Pub Date : 2024-11-02DOI: 10.1016/j.carbon.2024.119795
Guansheng Ma , Yuhao Liu , Kaili Zhang , Guangyu Qin , Yuefeng Yan , Tao Zhang , Xiaoxiao Huang
The tunable energy gap and distinctive layered configuration of transition metal dichalcogenides (TMDs) has sparked considerable interest in their capabilities for electromagnetic wave absorption. As a significant TMD, vanadium selenide (VSe2) is characterized by a superior electrical conductivity (1 × 10−3 S/m) and an expanded interlayer distance, which are advantageous for electromagnetic wave absorption performance. Nevertheless, the current research on VSe2 in electromagnetic wave absorption is relatively limited. In this study, flower-like VSe2 and shape-tunable VSe2/reduced graphene oxide (rGO) composites were fabricated via a simple solvothermal method, and the effect of their morphology on electromagnetic wave absorption performances was investigated. The VSe2/rGO composites exhibited remarkable electromagnetic wave absorption properties at a thickness of 2.01 mm, with a reflection loss value (RL) of up to −79.50 dB, and an effective absorption bandwidth (EAB) of 5.2 GHz (1.45 mm). This research has identified a novel approach to the study of TMDs in the field of electromagnetic wave absorption.
{"title":"Shape-tunable vanadium selenide/reduced graphene oxide composites with excellent electromagnetic wave absorption performance","authors":"Guansheng Ma , Yuhao Liu , Kaili Zhang , Guangyu Qin , Yuefeng Yan , Tao Zhang , Xiaoxiao Huang","doi":"10.1016/j.carbon.2024.119795","DOIUrl":"10.1016/j.carbon.2024.119795","url":null,"abstract":"<div><div>The tunable energy gap and distinctive layered configuration of transition metal dichalcogenides (TMDs) has sparked considerable interest in their capabilities for electromagnetic wave absorption. As a significant TMD, vanadium selenide (VSe<sub>2</sub>) is characterized by a superior electrical conductivity (1 × 10<sup>−3</sup> S/m) and an expanded interlayer distance, which are advantageous for electromagnetic wave absorption performance. Nevertheless, the current research on VSe<sub>2</sub> in electromagnetic wave absorption is relatively limited. In this study, flower-like VSe<sub>2</sub> and shape-tunable VSe<sub>2</sub>/reduced graphene oxide (rGO) composites were fabricated via a simple solvothermal method, and the effect of their morphology on electromagnetic wave absorption performances was investigated. The VSe<sub>2</sub>/rGO composites exhibited remarkable electromagnetic wave absorption properties at a thickness of 2.01 mm, with a reflection loss value (RL) of up to −79.50 dB, and an effective absorption bandwidth (EAB) of 5.2 GHz (1.45 mm). This research has identified a novel approach to the study of TMDs in the field of electromagnetic wave absorption.</div></div>","PeriodicalId":262,"journal":{"name":"Carbon","volume":"232 ","pages":"Article 119795"},"PeriodicalIF":10.5,"publicationDate":"2024-11-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142655840","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-02DOI: 10.1016/j.carbon.2024.119796
Leslie R. Sigmon , Jonathan Catazaro , Mohammed Abdel-Rahman , Casey Smith , Carsten Prasse , D. Howard Fairbrother
In this work, molecular-level events accompanying the photobleaching of carbon dots (CDs) synthesized from ethylenediamine and citric acid (CACDs) were identified using solution-phase NMR. By combining quantitative 13C NMR data with fluorescence measurements we show that this new approach is capable of identifying not only molecular fluorophores in CACDs, but also their contribution to the overall CACD fluorescence and their relative photostability. Specifically, imidazo[1,2-a]pyridine-7-carboxylic acid (IPCA) is found to be the dominant (84 %) species responsible for fluorescence in CACDs along with a second undetermined source, most likely associated with the aromatic core which is significantly (approximately 20 times) more photostable than IPCA. The presence of these two fluorescent species with different photostabilities rationalizes not only the photobleaching kinetics but also the evolution of the fluorescence spectrum during photobleaching Diffusion-ordered spectroscopy (DOSY) also reveals that all of the IPCA molecules are trapped within or covalently bound to the CACD, but are not present as isolated molecules freely rotating in solution. Singlet oxygen is confirmed as a key ROS responsible for photobleaching, with prototypical photoproducts identified from mass spectrometry studies of citrazinic acid. Quantitative 13C NMR of CACDs is possible because their extremely high colloidal stability enables high concentrations (667 mg/mL) to remain stable in solution. The approach described in this study could be extended to identify the structure of chromophores in other CDs and interrogate molecular level processes that accompany CD sensing.
