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Preparation of fluorine-doped α-Ni hydroxides as alkaline water electrolysis catalysts via the liquid phase deposition method† 通过液相沉积法制备掺氟 α-Ni 氢氧化物作为碱性水电解催化剂
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-08-27 DOI: 10.1039/D4SE00983E
Tomoyuki Watanabe, Kenko Tsuchimoto, Tomohiro Fukushima, Kei Murakoshi, Minoru Mizuhata and Hiro Minamimoto

A room-temperature liquid phase process was utilized to prepare α-Ni(OH)2 thin films with high crystallinity for use as oxygen evolution reaction catalysts under strongly alkaline conditions. It was discovered that the catalytic activity of the prepared catalyst is sensitive to pH during the liquid phase process. Specifically, under optimized reaction conditions, we found that the synthesized α-Ni(OH)2 thin film showed relatively high catalytic activity and high stability across potential scans. Our structural analyses revealed that the fluorine incorporation within the framework of α-Ni(OH)2 was the origin of the high catalytic activity. And also, the catalytic activity depending on the sample preparation conditions was discussed through the ex situ and in situ measurements of the electrode surface. This work provides insights into the potential of the solution process for preparing high crystal materials with high reproducibility as an electrode preparation procedure.

利用室温液相工艺制备了具有高结晶度的 α-Ni(OH)2 薄膜,用于强碱性条件下的氧进化反应催化剂。研究发现,在液相过程中,所制备催化剂的催化活性对 pH 值非常敏感。具体地说,在优化的反应条件下,我们发现合成的 α-Ni(OH)2 薄膜显示出相对较高的催化活性和跨电位扫描的高稳定性。我们的结构分析表明,α-Ni(OH)2 框架内的氟掺杂是高催化活性的来源。此外,通过对电极表面的原位和原位测量,我们还讨论了催化活性取决于样品制备条件的问题。这项研究深入探讨了溶液法制备高晶体材料的潜力,并将其作为一种电极制备程序,具有很高的可重复性。
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引用次数: 0
Sulfur vacancy induced radical generation in ZnIn2S4 for lignin photocatalytic Cα–Cβ cleavage† ZnIn2S4 中的硫空位诱导自由基生成,用于木质素光催化 Cα-Cβ 裂解
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-08-26 DOI: 10.1039/D4SE00741G
Jifang Zhang, Jinde Sun, Chengcheng Suo, Wei Li, Sha Luo, Bing Tian, Chunhui Ma and Shouxin Liu

The low efficiency of photogenerated charge transfer to generate reactive oxygen species is the main factor that limits the photocatalytic activity of ZnIn2S4 (ZIS)-based materials in lignin depolymerization. In this work, we prepared an efficient ZIS catalyst with a hexagonal crystal structure and three-dimensional flower-like micromorphology by a solvothermal method. The ZIS catalyst possessed abundant active sites and efficient light-harvesting ability. Sulfur vacancies (Sv) were introduced into the ZIS photocatalyst (ZIS-Sv) to enhance its electron-withdrawing ability and promote the separation and transfer of photogenerated charges. Using the ZIS-Sv photocatalyst, the conversion rate of Cα–Cβ bonds in the β-O-4 dimer reached 96.31% and the molar yields (selectivity) of phenol and acetophenone were 695.17 μmol g−1 h−1 (85.14%) and 610.66 μmol g−1 h−1 (74.73%), respectively (with a ZIS-Sv0.6 concentration of 1 mg ml−1, irradiation time of 6 h, ethanol content of 90%, pH of 5, and 2-phenoxyacetophenone concentration of 1 mg ml−1). The photocatalytic depolymerization of dioxane lignin by the ZIS-Sv photocatalyst reached an efficiency of 80.42%. Catalyst characterization results and mechanism studies indicated that Sv promoted effective electron adsorption to generate oxygen radicals ˙OH and ˙O2 through O2 single-electron reduction and H2O decomposition, respectively. Then, the oxygen radicals combined with C-centered radicals to form unstable intermediates, further breaking lignin linkages, which finally formed an efficient indirect oxidation process. It is expected that introducing Sv into ZIS materials is a useful strategy to obtain photocatalysts for Cα–Cβ cleavage to realize efficient photocatalytic lignin depolymerization.

