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A review of carbon-supported single-atom catalysts for electrochemical reactions
WANG Yi-cheng, MA Xiao-bo, , WANG Chen-xu, LI Yang, YANG Cheng-long, WANG Zhe-fan, WANG Chao, HU Chao, ZHANG Ya-ting
 doi: 10.1016/S1872-5805(24)60863-2
Abstract(43) HTML(13) PDF(9)
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Recent advances in the use of carbon-supported single-atom catalysts (SACs) for electrochemical reactions are comprehensively reviewed. The development and advantages of carbon-supported SACs are briefly introduced, followed by a detailed summary of the synthesis strategies used, including vapor phase transport, high temperature pyrolysis and wet chemical methods. Advanced characterization techniques for carbon-supported SACs are also reviewed. The use of carbon-supported SACs in different fields, such as the oxygen reduction reaction, carbon dioxide reduction reaction, nitrogen reduction reaction, hydrogen evolution reaction, and oxygen evolution reaction are summarized. Special emphasis is given to the modification strategies used to enable carbon-supported SACs to have an excellent electrocatalytic performance. Finally, the prospects and challenges associated with using carbon-supported SACs for electrochemical reactions are discussed.
Sulfonyl chloride-intensified metal chloride intercalation of graphite for efficient sodium storage
LAN Shu-qin, REN Wei-cheng, WANG Zhao, YU Chang, YU Jin-he, LIU Ying-bin, XIE Yuan-yang, ZHANG Xiu-bo, WANG Jian-jian, QIU Jie-shan
 doi: 10.1016/S1872-5805(24)60851-6
Abstract(41) HTML(15) PDF(13)
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Metal chloride-intercalated graphite with excellent conductivity and a large interlayer spacing is highly desired for use in sodium ion batteries. However, halogen vapor is usually indispensable in initiating the intercalation process, which makes equipment design and experiments challenging. In this work, SO2Cl2 was used as a chlorine generator to intensify the intercalation of BiCl3 into graphite (BiCl3-GICs), which avoided the potential risks, such as Cl2 leakage, in traditional methods. The operational efficiency in experiment was also improved. After the reaction of SO2Cl2, BiCl3, and graphite at 200 °C for 20 h, the synthesized BiCl3-GICs had a large interlayer spacing (1.26 nm) and a high amount of BiCl3 intercalation (42%), which gave SIBs a high specific capacity of 213 mAh g1 at 1 A g1 and an excellent rate performance (170 mAh g1 at 5 A g1). In-situ Raman spectra revealed that the electronic interaction between graphite and intercalated BiCl3 is weakened during the first discharge, which is favorable for the sodium storage. This work broadly enables the increased intercalation of other metal chloride-intercalated graphites, offering possibilities for developing advanced energy storage devices.
Boron and nitrogen co-doped sodium alginate-based porous carbons for durable and fast Zn-ion hybrid capacitors
LU Ya-ping, WANG Hong-xing, LIU Lan-tao, PANG Wei-wei, CHEN Xiao-hong
 doi: 10.1016/S1872-5805(24)60847-4
Abstract(35) HTML(15) PDF(9)
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In recent years, zinc-ion hybrid capacitors (ZIHCs) have attracted increasing attention due to their environmental friendliness and excellent electrochemical properties. However, their performance is mainly limited by the electrochemical performance of the cathode, so it is necessary to develop an advanced cathode material. In this work, the N, B co-doped sodium alginate-based porous carbon (NBSPC) was prepared by one-step co-carbonization using sodium alginate as the matrix and NH4B5O8 as the N and B source. This N, B co-doping strategy improves the pore structure of the carbon materials and increases the number of surface functional groups, greatly improving the capacitive behavior of the raw materials and thus improving their electrochemical performance. When used as the cathode in ZIHCs, the NBSPC had an excellent rate performance (85.4 mA h g1 even at ultra-high current density of 40 A g1) and cycling stability (15 000 cycles at 20 A g1 with a capacity retention rate of 94.5%).
Increasing the interlayer spacing and generating closed pores to produce petroleum coke-based carbon materials for sodium ion storage
ZHUANG Hong-kun, LI Wen-cui, HE Bin, LV Jia-he, WANG Jing-song, SHEN Ming-yuan, LU An-hui
 doi: 10.1016/S1872-5805(24)60858-9
Abstract(28) HTML(24) PDF(8)
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Petroleum coke (PC) is a valuable precursor for sodium-ion battery (SIB) anodes due to its high carbon content and low cost. The regulation of the microcrystalline state and pore structure of the easily-graphitized PC-based carbon is crucial for creating abundant Na+ storage sites. Here we used a precursor transformation strategy to increase the carbon interlayer spacing and generate abundant closed pores in PC-based carbon, significantly increasing its Na+ storage capacity in the plateau region. This was achieved by introducing a large number of oxygen functional groups through mixed acid treatment and then using high-temperature carbonization to decompose the oxygen functional groups and rearrange the carbon microcrystallites, resulting in a transition from open to closed pores. The optimized samples provide a large reversible capacity of 356.0 mAh g1 at 0.02 A g1, of which approximately 93% is below 1.0 V. Galvanostatic intermittent titration and in-situ X-ray diffraction analysis indicate that the sodium storage capacity in the low voltage plateau region involves a joint contribution of interlayer insertion and closed pore filling processes. This study presents a comprehensive method for the development of high-performance carbon anodes using low-cost and highly aromatic precursors.
