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A novel integrated gas diffusion layer based on one-dimensional carbon materials and its application to direct methanol fuel cells
SHU Qing-zhu, XIA Zhang-xun, WEI Wei, XU Xin-long, WANG Su-li, ZHAO Hong, SUN Gong-quan
 doi: 10.1016/S1872-5805(21)60017-3
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The gas diffusion layer (GDL) is an important component of the membrane electrode assembly (MEA) of fuel cells (FCs), which plays a key role in supporting the catalyst layer, collecting current, and transferring and redistributing materials. A conventional GDL consists of a backing layer (BL), typically made of commercial carbon paper or carbon cloth, but it still suffers from some challenges in terms of its high cost, narrow pore-size distribution, lack of flexibility, and poor conductivity. In that case, a micro-porous layer (MPL) is necessary for better gas/liquid management. In this study, a novel, flexible, integrated gas diffusion layer (GDL/CNT-CF) is successfully prepared through vacuum filtration by combining carbon fibres (CFs) with highly-dispersed multi-walled carbon nanotubes (MWCNTs) and polytetrafluoroethylene (PTFE) as a binder and water repellent. Scanning electron microscopy (SEM) combined with characterisation of conductivity, gas permeability, and porosity indicates that the highly-conductive MWCNTs in the GDL/CNT-CF are distributed in gradients in the CF networks, and can facilitate electron transport. Furthermore, the formed multi-level pore structure is beneficial to material distribution and the uniform distribution of PTFE contributes to improved water discharge. Therefore, it replaces the conventional diffusion layer consisting of carbon paper and MPL. When the GDL/CNT-CF is applied as the cathode, or both the cathode and anode, of a direct methanol fuel cell (DMFC), the maximum power density of the single cells is separately increased by 20% and 35% compared with that of a commercial GDL due to its excellent mass transfer performance.
Coal-based graphene as a promoter of TiO2 for photocatalytic degradation of rhodamine B and methyl orange
LIU Guo-yang, LI Ke-ke, JIA Jia, ZHANG Ya-ting
 doi: 10.1016/S1872-5805(21)60018-5
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A reduced graphene oxide (H-rGO)/TiO2–composite as a catalyst for photocatalytic degradation of rhodamine B (Rh B) and methyl orange (MO) was prepared by hydrothermal treating a dispersant of TiO2 nanoparticles with sizes of 5-10 nm and GO obtained by the Hummers method from coal-based graphite in water, which was compared with the M-rGO/TiO2 and GO/TiO2 composites by a wet mixing method. Results indicated that the TiO2 nanoparticles in H-TiO2@rGO were uniformly decorated on both sides of rGO sheet, forming a stacked-sheet structure while apparent aggregation of TiO2 nanoparticles was found for both M-rGO/TiO2 and GO/TiO2. H-rGO/TiO2 had the highest catalytic activity for degradation of Rh B and MO under visible light irradiation among the three, where incorporating rGO into TiO2 narrowed the band gap of TiO2, inhibited the recombination rate of electron–hole pairs and provided conductive networks for electron transfer.
A sustainable strategy to prepare porous carbons with tailored pores from shrimp shell for use as the supercapacitor electrode materials
Gao Feng, Xie Ya-qiao, Zang Yun-hao, ZHOU Gang, QU Jiang-ying, WU Ming-bo
 doi: 10.1016/S1872-5805(21)60019-7
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Highly efficient synthesis of nitrogen-doped carbons with different porous structures is reported using shrimp shell as the carbon and nitrogen source, and its CaCO3 component as the hard template and the activator. The content of CaCO3 in shrimp shell can be tuned easily in the range of 0-100% by leaching with an acetic acid solution for different times. CaO derived from decomposition of CaCO3 acts as the activator and template to tailor the pore sizes of the carbons. CO2 derived from decomposition of CaCO3 also plays an activating role. Their specific surface areas, pore volumes, ratios of micropore volumes to total pore volumes can be adjusted in the range of 117.6-1137 m2 g-1, 0.14-0.64 cm3 g-1, and 0-73.4%, respectively. When used as the electrodes of supercapacitor, the porous carbon obtained with a leaching time of 92 min exhibits the highest capacitances of 328 F g-1 at 0.05 A g-1 in a 6 M KOH electrolyte and 619.2 F g-1 at 0.05 A g-1 in a 1 M H2SO4 electrolyte. Its corresponding energy density at a power density of 1470.9 W kg-1 is 26.0 Wh kg-1. This work provides a low cost method for fabricating porous carbons to fulfill the high-value-added use of biomass.
Regulating the radial structure during pre-oxidation of polyacrylonitrile fibers and its effect on the mechanical properties of carbon fibers
WANG Yun-Feng, WANG Yi-Wei, XU Liang-Hua, WANG Yu
 doi: 10.1016/S1872-5805(20)60516-9
Abstract(27) HTML(5) PDF(2)
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The radial structure of pre-oxidized fibers and its distribution directly affect the performance of the resulting carbon fibers. Optimizing the radial distribution of pre-oxidized structure and establishing the relationship between the pre-oxidized structure of polyacrylonitrile fibers and the mechanical properties of the final carbon fibers will help to optimize the pre-oxidation conditions in the preparation of high-performance carbon fibers. Herein, solid-state nuclear magnetic resonance spectroscopy, optical microscopy, thermogravimetric analysis, and mechanical tests were used to investigate the effect of the pre-oxidation reaction rate on the radial structural distribution of pre-oxidized fibers and the mechanical properties of the resulting carbon fibers. The pre-oxidation reaction rates were controlled by regulating the pre-oxidation temperature gradient. The results showed that the pre-oxidation degree of pre-oxidized fibers increased with both the overall and initial rates of pre-oxidation. With increasing the overall pre-oxidation reaction rate, the pre-oxidized structure was deepened into the core region of the fibers, the content of oxygen-containing functional groups increased, the thermal stability of the fibers decreased, the graphitization degree of the corresponding carbon fibers increased, but the density of the carbon fibers decreased and the mechanical properties of the carbon fibers were degraded. With increasing the initial reaction rate of pre-oxidation, the radial distribution of the pre-oxidation structure was effectively improved, the content of oxygen-containing functional groups of the pre-oxidized fibers increased slightly, their thermal stability was improved, the degree of graphitization and density of the final carbon fibers increased, and the tensile strength and tensile modulus of the final carbon fibers were markedly increased. A new type of carbon fibers with high strength, medium modulus and a relatively large diameter was obtained under the optimized pre-oxidation conditions.
