新型炭材料

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2022, 37(6): 1-1.

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2022, 37(6): 1-7.

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Review of chemical recycling and reuse of carbon fiber reinforced epoxy resin composites

TIAN Zi-shang, WANG Yu-qi, HOU Xiang-lin

2022, 37(6): 1021-1045. doi: 10.1016/S1872-5805(22)60652-8

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Carbon fiber-reinforced epoxy resin composites (CFRCs) have been used in the transportation and aerospace fields because of their excellent mechanical properties. The recycling of CFRCs has attracted attention worldwide in recent years. Chemical recycling is a promising method, which can selectively destroy specific resin bonds to achieve controllable degradation. Matrix epoxy resins are degraded into monomers or oligomers, and the high-value carbon fibers can be recycled. First, we summarize progress on chemical recovery methods, mainly super- and subcritical fluids, oxidation, alcoholysis and electrochemical recycling etc. Then, we briefly introduce the synthesis and depolymerization mechanism of recyclable thermosetting resins by the insertion of reversible chemical bonds into the resin to prepare recyclable resins, which is beneficial for the recycling and reuse of components in CFRCs. Finally, possible developments in the chemical recycling of CFRCs and the preparation of high-performance recyclable epoxy resins are proposed.

A comprehensive review of the 3D printing of sp² carbons: Materials, properties and applications

Satendra Kumar, Manoj Goswami, Netrapal Singh, Sathish Natarajan, Surender Kumar

2022, 37(6): 1046-1065. doi: 10.1016/S1872-5805(22)60651-6

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Three dimensional (3D) printing is a modern technology that has the possibility to transform existing production methods. It offers a novel production method of layered manufacturing and layer-by-layer stacking, which radically simplifies the manufacturing process and enables large-scale customizable production. However, there are still numerous problems with this new technology. Except for pure graphene, sp² carbons can be 3D printed with little difficulty because of their hydrophilicity. The hydrophobic nature of pure graphene makes it difficult to print and process in water-based media, but advances in capillary inks allow for the 3D printing of pure graphene. This review focuses on the most recent developments in the 3D printing of sp² carbons. A concise overview of 3D printing technologies is presented, followed by a summary of 3D printed sp² carbons and their diverse applications. Finally, prospects and opportunities for this new field are discussed.

Electrospun carbon nanofibers for use in the capacitive desalination of water

Bethwel K Tarus, Yusufu A C Jande, Karoli N Njau

2022, 37(6): 1066-1088. doi: 10.1016/S1872-5805(22)60645-0

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Capacitive deionization (CDI) has rapidly become a promising approach for water desalination. The technique removes salt from water by applying an electric potential between two porous electrodes to cause adsorption of charged species on the electrode surfaces. The nature of CDI favors the use of nanostructured porous carbon materials with high specific surface areas and appropriate surface functional groups. Electrospun carbon nanofibers (CNFs) are ideal as they have a high specific surface area and surface characteristics for doping/grafting with electroactive agents. Compared with powdered materials, CNF electrodes are free-standing and don’t require binders that increase resistivity. CNFs with an appropriate distribution of mesopores and micropores have better desalination performance. Compositing CNFs with faradaic materials improve ion storage by adding pseudocapacitance to the electric double layer capacitance. The use of electrospun CNFs as electrodes for CDI is summarized with emphasis on the major precursor materials used in their preparation and structure modification, and their relations to the performance in salt electrosorption.

Graphdiyne: Synthesis, modification and application of a two-dimensional carbonaceous material

ZHANG Ting, WANG Yu-jing, YU Ling-min, SHI Li-min, CHAI Shou-ning, HE Chi

2022, 37(6): 1089-1115. doi: 10.1016/S1872-5805(22)60653-X

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Graphdiyne is a new kind of two-dimensional carbonaceous material that is composed of sp and sp² hybridized carbon atoms. The highly conjugated and adjustable carbocyclic molecular structure gives it special physicochemical properties, which also facilitate its functional modification and wide application. In the past ten years, there has been extensive theoretical and experimental research on graphdiyne, and a series of important advances has been made in many fields. The properties of graphdiyne are briefly introduced, and its main synthesis methods with different morphologies are summarized, including Glaser-Hay cross-coupling, chemical vapor deposition, van der Waals epitaxial growth, thermal explosion, interface- confined synthesis and a bipolar electrochemical method. Theoretical calculations and experimental studies on non-metal and metal atom doping and chemical group modification are summarized, and their corresponding effects on the graphdiyne properties are reviewed. Finally, urgent problems and challenges in the development of graphdiyne are discussed. This review provides fundamental information on graphdiyne and guidance for the design of its functionalized forms.

