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NbS2/Ti2CS2 heterostructure with excellent rate and storage performance as an anode material for Li/Na/K ion batteries: A first-principles calculation 具有优异速率和存储性能的 NbS2/Ti2CS2 异质结构可用作锂/纳/钾离子电池的负极材料:第一原理计算
IF 5.9 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-18 DOI: 10.1016/j.flatc.2024.100712
Zhongyong Zhang , Xian Yuan , Yifan Wu , Wenjing Ji , Yuntong Peng , Naigen Zhou , Shangquan Zhao

The limited specific capacity of graphite anodes constrains the advancement of lithium-ion batteries (LIBs), sodium-ion batteries (NIBs), and potassium-ion batteries (KIBs). To address this, we have explored the potential of van der Waals heterostructures for high-performance anode materials. Specifically, we designed and analyzed the NbS2/Ti2CS2 heterostructure through first-principles calculations. This heterostructure demonstrates superior thermal stability and metallic conductivity. Furthermore, it allows for the stable adsorption of Li/Na/K atoms, indicating strong interactions that are advantageous for battery applications. Notably, the Li/Na/K ion diffusion barriers on NbS2/Ti2CS2 are lower compared to other anodes, enhancing ion mobility. The average open-circuit voltages (OCVs) for NbS2/Ti2CS2 as an anode in NIBs/KIBs range from 0 to 1 V, with a remarkable specific capacity of 489 mAh/g for NIBs. These findings position NbS2/Ti2CS2 as an exceptional candidate for next-generation battery anodes, potentially revolutionizing the LIB/NIB/KIB landscape. Our research contributes to the ongoing development of advanced anode materials, offering new pathways for enhancing battery performance.

石墨负极的比容量有限,制约了锂离子电池(LIB)、钠离子电池(NIB)和钾离子电池(KIB)的发展。为此,我们探索了范德华异质结构在高性能负极材料方面的潜力。具体来说,我们通过第一原理计算设计并分析了 NbS2/Ti2CS2 异质结构。这种异质结构具有优异的热稳定性和金属导电性。此外,它还能稳定地吸附 Li/Na/K 原子,显示出强烈的相互作用,有利于电池应用。值得注意的是,与其他阳极相比,NbS2/Ti2CS2 上的 Li/Na/K 离子扩散阻力更低,从而提高了离子迁移率。NbS2/Ti2CS2 作为 NIBs/KIBs 阳极的平均开路电压 (OCV) 在 0 到 1 V 之间,NIBs 的比容量高达 489 mAh/g。这些发现使 NbS2/Ti2CS2 成为下一代电池阳极的理想候选材料,有可能彻底改变 LIB/NIB/KIB 的格局。我们的研究为先进阳极材料的持续开发做出了贡献,为提高电池性能提供了新的途径。
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引用次数: 0
Graphene encapsulated Fe-based nanoparticles synthesized from iron(II) sulfate heptahydrate containing precursors: Influence of chemical vapor deposition parameters 用含七水硫酸铁(II)的前驱体合成的石墨烯封装铁基纳米粒子:化学气相沉积参数的影响
IF 5.9 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-14 DOI: 10.1016/j.flatc.2024.100714
Sıddıka Mertdinç-Ülküseven , Derya Demirbaş , Frederik Winkelmann , Michael Felderhoff , M. Lütfi Öveçoğlu , Duygu Ağaoğulları

Importance of process parameters on thermal, microstructural, and magnetic properties of synthesized core/shell nanoparticles was investigated during their production via chemical vapor deposition (CVD). Herein, iron(II) sulfate heptahydrate and fumed silica powders were mixed in ethanol, and the solution was used for precursor preparation by utilizing spray dryer. These prepared precursors were treated in the CVD process under methane/hydrogen (CH4/H2) gas flow to synthesize graphene-encapsulated core/shell nanoparticles. CVD studies were performed at various temperatures (900–1000 °C), holding times (60, 90 min), and gas flow rates (100, 200 mL/min). After CVD studies, purification was applied to remove uncoated nanoparticles, and remaining fumed silica phases originated from the precursor via selective acid leaching using hydrofloric acid (HF) and hydrochloric acid (HCl) solutions. X-ray diffractometry, Raman and Mössbauer spectroscopy, Zeta potential measurement, thermogravimetry combined with differential scanning calorimetry, scanning and transmission electron microscopy/energy-dispersive spectroscopy, and vibrating sample magnetometry (VSM) results yielded the optimized CVD parameters as 950 °C, 60 min, CH4/H2: 1/1 and 50 mbar. The characterization results proved that multilayer graphene (d-spacing: 0.34 nm) encapsulated Fe/Fe3C nanoparticles (average core size: ∼46.9 nm, shell thickness: ∼16.6 nm) can be successfully synthesized by using CVD process followed by a leaching treatment. VSM results revealed that synthesized nanoparticles had soft ferromagnetic properties (Ms: 90.6–185 emu/g; Hc: 255.4–301.6 Oe). Characterization results deepen the understanding of process parameters of CVD system on characteristics of core/shell nanoparticles.

