电解水技术是一种生产高纯氢燃料的方法,能够增强可再生能源发电系统的消纳能力.相较于质子交换膜(PEM)电解槽,碱性(ALK)电解槽可以使用非贵金属基催化电极,拥有更高的经济效益和市场占有率.然而,由于ALK电解槽处于质子稀缺环境,阴极氢...电解水技术是一种生产高纯氢燃料的方法,能够增强可再生能源发电系统的消纳能力.相较于质子交换膜(PEM)电解槽,碱性(ALK)电解槽可以使用非贵金属基催化电极,拥有更高的经济效益和市场占有率.然而,由于ALK电解槽处于质子稀缺环境,阴极氢气演化反应(HER)动力学变得更加复杂,需要快速解离水分子提供动态质子微环境.硫化钼(MoS_(2))纳米片边缘具有合适的质子吸附和演化的活性位点,是制备HER催化剂的潜力材料.但其二维基面原子由于配位饱和,显示出较弱的质子吸附能力.如何调控MoS_(2)基面以实现水解动力与质子吸附演化动力的集成,提升MoS_(2)纳米片的碱性HER活性,具有重要的科学和应用意义.本文提出了一种Co/O双原子植入策略,精准调控双活性位点及其电子结构,实现了水解离动力和质子吸附演化动力的高效耦联.首先,利用刻蚀和电沉积的两步实验法,在MoS_(2)基面上成功引入O和Co原子;随后,结合高分辨透射电镜、高角环形暗场-扫描透射电子显微镜、同步辐射X射线吸收精细结构谱等表征分析技术,精准识别了掺杂Co/O原子的位置和配位情况:O原子替换部分S原子,Co原子占据Mo原子的上方,构建出立体凸起的“O-Co-S_(2)”配位构型.催化在线的原位表征分析结果表明:该独特的“O-Co-S_(2)”原子基序发挥着水解离与氢演化反应协同催化效应.密度泛函理论计算结果也证实了该协同机制,其中Co位点促进水的解离反应,而S位点则有助于质子的转化生成氢气.因此,Co/O掺杂MoS_(2)催化剂(Co-O@MoS_(2))表现出较好的碱性HER活性:仅需81 mV的过电位,即可达到100 mA cm^(‒2)的电流密度,Tafel斜率低至42 mV dec^(‒1),在600 mA cm^(‒2)的高电流密度测试中运行300 h活性无衰减.上述碱性HER性能不仅远高于原始的MoS_(2)纳米片,而且也领先于部分已报道结果.综上所述,本文在MoS_(2)基面上构筑了原子级协同催化活性中心,显著促进了碱性HER反应性能,为原子活化工程开发先进催化剂提供参考,在原子级基序构造、表征和功能分析方面提供借鉴.展开更多
Enabling lithium-ion batteries(LIBs)to operate in a wider temperature range,e.g.,as low or high as possible or capable of both,is an urgent need and shared goal.Here we report,for the first time,a low-temperature elec...Enabling lithium-ion batteries(LIBs)to operate in a wider temperature range,e.g.,as low or high as possible or capable of both,is an urgent need and shared goal.Here we report,for the first time,a low-temperature electrolyte consisting of traditional ethylene carbonate,methyl acetate,butyronitrile solvents,and 1 M LiPF_(6) salt,attributed to its very low freezing point(T_(f)=-126.3℃)and high ion conductivity at extremely low temperatures(0.21 m S/cm at-100℃),successfully extends the service temperature of a practical 9.6 Ah LIB down to-100℃(49.6%capacity retention compared to that at room temperature),which is the lowest temperature reported for practical cells so far as we know,and is lower than the lowest natural temperature(-89.2℃)recorded on earth.Meanwhile,the high-temperature performance of lithium-ion batteries is not affected.The capacity retention is 88.2%and 83.4%after 800 cycles at 25℃and 45℃,respectively.The progress also makes LIB a proper power supplier for space vehicles in astronautic explorations.展开更多
We report a single-frequency linearly polarized Q-switched fiber laser based on an Nb_(2)GeTe_(4)saturable absorber(SA).The Nb_(2)GeTe_(4)SA triggers passive Q-switching of the laser,and an un-pumped Yb-doped fiber to...We report a single-frequency linearly polarized Q-switched fiber laser based on an Nb_(2)GeTe_(4)saturable absorber(SA).The Nb_(2)GeTe_(4)SA triggers passive Q-switching of the laser,and an un-pumped Yb-doped fiber together with a 0.08-nmbandwidth polarization-maintaining fiber Bragg grating(FBG)acts as an ultra-narrow bandwidth filter to realize singlelongitudinal-mode(SLM)oscillation.The devices used in the laser are all kept polarized,so as to ensure linearly polarized laser output.Stable SLM linearly polarized Q-switching operation at 1064.6 nm is successfully achieved,producing a laser with a shortest pulse width of 1.36μs,a linewidth of 28.4 MHz,a repetition rate of 28.3 kHz-95.9 kHz,and a polarization extinction ratio of about 30 dB.It is believed that the single-frequency linearly polarized pulsed fiber laser studied in this paper has great application value in gravitational wave detection,beam combining,nonlinear frequency conversion,and other fields.展开更多