Incorporating TiO₂ nanoparticles into the multichannels of electrospun carbon fibers to increase the adsorption of polysulfides in room temperature sodium-sulfur batteries

YE Xin, LI Zhi-qi, SUN Hao, WU Ming-xia, AN Zhong-xun, PANG Yue-peng, YANG Jun-he, ZHENG Shi-you

2022, 37(6): 1116-1124. doi: 10.1016/S1872-5805(22)60607-3

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With the rapid development of electric vehicles and large-scale power grids, lithium-ion batteries inevitably face the problem that their limited energy density and high cost cannot meet the growing demand. Room temperature sodium-sulfur (RT Na-S) batteries, which have the potential to replace lithium-ion batteries, have become a focus of attention. However, the challenging problem of their poor cycling performance cause by the “shuttle effect” of the reaction intermediates (sodium polysulfides) needs to be addressed. We report a method to incorporate TiO₂ nano particles into the multichannels of electrospun carbon fibers (TiO₂@MCCFs) to stabilize the sulfur compounds and produce high-performance RT Na-S batteries. The TiO₂@MCCFs were prepared by electrospinning followed by heat treatment, and were infiltrated by molten sulfur to fabricate S/TiO₂@MCCF cathode materials. The addition of the TiO₂ nanoparticles increases the affinity of cathode materials for polysulfides and promotes the conversion of polysulfides to lower order products. This was verified by DFT calculations. A S/TiO₂@MCCF cathode with a S content of 54% has improved electrochemical rate and cycling performance, with a specific capacity of 445.1 mAh g⁻¹ after 100 cycles at 0.1 A g⁻¹ and a nearly 100% Coulombic efficiency. Even at 2 A g⁻¹, the cathode still has a capacity of 300.5 mAh g⁻¹ after 500 cycles. This work provides a new way to construct high performance RT Na-S battery cathodes.

Microstructures and electrochemical properties of coconut shell-based hard carbons as anode materials for potassium ion batteries

HUANG Tao, PENG Da-chun, CHEN Zui, XIA Xiao-hong, CHEN Yu-xi, LIU Hong-bo

2022, 37(6): 1125-1134. doi: 10.1016/S1872-5805(21)60069-0

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Hard carbons have recently attracted wide interest as anode materials for potassium ion batteries (PIBs) because of their high reversible capacity. But, their high preparation cost and poor cycling stability prevent their practical use. Coconut shell-derived hard carbons (CSHCs) were prepared from waste biomass coconut shell using a one-step carbonization method, and were used as anode materials for potassium ion batteries. The effects of the carbonization temperature on the microstructures and electrochemical properties of the CSHCs were investigated by X-ray diffraction, nitrogen adsorption, Raman spectroscopy, scanning electron microscopy, transmission electron microscopy, and cyclic voltammetry, etc. Results indicate that the CSHC carbonized at 1 000 °C (CSHC-10) has a suitable graphite microcrystal size, pore structure and surface defect content, and has the best electrochemical performance. Specifically, it has a high reversible specific capacity of 254 mAh·g⁻¹ at 30 mA·g⁻¹ with an initial Coulombic efficiency of 75.0%, and the capacity retention rates are 87.5% after 100 cycles and 75.9% after 400 cycles at 100 mA·g⁻¹, demonstrating its excellent potassium storage performance.

Oxygen-incorporated carbon nitride porous nanosheets for highly efficient photoelectrocatalytic CO₂ reduction to formate

WANG Hong-zhi, ZHAO Yue-zhu, YANG Zhong-xue, BI Xin-ze, WANG Zhao-liang, WU Ming-bo

2022, 37(6): 1135-1144. doi: 10.1016/S1872-5805(22)60619-X

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Using CO₂ as a renewable carbon source for the production of high-value-added fuels and chemicals has recently received global attention. The photoelectrocatalytic (PEC) CO₂ reduction reaction (CO₂RR) is one of the most realistic and attractive ways of achieving this, and can be realized effectively under sunlight illumination at a low overpotential. Oxygen-incorporated carbon nitride porous nanosheets (CNs) were synthesized from urea or melamine by annealing in nitrogen or N₂/O₂ gas mixtures. They were used as the photoanode with Bi₂CuO₄ as the photocathode to realize PEC CO₂ reduction to the formate. The electrical conductivity and the photoelectric response of the CNs were modified by changing the oxygen source. Oxygen in CNs obtained from an oxygen-containing precursor improved the conductivity because of its greater electronegativity, whereas oxygen in CNs obtained from the calcination atmosphere had a lower photoelectric response due to a down shift of the energy band structure. The CN prepared by annealing urea, which served as the source of oxygen and nitrogen, at 550 °C for 2 h in nitrogen is the best. It has a photocurrent density of 587 μA cm⁻² and an activity of PEC CO₂ reduction to the formate of 273.56 µmol cm⁻² h⁻¹, which is nearly 19 times higher than a conventional sample. The CN sample shows excellent stability with the photocurrent remaining constant for 24 h. This work provides a new way to achieve efficient catalysts for PEC CO₂ reduction to the formate, which may be expanded to different PEC reactions using different cathode catalysts.

