A novel type of composite electrode based on nmltiwalled carbon nanotubes coated with sheet-like cobalt hydroxide particles was used in supercapacitors. Cobalt hydroxide cathodlcally deposited fiom Co(NO3)O2 solutio...A novel type of composite electrode based on nmltiwalled carbon nanotubes coated with sheet-like cobalt hydroxide particles was used in supercapacitors. Cobalt hydroxide cathodlcally deposited fiom Co(NO3)O2 solution with carbon nanotubes as matrix exhibited large pseudo-capacitance of 322 F/g in 1 mol/L KOH. To characterize the cobalt hydroxide nanocomposite electrode, a charge-discharge cycling test, cyclic voltammetry, and an impedance test were done. This cobalt hydroxide composite exhibiting excellent pseudo-capacitive behavior (i.c. high reversibility, high specific capacitance, low impedance), was demonstrated to be a candidate for the application of electrochemical supercapacitors. A combined capacitor consisting of cobalt hydroxide composite as a cathode and activated carbon fiber as an anode was reported. The electrochemical pcrformance of the combined capacitor was characterized by cyclic voltammetry and a dc charge/discharge test. The combined capacitor showed ideal capacitor behavior with an extended operating voltage of 1.4 V. According to the extended operating voltage, the energy density of the combined capacitor at a current density of 100 mA/cm^2 was found to be 11 Wh/kg. The combined capacitor exhibited high-energy density and stable power characteristics,展开更多
Taking the nano-sized carbon black and aniline monomer as precursor and (NH4)2S2O6 as oxidant, the well coated C/polyaniline(C/PANI) composite materials were prepared by in situ polymerization of the aniline on th...Taking the nano-sized carbon black and aniline monomer as precursor and (NH4)2S2O6 as oxidant, the well coated C/polyaniline(C/PANI) composite materials were prepared by in situ polymerization of the aniline on the surface of well-dispersed nano-sized carbon black for supercapacitor. The micro-structure of the C/PANI composite electrode materials were analyzed by SEM. The electrochemical properties of C/ PANI and PANI composite electrode were characterized by means of the galvanostatic charge-discharge experiment, cyclic voltammetric measurement and impedance spectroscopy analysis. The results show that by adding the nano-sized carbon black in the process of chemical polymerization of the aniline, the polyaniline can be in situ polymerized and well-coated onto the carbon black particles, which may effectively improve the aggregation of particles and the electrolyte penetration. What’s more , the maximum of specific capacitance of C/PANI electrode 437.6F·g -1 can be attained. Compared with PANI electrode, C/PANI electrode shows more desired capacitance characteristics, smaller internal resistance and better cycle performance.展开更多
Efficient and affordable electrocatalysts for reversible oxygen reduction and oxygen evolution reactions(ORR and OER,respectively)are highly sought-after for use in rechargeable metal-air batteries.However,the constru...Efficient and affordable electrocatalysts for reversible oxygen reduction and oxygen evolution reactions(ORR and OER,respectively)are highly sought-after for use in rechargeable metal-air batteries.However,the construction of high-performance electrocatalysts that possess both largely accessible active sites and superior ORR/OER intrinsic activities is challenging.Herein,we report the design and successful preparation of a 3D hierarchically porous graphene framework with interconnected interlayer macropores and in-plane mesopores,enriched with pyridinic-nitrogen-cobalt(pyri-N-Co)active sites,namely,CoFe/3D-NLG.The pyri-N-Co bonding significantly accelerates sluggish oxygen electrocatalysis kinetics,in turn substantially improving the intrinsic ORR/OER activities per active site,while copious interlayer macropores and in-plane mesopores enable ultra-efficient mass transfer throughout the graphene architecture,thus ensuring sufficient exposure of accessible pyri-N-Co active sites to the reagents.Such a robust catalyst structure endows CoFe/3D-NLG with a remarkably enhanced reversible oxygen electrocatalysis performance,with the ORR half-wave potential identical to that of the benchmark Pt/C catalyst,and OER activity far surpassing that of the noble-metal-based RuO2 catalyst.Moreover,when employed as an air electrode for a rechargeable Zn-air battery,CoFe/3D-NLG manifests an exceedingly high open-circuit voltage(1.56 V),high peak power density(213 mW cm^(–2)),ultra-low charge/discharge voltage(0.63 V),and excellent charge/discharge cycling stability,outperforming state-of-the-art noble-metal electrocatalysts.展开更多
This work presents NiS/graphene/carbon nanotube (NiS/GNS/CNT) composites as electrode material for the supercapacitor application in sea flashing signal systems. NiS nanosheets were closely anchored on the conductiv...This work presents NiS/graphene/carbon nanotube (NiS/GNS/CNT) composites as electrode material for the supercapacitor application in sea flashing signal systems. NiS nanosheets were closely anchored on the conductive GNS-CNT networks. As a result, the NiS/GNS/CNT electrode showed a high specific capacitance of 2 377 F.g^-1 at 2 mV.s^-1 and good cycling stability compared with the pure NiS (1 599F.g^-1). The enhanced electrochemical performances are attributed to the synergetic effect between the conductive carbon and the pseudo-capacitive NiS. The high performance supercapacitor may provide application in the sea flashing signal system.展开更多