Controllable construction of CoP nanoparticles anchored on a nitrogen-doped porous carbon as an electrocatalyst for highly efficient oxygen reduction in Zn-air batteries
YAN Xiao-li, WANG Kui, HAO Shu-wei, ZHOU Guang-da, YANG Hao-wei, ZHANG Hua, GUO Jun-jie
 doi: 10.1016/S1872-5805(24)60848-6
Abstract(82) HTML(48) PDF(21)
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Exploring cost-efficient and high-efficient noble metal-free catalysts for the oxygen reduction reactions (ORRs) involved in sustainable energy devices remains a great challenge. Transition-metal phosphides supported on heteroatom-doped carbons have shown potential as alternative candidates for precious metals because of their tunable electronic structures and higher catalytic performance. Phosphating was used to construct CoP nanoparticles (NPs) anchored on a nitrogen-doped porous carbon framework (CoP@NC) from Co NPs loaded on NC, using PH3 gas released from NaH2PO2 during heat treatment. The dodecahedral structure of Co NPs was retained in their transformation to CoP NPs. The CoP@NC electrocatalyst shows remarkable ORR activity with a half-wave potential up to 0.92 V under alkaline conditions, which is attributed to the combined coupling between the well dispersed CoP nanoparticles on the nitrogen-doped carbon and the efficient mass transport in the porous structure. Zinc-air batteries assembled with the CoP@NC electrocatalyst as a cathode have a high open-circuit voltage of 1.51 V and power density of 210.1 mW cm2. This work provides a novel strategy to develop low-cost catalysts with excellent ORR performance to promote their practical use in metal-air batteries.
Controlled growth of a graphdiyne/cobalt hydroxide heterointerface for efficient chlorine production
LIU Hui-min, LUAN Xiao-yu, YAN Jia-yu, BU Fan-le, XUE Yu-rui, LI Yu-liang
 doi: 10.1016/S1872-5805(24)60861-9
Abstract(36) HTML(15) PDF(3)
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The chlor-alkali process plays a key and irreplaceable role in the chemical industry because of its use in various industrial processes. However, the low selectivity and efficiency of the reported chlorine evolution reaction (CER) electrocatalysts obviously hinder its practical use. We report a simple method for the controlled growth of high-performance CER electrocatalysts by first growing cobalt hydroxide on the surface of carbon cloth, followed by the in-situ growth of graphdiyne (GDY/Co(OH)2). As expected, the as-synthesized catalyst has a small overpotential of only 83 mV at 10 mA cm2, a maximum Faradaic Efficiency (FE) of 91.54%, and a high chlorine yield of 157.11 mg h1 cm2 in acidic simulated seawater. Experimental results demonstrate that the in-situ growth of GDY on the Co(OH)2 surface leads to the formation of heterointerfaces with strong electron transfer between GDY and Co atoms, resulting in a higher conductivity, larger active specific surface area and more active sites, thereby improving the overall electrocatalytic selectivity and efficiency.
A review of the synthesis, characterization, and mechanism of bimetallic catalysts for electrocatalytic CO2 reduction
LIAO Yin-li, HUANG Heng-bo, ZOU Ru-yu, SHEN Shu-ling, LIU Xin-juan, TANG Zhi-hong
 doi: 10.1016/S1872-5805(24)60860-7
Abstract(41) HTML(21) PDF(5)
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The electrocatalytic CO2 reduction reaction (CO2RR) is an environmentally friendly way to convert CO2 into valuable chemicals. However, CO2 conversion is a complex process, which contains 2, 4, 6, 8, and 12 electron transfer processes. It is very important to develop efficient catalysts to precisely control the number of electron transfers for the chemicals required. Single-metal catalysts have some deficiencies, including slow reaction kinetics, low product selectivity and inadequate stability. In response to these challenges, bimetallic catalysts have received significant attention owing to their unique structure and improved performance. The introduction of secondary metals alters the catalyst’s electronic structure, and creates novel active sites, as well as optimizing their interaction with the intermediates. This review provides a comprehensive account of atomically distributed bimetals based on carbon materials and non-atomic distributed bimetals such as alloys and heterostructures, including their synthesis methods, characterization, and the outcomes of different catalysts. Catalytic mechanisms of different bimetallic catalysts are proposed and challenges encountered in the CO2RR are considered.
A review of high-concentration processing, densification, and applications of graphene oxide and graphene
WANG Yue, LUO Jia-liang, LU Zhe-hong, DI Jun, WANG Su-wei, JIANG Wei
 doi: 10.1016/S1872-5805(24)60856-5
Abstract(22) HTML(16) PDF(1)
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Dense graphene assemblies, composed of tightly stacked graphene sheets, have outstanding chemical stability and excellent mechanical, thermal, and electrical properties. They also do not have the problems of low density, low mechanical strength, poor electrical conductivity, or poor thermal conductivity found in porous graphene aerogels, making them ideal materials for future portable electronic and smart devices. We summarize work on high-concentration graphene oxide (GO) and graphene dispersions prepared by mechanical dispersion, evaporation concentration, centrifugal concentration, and liquid phase exfoliation, as well as two-dimensional (2D) dense graphene-based films and three-dimensional (3D) dense graphene-based structures prepared by vacuum-assisted filtration, interfacial self-assembly, and press-forming, and evaluate the advantages and disadvantages of each method. The applications of dense graphene-based assemblies in energy storage, thermal management, and electromagnetic interference (EMI) shielding are summarized. Finally, their challenges and prospects in future research are outlined. This review provides a reference for exploring and developing their large-scale, cost-effective manufacture and use.