光生电荷转移产生活性氧的效率低是限制 ZnIn2S4(ZIS)基材料在木质素解聚过程中光催化活性的主要因素。在这项工作中,我们采用溶热法制备了一种具有六方晶体结构和三维花状微观形貌的高效 ZIS 催化剂。该 ZIS 催化剂具有丰富的活性位点和高效的光收集能力。在 ZIS 光催化剂(ZIS-Sv)中引入了硫空位(Sv),以增强其电子吸收能力,促进光生电荷的分离和转移。使用 ZIS-Sv 光催化剂,β-O-4 二聚体中 Cα-Cβ 键的转化率达到 96.31%,苯酚和苯乙酮的摩尔产率(选择性)分别为 695.17 μmol g-1 h-1 (85.14%) 和 610.66 μmol g-1 h-1 (74.73%)(ZIS-Sv0.6浓度为1 mg ml-1,辐照时间为6 h,乙醇含量为90%,pH值为5,2-苯氧基苯乙酮浓度为1 mg ml-1)。ZIS-Sv 光催化剂对二恶烷木质素的光催化解聚效率达到 80.42%。催化剂表征结果和机理研究表明,Sv 促进有效电子吸附,通过 O2 单电子还原和 H2O 分解分别生成氧自由基 ˙OH 和 ˙O2-。然后,氧自由基与 C 中心自由基结合形成不稳定的中间产物,进一步破坏木质素连接,最终形成高效的间接氧化过程。预计在 ZIS 材料中引入 Sv 是获得 Cα-Cβ 裂解光催化剂以实现高效光催化木质素解聚的有效策略。
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引用次数: 0
Synthesis of “all-in-one” hypercrosslinked organic polymers: experimental and kinetic models for CO2 chemical fixation and iodine adsorption† 一体化 "超交联有机聚合物的合成:二氧化碳化学固定和碘吸附的实验和动力学模型
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-08-23 DOI: 10.1039/D4SE01033G
Xuanbo Liu, Yongjing Hao, Xiuli Yan, Yuhang Zhang, Xionglei Wang, Zheng Zhu, Jiajia Yang, Shuangshuo Li, Tao Chang and Shenjun Qin

A series of “all-in-one” hypercrosslinked polymers (HCPOH-Cn) have been synthesized by Friedel–Crafts alkylation of phenols tethered with adjustable alkyl chains and the quaternization reaction of N,N-dimethylethylenediamine in one-pot in the presence of dibromomethylbenzene as the crosslinking and ammonium agent. After characterization, the polymers were implemented for sustainable CO2 conversion and iodine adsorption. The experimental results showed that HCPOH-C12 can effectively catalyze the CO2 cycloaddition reaction, and an excellent yield of 94% was confirmed after optimizing the conditions. The outstanding activity is attributed to the lower activation energy (69.52 kJ mol−1). The polymer of HCPOH-C12 exhibits excellent substrate adaptability and recyclability, and a possible catalytic mechanism has been proposed. Furthermore, HCPOH-C0 has showcased an impressive adsorption capacity for iodine, with the process aligning well with second-order adsorption kinetics and conforming to Langmuir adsorption isotherms. Iodine adsorption on HCPOH-C0 is characterized as a spontaneous and endothermic process, indicative of an increase in the disorder at the solid–liquid interface during the adsorption phase.

在二溴甲基苯作为交联剂和铵剂的存在下,通过对以可调烷基链为系链的苯酚进行弗里德尔-卡夫烷基化反应,以及对 N,N-二甲基乙二胺进行季铵化反应,我们合成了一系列 "一体化 "超交联聚合物(HCPOH-Cn)。经过表征后,聚合物被用于可持续的二氧化碳转化和碘吸附。实验结果表明,HCPOH-C12 能有效催化 CO2 环加成反应,在优化条件后,产率高达 94%。其出色的活性归功于较低的活化能(69.52 kJ mol-1)。HCPOH-C12 聚合物具有出色的底物适应性和可回收性,并提出了一种可能的催化机理。此外,HCPOH-C0 还显示出惊人的碘吸附能力,其吸附过程与二阶吸附动力学非常吻合,并符合朗缪尔吸附等温线。HCPOH-C0 对碘的吸附是一个自发的内热过程,表明在吸附阶段固液界面的无序性增加。
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引用次数: 0
Fiber-shaped aqueous zinc ion batteries for wearable energy solutions 用于可穿戴能源解决方案的纤维状锌离子水电池
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-08-22 DOI: 10.1039/D4SE00853G
Jiazhe Cheng, Shou-xiang Jiang and Hao Jia

The rising popularity of smart wearable electronic devices has spurred advancements in portable battery technology, particularly in the realm of aqueous zinc-ion batteries (AZIBs). This paper explores the advancements in AZIBs, and highlights their advantages – they are high in energy density, very safe, and cost effective. Notably, fiber-shaped AZIBs can be constructed with various structural configurations to meet different application requirements and seamlessly integrated into wearable products due to their compatibility with different types of fabrics. By weaving fiber-shaped AZIBs into textiles, a new type of energy textile can be obtained, which is flexible and breathable, with miniaturization potential previously unattainable with conventional power sources.