Nano sized powders of TiO2 (titanium dioxide) and Nb2O5 (Niobium (V) oxide) were used to fabricate TiO2/Nb2O5 composites thin films by EPD (electrophoretic deposition) technique. The metal oxide powders, toget...Nano sized powders of TiO2 (titanium dioxide) and Nb2O5 (Niobium (V) oxide) were used to fabricate TiO2/Nb2O5 composites thin films by EPD (electrophoretic deposition) technique. The metal oxide powders, together with magnesium nitrate hexahydrate pellets, were suspended in propan-2-ol inside an EPD cell. The electrodes, placed 1.2 cm apart, were partially immersed in the suspension and a DC potential applied across them. Key EPD process parameters, which include applied DC electric field, deposition time and solid concentration in suspension, were optimized through visual inspection and from UV-Vis-NIR spectrophotometer spectra. The highest (55%) transmittance was obtained for films with deposition time of 90 s, powder concentration of 0.01 g/40 mL, and 35 V DC (direct current) voltage. XRD micrographs confirmed that TiO2 and Nb2O5 particles were presented in the composite film. SEM (scanning electron microscope) micrographs of the composite electrode thin films showed that porous films of high quality with well controlled morphology were deposited by using the EPD technique.展开更多
Graphene-based three-dimensional (3D) macroscopic materials have recently attracted increasing interest by virtue of their exciting potential in electrochemical energy conversion and storage. Here we report a facile...Graphene-based three-dimensional (3D) macroscopic materials have recently attracted increasing interest by virtue of their exciting potential in electrochemical energy conversion and storage. Here we report a facile one-step strategy to prepare mechanically strong and electrically conductive graphene/Ni(OH)2 composite hydrogels with an interconnected porous network. The composite hydrogels were directly used as 3D supercapacitor electrode materials without adding any other binder or conductive additives. An optimized composite hydrogel containing -82 wt.% Ni(OH)2 exhibited a specific capacitance of -1,247 F/g at a scan rate of 5 mV/s and -785 F/g at 40 mV/s (-63% capacitance retention) with excellent cycling stability. The capacity of the 3D hydrogels greatly surpasses that of a physical mixture of graphene sheets and Ni(OH)2 nanoplates (-309 F/g at 40 mV/s). The same strategy was also applied to fabricate graphene-carbon nanotube/Ni(OH)2 ternary composite hydrogels with further improved specific capacitances (-1,352 F/g at 5 mV/s) and rate capability (-66% capacitance retention at 40 mV/s). Both composite hydrogels obtained here can deliver high energy densities (-43 and -47 Wh/kg, respectively) and power densities (-8 and -9 kW/kg, respectively), making them attractive electrode materials for supercapacitor applications. This study opens a new pathway to the design and fabrication of functional 3D graphene composite materials, and can significantly impact broad areas including energy storage and beyond.展开更多
Nanostructured Mn3O4 was introduced to activated C (AC) by a novel sonochemical reaction, and the resulting nanocomposites were examined as supercapacitor electrodes. The sonication not only catalyzed the redox reac...Nanostructured Mn3O4 was introduced to activated C (AC) by a novel sonochemical reaction, and the resulting nanocomposites were examined as supercapacitor electrodes. The sonication not only catalyzed the redox reaction but also promoted the diffusion of the precursors, causing the formation of coherent nanocomposites with Mn3O4 nanoparticles grown and uniformly distributed inside the mesopores of the AC. In addition, the extreme local condition in the sonochemical synthesis yielded an excessive amount of divalent manganese ions and oxygen vacancies. This novel microstructure endowed the sample with a superior performance, including a specific capacitance of 150 F/g compared with the value of 93 F/g for AC at a charge/discharge rate of 100 mA/g. A Li-ion capacitor delivered an energy density of 68 Wh/kg, compared with 41 Wh/kg for the AC capacitor at a power density of 210 W/kg.展开更多
Flexible supercapacitors (SCs) are attractive energy storage devices for wearable electronics, but their applications are hindered by their low volumetric energy densities. Two dimensional (2D) non-carbon nanomaterial...Flexible supercapacitors (SCs) are attractive energy storage devices for wearable electronics, but their applications are hindered by their low volumetric energy densities. Two dimensional (2D) non-carbon nanomaterials are the most promising pseudocapacitive materials for high volumetric capacitance electrodes. However, they are poorly conductive and prone to self-stacking, which results in unsatisfactory electrochemical performance. In this work, large-scale V2O5·nH2O ultrathin nanosheets are synthesized by a facile and scalable method and transformed into layered and compact composite films with one-dimensional carbon nanotubes (CNTs). The self-standing films show an optimized volumetric capacitance of 521.0Fcm^-3 with only 10 wt% of CNTs, which is attributed to dramatically enhanced electrical conductivity beyond the electrical percolation threshold, high dispersion of pseudocapacitive V2O5·nH2O nanosheets, and high mass density of the films. All-solid-state flexible SCs made of V2O5·nH2O/CNTs films show a maximum energy density of 17.4WhL^-1.展开更多