Electrochemical methods for the removal of impurities from the graphite anode in spent ternary lithium-ion batteries
ZHANG Rui, TIAN Yong, ZHANG Wei-li, SONG Jia-yin, MIN Jie, PANG Bo, CHEN Jian-jun
 doi: 10.1016/S1872-5805(24)60843-7
Abstract(140) HTML(63) PDF(20)
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The use of lithium-ion batteries (LIBs) is becoming increasingly widespread, and a large number are reaching their end of life. The recycling and re-use of spent LIBs has attracted great attention. Because of the unchanged layer structure of the graphite anode in these batteries, their recycling does not require high-temperature graphitization, and only focuses on the removal of internal impurities. In this study, we used electrochemical treatment for the deep removal of internal metal impurities after heat treatment, ultrasonic separation, and acid leaching of spent graphite. By comparing and analyzing the graphite in different recovery stages, it was found that the presence of organic impurities seriously affects the electrochemical performance. The presence of trace inorganic impurities such as Cu and Fe has little effect on the initial discharge specific capacity, but reduces the cycle stability of graphite. The content of main metal impurities in the final recycled graphite was less than 20 mg/kg. The discharge specific capacity reached 358.7 mAh/g at 0.1 C, and the capacity remained at 95.85% after 150 cycles. Compared with the reported methods for recycling spent graphite, this method can efficiently remove impurities in the graphite, solve the current problems of high acid and alkali consumption, incomplete impurity removal and high energy consumption. The recycled graphite anode has a good electrochemical performance. Our work provides a new recycling and regeneration path for spent LIB graphite anodes.
A review of graphdiyne in aqueous ion batteries
XU Xian-min, FENG Wen-cong, REN Jing-ke, LUO Wen
 doi: 10.1016/S1872-5805(24)60852-8
Abstract(102) HTML(25) PDF(20)
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Graphdiyne (GDY) is a novel carbon material with a special carbon hybrid arrangement, unique chemical and electronic structure and infinitely distributed [PT1] natural pores that has promising applications in electrochemical energy storage. Emerging aqueous ion batteries have advantages of low cost and high safety, but the development of high-performance electrode materials, the design of new membrane systems and ways of stabilizing the interface remain the main challenges in their manufacture. With its unique porous structure and excellent electrochemical properties, graphdiyne can improve ion transport, interface deposition behavior and electrolyte instability in the aspects of anode protection, cathode cladding, membrane design and stabilizing the pH value of the interface. A bottom-up molecular structural design strategy makes graphdiyen easy to modify and dope, improving the properties of its analogues and thus expanding their applications in aqueous ion batteries. We systematically summarize the structure, properties, and synthesis methods of graphdiyne, and summarize the research of graphdiyne in aqueous ion batteries. A comprehensive evaluation of the existing problems and challenges of the use of graphdiyen in aqueous ion batteries is given, and future trends and developments are suggested.
Revealing the correlation of high-frequency performance of supercapacitors with doped nitrogen species
FAN Ya-feng, YI Zong-lin, ZHOU Yi, XIE Li-jing, SUN Guo-hua, WANG Zhen-bing, Huang Xian-hong, SU Fang-yuan, CHEN Cheng-meng
 doi: 10.1016/S1872-5805(24)60849-8
Abstract(27) HTML(13) PDF(5)
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Nitrogen doping strategy has been widely used to enhance the performance of carbon electrodes in supercapacitors, particularly in terms of high-frequency response. However, the charge storage and ion response mechanisms of different nitrogen dopants at high frequencies are still unclear. In this study, we employ carbonized melamine foam with an open surface structure as a simplified model electrode material, enabling a comprehensive analysis of their impact on the ionic response behavior of high-frequency supercapacitors. Through a combination of experiments and first-principles calculations, we uncover that pyrrolic nitrogen, characterized by a higher adsorption energy, enhances the charge storage capacity of the electrode at high frequencies. On the other hand, graphitic nitrogen, with a lower adsorption energy, promotes rapid ion response. Furthermore, we propose the use of adsorption energy as a practical descriptor for electrode/electrolyte design in high-frequency applications, offering a more universal approach for optimizing the performance of N-doped carbon materials. This research contributes to the advancement of high-frequency supercapacitor technology and provides guidance for the development of improved N-doped carbon materials.
Recent progress in carbonaceous materials based Z-scheme and S-scheme heterojunctions for photocatalytic clean energy generation
Sahil Rana, Amit Kumar, WANG Tong-tong, Gaurav Sharma, Pooja Dhiman, Alberto García-Penas
 doi: 10.1016/S1872-5805(24)60857-7
Abstract(35) HTML(11) PDF(3)
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Carbonaceous materials including carbon nanotubes/nanofibers, graphene, graphene oxide, reduced graphene oxide, graphyne, graphdiyne, carbon quantum dots and fullerenes have gained considerable attention in the recent years for their unique properties such as high conductivity, excellent stability and biocompatibility. The integration of these carbonaceous materials into Z-scheme and S-scheme heterojunctions has emerged as a transformative strategy to enhance the photocatalytic efficiency for energy conversion applications. This review delves into the fundamental principles of clean energy generation such as photocatalytic H2 generation and CO2 reduction, elucidating their respective mechanisms and advantages. Furthermore, various types of carbonaceous materials, their synthesis and construction of Z-scheme and S-scheme heterojunctions are discussed emphasizing their role in promoting charge separation, reducing recombination losses and extending the spectral response range. With the focus on solar fuel production, the recent advancements in carbonaceous based Z-scheme and S-scheme heterojunctions are discussed and summarized for photocatalytic H2 generation and CO2 reduction. Lastly, the current bottlenecks and challenges in the field of carbonaceous based photocatalysts are discussed with the valuable insights for future development in this particular field.
