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2024 年 2 期中文目次

2024, 39(2): 1-1.

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2024年 2 期英文目次

2024, 39(2): 1-7.

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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

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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

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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.

石墨烯基材料在电磁屏蔽领域的研究进展

杨赏娟, 曹赟, 贺艳兵, 吕伟

2024, 39(2): 223-239. doi: 10.1016/S1872-5805(24)60840-1

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通信技术在为人类的生活带来便利的同时，其产生的电磁辐射对社会安全、人体健康产生的危害也受到了社会各界的广泛关注，宽屏蔽范围、高吸收效率和高稳定性的电磁屏蔽材料逐渐成为研究热点。石墨烯是一种导电性高、比表面积大且可调控性高的轻质材料，可有效实现电磁衰减，保护精密电子设备和人体健康，在电磁屏蔽领域具有广阔的应用前景。本综述从电磁屏蔽的基本原理与石墨烯基材料的结构特性角度，阐述了石墨烯及其衍生物的电磁屏蔽特点，总结了结构调控以及表面异质化、复合化策略在电磁屏蔽领域的应用。结构调控有利于提高石墨烯基材料对电磁波的吸收损耗和多重反射损耗；表面异质化和复合化策略有利于提高石墨烯基材料的界面极化和磁特性，从而加强对电磁波的吸收损耗和磁损耗。总结了石墨烯基电磁屏蔽材料的改性方法，旨在为开发新一代绿色、轻薄、高屏蔽带宽的电磁屏蔽材料提供启发，指明石墨烯基电磁屏蔽材料的未来发展方向。

三维整体式碳基光热转换材料在太阳能界面水蒸发中的应用研究进展

韩悦, 张鹏, 赵晓明

2024, 39(2): 240-253. doi: 10.1016/S1872-5805(24)60827-9

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光热驱动的海水淡化技术被认为是最具潜力的解决全球淡水资源短缺难题的方法之一。其中，太阳能界面水蒸发（SVG）是海水淡化效率的核心过程，是保证光热海水淡化技术具有能量转换效率高、设备简单、成本效益高的关键。在所有高效SVG候选材料中，三维整体式碳基光热转换材料具有成本低、吸光效率高、结构可调性好、水蒸发速率高、无二次污染等优点。本综述首先简述了SVG 的基本原理，以此为依据介绍了高效 SVG 材料的工作机制和设计原则，最后系统归纳和概述了4种不同类型的三维整体式碳基光热转换材料的研究进展。本综述为未来三维整体式碳基光热转换材料的构建及其在SVG领域的应用研究提供理论基础和研究指导。

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.

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·m⁻¹·K⁻¹, 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 cm⁻², the power density was 194 W cm⁻², and the energy density was 1997 mWh cm⁻², 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 g⁻¹ for 2000 cycles under 5.0 A g⁻¹ with an ultralow average capacity drop of 0.002% per cycle and an exceptional rate capability of 614 mAh g⁻¹ at 10.0 A g⁻¹. In SIBs, it also produces a significantly better electrochemical performance (reversible capacity of 242 mAh g⁻¹ under 2.0 A g⁻¹ for 2000 cycles and 261 mAh g⁻¹ under 5.0 A g⁻¹). 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·m⁻¹·K⁻¹ and 2.16 GPa at 309 ^oC to 1 078 W·m⁻¹·K⁻¹ 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.

柔性多功能Fe₂O₃/CC正极宿主实现高效吸附与催化多硫化物的锂硫电池

田真, 薛磊磊, 丁红元

2024, 39(2): 345-353. doi: 10.1016/S1872-5805(24)60825-5

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锂硫电池因其高能量密度和低成本而成为最有发展前景的电化学储能器件之一。然而，多硫化物的“穿梭效应”、硫导电率低是锂硫电池商业化面临的主要挑战。本工作中，以Fe(NO)₃·9H₂O为铁源，NH₄F为表面活性剂，通过简单的水热及煅烧处理制备了Fe₂O₃纳米棒修饰炭布（CC）的柔性Fe₂O₃/CC复合材料。其中，Fe₂O₃中介孔的存在有利于电解质的渗透和充放电过程中锂离子的传输和扩散，同时其密集阵列暴露出的丰富活性位点可以实现多硫化物的高效吸附和快速转化，降低多硫化物的穿梭效应。电化学分析显示：Fe₂O₃/CC正极在0.1 C（1 C=1672 mA g⁻¹）的电流密度下具有1250 mAh g⁻¹的高放电比容量，经100圈循环后比容量保持在789 mAh g⁻¹。在2 C的倍率下循环1000圈后仍能达到576 mAh g⁻¹的放电比容量，容量保持率为70%，明显优于对比样品。因此，Fe₂O₃/CC能够很好地抑制多硫化物的穿梭，提高电池倍率性能和循环稳定性。

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·mol⁻¹ 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·mol⁻¹ 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%.

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