智能可穿戴电子设备的日益普及推动了便携式电池技术的发展,尤其是在锌离子水电池(AZIBs)领域。本文探讨了 AZIB 的进展,并强调了其优势--能量密度高、非常安全且成本效益高。值得注意的是,纤维状 AZIB 可以通过不同的结构配置来满足不同的应用要求,并且由于其与不同类型织物的兼容性,可以无缝集成到可穿戴产品中。通过将纤维状 AZIB 编织到纺织品中,可以获得一种新型能源纺织品,这种纺织品具有柔韧性和透气性,而且具有传统能源无法实现的微型化潜力。
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引用次数: 0
Enhancing organic solar cell lifetime through humidity control using BCF in PM6 : Y6 active layers† 利用 PM6:Y6 活性层中的 BCF 控制湿度,延长有机太阳能电池的使用寿命
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-08-22 DOI: 10.1039/D4SE00598H
Kaike Pacheco, João Paulo Araújo Souza, Marlus Koehler, Eswaran Jayaraman, Daniel Garcia Martos, Vida Turkovic, Morten Madsen and Lucimara Stolz Romana

Enhancing the longevity of efficient organic solar cells (OSCs) remains a central focus in contemporary research. Many strategies have been explored, including material modifications in active layers, electrodes, interlayers, and encapsulation, all aiming at improving OSC lifetimes. This study introduces an innovative approach by incorporating a third element, the tris(pentafluorophenyl)borane (BCF) molecule, which interacts significantly with the active layer materials in OSCs. Functioning as a p-type dopant, BCF was carefully integrated into the active layer, resulting in power conversion efficiencies comparable to those of undoped devices. This allowed a detailed analysis of its influence on stability. Through systematic investigations, BCF's ability to react with water molecules, which acts in OSC degradation, was identified. Devices with BCF exhibited impressive enhancements in longevity, particularly evident in electrical properties, such as increased open-circuit voltage and hole mobility. Notably, the donor polymer experienced more pronounced alterations during degradation in the presence of BCF than the acceptor molecule. Quantum chemical calculations elucidated the regions of the polymer backbone interacting with BCF and the effects of this interaction. It is inferred that BCF's reaction with water generates protons, which subsequently associate with PBDB-T-2F (PM6) through the sulfur atom. In conclusion, this research demonstrates that BCF addition offers intrinsic protection to OSCs, leading to significant advancements in their durability.

提高高效有机太阳能电池(OSC)的使用寿命仍然是当代研究的核心重点。人们探索了许多策略,包括活性层、电极、中间层和封装的材料改性,所有这些都旨在提高有机太阳能电池的寿命。本研究引入了一种创新方法,即加入第三种元素--三(五氟苯基)硼烷(BCF)分子。作为一种 p 型掺杂剂,BCF 被小心地集成到有源层中,从而使功率转换效率与未掺杂器件相当。这样就可以详细分析 BCF 对稳定性的影响。通过系统研究,我们发现了 BCF 与水分子发生反应的能力,而水分子会导致 OCS 降解。含有 BCF 的器件在寿命方面表现出令人印象深刻的增强,尤其是在电性能方面,例如开路电压和空穴迁移率的增加。值得注意的是,在 BCF 存在的降解过程中,供体聚合物比受体分子发生了更明显的变化。量子化学计算阐明了与 BCF 发生相互作用的聚合物骨架区域以及这种相互作用的影响。据推断,BCF 与水反应产生质子,质子随后通过硫原子与 PBDB-T-2F (PM6) 结合。总之,这项研究表明,添加 BCF 可为 OSC 提供内在保护,从而显著提高其耐用性。
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引用次数: 0
Study on the impact of battery pack arrangement on temperature uniformity distribution 电池组排列对温度均匀性分布影响的研究
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-08-20 DOI: 10.1039/D4SE00459K
ZhongXing Ji and Chao Zhang