{"title":"Interrogating the photoluminescent properties of carbon dots using quantitative 13C NMR combined with systematic photobleaching","authors":"Leslie R. Sigmon , Jonathan Catazaro , Mohammed Abdel-Rahman , Casey Smith , Carsten Prasse , D. Howard Fairbrother","doi":"10.1016/j.carbon.2024.119796","DOIUrl":"10.1016/j.carbon.2024.119796","url":null,"abstract":"<div><div>In this work, molecular-level events accompanying the photobleaching of carbon dots (CDs) synthesized from ethylenediamine and citric acid (CACDs) were identified using solution-phase NMR. By combining quantitative <sup>13</sup>C NMR data with fluorescence measurements we show that this new approach is capable of identifying not only molecular fluorophores in CACDs, but also their contribution to the overall CACD fluorescence and their relative photostability. Specifically, imidazo[1,2-a]pyridine-7-carboxylic acid (IPCA) is found to be the dominant (84 %) species responsible for fluorescence in CACDs along with a second undetermined source, most likely associated with the aromatic core which is significantly (approximately 20 times) more photostable than IPCA. The presence of these two fluorescent species with different photostabilities rationalizes not only the photobleaching kinetics but also the evolution of the fluorescence spectrum during photobleaching Diffusion-ordered spectroscopy (DOSY) also reveals that all of the IPCA molecules are trapped within or covalently bound to the CACD, but are not present as isolated molecules freely rotating in solution. Singlet oxygen is confirmed as a key ROS responsible for photobleaching, with prototypical photoproducts identified from mass spectrometry studies of citrazinic acid. Quantitative <sup>13</sup>C NMR of CACDs is possible because their extremely high colloidal stability enables high concentrations (667 mg/mL) to remain stable in solution. The approach described in this study could be extended to identify the structure of chromophores in other CDs and interrogate molecular level processes that accompany CD sensing.</div></div>","PeriodicalId":262,"journal":{"name":"Carbon","volume":"232 ","pages":"Article 119796"},"PeriodicalIF":10.5,"publicationDate":"2024-11-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142655832","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
How to tailor electromagnetic parameters of multi-component materials is the fundamental issues for low-frequency electromagnetic wave absorbers (EMA). However, there remains a challenge to accurately elucidate the impact of respective components at heterogeneous interfaces on the EMAs, not to mentioning the further quantitative contribution of the interfacial effect to the electromagnetic loss. In this paper, we for the first time separated the Fe3O4(111)/C heterogeneous interface of Fe3O4@C via a controllable interfacial separation strategy, meanwhile ensuring the consistent microstructure and the ratio of each component, as well as the unchanged macroscopic structure of the particles. Once all potential influences on electromagnetic parameters have been independently studied, the unique difference in heterogeneous interfaces enabled us to quantitatively evaluate the effect of them on electromagnetic parameters. Both experimental and density functional theory (DFT) calculation results consistently demonstrate that the Fe3O4(111)/C heterointerface increases carrier concentration and conductivity, thereby enhancing the imaginary part of the dielectric constant. Very distinguished from traditional interfacial polarisation mechanism presented in previous publications, this study introduces a novel interfacial loss mechanism primarily characterized by conductivity loss, which is rigorously investigated in a quantitative way. This discovery offers a novel approach for designing controllable heterogeneous interfaces and manipulating electromagnetic parameters in multicomponent EMAs.
如何定制多组分材料的电磁参数是低频电磁波吸收器(EMA)的基本问题。然而,准确阐明异质界面上各组分对 EMA 的影响仍是一个挑战,更不用说界面效应对电磁损耗的进一步定量贡献了。在本文中,我们首次通过可控的界面分离策略分离了 Fe3O4@C 的 Fe3O4(111)/C 异构界面,同时确保了微观结构和各组分比例的一致性,以及颗粒宏观结构的不变。在对电磁参数的所有潜在影响因素进行独立研究之后,异质界面的独特差异使我们能够定量评估它们对电磁参数的影响。实验和密度泛函理论(DFT)计算结果一致表明,Fe3O4(111)/C 异质界面增加了载流子浓度和电导率,从而提高了介电常数的虚部。与以往出版物中介绍的传统界面极化机制截然不同,本研究引入了以电导率损失为主要特征的新型界面损失机制,并对其进行了严格的定量研究。这一发现为设计可控异质界面和操纵多组分 EMA 中的电磁参数提供了一种新方法。
