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Cellulose Reinforced Eutectogel Electrolyte for Flexible Zinc-Ion Hybrid Supercapacitors 用于柔性锌-离子混合超级电容器的纤维素增强共晶凝胶电解质
IF 6.4 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-12 DOI: 10.1021/acsaem.4c01463
Jiaming Zeng, Wang Yang, Wu Yang, Zhiyuan Zheng, Jianyun Gan, Qi Wang, Liubing Dong, Linxin Zhong, Ruidong Xia, Emmanuel Iheanyichukwu Iwuoha, Usisipho Feleni, Shimelis Admassie, Xinwen Peng
The eutectogel electrolyte has shown significant potential for zinc-ion hybrid supercapacitors (ZHSCs) due to its cost-effectiveness, temperature resistance, and high safety. However, the poor mechanical strength and complex preparation process of the eutectogel electrolyte have become the main barriers to the practical application of ZHSCs. Herein, we developed a cellulose reinforced polyacrylamide (PAM)-based eutectogel (CPG) electrolyte for ZHSCs via an in situ one-step radical polymerization process. The dispersed cellulosic fiber plays a crucial role in stabilizing the network structure and widening the pore size of eutectogel, which improves mechanical properties and ion transport rate. Furthermore, the ternary deep eutectic solvent including choline chloride, urea, ethylene glycol, and ZnCl2 endows eutectogel with intrinsic thermal stability, antidrying (with weight remaining almost unchanged after 20 days), and antifreezing properties. Thus, the as-prepared eutectogel electrolyte exhibits decent mechanical properties (tensile strength of 35.3 kPa and compressive strength of 117.0 kPa), high zinc ion transference number (0.68), superb flexibility, and good adhesion. With these superiorities, the symmetric cell employing the CPG electrolyte achieves stable cycling over 1390 h, and the assembled flexible ZHSC demonstrates favorable mechanical deformation adaptability under various severe conditions and operational feasibility in a wide temperature range from −15 to 60 °C. This work offers a promising strategy for designing multifunctional eutectogel electrolytes for applications in flexible ZHSCs.
共晶凝胶电解质因其成本效益高、耐高温和高安全性而在锌离子混合超级电容器(ZHSCs)中显示出巨大的潜力。然而,共晶凝胶电解质机械强度差、制备工艺复杂,已成为锌离子混合超级电容器实际应用的主要障碍。在此,我们通过一步原位自由基聚合工艺,开发出了一种纤维素增强聚丙烯酰胺(PAM)基共晶凝胶(CPG)电解质,用于 ZHSCs。分散的纤维素纤维在稳定网络结构和拓宽共晶凝胶孔径方面发挥了重要作用,从而改善了机械性能和离子传输速率。此外,包括氯化胆碱、尿素、乙二醇和氯化锌在内的三元深共晶溶剂赋予了共晶凝胶内在的热稳定性、抗干燥性(20 天后重量几乎保持不变)和抗冻性。因此,制备的共晶凝胶电解质具有良好的机械性能(拉伸强度为 35.3 千帕,压缩强度为 117.0 千帕)、高锌离子转移数(0.68)、极佳的柔韧性和良好的粘附性。凭借这些优势,采用 CPG 电解质的对称电池实现了 1390 小时的稳定循环,组装后的柔性 ZHSC 在各种恶劣条件下均表现出良好的机械变形适应性,并可在 -15 至 60 °C 的宽温度范围内运行。这项工作为设计应用于柔性 ZHSC 的多功能共晶凝胶电解质提供了一种前景广阔的策略。
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引用次数: 0
Assembly of Natural Clay Minerals as Highly Robust Evaporation-Driven Power Generator 将天然粘土矿物组装成高度稳健的蒸发驱动型发电装置
IF 6.4 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-12 DOI: 10.1021/acsaem.4c01184
Barsha Rani Bora, Nabamallika Nath, Mrityunjoy Dey, Kundan Saha, Kalyan Raidongia
Inexhaustible natural resources, such as water, wind, moisture, and ubiquitous natural processes such as evaporation or condensation, could offer optimal energy strategies for a sustainable future. Recently, there has been a surge in interest surrounding evaporation-driven power generators (EDPs), which rely on capillary-driven water flow through permselective nanochannels, followed by evaporation into the atmosphere. Despite huge potential, existing EDPs encounter hurdles like expensive and environmentally unfriendly active materials and complex fabrication processes. Here, we introduce a bilayer membrane composed of two distinct clay minerals, vermiculite (VM) and halloysite nanotube (HNT) clay, to develop an evaporation-driven energy generator capable of generating an open-circuit potential up to 406 mV along with short circuit currents of ∼3.4 μA, resulting in a power density up to 0.85 mW/cm3. Due to the affordability, biocompatibility of the materials employed, and simplicity of device fabrication, this energy generator can be upscaled to power low-energy electronic devices and sensors. The all-clay power generator can withstand extreme temperatures; exposure to 180 °C did not affect its power harvesting properties. Individual energy generators are connected in series to power small electronic devices, such as humidity meters, calculators, and LEDs.
