Nitrogen-doped graphene nanosheets (NGS) with the nitrogen level as high as 10.13 atom% were synthesized via a simple hydrothermal reaction of graphene oxide (GO) and urea. N-doping and reduction of GO were achieved simultaneously under the hydrothermal reaction. In the fabrication, the nitrogen-enriched urea plays a pivotal role in forming the NGS with a high nitrogen level. During the hydrothermal process, the N-dopant of urea could release NH 3 in a sustained manner, accompanied by the released NH 3 reacting with the oxygen functional groups of the GO and then the nitrogen atoms doped into graphene skeleton, leading to the formation of NGS. The nitrogen level and species could be conveniently controlled by easily tuning the experimental parameters, including the mass ratio between urea and GO and the hydrothermal temperature. Remarkably, in 6 M KOH electrolyte, the synthesized NGS with both high nitrogen (10.13 atom%) and large surface area (593 m 2 g 21 ) exhibits excellent capacitive behaviors (326 F g 21 , 0.2 A g 21 ), superior cycling stability (maintaining initial capacity even) and coulombic efficiency (99.58%) after 2000 cycles. The energy density of 25.02 Wh kg 21 could be achieved at power density of 7980 W kg 21 by a two-electrode symmetric capacitor test. A series of experiments results demonstrated that not only the N-content but also the N-type are very significant for the capacitive behaviors. In more detail, the pyridinic-N and pyrrolic-N play mainly roles for improving pseudo-capacitance by the redox reaction, while quaternary-N could enhance the conductivity of the materials which is favorable to the transport of electrons during the charge/discharge process. Hence, the approach in this work could provide a new way for preparing NGS materials which could be used as advanced electrodes in high performance supercapacitors.
An advanced supercapacitor material based on nitrogen-doped porous graphitic carbon (NPGC) with high a surface area was synthesized by means of a simple coordination-pyrolysis combination process, in which tetraethyl orthosilicate (TEOS), nickel nitrate, and glucose were adopted as porogent, graphitic catalyst precursor, and carbon source, respectively. In addition, melamine was selected as a nitrogen source owing to its nitrogen-enriched structure and the strong interaction between the amine groups and the glucose unit. A low-temperature treatment resulted in the formation of a NPGC precursor by combination of the catalytic precursor, hydrolyzed TEOS, and the melamine-glucose unit. Following pyrolysis and removal of the catalyst and porogent, the NPGC material showed excellent electrical conductivity owing to its high crystallinity, a large Brunauer-Emmett-Teller surface area (SBET =1027 m(2) g(-1) ), and a high nitrogen level (7.72 wt %). The unusual microstructure of NPGC materials could provide electrochemical energy storage. The NPGC material, without the need for any conductive additives, showed excellent capacitive behavior (293 F g(-1) at 1 A g(-1) ), long-term cycling stability, and high coulombic efficiency (>99.9 % over 5000 cycles) in KOH when used as an electrode. Notably, in a two-electrode symmetric supercapacitor, NPGC energy densities as high as 8.1 and 47.5 Wh kg(-1) , at a high power density (10.5 kW kg(-1) ), were achieved in 6 M KOH and 1 M Et4 NBF4 -PC electrolytes, respectively. Thus, the synthesized NPGC material could be a highly promising electrode material for advanced supercapacitors and other conversion devices.
A new ether-based electrolyte to match lithium metal electrode is prepared by introducing 1, 4-dioxane as co-solvent into lithium bis(fluorosulfonyl)imide/1,2-dimethoxyethane solution. Under the synergetic effect of solvents and salt, this simple liquid electrolyte presents stable Li cycling with dendrite-free Li deposition even at relatively high current rate, high coulombic efficiency of ca. 98%, and good anodic stability up to ~4.87 V vs Li RE. Its excellent performance will open up a new possibility for high energy-density rechargeable Li metal battery system.
Porous graphitic carbon nanosheets (PGCS) are synthesized by an in situ self-generating template strategy based on the carburized effect of iron with cornstalks. Cornstalks firstly coordinate with [Fe(CN)(6)](4-) ions to form the cornstalk-[Fe(CN)(6)](4-) precursor. After carbonization and removal of the catalyst, PGCS are obtained. Series experiments indicate that PGCS can only be formed when using an iron-based catalyst that can generate a carburized phase during the pyrolytic process. The unique structures of PGCS exhibit excellent capacitive performance. The PGCS-1-1100 sample (synthesized from 0.1 M [Fe(CN)(6)](4-) with a carbonization temperature of 1100 °C), which shows excellent electrochemical capacitance (up to 213 F g(-1) at 1 A g(-1)), cycling stability, and rate performance in 6 M KOH electrolyte. In the two-electrode symmetric supercapacitors, the maximum energy densities that can be achieved are as high as 9.4 and 61.3 Wh kg(-1) in aqueous and organic electrolytes, respectively. Moreover, high energy densities of 8.3 and 40.6 Wh kg(-1) are achieved at the high power density of 10.5 kW kg(-1) in aqueous and organic electrolytes, respectively. This strategy holds great promise for preparing PGCS from natural resources, including cornstalks, as advanced electrodes in supercapacitors.
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