{"title":"Quantifying heterogeneous interface effect of Fe3O4(111)/C for enhanced low-frequency electromagnetic wave absorption","authors":"Yukang Zhou, Chuanhao Tang, Siyue Li, Xiaohan Wu, Peiyuan Zuo, Ruoqi Wang, Siyu Rao, Qixin Zhuang","doi":"10.1016/j.carbon.2024.119792","DOIUrl":"10.1016/j.carbon.2024.119792","url":null,"abstract":"<div><div>How to tailor electromagnetic parameters of multi-component materials is the fundamental issues for low-frequency electromagnetic wave absorbers (EMA). However, there remains a challenge to accurately elucidate the impact of respective components at heterogeneous interfaces on the EMAs, not to mentioning the further quantitative contribution of the interfacial effect to the electromagnetic loss. In this paper, we for the first time separated the Fe<sub>3</sub>O<sub>4</sub>(111)/C heterogeneous interface of Fe<sub>3</sub>O<sub>4</sub>@C via a controllable interfacial separation strategy, meanwhile ensuring the consistent microstructure and the ratio of each component, as well as the unchanged macroscopic structure of the particles. Once all potential influences on electromagnetic parameters have been independently studied, the unique difference in heterogeneous interfaces enabled us to quantitatively evaluate the effect of them on electromagnetic parameters. Both experimental and density functional theory (DFT) calculation results consistently demonstrate that the Fe<sub>3</sub>O<sub>4</sub>(111)/C heterointerface increases carrier concentration and conductivity, thereby enhancing the imaginary part of the dielectric constant. Very distinguished from traditional interfacial polarisation mechanism presented in previous publications, this study introduces a novel interfacial loss mechanism primarily characterized by conductivity loss, which is rigorously investigated in a quantitative way. This discovery offers a novel approach for designing controllable heterogeneous interfaces and manipulating electromagnetic parameters in multicomponent EMAs.</div></div>","PeriodicalId":262,"journal":{"name":"Carbon","volume":"232 ","pages":"Article 119792"},"PeriodicalIF":10.5,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142573270","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-01DOI: 10.1016/j.carbon.2024.119789
Shi Jin , Haixia Huang , Xianlong Zhang , Xueping Wu , Kui Wang
The increasing demand for advanced detection technologies has highlighted the need for materials with efficient electromagnetic wave absorption (EMWA) and thermal stealth, crucial for radar-infrared compatibility. In this study, we synthesized honeycomb-like porous MnO@C aerogels via the sol-gel method, achieving remarkable multifunctional properties. The MnO@C-10 wt% (10 wt% Mn) exhibited a minimum reflection loss (RLmin) of −54.08 dB at an optimum thickness of 3.2 mm and a maximum effective absorption bandwidth (EAB) of 5.96 GHz at 2.6 mm. Additionally, it demonstrated a significant reduction in radar scattering cross section (RCS) of 27.2 dB m2 at 0o detection angle. The material's infrared stealth was confirmed by its ability to maintain a surface color consistent with its surroundings and a surface temperature of approximately 30 °C after heating at 90 °C for 1 h, highlighting its superior infrared stealth and thermal insulation capabilities. Furthermore, MnO@C-10 wt% showed exceptional mechanical robustness, supporting a load of 57,594 times its weight, and exhibited excellent flame resistance, retaining its integrity under an alcohol lamp flame. The synergistic interaction between MnO and biomass-derived carbon offers a novel approach to developing multifunctional materials with integrated radar and infrared stealth functionalities, paving the way for advanced stealth technologies.
对先进探测技术日益增长的需求凸显了对高效电磁波吸收(EMWA)和热隐身材料的需求,这对雷达-红外兼容至关重要。在本研究中,我们通过溶胶-凝胶法合成了蜂窝状多孔 MnO@C 气凝胶,实现了显著的多功能特性。在最佳厚度为 3.2 mm 时,MnO@C-10 wt%(10 wt% Mn)的最小反射损耗(RLmin)为 -54.08 dB;在 2.6 mm 时,最大有效吸收带宽(EAB)为 5.96 GHz。此外,它还显著降低了雷达散射截面(RCS),在 0o 检测角时降低了 27.2 dB m2。该材料的红外隐身性能得到了证实,其表面颜色与周围环境保持一致,在 90 °C 下加热 1 小时后,表面温度约为 30 °C,凸显了其卓越的红外隐身和隔热能力。此外,MnO@C-10 wt%显示出卓越的机械坚固性,可承受其重量 57,594 倍的载荷,并表现出优异的阻燃性,在酒精灯火焰下仍能保持其完整性。氧化锰与生物质衍生碳之间的协同作用为开发集成雷达和红外隐身功能的多功能材料提供了一种新方法,为先进的隐身技术铺平了道路。
{"title":"Multifunctional chitosan-derived MnO@C aerogels with high radar-infrared compatible stealth","authors":"Shi Jin , Haixia Huang , Xianlong Zhang , Xueping Wu , Kui Wang","doi":"10.1016/j.carbon.2024.119789","DOIUrl":"10.1016/j.carbon.2024.119789","url":null,"abstract":"<div><div>The increasing demand for advanced detection technologies has highlighted the need for materials with efficient electromagnetic wave absorption (EMWA) and thermal stealth, crucial for radar-infrared compatibility. In this study, we synthesized honeycomb-like porous MnO@C aerogels via the sol-gel method, achieving remarkable multifunctional properties. The MnO@C-10 wt% (10 wt% Mn) exhibited a minimum reflection loss (RL<sub>min</sub>) of −54.08 dB at an optimum thickness of 3.2 mm and a maximum effective absorption bandwidth (EAB) of 5.96 GHz at 2.6 mm. Additionally, it demonstrated a significant reduction in radar scattering cross section (RCS) of 27.2 dB m<sup>2</sup> at 