取之不尽、用之不竭的自然资源,如水、风、湿气,以及无处不在的自然过程,如蒸发或冷凝,可以为可持续发展的未来提供最佳能源战略。最近,人们对蒸发驱动发电装置(EDPs)的兴趣大增,这种装置依靠毛细管驱动的水流通过过选择性纳米通道,然后蒸发到大气中。尽管潜力巨大,但现有的 EDP 仍面临着各种障碍,如昂贵且不环保的活性材料和复杂的制造工艺。在这里,我们引入了由两种不同的粘土矿物--蛭石(VM)和海泡石纳米管(HNT)粘土--组成的双层膜,开发出一种蒸发驱动型能源发生器,能够产生高达 406 mV 的开路电位和 3.4 μA 的短路电流,功率密度高达 0.85 mW/cm3。由于价格低廉、所用材料的生物相容性和设备制造的简易性,这种能量发生器可升级用于为低能量电子设备和传感器供电。全粘土能量发生器可以承受极端温度;暴露在 180 °C 的环境中不会影响其能量收集特性。将单个能量发生器串联起来,可为湿度计、计算器和发光二极管等小型电子设备供电。
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引用次数: 0
Pd Nanoparticles Decorated Hollow TiO2 Nanospheres for Highly Sensitive and Selective UV-Assisted Hydrogen Gas Sensors 用于高灵敏度和选择性紫外线辅助氢气传感器的钯纳米颗粒装饰中空二氧化钛纳米球
IF 6.4 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-12 DOI: 10.1021/acsaem.4c01039
Thilini Thathsara, Christopher James Harrison, Daniela Schönauer-Kamin, Ulrich Mansfeld, Ralf Moos, François Marie Malherbe, Rosalie K. Hocking, Mahnaz Shafiei
Hydrogen (H2) gas has great potential as an energy carrier in the emerging renewable energy market, emitting zero CO2. However, its high explosive potential and flammability pose substantial risk across production, storage, transport, and consumption; thus, rapid detection of leaks is essential. In this research, hollow TiO2 nanospheres (h-TiO2 NS) with a mean diameter of ∼216 nm are fabricated via a solvothermal method. The TiO2 NS were then chemically decorated with Pd nanoparticles with ∼3.0 nm diameter (Pd/h-TiO2 NS). The Pd/h-TiO2 NS enables permeation by H2, maximizing active sites due to their high specific surface area of ∼80 m2/g and mesoporous structure with an average pore size of 5.6 nm. The chemiresistive Pd/h-TiO2 NS sensor shows promising results toward H2 at 80 °C under 9 V bias and 365 nm UV light with an exceptional response (4.1 for 0.1% H2 and ∼88 for 1% H2), a response time of 36 s for 0.1% H2 and 76 s for 1% H2, and fast recovery (38 and 39 s for 0.1% and 1% H2, respectively). Even under dark conditions, the sensor exhibits a high response (2.3 for 0.1% H2 and ∼47 for 1% H2) with a response time of 52 s for 0.1% H2 and 39 s for 1% H2 and efficient recovery (68 and 39 s for 0.1% and 1% H2, respectively). Additionally, a wide range of H2 concentrations from 50 to 10,000 ppm can be detected under both light and dark conditions. CH4 or CO2 does not affect sensor response, NH3, NO2, or acetone only marginally affects response. Even the influence of humidity is very low. The response remained stable across three months. The results confirm that Pd/h-TiO2 NS are promising for H2 sensing and establish a benchmark in this field.
