is still greatly challenging.Herein,we developed a facile and cost-effective strategy to in situ grow a layer of Ni(OH)_(2)/Ti_(3)C_(2)T_(x)composite on the nickel foam(NF)collector,where Ti_(3)C_(2)T_(x)is not only a conductive component,but also a catalyst that accelerates the oxidation of NF to Ni(OH)_(2).Detailed analysis reveals that the crystallinity,morphology,and electronic structure of the integrated electrode can be tuned via the electrochemical activation,which is beneficial for improving electrical conductivity and redox activity.As expected,the integrated electrode shows a specific capacity of 1.09 C cm^(-2)at 1 mA cm^(-2)after three custom activation cycles and maintains 92.4%of the initial capacity after 1500 cycles.Moreover,a hybrid supercapacitor composed of Ni(OH)_(2)/Ti_(3)C_(2)T_(x)/NF cathode and activated carbon anode provides an energy density of 0.1 mWh cm^(-2)at a power density of 0.97 mW cm^(-2),and excellent cycling stability with about 110%capacity retention rate after 5000 cycles.This work would afford an economical and convenient method to steer commercial Ni foam into advanced Ni(OH)_(2)-based composite materials as binder-free electrodes for hybrid supercapacitors.
基金supported by the National Natural Science Foundation of China(Grant Nos.U22A20184,52250077,and 52272080)the Jilin Province Natural Science Foundation of China(No.20220201093GX)+2 种基金the Fundamental Research Funds for the Central Universitiessupported by the National Research Foundation of Korea(2018R1A3B1052702 to JSK)the Starting growth Technological R&D Program(TIPS Program,No.S3201803,2021,MW)funded by the Ministry of SMEs and Startups(MSS,Korea).
文摘The rising flexible and intelligent electronics greatly facilitate the noninvasive and timely tracking of physiological information in telemedicine healthcare.Meticulously building bionic-sensitive moieties is vital for designing efficient electronic skin with advanced cognitive functionalities to pluralistically capture external stimuli.However,realistic mimesis,both in the skin’s three-dimensional interlocked hierarchical structures and synchronous encoding multistimuli information capacities,remains a challenging yet vital need for simplifying the design of flexible logic circuits.Herein,we construct an artificial epidermal device by in situ growing Cu_(3)(HHTP)_(2) particles onto the hollow spherical Ti_(3)C_(2)T_(x) surface,aiming to concurrently emulate the spinous and granular layers of the skin’s epidermis.The bionic Ti_(3)C_(2)T_(x)@Cu_(3)(HHTP)_(2) exhibits independent NO_(2) and pressure response,as well as novel functionalities such as acoustic signature perception and Morse code-encrypted message communication.Ultimately,a wearable alarming system with a mobile application terminal is self-developed by integrating the bimodular senor into flexible printed circuits.This system can assess risk factors related with asthmatic,such as stimulation of external NO_(2) gas,abnormal expiratory behavior and exertion degrees of fingers,achieving a recognition accuracy of 97.6%as assisted by a machine learning algorithm.Our work provides a feasible routine to develop intelligent multifunctional healthcare equipment for burgeoning transformative telemedicine diagnosis.
文摘(C_(6)H_(14)N_(2))[Na(ClO_(4))_(3)]是新型含能钙钛矿化合物的典型代表,需明确其热分解行为、热分解机制及感度特性,以推动其在配方中的应用。以差示扫描量热-热重分析方法实现了分解放热量、分解温度等参数的获取;以动力学模拟计算解析了相关分解机理;以同步热分析-红外-质谱联用技术结合原位红外技术探索了(C_(6)H_(14)N_(2))[Na(ClO_(4))_(3)]的分解产物及分解历程;以国军标法获得了热感度、摩擦感度与撞击感度参数。结果表明:在10℃·min^(-1)的升温速率下,(C_(6)H_(14)N_(2))[Na(ClO_(4))_(3)]分解放热量为4227 J·g^(-1),分解温度则达到345℃,高于黑索今(RDX)、奥克托今(HMX)、六硝基六氮杂异伍兹烷(CL-20)等多数现役含能材料,显示了优异的热稳定性;分解产物研究表明其立方笼状骨架有效稳定了内部结合的有机物分子,使其热稳定性较高。此外,(C_(6)H_(14)N_(2))[Na(ClO_(4))_(3)]在100℃下加热48 h的放气量约0.04 m L·g^(-1),撞击感度与机械感度分别为32%和80%,优于RDX和HMX。
基金supported by the National Natural Science Foundation of China (Grant No. 51925605)Fujian Institute of Innovation,Chinese Academy of Sciences(Grant No. FJCXY18040303)the Youth Innovation Promotion of the Chinese Academy of Sciences (Grant No. 2013004)。
文摘Structural properties of the organic-inorganic hybrid(C_(2)H_(5)NH_(3))_(2)CuCl_(4) have been investigated by means of x-ray powder diffraction and Rietveld analysis. A structural phase transition from Pbca to Aba2 occurs at T_(4)= 240 K, which results in a paraelectric–ferroelectric phase transition. The release of the Jahn–Teller distortion with increasing temperature toward T_(4) is revealed by the structural analysis.
