2017 Vol. 32, No. 6

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2017, 32(6): .
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2017, 32(6): .
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A review of nanocarbon current collectors used in electrochemical energy storage devices
KONG Long, YAN Chong, HUANG Jia-qi
2017, 32(6): 481-500.
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Electrochemical energy storage is critical for the exploration of renewable but occasional use energy sources and for powering electronic devices. Nanocarbon current collectors, such as carbon nanotubes, carbon nanofibers and graphene in both 2D lamellar and 3D network forms, have high specific surface areas, good electrical conductivities, tunable interfacial chemical properties and excellent flexibility, which provide viable platforms for the exploration of lithium-sulfur batteries, lithium ion batteries and supercapacitors. This review focuses on the use of nanocarbon current collectors in electrochemical energy storage devices and probes their interfacial mechanisms. A brief introduction to lithium ion batteries and electrochemical capacitors with high-energy/power-densities enabled by nanocarbon current collectors is also included. Conclusions and perspectives are presented on problems related to the use of nanocarbon current collectors in advanced electrochemical energy storage systems and their solutions.
Recent progress in device configuration and electrode fabrication for micro-supercapacitors
WANG Sen, ZHENG Shuang-hao, HUANG Hai-bo, SUN Cheng-lin, WU Zhong-shuai
2017, 32(6): 501-508.
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Micro-supercapacitors are a new class of high-power miniaturized electrochemical energy-storage devices, which not only offer a balanced energy and power density, bridging the gap between thin-film batteries and electrolytic capacitors, but can also be directly integrated with micro-/nano-scale electronic devices to offer sufficient peak power. This review summarizes recent progress in the device configuration and electrode fabrication of micro-supercapacitors, and discusses the main challenges and future possibilities they offer.
SAPO-34 templated growth of hierarchical porous graphene cages as electrocatalysts for both oxygen reduction and evolution
ZHONG Ling, TANG Cheng, WANG Bin, WANG Hao-fan, GAO Shang, WANG Yao, ZHANG Qiang
2017, 32(6): 509-516. doi: 10.1016/S1872-5805(17)60136-7
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Three-dimensional hierarchical porous graphene materials with unique properties are of significant importance for the exploration of advanced electrocatalysts for both the oxygen reduction and evolution reactions (ORR/OER). Templated chemical vapor deposition is a favorable strategy to fabricate this kind of graphene, but the number of effective templates is limited. Here, silicoaluminophosphate (SAPO-34) zeolite crystals were used as the catalytic templates for the deposition of hierarchical porous graphene. The graphene obtained consisted of micron-size hollow cubes with mesoporous/nanoporous facets, and ultrathin walls, precisely replicating the structure of the cube-like SAPO-34 zeolite particles. A high doping level of nitrogen (6.84 at%) was achieved by subsequent annealing at 700℃ under ammonia before template removal. Because of the unique porosity, abundant defects, and favorable N-doping, the N-doped graphene exhibited considerable reactivity for both ORR and OER.
N, S co-doped porous carbon nanospheres with a high cycling stability for sodium ion batteries
ZHANG Hong-wei, LU Jia-min, YANG Le, HU Ming-xiang, HUANG Zheng-hong, LU Rui-tao, KANG Fei-yu
2017, 32(6): 517-526. doi: 10.1016/S1872-5805(17)60137-9
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Developing high-performance and low-cost anode materials is crucial for the practical use of sodium-ion batteries (SIBs) at room-temperature. Porous carbon nanospheres with a uniform diameter for use as SIB anode materials were synthesized by the hydrothermal treatment of glucose to obtain the spheres, and subsequent carbonization and modification with KOH activation and N, S co-doping during or after the activation using thiourea as the N and S sources. Nanospheres doped with N and S after KOH activation have a high initial specific capacity of 527 mAh g-1 at a current density of 20 mA g-1 and an excellent cycling stability with a 95.2% capacity retention after 1 000 cycles at a high current density of 500 mA g-1. The capacity retention rate is higher than that of most of the state-of-the-art anode materials for SIBs. This good performance is attributed to the abundant micro-pores, the enlarged interlayer spacing produced by the co-doping, and the high conductivity of the carbon nanospheres.