在通过化学气相沉积(CVD)生产核/壳纳米粒子的过程中,研究了工艺参数对其热性能、微观结构和磁性能的重要性。在此,七水硫酸铁和气相二氧化硅粉末在乙醇中混合,利用喷雾干燥器将溶液用于制备前驱体。这些制备好的前驱体在甲烷/氢气(CH4/H2)气流下进行 CVD 处理,合成出石墨烯封装的核/壳纳米粒子。CVD 研究在不同的温度(900-1000 °C)、保温时间(60、90 分钟)和气体流速(100、200 mL/min)下进行。CVD 研究结束后,通过使用氢氟酸 (HF) 和盐酸 (HCl) 溶液进行选择性酸浸出,纯化去除未涂层的纳米颗粒和源自前驱体的剩余气相二氧化硅相。X 射线衍射仪、拉曼光谱和莫斯鲍尔光谱、Zeta 电位测量、热重仪结合差示扫描量热仪、扫描和透射电子显微镜/能量色散光谱以及振动样品磁力计 (VSM) 结果表明,优化的 CVD 参数为 950 ℃、60 分钟、CH4/H2:1/1 和 50 毫巴。表征结果证明,采用 CVD 工艺,然后进行浸出处理,可以成功合成多层石墨烯(d 间距:0.34 nm)封装的 Fe/Fe3C 纳米粒子(平均核心尺寸:∼46.9 nm,外壳厚度:∼16.6 nm)。VSM 结果表明,合成的纳米粒子具有软铁磁性(Ms:90.6-185 emu/g;Hc:255.4-301.6 Oe)。表征结果加深了人们对 CVD 系统工艺参数对核/壳纳米粒子特性的影响的理解。
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引用次数: 0
Electrochemical functionalization of graphene nanosheets with iodoacetic acid towards supercapacitor electrodes 用碘乙酸对石墨烯纳米片进行电化学功能化,使其用于超级电容器电极
IF 5.9 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-14 DOI: 10.1016/j.flatc.2024.100710
Sergio García-Dalí, Daniel F. Carrasco, Silvia Villar-Rodil, Juan I. Paredes, Juan M.D. Tascón

Graphene nanosheets show great potential as electrode materials for supercapacitors due to their high surface area and excellent electrical conductivity. However, the low hydrophilicity of graphene nanosheets limits their electrochemical performance in aqueous supercapacitor applications. To enhance their electrochemical performance, we investigate the use of iodoacetic acid as an electrolytic functionalization agent for graphene nanosheets. Here, we demonstrate the successful electrolytic functionalization of graphene nanosheets under cathodic conditions in aqueous medium. The resulting material exhibits a high structural quality and carboxyl groups on the surface, which increases the hydrophilicity and wettability of the material. The applied voltage and the concentration of iodoacetic acid have been found to be key factors to optimize the process in order to get the maximum functionalization degree. The electrochemical performance demonstrates that iodoacetic acid functionalized graphene nanosheets exhibit significantly improved specific capacitance (220F/g at 0.5 A/g) and cycling stability of the symmetric cell compared to pristine graphene nanosheets, highlighting the potential of electrochemical functionalization to improve the performance of graphene-based materials in energy storage applications.

