Electric double-layer capacitors(EDLCs)with fast frequency response are regarded as small-scale alternatives to the commercial bulky aluminum electrolytic capacitors.Creating carbon-based nanoarray electrodes with pre...Electric double-layer capacitors(EDLCs)with fast frequency response are regarded as small-scale alternatives to the commercial bulky aluminum electrolytic capacitors.Creating carbon-based nanoarray electrodes with precise alignment and smooth ion channels is crucial for enhancing EDLCs’performance.However,controlling the density of macropore-dominated nanoarray electrodes poses challenges in boosting the capacitance of line-filtering EDLCs.Herein,a simple technique to finely adjust the vertical-pore diameter and inter-spacing in three-dimensional nanoporous anodic aluminum oxide(3D-AAO)template is achieved,and 3D compactly arranged carbon tube(3D-CACT)nanoarrays are created as electrodes for symmetrical EDLCs using nanoporous 3D-AAO template-assisted chemical vapor deposition of carbon.The 3D-CACT electrodes demonstrate a high surface area of 253.0 m^(2) g^(−1),a D/G band intensity ratio of 0.94,and a C/O atomic ratio of 8.As a result,the high-density 3D-CT nanoarray-based sandwich-type EDLCs demonstrate a record high specific areal capacitance of 3.23 mF cm^(-2) at 120 Hz and exceptional fast frequency response due to the vertically aligned and highly ordered nanoarray of closely packed CT units.The 3D-CT nanoarray electrode-based EDLCs could serve as line filters in integrated circuits,aiding power system miniaturization.展开更多
Transition metal oxides are regarded as promising candidates of anode for next-generation lithium-ion batteries(LIBs)due to their ultrahigh theoretical capacity and low cost,but are restricted by their low conductivit...Transition metal oxides are regarded as promising candidates of anode for next-generation lithium-ion batteries(LIBs)due to their ultrahigh theoretical capacity and low cost,but are restricted by their low conductivity and large volume expansion during Li^(+)intercalation.Herein,we designed and constructed a structurally integrated 3D carbon tube(3D-CT)grid film with Mn_(3)O_(4)nanoparticles(Mn_(3)O_(4)-NPs)and carbon nanotubes(CNTs)filled in the inner cavity of CTs(denoted as Mn_(3)O_(4)-NPs/CNTs@3D-CT)as high-performance free-standing anode for LIBs.The Mn_(3)O_(4)-NPs/CNTs@3D-CT grid with Mn_(3)O_(4)-NPs filled in the inner cavity of 3D-CT not only afford sufficient space to overcome the damage caused by the volume expansion of Mn_(3)O_(4)-NPs during charge and discharge processes,but also achieves highly efficient channels for the fast transport of both electrons and Li+during cycling,thus offering outstanding electrochemical performance(865 mAh g^(-1)at 1 A g^(-1)after 300 cycles)and excellent rate capability(418 mAh g^(-1)at 4 A g^(-1))based on the total mass of electrode.The unique 3D-CT framework structure would open up a new route to the highly stable,high-capacity,and excellent cycle and high-rate performance free-standing electrodes for highperformance Li-ion storage.展开更多
二氧化锡(SnO_(2))具有高的理论比容量,有望作为下一代锂离子电池负极材料.然而,Sn向SnO_(2)的不可逆转化以及充放电过程中巨大的体积变化限制了其实际的应用.本文基于三维互连多孔氧化铝模板,设计合成了一种由内腔同时填充NiO和SnO_(2...二氧化锡(SnO_(2))具有高的理论比容量,有望作为下一代锂离子电池负极材料.然而,Sn向SnO_(2)的不可逆转化以及充放电过程中巨大的体积变化限制了其实际的应用.本文基于三维互连多孔氧化铝模板,设计合成了一种由内腔同时填充NiO和SnO_(2)纳米颗粒的碳管基元相互连接组成的三维碳管网格膜,可以直接作为自支撑的高性能锂离子电池负极.该复合框架利用了NiO和SnO_(2)纳米颗粒的协同作用,不仅能够促进Sn向SnO_(2)的可逆转变,提高首次库伦效率,而且还可以缓释充放电过程中SnO_(2)剧烈的体积变化.此外,相互连接的三维碳管框架可以负载大量NiO和SnO_(2)纳米颗粒,缩短Li+的扩散距离,并作为快速的电子传输通道.因此,这种独特的结构赋予了该电极超高的储锂容量和倍率性能在1 A g^(-1)循环200次后,比容量达到928.5 mA h g^(-1),并且在4 A g^(-1)的高电流密度下仍然具有633.5 mA h g^(-1)的比容量.总之,这种独特的一体化结构在锂离子电池等储能领域具有广阔的应用前景.展开更多