Hydrothermal synthesis of Ni(OH)2/RGO nanocomposites with superior electrochemical performance
LI Qian, LU Chun-xiang, CHEN Cheng-meng, XIE Li-jing, YUAN Shu-xia
2017, 32(6): 527-534.
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Ni(OH)2/reduced graphene oxide (RGO) nanocomposites for use as electrodes in electrochemical capacitors were prepared from GO and nickel nitrate by a one-step hydrothermal method. The content of RGO in the composites was controlled by changing the GO/nickel nitrate mass ratio. Results indicate that Ni(OH)2 nanobelts are dispersed uniformly in the three-dimensional conducting network constructed by the RGO, which is favorable for their capacitive performance. The RGO content to achieve the best performance is 26.7 wt%. The best sample has a high specific capacity of 1 804 F/g at 1 A/g, a remarkable capacitance retention rate of 46% even at 25 A/g, and an excellent cycle life with 90.3% capacitance retention after 2 000 cycles at 2 A/g.
Nitrogen-doped CMK-3@graphene hybrids as a sulfur host material for use in lithium-sulfur batteries
TANG Xiao-nan, SUN Zhen-hua, ZHUO Shu-ping, LI Feng
2017, 32(6): 535-541.
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Sulfur as a cathode material has the advantages of low cost, high theoretical energy density and safety. However, the capacity decay and a shuttle effect are major problems that cause poor coulombic efficiency and a short cycling life. An ordered mesoporous carbon, CMK-3 was oxidized by 67% HNO3, added to a graphene oxide suspension, sonicated, freeze-dried and annealed in NH3 to obtain a nitrogen-doped CMK-3@graphene hybrid, which was melt-infiltrated with sulfur to prepare a cathode material for lithium-sulfur batteries. Results indicate that the CMK-3 particles are uniformly dispersed in graphene sheets and their surfaces are coated with graphene. The N-(CMK-3@G)/S has a reversible discharge capacity of 867.3 mAh·g-1 after 300 cycles at a current density of 335 mA·g-1 with a capacity retention of 82%. Compared with N-CMK-3/S and N-G/S cathodes, the rate performance and polarization characteristics are also improved. The graphene coating on CMK-3 traps soluble polysulfides during the charge/discharge process and nitrogen doping facilitates chemical adsorption of polysulfides to inhibit the shuttle effect, which together improve the performance of the battery.
The capacitances of the negative and positive electrodes of supercapacitors, using nitrogen-doped mesoporous carbons as the active materials, in different electrolytes
CHEN Ming-qi, PAN Min, TIAN Meng, WANG Ji-tong, LONG Dong-hui
2017, 32(6): 542-549.
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Nitrogen-doped mesoporous carbons (NMCs) with controllable nitrogen contents and similar pore structures were prepared by a sol-gel process coupled with hard templating method, using melamine, phenol and formaldehyde as precursors, and colloidal silica as hard templating. The effects of nitrogen doping content on the asymmetric capacitance of the mesoporous carbon in H2SO4, KOH and Et4NBF4/PC electrolyte were systematically investigated. The nitrogen-doping has significantly improved the capacitance performance, and both positive and negative electrodes deliver the highest specific capacitance at a nitrogen-doping content of around 8%. In the KOH electrolyte, the negative pseudo-capacitances is significantly higher than that of the positive ones, and the capacity difference is up to 57.9 F/g. In H2SO4 electrolyte, the nearly same capacitances for each electrode are found for all samples. And in the organic Et4NBF4/PC system, the increased capacitance is mainly attributed to the negative. The study on asymmetrical capacitance response of nitrogen-doped mesoporous carbon paves the way for optimizing the ratio of positive and negative electrode active materials, leading a higher energy density.
Structure control of powdery carbon aerogels and their use in high-voltage aqueous supercapacitors
CAI Li-feng, XU Jing, HUANG Jian-yu, XU Hong-ji, XU Fei, LIANG Ye-ru, FU Ruo-wen, WU Ding-cai
2017, 32(6): 550-556.