石墨烯纳米片具有高比表面积和优异的导电性,因此作为超级电容器的电极材料显示出巨大的潜力。然而,石墨烯纳米片的低亲水性限制了其在水性超级电容器应用中的电化学性能。为了提高它们的电化学性能,我们研究了使用碘乙酸作为石墨烯纳米片的电解功能化剂。在此,我们展示了在水介质中的阴极条件下成功实现石墨烯纳米片的电解功能化。所得到的材料具有很高的结构质量,表面的羧基增加了材料的亲水性和润湿性。研究发现,为了获得最大的官能化程度,施加电压和碘乙酸浓度是优化工艺的关键因素。电化学性能表明,与原始石墨烯纳米片相比,碘乙酸功能化石墨烯纳米片的比电容(0.5 A/g时为220F/g)和对称电池的循环稳定性都有显著提高,凸显了电化学功能化在提高石墨烯基材料储能应用性能方面的潜力。
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引用次数: 0
Insight into the role of nickel carbide nanoparticles in improving photocatalytic H2 generation over ZnIn2S4 under visible light 洞察碳化镍纳米颗粒在可见光条件下改善 ZnIn2S4 光催化产生 H2 的作用
IF 5.9 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-14 DOI: 10.1016/j.flatc.2024.100711
Longfei Wang , Qingru Zeng , Yufeng Gan , Yuezhou Wei , Xinpeng Wang , Deqian Zeng

Zinc indium sulfide (ZnIn2S4) is a Cd-free semiconductor with great potential in various photocatalytic applications. However, its rapid photogenerated charge combination poses some challenges. Constructing ZnIn2S4-based heterojunction photocatalysts to address this has proven an effective solution. In this study, we loaded uniform Ni3C nanoparticles as cocatalysts on layered ZnIn2S4 nanostructures to promote photocatalytic H2 production activity. The optimal 3 % Ni3C/ZnIn2S4 exhibited the highest H2 generation rate of 393 μmol·g−1·h−1, 4.5 times greater than pure ZnIn2S4. The enhanced photocatalytic performance was ascribed to the incorporation of metallic Ni3C, which provides more catalytically active sites and establishes electron transfer channels at the interfaces, facilitating the photogenerated carrier separation and H2 production. The photocatalytic mechanism of Ni3C/ZnIn2S4 was proposed through experimental measurements and DFT calculations. This study offers a way to develop efficient ZnIn2S4-based visible-light-driven photocatalysts.

硫化锌铟(ZnIn2S4)是一种无镉半导体,在各种光催化应用中具有巨大潜力。然而,其快速的光生电荷结合带来了一些挑战。事实证明,构建基于 ZnIn2S4 的异质结光催化剂是解决这一问题的有效方法。在本研究中,我们在层状 ZnIn2S4 纳米结构上负载了均匀的 Ni3C 纳米颗粒作为协同催化剂,以提高光催化产生 H2 的活性。最佳的 3 % Ni3C/ZnIn2S4 的 H2 生成率高达 393 μmol-g-1-h-1,是纯 ZnIn2S4 的 4.5 倍。光催化性能的提高归因于金属 Ni3C 的加入,它提供了更多的催化活性位点,并在界面上建立了电子传递通道,促进了光生载流子的分离和 H2 的产生。通过实验测量和 DFT 计算,提出了 Ni3C/ZnIn2S4 的光催化机理。这项研究为开发基于 ZnIn2S4 的高效可见光驱动光催化剂提供了一条途径。
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引用次数: 0
Influence of bonding variance on electron affinity in graphene quantum dot-barium titanate nanocomposites for drug delivery system 用于药物输送系统的石墨烯量子点-钛酸钡纳米复合材料中键合差异对电子亲和力的影响
IF 5.9 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-14 DOI: 10.1016/j.flatc.2024.100713
Jung-Hua Lin , Li Chen , Er-Chieh Cho , Kuen-Chan Lee