Preparation of molded biomass carbon from coffee grounds and its CH₄/N₂ separation performance

GAO Yu-zhou, Xu Shuang, WANG Cheng-tong, ZHANG Xue-jie, LIU Ru-shuai, LU An-Hui

2022, 37(6): 1145-1153. doi: 10.1016/S1872-5805(22)60626-7

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Coffee grounds are promising precursors for excellent porous carbon adsorbents. During the preparation of the porous carbons, sodium silicate was used as a binder and pore-forming agent, and extrusion molding technology was used to prepare them in a columnar form. After carbonization, steam activation and silica removal by alkaline washing, high-strength columnar porous carbon adsorbents (CGCs) were obtained. Their CH₄/N₂ separation performance was studied by multicomponent breakthrough experiments. The Brunauer-Emmett-Teller (BET) surface area of CGC-1.5 (where 1.5 is the mass ratio of a 9 wt% sodium silicate aqueous solution to the coffee grounds) is 527 m²·g⁻¹. Both the N₂ and CO₂ adsorption isotherms show that the CGCs are rich in micropores and mesopores, with the micropores mainly centered at about 0.48 nm. FT-IR results show that CGC-1.5 has abundant oxygen-containing functional groups. At 298 K and 1 bar, its equilibrium adsorption capacity for CH₄ is 0.87 mmol·g⁻¹, and the separation selectivity for a CH₄/N₂ mixture (3/7, vol/vol) is 10.3, which is better than most biomass-based porous carbon adsorbents and crystalline materials. Dynamic breakthrough tests show that CGC-1.5 has an excellent CH₄/N₂ separation performance at both high and atmospheric pressures. The dynamic selectivities at 298 K, 1.1 bar and 5 bar are 10.4 and 17.9, respectively. The adsorption capacity is unchanged after 10 adsorption-desorption cycles. The mechanical strength of CGC-1.5 is as high as 123 N·cm⁻¹, which meets the criteria of industrial applications.

A flexible hard carbon microsphere/MXene film as a high-performance anode for sodium-ion storage

CAO Hai-liang, YANG Liang-tao, ZHAO Min, LIU Pei-zhi, GUO Chun-li, XU Bing-she, GUO Jun-jie

2022, 37(6): 1154-1162. doi: 10.1016/S1872-5805(22)60616-4

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Hard carbon is considered the most promising anode material for sodium-ion batteries, but its volume change during sodiation/desodiation limits its cycle life. Hard carbon microspheres (HCSs) with no binder were composited with a MXene film to form an electrode and its sodium storage properties were studied. The microspheres were prepared using Shanxi aged vinegar as a liquid carbon source. Two-dimensional Ti₃C₂T_x MXene (T is a functional group) was used as a multifunctional conductive binder to fabricate the flexible electrodes. Remarkably, because of the three-dimensional conductive network, the HCS/Ti₃C₂T_x film electrode has a high capacity of 346 mAh g⁻¹, excellent rate performance and outstanding cycling stability over 1 000 cycles. This remarkable electrochemical performance indicates that the flexible film is a very promising anode for next-generation sodium-ion batteries.

Preparation and lithium storage of anthracite-based graphite anode materials

LI Yuan, TIAN Xiao-dong, SONG Yan, YANG Tao, WU Shi-jie, LIU Zhan-jun

2022, 37(6): 1163-1171. doi: 10.1016/S1872-5805(21)60057-4

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Several graphite samples with different microstructures were prepared from anthracite using industrial silicon powders as catalyst. The mechanism of the catalytic reaction and the electrochemical properties of the prepared coal-based graphite in lithium anodes were investigated. The correlation between the microstructure and the properties of the graphite is discussed. Results show that the sample with 5% silicon (G-2800-5%) has the best lithium storage. It has the well-developed graphitic structure with a degree of graphitization of 91.5% as determined from the interlayer spacing. When used as an anode material, a high reversible capacity of 369.0 mAh g⁻¹ was achieved at 0.1 A g⁻¹ and its reversible capacity was 209.0 mAh g⁻¹ at a current density of 1 A g⁻¹. It also exhibits good cycling stability with a capacity retention of 92.2% after 200 cycles at 0.2 A g⁻¹. The highly developed graphite structure, which is favorable for the formation of a stable SEI and therefore reduces lithium ion loss, is responsible for the superior electrochemical performance.