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Powdery carbon aerogels (PCAs) for use as electrode materials in high-voltage aqueous supercapacitors were prepared from nanospheres of 1,2-divinylbenzene-styrene copolymer after carbonyl crosslinking. The effect of the size and carbonyl crosslinking conditions of the nanospheres on the microstructure and electrochemical properties of the PCAs were investigated. Results indicated that the size of the nanospheres, the crosslinking temperature and time played important roles in tailoring the nanostructures and electrochemical performance of the PCAs. All the PCAs had a well-defined 3D network and a hierarchical pore structure with a high porosity. The network units were between 25 and 100 nm in size, and the Brunauer-Emmett-Teller (BET) specific surface areas were from 392 to 767 m2g-1. The PCA with a BET surface area of 657 m2g-1 had a high electrochemical active surface area, a large capacitance and high capacitance retention rates at high current densities when used as electrodes in a 1.8 V aqueous supercapacitor using a Na2SO4 aqueous electrolyte. The use of a high-voltage aqueous electrolyte significantly increased the energy density of the supercapacitors.
Synthesis of biomass-derived carbon sheets decorated with metal nanoparticles and their catalytic performance in the oxygen evolution reaction
HUANG Hong-ling, YU Chang, HUANG Hua-wei, YAO Xiu-chao, TAN Xin-yi, HONG Jia-fu, QIU Jie-shan
2017, 32(6): 557-563.
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Biomass-derived carbons decorated with ultrafine metal nanoparticles were prepared by the carbonization of gelatin that had absorbed Ni and/or Fe ions. The morphology and structure of the samples were characterized by XRD, SEM, TEM, and their catalytic performance for the oxygen evolution reaction was evaluated by linear sweep voltammetry, electrochemical impedance spectroscopy and the Tafel polarization test. Results indicate that the metal nanoparticles are uniformly loaded on the carbon sheets. The FeNi alloy/carbon (FeNi/C) nanocomposite has the highest current density of 10 mA cm-2 at the lowest overpotential of 366 mV, and features the smallest Tafel slope of 46.6 mV dec-1 and the lowest charge transfer resistance of 13.76 ohm. Moreover, the FeNi/C nanocomposite also exhibits a long-term stability and is able to operate at 5 mA cm-2 for 25 h. The combination of conductive carbon sheets, uniformly loaded FeNi nanoparticles and abundant pores is responsible for the increased catalytic activity and fast reaction kinetics of the FeNi/C nanocomposite for the oxygen evolution reaction.
Preparation of three-dimensional hierarchical porous carbon microspheres for use as a cathode material in lithium-air batteries
YANG Ning, HU Dong-run, CAO Bo-kai, CHEN Yong, LI De, CHEN Da-ming
2017, 32(6): 564-571.
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Urea-formaldehyde resin microspheres were prepared by a polymerization method using urea and formaldehyde as the raw materials and hydrochloric acid as the catalyst. The microspheres were pre-oxidized and carbonized to obtain carbon microspheres, then activated with KOH. The morphology and pore structure of products were characterized by SEM, TEM and N2 adsorption. Results indicate that the microstructure of the microspheres is highly dependent on the mass ratio of urea to formaldehyde and the concentration of hydrochloric acid. The specific surface area of the carbon microspheres is 498 m2·g-1, which is increased to 827 m2·g-1 after KOH activation. When used as the electrode materials of lithium-air batteries, the initial charge and discharge capacities are 2 017 and 2 075 mAh·g-1, respectively, at a current density of 100 mA·g-1.
The influence of conductive additives on the performance of a SiO/C composite anode in lithium-ion batteries
TENG Xin, XU Hong-liang, LIU Qi, SHI Li-li, GAI Liang, WANG Lei, YANG Yu-sheng, WU Feng
2017, 32(6): 572-580. doi: 10.1016/S1872-5805(17)60138-0
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Two conductive additives, carbon black (Super-P) and vapor-grown carbon fibers (VGCFs), were used in 2.5 Ah Li ion batteries using LiCoO2 as the cathode and a SiO/C composite as the anode. The electrode shape, peel strength, electrolyte absorption, electrolyte storage capacity, volume change and the electrochemical performance were investigated. Results indicate that both batteries have high energy densities (more than 600 Wh/L), but the batteries with VGCFs have the better low temperature performance, longer cycle life, higher rate capability and lower volume expansion, which is ascribed to the superior conductive network formed by the VGCFs.