Although chemotherapy remains a prevalent option in cancer treatment, its adverse effects on normal cells and suboptimal pharmacokinetics often limits its effectiveness. To address these challenges, this study successfully developed a new multifunctional drug delivery system comprising a covalent composite of graphene quantum dots and barium titanate nanoparticles. Notably, despite numerous reports on the surface modification of graphene quantum dots, studies focusing on cancer cell inhibition via different covalent bonds are scarce. To bridge this gap, this system was synthesized using eco-friendly esterification and amidation pathways. The anticancer drug doxorubicin was employed as a model drug, and hyaluronic acid was used to encapsulate the delivery system, enhancing its sustained release capabilities. Comprehensive material characterization confirmed the successful synthesis of the system. Its high drug loading capacity and acid-sensitive release can be attributed to the unique structure of the graphene quantum dots. Subsequent in vitro and in vivo biological evaluations not only demonstrated the system’s remarkable cancer inhibition efficacy but also accentuated the distinct impacts of the two bonding types. The underlying mechanism is believed to involve bonding affinity and electron transfer, findings that are corroborated by the experimental data. Additionally, results from animal models provide clear evidence for the potential application of this system (HA-DOX-GQD@BTNPs) in cancer therapeutics and imaging. In conclusion, this research elucidates the variances in drug carrier efficacy based on different covalent bond modifications for cancer treatment and introduces a novel drug delivery system that synergistically combines imaging and targeting capabilities.

尽管化疗仍是癌症治疗中的普遍选择,但其对正常细胞的不良影响和不理想的药代动力学往往限制了化疗的效果。为了应对这些挑战,本研究成功开发了一种新型多功能给药系统,该系统由石墨烯量子点和钛酸钡纳米颗粒共价复合而成。值得注意的是,尽管有关石墨烯量子点表面修饰的报道很多,但通过不同共价键抑制癌细胞的研究却很少。为了弥补这一空白,我们采用环保的酯化和酰胺化途径合成了这一系统。抗癌药物多柔比星被用作模型药物,透明质酸被用于包裹该递送系统,从而增强了其持续释放能力。全面的材料表征证实了该系统的成功合成。石墨烯量子点的独特结构造就了它的高载药量和酸敏释放特性。随后进行的体外和体内生物评估不仅证明了该系统显著的抑癌功效,还凸显了两种键合类型的不同影响。其基本机制被认为涉及键合亲和力和电子转移,实验数据也证实了这一结论。此外,动物模型的研究结果为该系统(HA-DOX-GQD@BTNPs)在癌症治疗和成像中的潜在应用提供了明确证据。总之,这项研究阐明了基于不同共价键修饰的药物载体在癌症治疗中的功效差异,并介绍了一种新型的药物输送系统,它能协同结合成像和靶向功能。
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引用次数: 0
Enhanced performance of Na4Ti5O12 nanowall arrays for next-generation pseudocapacitors through sodiation treatment 通过钠化处理提高用于下一代伪电容器的 Na4Ti5O12 纳米壁阵列的性能
IF 5.9 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-14 DOI: 10.1016/j.flatc.2024.100715
Nawishta Jabeen , Ahmad Hussain , Faiqa Shahid , Mahmoud M. Hessien

Pseudocapacitors are well-known for performing redox reactions at the interfaces of electrode and electrolyte for storing and releasing energy competently. TiO2 is thought to be a potential anode material for Na-ions batteries as it possesses the ability to store large sodium content at the interplanar spacing to amplify the electrochemical performances. However, for pseudocapacitors as anodes, the exact chemical mechanisms and the interaction among surface behavior and electrochemical properties are still needed to be explored. Herein this research, for the first time, monoclinic Na4Ti5O12 nanowall arrays electrode (M−NTO NWAs) has been synthesized to investigate its structure, morphology and electrochemical characterizations as anode for supercapacitors (SCs). The mechanism of sodiation treatment for M−NTO NWAs as anode has elevated its excellent electrochemical properties. M−NTO NWAs is operated at a highly negative potential window between −1.0 and 0.0 V to achieve an excellent specific capacitance of 429 F/g, which is much superior compared to the HTO NSA electrode (295 F/g) and outstanding capacitance retention of ∼97 % is achieved after 3000 successive cycles at a high current density of 1 A/g. Enhanced electrochemical properties display the complementary contributions of structural involvement via the sodiation mechanism of M−NTO NWAs. Also, this work propels a new direction in utilizing ions insertion strategies to enhance electrode’s high performance for energy storage devices.