Photodetectors based on graphene/molybdenum dichalcogenide van der Waals heterostructure: A review
ZHANG Xin-hua, LIU Wei-di, GONG You-pin, LIU Qing-feng, CHEN Zhi-gang
 doi: 10.1016/S1872-5805(24)60853-X
Abstract(80) HTML(21) PDF(18)
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Graphene is widely used in photodetection owing to its high carrier mobility and wide spectral absorption range. However, the high dark current due to its low light absorption severely limits the performance of photodetection. Molybdenum dihalide (MoX2, X= S, Se and Te) has a high absorption coefficient, which can compensate high dark current in graphene-based photodetectors and result in outstanding photoelectronic properties of photodetectors based on graphene/MoX2 van der Waals heterostructure (vdWH). In this review, we firstly review working principles, performance indicators, and structures of photodetectors. After that, the significance of graphene/MoX2 vdWH photodetectors are highlighted from a material fundamental perspective. Preparation methodologies and performance enhancement strategies of graphene/MoX2 vdWH photodetectors are summarized. In the end, we discuss the current challenges and future directions of the graphene/MoX2 vdWH photodetectors. This review will guide the design of high-performance vdWH photodetectors.
A Review on Catalytic Preparation of Mesophase Pitch
MA Zi-hui, YANG Tao, SONG Yan, CHEN Wen-sheng, DUAN Chun-feng, SONG Huai-he, TIAN Xiao-dong, GONG Xiang-jie, LIU Zheng-yang, LIU Zhan-jun
 doi: 10.1016/S1872-5805(24)60862-0
Abstract(49) HTML(17) PDF(4)
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Mesophase pitch, due to its high purity and orientation, is a superior precursor for high-performance carbon materials. However, the preparation of top-notch mesophase pitch faces challenges. Catalytic polycondensation at low temperature is more favorable to synthesize mesophase pitch which circumvents the high-temperature free radical reaction of other thermal polycondensation approaches. Besides, the reaction is gentle and easily controlled. It has the potential to significantly improve the yield of mesophase pitch and easily introduce the naphthenic characteristics into the molecules, hence, catalytic polycondensation is a preferentially recommended methodology to synthesize highly spinnability mesophase pitch. This paper furnishes a synopsis of the selection pretreatment of raw materials to prepare diverse mesophase pitches, and explains the reaction mechanism and associated research advancements of different catalytic systems in recent years. Ultimately, how to manufacture high-quality mesophase pitch by employing a catalyst-promoter system is summarized and prospected, it is expected to present original concepts and dependable theoretical direction for the design of high-quality pitch molecular in the future.
Study on PES-C toughened E51/DETDA epoxy resin and its carbon fiber composites
WU Rong-peng, ZHANG Xing-hua, WEI Xing-hai, JING De-qi, SU Wei-guo, ZHANG Shou-chun
 doi: 10.1016/S1872-5805(23)60741-3
Abstract(211) HTML(130) PDF(51)
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A toughener that can effectively improve the interlaminar toughness in carbon fiber composites even with a low dosage is crucial for various applications and the pursuit of such, in worthwhile. In this paper, the toughening effect of phenolphthalein-based poly (ether sulfone) (PES-C) on E51/ DETDA epoxy and its carbon fiber composites (CFCs) was investigated. The SEM results showed that PES-C/epoxy blends formed sea-island phase and bicontinuous phase structure, associated with reaction-induced phase separation. After adding 15 g m−2 PES-C, the glass transition temperature (Tg) of the blends was increased by 51.5 °C. Meanwhile, the flexural strength, impact strength and fracture toughness of the blends were improved by 41.1%, 186.2% and 42.7%, respectively. These improvements could be attributed to the phase separation structure of the PES-C/epoxy system. Moreover, PES-C film was used to improve the mode-II fracture toughness (GIIC) of CFCs. GIIC value of the 7 μm PES-C film toughened laminate was improved by 80.3% compared to that of the control laminate. The increase in GIIC could be attributed to cohesive failure and plastic deformation in the interleaving region.
Plasma-assisted preparation of NiCoAl-LDHs with enhanced interlayer space on carbon cloth for electrochemical deionization
JIANG Qiu-tong, WANG Guo-qing, LI Yi, HUANG Hong-wei, LI Qian, YANG Jian
 doi: 10.1016/S1872-5805(24)60854-1
Abstract(66) HTML(31) PDF(19)
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Capacitive deionization technology has been considered as an emerging desalination technique in recent years, especially for its economic and energy-saving characteristics within the brackish water range. However, there are currently few studies on chloride ion removal electrodes, and the slow desalination kinetics limits their development. In this work, Ar-NiCoAl-LDHs@ACC materials with enhanced interlayer space were prepared by in-situ growth of NiCoAl-LDHs nanosheets arrays on acid-treated carbon cloth and subsequent argon plasma treatment. The carbon cloth suppresses the agglomeration of NiCoAl-LDHs nanosheets and improves the electrical conductivity, while the plasma treatment further expands the interlayer space of NiCoAl-LDHs and enhances the hydrophilicity. This provides a rapid diffusion channel and more interlayer active sites for chloride ions, achieving high desalination kinetics. A hybrid capacitive deionization (HCDI) cell was assembled using the Ar-NiCoAl-LDHs@ACC as chloride ion removal electrode and activated carbon as sodium ion removal electrode. This HCDI cell achieves a high desalination capacity of 93.26 mg g−1 at 1.2 V in 1000 mg L−1 NaCl solution, remarkable desalination rate of 0.27 mg g−1 s−1, and good charge efficiency of 0.97. In 300 mg L−1 NaCl solution at 0.8 V, the capacity retention rate remains above 85% after 100 cycles. This work provides new ideas for the controllable preparation of two-dimensional metal hydroxide materials with large interlayer space and the design of high-performance electrochemical chlorine ion removal electrodes.