Lithium-ion batteries are widely used in portable electronic devices and electric vehicles. However, the thermal performance of lithium-ion batteries is a major concern, as overheating can lead to safety hazards. This study aims to investigate the impact of structural parameters on the temperature field of battery packs, with a focus on, the width of wedge-shaped channels, inclination angles, and gaps between battery cells. Through numerical simulation analysis and experimental validation, the results demonstrate that different structural parameters have a significant influence on the temperature distribution and thermal management performance within the battery pack. Optimizing the wedge-shaped flow channel in the upper section of the battery pack (width: 20 mm to 60 mm) improves cooling efficiency and temperature uniformity, with a narrower width (20 mm) resulting in a lower maximum temperature (311.5 K) and smaller temperature difference between cells (1.8 K). By optimizing the inclination angle in battery pack configurations, the temperature distribution can be significantly improved, with a 12° inclination angle resulting in a maximum temperature reduction to 311.2 K and a maximum temperature difference reduction to 1.5 K, thus enhancing the thermal performance and lifespan of the battery pack. The gap dimension between batteries can significantly affect the heat dissipation performance of the battery pack, and the smaller gap makes the temperature distribution between each battery cell more uniform, and the highest temperature can be reduced by about 10 K, which enhances the stability and service life of the battery pack. In conclusion, by carefully designing and optimizing the structural parameters of battery packs, manufacturers can enhance the thermal management effectiveness of battery systems, improve performance and reliability, and drive the development of electric vehicles (EV) and renewable energy storage technologies.

锂离子电池广泛应用于便携式电子设备和电动汽车。然而,锂离子电池的热性能是一个主要问题,因为过热会导致安全隐患。本研究旨在探讨结构参数对电池组温度场的影响,重点是楔形通道的宽度、倾斜角度和电池单元之间的间隙。通过数值模拟分析和实验验证,结果表明不同的结构参数对电池组内的温度分布和热管理性能有显著影响。优化电池组上部的楔形流道(宽度:20 毫米至 60 毫米)可提高冷却效率和温度均匀性,较窄的宽度(20 毫米)可降低最高温度(311.5 K),缩小电池单元之间的温差(1.8 K)。通过优化电池组配置中的倾角,可显著改善温度分布,12°倾角可使最高温度降至 311.2 K,最大温差降至 1.5 K,从而提高电池组的散热性能和使用寿命。电池之间的间隙尺寸会显著影响电池组的散热性能,间隙越小,每个电池单元之间的温度分布越均匀,最高温度可降低约 10 K,从而提高了电池组的稳定性和使用寿命。总之,通过精心设计和优化电池组的结构参数,制造商可以增强电池系统的热管理效果,提高性能和可靠性,推动电动汽车(EV)和可再生能源存储技术的发展。
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引用次数: 0
A surface sulfurization strategy for tuning the lithiophilicity of garnet electrolyte pellets towards advanced solid-state lithium metal electrolyte† 调整石榴石电解质颗粒亲锂性的表面硫化策略,实现先进的固态锂金属电解质†。
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-08-19 DOI: 10.1039/D4SE00784K
Genxi Yu, Youchun Wu, Dawei Sha, Jianwen Cai, Gaofa Nie, Yaping Wang, Long Pan and ZhengMing Sun

Garnet solid-state electrolytes (SSEs) have extraordinary application prospects due to their high room temperature ionic conductivity and high stability to lithium metal. However, when exposed to air during the preparation process, contaminants are inevitably generated on the electrolyte surface, resulting in poor wettability of the Li/garnet interface and high interfacial resistance. Moreover, solid-state batteries assembled with contaminated electrolytes can easily lead to the formation and expansion of lithium dendrites. Herein, we demonstrate a surface chemistry strategy of rapid vulcanization treatment to improve interface problems by introducing lithium sulfides into the garnet electrolyte. Compared to the surface contaminants (e.g., Li2CO3) on garnet, lithium sulfides (e.g., Li2S) have several advantages; it is a good Li+ conductor and has good wettability to both the garnet surface and Li metal anode. The interfacial resistance of the vulcanized garnet-SSE pellets decreased from 2961 Ω cm2 for LLZT@LC to 391 Ω cm2 for LLZT@LS. In addition, the lithium symmetric battery assembled by using LLZT@LS pellets exhibits stable plating/stripping cycling performance and ultralow overpotential at a current of 0.2 mA cm−2 without Li dendrite growth. Moreover, the LiFePO4/Li batteries with LLZT@LS pellets show excellent rate performances and cycling stability (114.3 mA h g−1 @ 0.5C after 150 cycles) with a capacity retention of 86%. These results demonstrate that the rapid treatment of garnet contaminants by a surface chemistry strategy is not only a simple and efficient solution but also provides strong support for the realization of high-performance solid-state lithium metal batteries (SSLMBs).