众所周知,伪电容器能在电极和电解质界面上进行氧化还原反应,从而有效地储存和释放能量。二氧化钛被认为是一种潜在的纳离子电池阳极材料,因为它能够在平面间距处储存大量钠,从而放大电化学性能。然而,对于作为阳极的伪电容器,其确切的化学机制以及表面行为与电化学性能之间的相互作用仍有待探索。本研究首次合成了单斜Na4Ti5O12纳米孔阵列电极(M-NTO NWAs),研究了其作为超级电容器(SCs)阳极的结构、形貌和电化学特性。M-NTO NWAs 作为阳极的钠化处理机制提升了其优异的电化学性能。M-NTO NWAs 在-1.0 至 0.0 V 的高负电位窗口下工作,可获得 429 F/g 的优异比电容,远高于 HTO NSA 电极(295 F/g),并且在 1 A/g 的高电流密度下连续循环 3000 次后,电容保持率达到 97%。电化学性能的增强显示了 M-NTO NWAs 通过钠化机制参与结构的互补贡献。此外,这项研究还为利用离子注入策略提高储能设备电极的高性能指明了新方向。
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引用次数: 0
Battery-free flexible wireless temperature sensing for food storage 用于食品储存的免电池灵活无线温度传感器
IF 5.9 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-06-29 DOI: 10.1016/j.flatc.2024.100709
Zhengzhong Wan , Xujun Chen , Danyao Song , Zihao Wu , Ruihua Zhang , Meng Wang , Xinqing Xiao

The method of monitoring food temperature during food storage needs to be improved to continuously and accurately perceive the temperature of the food in the package to ensure the quality and safety of the food during storage. This paper proposes and develops a battery-free flexible wireless temperature sensing system (BFTS) for food storage. The BFTS consists of a battery-free flexible wireless temperature sensing tag (BFTT), a wireless reader, and a personal computer (PC). The BFTT developed in this paper has good flexibility and can be placed inside the food package to realize the continuous monitoring of temperature changes. The flexible circuits of the BFTT were fabricated by laser engraving laser-induced graphene (LIG) −copper (Cu) plating film made with Cu plating on LIG. The LIG-Cu plating film has good thickness uniformity, electrical conductivity, and laser engraving processability. The antenna of BFTT has good performance. The wireless reader is connected to the PC using a data line, and the BFTT communicates wirelessly with the wireless reader using ultra-high frequency (UHF) radio frequency identification (RFID). The BFTT was realized by the wireless radio frequency (RF) as the supply power from the wireless reader. The BFTS could realize the temperature monitoring of food stored at 0℃ and −18℃, and it has the advantages of low cost, simple manufacturing process, and low energy consumption, which could be used to continuously and accurately monitor the inside temperature of the food packages. Overall, the LIG-Cu plating film developed in this paper could be used in the fabrication of flexible circuits, and the temperature monitoring inside food packages realized by the BFTS has potential applications in actual food storage.

食品储存过程中的温度监测方法亟待改进,以便持续、准确地感知包装中食品的温度,确保食品在储存过程中的质量和安全。本文提出并开发了一种用于食品储存的无电池柔性无线温度传感系统(BFTS)。该系统由一个免电池柔性无线温度传感标签(BFTT)、一个无线读取器和一台个人电脑(PC)组成。本文开发的 BFTT 具有良好的柔性,可以放置在食品包装内部,实现对温度变化的连续监测。BFTT 的柔性电路是通过激光雕刻激光诱导石墨烯(LIG)-铜(Cu)电镀膜制成的。LIG-Cu 电镀膜具有良好的厚度均匀性、导电性和激光雕刻加工性。BFTT 的天线性能良好。无线读取器通过数据线与电脑连接,BFTT 利用超高频(UHF)射频识别(RFID)技术与无线读取器进行无线通信。BFTT 通过无线射频(RF)作为无线阅读器的供电电源来实现。BFTS 可实现对 0℃ 和 -18℃ 食品储存温度的监测,具有成本低、制造工艺简单、能耗低等优点,可用于连续、准确地监测食品包装内部温度。总之,本文开发的 LIG-Cu 电镀膜可用于柔性电路的制造,而 BFTS 实现的食品包装内部温度监测在实际食品储存中也有潜在的应用前景。
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引用次数: 0
Selective mass transport mediated by two-dimensional confined water: A comprehensive review 二维封闭水介导的选择性质量传输:综述
IF 5.9 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-06-28 DOI: 10.1016/j.flatc.2024.100708
Xiaorui Jin , Yuan Chen , Xiaofen Liu , Lan Lan , Yunfei Sun , Meiling Wu , Kai-Ge Zhou

