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1.
The limited potassium-ion intercalation capacity of graphite hampers development of potassium-ion batteries (PIB). Edge-nitrogen doping is an effective approach to enhance K-ion storage in carbonaceous materials. One shortcoming is the lack of precise control over producing the edge-nitrogen configuration. Here, a molecular-scale copolymer pyrolysis strategy is used to precisely control edge-nitrogen doping in carbonaceous materials. This process results in defect-rich, edge-nitrogen doped carbons (ENDC) with a high nitrogen-doping level (up to 10.5 at %) and a high edge-nitrogen ratio (87.6 %). The optimized ENDC exhibits a high reversible capacity of 423 mAh g−1, a high initial Coulombic efficiency of 65 %, superior rate capability, and long cycle life (93.8 % retention after three months). This strategy can be extended to design other edge-heteroatom-rich carbons through pyrolysis of copolymers for efficient storage of various mobile ions.  相似文献   

2.
Although the insertion of potassium ions into graphite has been proven to be realistic, the electrochemical performance of potassium-ion batteries (PIBs) is not yet satisfactory. Therefore, more effort is required to improve the specific capabilities and achieve a long cycling life. The mild carbonization process in molten salt (NaCl-KCl) is used to synthesize nitrogen/oxygen co-doped hierarchically porous carbon (NOPC) for PIBs by using cyanobacteria as the carbon source. This exhibits highly reversible capacities and ultra-long cycling stability, retaining a capacity of 266 mA h g−1 at 50 mA g−1 (100 cycles) and presents a capacity of 104.3 mA h g−1 at 1000 mA g−1 (1000 cycles). Kinetics analysis reveals that the potassium ion (K+) storage of NOPC is controlled by a capacitive process, which plays a crucial role in the excellent rate performance and superior reversible ability. The high proportion of capacitive behavior can be ascribed to the hierarchically porous structure and improved conductivity resulting from nitrogen and oxygen doping. Furthermore, density functional theory (DFT) calculations theoretically validate the enhanced potassium storage effect of the as-obtained NOPC. More importantly, the route to NOPC from cyanobacteria in molten salt provides a green approach to the synthesis of porous carbon materials.  相似文献   

3.
Dual-ion batteries (DIBs) is a promising technology for large-scale energy storage. However, it is still questionable how material structures affect the anion storage behavior. In this paper, we synthesis graphite with an ultra-large interlayer distance and heteroatomic doping to systematically investigate the combined effects on DIBs. The large interlayer distance of 0.51 nm provides more space for anion storage, while the doping of the heteroatoms reduces the energy barriers for anion intercalation and migration and enhances rapid ionic storage at interfaces simultaneously. Based on the synergistic effects, the DIBs composed of carbon cathode and lithium anode afford ultra-high capacity of 240 mAh g−1 at current density of 100 mA g−1. Dual-carbon batteries (DCBs) using the graphite as both of cathode and anode steadily cycle 2400 times at current density of 1 A g−1. Hence, this work provides a reference to the strategy of material designs of DIBs and DCBs.  相似文献   

4.
The limited potassium‐ion intercalation capacity of graphite hampers development of potassium‐ion batteries (PIB). Edge‐nitrogen doping is an effective approach to enhance K‐ion storage in carbonaceous materials. One shortcoming is the lack of precise control over producing the edge‐nitrogen configuration. Here, a molecular‐scale copolymer pyrolysis strategy is used to precisely control edge‐nitrogen doping in carbonaceous materials. This process results in defect‐rich, edge‐nitrogen doped carbons (ENDC) with a high nitrogen‐doping level (up to 10.5 at %) and a high edge‐nitrogen ratio (87.6 %). The optimized ENDC exhibits a high reversible capacity of 423 mAh g?1, a high initial Coulombic efficiency of 65 %, superior rate capability, and long cycle life (93.8 % retention after three months). This strategy can be extended to design other edge‐heteroatom‐rich carbons through pyrolysis of copolymers for efficient storage of various mobile ions.  相似文献   