石榴石固态电解质(SSE)具有高室温离子电导率和对锂金属的高稳定性,因此具有非凡的应用前景。然而,在制备过程中暴露于空气中时,电解质表面不可避免地会产生污染物,导致锂/石榴石界面润湿性差和界面电阻高。此外,用受污染的电解质组装固态电池很容易导致锂枝晶的形成和扩展。在此,我们展示了一种快速硫化处理的表面化学策略,通过在石榴石电解液中引入锂硫化物来改善界面问题。与石榴石的表面污染物(如 Li2CO3)相比,锂硫化物(如 Li2S)有几个优点:它是一种良好的 Li+ 导体,对石榴石表面和锂金属阳极都有良好的润湿性。硫化石榴石-SSE 颗粒的界面电阻从 LLZT@LC 的 2961 Ω cm2 降至 LLZT@LS 的 391 Ω cm2。此外,使用 LLZT@LS 颗粒组装的锂对称电池具有稳定的电镀/剥离循环性能,在 0.2 mA cm-2 电流下具有超低的过电位,且无锂枝晶生长。此外,使用 LLZT@LS 颗粒的磷酸铁锂/锂电池显示出优异的速率性能和循环稳定性(150 次循环后,114.3 mA h g-1 @ 0.5C),容量保持率高达 86%。这些结果表明,通过表面化学策略快速处理石榴石污染物不仅是一种简单高效的解决方案,而且还为实现高性能固态锂金属电池(SSLMB)提供了强有力的支持。
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引用次数: 0
Intermittent control switch characteristics of triboelectric electric hybrid energy harvesting devices and power management circuits† 三电混合电动能量收集装置和电源管理电路的间歇控制开关特性
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-08-19 DOI: 10.1039/D4SE00754A
Xin Yu, Mingxing Cui, Wendong Qi, Xinrui Li, Yuhang Xing, Xiaolei Lu, Shitong Yang, Jing Zhao and Changhong Jiang

Renewable energy sources such as wind, vibration, and tidal energy are widely available in everyday life, with scenarios where multiple renewable energy sources coexist. If multiple energy sources are collected efficiently, energy collection utilization and power generation will be increased. In this study, a triboelectric electric hybrid energy harvesting device (HEH-TENG) capable of harvesting rotational and vibrational mechanical energy is proposed in addition to a hybrid energy harvesting circuit (HEH-PMC) with intermittent control switches. The HEH-TENG is divided into a rotational triboelectric nanogenerator (R-TENG), which collects rotational mechanical energy, and a vibrational triboelectric nanogenerator (V-TENG), which collects vibrational mechanical energy. The HEH-PMC includes a rectifier module, energy storage module, comparison and detection module, switching module, and filtering module. The comparison and detection module includes a PNP-type triode and a detection capacitor, and the detection capacitor is connected to the emitter of the triode. The TENG is charged for the detection capacitor. When the voltage of the detection capacitor reaches a certain value, the triode is turned on. The thyristor SCR of the switching module is triggered after the transistor conducts, thus transferring the electrical energy in the storage capacitor to the back-end circuit. A new charging process is generated once the discharge of the storage capacitor is completed, thus realising intermittent control of switching conductivity. The HEH-PMC achieves stable power output, and the charging efficiency of the HEH-PMC is improved by 892% compared to a normal charging circuit when the R-TENG and V-TENG are operated simultaneously under the condition of charging a filter capacitor with a capacitance of 22 μF to 5 V without a load. The circuit was tested for its ability to carry a load. To simulate a micropower sensor, resistors with resistance values ranging from 100 kΩ to 3 MΩ were selected as loads for testing. A comparison of the back-end load voltages of the HEH-TENG and general-purpose power supply circuits under the same conditions shows that the output voltage of the HEH-PMC is higher than that of the general-purpose power supply circuit. When a 220 kΩ resistor is used as the load, the voltage increases from 0.53 V to 3.9 V, which is 7.36 times the voltage of the general power supply circuit and 54.15 times its power, indicating that the HEH-PMC has higher load capacity. Thus, this study provides a strategy for a hybrid energy harvesting approach for TENGs as well as hybrid energy harvesting power management circuits, and the approach is expected to expand the practical applications of TENGs.