0<sup>o</sup> detection angle. The material's infrared stealth was confirmed by its ability to maintain a surface color consistent with its surroundings and a surface temperature of approximately 30 °C after heating at 90 °C for 1 h, highlighting its superior infrared stealth and thermal insulation capabilities. <span>Furthermore</span>, MnO@C-10 wt% showed exceptional mechanical robustness, supporting a load of 57,594 times its weight, and exhibited excellent flame resistance, retaining its integrity under an alcohol lamp flame. The synergistic interaction between MnO and biomass-derived carbon offers a novel approach to developing multifunctional materials with integrated radar and infrared stealth functionalities, paving the way for advanced stealth technologies.</div></div>","PeriodicalId":262,"journal":{"name":"Carbon","volume":"232 ","pages":"Article 119789"},"PeriodicalIF":10.5,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142656268","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-01DOI: 10.1016/j.carbon.2024.119791
Sijin Dong , Xin Gu , Yapeng Li , Longfei Du , Xinyu Lv , Fei Pang , Akang Cui , Kaiyuan Zhang , Mengdi Zhang , Qingshan Zhao , Bin Wang , Han Hu , Mingbo Wu
Enhancing carbon materials' low-potential K+ intercalation capacity is an essential topic in potassium-ion batteries (PIBs). Nevertheless, conventional methods effectively improve performance by increasing the surface area and active sites, but always at the expense of initial coulombic efficiency (ICE). Herein, an efficient and convenient strategy is proposed to construct self-doped defective carbon nanosheets (SDCS) using the mechanical ball-milling technique. This in situ defect engineering increases K+ intercalation sites and shortens the ionic pathway, enhancing the ionic intercalation kinetics, specific capacity, and ICE. As expected, the SDCS-24 electrode delivers an ultra-high low-potential capacity of 314.3 mAh g−1 below 0.5 V, high ICE of 76.1 %, and long-term cycle stability (300.1 mAh g−1 after 1800 cycles at 1 C). The K+ storage mechanism is determined by ex situ XRD and in situ Raman. The full-cell with 3,4,9,10-Perylenetetracarboxylic dianhydride cathode and SDCS-24 anode further confirms its promising application. This work presents a strategy for designing self-doped defective carbons in situ and provides insights into the potassium storage mechanism at low potential.
提高碳材料的低电位 K+ 插层能力是钾离子电池(PIB)的一个重要课题。然而,传统方法通过增加表面积和活性位点来有效提高性能,但总是以牺牲初始库仑效率(ICE)为代价。本文提出了一种高效便捷的策略,利用机械球磨技术构建自掺杂缺陷碳纳米片(SDCS)。这种原位缺陷工程增加了 K+ 插层位点,缩短了离子通道,从而提高了离子插层动力学、比容量和 ICE。正如预期的那样,SDCS-24 电极在 0.5 V 以下具有 314.3 mAh g-1 的超高低电位容量、76.1 % 的高 ICE 和长期循环稳定性(在 1 C 下循环 1800 次后达到 300.1 mAh g-1)。K+ 储存机制是通过原位 XRD 和原位拉曼来确定的。使用 3,4,9,10-Perylenetetracarboxylic dianhydride 阴极和 SDCS-24 阳极的全电池进一步证实了其应用前景。这项工作提出了一种原位设计自掺杂缺陷碳的策略,并为低电位下的钾存储机制提供了深入的见解。
{"title":"Mechanically induced surface defect engineering in expanded graphite to boost the low-voltage intercalation kinetics for advanced potassium-ion batteries","authors":"Sijin Dong , Xin Gu , Yapeng Li , Longfei Du , Xinyu Lv , Fei Pang , Akang Cui , Kaiyuan Zhang , Mengdi Zhang , Qingshan Zhao , Bin Wang , Han Hu , Mingbo Wu","doi":"10.1016/j.carbon.2024.119791","DOIUrl":"10.1016/j.carbon.2024.119791","url":null,"abstract":"<div><div>Enhancing carbon materials' low-potential K<sup>+</sup> intercalation capacity is an essential topic in potassium-ion batteries (PIBs). Nevertheless, conventional methods effectively improve performance by increasing the surface area and active sites, but always at the expense of initial coulombic efficiency (ICE). Herein, an efficient and convenient strategy is proposed to construct self-doped defective carbon nanosheets (SDCS) using the mechanical ball-milling technique. This in situ defect engineering increases K<sup>+</sup> intercalation sites and shortens the ionic pathway, enhancing the ionic intercalation kinetics, specific capacity, and ICE. As expected, the SDCS-24 electrode delivers an ultra-high low-potential capacity of 314.3 mAh g<sup>−1</sup> below 0.5 V, high ICE of 76.1 %, and long-term cycle stability (300.1 mAh g<sup>−1</sup> after 1800 cycles at 1 C). The K<sup>+</sup> storage mechanism is determined by ex situ XRD and in situ Raman. The full-cell with 3,4,9,10-Perylenetetracarboxylic dianhydride cathode and SDCS-24 anode further confirms its promising application. This work presents a strategy for designing self-doped defective carbons in situ and provides insights into the potassium storage mechanism at low potential.