Synergistic enhancement of toughness and viscosity of carbon nanotubes/polyether imide/polyether ether ketone nanocomposites
SONG Jiu-peng, ZHAO Yan, LI Xue-kuan, XIONG Shu, LI Shuang, WANG Kai
 doi: 10.1016/S1872-5805(22)60643-7
Abstract(475) HTML(249) PDF(38)
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Polyether ether ketone (PEEK) has favorable mechanical properties. However, its high melt viscosity limits its applications because it is hard to process. In this study, PEEK nanocomposites modified with carbon nanotubes (CNTs) and polyether imide (PEI) were prepared using a direct wet powder blending method. The melt viscosity of the nanocomposites decreased by approximately 50%. Under optimal conditions, the addition of CNTs and PEI resulted in a synergistic increase in the toughness of the nanocomposites. The elongation at break increased by 129%, and the fracture energy increased by 97%. The uniformly dispersed CNTs/PEI powder reduces the processing difficulty of PEEK nanocomposites without affecting the heat resistance. The nanocomposites prepared by this method have lower melt viscosity. This improvement of the properties of PEEK would facilitate its use in the preparation of thermoplastic composites by powder impregnation or laser sintering technology.
Ablation behaviour and mechanical performance of ZrB2-ZrC-SiC modified carbon/carbon composites prepared by vacuum filtration combined with reactive melt infiltration
ZHANG Jia-ping, SU Xiao-xuan, LI Xin-gang, WANG Run-ning, FU Qian-gang
 doi: 10.1016/S1872-5805(24)60841-3
Abstract(169) HTML(103) PDF(47)
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The development of advanced aircrafts relies on high performance thermal-structural materials and composites of carbon/carbon (C/C) with ultrahigh-temperature ceramics are ideal candidates. However, traditional routes of compositing are either inefficient and expensive or lead to non-uniform distribution of ceramics in the matrix. Here, vacuum filtration of ZrB2 was successfully applied to introduce ZrB2-ZrC-SiC into C/C as a supplement for reactive melt infiltration ZrSi2, which contributed to the content increase and uniform distribution of the introduced ceramic phases. The mass and linear ablation rates of the composites were reduced by 68.9% and 29.7%, respectively, compared to those of C/C-ZrC-SiC composites prepared through reactive melt infiltration. The ablation performance was improved because of the volatilization of B2O3, taking a part of the heat away, and more uniformly distributed ZrO2 that could promote the formation of ZrO2-SiO2 continuous protective layer. This efficiently resisted the mechanical denudation and hindered the oxygen infiltration.
Wet-composition-induced amorphous adhesion toward a high interfacial shear strength between carbon fiber and polyetherketoneketone
ZHANG Feng, LI Bo-lan, JIAO Meng-xiao, LI Yan-bo, WANG Xin, YANG Yu, YANG Yu-qiu, ZHANG Xiao-hua
 doi: 10.1016/S1872-5805(22)60646-2
Abstract(393) HTML(260) PDF(54)
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Interfacial adhesion between carbon fiber (CF) and polyetherketoneketone (PEKK) is a key factor that affects the mechanical performances of their composites. Therefore, it is of great importance to impregnate PEKK into CF bundles as efficiently as possible. Here we report that owing to the high dissolubility, PEKK can be introduced onto CF surfaces via a wet strategy. The excellent wettability of PEKK guarantees a full covering and tight binding on CFs, making it possible to evaluate the interfacial shear strength (IFSS) with the microdroplet method. Furthermore, the interior of CF bundles can be completely and uniformly filled with PEKK by the solution impregnation, leading to a high interlaminar shear strength (ILSS). The maximum IFSS and ILSS can reach 107.8 and 99.3 MPa, respectively. Such superior shear properties are ascribed to the formation of amorphous PEKK confined in the limited spacing between CFs.
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2024, 39(2): 1-1.  
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2024, 39(2): 1-7.  
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Reviews
A review of graphdiyne: A new material for synthesizing effective adsorbents for aqueous contaminants
Gaurav Sharma, Yaksha Verma, Amit Kumar, Pooja Dhiman, WANG Tong-tong, Florian J. Stadler
2024, 39(2): 173-200.   doi: 10.1016/S1872-5805(24)60830-9
Abstract(326) HTML(72) PDF(123)
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Graphdiyne (GDY), a new two-dimensional (2D) carbon molecule, is expected to have applications in the removal of contaminants from aqueous media. It has superior conjugation, unusual and varied electronic properties, and exceptional chemical and thermal stability because of its framework of sp and sp2 hybridized carbon bonds that are combined to produce benzene rings and diacetylenic bonds in a two-dimensional symmetrical network. Its molecular chemistry is the result of it having carbon-carbon triple bonds, with a regular distribution of triangular pores in its structure, which provide reaction sites and various reaction pathways. GDY is an adsorbent with an excellent efficiency for the removal of oil, organic pollutants, dyes, and metals from contaminated water, but there is limited evidence of it being used as an adsorbent in the literature. This review discusses its synthesis and its use as an adsorbent together with its prospects for pollutant removal.