Application of graphene and its composites to suppress the shuttle effect in lithium-sulfur batteries: A review
LI Li-bo, SHAN Yu-hang
 doi: 10.19869/j.ncm.1007-8827.20200153
Abstract(39) HTML(14) PDF(10)
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Lithium sulfur battery has the advantages of high theoretical energy of 1675 mAh g-1, low price and environmental friendliness, which make it a very promising secondary battery. However, its cycling stability cannot meet the requirements of the industrialization due to the shuttle effect caused by the dissolution of polysulfides in the discharge process, the sulfur insulation and the volume expansion of the sulfur electrode. Graphene has excellent electrical conductivity, extremely large specific surface area, good mechanical flexibility, and thermal and chemical stability, so graphene and its derivatives are promising candidates to modify both the electrodes of the all-solid-state lithium-sulfur batteries and the separator. Herein, the mechanisms by which graphene and its derivatives inhibit the shuttle effect have been summarized. The graphene network is very favorable for the electron transfer, limiting volume expansion of sulfur electrodes and facilitating ion migration in all-solid-state lithium-sulfur batteries. As the modifiers of the separator, the hexagonal and layered structure of graphene and its derivates form the lithium ion transport channel and capture sulfur. The development strategy using graphene and its derivatives in lithium-sulfur batteries are proposed.
Micro/mesopore carbon spheres derived from sucrose for high performance supercapacitors
SHI Jing, TIAN Xiao-dong, LI Xiao, LIU Ye-qun, SUN Hai-zhen
 doi: 10.1016/S1872-5805(21)60021-5
Abstract(13) HTML(7) PDF(1)
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Micro/mesopore carbon spheres as electrode materials of supercapacitors were prepared by hydrothermal carbonization followed by KOH/NaOH activation using sucrose as the carbon precursor. The effects of KOH and NaOH activation parameters on the specific surface area, pore size distribution and electrochemical performance of the carbon spheres were investigated. Results indicate that the use of NaOH leads to the development of mesopores while the use of KOH is favorable to increase specific surface area and micropore volume. The pore size distribution of carbon spheres could be adjusted by varying the fraction of NaOH in the activation agent. A balanced capacitance and rate performance of the supercapacitor electrode in both 6 M KOH aqueous electrolyte and 1 M MeEt3NBF4/PC electrolyte is achieved when the carbonized product is activated at a mass ratio of NaOH+KOH/ carbonized product of 3∶1 with a NaOH/KOH mass ratio of 2∶1. As-prepared porous carbon delivers a capacitance of 235 F/g at 0.1 A/g and capacitance retention rate of 81.5% at 20 A/g in the 6 M KOH aqueous electrolyte. In 1 M MeEt3NBF4/PC, the cell based on the porous carbon delivers the highest energy and power output of 30.4 Wh kg-1 and 18.5 kW kg-1, respectively.
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Preface
2021, 36(1): 1-2.  
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Contents in Chinese
2021, (1): 1-1.  
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Graphical Contents
2021, 36(1): 1-7.  
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Reviews
A review of covalent organic framework electrode materials for rechargeable metal-ion batteries
ZENG Shu-mao, HUANG Xiao-xiong, MA Ying-jie, ZHI Lin-jie
2021, 36(1): 1-18.   doi: 10.1016/S1872-5805(21)60001-X
Abstract(147) HTML(52) PDF(44)
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Covalent organic frameworks (COFs) are highly promising electrode materials for next-generation rechargeable metal-ion batteries owing to their robust framework, abundant electrochemically active sites, well-defined and tunable pores and channels for metal ion transfer, and adjustable molecular structures for improving electrochemical performance. Moreover, COFs do not have the problems caused by expensive or toxic elements in conventional inorganic electrode materials or the cycling stability challenges existing in small organic molecules, and thus have great potential as electrode materials in next-generation rechargeable metal-ion batteries. We summarize the electrochemically active sites of these materials for charge storage, and most importantly, we focus on strategies for improving their electrochemical performance, including energy density, rate performance and cycling life by changing their frameworks, pores, active sites, and electronic structures. To fabricate high performance COF electrodes, much more effort is needed to improve their ionic and electronic conductivities, increase their operating voltage, and reveal their mechanisms of energy storage. This review may shed light on developing high performance COF electrode materials for next-generation rechargeable metal-ion batteries.