氢气(H2)作为一种能源载体,在新兴的可再生能源市场中具有巨大潜力,其二氧化碳排放量为零。然而,氢气的高爆炸性和易燃性给生产、储存、运输和消费带来了巨大风险;因此,快速检测泄漏至关重要。本研究采用溶热法制备了平均直径为 216 纳米的中空二氧化钛纳米球(h-TiO2 NS)。然后用直径为 3.0 nm 的 Pd 纳米颗粒对 TiO2 NS 进行化学装饰(Pd/h-TiO2 NS)。由于 Pd/h-TiO2 NS 的比表面积高达 80 m2/g,且具有平均孔径为 5.6 nm 的介孔结构,因此可以最大限度地增加活性位点,从而实现 H2 的渗透。化学电阻式 Pd/h-TiO2 NS 传感器在 9 V 偏压和 365 nm 紫外光条件下于 80 °C,对 H2 的反应速度极快(0.1% H2 的反应速度为 4.1,1% H2 的反应速度为 88),0.1% H2 的反应时间为 36 秒,1% H2 的反应时间为 76 秒,而且恢复速度很快(0.1% H2 和 1%H2的恢复时间分别为 38 秒和 39 秒)。即使在黑暗条件下,传感器也能表现出较高的响应能力(0.1% H2 时为 2.3,1% H2 时为 ∼47),0.1% H2 时的响应时间为 52 秒,1% H2 时的响应时间为 39 秒,并能快速恢复(0.1% H2 时为 68 秒,1% H2 时为 39 秒)。此外,在光照和黑暗条件下都能检测到 50 至 10,000 ppm 的各种 H2 浓度。CH4 或 CO2 不会影响传感器的响应,NH3、NO2 或丙酮对响应的影响微乎其微。湿度的影响也非常小。三个月内的响应保持稳定。研究结果证实,Pd/h-TiO2 NS 有希望用于 H2 传感,并在该领域树立了一个标杆。
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引用次数: 0
Influence of A-Site Deficiency and Ca Concentration on the Electrical and Crystallographic Properties of (Nd0.2Sr0.7–xCax)yTi0.95Fe0.05O3−δ-Based Fuel Electrode for Solid Oxide Cells A 盐缺失和 Ca 浓度对(Nd0.2Sr0.7-xCax)yTi0.95Fe0.05O3-δ基固体氧化物电池燃料电极的电学和晶体学特性的影响
IF 6.4 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-12 DOI: 10.1021/acsaem.4c00824
S. Paydar, K. Kooser, O. Volobujeva, S. Granroth, G. Nurk
This study explores the impact of A-site deficiency and Sr/Ca ratio on the electrochemical and crystallographic properties of a (Nd0.2Sr0.7–xCax)yTi0.95Fe0.05O3−δ hydrogen electrode for solid oxide cells under reducing and air atmospheres. 5% and 10% A-site deficient (Nd0.2Sr0.7–xCax)yTi0.95Fe0.05O3−δ (x = 0.35–0.45, y = 1.05, 1) (referred to as 5NSCTF-x and 10NSCTF-x) materials were studied, while the ratio between A-site cations was kept the same with both deficiencies. The results demonstrate that the extent of A-site deficiency and the Ca concentration in the A-site have a significant impact on the microstructure (sinterability), conductivity, and catalytic activity of electrodes. Segregation of Nd from the lattice with 5% A-site deficiency was observed as a result of thermal treatment at low pO2. Among the studied materials, the highest total electrical conductivity of porous electrode layer at 850 °C and in 97% H2 + 3% H2O atmosphere was 4.8 S cm–1 observed for the Nd0.2Sr0.35Ca0.35Ti0.95Fe0.05O3−δ (10NSCTF-35). The highest electrochemical performance was observed in the case of Nd0.2Sr0.25Ca0.45Ti0.95Fe0.05O3−δ (10NSCTF-45), which showed a polarization resistance value equal to 0.19 Ω cm2 after 100 h of stabilization at 800 °C in a humidified (1.7% H2O) H2 atmosphere. The best electrochemical performance with 606 mW cm–2 power density at 850 °C in 98.3% H2 + 1.7% H2O atmosphere was demonstrated by a 50 wt % Nd0.2Sr0.25Ca0.45Ti0.95Fe0.05O3−δ + 50 wt % Ce0.9Gd0.1O2−δ composite.
