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1.
首次报道了用355 nm脉冲激光沉积非晶态Ni-V2O5复合薄膜电极的电化学性能.采用不同摩尔比的NixV2O5 靶(x=0.1,0.3,0.5),在不同的基片温度(Ts)和O2气压力下制备了Ni-V2O5复合薄膜.XRD 和SEM测定表明, 在不锈钢基片上, Ts=300℃和氧气压力为14 Pa沉积0.5 h得到的是非晶态的Ni-V2O5薄膜.将此非晶态的Ni0.3V2O5薄膜电极用于锂电池的正极,与纯V2O5薄膜相比,不仅具有良好的放电速率性能和高的比容量,而且其充放电循环稳定性优异.该薄膜电极在放电速率为20 C时测得的比容量达200 mAh/g,并经1000次以上的充放电循环无明显的衰减.  相似文献   

2.
Layered mixed oxides LiNi(x)Co(y)Mn(1-x-y)O(2) (0 ≤x, y≤ 0.5) synthesized by a sol-gel method using tartaric acid as a chelating agent, and their structural and electrochemical properties are investigated by thermal analysis, XRD, SEM, FT-IR and XPS studies. The higher composition of Co leads to cation disorder and shrinks the cell volume. Electrochemical behaviour of the synthesized materials is evaluated by Galvanostatic charge/discharge studies using 2016 type coin cells. The cycling studies are carried out in the voltage limits of 2.7 to 4.6, 4.8 and 4.9 V at current rates of C/10 and C/5 respectively. The composition LiNi(0.4)Co(0.1)Mn(0.5)O(2) exhibits an average discharge capacity of 192 mA h g(-1) at the current density of 0.612 mA cm(-2) (C/5) in the voltage range of 2.7-4.9 V as compared to the discharge capacity of 155 and 175 mA h g(-1) in the potential range of 2.7-4.6 and 2.7-4.8 V over the 50 investigated cycles. The effect of higher charge voltage at 4.9 V on the electrochemical performance of LiNi(x)Co(y)Mn(1-x-y)O(2) oxide materials has not previously been reported.  相似文献   

3.
Laccase was earlier wired to yield an O2 electroreduction catalyst greatly outperforming platinum and its alloys. Here we describe the design, synthesis optimization of the composition, and characterization of the +0.55 V (AgAgCl) laccase-wiring redox hydrogel, with an apparent electron diffusion coefficient (D(app)) of 7.6 x 10(-7) cm2 s(-1). The high D(app) results in the tethering of redox centers to the polymer backbone through eight-atom-long spacer arms, which facilitate collisional electron transfer between proximal redox centers. The O2 flux-limited, true-area-based current density was increased from the earlier reported 560 to 860 microA cm(-2). When the O2 diffusion to the 7-microm-diameter carbon fiber cathode was cylindrical, half of the O2 flux-limited current was reached already at 0.62 V and 90% at 0.56 V vs Ag/AgCl, merely -0.08 and -0.14 V versus the 0.7 V (Ag/AgCl) reversible O2/H2O half-cell potential at pH 5.  相似文献   

4.
O2 was electroreduced to water, at a true-surface-area-based current density of 0.5 mA cm-2, at 37 degrees C and at pH 5 on a "wired" laccase bioelectrocatalyst-coated carbon fiber cathode. The polarization (potential vs the reversible potential of the O2 /H2O half-cell in the same electrolyte) of the cathode was only -0.07 V, approximately one-fifth of the -0.37 V polarization of a smooth platinum fiber cathode, operating in its optimal electrolyte, 0.5 M H2SO4. The bioelectrocatalyst was formed by "wiring" laccase to carbon through an electron conducting redox hydrogel, its redox functions tethered through long and flexible spacers to its cross-linked and hydrated polymer. Incorporation of the tethers increased the apparent electron diffusion coefficient 100-fold to (7.6 +/- 0.3) x 10-7 cm 2 s-1. A miniature single-compartment glucose-O2 biofuel cell made with the novel cathode operated optimally at 0.88 V, the highest operating voltage for a compartmentless miniature fuel cell.  相似文献   

5.
Muchattentionhasbeenpaidtothedevelopmentofnewpolymerelectrolytewithspecialmorphology,soastoimprovetheirelectrochemicalpropertiestomeettheneedsoflithium(ion)battery.Inthiswork,PEMlatexwassynthesizedbyemulsion-fi-eepolymerization.ThemicrophotoofPEMlate...  相似文献   