Recent advances in multilevel nickel-nitrogen-carbon catalysts for CO2 electroreduction to CO
ZHANG Ya-fang, YU Chang, TAN Xin-yi, CUI Song, LI Wen-bin, QIU Jie-shan
2021, 36(1): 19-33.   doi: 10.1016/S1872-5805(21)60002-1
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As an emerging CO2 conversion technology, the electrochemical CO2 reduction (ECR) reaction has received widespread attention. For the ECR process, the accurate and rational design of electrocatalysts is essential and significant for improving the catalytic performance. Carbon-based materials are considered one of the promising electrocatalysts for ECR because of their variety of abundant sources, high specific surface area, high porosity, and multilevel dimensionality and tunable active sites. Furthermore, doping by heteroatoms and introducing metal atoms in the frameworks or substrates of the carbon materials are effective strategies for further improving the ECR activity. Particularly, nickel-nitrogen-carbon (Ni-N-C) materials show excellent reactivities for the ECR to CO and have the potential for large-scale applications. We summarize the recent development of Ni-N-C catalysts with a multilevel structure for the ECR to CO and also the key principles and primary parameters of the ECR. Furthermore, the rational and precise design of multilevel Ni-N-C catalysts on different carbon frameworks or substrates is discussed and presented, especially including carbon quantum dots, one dimensional (1D) carbon-based materials, two dimensional (2D) carbon-based materials and nanoporous carbon-based materials. The effects of microstructure on ECR performance are also analyzed. Finally, the challenges and outlook for Ni-N-C catalysts in an ECR system are presented. This review provides some new insights and guidelines for rationally designing and preparing Ni-N-C catalysts with a multilevel structure and high performance.
A review of the synthesis of carbon materials for energy storage from biomass and coal/heavy oil waste
GAO Feng, ZANG Yun-hao, WANG Yan, GUAN Chun-qian, QU Jiang-ying, WU Ming-bo
2021, 36(1): 34-48.   doi: 10.1016/S1872-5805(21)60003-3
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Recent progress in the synthesis of carbon materials from biomass and coal/heavy oil waste and their use as the electrode materials of supercapacitors and Li-ion batteries is reviewed. The carbon precursors include seafood and agricultural waste, and coal and heavy oil by-products. The carbon materials include 0D carbon quantum dots, 1D carbon nanofibers, 2D carbon nanosheets, and 3D carbon frameworks. Techniques to tailor the carbon porosity/surface include KOH activation with and without self-templating, self-activation and/or in-situ templating, and heteroatom doping with N, O, P and their co-doping. The effects of porosity and heteroatom doping on the electrochemical performance are summarized. The challenges for the synthesis, microstructural tailoring of these materials and their potential use in supercapacitors and Li-ion batteries are analyzed.
A review of charge storage in porous carbon-based supercapacitors
LUO Xian-you, CHEN Yong, MO Yan
2021, 36(1): 49-68.   doi: 10.1016/S1872-5805(21)60004-5
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Porous carbon-based electrode materials have been widely used in supercapacitors (SCs) because of their good physicochemical stability, high specific surface area, adjustable pore structure, and excellent electrical conductivity. The factors influencing their SC performance are analyzed, which include specific surface area, pore structure, surface heteroatoms, structural defects and electrode structure. The high surface area accessible to ions provides abundant active sites for their storage, while a suitable pore structure is important for the accommodation and diffusion of ions, thereby influencing the specific capacitance and rate performance of the electrodes. An appropriate pore size with a narrow distribution is required to increase the volumetric energy density while mesopores are favorable for ion transport, so a good balance between micro and mesopore volumes is important to improve both the energy and power densities of the SCs. Structural defects, surface heteroatoms and a rational electrode structural design all play significant roles in the capacitance performance.
A review of porous carbons produced by template methods for supercapacitor applications
ZHANG Wei, CHENG Rong-rong, BI Hong-hui, LU Yao-hui, MA Lian-bo, HE Xiao-jun
2021, 36(1): 69-81.   doi: 10.1016/S1872-5805(21)60005-7
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Porous carbons are widely used in the energy storage and conversion field because of their excellent electrical conductivity, high specific surface area and superb electrochemical stability. The template method is one of the most advanced approaches to prepare porous carbons with well-defined pore structures and suitable pore size distributions. The pore formation mechanism and structure-property relationships of porous carbons obtained by template methods for supercapacitor electrodes are summarized. They include hard templates (magnesium-based, silica-based, zinc-based, calcium-based templates), soft templates (conventional soft template, ionic liquids, deep eutectic solvent) and self-templates (biomass, MOFs). Furthermore, the problems in tailoring the pore texture of porous carbons are clarified, and proposals are made for future research.
Applications of nanocarbons in redox flow batteries
ZHANG Feng-jie, ZHANG Hai-tao
2021, 36(1): 82-92.   doi: 10.1016/S1872-5805(21)60006-9
Abstract(56) HTML(23) PDF(14)
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Redox flow batteries (RFBs), regarded as the most effective grid-scale electrochemical energy storage technology, are attracting wide attention because of the problems of the energy crisis and environmental pollution. Charge transport properties are critical factors related to the electrochemical performance of energy storage devices. Nanocarbons, which have special morphologies and many physicochemical properties, such as high ionic conductivity, high thermal conductivity and excellent mechanical properties, can play an indispensable role in electrochemical energy storage. Adjusting the microstructure of carbon materials is an effective strategy to improve their electron and ion transport behavior. In this work, the functions of nanocarbons in RFBs are reviewed, especially focusing on the modification and design of nanocarbons used in the electrodes, suspended electrodes in semi-solid RFBs, and bipolar plates (collectors) used to improve the energy efficiency, power density and the stability of high-performance RFBs. A more systematic and comprehensive understanding of the role that nanocarbons play in RFBs could provide a new perspective for the design of high-performance RFB electrodes.