Micro-supercapacitors(MSCs) have emerged as one competitive candidate of high-performance, flexible, safe,portable and wearable energy storage devices. However, improving their electrochemical performance from elect...Micro-supercapacitors(MSCs) have emerged as one competitive candidate of high-performance, flexible, safe,portable and wearable energy storage devices. However, improving their electrochemical performance from electrode materials to assembled devices still remains huge challenges.Here, we for the first time synthesized two-dimensional(2D),ultrathin, mesoporous polypyrrole-based graphene nanosheets uniformly anchored with redox polyoxometalate(mPPy@rGO-POM) by soft template approach. Further, using a layer-by-layer deposition and mask-assisted technique, the compactly stacked and sandwich-like hybrid film(mPGM)based on pseudocapacitive mPPy@rGO-POM nano sheets and electrochemically exfoliated graphene was directly fabricated as binder-and additive-free interdigital electrodes for all-solid-state planar micro-supercapacitors(mPGM-MSCs). Notably, the resulted mPGM-MSCs exhibited outstanding areal capacitance(115 mF cm^-2), remarkably enhanced volumetric capacitance(137 F cm^-3 at 1 mV s^-1) in comparison with MSCs based on the films of mPPy@rGO without POM anchoring(95 F cm^-3), and non-porous polypyrrole-graphene(68 F cm^-3).Further, mPGM-MSCs disclosed robust mechanical flexibility with ~96% of capacitance retention at a highly bending angle of 180°, and impressive parallel or serial interconnection for boosting capacitance or voltage output. As a consequence, our proposed strategy of filling the redox species into mesoporous graphene and other 2D nanosheets will open up new ways to manufacture high-compact and flexible energy storage devices ranging from supercapacitors to batteries.展开更多
Chalcogenide perovskites(CPs) exhibiting lower band gaps than oxide perovskites and higher stability than halide perovskites are promising materials for photovoltaic and optoelectronic applications. For such applicati...Chalcogenide perovskites(CPs) exhibiting lower band gaps than oxide perovskites and higher stability than halide perovskites are promising materials for photovoltaic and optoelectronic applications. For such applications, the absence of deep defect levels serving as recombination centers(dubbed defect tolerance) is a highly desirable property. Here,using density functional theory(DFT) calculations, we study the intrinsic defects in BaZrS_(3), a representative CP material.We compare Hubbard-U and hybrid functional methods, both of which have been widely used in addressing the band gap problem of semi-local functionals in DFT. We find that tuning the U value to obtain experimental bulk band gap and then using the obtained U value for defect calculations may result in over-localization of defect states. In the hybrid functional calculation, the band gap of BaZrS_(3)can be accurately obtained. We observe the formation of small S-atom clusters in both methods, which tend to self-passivate the defects from forming mid-gap levels. Even though in the hybrid functional calculations several relatively deep defects are observed, all of them exhibit too high formation energy to play a significant role if the materials are prepared under thermal equilibrium.BaZrS_(3)is thus expected to exhibit sufficient defect tolerance promising for photovoltaic and optoelectronic applications.展开更多
As an im portant branch of fiber-shaped energy storage devices, the fiber-shaped supercapacitor has been widely studied recently. However, it remains challenging to simultaneously achieve fast electron transport and e...As an im portant branch of fiber-shaped energy storage devices, the fiber-shaped supercapacitor has been widely studied recently. However, it remains challenging to simultaneously achieve fast electron transport and excellent ion accessibility in one single fiber electrode of the fibershaped supercapacitor. Herein, a novel family of amphiphilic core-sheath structured carbon nanotube composite fibers has been developed and applied to the fiber-shaped supercapacitor to address the above challenge. The polyaniline-modified hydrophilic sheath of the composite fiber electrode effectively enhanced the electrochemical property via advancing ion accessibility, while Au-deposited hydrophobic core demonstrated improved electrical conductivity by fast electron supply. On the basis of a synergistic effect, a remarkable specific capacitance of 324 F cm^-3 at 0.5 A cm^-3 and greatly enhanced rate performance were achieved, i.e” a 79% retention (256 F cm 3) at 50 A cm^-3. The obtained fiber-shaped supercapacitor finally displayed remarkable energy and power densities of 7.2 mW h cm 3 and 10 W cm^-3, respectively. The strategy developed herein also presents a general pathway towards novel fiber electrodes for high-performance wearable devices.展开更多
A novel all-solid-state, coaxial, fiber-shaped asymmetric supercapacitor has been fabricated by wrapping a conducting carbon paper on a MnO2-modified nanoporous gold wire. This energy wire exhibits high capacitance of...A novel all-solid-state, coaxial, fiber-shaped asymmetric supercapacitor has been fabricated by wrapping a conducting carbon paper on a MnO2-modified nanoporous gold wire. This energy wire exhibits high capacitance of 12 mF.cm^-2 and energy density of 5.4 μW.h.cm^-2 with excellent cycling stability. Hierarchical nanostructures and coaxial architectural design facilitate effective contacts between the two core@sheath electrodes and active layers with high flexibility and high performance. This work provides the first example of coaxial fiber- shaped asymmetric supercapacitors with an operation voltage of 1.8 V, and holds great potential for future flexible electronic devices.展开更多