6.
In the present investigation, we report the transformation of alpha-LiVOPO 4 to alpha-Li 3V 2(PO 4) 3, leading to an enhancement of capacity. The alpha-LiVOPO 4 sample was synthesized by a sol-gel method, followed by sintering at 550-650 degrees C in a flow of 5% H 2/Ar. The structural transformation of a triclinic alpha-LiVOPO 4 structure to a monoclinic alpha-Li 3V 2(PO 4) 3 structure was observed at higher sintering temperatures (700-800 degrees C in a flow of 5% H 2/Ar). The alpha-Li 3V 2(PO 4) 3 phase was characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, thermal gravimetric analysis, and X-ray absorption near edge spectrum (XANES) techniques. The valence shift of vanadium ions from +4 to +3 states was observed using in situ XANES experiments at V K-edge. The structural transformation is ascertained by the shape changes in pre-edge and near edge area of X-ray absorption spectrum. It was observed that the capacity was enhanced from 140 mAh/g to 164 mAh/g via structural transformation process of LiVOPO 4 to Li 3V 2(PO 4) 3.  相似文献   

7.
T Uma  M Nogami 《Chemphyschem》2007,8(15):2227-2234
A new glass electrolyte formed by constant amounts of titanium oxide (TiO2) and various amount of phosphotungstic acid (PWA) doped P2O5-SiO2 is prepared using the sol-gel process. The structural formation is confirmed by Fourier infrared spectroscopy (FTIR) and from thermogravimetric and differential thermal analysis (TG/DTA) measurements, the glasses display good thermal stability. Further characterisation is undertaken by N2 adsorption/desorption measurements, proton conductivity and hydrogen permeability analyses and a H2/O2 fuel cell test is also performed. The glass materials with large pores and specific surface area are suitable for use as the electrolyte in H2/O2 fuel cells. The effect of TiO2 processing with constant amount of PWA in phosphosilicate glasses, is investigated and discussed. The hydrogen permeability is 1.57x10(-11) mol cm(-1) s(-1) Pa(-1) at 110 degrees C for 0.8 mm thick glass; a power density of 46.3 mW cm(-2) at 125 mA cm(-2) and a current density of 175 mA cm(-2) is obtained (T=28 degrees C, relative humidity).  相似文献   

8.
Using LiI as the reducing agent, the compound O2-Li(2/3)+x(Ni1/3Mn2/3)O2, x∼1/3 (O2(Li+x)) has been prepared from the O2-Li2/3(Ni1/3Mn2/3)O2 (O2(Li)). Cyclic voltammetry and voltage-capacity profiles of the O2(Li+x) phase are qualitatively different from that of O2(Li) phase. The first extraction capacity of O2(Li+x) at C/10 rate is 190 mAh/g corresponding to the removal of 2/3 mole of Li from the compound. At C/5 rate it delivers a reversible capacity of 158 mAh/g at 25 °C and 184 mAh/g at 50 °C (vs Li metal; voltage window 2.5–4.6 V). In Li-ion cells, with MCMB anode and O2(Li+x) as cathode, a discharge capacity of 140 mAh/g was obtained at C/5 rate in the voltage window 2.5–4.5 V (25 °C). The charge–discharge cycling performance and the cyclic voltammograms reveal that O2(Li) and O2(Li+x) do not convert to the spinel structure.  相似文献   

9.
以无模板生长法制备了泡沫镍载NiCo2O4纳米线正极材料, XRD和SEM表征结果表明, 所得材料为NiCo2O4纳米线, 以循环伏安法和计时电流法研究了泡沫镍载NiCo2O4纳米线对H2O2电还原的催化性能. 结果显示, 在0.4 mol/L H2O2 和 3.0 mol/L NaOH 溶液中, 当电压为-0.4 V(vs. Ag/AgCl)时, 循环伏安的电流密度达到125 mA/cm2; 当电压为-0.2, -0.3和 -0.4 V 时, 在30 min 的测试时间内, 计时电流密度几乎均为一常数, 表明以泡沫镍载NiCo2O4纳米线为催化剂电还原H2O2具有很高的活性和很好的稳定性.  相似文献   