The use of in-situ Raman spectroscopy in investigating carbon materials as anodes of alkali metal-ion batteries
CHENG Xiao-qin, LI Hui-jun, ZHAO Zhen-xin, WANG Yong-zhen, WANG Xiao-min
2021, 36(1): 93-105.   doi: 10.1016/S1872-5805(21)60007-0
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Raman spectroscopy is a fast, non-destructive and high-resolution characterization tool based on laser physics that can be applied to a wide range of materials science problems. It has proven to be an effective tool in studying phase transitions induced by variables such as temperature, pressure or electrochemical reactions. In-situ Raman spectroscopy can be used to track any microstructural changes of the electrode materials and interface reactions in alkali metal-ion batteries during charging and discharging. Carbon materials have become the most widely used anode materials for lithium-ion batteries because of their good electrochemical reversibility, excellent stability, low electrochemical charge/discharge potential platform, and low cost. The use of in-situ Raman spectroscopy in understanding the reactions occurring in alkali metal-ion batteries using carbon anode materials is summarized with a focus on the energy storage mechanism in Li+/Na+/K+ ion batteries using carbon materials such as graphite and hard carbon as the anode materials. The effects of size, stress, doping, and the solvation-assisted co-intercalation of Li+/Na+/K+ ions on the energy storage behavior in alkali metal-ion batteries are analyzed. Based on the strength and weakness of in-situ Raman spectroscopy, its combination with AFM, in situ XRD and other high-resolution in situ technologies is used to reveal the energy storage mechanisms.
Recent progress in the carbon-based frameworks for high specific capacity anodes/cathode in lithium/sodium ion batteries
LI Xu, WANG Xiao-yi, SUN Jie
2021, 36(1): 106-116.   doi: 10.1016/S1872-5805(21)60008-2
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Secondary-ion batteries, such as lithium-ion (LIBs) and sodium-ion batteries (SIBs), have become a hot research topic owing to their high safety and long cycling life. The electrode materials for LIB/SIBs need to be further developed to achieve high energy and power densities. Anode/cathode active materials based on their alloying/dealloying with lithium, such as the anode materials of silicon, phosphorus, germanium and tin, and the cathode material of sulfur, have a high specific capacity. However, their large volume changes during charging/discharging, the insulating nature of phosphorus and sulfur, as well as the shuttling of polysulfides in a battery with a sulfur cathode decrease their specific capacity and cycling performance. The formation of dendrites in anodes during the deposition/dissolution of Li and Na leads to severe safety issue and hinders their practical use. Carbon materials produced from abundant natural resources have a variety of structures and excellent conductivity making them suitable host frameworks for loading high specific capacity anode/cathode materials. Recent progress in this area is reviewed with a focus on the factors affecting their electrochemical performance as the hosts of active materials. It is found that the mass loading of the active materials and the energy density of the batteries can be enhanced by increasing the specific surface area and pore volume of the carbon frameworks. Large volume changes can be efficiently accommodated using high pore volume carbon frameworks and a moderate loading of the active material. Suppression of the shuttling of polysulfides and therefore a long cycling life can be achieved by increasing the number of binding sites and their binding affinity with polysulfides by surface modification of the carbon frameworks. Dendrite growth can be inhibited by a combination of a high specific surface area and appropriate interface modification. Rate performance can be improved by designing the pore structure to shorten Li+/Na+ diffusion paths and increasing the electrical conductivity of the carbon frameworks. DFT calculations and simulations can be used to design the structures of carbon frameworks and predict their electrochemical performance.
A review of metal-organic framework-derived carbon electrode materials for capacitive deionization
WENG Jia-ze, WANG Shi-yong, ZHANG Pei-xin, LI Chang-ping, WANG Gang
2021, 36(1): 117-132.   doi: 10.1016/S1872-5805(21)60009-4
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Capacitive deionization (CDI), in which electrode materials play an important role, is considered a novel desalination technology because of its advantages of low energy consumption, low cost and low pollution. Porous electrode materials with a high accessible surface area, hydrophilic surfaces and excellent electrochemical performance have proved to be ideal. Carbons derived from metal-organic frameworks (MOFs) are most suitable for this purpose because of their controllable morphology and microstructure, suitable pore size distribution, and excellent electrical conductivity. The preparation and of MOF-derived carbon materials and their performance for the use as CDI electrode materials are reviewed. These include MOF-derived carbons, modified MOF-derived carbons, doped MOF-derived carbons and MOF-derived carbon composites with graphene, carbon nanofibers and carbon nanotubes. The advantages and challenges of these carbon electrode materials for CDI are summarized and future development is proposed.
Coal-derived carbon nanomaterials for sustainable energy storage applications
LI Ke-ke, LIU Guo-yang, ZHENG Li-si, JIA Jia, ZHU You-yu, ZHANG Ya-ting
2021, 36(1): 133-154.   doi: 10.1016/S1872-5805(21)60010-0
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As a natural abundant high-carbon resource, the use of coal to develop carbon nanomaterials is an important research topic. In recent years, a variety of carbon materials with different morphologies and nanotextures have been designed and constructed using coal and their derivatives as precursors, and their use in energy storage, catalysis, adsorption and absorption have been explored. State-of-the-art research on carbon nanomaterials derived from coals of different rank and their derivatives are summarized with specific attention to the synthesis strategies and structure control. The use of these coal-derived carbons for energy storage, such as secondary batteries and supercapacitors, is also discussed in terms of their structural features. The review aims to provide valuable insight into the present challenges and inspire new ideas for the development of advanced coal-derived carbon materials.
A review of carbon-based cathode materials for zinc-ion capacitors
WANG Man, CHE Xiao-gang, LIU Si-yu, YANG Juan
2021, 36(1): 155-166.   doi: 10.19869/j.ncm.1007-8827.20200264
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Zinc-ion capacitors are high-performance hybrid capacitors that have great advantages because of the abundance of zinc resources and their high theoretical capacitance. As a result they have become a hot research topic in the field of energy storage devices. Carbon-based materials are usually used as the cathode materials for these capacitors because of the wide range of available materials, and their easily tuned surface properties and simple fabrication. This review summarizes recent research progress on carbon cathode materials for flexible/non-flexible zinc ion capacitors, and gives a concise description of their novel structures and outstanding performance. It then discusses research on the energy storage mechanisms in the cathode materials and suggests directions for the development of carbon cathodes for zinc-ion capacitors.