基金support from the National Natural Science Foundation of China(51402100,21905088,21573066 and U19A2017)the Provincial Natural Science Foundation of Hunan(2020JJ5044,2022JJ10006)。
文摘Rationally manipulating surface reconstruction of catalysts for water oxidation,inducing formation and dynamic accumulation of catalytically active centers still face numerous challenges.Herein,the introduction of[Cr(C_(2)O_(4))_(3)]^(3-)into NiFe LDHs by intercalation engineering to promote surface reconstruction achieves an advanced oxygen evolution reaction(OER)activity.In view of the weak electronegativity of Cr^(3+) in[Cr(C_(2)O_(4))_(3)]^(3-),the intercalation of[Cr(C_(2)O_(4))_(3)]^(3-)is expected to result in an electron-rich structure of Fe sites in NiFe LDHs,and higher valence state of Ni can be formed with the charge transfer between Fe and Ni.The optimized electronic structure of NiFe-[Cr(C_(2)O_(4))_(3)]^(3-)-LDHs with more active Ni^(3+) species and the expedited dynamic generation of Ni^(3+) (Fe)OOH phase during the OER process contributed to its excellent catalytic property,revealed by in situ X-ray absorption spectroscopy,Raman spectroscopy,and quasi-in situ X-ray photoelectron spectroscopy.With the modulated electronic structure of metal sites,NiFe-[Cr(C_(2)O_(4))_(3)]^(3-)-LDHs exhibited promoted OER property with a lower overpotential of 236 mV at the current density of 10 mA cm^(-2).This work illustrates the intercalation of conjugated anion to dynamically construct desired Ni^(3+) sites with the optimal electronic environment for improved OER electrocatalysis.
基金financially supported by the Natural Science Foundation of Hebei(Nos.F2020202027 and F2020202067)the Major National Science and Technology Special Projects(No.2016ZX02301003-004-007)+1 种基金the National Natural Science Foundation of China(No.21271139)the Natural Science Foundation of Tianjin(No.17JCTPJC54500)。
文摘P-xylene(p-C_(8)H_(10))is extremely harmful and dangerous to human health due to high toxicity and strong carcinogenicity.Exploring sensitive material to effectively detect p-xylene is of importance.In this paper,perovskite single crystal(C_(4)H_(9)NH_(3))_(2)PbI_(4) has been successfully synthesized via solution method.The obtained product was analyzed by single crystal X-ray diffraction.With the space group Pbca,orthorhombic(C_(4)H_(9)NH_(3))_(2)PbI_(4) layered perovskite structure consists of an extended two-dimensional network of corner-sharing PbI_(6) octahedron.Single layer perovskite sheets of distorted PbI_(6) octahedron alternated with protonated n-butylammonium cation bilayers,which offers many advantages and provides the possibility of forming a gas sensor device based on the change of resistances.Density functional theory(DFT)simulations regarding the adsorption energy revealed that this organicinorganic hybrid perovskite compound has excellent selectivity toward p-xylene compared with other gases including C_(2)H_(5)OH,C_(6)H_(6),CH_(2)Cl_(2),HCHO,CH_(3)COCH_(3) and C_(7)H_(8).The calculation of electron density,density of states and electron density difference showed the sensing mechanism of p-C_(8)H_(10) is mainly derived from physical adsorption-desorption in view of electron transfer.
基金support by National Natural Science Foundation of China(No.U2004212).
文摘KTi_(2)(PO_(4))_(3)is a promising anode material for potassium storage,but suffers from low conductivity and difficult balance between high capacity and good structural stability.Herein,the Ti_(3)C_(2)T_(x)MXene is used as a multifunctional binder to fabricate the KTi_(2)(PO_(4))_(3)electrode by the traditional homogenizing-coating method.The MXene nanosheets,together with the conductive agent super P nanoparticles,construct a multiple conductive network for fast electron/ion transfer and high electrochemical kinet-ics.Moreover,the network ensures the structural stability of the KTi_(2)(PO_(4))_(3)electrode during the de-intercalation/intercalation of 4 K^(+)ions,which is beneficial for simultaneously achieving high capacity and good cycle performance.Therefore,the MXene-bonded KTi_(2)(PO_(4))_(3)electrode delivers a reversible capacity of 255.2 mAh/g at 50 mA/g,outstanding rate capability with 132.3 mAh/g at 2 A/g,and ex-cellent cycle performance with 151.6 mAh/g at 1 A/g after 2000 cycles.This work not only suggests a high-performance anode material for potassium-ion batteries,but also demonstrates that the MXene is a promising binder material for constructing conductive electrodes in rechargeable batteries.