The charge carrier concentration profile is a critical factor that determines semiconducting material properties and device performance.Dielectric force microscopy(DFM)has been previously developed to map charge carri...The charge carrier concentration profile is a critical factor that determines semiconducting material properties and device performance.Dielectric force microscopy(DFM)has been previously developed to map charge carrier concentrations with nanometer-scale spatial resolution.However,it is challenging to quantitatively obtain the charge carrier concentration,since the dielectric force is also affected by the mobility.Here,we quantitative measured the charge carrier concentration at the saturation mobility regime via the rectification effect-dependent gating ratio of DFM.By measuring a series of n-type GaAs and GaN thin films with mobility in the saturation regime,we confirmed the decreased DFM-measured gating ratio with increasing electron concentration.Combined with numerical simulation to calibrate the tip–sample geometry-induced systematic error,the quantitative correlation between the DFM-measured gating ratio and the electron concentration has been established,where the extracted electron concentration presents high accuracy in the range of 4×10^(16)–1×10^(18)cm^(-3).We expect the quantitative DFM to find broad applications in characterizing the charge carrier transport properties of various semiconducting materials and devices.展开更多
As metallic nanoparticles are arranged to form a 2D periodic nano-array,the coupling of the localized surface plasmonic resonance(LSPR)results in the well-known phenomenon of surface lattice resonances(SLRs).We theore...As metallic nanoparticles are arranged to form a 2D periodic nano-array,the coupling of the localized surface plasmonic resonance(LSPR)results in the well-known phenomenon of surface lattice resonances(SLRs).We theoretically investigate the SLR effect of the circular nano-array fabricated on the fiber tips.The difference between the 2D periodic and circular periodic arrays results in different resonant characteristics.For both structures,the resonant peaks due to the SLRs shift continuously as the array structures are adjusted.For some specific arrangements,the circular nano-array may generate a single sharp resonant peak with extremely high enhancement,which originates from the collective coupling of the whole array.More interestingly,the spatial pattern of the vector near-field corresponding to the sharp peak is independent of the polarization state of the incidence,facilitating its excitation and regulation.This finding may be helpful for designing multifunctional all-fiber devices.展开更多
金属锂负极由于比容量高(3860 mAh·g^(-1))及氧化还原电位极低(-3.04 V vs.标准氢气电极(SHE)),被认为是实现高能量密度锂电池的理想负极。然而,金属锂电极与电解液反应剧烈,且锂离子在电极表面沉积不均匀容易产生枝晶,导致其循环...金属锂负极由于比容量高(3860 mAh·g^(-1))及氧化还原电位极低(-3.04 V vs.标准氢气电极(SHE)),被认为是实现高能量密度锂电池的理想负极。然而,金属锂电极与电解液反应剧烈,且锂离子在电极表面沉积不均匀容易产生枝晶,导致其循环稳定性和安全性都较差,限制了其应用推广。我们前期通过构建金属锂-碳纳米管(Li-CNT)复合结构,极大的提高了金属锂的比表面积,降低了电极电流密度,从而有效地抑制了锂枝晶的生长,提高了金属锂电极的循环稳定性和安全性能。本工作在前期工作基础上,采用简单的液相反应,利用4-氟苯乙烯(FPS)对Li-CNT进行表面修饰并进行原位聚合,得到了表面富含氟化锂(Li F)保护层的Li-CNT(FPS-Li-CNT)。该表面修饰层能够有效抑制电解液和空气对Li-CNT的侵蚀,显著的提高了LiCNT电极的界面稳定性。FPS-Li-CNT与磷酸铁锂正极(LFP)组成的LFP||FPS-Li-CNT全电池,在正负极容量配比为1:6条件下,能够稳定循环280圈,库伦效率达到97.7%。展开更多