本研究探讨了在还原气氛和空气气氛下,A-位缺陷和 Sr/Ca 比率对用于固体氧化物电池的 (Nd0.2Sr0.7-xCax)yTi0.95Fe0.05O3-δ 氢电极的电化学和晶体学特性的影响。研究了 5%和 10%A-位缺陷(Nd0.2Sr0.7-xCax)yTi0.95Fe0.05O3-δ(x = 0.35-0.45, y = 1.05, 1)(简称 5NSCTF-x 和 10NSCTF-x)材料,而两种缺陷的 A-位阳离子之间的比例保持不变。结果表明,A 位点缺失程度和 A 位点中的 Ca 浓度对电极的微观结构(烧结性)、导电性和催化活性有显著影响。在低 pO2 条件下进行热处理时,观察到 A 位缺失 5% 的钕从晶格中分离出来。在所研究的材料中,Nd0.2Sr0.35Ca0.35Ti0.95Fe0.05O3-δ(10NSCTF-35)在 850 ℃ 和 97% H2 + 3% H2O 大气中的多孔电极层总电导率最高,达到 4.8 S cm-1。Nd0.2Sr0.25Ca0.45Ti0.95Fe0.05O3-δ (10NSCTF-45) 的电化学性能最高,在 800 °C 的加湿(1.7% H2O)H2 大气中稳定 100 小时后,其极化电阻值等于 0.19 Ω cm2。50 wt % Nd0.2Sr0.25Ca0.45Ti0.95Fe0.05O3-δ + 50 wt % Ce0.9Gd0.1O2-δ复合材料在 98.3% H2 + 1.7% H2O 大气中于 850 °C 下的电化学性能最佳,功率密度为 606 mW cm-2。
{"title":"Influence of A-Site Deficiency and Ca Concentration on the Electrical and Crystallographic Properties of (Nd0.2Sr0.7–xCax)yTi0.95Fe0.05O3−δ-Based Fuel Electrode for Solid Oxide Cells","authors":"S. Paydar, K. Kooser, O. Volobujeva, S. Granroth, G. Nurk","doi":"10.1021/acsaem.4c00824","DOIUrl":"https://doi.org/10.1021/acsaem.4c00824","url":null,"abstract":"This study explores the impact of A-site deficiency and Sr/Ca ratio on the electrochemical and crystallographic properties of a (Nd<sub>0.2</sub>Sr<sub>0.7–<i>x</i></sub>Ca<sub><i>x</i></sub>)<sub><i>y</i></sub>Ti<sub>0.95</sub>Fe<sub>0.05</sub>O<sub>3−δ</sub> hydrogen electrode for solid oxide cells under reducing and air atmospheres. 5% and 10% A-site deficient (Nd<sub>0.2</sub>Sr<sub>0.7–<i>x</i></sub>Ca<sub><i>x</i></sub>)<sub><i>y</i></sub>Ti<sub>0.95</sub>Fe<sub>0.05</sub>O<sub>3−δ</sub> (<i>x</i> = 0.35–0.45, <i>y</i> = 1.05, 1) (referred to as 5NSCTF-<i>x</i> and 10NSCTF-<i>x</i>) materials were studied, while the ratio between A-site cations was kept the same with both deficiencies. The results demonstrate that the extent of A-site deficiency and the Ca concentration in the A-site have a significant impact on the microstructure (sinterability), conductivity, and catalytic activity of electrodes. Segregation of Nd from the lattice with 5% A-site deficiency was observed as a result of thermal treatment at low pO<sub>2</sub>. Among the studied materials, the highest total electrical conductivity of porous electrode layer at 850 °C and in 97% H<sub>2</sub> + 3% H<sub>2</sub>O atmosphere was 4.8 S cm<sup>–1</sup> observed for the Nd<sub>0.2</sub>Sr<sub>0.35</sub>Ca<sub>0.35</sub>Ti<sub>0.95</sub>Fe<sub>0.05</sub>O<sub>3−δ</sub> (10NSCTF-35). The highest electrochemical performance was observed in the case of Nd<sub>0.2</sub>Sr<sub>0.25</sub>Ca<sub>0.45</sub>Ti<sub>0.95</sub>Fe<sub>0.05</sub>O<sub>3−δ</sub> (10NSCTF-45), which showed a polarization resistance value equal to 0.19 Ω cm<sup>2</sup> after 100 h of stabilization at 800 °C in a humidified (1.7% H<sub>2</sub>O) H<sub>2</sub> atmosphere. The best electrochemical performance with 606 mW cm<sup>–2</sup> power density at 850 °C in 98.3% H<sub>2</sub> + 1.7% H<sub>2</sub>O atmosphere was demonstrated by a 50 wt % Nd<sub>0.2</sub>Sr<sub>0.25</sub>Ca<sub>0.45</sub>Ti<sub>0.95</sub>Fe<sub>0.05</sub>O<sub>3−δ</sub> + 50 wt % Ce<sub>0.9</sub>Gd<sub>0.1</sub>O<sub>2−δ</sub> composite.","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":6.4,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141614928","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Empirical Study of a Polymer-in-Perovskite Precursor: Correlation of the Morphological Changes to the Optoelectronics 聚合物包覆过氧化物前驱体的经验研究:形态变化与光电子学的相关性
IF 6.4 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-12 DOI: 10.1021/acsaem.4c00982
Kartiki Chandratre, Punit Sharma, Suzanne Thomas, Ershad Parvazian, Rahul Patidar, Rodrigo Garcia-Rodriguez, Emmanuel Pean, Rakesh Suthar, Thomas Oliver Dunlop, Sandeep Kumar Pathak, Trystan M. Watson, Supravat Karak