10.
铜掺杂五氧化二钒的制备及电化学性质   总被引:1,自引:0,他引:1  
采用沉淀法于300 和600 ℃制备了结晶状的Cu0.04V2O5材料. 扫描电镜显示, 300 ℃时制备的样品具有多孔特征, 而600 ℃时制备的样品具有很高的结晶度. X射线研究表明, 少量铜掺杂不会改变V2O5的正交晶体结构. 红外光谱研究表明, 300 ℃时制备的Cu0.04V2O5样品含有少量水. 热失重分析确定了样品中所含水分是以吸附水的形式存在, 1 mol材料分子吸附水的摩尔数约为0.18 mol. 铜掺杂显著改善了V2O5的结构稳定性, 进而提高了材料的充放电循环性能. 于600 ℃制备的样品在C/5.6倍率下具有160 mAh·g-1的可逆比容量, 但提高放电倍率明显降低了材料的循环性能. 于300 ℃制备的样品在C/5.6倍率时的循环性能不如600 ℃样品, 但该材料在C/1.9倍率时仍具有100 mAh·g-1左右的可逆比容量. 两种材料在电化学性能上的差异与材料的微结构有关. 低温样品在较高放电倍率时良好的循环性能得益于其多孔的微结构, 而高温样品由于其较高的结晶度而表现出优异的低倍率充放电性能.  相似文献   

11.
Dinuclear (V(IV)V(V)) oxophenoxovanadates of general formula [V2O3L] have been synthesized in excellent yields by reacting bis(acetylacetonato)oxovanadium(IV) with H3L in a 2:1 ratio in acetone under an N2 atmosphere. Here L3- is the deprotonated form of 2,6-bis[{{(2-hydroxybenzyl)(N',N'-(dimethylamino)ethyl)}amino}methyl]-4-methylphenol (H3L1), 2,6-bis[{{(5-methyl-2-hydroxybenzyl)(N',N'-(dimethylamino)ethyl)}amino}methyl]-4-methylphenol (H3L2), 2,6-bis[{{(5-tert-butyl-2-hydroxybenzyl)(N',N'-(dimethylamino)ethyl)}amino}methyl]-4-methylphenol (H3L3), 2,6-bis[{{(5-chloro-2-hydroxybenzyl)(N',N'-(dimethylamino)ethyl)}amino}methyl]-4-methylphenol(H3L4), 2,6-bis[{{(5-bromo-2-hydroxybenzyl)(N'N'-(dimethylamino)ethyl)}amino}methyl]-4-methylphenol (H3L5), or 2,6-bis[{{(5-methoxy-2-hydroxybenzyl)(N'N'-(dimethylamino)ethyl)}methyl]-4-methylphenol (H3L6). In [V2O3L1], both the metal atoms have distorted octahedral geometry. The relative disposition of two terminal V=O groups in the complex is essentially cis. The O=V...V=O torsion angle is 24.6(2) degrees . The V-O(oxo)-V and V-O(phenoxo)-V angles are 117.5(4) and 93.4(3) degrees , respectively. The V...V bond distance is 3.173(5) A. X-ray crystallography, IR, UV-vis, and 1H and 51V NMR measurements show that the mixed-valence complexes contain two indistinguishable vanadium atoms (type III). The thermal ellipsoids of O2, O4, C10, C14, and C15 also suggests a type III complex in the solid state. EPR spectra of solid complexes at 77 K display a single line indicating the localization of the odd electron (3d(xy)1). Valence localization at 77 K is also consistent with the 51V hyperfine structure of the axial EPR spectra (3d(xy)1 ground state) of the complexes in frozen (77 K) dichloromethane solution: S = 1/2, g(parallel) approximately 1.94, g(perpendicular) approximately 1.98, A(parallel) approximately 166 x 10(-4) cm(-1), and A(perpendicular) approximately 68 x 10(-4) cm(-1). In contrast isotropic room-temperature solution spectra of the family have 15 hyperfine lines (g(iso) approximately 1.974 and A(iso) approximately 50 x 10(-4) cm(-1)) revealing that the unpaired electron is delocalized between the metal centers. Crystal data for the [V2O3L1].CH2Cl2 complex are as follows: chemical formula, C32H43O6N4Cl2V2; crystal system, monoclinic; space group, C2/c; a = 18.461(4), b = 17.230(3), c = 13.700(3) A; beta = 117.88(3) degrees ; Z = 8.  相似文献   