A review of the use of metal oxide/carbon composite materials to inhibit the shuttle effect in lithium-sulfur batteries
ZHOU Zhi-qiang, WANG Hui-min, YANG Lu-bin, MA Cheng, WANG Ji-tong, QIAO Wen-ming, LING Li-cheng
2024, 39(2): 201-222.   doi: 10.1016/S1872-5805(24)60838-3
Abstract(268) HTML(78) PDF(109)
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Lithium-sulfur (Li-S) batteries are among the most promising next-generation electrochemical energy-storage systems due to their exceptional theoretical specific capacity, inexpensive production cost and environmental friendliness. However, the poor conductivity of S and Li2S, severe lithium polysulfide (LiPS) shuttling and the sluggish redox kinetics of the phase transformation greatly hinder their commercialization. Carbonaceous materials could be potentially useful in Li-S batteries to tackle these problems with their high specific surface area to host LiPSs and sulfur and excellent electrical conductivity to increase electron transfer rate. However, non-polar carbon materials are unable to interact closely with the highly polar polysulfides, resulting in a low sulfur utilization and a serious shuttle effect. Because of their advantages of strong polarity and a large number of adsorption sites, integrating transition metal oxides (TMOs) with carbon-based materials (CMs) increases the chemical adsorption of LiPSs and electrochemical reaction activity for LiPSs. The working principles and main challenges of Li-S batteries are discussed followed by a review of recent research on the ex-situ and in-situ synthesis of TMO/CM composites. The formation of TMO/CMs with the dimensionalities of CMs from 1D to 3D are then reviewed together with ways of changing their structure, including heterostructure design, vacancy engineering and facet manipulation. Finally, the outlook for using TMO/CMs in Li-S batteries is considered.
A review of the use of graphene-based materials in electromagnetic-shielding
YANG Shang-juan, CAO Yun, HE Yan-bing, LV Wei
2024, 39(2): 223-239.   doi: 10.1016/S1872-5805(24)60840-1
Abstract(535) HTML(235) PDF(153)
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The development of communication technology has had great benefits but the detrimental effects of electromagnetic radiation have also become important. There has therefore been growing research on electromagnetic shielding materials that have a wide shielding range, high absorption efficiency and stability. Graphene, a lightweight material with an exceptional electrical conductivity and a large specific surface area, has remarkable potential in this application. We first elucidate the fundamental principles of electromagnetic shielding and the structural characteristics of graphene-based materials while highlighting their unique electromagnetic shielding properties. We also provide an overview of common strategies for changing graphene-based materials including structural modification, heteroatom doping, and their incorporation in composite materials to improve this property. Structural modification can increase the losses of electromagnetic waves by absorption and multiple reflection, and heteroatom doping and incorporation in composite materials can increase the losses by interface polarization and magnetic effects. We also summarize various ways of modifying the materials so that they are lightweight and have a high shielding bandwidth.

A review of 3D monolithic carbon-based materials with a high photothermal conversion efficiency used for solar water vapor generation
HAN Yue, ZHANG Peng, ZHAO Xiao-ming
2024, 39(2): 240-253.   doi: 10.1016/S1872-5805(24)60827-9
Abstract(388) HTML(357) PDF(116)
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In recent years, photothermal-driven desalination has been regarded as one of the most promising methods to solve the global crisis of freshwater scarcity. The solar generation of water vapor (SGWV) is a key process in seawater desalination which uses simple equipment and has a high cost-benefit. Among alternative photothermal conversion materials for a SGWV system, three-dimensional (3D) monolithic carbon-based materials have many advantages, including low cost, good structure control, and high light-harvesting efficiency which gives a high evaporation rate. 3D monolithic carbon-based materials with a high photothermal conversion efficiency are reviewed together with their use in interface SGWV. The working mechanism of SGWV and the classification of SGWV materials are first considered, followed by detailed consideration of 3D monolithic carbon materials, including their design, preparation and working mechanism in SGWV. Finally, both the advantages and disadvantages of 3D monolithic carbon materials with a high photothermal conversion efficiency are examined.

Carbon electrodes for the electrocatalytic synthesis of hydrogen peroxide: A review
HUANG Xian-huai, YANG Xin-ke, GUI Ling, LIU Shao-gen, WANG Kun, RONG Hong-wei, WEI Wei
2024, 39(2): 254-270.   doi: 10.1016/S1872-5805(24)60846-2
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Electrocatalytic oxygen reduction by a 2e pathway enables the instantaneous synthesis of H2O2, a process that is far superior to the conventional anthraquinone process. In recent years, the electrocatalytic synthesis of H2O2 using carbon electrodes has attracted more and more attention because of its excellent catalytic performance and superior stability. The relationship between material modification, wettability and the rate of H2O2 synthesis and service life is considered together with the three-phase interface. The structure of the carbon electrodes and the principles of electrocatalytic H2O2 synthesis are first introduced, and four major catalysts are reviewed, namely, monolithic carbon materials, metal-free catalysts, noble metal catalysts and non-precious metal catalysts. The effects of the metal anode and the electrolyte on the three-phase interface are described. The relationship between carbon electrode wettability and the three-phase interface is described, pointing out that modification focusing on improving the selectivity of the 2e pathway can also impact electrode wettability. In addition, the relationship between the design of the components in the electrochemical system and their effect on the efficiency of H2O2 synthesis is discussed for carbon electrodes. Finally, we present our analysis of the current problems in the electrocatalytic synthesis of H2O2 for carbon electrodes and future research directions.
Research articles
Polyimide-assisted fabrication of highly oriented graphene-based all-carbon foams for increasing the thermal conductivity of polymer composites
XIONG Ke, SUN Zhi-peng, HU Ji-chen, MA Cheng, WANG Ji-tong, GE Xiang, QIAO Wen-ming, LING Li-cheng
2024, 39(2): 271-282.   doi: 10.1016/S1872-5805(24)60835-8
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Graphene and its derivatives are often preferentially oriented horizontally during processing because of their two-dimensional (2D) layer structure. As a result, thermal interface materials (TIMs) composed of a polymer matrix and graphene-derived fillers often have a high in-plane (IP) thermal conductivity (K), however, the low through-plane (TP) K makes them unsuitable for practical use. We report the development of high-quality polyimide/graphite nanosheets (PG) perpendicular to the plane using a directional freezing technique that increase the TP K of polymer-based composites. Graphene-derived nanosheets (GNs) were obtained by the crushing of scraps of highly thermally conductive graphene films. A water-soluble polyamic acid salt solution was used to disperse the hydrophobic GNs filler to achieve directional freezing. The polyimide, which facilitated the directional alignment of the GNs, was then graphitized. The introduction of the GNs increases the order and density of the PG, thus improving the strength and heat transfer performance of its polydimethylsiloxane (PDMS) composite. The obtained PG/PDMS composite (21.1% PG, mass fraction) has an impressive TP K of14.56 W·m1·K1, 81 times that of pure PDMS. This simple polyimide-assisted 2D hydrophobic fillers alignment method provides ideas for the widespread fabrication of anisotropic TIMs and enables the reuse of scraps of graphene films.