From a wider perspective, the functioning of perovskite-based optoelectronic devices such as solar cells, light-emitting diodes, transistors, and sensors is hugely dependent on the material fabrication of a perovskite active layer, integrating this active layer in the appropriate device architecture and optimizing the device performance by altering various components. An in-depth understanding of the structure-property correlation is, therefore, a key factor for the development of this technology, particularly for industrial large-scale applications. This study aims to comprehend the effect of the material fabrication modifications done at a macroscale, providing insights into the microscale charge-carrier dynamics. Micrograins larger than 100 μm were achieved for the poly(methyl methacrylate) (PMMA)-incorporated triple-cation perovskite precursor with compact film morphology without any antisolvent treatment. A detailed investigation of the crystallization dynamics is strived for. Enhancement in the radiative recombination lifetime from 0.88 μs (for the pristine FAMACs film) to 1.45 μs for the FAMACs film through PMMA incorporation, devoid of any antisolvent treatment, was achieved. Additionally, we appraised our microstructural findings of the photoactive layer against the operating conditions in a device by means of transient photocurrent measurements, aiming for a deeper understanding of the polymer-in-perovskite approach for precursor development.
从更广阔的角度来看,太阳能电池、发光二极管、晶体管和传感器等基于包晶石的光电设备的功能在很大程度上取决于包晶石活性层的材料制造、将活性层集成到适当的设备结构中以及通过改变各种组件优化设备性能。因此,深入了解结构与性能的相关性是该技术发展的关键因素,尤其是在大规模工业应用中。本研究旨在理解在宏观尺度上进行的材料制造改性所产生的影响,从而深入了解微观尺度上的电荷载流子动力学。聚(甲基丙烯酸甲酯)(PMMA)掺杂的三阳离子包晶石前驱体实现了大于 100 μm 的微晶粒,且薄膜形态紧凑,无需任何反溶剂处理。对结晶动力学进行了详细研究。在未进行任何防溶剂处理的情况下,通过加入 PMMA,FAMACs 薄膜的辐射重组寿命从 0.88 μs (原始 FAMACs 薄膜)提高到了 1.45 μs。此外,我们还通过瞬态光电流测量,评估了光活性层的微观结构与设备运行条件之间的关系,旨在加深对聚合物包覆过氧化物前驱体开发方法的理解。
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引用次数: 0
Core–Shell NCM Cathode Particles Mechanical Failure: Particle Cracking and Interfacial Debonding 核壳 NCM 阴极粒子机械故障:粒子开裂和界面脱粘
IF 6.4 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-12 DOI: 10.1021/acsaem.4c01099
Weijia Shen, Ke Li, Jundi Huang, Xinyi Qu, Xiang Chen, Gaoming Fu, Yunfan Li, Yuxiao Zhang, Yixin Lin
The core–shell NCM electrode particles are extensively utilized in lithium-ion batteries (LIBs), exhibiting higher electrochemical performance. However, particle cracking and core/shell interfacial debonding seriously reduce the mechanical stability and lifespan of LIBs. Traditional experimental observations ignore the emergence and evolution of particle cracking and interfacial debonding during cycles. Existing simulation studies mainly focus on predicting whether cracking propagation and interfacial debonding will occur, and lack a comprehensive understanding of the formation and influence mechanisms of cracking and debonding. Therefore, we develop a fracture phase-field model coupling Li+ diffusion and mechanical stress to study the particle cracking and interfacial debonding of spherical core–shell NCM electrode particles in a full lithiation-relaxation-delithiation process. The influence mechanisms of geometrical dimensions (particle size and shell thickness) and mechanical properties (shell Young’s modulus and interfacial fracture toughness) on particle cracking and interfacial debonding are explored. Focusing on the more serious core/shell interfacial debonding, the phase diagrams are constructed to determine the parameters window to prevent core/shell interfacial failure. This work provides a theoretical foundation for understanding the particle cracking and debonding of core–shell NCM electrode particles and supplies the strategies to inhibit interfacial debonding.