The rational design of electrodes is the key to achieving ultrahigh-power performance in electrochemical energy storage devices.Recently,we have constructed well-organized and integrated three-dimensional(3D)carbon tu...The rational design of electrodes is the key to achieving ultrahigh-power performance in electrochemical energy storage devices.Recently,we have constructed well-organized and integrated three-dimensional(3D)carbon tube(CT)grids(3D-CTGs)using a 3D porous anodic aluminum oxide template-assisted method as electrodes of electrical double-layer capacitors(EDLCs),showing excellent frequency response performance.The unique design warrants fast ion migration channels,excellent electronic conductivity,and good structural stability.This study achieved one of the highest carbon-based ultrahigh-power EDLCs with the 3D-CTG electrodes,resulting in ultrahigh power of 437 and 1708 W·cm−3 with aqueous and organic electrolytes,respectively.Capacitors constructed with these electrodes would have important application prospects in the ultrahigh-power output.The rational design and fabrication of the 3D-CTGs electrodes have demonstrated their capability to build capacitors with ultrahighpower performance and open up new possibilities for applications requiring high-power output.展开更多
Surface-enhanced Raman spectroscopy (SERS) is a fast analytical technique for trace chemicals; however, it requires the active SERS-substrates to adsorb analytes, thus limiting target species to those with the desir...Surface-enhanced Raman spectroscopy (SERS) is a fast analytical technique for trace chemicals; however, it requires the active SERS-substrates to adsorb analytes, thus limiting target species to those with the desired affinity for substrates. Here we present networked polyacrylic acid sodium salt (PAAS) film entrapped Ag-nanocubes (denoted as Ag-nanocubes@PAAS) as an effective SERS-substrate for analytes with and without high affinity. Once the analyte aqueous solution is cast on the dry Ag-nanocubes@PAAS substrate, the bibulous PAAS becomes swollen forcing the Ag-nanocubes loose, while the analytes diffuse in the interstices among the Ag-nanocubes. When dried, the PAAS shrinks and pulls the Ag-nanocubes back to their previous aggregated state, while the PAAS network "detains" the analytes in the small gaps between the Ag-nanocubes for SERS detection. The strategy has been proven effective for not only single- analytes but also multi-analytes without strong affinity for Ag, showing its potential in SERS-based simultaneous multi-analyte detection of both adsorbable and non-adsorbable pollutants in the environment.展开更多
By treating information transmission as tiling over the time-frequency plane, we propose a digital signal transmission scheme employing overcomplete frames as modulation pulses. The new scheme can achieve a signaling ...By treating information transmission as tiling over the time-frequency plane, we propose a digital signal transmission scheme employing overcomplete frames as modulation pulses. The new scheme can achieve a signaling rate larger than the Nyquist rate. We first analyze the capacity performance of the frame transmission scheme over additive white Gaussian noise (AWGN) channels, k proves that the proposed scheme can achieve the Shannon capacity asymptotically. Next, we design the Gabor frame system parameters in time-frequency dispersive channels. It is shown that the pulses shape and the time-frequency separation should be matched to the channel dispersion parameters to achieve the minimum energy perturbation. Numerical results are presented to verify the theoretical findings.展开更多
基金supported by the National Natural Science Foundation of China(91963202,52072372,52372241,52232007,12325203)HFIPS Director’s Fund(BJPY2023A07,YZJJ-GGZX-2022-01).