</div></div>","PeriodicalId":262,"journal":{"name":"Carbon","volume":"232 ","pages":"Article 119791"},"PeriodicalIF":10.5,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142573274","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The sluggish redox kinetics of S species and the notorious shuttling effect of lithium polysulfides (LiPSs) severely impeded the practical application of lithium-sulfur (Li–S) batteries. Herein, we successfully synthesized WC-WO3 heterogeneous nanoparticles dispersed on porous carbon substrate (WC-WO3/C) as the promoter for high-efficiency LiPSs conversion. These nanoparticles combine the robust adsorption capacity of WO3 with the excellent electrical conductivity of WC. Additionally, we studied the dynamic sulfidation behavior of WC-WO3 heterogeneous nanoparticles during the electrochemical process through in situ characterization. A new active phase of WS2 was generated, effectively enhancing the bidirectional redox of Li2S. The Li–S battery armed with the WC-WO3-WS2/C@S cathode demonstrated outstanding cycling stability, with a capacity retention of 95.3 % at 2C after 800 cycles. The pouch cell exhibited an impressive energy density of 423.3 Wh kg−1. This work not only contributes to a thorough understanding of the mechanism behind sulfidation behavior in regulating redox kinetics of LiPSs but also offers guidance for the design of electrocatalysts for high-performance Li–S batteries based on sulfidation.
{"title":"Revealing dynamic sulfidation of WC-WO3 heterogeneous nanoparticles: In situ formation of WS2 facilitates sulfur redox in Li–S battery","authors":"Yongzheng Zhu, Shanfeng Yang, Zheng Wei, Huibing He, Yanqiu Zhu, Jinliang Zhu","doi":"10.1016/j.carbon.2024.119790","DOIUrl":"10.1016/j.carbon.2024.119790","url":null,"abstract":"<div><div>The sluggish redox kinetics of S species and the notorious shuttling effect of lithium polysulfides (LiPSs) severely impeded the practical application of lithium-sulfur (Li–S) batteries. Herein, we successfully synthesized WC-WO<sub>3</sub> heterogeneous nanoparticles dispersed on porous carbon substrate (WC-WO<sub>3</sub>/C) as the promoter for high-efficiency LiPSs conversion. These nanoparticles combine the robust adsorption capacity of WO<sub>3</sub> with the excellent electrical conductivity of WC. Additionally, we studied the dynamic sulfidation behavior of WC-WO<sub>3</sub> heterogeneous nanoparticles during the electrochemical process through in situ characterization. A new active phase of WS<sub>2</sub> was generated, effectively enhancing the bidirectional redox of Li<sub>2</sub>S. The Li–S battery armed with the WC-WO<sub>3</sub>-WS<sub>2</sub>/C@S cathode demonstrated outstanding cycling stability, with a capacity retention of 95.3 % at 2C after 800 cycles. The pouch cell exhibited an impressive energy density of 423.3 Wh kg<sup>−1</sup>. This work not only contributes to a thorough understanding of the mechanism behind sulfidation behavior in regulating redox kinetics of LiPSs but also offers guidance for the design of electrocatalysts for high-performance Li–S batteries based on sulfidation.</div></div>","PeriodicalId":262,"journal":{"name":"Carbon","volume":"232 ","pages":"Article 119790"},"PeriodicalIF":10.5,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142578896","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-31DOI: 10.1016/j.carbon.2024.119787
Yao Xue , Zhiming Wang , Yanfeng Zhang , Zhu Zhu , Xiaoyu Li , Xin Du
Constructing nitrogen-doped porous carbons with high specific surface area, rapid mass transfer channels, and positive charge is a crucial requirement for high-performance adsorbents. Herein, by the kinetic self-assembly synthesis strategy, we prepared nitrogen-doped hierarchical porous carbon spheres (N-HPCS) with adjustable pore structure, high specific surface area, and high nitrogen doping content (8.88 %). By using ethylenediamine as an assisted polymerization and assembly agent, the hydrolysis and condensation rate of tetraethyl orthosilicate (TEOS) as the silica source and the condensation rate of 3-aminophenol and formaldehyde as the phenolic resin precursor were controlled by adjusting ammonia volume as the alkaline catalyst to tune kinetic self-assembly of silica and phenolic resin components, thus achieving their simultaneous or sequential nucleus and growth. After carbonization and selective silica etching, three types of carbon nanospheres with center-radial pores, hollow center-radial pores and hollow structure were obtained. High nitrogen doping content endowed the nanospheres with positive charge. Through adsorption experiments on the bovine serum albumin (BSA) and Hemoglobin (Hb) as typical biological macromolecules, hollow carbon nanospheres with center-radial pores exhibited excellent adsorption performance for BSA(622.34 mg g−1) and Hb(759.96 mg g−1). Our fabricated N-HPCS may become a potential candidate for high-performance adsorption materials.