High-performance flexible wire-shaped electrochemical capacitors based on gold wire@reduced graphene oxide
CHANG Yun-zhen, HAN Gao-yi, XIAO Yao-ming, ZHOU Hai-han, LI Miao-yu, FU Dong-ying, ZHOU Wen
2017, 32(6): 581-591. doi: 10.1016/S1872-5805(17)60139-2
Abstract(331) PDF(366)
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Flexible gold@reduced graphene oxide sheathed wires (WAu@rGO) were prepared by soaking a gold wire (100 μm in diameter) in the center of glass capillaries with inner diameters of 1.0, 1.3 and 1.8 mm in a suspension of graphene oxide (GO) in a L-ascorbic acid aqueous solution at 30℃ for 48 h. The WAu@rGO wires were obtained after removal of the capillaries, and their microstructures were characterized by SEM and their electrochemical properties as flexible electrodes in electrochemical capacitors were investigated by electrochemical tests. Results show that the specific capacitance of the WAu@rGO wire with the smallest diameter is 5.47 mF cm-1 or 176.7 F g-1 at a scan rate of 1 mV s-1. A symmetric all-solid-state flexible electrochemical capacitor based on the two smallest wires and a polyvinyl alcohol/H3PO4 gel electrolyte shows a maximum capacitance of 2.06 mF cm-1, or 6.87 mF cm-2 or 411.9 mF cm-3. The solid-state capacitor has energy and power densities of 9.48×10-4 mWh cm-2 and 0.017 mW cm-2, respectively, based on the whole device. Three devices connected in series can light a light-emitting diode with a threshold voltage of 2.5 V. Moreover, the device also shows a long cyclic stability and a good bending ability.
An activated carbon derived from tobacco waste for use as a supercapacitor electrode material
CHEN Hui, GUO Yan-chuan, WANG Fu, WANG Gang, QI Pei-rong, GUO Xu-hong, DAI Bin, YU Feng
2017, 32(6): 592-599. doi: 10.1016/S1872-5805(17)60140-9
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A tobacco-derived activated carbon (TAC) was prepared from tobacco waste using KOH activation with a KOH/tobacco carbon mass ratio of 3 at 800℃ for 1 h, and was used as an electrode material for a supercapacitor. The tobacco waste was hydrothermally treated in a 10%(v/v) HCl solution to remove metallic impurities and carbonized before activation. The carbonized tobacco has a low Brunauer-Emmett-Teller (BET) surface area of 111.25 m2·g-1, a pore volume of 0.11 cm3·g-1, an average pore diameter of 1.77 nm and a specific capacitance of 37 F·g-1 at a current density of 0.5 A·g-1. The TAC has a high BET surface area of 1 297.6 m2·g-1, a large pore volume of 0.52 cm3·g-1, and a pore size distribution with a median pore size of 0.52 nm. It has a specific capacitance of 148 F·g-1 at a current density of 0.5 A·g-1 in a 6 M KOH electrolyte, and an excellent cycling stability with no capacitance fade after 9 000 cycles at a current density of 1 A·g-1.
Dendrite-free carbon/lithium metal anodes for use in flexible lithium metal batteries
CHEN Xiao-ru, ZHANG Rui, CHENG Xin-bing, ZHANG Qiang
2017, 32(6): 600-604.
Abstract(549) PDF(816)
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Flexible energy storage devices are of great importance for the rapid growth of flexible electronic devices. Metallic lithium is considered a core anode material in high energy density rechargeable batteries because of its high theoretical specific energy density, the lowest redox potential, and high mechanical flexibility. However, safety issues and a short cycle life induced by lithium dendrites restrict the practical uses of lithium metal batteries. Here we described a nitrogen-doped graphene/lithium metal composite as an anode, in which the Li metal nucleation and growth was guided by doped heteroatoms in the graphene framework. Dendrite-free plating/stripping behavior was detected on the composite anode and its use in flexible lithium-sulfur batteries was validated.

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