文摘Electric double-layer capacitors(EDLCs)with fast frequency response are regarded as small-scale alternatives to the commercial bulky aluminum electrolytic capacitors.Creating carbon-based nanoarray electrodes with precise alignment and smooth ion channels is crucial for enhancing EDLCs’performance.However,controlling the density of macropore-dominated nanoarray electrodes poses challenges in boosting the capacitance of line-filtering EDLCs.Herein,a simple technique to finely adjust the vertical-pore diameter and inter-spacing in three-dimensional nanoporous anodic aluminum oxide(3D-AAO)template is achieved,and 3D compactly arranged carbon tube(3D-CACT)nanoarrays are created as electrodes for symmetrical EDLCs using nanoporous 3D-AAO template-assisted chemical vapor deposition of carbon.The 3D-CACT electrodes demonstrate a high surface area of 253.0 m^(2) g^(−1),a D/G band intensity ratio of 0.94,and a C/O atomic ratio of 8.As a result,the high-density 3D-CT nanoarray-based sandwich-type EDLCs demonstrate a record high specific areal capacitance of 3.23 mF cm^(-2) at 120 Hz and exceptional fast frequency response due to the vertically aligned and highly ordered nanoarray of closely packed CT units.The 3D-CT nanoarray electrode-based EDLCs could serve as line filters in integrated circuits,aiding power system miniaturization.
基金supported by the Natural Science Foundation of China(91963202 and 52072372)the Key Research Program of Frontier Sciences(CAS,Grant,QYZDJ-SSW-SLH046)the CAS/SAFEA International Partnership Program for Creative Research Teams,and the Hefei Institutes of Physical Science,Chinese Academy of Sciences Director’s Fund(YZJ ZX202018)
文摘Transition metal oxides are regarded as promising candidates of anode for next-generation lithium-ion batteries(LIBs)due to their ultrahigh theoretical capacity and low cost,but are restricted by their low conductivity and large volume expansion during Li^(+)intercalation.Herein,we designed and constructed a structurally integrated 3D carbon tube(3D-CT)grid film with Mn_(3)O_(4)nanoparticles(Mn_(3)O_(4)-NPs)and carbon nanotubes(CNTs)filled in the inner cavity of CTs(denoted as Mn_(3)O_(4)-NPs/CNTs@3D-CT)as high-performance free-standing anode for LIBs.The Mn_(3)O_(4)-NPs/CNTs@3D-CT grid with Mn_(3)O_(4)-NPs filled in the inner cavity of 3D-CT not only afford sufficient space to overcome the damage caused by the volume expansion of Mn_(3)O_(4)-NPs during charge and discharge processes,but also achieves highly efficient channels for the fast transport of both electrons and Li+during cycling,thus offering outstanding electrochemical performance(865 mAh g^(-1)at 1 A g^(-1)after 300 cycles)and excellent rate capability(418 mAh g^(-1)at 4 A g^(-1))based on the total mass of electrode.The unique 3D-CT framework structure would open up a new route to the highly stable,high-capacity,and excellent cycle and high-rate performance free-standing electrodes for highperformance Li-ion storage.