核壳 NCM 电极颗粒被广泛应用于锂离子电池(LIB)中,表现出较高的电化学性能。然而,颗粒开裂和核壳界面脱粘严重降低了锂离子电池的机械稳定性和使用寿命。传统的实验观察忽略了颗粒开裂和界面脱粘在循环过程中的出现和演变。现有的模拟研究主要集中在预测裂纹扩展和界面脱粘是否会发生,对裂纹和脱粘的形成和影响机理缺乏全面的了解。因此,我们建立了一个耦合 Li+ 扩散和机械应力的断裂相场模型,以研究球形核壳 NCM 电极颗粒在完全锂化-松弛-脱锂过程中的颗粒开裂和界面脱粘。研究探讨了几何尺寸(颗粒尺寸和外壳厚度)和机械性能(外壳杨氏模量和界面断裂韧性)对颗粒开裂和界面脱粘的影响机制。针对更严重的核/壳界面脱粘现象,构建了相图,以确定防止核/壳界面失效的参数窗口。这项研究为理解核壳 NCM 电极颗粒的开裂和脱粘提供了理论基础,并为抑制界面脱粘提供了策略。
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引用次数: 0
Boosting Lithium Ion Storage of Copper Squarate Via Unsaturated Coordination Frameworks 通过不饱和配位框架提高宝瓶酸铜的锂离子储量
IF 6.4 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-11 DOI: 10.1021/acsaem.4c01257
Heng Lv, Yongwen Wang, Xinyu Gao, Yunfei Shen, Ping Liu, Gang Wang, Long Chen, Tiantian Gu
Metal–organic frameworks (MOFs) have received extreme attention for their applications in lithium-ion batteries due to their large-specific surface area and adjustable composition. However, the limited active sites and low-ion diffusion of the MOF limit its practical applications. In this article, the coordination structure of SA–Cu–SQ is modulated by partially substituting acetic acid for squaric acid (SQ), thereby creating unsaturated coordination sites and exposing some of the metal’s active sites. The electrochemical tests show that the introduction of the unsaturated coordination enables SA–Cu–SQ to possess a higher capacity (1012.5 mA h g–1 after 100 cycles at 0.1 A g–1) than that of Cu–SQ. Furthermore, kinetic tests and ex-situ characterization indicate that the unsaturated coordination not only facilitates Li+ diffusion but also generates additional active sites. Further introducing the unsaturated coordination strategy into rhodizonic acid (RA) gave SA–Cu–RA, which obtained a capacity of 1126.9 mA h g–1 at 0.1 A g–1. This work provides avenues to construct frameworks for high-performance electrochemical materials.