Coal-based graphene as a promoter of TiO₂ catalytic activity for the photocatalytic degradation of organic dyes

LIU Guo-yang, LI Ke-ke, JIA Jia, ZHANG Ya-ting

2022, 37(6): 1172-1182. doi: 10.1016/S1872-5805(21)60047-1

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Graphene oxide (GO) obtained from coal-based graphite by the Hummers method was hydrothermally treated to obtain reduced GO (rGO). TiO₂ was mixed with aqueous suspensions of GO and rGO and dried at 70 ^oC to obtain GO-TiO₂ and rGO-TiO₂ with 95% (mass fraction) TiO₂. TiO₂ was also combined with a GO suspension by hydrothermal treatment to obtain rGO-hTiO₂ with 95% TiO₂. The three hybrids were used as catalysts for the photocatalytic degradation of rhodamine B (Rh B) and methyl orange (MO). Of the three materials, rGO-hTiO₂ had the highest catalytic activity for the degradation of Rh B and MO under visible light irradiation. The reasons for having the best catalytic activity are that the incorporation of rGO into TiO₂ helps increase its adsorption capacities for Rh B and MO as evidenced by adsorption in dark, and a narrowing of the TiO₂ band gap as revealed by diffuse UV reflectance spectroscopy. This reduces the rate of recombination of electron–hole pairs by there being intimate contact between the TiO₂ particles and rGO, forming Ti-O-C bonds as confirmed by XPS, with the TiO₂ particles being uniformly decorated on the rGO sheets.

Chemical vapor deposition of two-dimensional transition metal sulfides on carbon paper for electrocatalytic hydrogen evolution

WANG Ke, TANG Fei, YAO Xiao-zhang, Hitanshu Kumar, GAN Lin

2022, 37(6): 1183-1192. doi: 10.1016/S1872-5805(21)60078-1

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Hydrogen is considered the most likely alternative clean energy fuel to traditional fossil fuels. One of the most attractive hydrogen production strategies is water splitting, but the need for expensive Pt precious metal catalysts to catalyze the hydrogen evolution reaction (HER) is a problem. Recently, two-dimensional transition metal dichalcogenides (TMDs), especially MoS₂, have attracted intense interest as a non-precious metal HER catalyst due to their low cost and relatively high catalytic activity. However, their poor electron conductivity and the limited number of active sites at their edges have greatly limited their overall catalytic performance. We report the direct growth of three representative TMDs (MoS₂, NbS₂ and WS₂) on a conductive carbon paper substrate using chemical vapor deposition and have studied the effects of temperature and gas flow rate on their morphology and structure. All the as-grown TMDs have a 2D nanosheet morphology and were aligned perpendicular to the carbon paper. The WS₂ nanosheets had the smallest sheet size with a diameter of ca. 100-200 nm and, more interestingly, were assembled into a one-dimensional nanofiber, leading to the highest HER activity. Additional electrochemical cathodic activation further improved the HER activity of the TMDs, and the structural changes after the activation were investigated by TEM combined with in-situ electrochemical Raman spectroscopy. The activated NbS₂ contained large triangular or truncated triangular S vacancy areas, which is distinctly different from the individual S vacancies in MoS₂.

Preparation and electrochemical properties of Ni(OH)₂/graphitized carbon nitride/graphene ternary composites

LIU Bin, WANG Yan-min, MA Qian, CUI Jin-long, ZHANG Yong-qiang, HE Wen-xiu

2022, 37(6): 1193-1200. doi: 10.1016/S1872-5805(22)60625-5

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Ni(OH)₂/graphitized carbon nitride(g-C₃N₄)/reduced graphene oxide (RGO) ternary synthetics were prepared by a hydrothermal method. The effect of different mass ratios of the three components on the microstructure, morphology and electrochemical properties of the synthetics was investigated. The outside microstructure and extent of redox of the material were characterized by XRD, SEM, FTIR, nitrogen adsorption and TEM. The composite properties of the synthetics were examined use cyclic voltammetry(CV), galvanostatic charge-discharge(GCD) and electrochemical impedance spectroscopy(EIS). The consequences reveal that the ternary composite represents three-dimensional slice space interlaced structure when the quality proportion of Ni(OH)₂, g-C₃N₄ and RGO are 16∶1∶1, and the ΔE is 0.218 V. When the current density is 1 A/g, the specific capacitance of the synthetic material is 516.9 F/g. After 3 000 cycles of charge-discharge, the capacity retention rate is 74.3%, which revealedoutstanding electrochemical performance.

2022 Vol. 37, No. 6

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