12.
以Li2CO3,NH4H2PO4,V2O5和MoO3为原料,柠檬酸为络合剂和碳源,采用溶胶凝胶法制备了锂离子正极材料Li3MoxV2-x(PO4)3/C (x = 0.01, 0.02和0.03). X射线衍射(XRD)表明,合成的材料具有单一的单斜晶系结构,空间群为P21/n. 扫描电镜(SEM)显示Li3Mo0.02V1.98(PO4)3/C具有均一的表面形貌。恒流充放电测试表明,当x = 0.02时,掺杂后的Li3Mo0.02V1.98(PO4)3具有最佳的电化学性能. 在1C倍率下,3.0 ~ 4.3 V电位区间,Li3Mo0.02V1.98(PO4)3/C的首次放电比容量达到122.3 mAh?g-1,循环50周之后,容量没有衰减的迹象;而当x = 0, 0.01和0.03时,首次放电比容量仅分别为117.1 mAh?g-1,115.1 mAh?g-1和116.0 mAh?g-1. 在3C和5C倍率下,样品Li3Mo0.02V1.98 (PO4)3/C仍能保持优异的循环稳定性.  相似文献   

13.
The adsorption of water on V2O3(0001) surfaces has been investigated by thermal desorption spectroscopy, high-resolution electron energy loss spectroscopy, and X-ray photoelectron spectroscopy with use of synchrotron radiation. The V2O3(0001) surfaces have been generated in epitaxial thin film form on a Rh(111) substrate with three different surface terminations according to the particular preparation conditions. The stable surface in thermodynamic equilibrium with the bulk is formed by a vanadyl (VO) (1x1) surface layer, but an oxygen-rich (radical3xradical3)R30 degrees reconstruction can be prepared under a higher chemical potential of oxygen (microO), whereas a V-terminated surface consisting of a vanadium surface layer requires a low microO, which can be achieved experimentally by the deposition of V atoms onto the (1x1) VO surface. The latter two surfaces have been used to model, in a controlled way, oxygen and vanadium containing defect centres on V2O3. On the (1x1) V=O and (radical3xradical3)R30 degrees surfaces, which expose only oxygen surface sites, the experimental results indicate consistently that the molecular adsorption of water provides the predominant adsorption channel. In contrast, on the V-terminated (1/radical3x1/radical3)R30 degrees surface the dissociation of water and the formation of surface hydroxyl species at 100 K is readily observed. Besides the dissociative adsorption a molecular adsorption channel exists also on the V-terminated V2O3(0001) surface, so that the water monolayer consists of both OH and molecular H2O species. The V surface layer on V2O3 is very reactive and is reoxidised by adsorbed water at 250 K, yielding surface vanadyl species. The results of this study indicate that V surface centres are necessary for the dissociation of water on V2O3 surfaces.  相似文献   

14.
Nanotube arrays of amorphous vanadium pentoxide (V(2)O(5)) were synthesized via template-based electrodeposition, and its electrochemical properties were investigated for Li-ion intercalation applications. The nanotubes have a length of 10 microm, outer diameter of 200 nm and inner diameter of 100 nm. Electrochemical analyses demonstrate that the V(2)O(5) nanotube array delivers a high initial capacity of 300 mAh/g, about twice that of the electrochemically prepared V(2)O(5) film. Although the V(2)O(5) nanotube array shows a more drastic degradation than the film under electrochemical redox cycles, the nanotube array reaches a stabilized capacity of 160 mAh/g, which remains about 1.3 times the stabilized capacity of the film.  相似文献   