金属有机框架(MOF)因其较大的比表面积和可调节的成分而在锂离子电池中的应用受到极大关注。然而,MOF 有限的活性位点和低离子扩散性限制了其实际应用。本文通过用醋酸部分取代方酸(SQ)来调节 SA-Cu-SQ 的配位结构,从而产生不饱和配位位点并暴露出部分金属活性位点。电化学测试表明,不饱和配位的引入使 SA-Cu-SQ 比 Cu-SQ 具有更高的容量(在 0.1 A g-1 条件下循环 100 次后,容量为 1012.5 mA h g-1)。此外,动力学测试和原位表征表明,不饱和配位不仅有利于 Li+ 扩散,还能产生额外的活性位点。进一步将不饱和配位策略引入到罗地佐酸(RA)中,得到了 SA-Cu-RA,在 0.1 A g-1 的条件下,其容量为 1126.9 mA h g-1。这项工作为构建高性能电化学材料框架提供了途径。
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引用次数: 0
Ultrathin Poly(3-hexylthiophene) Nanowires as Chemically Robust and Versatile Surface Passivators of Perovskite Solar Absorbers 超细聚(3-己基噻吩)纳米线作为化学性质稳定、用途广泛的 Perovskite 太阳能吸收器表面钝化剂
IF 6.4 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-11 DOI: 10.1021/acsaem.4c01393
Dayeon Ko, Heesuk Jung, Minwoo Park
Surface passivation of perovskite solar absorbers is essential for improving device performance and stability. Various defects, such as ionic vacancies and grain boundaries, serve as charge-trapping sites. Suppressing charge recombination through passivation promotes carrier injection/transfer at the interfaces between the perovskite and charge transport layers (CTLs). However, during the fabrication of solar cells, the passivation layers can be damaged during the spin coating of the solutions for the deposition of CTLs. Organic semiconducting passivators can dissolve in nonpolar solvents. Passivators with a high resistance to dissolution in these solutions are necessary to preserve the passivated perovskite surface. In this study, poly(3-hexylthiophene) nanowires (P3HT-NWs) were used to achieve sustainable surface passivation. They were synthesized by cooling P3HT/m-xylene solutions. Ultrathin P3HT-NW layers (2.5 nm thick) uniformly cover the perovskite surface. The lone pair electrons of the thiophene backbones readily coordinate with Pb2+, leading to a significant reduction in the defect density. The band alignment of perovskite and 2,2′,7,7′-tetrakis[N,N-di(4-methoxyphenyl)amino]-9,9′-spirobifluorene (spiro-OMeTAD), which was improved by incorporating P3HT-NW layers, facilitated carrier injection/transfer at their interfaces. The highly crystalline and robust P3HT-NW films remained intact during the spin-coating of the spiro-OMeTAD solutions. The resulting power conversion efficiency (PCE) increased significantly from 18.89% to 20.49%. Furthermore, the normalized PCE of the unencapsulated device was retained at 81.7% of its initial value after 1000 h under 1 sun illumination because the hydrophobic P3HT-NW layers effectively protected the perovskite against moisture.
过氧化物太阳能吸收体的表面钝化对于提高设备性能和稳定性至关重要。离子空位和晶界等各种缺陷是电荷捕获点。通过钝化抑制电荷重组可促进载流子在包晶和电荷传输层(CTL)之间的界面注入/转移。然而,在太阳能电池的制造过程中,钝化层可能会在沉积 CTL 溶液的旋涂过程中受损。有机半导体钝化剂会溶解在非极性溶剂中。要保持钝化的包晶表面,就必须使用在这些溶液中具有高抗溶解性的钝化剂。本研究采用聚(3-己基噻吩)纳米线(P3HT-NWs)来实现可持续的表面钝化。它们是通过冷却 P3HT/m-xylene 溶液合成的。超薄的 P3HT-NW 层(2.5 纳米厚)均匀地覆盖在过氧化物表面。噻吩骨架的孤对电子很容易与 Pb2+ 配位,从而显著降低了缺陷密度。包晶和 2,2′,7,7′-四[N,N-二(4-甲氧基苯基)氨基]-9,9′-螺二芴(spiro-OMeTAD)的能带排列通过加入 P3HT-NW 层而得到改善,从而促进了它们界面上的载流子注入/转移。在螺-OMeTAD 溶液的旋涂过程中,高度结晶和坚固的 P3HT-NW 薄膜保持完好无损。由此产生的功率转换效率(PCE)从 18.89% 显著提高到 20.49%。此外,由于疏水性 P3HT-NW 膜层有效地保护了过氧化物免受湿气的影响,因此在太阳光照射 1000 小时后,未封装器件的归一化 PCE 仍保持在初始值的 81.7%。
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引用次数: 0
Large Area Graphene–MXene Quantum Dot Based High Performance Photochargeable Supercapacitor 基于大面积石墨烯-茂金属量子点的高性能光电超级电容器
IF 6.4 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-11 DOI: 10.1021/acsaem.4c00902
Ayon Das Mahapatra, Sumana Kumar, Pankaj S. Chauhan, Anindita Mondal, Agnimitra Sutradhar, Abha Misra
Photochargeable supercapacitors enable the storage of light induced electrochemical energy. A few layers of graphene and MXene (Ti3C2Tx) quantum dots (QDs) are composited in this work for large photochargeable supercapacitor electrodes. Planar graphene allows overcoming limitations of charge carrier scattering, and MXene QDs on the surface facilitate an efficient light interaction due to the wide band gap. The generated electron–hole pairs in QDs under ultraviolet (UV) illumination are trapped at the interface of graphene and stored in the supercapacitor. An enhancement of 126% in the areal capacitance was observed under UV illumination at a scan rate of 50 mV s–1 . The effect of light interaction on charge storage was further verified by phototransient response and electrochemical impedance spectroscopy under UV illumination. Excellent stability up to 5000 cycles was achieved with a negligible change in capacitance (capacitance retention of ∼105%). A high Coulombic efficiency of ∼95.2% was measured by the galvanic charge–discharge method at a current density of 1 μA cm–2. The photochargeable supercapacitor provides broad future prospects by exploiting the interface of QDs with graphene to obtain enhanced charge storage capacity.