Confined mass transport based on two-dimensional (2D) materials breaks the trade-off effect between permeability and selectivity, significantly enhancing the efficiency of mass transport. However, the prevailing view that mass transport performance is primarily determined by the structural design of molecules or ions within channels and the regulation of channel walls has led to the neglect of surrounding hydration layers. Recent studies indicate that the interactions between confined water and transport substances, particularly the formation of hydration shells, significantly influence the mass transport process. Therefore, a thorough investigation of the behavior and properties of confined water, especially its presence, regulation methods, and the enhanced mechanisms of mass transport in 2D channels is particularly urgent and constitutes an indispensable research direction for the future development of materials science and engineering technologies. This review summarizes the latest progress on 2D confined water including its structure, properties, and behavior under natural conditions or environmental influences, the mechanisms enhancing mass transport, and regulatory approaches, as well as multiple applications such as membrane separation, drug delivery, and confined reactions. Lastly, we present instructive perspectives on the current challenges and future directions in the study of confined water.

基于二维(2D)材料的封闭质量传输打破了渗透性和选择性之间的权衡效应,大大提高了质量传输的效率。然而,由于人们普遍认为质量传输性能主要取决于通道内分子或离子的结构设计以及通道壁的调节,因此忽略了周围的水合层。最近的研究表明,封闭水和传输物质之间的相互作用,特别是水合壳的形成,对质量传输过程有重大影响。因此,深入研究封闭水的行为和特性,特别是其存在、调节方法以及二维通道中质量输运的增强机制尤为迫切,是材料科学与工程技术未来发展不可或缺的研究方向。本综述总结了二维约束水的最新研究进展,包括其结构、性质、在自然条件或环境影响下的行为、质量输运的增强机制和调控方法,以及在膜分离、药物输送和约束反应等方面的多种应用。最后,我们就封闭水研究的当前挑战和未来方向提出了具有启发性的观点。
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引用次数: 0
Simultaneous engineering of the conductivity and work function of biphenylene via fluorine adsorption 通过氟吸附同时设计联苯的电导率和功函数
IF 5.9 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-06-28 DOI: 10.1016/j.flatc.2024.100704
Jiao Zhang , Ying Xie , Yinan Tang , Yinyin Qian , Jing He , Zhe Wang , Yanchang Zhang , Jiankang Chen , Lin Yang , Bing Zheng

Biphenylene (BP) is a new member of the two-dimensional C nanomaterial family, and successful fabrication of BP offers an excellent opportunity for developing innovative C-based electronics. However, its unusual metallicity critically restricts its applications in field-effect transistors (FETs) and photocatalysis. Simultaneously, its relatively low work function (ϕ, 4.33 eV) seriously restricts its applications in anode materials of electronic devices. Therefore, understanding the tunabilities of electronic properties and ϕ of BP-based nanomaterials is crucial to guide experimental exploration; nevertheless, to date, little attention has been paid to this area. Herein, we theoretically demonstrate that conductivity of fluorinated BP (Fn-BP) evolves in the order metallic → semimetallic → semiconductivity with increasing F concentration, attributed to a bonding transition of BP (sp2 → sp2 + sp3 → sp3). Particularly, ϕ of BP can be significantly improved (4.82–6.97 eV) by fluorination, approximately two-fold higher than that of Fn-graphene owing to p electron transfer between F and BP. Consequently, metallic F2D-BP and semimetallic F4S-BP with favorable ϕs can be utilized as substitutes for Au and Pt anodes, respectively. Specifically, F8D-BP, F16D-BP, and F24D-BP with exceptional band gaps of 0.40, 2.80, and 3.44 eV, respectively, exhibit high potentials for making channel materials in FETs, candidate materials in photocatalysis, and buffer layers in solar cells, respectively.