The production of electrodes for microsupercapacitors based on MoS2-modified reduced graphene oxide aerogels by 3D printing
WANG Meng-ya, LI Shi-you, GAO Can-kun, FAN Xiao-qi, QUAN Yin, LI Xiao-hua, LI Chun-lei, ZHANG Ning-shuang
2024, 39(2): 283-296.   doi: 10.1016/S1872-5805(24)60823-1
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Micro-supercapacitors (MSCs) are of interest because of their high power density and excellent cycling performance, offering a broad array of potential applications. However, preparing electrodes for the MSCs with an extremely high areal capacitance and energy density remains a challenge. We constructed MSC electrodes with an ultra-high area capacitance and a high energy density, using reduced graphene oxide aerogel (GA) and MoS2 as the active materials, combined with 3D printing and surface modification. Using 3D printing, we obtained electrodes with a stable macrostructure and a GA-crosslinked micropore structure. We also used a solution method to load the surface of the printed electrode with molybdenum disulfide nanosheets, further improving the electrochemical performance. The surface capacitance of the electrode reached 3.99 F cm2, the power density was 194 W cm2, and the energy density was 1997 mWh cm2, confirming its excellent electrochemical performance and cycling stability. This work provides a simple and efficient method for preparing MSC electrodes with a high areal capacitance and energy density, making them ideal for portable electronic devices.
N, S co-doped coal-based hard carbon prepared by two-step carbonization and a molten salt template method for sodium storage
NIU Hui-zhu, WANG Hai-hua, SUN Li-yu, YANG Chen-rong, WANG Yu, CAO Rui, YANG Cun-guo, WANG Jie, SHU Ke-wei
2024, 39(2): 297-307.   doi: 10.1016/S1872-5805(24)60842-5
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Hard carbon, known for its abundant resources, stable structure and high safety, has emerged as the most popular anode material for sodium-ion batteries (SIBs). Among various sources, coal-derived hard carbon has attracted extensive attention. In this work, N and S co-doped coal-based carbon material (NSPC1200) was synthesized through a combination of two-step carbonization process and heteroatom doping using long-flame coal as a carbon source, thiourea as a nitrogen and sulfur source, and NaCl as a template. The two-step carbonization process played a crucial role in adjusting the structure of carbon microcrystals and expanding the interlayer spacing. The N and S co-doping regulated the electronic structure of carbon materials, endowing more active sites. Additionally, the introduction of NaCl as a template contributed to the construction of pore structure, which facilitates better contact between electrodes and electrolytes, enabling more efficient transport of Na+ and electrons. Under the synergistic effect, NSPC1200 exhibited exceptional sodium storage capacity, reaching 314.2 mAh g−1 at 20 mA g−1. Furthermore, NSPC1200 demonstrated commendable cycling stability, maintaining a capacity of 224.4 mAh g−1 even after 200 cycles. This work successfully achieves the strategic tuning of the microstructure of coal-based carbon materials, ultimately obtaining hard carbon anode with excellent electrochemical performance.
A new anode material for high rate and long life lithium/sodium storage
ZHANG Chun-hui, ZHANG Jia-yuan, ZHAN Jie-yang, YU Jian, FAN Lin-lin, YANG An-ping, LIU hong, GAO Guang-gang
2024, 39(2): 308-320.   doi: 10.1016/S1872-5805(24)60845-0
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It is imperative to design suitable anode materials for both lithium-ion (LIBs) and sodium-ion batteries (SIBs) with a high-rate performance and ultralong cycling life. We fabricated a MoO2/MoS2 heterostructure that was then homogeneously distributed in N,S-doped carbon nanofibers (MoO2/MoS2@NSC) by electrospinning and sulfurization. The one-dimensional carbon fiber skeleton serves as a conductive frame to decrease the diffusion pathway of Li+/Na+, while the N/S doping creates abundant active sites and significantly improves the ion diffusion kinetics. Moreover, the deposition of MoS2 nanosheets on the MoO2 bulk phase produces an interface that enables fast Li+/Na+ transport, which is crucial for achieving high efficiency energy storage. Consequently, as the anode for LIBs, MoO2/MoS2@NSC gives an excellent cycling stability of 640 mAh g1 for 2000 cycles under 5.0 A g1 with an ultralow average capacity drop of 0.002% per cycle and an exceptional rate capability of 614 mAh g1 at 10.0 A g1. In SIBs, it also produces a significantly better electrochemical performance (reversible capacity of 242 mAh g1 under 2.0 A g1 for 2000 cycles and 261 mAh g1 under 5.0 A g1). This work shows how introducing a novel interface in the anode can produce rapid Li+/Na+ storage kinetics and a long cycling performance.