文摘电解水技术是一种生产高纯氢燃料的方法,能够增强可再生能源发电系统的消纳能力.相较于质子交换膜(PEM)电解槽,碱性(ALK)电解槽可以使用非贵金属基催化电极,拥有更高的经济效益和市场占有率.然而,由于ALK电解槽处于质子稀缺环境,阴极氢气演化反应(HER)动力学变得更加复杂,需要快速解离水分子提供动态质子微环境.硫化钼(MoS_(2))纳米片边缘具有合适的质子吸附和演化的活性位点,是制备HER催化剂的潜力材料.但其二维基面原子由于配位饱和,显示出较弱的质子吸附能力.如何调控MoS_(2)基面以实现水解动力与质子吸附演化动力的集成,提升MoS_(2)纳米片的碱性HER活性,具有重要的科学和应用意义.本文提出了一种Co/O双原子植入策略,精准调控双活性位点及其电子结构,实现了水解离动力和质子吸附演化动力的高效耦联.首先,利用刻蚀和电沉积的两步实验法,在MoS_(2)基面上成功引入O和Co原子;随后,结合高分辨透射电镜、高角环形暗场-扫描透射电子显微镜、同步辐射X射线吸收精细结构谱等表征分析技术,精准识别了掺杂Co/O原子的位置和配位情况:O原子替换部分S原子,Co原子占据Mo原子的上方,构建出立体凸起的“O-Co-S_(2)”配位构型.催化在线的原位表征分析结果表明:该独特的“O-Co-S_(2)”原子基序发挥着水解离与氢演化反应协同催化效应.密度泛函理论计算结果也证实了该协同机制,其中Co位点促进水的解离反应,而S位点则有助于质子的转化生成氢气.因此,Co/O掺杂MoS_(2)催化剂(Co-O@MoS_(2))表现出较好的碱性HER活性:仅需81 mV的过电位,即可达到100 mA cm^(‒2)的电流密度,Tafel斜率低至42 mV dec^(‒1),在600 mA cm^(‒2)的高电流密度测试中运行300 h活性无衰减.上述碱性HER性能不仅远高于原始的MoS_(2)纳米片,而且也领先于部分已报道结果.综上所述,本文在MoS_(2)基面上构筑了原子级协同催化活性中心,显著促进了碱性HER反应性能,为原子活化工程开发先进催化剂提供参考,在原子级基序构造、表征和功能分析方面提供借鉴.
基金supported by the National Key Research and Development Program of China(Grant No.2022YFE0207300)Key Program of the National Natural Science Foundation of China(Grant No.U1964205)Talent of Mass Entrepreneurship and Innovation in Jiangsu Province(2020)。
文摘Enabling lithium-ion batteries(LIBs)to operate in a wider temperature range,e.g.,as low or high as possible or capable of both,is an urgent need and shared goal.Here we report,for the first time,a low-temperature electrolyte consisting of traditional ethylene carbonate,methyl acetate,butyronitrile solvents,and 1 M LiPF_(6) salt,attributed to its very low freezing point(T_(f)=-126.3℃)and high ion conductivity at extremely low temperatures(0.21 m S/cm at-100℃),successfully extends the service temperature of a practical 9.6 Ah LIB down to-100℃(49.6%capacity retention compared to that at room temperature),which is the lowest temperature reported for practical cells so far as we know,and is lower than the lowest natural temperature(-89.2℃)recorded on earth.Meanwhile,the high-temperature performance of lithium-ion batteries is not affected.The capacity retention is 88.2%and 83.4%after 800 cycles at 25℃and 45℃,respectively.The progress also makes LIB a proper power supplier for space vehicles in astronautic explorations.
基金Project supported by the National Natural Science Foundation of China(Grant No.62275272)the Training Program for Excellent Young Innovators of Changsha,China(Grant No.KQ2206003).
文摘We report a single-frequency linearly polarized Q-switched fiber laser based on an Nb_(2)GeTe_(4)saturable absorber(SA).The Nb_(2)GeTe_(4)SA triggers passive Q-switching of the laser,and an un-pumped Yb-doped fiber together with a 0.08-nmbandwidth polarization-maintaining fiber Bragg grating(FBG)acts as an ultra-narrow bandwidth filter to realize singlelongitudinal-mode(SLM)oscillation.The devices used in the laser are all kept polarized,so as to ensure linearly polarized laser output.Stable SLM linearly polarized Q-switching operation at 1064.6 nm is successfully achieved,producing a laser with a shortest pulse width of 1.36μs,a linewidth of 28.4 MHz,a repetition rate of 28.3 kHz-95.9 kHz,and a polarization extinction ratio of about 30 dB.It is believed that the single-frequency linearly polarized pulsed fiber laser studied in this paper has great application value in gravitational wave detection,beam combining,nonlinear frequency conversion,and other fields.