15.
Kinetic and thermodynamic properties of the aminoxyl (NH2O*) radical   总被引:1,自引:0,他引:1  
The product of one-electron oxidation of (or H-atom abstraction from) hydroxylamine is the H2NO* radical. H2NO* is a weak acid and deprotonates to form HNO-*; the pKa(H2NO*) value is 12.6+/-0.3. Irrespective of the protonation state, the second-order recombination of the aminoxyl radical yields N2 as the sole nitrogen-containing product. The following rate constants were determined: kr(2H2NO*)=1.4x10(8) M-1 s-1, kr(H2NO*+HNO-*)=2.5x10(9) M-1 s-1, and kr(2HNO-*)=4.5x10(8) M-1 s-1. The HNO-* radical reacts with O2 in an electron-transfer reaction to yield nitroxyl (HNO) and superoxide (O2-*), with a rate constant of ke(HNO-*+O2-->HNO+O2-*)=2.2x10(8) M-1 s-1. Both O2 and O2-* seem to react with deprotonated hydroxylamine (H2NO-) to set up an autoxidative chain reaction. However, closer analysis indicates that these reactions might not occur directly but are probably mediated by transition-metal ions, even in the presence of chelators, such as ethylenediamine tetraacetic acid (EDTA) or diethylenetriamine pentaacetic acid (DTPA). The following standard aqueous reduction potentials were derived: E degrees (H2NO*,2H+/H3NOH+)=1.25+/-0.01 V; E degrees (H2NO*,H+/H2NOH)=0.90+/-0.01 V; and E degrees (H2NO*/H2NO-)=0.09+/-0.01 V. In addition, we estimate the following: E degrees (H2NOH+*/H2NOH)=1.3+/-0.1 V, E degrees (HNO, H+/H2NO*)=0.52+/-0.05 V, and E degrees (HNO/HNO-*)=-0.22+/-0.05 V. From the data, we also estimate the gaseous O-H and N-H bond dissociation enthalpy (BDE) values in H2NOH, with BDE(H2NO-H)=75-77 kcal/mol and BDE(H-NHOH)=81-82 kcal/mol. These values are in good agreement with quantum chemical computations.  相似文献   

16.
Sodium vanadium oxide gels, Na(x)V(2)O(5)·nH(2)O, of varying sodium content (0.12 < x < 0.32) were prepared by careful control of an ion exchange process. The water content (0.23 > n > 0.01) and interlayer spacing were found to be inversely proportional to the sodium level (x), thus control of sodium (x) content provided a direct, chimie douce approach for control of hydration level (n) and interlayer spacing, without the need for high temperature treatment to affect dehydration. Notably, the use of high temperatures to modify hydration levels can result in crystallization and collapse of the interlayer structure, highlighting the distinct advantage of our novel chimie douce synthesis strategy. Subsequent to synthesis and characterization, results from an electrochemical study of a series of Na(x)V(2)O(5)·nH(2)O samples highlight the significant impact of interlayer water on delivered capacity of the layered materials. Specifically, the sodium vanadium oxide gels with higher sodium content and lower water content provided higher capacities in lithium based cells, where capacity delivered to 2.0 V under C/20 discharge ranged from 170 mAh/g for Na(0.12)V(2)O(5)·0.23H(2)O to 300 mAh/g for Na(0.32)V(2)O(5)·0.01H(2)O. The capacity differences were maintained as the cells were cycled.  相似文献   

17.
以LiOH·H2O、Ni(CH3COO)2·4H2O 和 Co(CH3COO)2·4H2O为原料,在水-乙醇体系中,采用微粒溶胶凝胶方法(PSG)成功地制备了锂离子电池用正极材料LiNi0.85Co0.15O2。使用差热-热重(DTA-TG)方法来研究凝胶的热分解过程。粉末X-射线衍射(XRD)测试表明,在700 ℃、氧气氛中,原料混合物能形成具有较好α-NaFeO2层状结构的晶型化合物。扫描电镜(SEM)显示,与固相合成方法相比,PSG制备的LiNi0.85Co0.15O2颗粒较细、且颗粒大小分布均匀。充放电实验结果表明,PSG合成的LiNi0.85Co0.15O2首次放电容量为196.4 mAh/g, 10次循环之后,容量还有189.1 mAh/g (3.0~4.3V、18 mA/g),显示其具有良好的循环性能;而同样条件下,固相法合成的样品,首次放电容量为187.3 mAh/g,10次循环之后,容量衰减为167.1 mAh/g。  相似文献   