{"title":"Controlled fabrication of hierarchical porous carbon nanospheres with high doped nitrogen content for high-performance adsorbent of biomacromolecule","authors":"Yao Xue , Zhiming Wang , Yanfeng Zhang , Zhu Zhu , Xiaoyu Li , Xin Du","doi":"10.1016/j.carbon.2024.119787","DOIUrl":"10.1016/j.carbon.2024.119787","url":null,"abstract":"<div><div>Constructing nitrogen-doped porous carbons with high specific surface area, rapid mass transfer channels, and positive charge is a crucial requirement for high-performance adsorbents. Herein, by the kinetic self-assembly synthesis strategy, we prepared nitrogen-doped hierarchical porous carbon spheres (N-HPCS) with adjustable pore structure, high specific surface area, and high nitrogen doping content (8.88 %). By using ethylenediamine as an assisted polymerization and assembly agent, the hydrolysis and condensation rate of tetraethyl orthosilicate (TEOS) as the silica source and the condensation rate of 3-aminophenol and formaldehyde as the phenolic resin precursor were controlled by adjusting ammonia volume as the alkaline catalyst to tune kinetic self-assembly of silica and phenolic resin components, thus achieving their simultaneous or sequential nucleus and growth. After carbonization and selective silica etching, three types of carbon nanospheres with center-radial pores, hollow center-radial pores and hollow structure were obtained. High nitrogen doping content endowed the nanospheres with positive charge. Through adsorption experiments on the bovine serum albumin (BSA) and Hemoglobin (Hb) as typical biological macromolecules, hollow carbon nanospheres with center-radial pores exhibited excellent adsorption performance for BSA(622.34 mg g<sup>−1</sup>) and Hb(759.96 mg g<sup>−1</sup>). Our fabricated N-HPCS may become a potential candidate for high-performance adsorption materials.</div></div>","PeriodicalId":262,"journal":{"name":"Carbon","volume":"232 ","pages":"Article 119787"},"PeriodicalIF":10.5,"publicationDate":"2024-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142573271","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-30DOI: 10.1016/j.carbon.2024.119774
Xin Zhou , Yifan He , Yiming Yang , Zilong Wang , Wenlong Jiang , Ying Guo , Kun Zheng , Heng Zhou , Tong Zhao
Although graphene-based polymer electrothermal films have received great attention, the graphene aggregation restricts the improvement in electrothermal performance. This study reports graphene (GN)/two-dimensional polyarylamide nanosheets (2DPA) filled poly (hexamethylene terephthalamide) (PA6T) composite film with outstanding electrothermal and mechanical performance. Owing to the addition of 2DPA, the as-prepared 2DPA-GN/PA6T composite film can attain a high heating-up rate of 25.5 °C/s, 1.8 times higher than that of GN/PA6T composite film (14.1 °C/s). Furthermore, the 2DPA-modified composite film showed a remarkable heating temperature rise to ∼230 °C, 80 °C higher than that of GN/PA6T composite film (∼150 °C). Additionally, the film had excellent mechanical performance with tensile strength and modulus of elasticity of 32.5 MPa and 4.6 GPa, which were 24.2 % and 52.3 % higher than that of GN/PA6T composite film, respectively. Such outstanding performance came from strong interfacial adhesion between GN and PA6T, induced by 2DPA nanosheets through hydrogen bonding and π-π interactions, which were confirmed by FTIR and UV–Vis measurements. Besides improving interfacial adhesion, 2DPA can also reduce the surface defect density of the GN through π-π conjugation. Both improved interfacial adhesion and reduced defects of GN contributed to the formation of electrically conductive and stress transfer pathways, which supported the excellent electrothermal and mechanical properties of 2DPA-GN/PA6T composite films. This study demonstrates an effective way to prepare high-performance graphene composites for electrothermal applications, with expected uses in aerospace, industry, and other technological fields.