基金Project supported by the National Key R&D Program of China (Grant No. 2021YFA1202802)the National Natural Science Foundation of China (Grant Nos. 21875280,21991150, 21991153, and 22022205)+1 种基金the CAS Project for Young Scientists in Basic Research (Grant No. YSBR-054)the Special Foundation for Carbon Peak Neutralization Technology Innovation Program of Jiangsu Province,China(Grant No. BE2022026)
文摘The charge carrier concentration profile is a critical factor that determines semiconducting material properties and device performance.Dielectric force microscopy(DFM)has been previously developed to map charge carrier concentrations with nanometer-scale spatial resolution.However,it is challenging to quantitatively obtain the charge carrier concentration,since the dielectric force is also affected by the mobility.Here,we quantitative measured the charge carrier concentration at the saturation mobility regime via the rectification effect-dependent gating ratio of DFM.By measuring a series of n-type GaAs and GaN thin films with mobility in the saturation regime,we confirmed the decreased DFM-measured gating ratio with increasing electron concentration.Combined with numerical simulation to calibrate the tip–sample geometry-induced systematic error,the quantitative correlation between the DFM-measured gating ratio and the electron concentration has been established,where the extracted electron concentration presents high accuracy in the range of 4×10^(16)–1×10^(18)cm^(-3).We expect the quantitative DFM to find broad applications in characterizing the charge carrier transport properties of various semiconducting materials and devices.
基金supported by the National Natural Science Foundation of China (Grant No.12174085)the Fundamental Research Funds for the Central Universities (Grant No.B220202018)+1 种基金the Changzhou Science and Technology Program (Grant No.CJ20210130)CAS Key Laboratory of Nanodevices and Applications (Grant No.21YZ03)。
文摘As metallic nanoparticles are arranged to form a 2D periodic nano-array,the coupling of the localized surface plasmonic resonance(LSPR)results in the well-known phenomenon of surface lattice resonances(SLRs).We theoretically investigate the SLR effect of the circular nano-array fabricated on the fiber tips.The difference between the 2D periodic and circular periodic arrays results in different resonant characteristics.For both structures,the resonant peaks due to the SLRs shift continuously as the array structures are adjusted.For some specific arrangements,the circular nano-array may generate a single sharp resonant peak with extremely high enhancement,which originates from the collective coupling of the whole array.More interestingly,the spatial pattern of the vector near-field corresponding to the sharp peak is independent of the polarization state of the incidence,facilitating its excitation and regulation.This finding may be helpful for designing multifunctional all-fiber devices.
文摘金属锂负极由于比容量高(3860 mAh·g^(-1))及氧化还原电位极低(-3.04 V vs.标准氢气电极(SHE)),被认为是实现高能量密度锂电池的理想负极。然而,金属锂电极与电解液反应剧烈,且锂离子在电极表面沉积不均匀容易产生枝晶,导致其循环稳定性和安全性都较差,限制了其应用推广。我们前期通过构建金属锂-碳纳米管(Li-CNT)复合结构,极大的提高了金属锂的比表面积,降低了电极电流密度,从而有效地抑制了锂枝晶的生长,提高了金属锂电极的循环稳定性和安全性能。本工作在前期工作基础上,采用简单的液相反应,利用4-氟苯乙烯(FPS)对Li-CNT进行表面修饰并进行原位聚合,得到了表面富含氟化锂(Li F)保护层的Li-CNT(FPS-Li-CNT)。该表面修饰层能够有效抑制电解液和空气对Li-CNT的侵蚀,显著的提高了LiCNT电极的界面稳定性。FPS-Li-CNT与磷酸铁锂正极(LFP)组成的LFP||FPS-Li-CNT全电池,在正负极容量配比为1:6条件下,能够稳定循环280圈,库伦效率达到97.7%。
基金The project was supported by the National Natural Science Foundation of China(21625304,21733012,21773290)the “Strategic Priority Research Program” of CAS(XDA09010600)the Ministry of Science and Technology of China(2016YFA0200703)~~
基金supported by the National Natural Science Foundation of China(21625304,21733012,and 21772190)the Ministry of Science and Technology of China(2016YFB0100102)。