18.
Lithium nickel vanadate thin films were prepared by radio frequency magnetron sputtering at various substrate temperatures (Ts). These thin films have been investigated as anode electrode material in the use of microbatteries. Films were characterized by Rutherford backscattering spectroscopy, nuclear reaction analysis, Auger electron spectroscopy, glancing-incidence X-ray diffraction analysis, Raman spectroscopy, scanning electron microscopy, atomic force microscopy, and high-resolution transmission electron microscopy techniques. The anodic electrochemical performances of the films have been evaluated by cyclic voltammetry at a scan rate of 1 mV/s and by galvanostatic cycling, with lithium metal as the counter and the reference electrode, and cycled in the range of 0.02-3.0 V at a current density of 75 microA/cm2. Thin films prepared at a Ts of 650 degrees C show a discharge capacity at the 20th cycle of 1100 (+/-10) mAh/g, which exhibited excellent capacity retention with a small capacity fade.  相似文献   

19.
Zheng YQ  Lin JL  Kong ZP 《Inorganic chemistry》2004,43(8):2590-2596
Reactions of 4,4'-bipyridine (bpy) with Mn(C(4)H(4)O(4)).4H(2)O and Mn(C(5)H(6)O(4)).4H(2)O in methanolic aqueous solutions yielded [Mn(bpy)(H(2)O)(C(4)H(4)O(4))].0.5bpy (1) and Mn(bpy)(C(5)H(6)O(4)) (2), respectively, and reactions of freshly prepared Mn(OH)(2)(-)(2)(x)(CO(3))(x).yH(2)O, adipic acid and 4,4'-bipyridine in a methanolic aqueous solution afforded Mn(bpy)(C(6)H(8)O(4)) (3). The six-coordinate Mn atoms in 1 are interlinked by flexible succinato ligands to form layers, which are sustained by rigid bpy ligands into an 3D open framework with the free bpy molecules in tunnels. The ribbonlike chains in 2 result from Mn atoms bridged by glutarato ligands and are connected by bpy ligands into open layers. In 3, the Mn atoms are bridged by both bpy and adipato ligands to form 3D nanoporous frameworks and 2-fold interpenetration of the resulting 3D frameworks completes the crystal structure. In comparison with 1 and 2, compound 3 displays significant antiferromagnetic behavior at low temperature. The antiferromagnetic exchange becomes stronger from 1 through 2 to 3, and the antiferromagnetic ordering of Mn(2+) centers is related to the syn-syn bridging mode of the terminal carboxylate groups of alpha,omega-dicarboxylate anions. Crystal data: C(19)H(18)MnN(3)O(5) (1), monoclinic P2(1)/c, a= 11.686(2) A, b = 17.847(2) A, c = 8.852(1) A, beta = 99.67(1) degrees, V = 1819.9(4) A(3), Z = 4, D(c) = 1.545 g.cm(-3); C(15)H(14)MnN(2)O(4) (2), triclinic P, a = 8.145(2) A, b = 9.574(2) A, c = 10.180(1) A, alpha = 108.01(3) degrees, beta = 93.55(3) degrees, gamma = 105.30(1) degrees, V = 719.2(2) A(3), Z = 2, D(c) = 1.576 g.cm(-3); C(15)H(14)MnN(2)O(4) (3), triclinic P, a = 8.544(1) A, b= 8.881(1) A, c = 10.949(2) A, alpha = 108.81(1) degrees, beta = 95.40(1) degrees, gamma = 101.94(1) degrees, V = 757.7(2) A(3), Z = 2, D(c) = 1.557 g.cm(-3).  相似文献   

20.
We have prepared Ni-V(2)O(5).nH(2)O core-shell nanocable arrays for Li(+) intercalation applications. Ni-V(2)O(5).nH(2)O nanocables were prepared via formation of Ni nanorod arrays through the template based electrochemical deposition, followed by coating of V(2)O(5).nH(2)O on Ni nanorods through electrophoretic deposition. Transmission electron microscopy (TEM) micrograph clearly shows the Ni core was covered completely by a V(2)O(5).nH(2)O shell. Electrochemical analysis demonstrates that in a current density of 1.6 A/g, the Li(+) intercalation capacity of Ni-V(2)O(5).nH(2)O nanocable array is approximately 10 times higher than that of single-crystal V(2)O(5) nanorod array and 20 times higher than that of sol-gel-derived V(2)O(5) film. Both energy density and power density of such nanocable-array electrodes are higher than the V(2)O(5) film electrode by at least 1 order of magnitude. Such significant improvement in electrochemical performance is due to the large surface area and short diffusion path offered by the nanostructured V(2)O(5).nH(2)O.  相似文献   

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