{"title":"Achieving high electrothermal and mechanical performance for Graphene/Poly(hexamethylene terephthalamide) composite films via interfacial engineering with two-dimensional polyarylamide nanosheets","authors":"Xin Zhou , Yifan He , Yiming Yang , Zilong Wang , Wenlong Jiang , Ying Guo , Kun Zheng , Heng Zhou , Tong Zhao","doi":"10.1016/j.carbon.2024.119774","DOIUrl":"10.1016/j.carbon.2024.119774","url":null,"abstract":"<div><div>Although graphene-based polymer electrothermal films have received great attention, the graphene aggregation restricts the improvement in electrothermal performance. This study reports graphene (GN)/two-dimensional polyarylamide nanosheets (2DPA) filled poly (hexamethylene terephthalamide) (PA6T) composite film with outstanding electrothermal and mechanical performance. Owing to the addition of 2DPA, the as-prepared 2DPA-GN/PA6T composite film can attain a high heating-up rate of 25.5 °C/s, 1.8 times higher than that of GN/PA6T composite film (14.1 °C/s). Furthermore, the 2DPA-modified composite film showed a remarkable heating temperature rise to ∼230 °C, 80 °C higher than that of GN/PA6T composite film (∼150 °C). Additionally, the film had excellent mechanical performance with tensile strength and modulus of elasticity of 32.5 MPa and 4.6 GPa, which were 24.2 % and 52.3 % higher than that of GN/PA6T composite film, respectively. Such outstanding performance came from strong interfacial adhesion between GN and PA6T, induced by 2DPA nanosheets through hydrogen bonding and π-π interactions, which were confirmed by FTIR and UV–Vis measurements. Besides improving interfacial adhesion, 2DPA can also reduce the surface defect density of the GN through π-π conjugation. Both improved interfacial adhesion and reduced defects of GN contributed to the formation of electrically conductive and stress transfer pathways, which supported the excellent electrothermal and mechanical properties of 2DPA-GN/PA6T composite films. This study demonstrates an effective way to prepare high-performance graphene composites for electrothermal applications, with expected uses in aerospace, industry, and other technological fields.</div></div>","PeriodicalId":262,"journal":{"name":"Carbon","volume":"232 ","pages":"Article 119774"},"PeriodicalIF":10.5,"publicationDate":"2024-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142592525","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-30DOI: 10.1016/j.carbon.2024.119762
Haijun Chen , Jiaying Pei , Zhibin Zhang , Yanbing Sun , Nan Xu , Yan Chen , Yunhai Liu
Lignin has deemed to be the main polluting component of paper industry wastewater. But developing a potential strategy for utilization of lignin is a challenges problem. Lignin derived materials present potential performance for heavy metal wastewater treatment due to their unique physicochemical properties, and were found to be promising candidate materials in U(VI) removal. However, it is still lacking of a comprehensive understanding that the influences of surface oxygen-defect and grain-size on U(VI) removal processes. Here, using lignin as the raw material, combining plasma treatment technology to prepare defect states Lignin Derived Carbon (LDC), and exploring the influences of surface oxygen-defect and grain-size on their removal U(VI) process. The results indicated that with the reducing of LDC particle size (from ∼4 to ∼ 1 μm), the removal performance of U(VI) was improved. And the U(VI) removal performance of LDC was further improved by introducing of oxygen defect via H2 plasma etch. The characterization analysis of defect states LDC before and after reaction with U(VI) shown that the U(VI) removal mechanism was dominated by defects site complexation. These finding provide deep insight into the recycling of industrial solid wastes lignin and improving of U(VI) removal performance via defect controlling technology.