光充电超级电容器能够储存光诱导的电化学能量。在这项工作中,几层石墨烯和 MXene(Ti3C2Tx)量子点(QDs)被复合在一起,制成了大型光充电超级电容器电极。平面石墨烯可以克服电荷载流子散射的限制,而表面上的 MXene 量子点由于具有宽带隙,可以促进有效的光相互作用。在紫外线(UV)照射下,QDs 中产生的电子-空穴对被截留在石墨烯界面上,并储存在超级电容器中。在紫外线照射下,扫描速率为 50 mV s-1 时,电容值提高了 126%。紫外线照射下的光瞬态响应和电化学阻抗光谱进一步验证了光相互作用对电荷存储的影响。在电容变化几乎可以忽略不计(电容保持率为 ∼105%)的情况下,实现了高达 5000 次循环的卓越稳定性。在电流密度为 1 μA cm-2 时,通过电化学充放电法测得的库仑效率高达 95.2%。通过利用 QDs 与石墨烯的界面来获得更强的电荷存储容量,这种可光充电超级电容器具有广阔的前景。
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引用次数: 0
Sub-bandgap Photocurrent Spectra of p–i–n Perovskite Solar Cells with n-Doped Fullerene Electron Transport Layers and Bias Illumination 具有 n 掺杂富勒烯电子传输层和偏置照明的 pi-n Perovskite 太阳能电池的亚带隙光电流光谱
IF 6.4 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-11 DOI: 10.1021/acsaem.4c01077
Bas T. van Gorkom, Aron Simons, Willemijn H. M. Remmerswaal, Martijn M. Wienk, René A. J. Janssen
In p–i–n perovskite solar cells optical excitation of defect states at the interface between the perovskite and fullerene electron transport layer (ETL) creates a photocurrent responsible for a distinct sub-bandgap external quantum efficiency (EQE). The precise nature of these signals and their impact on cell performance are largely unknown. Here, the effect of n-doping the fullerene on the EQE spectra is studied. The n-doped fullerene is either deposited from solution or by coevaporation. The latter method is used to create undoped–doped fullerene bilayers and investigate the effect of the proximity of the doped region on the EQE spectra. The intensity of the sub-bandgap EQE increases when the ETL is n-doped and also when the device is biased with green light. Using these results, the sub-bandgap EQE signal is attributed to originate from electron trap states in the perovskite with an energy below the conduction band that are filled by excitation with low-energy photons. The trapped electrons give rise to photocurrent when they are collected at a nearby electrode. The enhanced sub-bandgap EQE observed when the ETL is n-doped or bias light is applied, is related to a higher probability to extract trapped electrons under these conditions.
在 pi-i-n 包晶体太阳能电池中,包晶体和富勒烯电子传输层(ETL)界面上的缺陷态的光激发会产生光电流,从而产生明显的亚带隙外部量子效率(EQE)。这些信号的确切性质及其对电池性能的影响在很大程度上是未知的。本文研究了富勒烯 n 掺杂对 EQE 光谱的影响。n 掺杂富勒烯可以从溶液中沉积,也可以通过共蒸发沉积。后一种方法用于创建未掺杂富勒烯双层膜,并研究掺杂区域的接近程度对 EQE 光谱的影响。当 ETL 为 n 掺杂时,亚带隙 EQE 的强度会增加,当器件使用绿光偏压时,亚带隙 EQE 的强度也会增加。根据这些结果,亚带隙 EQE 信号可归因于过氧化物中能量低于导带的电子捕获态,这些捕获态在低能量光子的激发下被填充。当被捕获的电子被收集到附近的电极时,就会产生光电流。当 ETL 为正掺杂或施加偏置光时,所观察到的亚带隙 EQE 会增强,这与在这些条件下提取被困电子的概率较高有关。
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引用次数: 0
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