5.
Although, in the carbon family, graphite is the most thermodynamically stable allotrope, conversion of other carbon allotropes, even amorphous carbons, into graphite is extremely hard. We report a simple electrochemical route for the graphitization of amorphous carbons through cathodic polarization in molten CaCl2 at temperatures of about 1100 K, which generates porous graphite comprising petaloid nanoflakes. This nanostructured graphite allows fast and reversible intercalation/deintercalation of anions, promising a superior cathode material for batteries. In a Pyr14TFSI ionic liquid, it exhibits a specific discharge capacity of 65 and 116 mAh g−1 at a rate of 1800 mA g−1 when charged to 5.0 and 5.25 V vs. Li/Li+, respectively. The capacity remains fairly stable during cycling and decreases by only about 8 % when the charge/discharge rate is increased to 10000 mA g−1 during cycling between 2.25 and 5.0 V.  相似文献   

6.
Quick capacity loss due to the polysulfide shuttle effects and poor rate performance caused by low conductivity of sulfur have always been obstacles to the commercial application of lithium sulfur batteries. Herein, an in-situ doped hierarchical porous biochar materials with high electron-ion conductivity and adjustable three-dimensional (3D) macro-meso-micropore is prepared successfully. Due to its unique physical structure, the resulting material has a specific surface area of 2124.9 m2 g−1 and a cumulative pore volume of 1.19 cm3 g−1. The presence of micropores can effectively physically adsorb polysulfides and mesopores ensure the accessibility of lithium ions and active sites and give the porous carbon material a high specific surface area. The large pores provide channels for the storage of electrolyte and the transmission of ions on the surface of the substrate. The combined effect of these three kinds of pores and the N doping formed in-situ can effectively promote the cycle and rate performance of the battery. Therefore, prepared cathode can still reach a reversible discharge capacity of 616 mAh g−1 at a rate of 5 C. After 400 charge–discharge cycles at 1 C, the reversible capacity is maintained at 510.0 mAh g−1. This new strategy has provided a new approach to the research and industrial-scale production of adjustable hierarchical porous biochar materials.  相似文献   

7.
Poor cyclability and rate performance always impede the development of transition metal phosphide-based anode materials. Many strategies have been used to address the above problems, such as the designing of hierarchical structures, combination with carbon materials, and doping with other metal elements. Considering those strategies, a flower-like Fe-doped CoP material is designed. The synthesis consists of microsheets grown on a carbon membrane (CM, leaves as precursor) through a hydrothermal method and in situ phosphorization. The Fe doping and carbon membrane synergistically induce the formation of a flower-like hierarchical microstructure during the crystal-growing process. The unique hierarchical microstructure increases the contact area between electrode and electrolyte, and accommodates the volume expansion during cycling. The hierarchical Fe-doped CoP grown directly on the carbon membrane increases the active sites for intercalation of sodium species and further promotes the internal electron conduction in the Fe-doped CoP/CM electrode. Thereby, the Fe-doped CoP/CM as the anode electrode for sodium ion batteries exhibits a high specific capacity of 515 mA h g−1 at 100 mA g−1 after 100 cycles. Even if the current density rises to 500 mA g−1, the specific capacity is still maintained at 324 mA h g−1 after 500 cycles, showing superior rate performances and cyclability.  相似文献   

8.
Surface oxygen functionalities (particularly C−O configuration) in carbon materials have negative influence on their electrical conductivity and Na+ storage performance. Herein, we propose a concept from surface chemistry to regulate the oxygen configuration in hierarchically porous carbon nanosheets (HPCNS). It is demonstrated that the C−O/C=O ratio in HPCNS reduces from 1.49 to 0.43 and its graphitization degree increases by increasing the carbonization temperature under a reduction atmosphere. Remarkably, such high graphitization degree and low C−O content of the HPCNS-800 are favorable for promoting its electron/ion transfer kinetics, thus endowing it with high-rate (323.6 mAh g−1 at 0.05 A g−1 and 138.5 mAh g−1 at 20.0 A g−1) and durable (96 % capacity retention over 5700 cycles at 10.0 A g−1) Na+ storage performance. This work permits the optimization of heteroatom configurations in carbon for superior Na+ storage.  相似文献   