MnO2/carbon nanocomposites with hierarchical pore structure and controllable MnO2 loading have been synthesized using a self-limiting growth method. This was achieved by the redox reactions of KMnO4 with sacrificed ca...MnO2/carbon nanocomposites with hierarchical pore structure and controllable MnO2 loading have been synthesized using a self-limiting growth method. This was achieved by the redox reactions of KMnO4 with sacrificed carbon substrates that contain hierarchical pores. The unique pore structure allows the synthesis of nanocomposites with tunable MnO2 loading up to 83 wt.%. The specific capacitance of the nanocomposites increased with the MnO2 loading; the conductivity measured by electrochemical impedance spectroscopy, on the other hand, decreased with increasing MnO2 loading. Optimization of the MnO2 loading resulted in nanocomposites with high specific capacitance and excellent rate capability. This work provides important fundamental understanding which will facilitate the design and fabrication of high-performance supercapacitor materials for a large variety of applications.展开更多
The interlayer space of the layered materials is not always the electrochemical active area for contributing to the pseudocapacitive process. To our knowledge, few efforts have been devoted to investigating the effect...The interlayer space of the layered materials is not always the electrochemical active area for contributing to the pseudocapacitive process. To our knowledge, few efforts have been devoted to investigating the effect of interlayer distance of layered double hydroxides(LDHs) on pseudocapacitors. Here, we obtained the CoAl-LDH with different interlayer distance via the reaction in aqueous media hydrothermally. Electrochemical characterization reveals that the CoAl(DS^-(dodecyl sulfate))-LDHs with an interlayer distance of 2.58 nm can deliver higher specific capacitance of 1481.7 F g^-1 than CoAl(SO4^2-)-LDH(0.87 nm, 1252.7 F g^-1) and CoAl(CO3^2-)-LDH(0.76 nm, 1149.2 Fg^-1) at a discharge current density of 1 A g^-1. An asymmetric supercapacitor with the CoAl(DS^-)-LDHs‖activated carbon also shows a better electrochemical performance, including a high energy density of54.2 W h kg^-1 at a power density of 0.9 kW kg^-1 and a longterm stability, in comparison with CoAl(SO4^2-)-LDH and CoAl(CO3^2-)-LDH ‖activated carbon.展开更多
Despite demonstrating remarkable power conversion efficiencies(PCEs), perovskite solar cells(PSCs) have not yet achieved their full potential. In particular, the interfaces between the perovskite and charge transport ...Despite demonstrating remarkable power conversion efficiencies(PCEs), perovskite solar cells(PSCs) have not yet achieved their full potential. In particular, the interfaces between the perovskite and charge transport layers account for the vast majority of the recombination losses.Interfacial contact and band alignment between the lowtemperature-processed TiO_(2) electron transport layer(ETL)and the perovskite are essential to minimize nonradiative recombination losses. In this study, a CeOx interlayer is employed to modify the perovskite/TiO_(2) interface, and the charge transport properties of the devices are investigated. The bilayer-structured TiO_(2)/CeOx ETL leads to the modification of the interface energetics, resulting in improved electron extraction and reduced nonradiative recombination in the PSCs.Devices based on TiO_(2)/CeOx ETL exhibit a high open-circuit voltage(Voc) of 1.13 V and an enhanced PCE of more than 20%as compared with Vocof 1.08 V and a PCE of approximately 18% for TiO^(2-)based devices. Moreover, PSCs based on TiO_(2)/CeOx ETL maintain over 88% of their initial PCEs after light illumination for 300 min, whereas PSCs based on TiO_(2) ETL almost failed. This study provides an efficient strategy to enhance the PCE and stability of PSCs based on a lowtemperature-processed TiO_(2) ETL.展开更多
Electrochemical ion exchange has been used to tailor the composition of transition metal oxides (Co3O4) electrode with enhanced capacity while maintaining its crystal structure and morphology. Specifically, Ni ions ...Electrochemical ion exchange has been used to tailor the composition of transition metal oxides (Co3O4) electrode with enhanced capacity while maintaining its crystal structure and morphology. Specifically, Ni ions were incorporated to C03O4 nanosheets sandwiched by nanoneedles to form Co3O4/NiCo2O4 composite. As positive electrode for supercapacitors, the Co3O4/NiCo2O4 composite presents a high areal capacitance of 3.2 F cm^-2 (1060 F g^-1) at a current density of 5 mA cm^-2 and outstanding rate capability as well as long cycle stability. Moreover, the assembled aqueous asymmetric supercapacitor based on Co3O4/NiCo2O4//carbon cloth electrodes delivers a considerable energy density of 3.0 mW hcm^-3 at power density of 136 mW cm^-3, and high rate capability (85% retention at a current density of 30 mA cm^-2). A safety light composed of ten green LEDs in parallel was lit for -360 s using two identical supercapacitors in series, indicating a promising practical application.展开更多