{"title":"Controlling synthesis of defect state lignin-derived carbon and application for U(VI) removal from aqueous solution: Effects of oxygen-defect and grain-size","authors":"Haijun Chen , Jiaying Pei , Zhibin Zhang , Yanbing Sun , Nan Xu , Yan Chen , Yunhai Liu","doi":"10.1016/j.carbon.2024.119762","DOIUrl":"10.1016/j.carbon.2024.119762","url":null,"abstract":"<div><div>Lignin has deemed to be the main polluting component of paper industry wastewater. But developing a potential strategy for utilization of lignin is a challenges problem. Lignin derived materials present potential performance for heavy metal wastewater treatment due to their unique physicochemical properties, and were found to be promising candidate materials in U(VI) removal. However, it is still lacking of a comprehensive understanding that the influences of surface oxygen-defect and grain-size on U(VI) removal processes. Here, using lignin as the raw material, combining plasma treatment technology to prepare defect states Lignin Derived Carbon (LDC), and exploring the influences of surface oxygen-defect and grain-size on their removal U(VI) process. The results indicated that with the reducing of LDC particle size (from ∼4 to ∼ 1 μm), the removal performance of U(VI) was improved. And the U(VI) removal performance of LDC was further improved by introducing of oxygen defect via H<sub>2</sub> plasma etch. The characterization analysis of defect states LDC before and after reaction with U(VI) shown that the U(VI) removal mechanism was dominated by defects site complexation. These finding provide deep insight into the recycling of industrial solid wastes lignin and improving of U(VI) removal performance via defect controlling technology.</div></div>","PeriodicalId":262,"journal":{"name":"Carbon","volume":"232 ","pages":"Article 119762"},"PeriodicalIF":10.5,"publicationDate":"2024-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142592524","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-30DOI: 10.1016/j.carbon.2024.119781
Minghao Liu , Hao Shi , Lei Guo , Zhouyu Fang , Di Chen , Wenmiao Li , Bowen Deng , Wei Li , Kaifa Du , Huayi Yin , Dihua Wang
Molten salt electrolysis of CO2 represents a promising technology for highly efficient CO2 capture and the production of economically valuable CO2-derived carbon materials. In this study, we established a 100-A-scale molten salt CO2 electrolysis cell to synthesize hundreds of grams of CO2-derived carbon. Subsequent Joule heating at 2800 °C transformed these materials into high-quality graphite. Further composite modification with asphalt and petroleum coke effectively reduced surface area, resulting in high-performance graphite for lithium-ion battery. The CO2-derived graphite anodes demonstrated high reversible capacities ranging from 297.7 to 378.1 mAh g−1, exhibiting outstanding rate capability and stability over 300 charge-discharge cycles at a current density of 1 A g−1. Finally, we assembled a coin full-cell using AG-2/2/6 anode and LFP cathode, which demonstrated good cycling performance. XPS analysis revealed a significant reduction in oxygen content by the post-reformation, facilitating the formation of highly graphitized structures. This study not only pioneers the up-class synthesis of CO2-derived carbon but also underscores its potential for sustainable energy applications, particularly in lithium-ion battery technology.
熔盐电解二氧化碳是一种很有前景的高效二氧化碳捕集技术,也是一种生产具有经济价值的二氧化碳衍生碳材料的技术。在这项研究中,我们建立了一个 100-A 规模的二氧化碳熔盐电解池,合成了数百克二氧化碳衍生碳。随后在 2800 °C 下进行焦耳加热,将这些材料转化为优质石墨。进一步用沥青和石油焦进行复合改性,可有效减少表面积,从而获得用于锂离子电池的高性能石墨。二氧化碳衍生石墨阳极表现出 297.7 至 378.1 mAh g-1 的高可逆容量,在电流密度为 1 A g-1 的条件下,经过 300 次充放电循环,表现出卓越的速率能力和稳定性。最后,我们使用 AG-2/2/6 阳极和 LFP 阴极组装了一个硬币全电池,显示出良好的循环性能。XPS 分析表明,后转化过程中氧含量显著降低,促进了高度石墨化结构的形成。这项研究不仅开创了二氧化碳衍生碳的高端合成技术,还凸显了其在可持续能源应用(尤其是锂离子电池技术)方面的潜力。
{"title":"Enhanced graphitization of CO2-derived carbon anodes via Joule heating reformation for high-performance lithium-ion batteries","authors":"Minghao Liu , Hao Shi , Lei Guo , Zhouyu Fang , Di Chen , Wenmiao Li , Bowen Deng , Wei Li , Kaifa Du , Huayi Yin , Dihua Wang","doi":"10.1016/j.carbon.2024.119781","DOIUrl":"10.1016/j.carbon.2024.119781","url":null,"abstract":"<div><div>Molten salt electrolysis of CO<sub>2</sub> represents a promising technology for highly efficient CO<sub>2</sub> capture and the production of economically valuable CO<sub>2</sub>-derived carbon materials. In this study, we established a 100-A-scale molten salt CO<sub>2</sub> electrolysis cell to synthesize hundreds of grams of CO<sub>2</sub>-derived carbon. Subsequent Joule heating at 2800 °C transformed these materials into high-quality graphite. Further composite modification with asphalt and petroleum coke effectively reduced surface area, resulting in high-performance graphite for lithium-ion battery. The CO<sub>2</sub>-derived graphite anodes demonstrated high reversible capacities ranging from 297.7 to 378.1 mAh g<sup>−1</sup>, exhibiting outstanding rate capability and stability over 300 charge-discharge cycles at a current density of 1 A g<sup>−1</sup>. Finally, we assembled a coin full-cell using AG-2/2/6 anode and LFP cathode, which demonstrated good cycling performance. XPS analysis revealed a significant reduction in oxygen content by the post-reformation, facilitating the formation of highly graphitized structures. This study not only pioneers the up-class synthesis of CO<sub>2</sub>-derived carbon but also underscores its potential for sustainable energy applications, particularly in lithium-ion battery technology.</div></div>","PeriodicalId":262,"journal":{"name":"Carbon","volume":"232 ","pages":"Article 119781"},"PeriodicalIF":10.5,"publicationDate":"2024-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142655822","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}