基金supported by the National Natural Science Foundation of China (91963202 and 52072372)the Key Research Program of Frontier Sciences (CAS, QYZDJ-SSW-SLH046)+1 种基金the CAS/SAFEA International Partnership Program for Creative Research TeamsHefei Institutes of Physical Science, Chinese Academy of Sciences Director’s Fund (YZJJZX202018)。
文摘二氧化锡(SnO_(2))具有高的理论比容量,有望作为下一代锂离子电池负极材料.然而,Sn向SnO_(2)的不可逆转化以及充放电过程中巨大的体积变化限制了其实际的应用.本文基于三维互连多孔氧化铝模板,设计合成了一种由内腔同时填充NiO和SnO_(2)纳米颗粒的碳管基元相互连接组成的三维碳管网格膜,可以直接作为自支撑的高性能锂离子电池负极.该复合框架利用了NiO和SnO_(2)纳米颗粒的协同作用,不仅能够促进Sn向SnO_(2)的可逆转变,提高首次库伦效率,而且还可以缓释充放电过程中SnO_(2)剧烈的体积变化.此外,相互连接的三维碳管框架可以负载大量NiO和SnO_(2)纳米颗粒,缩短Li+的扩散距离,并作为快速的电子传输通道.因此,这种独特的结构赋予了该电极超高的储锂容量和倍率性能在1 A g^(-1)循环200次后,比容量达到928.5 mA h g^(-1),并且在4 A g^(-1)的高电流密度下仍然具有633.5 mA h g^(-1)的比容量.总之,这种独特的一体化结构在锂离子电池等储能领域具有广阔的应用前景.
基金supported by the National Natural Science Foundation of China(Nos.91963202,52072372,and 52232007).
文摘The rational design of electrodes is the key to achieving ultrahigh-power performance in electrochemical energy storage devices.Recently,we have constructed well-organized and integrated three-dimensional(3D)carbon tube(CT)grids(3D-CTGs)using a 3D porous anodic aluminum oxide template-assisted method as electrodes of electrical double-layer capacitors(EDLCs),showing excellent frequency response performance.The unique design warrants fast ion migration channels,excellent electronic conductivity,and good structural stability.This study achieved one of the highest carbon-based ultrahigh-power EDLCs with the 3D-CTG electrodes,resulting in ultrahigh power of 437 and 1708 W·cm−3 with aqueous and organic electrolytes,respectively.Capacitors constructed with these electrodes would have important application prospects in the ultrahigh-power output.The rational design and fabrication of the 3D-CTGs electrodes have demonstrated their capability to build capacitors with ultrahighpower performance and open up new possibilities for applications requiring high-power output.
文摘Surface-enhanced Raman spectroscopy (SERS) is a fast analytical technique for trace chemicals; however, it requires the active SERS-substrates to adsorb analytes, thus limiting target species to those with the desired affinity for substrates. Here we present networked polyacrylic acid sodium salt (PAAS) film entrapped Ag-nanocubes (denoted as Ag-nanocubes@PAAS) as an effective SERS-substrate for analytes with and without high affinity. Once the analyte aqueous solution is cast on the dry Ag-nanocubes@PAAS substrate, the bibulous PAAS becomes swollen forcing the Ag-nanocubes loose, while the analytes diffuse in the interstices among the Ag-nanocubes. When dried, the PAAS shrinks and pulls the Ag-nanocubes back to their previous aggregated state, while the PAAS network "detains" the analytes in the small gaps between the Ag-nanocubes for SERS detection. The strategy has been proven effective for not only single- analytes but also multi-analytes without strong affinity for Ag, showing its potential in SERS-based simultaneous multi-analyte detection of both adsorbable and non-adsorbable pollutants in the environment.
文摘By treating information transmission as tiling over the time-frequency plane, we propose a digital signal transmission scheme employing overcomplete frames as modulation pulses. The new scheme can achieve a signaling rate larger than the Nyquist rate. We first analyze the capacity performance of the frame transmission scheme over additive white Gaussian noise (AWGN) channels, k proves that the proposed scheme can achieve the Shannon capacity asymptotically. Next, we design the Gabor frame system parameters in time-frequency dispersive channels. It is shown that the pulses shape and the time-frequency separation should be matched to the channel dispersion parameters to achieve the minimum energy perturbation. Numerical results are presented to verify the theoretical findings.