9.
SeS2 shows attractive advantages beyond bare S and Se as a cathode material for lithium storage. Here, a freestanding lotus root‐like carbon fiber network decorated with CoS2 nanoparticles (denoted as CoS2@LRC) has been designed and prepared as the SeS2 host for enhancing the lithium storage performance. The integrated electrode is constructed by three‐dimensional interconnected multichannel carbon fibers, which can not only accommodate high content of SeS2 (70 wt %), but also promise excellent electron and ion transport for achieving high capacity utilization of 1015 mAh g−1 at 0.2 A g−1. What is more, there are numerous CoS2 nanoparticles decorated all over the inner walls and surfaces of the carbon fibers, providing efficient sulfiphilic sites for restricting the dissolution of polysulfides and polyselenides during the electrochemical processes, thus successfully suppressing the shuttle effect and maintaining excellent cycling stability over 400 cycles at 0.5 A g−1.  相似文献   

10.
Porous carbon with high specific surface area (SSA), a reasonable pore size distribution, and modified surface chemistry is highly desirable for application in energy storage devices. Herein, we report the synthesis of nitrogen‐containing mesoporous carbon with high SSA (1390 m2 g?1), a suitable pore size distribution (1.5–8.1 nm), and a nitrogen content of 4.7 wt % through a facile one‐step self‐assembly process. Owing to its unique physical characteristics and nitrogen doping, this material demonstrates great promise for application in both supercapacitors and encapsulating sulfur as a superior cathode material for lithium–sulfur batteries. When deployed as a supercapacitor electrode, it exhibited a high specific capacitance of 238.4 F g?1 at 1 A g?1 and an excellent rate capability (180 F g?1, 10 A g?1). Furthermore, when an NMC/S electrode was evaluated as the cathode material for lithium–sulfur batteries, it showed a high initial discharge capacity of 1143.6 mA h g?1 at 837.5 mA g?1 and an extraordinary cycling stability with 70.3 % capacity retention after 100 cycles.  相似文献   

11.
The current study discusses application of the lanthanum ions (La3+) as an activating agent incorporated /immobilized into coconut shell–based granular activated carbon (GAC) for porosity development; subsequently, the carbon material is used for the adsorption of phenol from aqueous solutions. The new carbons were characterized using FTIR, XRD, CHNO, burn off, and carbon yield. The surface functional groups were determined by Boehm titration. The Brunauer–Emmett–Teller (BET) surface area of the carbons is 953 m2 g−1 (GACLa1073), 997 m2 g−1 (GAC383), and 973 m2 g−1 (GACO383). Langmuir, Freundlich, Dubinin–Radushkevich, and John–Sivanandan Achari (J-SA) isotherm models on the equilibrium isotherm data were examined for the new carbon-phenol system. It is found that the Langmuir isotherm fits better with a monolayer adsorption capacity, highest for GACLa1073 (387.59 mg g−1) followed by GAC383 (303.03 mg g−1) and GACO383 (197.62 mg g−1). Kinetic studies reveal that the adsorption system follows the pseudo–second-order kinetic model. Isotherm analysis by the phase change method of John-Sivanandan Achari (J-SA) isotherm gives a better insight into adsorption phenomena, which is accompanied by regeneration studies of carbon with >75% for GACLa1073 after three cycles.  相似文献   

12.
Inspired by the spongy bone structures, three-dimensional (3D) sponge-like carbons with meso-microporous structures are synthesized through one-step electro-reduction of CO2 in molten carbonate Li2CO3−Na2CO3−K2CO3 at 580 °C. SPC4-0.5 (spongy porous carbon obtained by electrolysis of CO2 at 4 A for 0.5 h) is synthesized with the current efficiency of 96.9 %. SPC4-0.5 possesses large electrolyte ion accessible surface area, excellent wettability and electronical conductivity, ensuring the fast and effective mass and charge transfer, which make it an advcanced supercapacitor electrode material. SPC4-0.5 exhibits a specific capacitance as high as 373.7 F g−1 at 0.5 A g−1, excellent cycling stability (retaining 95.9 % of the initial capacitance after 10000 cycles at 10 A g−1), as well as high energy density. The applications of SPC4-0.5 in quasi-solid-state symmetric supercapacitor and all-solid-state flexible devices for energy storage and wearable piezoelectric sensor are investigated. Both devices show considerable capacitive performances. This work not only presents a controllable and facile synthetic route for the porous carbons but also provides a promising way for effective carbon reduction and green energy production.  相似文献   