Research articles
Salt-assisted in-situ formation of N-doped porous carbons for boosting K+ storage capacity and cycling stability
ZHANG Wen-zhe, WANG Huan-lei, LIAO Ran-xia, WEI Wen-rui, LI Xue-chun, LIU Shuai, HUANG Ming-hua, SHI Zhi-cheng, SHI Jing
2021, 36(1): 167-178.   doi: 10.1016/S1872-5805(21)60011-2
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Potassium-ion batteries (PIBs) have the potential to be used in future large-scale energy storage devices because of the abundance of potassium resources and their relatively high energy density. However, low reversible capacity and poor cycling stability caused by the large size of the potassium ions limit their practical application. N-doped bacterial cellulose-derived carbons (NBCCs) were prepared by impregnating bacterial cellulose with Mg(NO3)2 solutions (0.03, 0.05 and 0.07 mol L−1) as a pore template and nitrogen source, followed by carbonization and acid washing. The effects of the Mg(NO3)2 concentration on the morphology, porosity, N doping level and electrochemical performance of the NBCCs were investigated. NBCC (0.05) is the best of the three because it has an interconnected pore network structure with a homogeneous distribution of N at a concentration of 3.38 at% and a high specific surface area of 1 355 m2 g−1. It delivers an excellent rate capability of 134 mAh g−1 at 5 A g−1 and a capacity of 307 mAh g−1 after 2 500 cycles at 2 A g−1. A NBCC (0.05)-based anode in a potassium ion hybrid capacitor has a high energy density of 166 W h kg−1 at a power density 493 W kg−1 and excellent cyclability with a capacity retention of nearly 95% after 2 000 cycles. This simple synthesis strategy for fabricating carbon anode materials with an excellent electrochemical performance should promote the development of green and large-scale energy storage devices.
N-doped layered porous carbon electrodes with high mass loadings for high-performance supercapacitors
SHENG Lizhi, ZHAO Yunyun, HOU Baoquan, XIAO Zhenpeng, JIANG Lili, FAN Zhuangjun
2021, 36(1): 179-188.   doi: 10.1016/S1872-5805(21)60012-4
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We report a porous carbon material (NPCM) with a high N content as a high-performance supercapacitor electrode material which was prepared by a simple activation-doping process using Metaplexis Japonica shell as the carbon precursor, ammonium chloride as the nitrogen source and zinc chloride as the activation agent. Its high electrical conductivity, large ion-accessible surface area and fast ion transport ability make it possible to achieve a high mass loading of NPCM per area of the electrode and a high energy and high power density supercapacitor. An electrode with a low NPCM mass loading of 1 mg cm−2 has a gravimetric specific capacitance of 457 F g−1 and an areal specific capacitance of 47.8 μF cm−2. At a much high NPCM loading of 17.7 mg cm−2 it has a high gravimetric capacitance of 161 F g−1. Furthermore, an assembled NPCM//NPCM symmetric supercapacitor with an optimal NPCM loading of 12.3 mg cm−2 delivered a high specific energy of 12.5 Wh kg−1 at an ultrahigh power of 80 kW kg−1 in 1 mol L-1 Na2SO4. The achievement of such high-energy and high-power densities using NPCM will open exciting opportunities for carbon-based supercapacitors in many different applications.
A three-dimensional polyoxometalate/graphene aerogel as a highly efficient and recyclable absorbent for oil/water separation
WANG Sen, WANG Xiao, SHI Xiao-yu, MENG Cai-xia, SUN Cheng-lin, WU Zhong-Shuai
2021, 36(1): 189-197.   doi: 10.1016/S1872-5805(21)60013-6
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Three-dimensional (3D) graphene aerogels (GAs) with a tunable pore structure, a highly accessible surface area, and exceptional compressibility, elasticity and wettability have been explored as promising absorbents for efficient oil/water separation. However, the strategies for assembling 3D GAs usually involve a high-temperature process, resulting in high cost. We report the synthesis of a 3D porous polyoxometalate (POM)-hybridized GA (POM-GA) as a highly efficient and recyclable absorbent for oil/water separation. The material was fabricated at room temperature by the self-assembly and reduction of graphene oxide using POM as a functional cross-linker and hydrazine hydrate as a reductant. It had a 3D interconnected macroporous structure, a large specific surface area, and exceptional compressibility, elasticity and wettability, and had excellent absorption capacities of 100-210 g g−1 for the rapid removal of various organic pollutants from water, outperforming most of the previously reported graphene-based macro-assemblies synthesized at high temperatures. Moreover, the absorbed oils can be readily removed by squeezing or first squeezing and then burning the remaining organic from the 3D POM-GA. The oil-absorption capacity retention rates of the 3D POM-GA are 96 and 90% after 10 absorbing-squeezing and absorbing-squeezing-burning cycles, respectively. The material therefore has great potential for efficient oil/water separation with wide applicability and excellent durability.
Preparation of gelatin-derived nitrogen-doped large pore volume porous carbons as sulfur hosts for lithium-sulfur batteries
SUN Chun-shui, GUO De-cai, SHAO Qin-jun, CHEN Jian
2021, 36(1): 198-208.   doi: 10.1016/S1872-5805(21)60014-8
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Gelatin-derived N-doped porous carbons (GPCs) with a large pore volume were synthesized by a method combining templating, freeze-drying and carbonization, using amino acid rich gelatin as the carbon and nitrogen sources, and silica sol and ice as the templates. The pore volume of the GPCs was regulated by adjusting the mass ratio of the silica sol to ice. Lithium polysulfide (LiPS) adsorption experiments show that the materials have a strong chemisorption for LiPSs. Electrochemical measurements show that N-doping accelerates the sulfur reduction kinetics and inhibits the shuttling of LiPSs. In addition, the larger the pore volume of the GPC, the better the cycling stability of the sulfur cathode. A highly N-doped (7.00%) GPC with a pore volume of 2.98 cm3 g−1 could adsorb a high sulfur content of 78.4% and had a high sulfur utilization rate. Its composite with sulfur as a cathode material gave a high initial specific capacity of 1 384 mAh g−1 at 0.1 C, which dropped to 608 mAh g−1 after 100 cycles.