文摘A novel type of composite electrode based on nmltiwalled carbon nanotubes coated with sheet-like cobalt hydroxide particles was used in supercapacitors. Cobalt hydroxide cathodlcally deposited fiom Co(NO3)O2 solution with carbon nanotubes as matrix exhibited large pseudo-capacitance of 322 F/g in 1 mol/L KOH. To characterize the cobalt hydroxide nanocomposite electrode, a charge-discharge cycling test, cyclic voltammetry, and an impedance test were done. This cobalt hydroxide composite exhibiting excellent pseudo-capacitive behavior (i.c. high reversibility, high specific capacitance, low impedance), was demonstrated to be a candidate for the application of electrochemical supercapacitors. A combined capacitor consisting of cobalt hydroxide composite as a cathode and activated carbon fiber as an anode was reported. The electrochemical pcrformance of the combined capacitor was characterized by cyclic voltammetry and a dc charge/discharge test. The combined capacitor showed ideal capacitor behavior with an extended operating voltage of 1.4 V. According to the extended operating voltage, the energy density of the combined capacitor at a current density of 100 mA/cm^2 was found to be 11 Wh/kg. The combined capacitor exhibited high-energy density and stable power characteristics,
基金Project(2005CB623703) supported by the National Basic Research Program of China project(5JJ30103) supported bythe Natural Science Foundation of Hunan Province
文摘Taking the nano-sized carbon black and aniline monomer as precursor and (NH4)2S2O6 as oxidant, the well coated C/polyaniline(C/PANI) composite materials were prepared by in situ polymerization of the aniline on the surface of well-dispersed nano-sized carbon black for supercapacitor. The micro-structure of the C/PANI composite electrode materials were analyzed by SEM. The electrochemical properties of C/ PANI and PANI composite electrode were characterized by means of the galvanostatic charge-discharge experiment, cyclic voltammetric measurement and impedance spectroscopy analysis. The results show that by adding the nano-sized carbon black in the process of chemical polymerization of the aniline, the polyaniline can be in situ polymerized and well-coated onto the carbon black particles, which may effectively improve the aggregation of particles and the electrolyte penetration. What’s more , the maximum of specific capacitance of C/PANI electrode 437.6F·g -1 can be attained. Compared with PANI electrode, C/PANI electrode shows more desired capacitance characteristics, smaller internal resistance and better cycle performance.
文摘Efficient and affordable electrocatalysts for reversible oxygen reduction and oxygen evolution reactions(ORR and OER,respectively)are highly sought-after for use in rechargeable metal-air batteries.However,the construction of high-performance electrocatalysts that possess both largely accessible active sites and superior ORR/OER intrinsic activities is challenging.Herein,we report the design and successful preparation of a 3D hierarchically porous graphene framework with interconnected interlayer macropores and in-plane mesopores,enriched with pyridinic-nitrogen-cobalt(pyri-N-Co)active sites,namely,CoFe/3D-NLG.The pyri-N-Co bonding significantly accelerates sluggish oxygen electrocatalysis kinetics,in turn substantially improving the intrinsic ORR/OER activities per active site,while copious interlayer macropores and in-plane mesopores enable ultra-efficient mass transfer throughout the graphene architecture,thus ensuring sufficient exposure of accessible pyri-N-Co active sites to the reagents.Such a robust catalyst structure endows CoFe/3D-NLG with a remarkably enhanced reversible oxygen electrocatalysis performance,with the ORR half-wave potential identical to that of the benchmark Pt/C catalyst,and OER activity far surpassing that of the noble-metal-based RuO2 catalyst.Moreover,when employed as an air electrode for a rechargeable Zn-air battery,CoFe/3D-NLG manifests an exceedingly high open-circuit voltage(1.56 V),high peak power density(213 mW cm^(–2)),ultra-low charge/discharge voltage(0.63 V),and excellent charge/discharge cycling stability,outperforming state-of-the-art noble-metal electrocatalysts.
基金Foundation item: Supported by the National Natural Science Foundation of China (Nos. 51077014, 21003028 and 51202043): the Fundamental Research funds for the Central Universities, the Program for New Century Excellent Talents in University (NCET-10-0050), and the Excellent Youth Foundation of Heilongjiang Province of China.
文摘This work presents NiS/graphene/carbon nanotube (NiS/GNS/CNT) composites as electrode material for the supercapacitor application in sea flashing signal systems. NiS nanosheets were closely anchored on the conductive GNS-CNT networks. As a result, the NiS/GNS/CNT electrode showed a high specific capacitance of 2 377 F.g^-1 at 2 mV.s^-1 and good cycling stability compared with the pure NiS (1 599F.g^-1). The enhanced electrochemical performances are attributed to the synergetic effect between the conductive carbon and the pseudo-capacitive NiS. The high performance supercapacitor may provide application in the sea flashing signal system.
文摘Nano sized powders of TiO2 (titanium dioxide) and Nb2O5 (Niobium (V) oxide) were used to fabricate TiO2/Nb2O5 composites thin films by EPD (electrophoretic deposition) technique. The metal oxide powders, together with magnesium nitrate hexahydrate pellets, were suspended in propan-2-ol inside an EPD cell. The electrodes, placed 1.2 cm apart, were partially immersed in the suspension and a DC potential applied across them. Key EPD process parameters, which include applied DC electric field, deposition time and solid concentration in suspension, were optimized through visual inspection and from UV-Vis-NIR spectrophotometer spectra. The highest (55%) transmittance was obtained for films with deposition time of 90 s, powder concentration of 0.01 g/40 mL, and 35 V DC (direct current) voltage. XRD micrographs confirmed that TiO2 and Nb2O5 particles were presented in the composite film. SEM (scanning electron microscope) micrographs of the composite electrode thin films showed that porous films of high quality with well controlled morphology were deposited by using the EPD technique.