13.
Mesoporous carbons (MCs) were used as the matrixes to load sulfur for lithium sulfur (Li-S) batteries, and pore sizes were tuned by heat treatment at different high temperatures. The cathode material shows the highest discharge capacity of 1158.2 mAh g?1 at the pore size of 4.1 nm among as-prepared nitrogen-free materials with different sizes. Meanwhile, the nitrogen doping of mesoporous carbon helps to inhibit the diffusion of polysulfide species via an enhanced surface adsorption. The carbon/sulfur containing N (4.56%) shows a high initial discharge capacity of 1315.8 mAh g?1 and retains about 939 mAh g?1 after 100 cycles at 0.2 C. The improved electrochemical performance is ascribed to the proper pore size, surface chemical property, and conductivity of the N-doped carbon material.  相似文献   

14.
Paper cup composed of crude cellulose is a common waste in daily life. In this paper, hierarchical porous carbons have been successfully prepared by an initial hydrothermal treatment and subsequent activation route from abandoned paper cup, and then paper cup derived carbons are used as scaffolds to fabricate serial carbon/Se composites. The optimal composite presents unique 3D porous structure, with amorphous selenium uniformly confined into the micropores of carbon. As the cathode materials of Li-Se battery, this composite reveals an initial reversible discharge capacity of 517.2 mAh g−1 at 0.2C, and a capacity value of 431.9 mAh g−1 can be retained after 60 cycles. Even at a high rate of 4C, a capacity value of 295.8 mAh g−1 can be obtained. By comparison, the improved electrochemical performance of the optimal composite should be attributed to reasonable porous structure and effective encapsulation of amorphous selenium.  相似文献   

15.
To investigate the effects of oxygen-containing functional groups on the adsorption of volatile organic compounds (VOCs) with different polarity, oxygen-rich porous carbon materials (OPCs) were synthesized by heat treatment of glucose/potassium oxalate material. The carbon material had a large specific surface area (1697 m2 g−1) and a high oxygen content (18.95 at.%). OPC exhibited high adsorption capacity of toluene (309 mg g−1) and methanol (447 mg g−1). The specific surface area and total pore volume determined the adsorption capacity of toluene and methanol at the high-pressure range, while the oxygen-containing groups became the main factor affecting the methanol adsorption at the low-pressure range due to the hydrogen bond interaction through the density functional theory (DFT) calculations. This study provides an important hint for developing a novel O-doped adsorbent for the VOCs adsorption applications and analyzing the role of oxygen-containing groups in the VOCs adsorption under the low-pressure range.  相似文献   

16.
In this work, we proposed a facile one-pot pyrolysis method to conveniently manufacture lignin-derived carbon materials with graded porous construction for use in supercapacitors. The renewable lignin was selected as precursor, while the potassium citrate was used as a pore-forming agent. The properties of the prepared lignin-derived carbon (LAC) and the performance for supercapacitor application were thoroughly evaluated. The LAC at optimal preparation conditions shows a layered porous structure with a large specific surface area of 3174 cm2 g−1 and pore volume of 2.796 cm3 g−1, where the specific capacitance reach to 241 F g−1 at 1 A g−1 scan rate in 6 M KOH electrolyte solution. At the same time, the specific capacitance remains at 220 F g−1 even at an excessive scan velocity of 20 A g−1, while the capacitance retention is still close to 91.3%. The capacitance retention rate is stable above 95% after 10,000 charge/discharge cycles, which shows the desired long-time stability. All these results demonstrate the outstanding properties of the new prepared LAC material and the considerable application potential in the field of electrical energy storage.  相似文献   