Co, N co-doped porous carbons as high-performance oxygen reduction electrocatalysts
ZHANG Jing, SONG Liang-hao, ZHAO Chen-fei, YIN Xiu-ping, ZHAO Yu-feng
2021, 36(1): 209-218.   doi: 10.1016/S1872-5805(21)60016-1
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Although the Co and N co-doped carbon catalyst (Co-NC) has attracted much attention because of its low cost and the natural abundance of the dopants, it has a low oxygen reduction reaction (ORR) activity and a high selectivity for the two-electron (2e-) reduction of oxygen to H2O2, which affects its use in fuel cells. Co-NC catalysts were prepared by the pyrolysis of a mixture of cobalt chloride and chitosan pretreated with zinc chloride at 650, 750 and 850 oC, followed by washing with nitric acid and annealing at 900 oC. The results indicate that zinc chloride helps the complexing of chitosan with Co2+, which is also a chemical activator that generates pores, and annealing caused the evaporation of the spherical Zn metal nanoparticles formed by the carbothermal reduction of Zn ions, leading to a unique porous structure of the catalysts with spherical pores filled with spherical carbon nanoparticles formed by the growth of nitrogen-doped carbon as a result of the Co catalyst. The degree of graphitization is also improved by the Co catalyst. The Co-NC catalyst obtained at a pyrolysis temperature of 750 oC shows the same four-electron (4e-) reduction of oxygen as a commercial Pt/C catalyst, and a significantly higher ORR catalytic activity, longer-term stability and better methanol tolerance than a commercial Pt/C catalyst. These are due to its large specific surface area, high contents of pyridinic nitrogen and graphitic nitrogen that disperse the Co species and its excellent electrical conductivity.
Carbon nanotube-supported MoSe2 nanoflakes as an interlayer for lithium-sulfur batteries
SHAO Zhi-tao, WU Li-li, YANG Yue, MA Xin-zhi, LI Lu, YE Hong-feng, ZHANG Xi-tian
2021, 36(1): 219-226.   doi: 10.1016/S1872-5805(21)60015-X
Abstract(106) HTML(18) PDF(54)
Abstract:
Intrinsic polysulfide shuttling is the most fatal problem with Li-S batteries but it can be suppressed by functionalizing the separators with strong lithium polysulfide absorbents. Carbon nanotube (CNT)-supported MoSe2 nanoflakes with a large interlayer spacing were coated on a commercial polypropylene separator to build an efficient barrier (M/C-PP) to polysulfide shuttling for Li-S batteries. The battery with the separator had initial specific capacities of 1 485 and 880 mAh g−1 at 0.1 and 2 C, respectively, and an excellent long-term cycling stability with a low decay rate of 0.093% per cycle at 0.5 C after 300 cycles. This excellent performance was attributed to the strong adsorption of polysulfides by MoSe2 and the fast charge transport channels provided by the CNTs.
Preparation of pitch/polyacrylonitrile carbon nanofiber non-woven fabrics as the electrode for supercapacitors
HE Yi-ting, LI Xiao, YANG Tao, TIAN Xiao-dong, XU Xiao-tong, SONG Yan, LIU Zhan-jun
2021, 36(1): 227-234.   doi: 10.19869/j.ncm.1007-8827.20180141
Abstract(34) HTML(8) PDF(18)
Abstract:
Pitch/polyacrylonitrile carbon nanofiber non-woven fabrics (P/PAN CNFs) for use as supercapacitor electrode materials were prepared by electrospinning a mixed solution of pitch and PAN, followed by stabilization and carbonization. Results indicate that P/PAN CNFs have a smaller fiber diameter, higher conductivity, larger specific surface area and moderate pore size compared with PAN CNFs, which increases the capacitance and rate capability of the supercapacitors. When the mass ratio of pitch to PAN was 1/1.5, the P/PAN CNF (P/PAN-1/1.5) showed a high capacitance of 219 F g−1 at a current density of 0.1 A g−1, a value 1.38 times that of PAN CNF. When the current density was increased to 50 A g−1, the capacitance retention of the P/PAN-1/1.5 was 69.4%, 42.8% larger than that of PAN CNF. A symmetrical supercapacitor based on P/PAN-1/1.5 had an energy density of 4.8 Wh kg−1 at a power density of 14.8 kW kg−1 and a capacitance retention rate of 94.1% after 20 000 cycles.
Research progress on electrode materials and electrolytes for supercapacitors
JIAO Chen, ZHANG Wei-ke, SU Fang-yuan, YANG Hong-yan, LIU Rui-xiang, CHEN Cheng-meng
2017, 32(2): 106-115.  