文摘Graphene-based three-dimensional (3D) macroscopic materials have recently attracted increasing interest by virtue of their exciting potential in electrochemical energy conversion and storage. Here we report a facile one-step strategy to prepare mechanically strong and electrically conductive graphene/Ni(OH)2 composite hydrogels with an interconnected porous network. The composite hydrogels were directly used as 3D supercapacitor electrode materials without adding any other binder or conductive additives. An optimized composite hydrogel containing -82 wt.% Ni(OH)2 exhibited a specific capacitance of -1,247 F/g at a scan rate of 5 mV/s and -785 F/g at 40 mV/s (-63% capacitance retention) with excellent cycling stability. The capacity of the 3D hydrogels greatly surpasses that of a physical mixture of graphene sheets and Ni(OH)2 nanoplates (-309 F/g at 40 mV/s). The same strategy was also applied to fabricate graphene-carbon nanotube/Ni(OH)2 ternary composite hydrogels with further improved specific capacitances (-1,352 F/g at 5 mV/s) and rate capability (-66% capacitance retention at 40 mV/s). Both composite hydrogels obtained here can deliver high energy densities (-43 and -47 Wh/kg, respectively) and power densities (-8 and -9 kW/kg, respectively), making them attractive electrode materials for supercapacitor applications. This study opens a new pathway to the design and fabrication of functional 3D graphene composite materials, and can significantly impact broad areas including energy storage and beyond.
基金This work was supported by the "Thousands Talents" Program for Pioneer Researcher and His Innovation Team, China. This work was also supported by the National Natural Science Foundation of China (No.51374029), Program for New Century Excellent Talents in University (No. NCET-13-0668), Fundamental Research Funds for the Central Universities (No. FRF-TP-14-008C1) and China Postdoctoral Science Foundation (No. 2014M550675).
文摘Nanostructured Mn3O4 was introduced to activated C (AC) by a novel sonochemical reaction, and the resulting nanocomposites were examined as supercapacitor electrodes. The sonication not only catalyzed the redox reaction but also promoted the diffusion of the precursors, causing the formation of coherent nanocomposites with Mn3O4 nanoparticles grown and uniformly distributed inside the mesopores of the AC. In addition, the extreme local condition in the sonochemical synthesis yielded an excessive amount of divalent manganese ions and oxygen vacancies. This novel microstructure endowed the sample with a superior performance, including a specific capacitance of 150 F/g compared with the value of 93 F/g for AC at a charge/discharge rate of 100 mA/g. A Li-ion capacitor delivered an energy density of 68 Wh/kg, compared with 41 Wh/kg for the AC capacitor at a power density of 210 W/kg.
基金supported by the National Natural Science Foundation of China (51702048 and 21603157)the National Basic Research Program of China (2015CB932600)Jiangxi Provincial Department of Education (GJJ170459 and GJJ170457)
文摘Flexible supercapacitors (SCs) are attractive energy storage devices for wearable electronics, but their applications are hindered by their low volumetric energy densities. Two dimensional (2D) non-carbon nanomaterials are the most promising pseudocapacitive materials for high volumetric capacitance electrodes. However, they are poorly conductive and prone to self-stacking, which results in unsatisfactory electrochemical performance. In this work, large-scale V2O5·nH2O ultrathin nanosheets are synthesized by a facile and scalable method and transformed into layered and compact composite films with one-dimensional carbon nanotubes (CNTs). The self-standing films show an optimized volumetric capacitance of 521.0Fcm^-3 with only 10 wt% of CNTs, which is attributed to dramatically enhanced electrical conductivity beyond the electrical percolation threshold, high dispersion of pseudocapacitive V2O5·nH2O nanosheets, and high mass density of the films. All-solid-state flexible SCs made of V2O5·nH2O/CNTs films show a maximum energy density of 17.4WhL^-1.