17.
Lithium-sulfur batteries are promising secondary energy storage devices that are mainly limited by its unsatisfactory cyclability owing to inefficient reversible conversion of sulfur and lithium sulfide on the cathode during the discharge/charging process. In this study, nitrogen-doped three-dimensional porous carbon material loaded with CoSe2 nanoparticles (CoSe2-PNC) is developed as a cathode for lithium-sulfur battery. A combination of CoSe2 and nitrogen-doped porous carbon can efficiently improve the cathode activity and its conductivity, resulting in enhanced redox kinetics of the charge/discharge process. The obtained electrode exhibits a high discharge specific capacity of 1139.6 mAh g−1 at a current density of 0.2 C. After 100 cycles, its capacity remained at 865.7 mAh g−1 thus corresponding to a capacity retention of 75.97 %. In a long-term cycling test, discharge specific capacity of 546.7 mAh g−1 was observed after 300 cycles performed at a current density of 1 C.  相似文献   

18.
Sb-based materials have attracted much attention owing to their ability to undergo a multi-electron alloy reaction with K+. However, there are still the serious problems of volume change and aggregation of particles, which lead to rapid capacity fading and a limited lifespan. In this work, a graphene/amorphous carbon restriction structure is proposed, in which the amorphous carbon layer on the surface of Sb nanoparticles can protect the particles from pulverization, and the graphene can buffer the volume change of the material. In addition, the conductive network formed by the dual carbon structure effectively improves the rate performance of the material. Thus, the material delivers a high capacity of 550 mA h g−1 at 100 mA g−1, a rate capability of 370 mA h g−1 at 2000 mA g−1, and a long lifespan of 350 cycles without significant capacity fading. The dual carbon strategy proposed offers a reference for the design of high-performance anode materials.  相似文献   

19.
Sodium- and potassium-ion batteries have attracted intensive attention recently as low-cost alternatives to lithium-ion batteries with naturally abundant resources. However, the large ionic radii of Na+ and K+ render their slow mobility, leading to sluggish diffusion in host materials. Herein, hierarchical FeSe2 microspheres assembled by closely packed nano/microrods are rationally designed and synthesized through a facile solvothermal method. Without carbonaceous material incorporation, the electrode delivers a reversible Na+ storage capacity of 559 mA h g−1 at a current rate of 0.1 A g−1 and a remarkable rate performance with a capacity of 525 mA h g−1 at 20 A g−1. As for K+ storage, the FeSe2 anode delivers a high reversible capacity of 393 mA h g−1 at 0.4 A g−1. Even at a high current rate of 5 A g−1, a discharge capacity of 322 mA h g−1 can be achieved, which is among the best high-rate anodes for K+ storage. The excellent electrochemical performance can be attributed to the favorable morphological structure and the use of an ether-based electrolyte during cycling. Moreover, quantitative study suggests a strong pseudocapacitive contribution, which boosts fast kinetics and interfacial storage.  相似文献   

20.
Utilizing cost-effective raw materials to prepare high-performance silicon-based anode materials for lithium-ion batteries (LIBs) is both challenging and attractive. Herein, a porous SiFe@C (pSiFe@C) composite derived from low-cost ferrosilicon is prepared via a scalable three-step procedure, including ball milling, partial etching, and carbon layer coating. The pSiFe@C material integrates the advantages of the mesoporous structure, the partially retained FeSi2 conductive phase, and a uniform carbon layer (12–16 nm), which can substantially alleviate the huge volume expansion effect in the repeated lithium-ion insertion/extraction processes, effectively stabilizing the solid–electrolyte interphase (SEI) film and markedly enhancing the overall electronic conductivity of the material. Benefiting from the rational structure, the obtained pSiFe@C hybrid material delivers a reversible capacity of 1162.1 mAh g−1 after 200 cycles at 500 mA g−1, with a higher initial coulombic efficiency of 82.30 %. In addition, it shows large discharge capacities of 803.1 and 600.0 mAh g−1 after 500 cycles at 2 and 4 A g−1, respectively, manifesting an excellent electrochemical lithium storage. This work provides a good prospect for the commercial production of silicon-based anode materials for LIBs with a high lithium-storage capacity.  相似文献   

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