Abstract(315) PDF(3132)
摘要:
超级电容器具有高功率密度、长循环寿命、良好的低温使用性能和安全性的优点,已经广泛应用到电子产品、能量回收和储能等领域。电极材料和电解液是决定超级电容器性能的两大关键因素,超级电容器常用的电极材料包括碳质材料(活性炭、碳纳米管、石墨烯、炭纤维、纳米洋葱碳等)、金属氧化物(金属氢氧化物)、导电聚合物及复合材料等;电解液主要有水系电解液、有机系电解液与离子液体。本文综述了超级电容器电极材料与电解液的研究现状,详细介绍了电极材料、电解液的性能及优缺点,并对新型电极材料和电解液的研究趋势提出展望。
Influence of graphene oxide additions on the microstructure and mechanical strength of cement
WANG Qin, WANG Jian, LU Chun-xiang, LIU Bo-wei, ZHANG Kun, LI Chong-zhi
2015, 30(4): 349-356.   doi: 10.1016/S1872-5805(15)60194-9
Abstract(502) PDF(410)
摘要:
研究了不同掺量下氧化石墨烯(GO)对水泥石以及胶砂微观结构和力学性能的影响。含16.5%水的水泥浆、0.05%GO及3倍于水泥的沙子共混物作为添加剂制备成砂浆。通过SEM、液氮吸附仪和一系列标准实验分别对水泥石的微观形态、孔隙结构、抗压抗折强度以及水泥净浆的流动度、黏度、凝结时间进行表征;考察不同GO掺量下水泥水化放热的变化情况。结果表明:GO对水泥浆有显著增稠和促凝作用;GO的掺入可以有效降低水泥的水化放热量;GO对水泥石有显著的增强增韧效果,28天龄期时,GO质量分数为0.05%的水泥石,3、7和28 d抗压强度和抗折强度同比对照组分别增加52.4%、46.5%、40.4%和86.1%、68.5%、90.5%,胶砂的抗压强度和抗折强度同比对照组分别增加43.2%、33%、24.4%和69.4%、106.4%、70.5%;GO在水泥硬化过程中对水泥石中晶体产物的产生有促进作用并能规整晶体的排布而形成针状晶体簇,改善水泥石中的孔结构,降低水泥石中微孔的体积,增加水泥石的密实度,对水泥石有显著地增强增韧效果。
Advances in the ablation resistance of C/C composites
FU Qian-gang, ZHANG Jia-ping, LI He-jun
2015, 30(2): 97-105.  
Abstract(713) PDF(1250)
摘要:
C/C复合材料因优异的高温性能被认为是高温结构件的理想材料。然而,C/C复合材料在高温高速粒子冲刷环境下的氧化烧蚀问题严重制约其应用。因此,如何提高C/C复合材料的抗烧蚀性能显得尤为重要。笔者综述C/C复合材料抗烧蚀的研究现状。目前,提高C/C复合材料抗烧蚀性能的途径主要集中于优化炭纤维预制体结构、控制热解炭织构、基体中陶瓷掺杂改性和表面涂覆抗烧蚀涂层等4种方法。主要介绍以上4种方法的研究现状,重点介绍基体改性和抗烧蚀涂层的最新研究进展。其中,涂层和基体改性是提高C/C复合材料抗烧蚀性能的两种有效方法。未来C/C 复合材料抗烧蚀研究的潜在方向主要集中于降低制造成本、控制热解炭织构、优化掺杂的陶瓷相以及将基体改性和涂层技术相结合。
Preparation and properties of reduced graphene oxide/polyimide composites produced by in-situ polymerization and solution blending methods
MA Lang, WANG Guo-jian, DAI Jin-feng
2016, 31(2): 129-134.  
Abstract(523) PDF(1331)
摘要:
利用化学氧化还原法制备出石墨烯。通过原位聚合法及溶液混合法制备出石墨烯/聚酰亚胺复合材料,考察不同复合材料制备方法对其机械性能及导电性能的影响,并对其作用机理进行探讨。结果表明,制备的石墨烯为二维的单层或寡层材料,加入到聚酰亚胺中能够增强其机械性能及电导率。相比溶液混合法,采用原位聚合法时石墨烯在聚酰亚胺基体中分散更均匀,对其团聚作用有更好的抑制作用,制备的复合材料性能更优异。采用该法加入石墨烯的量为1.0 wt%时,拉伸强度达到了132.5 MPa,提高了68.8%;加入量增加到3.0 wt%时,电导率达6.87×10-4S·m-1,提高了8个数量级,对聚酰亚胺的性能有显著的增强作用。
A review of carbon-carbon composites for engineering applications
SU Jun-ming, ZHOU Shao-jian, LI Rui-zhen, XIAO Zhi-chao, CUI Hong
2015, 30(2): 106-114.  
Abstract(618) PDF(1129)
摘要:
评价了中国40多年来在航天、航空、光伏、粉末冶金、工业高温炉领域成功应用的针刺C/C,正交3D C/C、径编C/C、穿刺C/C、轴编C/C等五类C/C复合材料的物理、力学、热学、烧蚀、摩擦磨损、使用寿命等性能及特点,并与其他国家相应材料性能进行分析对比,为建立工程应用C/C复合材料共享的数据库平台奠定基础。揭示了炭纤维预制体、炭基体类型、界面结合状态与材料性能的关联度。指出炭纤维预制体结构单元精细化研究和其结构的梯度设计,以及炭基体的优化组合匹配技术,仍是C/C复合材料性能稳定化提升的重点研究方向。
Hydrothermal synthesis of porous phosphorus-doped carbon nanotubes and their use in the oxygen reduction reaction and lithium-sulfur batteries
GUO Meng-qing, HUANG Jia-qi, KONG Xiang-yi, PENG Hong-jie, SHUI Han, QIAN Fang-yuan, ZHU Lin, ZHU Wan-cheng, ZHANG Qiang
2016, 31(3): 352-362.  