基金supported by the National Natural Science Foundation of China (51572259)National Key R&D Program of China (2016YBFO100100 and 2016YFA0200200)+3 种基金Natural Science Foundation of Liaoning Province (201602737)Recruitment Program of Global Expert (1000 Talent Plan),DICPChina Postdoctoral Science Foundation (2016M601348)Exploratory Research Program of Shaanxi Yanchang Petroleum (Group) Co.,LTD & DICP
文摘Micro-supercapacitors(MSCs) have emerged as one competitive candidate of high-performance, flexible, safe,portable and wearable energy storage devices. However, improving their electrochemical performance from electrode materials to assembled devices still remains huge challenges.Here, we for the first time synthesized two-dimensional(2D),ultrathin, mesoporous polypyrrole-based graphene nanosheets uniformly anchored with redox polyoxometalate(mPPy@rGO-POM) by soft template approach. Further, using a layer-by-layer deposition and mask-assisted technique, the compactly stacked and sandwich-like hybrid film(mPGM)based on pseudocapacitive mPPy@rGO-POM nano sheets and electrochemically exfoliated graphene was directly fabricated as binder-and additive-free interdigital electrodes for all-solid-state planar micro-supercapacitors(mPGM-MSCs). Notably, the resulted mPGM-MSCs exhibited outstanding areal capacitance(115 mF cm^-2), remarkably enhanced volumetric capacitance(137 F cm^-3 at 1 mV s^-1) in comparison with MSCs based on the films of mPPy@rGO without POM anchoring(95 F cm^-3), and non-porous polypyrrole-graphene(68 F cm^-3).Further, mPGM-MSCs disclosed robust mechanical flexibility with ~96% of capacitance retention at a highly bending angle of 180°, and impressive parallel or serial interconnection for boosting capacitance or voltage output. As a consequence, our proposed strategy of filling the redox species into mesoporous graphene and other 2D nanosheets will open up new ways to manufacture high-compact and flexible energy storage devices ranging from supercapacitors to batteries.
基金supported by the National Natural Science Foundation of China (11774365)the Natural Science Foundation of Shanghai (19ZR1421800)+4 种基金Shanghai International Cooperation Project (20520760900)the Opening Project and Science Foundation for Youth Scholar of State Key Laboratory of High Performance Ceramics and Superfine Microstructures (SKL201804 and SKL201803SIC) support by US National Science Foundation (NSF) (CBET1510121)US Department of Energy (DOE) (DEEE0007364)support by US NSF (CBET-1510948).support by US NSF (DMR-1506669)support by the Fundamental Research Funds for the Central Universities (DUT21RC(3) 033)。
文摘Chalcogenide perovskites(CPs) exhibiting lower band gaps than oxide perovskites and higher stability than halide perovskites are promising materials for photovoltaic and optoelectronic applications. For such applications, the absence of deep defect levels serving as recombination centers(dubbed defect tolerance) is a highly desirable property. Here,using density functional theory(DFT) calculations, we study the intrinsic defects in BaZrS_(3), a representative CP material.We compare Hubbard-U and hybrid functional methods, both of which have been widely used in addressing the band gap problem of semi-local functionals in DFT. We find that tuning the U value to obtain experimental bulk band gap and then using the obtained U value for defect calculations may result in over-localization of defect states. In the hybrid functional calculation, the band gap of BaZrS_(3)can be accurately obtained. We observe the formation of small S-atom clusters in both methods, which tend to self-passivate the defects from forming mid-gap levels. Even though in the hybrid functional calculations several relatively deep defects are observed, all of them exhibit too high formation energy to play a significant role if the materials are prepared under thermal equilibrium.BaZrS_(3)is thus expected to exhibit sufficient defect tolerance promising for photovoltaic and optoelectronic applications.
基金supported by the Ministry of Science and Technology (2016YFA0203302)the National Natural Science Foundation of China (21634003, 51573027, 51673043, 21604012, 21805044 and 21875042)+1 种基金Shanghai Science and Technology Committee (16JC1400702, 17QA1400400, 18QA1400700 and 18QA1400800)SHMEC (2017-01-07-00-07-E00062)
文摘As an im portant branch of fiber-shaped energy storage devices, the fiber-shaped supercapacitor has been widely studied recently. However, it remains challenging to simultaneously achieve fast electron transport and excellent ion accessibility in one single fiber electrode of the fibershaped supercapacitor. Herein, a novel family of amphiphilic core-sheath structured carbon nanotube composite fibers has been developed and applied to the fiber-shaped supercapacitor to address the above challenge. The polyaniline-modified hydrophilic sheath of the composite fiber electrode effectively enhanced the electrochemical property via advancing ion accessibility, while Au-deposited hydrophobic core demonstrated improved electrical conductivity by fast electron supply. On the basis of a synergistic effect, a remarkable specific capacitance of 324 F cm^-3 at 0.5 A cm^-3 and greatly enhanced rate performance were achieved, i.e” a 79% retention (256 F cm 3) at 50 A cm^-3. The obtained fiber-shaped supercapacitor finally displayed remarkable energy and power densities of 7.2 mW h cm 3 and 10 W cm^-3, respectively. The strategy developed herein also presents a general pathway towards novel fiber electrodes for high-performance wearable devices.
文摘A novel all-solid-state, coaxial, fiber-shaped asymmetric supercapacitor has been fabricated by wrapping a conducting carbon paper on a MnO2-modified nanoporous gold wire. This energy wire exhibits high capacitance of 12 mF.cm^-2 and energy density of 5.4 μW.h.cm^-2 with excellent cycling stability. Hierarchical nanostructures and coaxial architectural design facilitate effective contacts between the two core@sheath electrodes and active layers with high flexibility and high performance. This work provides the first example of coaxial fiber- shaped asymmetric supercapacitors with an operation voltage of 1.8 V, and holds great potential for future flexible electronic devices.