联苯(BP)是二维 C 纳米材料家族中的新成员,成功制备 BP 为开发基于 C 的创新电子器件提供了绝佳机会。然而,其不寻常的金属性严重限制了它在场效应晶体管(FET)和光催化领域的应用。同时,其相对较低的功函数(j,4.33 eV)也严重限制了其在电子设备阳极材料中的应用。因此,了解基于 BP 的纳米材料的电子特性和 ϕ 的可调性对于指导实验探索至关重要。在本文中,我们从理论上证明了氟化 BP(Fn-BP)的导电性随着 F 浓度的增加按金属→半金属→半导的顺序演变,这归因于 BP 的成键转变(sp2 → sp2 + sp3 → sp3)。特别是,由于 F 和 BP 之间的对电子转移,BP 的 ϕ 可以通过氟化显著提高(4.82-6.97 eV),比 Fn 石墨烯的 ϕ 高出约两倍。因此,具有良好ϕs的金属 F2D-BP 和半金属 F4S-BP 可分别用作金和铂阳极的替代物。具体来说,F8D-BP、F16D-BP 和 F24D-BP 分别具有 0.40、2.80 和 3.44 eV 的优异带隙,在制作场效应晶体管的沟道材料、光催化的候选材料和太阳能电池的缓冲层方面具有很大的潜力。
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引用次数: 0
Optimizing doping thresholds for enhanced scintillation in 2D hybrid organic–inorganic perovskites 优化掺杂阈值以增强二维有机-无机混合包晶石的闪烁能力
IF 5.9 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-06-28 DOI: 10.1016/j.flatc.2024.100701
Francesco Maddalena , Michal Makowski , Chengyuan Xiao , Md Abdul Kuddus Sheikh , Dominik Kowal , Marcin E. Witkowski , Konrad J. Drozdowski , Somnath Mahato , Christophe Dujardin , Roberto Calà , Etiennette Auffray , Muhammad Haris Mahyuddin , Winicjusz Drozdowski , Muhammad Danang Birowosuto , Cuong Dang

Two-dimensional hybrid organic–inorganic perovskite (2D-HOIP) crystals, in particular lead-bromide perovskites, exhibit great promise as scintillators due to their superior environmental stability compared to their 3D counterparts, offering high light yields and rapid decay times. These cost-effective, solution-processable materials demonstrate potential for efficient wide-energy radiation detection. In this paper we focus on investigating the effect of partial substitution of n-butylammonium (BA) cation with tert-butylammonium (t-Bu) cation within the butylammonium lead bromide (BA2-xtBuxPbBr4) structure and its impact on luminescence and scintillation properties. We observe that inclusion up to 5 % of t-Bu (x = 0.1) within the structure leads to a narrowing of the bandgap, leading also to an improvement of the light yield by 10 % and lowering of the energy resolution, compared to pristine BA2PbBr4. The bandgap widens, compared to pristine BA2PbBr4, with higher concentrations above 5 %, resulting in effects for the scintillating properties of the 2D-HOIP at room temperature at t-Bu concentrations above 5 %, with reduced light yield and broadened energy resolution. Higher t-Bu concentration (x = 0.4) show very poor room temperature scintillation but increased efficiency at cryogenic temperatures below 50 K. The results shown in this paper demonstrate the fundamental limitation of organic cation mixing levels for scintillation efficiency enhancement.

二维杂化有机-无机包晶石(2D-HOIP)晶体,特别是溴化铅包晶石,由于其环境稳定性优于三维同类晶体,具有高光产率和快速衰减时间,因此作为闪烁体大有可为。这些成本效益高、可溶液加工的材料展示了高效宽能辐射探测的潜力。在本文中,我们重点研究了在丁基溴化铵铅(BA2-xtBuxPbBr4)结构中用叔丁基铵(t-Bu)阳离子部分取代正丁基铵(BA)阳离子的效果及其对发光和闪烁特性的影响。我们观察到,与原始的 BA2PbBr4 相比,在该结构中加入高达 5% 的 t-Bu(x = 0.1)会导致带隙变窄,从而将光产率提高 10%,并降低能量分辨率。与原始的 BA2PbBr4 相比,带隙随着浓度超过 5% 而变宽,从而影响了二维-HOIP 在室温下 t-Bu 浓度超过 5% 时的闪烁特性,降低了光产率,扩大了能量分辨率。更高的 t-Bu 浓度(x = 0.4)显示出室温闪烁性能很差,但在 50 K 以下的低温条件下却能提高效率。
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