Abstract(378) PDF(661)
摘要:
碳纳米管优异的物理性质和可调的化学组成使其拥有广泛的应用前景。采用低温过程在碳骨架中引入磷原子预期带来可调的化学特性。本研究采用170℃下水热处理碳纳米管-磷酸混合物获得磷掺杂的碳纳米管。磷掺杂的碳管的磷含量为1.66%,比表面积为132 m2/g,热失重峰在纯氧环境下提升至694℃。当掺磷碳纳米管用于氧还原反应时,其起始电位为-0.20 V,电子转移数为2.60,反应电流显著高于无掺杂的碳纳米管。当其用作锂硫电池正极导电材料时,电极的起始容量为1106 mAh/g,电流密度从0.1 C提升至1 C时容量保留率为80%,100次循环的衰减率为每圈0.25%。
Rheological behavior of fresh cement pastes with a graphene oxide additive
WANG Qin, WANG Jian, LU Chun-xiang, CUI Xin-you, LI Shi-yu, WANG Xi
2016, 31(6): 574-584.   doi: 10.1016/S1872-5805(16)60033-1
Abstract(358) PDF(682)
摘要:
采用流变仪和激光共聚焦显微镜对不同氧化石墨烯(GO)掺量的新拌水泥浆体的流变参数以及浆体微观形态进行了定量化研究,并采用Modified-Bingham(M-B)模型和Herschel-Bulkley(H-B)模型对所测数据进行了拟合处理,提出了GO影响新拌水泥浆体的作用机理。结果表明,GO的掺入可以使新拌浆体中在减水剂作用下分散的水泥颗粒发生再次凝聚,形成重组絮凝结构,且随着GO掺量的增加,重组絮凝结构的数量越多,从而使得浆体流变性发生显著变化。一方面,新拌浆体的塑性粘度、屈服应力以及触变性随GO掺量的提高而显著增加。另一方面,GO的掺入提高了新拌浆体的临界剪切速率,使其在较大剪切速率下的流变行为仍然表现为剪切变稀;降低了浆体的剪切增稠程度,提高了浆体的稳定性。
Adsorption of low-concentration methylene blue onto a palygorskite/carbon composite
WU Xue-ping, XU Yan-qing, ZHANG Xian-long, WU Yu-cheng, GAO Peng
2015, 30(1): 71-78.   doi: 10.1016/S1872-5805(15)60176-7
Abstract(599) PDF(1060)
摘要:
通过水热处理凹凸棒石和纤维素获得凹凸棒石/炭纳米复合材料,研究该复合材料对亚甲基蓝的吸附性能。考察吸附条件对吸附行为的影响,以及吸附动力学和热力学研究。亚甲基蓝的吸附行为符合二级吸附速率方程,吸附等温方程符合Langmuir方程。吸附热力学参数的计算值表明,亚甲基蓝在该复合材料上的吸附是自发、吸热的过程。
A graphene/carbon black hybrid material: a novel binary conductive additive for lithium-ion batteries
LI Yong, LU Xiao-hui, SU Fang-yuan, HE Yan-bing, LI Bao-hua, YANG Quan-hong, KANG Fei-yu
2015, 30(2): 128-132.  
Abstract(565) PDF(1558)
摘要:
采用CTAB为表面活性剂将氧化石墨烯和炭黑均匀分散,经水热过程将二者组装到一起,进而高温热处理得到石墨烯/炭黑杂化材料。该材料是一种具有独特结构和良好性能的石墨烯/炭黑杂化材料作为锂离子电池二元导电剂。炭黑颗粒均匀分布在石墨烯表面,可防止石墨烯片层团聚并进一步提高电子导电效率。由于炭黑可增加对电解液的吸附,促进电极内部锂离子的传输过程,最终提高锂离子电池的倍率性能。结果表明,使用质量分数5% 900 ℃热处理之后的二元导电剂的LiFePO4,在10 C时比容量为73 mAh/g,优于使用10%炭黑导电剂时的LiFePO4 (10 C比容量为62 mAh/g)。按照整个电极质量计算,前者的比容量性能比后者提高了近25%,同时在循环性能方面,前者的稳定性也优于后者。
Research progress and potential applications for graphene/polymer composites
ZENG You, WANG Han, CHENG Hui-ming
2016, 31(6): 555-567.  
Abstract(412) PDF(1544)
摘要:
随着石墨烯低成本宏量制备技术的突破,石墨烯的工业化应用进程已引起人们广泛关注。本文介绍了石墨烯在聚合物基复合材料领域的研究进展,侧重阐述石墨烯/聚合物复合材料在力学增强、导电/导热网络构建、防腐阻燃等方面的代表性研究成果,同时对商业化石墨烯产品及其复合材料应用进行了简单评述,探讨了石墨烯/聚合物复合材料领域目前存在的主要问题及未来发展趋势。
Recent progress in the preparation of ordered mesoporous carbons using a self-assembled soft template
HUANG Zheng-hong
2012, 27(05): 321-336.  
Abstract(1682) PDF(1)
Abstract:
The preparation of self-assembled ordered mesoporous carbons (SA-OMCs) using a soft template method has many advantages, such as low cost, ease of preparation and control. This paper review the development periods, the basic principles and preparation procedures with an emphasis on the control of morphology and multi-level pore structure of OMCs based on SA-OMCs. And suggest that further research in this area can be focused on expanding the scope of the precursor, improving the flexibility and conductivity of the shaped products, such as fibers and membranes.
Preparation of graphene by chemical vapor deposition
REN Wen-cai, GAO Li-bo, MA Lai-peng, CHENG Hui-ming
2011, 26(01): 71-80.  
Abstract(2091) PDF(2)
Abstract:
Chemical vapor deposition (CVD) is an effective way for the preparation of graphene with large area and high quality. In this review, the mechanism and characteristics of the four main preparation methods of graphene are briefly introduced, including micromechanical cleavage, chemical exfoliation, SiC epitaxial growth and CVD. The recent advances in the CVD growth of graphene and the related transfer techniques in terms of structure control, quality improvement and large area graphene synthesis were discussed. Other possible methods for the CVD growth of graphene were analyzed including the synthesis and nondestructive transfer of large area single crystalline graphene, graphene nanoribbons and graphene macrostructures.