N-doped hollow carbon nanospheres embedded in N-doped graphene loaded with palladium nanoparticles as an efficient electrocatalyst for formic acid oxidation
FANG Yue, YANG Fu-kai, QU Wei-li, DENG Chao, WANG Zhen-bo
2024, 39(2): 321-333.   doi: 10.1016/S1872-5805(24)60844-9
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Efficient electrocatalysts with a low cost, high activity and good durability play a crucial role in the use of direct formic acid fuel cells. Pd nanoparticles supported on N-doped hollow carbon nanospheres (NHCNs) embedded in an assembly of N-doped graphene (NG) with a three-dimensional (3D) porous structure by a simple and economical method were investigated as direct formic acid fuel cell catalysts. Because of the unique porous configuration of interconnected layers doped with nitrogen atoms, the Pd/NHCN@NG catalyst with Pd nanoparticles has a large catalytic active surface area, superior electrocatalytic activity, a high steady-state current density, and a strong resistance to CO poisoning, far surpassing those of conventional Pd/C, Pd/NG, and Pd/NHCN catalysts for formic acid electrooxidation. When the HCN/GO mass ratio was 1∶1, the Pd/NHCN@NG catalyst had an outstanding performance in the catalytic oxidation of formic acid, with an activity 4.21 times that of Pd/C. This work indicates a way to produce superior carbon-based support materials for electrocatalysts, which will be beneficial for the development of fuel cells.
Improving the mechanical properties and thermal conductivity of mesophase-pitch-based carbon fibers by controlling the temperature in industrial spinning equipment
YE Gao-ming, SHI Kui, WU Huang, HUANG Dong, YE Chong, OUYANG Ting, ZHU Shi-peng, FAN Zhen, LIU Hong-bo, LIU Jin-shui
2024, 39(2): 334-344.   doi: 10.1016/S1872-5805(24)60826-7
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Mesophase-pitch-based carbon fibers (MPCFs) were prepared using industrial equipment with a constant extrusion rate of pitch while controlling the spinning temperature. The influence of spinning temperature on their microstructures, mechanical properties and thermal conductivities was investigated. SEM images of the fractured surface of MPCFs show that the graphite layers have a radiating structure at all spinning temperatures, but change from the fine-and-folded to the large-and-flat morphology when increasing the spinning temperature from 309 to 320 oC . At the same time the thermal conductivity and tensile strength of the MPCFs respectively increase from 704 W·m1·K1 and 2.16 GPa at 309 oC to 1 078 W·m1·K1 and 3.23 GPa at 320 oC. The lower viscosity and the weaker die-swell effect of mesophase pitch at the outlets of the spinnerets at the higher spinning temperature contribute to the improved orientation of mesophase pitch molecules in the pitch fibers, which improves the crystallite size and orientation of the MPCFs.
A highly efficient absorptive and catalytic self-supporting Fe2O3/CC host for high performance Li-S batteries
TIAN Zhen, XUE Lei-lei, DING Hong-yuan
2024, 39(2): 345-353.   doi: 10.1016/S1872-5805(24)60825-5
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Abstract:

The lithium−sulfur (Li-S) battery is a promising energy storage system because of its high energy density and low cost. However, the shuttling of lithium polysulfides (LiPSs) and low conductivity of the S cathode are barriers to its practical application. Fe2O3 nanorods were grown on a carbon cloth (Fe2O3/CC) by a solvothermal reaction and calcination to obtain a cathode for the battery. The mesoporous structure of the Fe2O3 and the CC conducting network facilitates lithium-ion and electron transport. Meanwhile, the nanorod arrangement results in the exposure of more Fe2O3 active sites, which improves the adsorption and rapid conversion of LiPSs. As a result, a Li–S cell using a Fe2O3/CC cathode has a high capacity of 1250 mAh g1 at 0.1 C with an excellent life of over 100 cycles with a capacity retention of 67%. It also has a 70% capacity retention after 1000 cycles at 0.2 C. The excellent electrochemical performance of the Fe2O3/CC cathode indicates its potential applications in Li-S batteries.

The oxidation reaction mechanism and its kinetics for a carbonaceous precursor prepared from ethylene tar for use as an anode material for lithium-ion batteries
GUO Tian-rui, CHEN Rong-qi, GAO Wei, WANG Yan-li, ZHAN Liang
2024, 39(2): 354-366.   doi: 10.1016/S1872-5805(22)60597-3
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The oxidation reaction mechanism and its kinetics for ethylene tar were investigated in order to obtain a suitable anode material for Li-ion batteries. The oxidation of ethylene tar was divided into 3 stages (350–550, 550–700 and 700–900 K) according to the thermogravimetric curve. To reveal the oxidation reaction mechanism, the components of the gases evolved at different stages were analyzed by mass spectrometry and infrared technology. Based on these results the reaction was divided into 4 stages (323–400, 400–605, 605–750 and 750–860 K) to perform simulation calculations of the kinetics. Using the iso-conversion method (Coats-Redfern) to analyze the linear regression rates (R2) between 17 common reaction kinetics models and experimental data, an optimum reaction kinetics model for expressing the oxidation of ethylene tar was determined and the results were as follows. (1) During oxidation, the side chains of aromatic compounds first react with oxygen to form alcohols and aldehydes, leaving peroxy-radicals on aromatic rings. Subsequently, the aromatic compounds with peroxy-radicals undergo polymerization/condensation reactions to form larger molecules. (2) A fourth-order reaction model was used to describe the first 3 stages in the oxidation process, and the activation energies are 47.33, 18.69 and 9.00 kJ·mol1 at 323–400, 400–605, 605–750 K, respectively. A three-dimensional diffusion model was applied to the fourth stage of the oxidation process, and the activation energy is 88.37 kJ·mol1 at 750–860 K. A high softening point pitch was also produced for use as a coating of the graphite anode, and after it had been applied the capacity retention after 300 cycles increased from 51.54% to 79.07%.
Recent progress in the preparation of ordered mesoporous carbons using a self-assembled soft template
HUANG Zheng-hong
2012, 27(05): 321-336.  
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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(3469) PDF(416)
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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.