文摘MnO2/carbon nanocomposites with hierarchical pore structure and controllable MnO2 loading have been synthesized using a self-limiting growth method. This was achieved by the redox reactions of KMnO4 with sacrificed carbon substrates that contain hierarchical pores. The unique pore structure allows the synthesis of nanocomposites with tunable MnO2 loading up to 83 wt.%. The specific capacitance of the nanocomposites increased with the MnO2 loading; the conductivity measured by electrochemical impedance spectroscopy, on the other hand, decreased with increasing MnO2 loading. Optimization of the MnO2 loading resulted in nanocomposites with high specific capacitance and excellent rate capability. This work provides important fundamental understanding which will facilitate the design and fabrication of high-performance supercapacitor materials for a large variety of applications.
基金financially supported by the National Natural Science Foundation of China (21501152,21571159,21671178,21441003,51521091 and 51525206)China Postdoctoral Science Foundation (2017M611282)+5 种基金Program for Changjiang Scholars and Innovative Research Team in University (IRT15R61)Ministry of Science and Technology of China (2016YFA0200100 and 2016YBF0100100)Foundation of Zhengzhou University of Light Industry (2014BSJJ054)Strategic Priority Research Program of the Chinese Academy of Sciences (XDA09010104)Projects for Public Entrepreneurship and Public Innovation of ZZULI (2017ZCKJ215)Key Program of Henan Province for Science and Technology (162102210212)
文摘The interlayer space of the layered materials is not always the electrochemical active area for contributing to the pseudocapacitive process. To our knowledge, few efforts have been devoted to investigating the effect of interlayer distance of layered double hydroxides(LDHs) on pseudocapacitors. Here, we obtained the CoAl-LDH with different interlayer distance via the reaction in aqueous media hydrothermally. Electrochemical characterization reveals that the CoAl(DS^-(dodecyl sulfate))-LDHs with an interlayer distance of 2.58 nm can deliver higher specific capacitance of 1481.7 F g^-1 than CoAl(SO4^2-)-LDH(0.87 nm, 1252.7 F g^-1) and CoAl(CO3^2-)-LDH(0.76 nm, 1149.2 Fg^-1) at a discharge current density of 1 A g^-1. An asymmetric supercapacitor with the CoAl(DS^-)-LDHs‖activated carbon also shows a better electrochemical performance, including a high energy density of54.2 W h kg^-1 at a power density of 0.9 kW kg^-1 and a longterm stability, in comparison with CoAl(SO4^2-)-LDH and CoAl(CO3^2-)-LDH ‖activated carbon.
基金supported by the National Key Research and Development Program of China (2018YFB1500101)the 111 Project (B16016)+1 种基金the National Natural Science Foundation of China (U1705256,51702096 and 61904053)the Fundamental Research Funds for the Central Universities (2019MS026,2019MS027 and 2020MS080)。
文摘Despite demonstrating remarkable power conversion efficiencies(PCEs), perovskite solar cells(PSCs) have not yet achieved their full potential. In particular, the interfaces between the perovskite and charge transport layers account for the vast majority of the recombination losses.Interfacial contact and band alignment between the lowtemperature-processed TiO_(2) electron transport layer(ETL)and the perovskite are essential to minimize nonradiative recombination losses. In this study, a CeOx interlayer is employed to modify the perovskite/TiO_(2) interface, and the charge transport properties of the devices are investigated. The bilayer-structured TiO_(2)/CeOx ETL leads to the modification of the interface energetics, resulting in improved electron extraction and reduced nonradiative recombination in the PSCs.Devices based on TiO_(2)/CeOx ETL exhibit a high open-circuit voltage(Voc) of 1.13 V and an enhanced PCE of more than 20%as compared with Vocof 1.08 V and a PCE of approximately 18% for TiO^(2-)based devices. Moreover, PSCs based on TiO_(2)/CeOx ETL maintain over 88% of their initial PCEs after light illumination for 300 min, whereas PSCs based on TiO_(2) ETL almost failed. This study provides an efficient strategy to enhance the PCE and stability of PSCs based on a lowtemperature-processed TiO_(2) ETL.
基金supported by the National Natural Science Foundation of China (61376011)Gansu Provincial Natural Science Foundation of China (17JR5RA198)the Fundamental Research Funds for the Central Universities (lzujbky-2017-k21)
文摘Electrochemical ion exchange has been used to tailor the composition of transition metal oxides (Co3O4) electrode with enhanced capacity while maintaining its crystal structure and morphology. Specifically, Ni ions were incorporated to C03O4 nanosheets sandwiched by nanoneedles to form Co3O4/NiCo2O4 composite. As positive electrode for supercapacitors, the Co3O4/NiCo2O4 composite presents a high areal capacitance of 3.2 F cm^-2 (1060 F g^-1) at a current density of 5 mA cm^-2 and outstanding rate capability as well as long cycle stability. Moreover, the assembled aqueous asymmetric supercapacitor based on Co3O4/NiCo2O4//carbon cloth electrodes delivers a considerable energy density of 3.0 mW hcm^-3 at power density of 136 mW cm^-3, and high rate capability (85% retention at a current density of 30 mA cm^-2). A safety light composed of ten green LEDs in parallel was lit for -360 s using two identical supercapacitors in series, indicating a promising practical application.