风能、振动能和潮汐能等可再生能源广泛存在于日常生活中,并存在多种可再生能源共存的情况。如果能有效收集多种能源,就能提高能源收集利用率和发电量。本研究提出了一种能够收集旋转和振动机械能的三电混合能量收集装置(HEH-TENG),以及一种带有间歇控制开关的混合能量收集电路(HEH-PMC)。HEH-TENG 分为收集旋转机械能的旋转三电纳米发电机 (R-TENG) 和收集振动机械能的振动三电纳米发电机 (V-TENG)。HEH-PMC 包括整流器模块、储能模块、比较和检测模块、开关模块以及滤波模块。比较和检测模块包括一个 PNP 型三极管和一个检测电容器,检测电容器连接到三极管的发射极。TENG 为检测电容器充电。当检测电容器的电压达到一定值时,三极管被接通。三极管导通后,开关模块的晶闸管可控硅被触发,从而将存储电容器中的电能传输到后端电路。存储电容器放电完成后,会产生一个新的充电过程,从而实现开关导电性的间歇控制。HEH-PMC 实现了稳定的功率输出,当 R-TENG 和 V-TENG 同时工作时,在无负载的条件下将电容为 22 μF 的滤波电容器充电至 5 V,HEH-PMC 的充电效率比普通充电电路提高了 892%。对电路的负载能力进行了测试。为模拟微功率传感器,选择了阻值从 100 kΩ 到 3 MΩ 的电阻器作为测试负载。对相同条件下 HEH-TENG 和通用电源电路的后端负载电压进行比较后发现,HEH-PMC 的输出电压高于通用电源电路。当使用 220 kΩ 电阻作为负载时,电压从 0.53 V 上升到 3.9 V,是通用电源电路电压的 7.36 倍,功率的 54.15 倍,这表明 HEH-PMC 具有更高的负载能力。因此,本研究为 TENG 的混合能量采集方法以及混合能量采集电源管理电路提供了一种策略,该方法有望拓展 TENG 的实际应用。
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引用次数: 0
Experimental and theoretical insights into benzene-1,4-dicarboxylic acid based Co-MOFs: an anodic material for expedient battery-supercapacitor hybrids† 基于苯-1,4-二羧酸的 Co-MOFs 的实验和理论研究:一种用于电池和超级电容器混合材料的阳极材料†。
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-08-19 DOI: 10.1039/D4SE00590B
Junaid Khan, Anique Ahmed, Muhammad Imran Saleem and Abdullah A. Al-Kahtani

Hybrid supercapacitors, integrating both faradaic and non-faradaic mechanisms, have emerged as promising energy storage devices owing to their high energy density and excellent cycling stability. In the pursuit of sustainable energy storage solutions, the development of advanced materials has garnered significant attention. Herein, we report benzene-1,4-dicarboxylic acid-based cobalt metal-organic frameworks (Co-MOFs) for application in battery supercapacitor hybrid configuration. The Co-MOFs were synthesized via a simple and scalable hydrothermal method, resulting in a mixed nanoflower structure. The electrochemical setup of a bare electrode uncovers its marvelous advantages with a specific capacity of 500.80 C g−1 (3 mV s−1) and 411.13 C g−1 (1.0 A g−1). A predominant diffusive nature of the Co-MOFs (89.11% at 3 mV s−1) was revealed via a simulation approach that back these merits. Furthermore, an asymmetric supercapacitor assembled with the Co-MOFs and activated carbon exhibited high specific capacity (254.45 C g−1), along with outstanding specific energy and power (60.07 W h kg−1 and 850 W kg−1, respectively). Besides, satisfactory rate capability (retains 58.47% of its specific capacity and energy while boosting specific power by 6 times) and a stable cycling life were observed. The simulation of experimental outcomes revealed the hybrid nature of the device with 80.01% diffusive and 76.72% capacitive contribution at 3 and 100 mV s−1, respectively. The findings unveil the Co-MOFs as an excellently tailored and eco-conscious choice for electrode materials in advanced energy storage devices, driving advancements in sustainable energy technologies.

混合超级电容器融合了法拉第和非法拉第两种机制,具有高能量密度和出色的循环稳定性,已成为前景广阔的储能设备。在追求可持续储能解决方案的过程中,先进材料的开发备受关注。在此,我们报告了苯-1,4-二羧酸基钴金属有机框架(Co-MOFs)在电池超级电容器混合配置中的应用。Co-MOFs 是通过一种简单且可扩展的水热法合成的,形成了一种混合纳米花结构。裸电极的电化学设置揭示了其惊人的优势,比容量为 500.80 C g-1(3 mV s-1)和 411.13 C g-1(1.0 A g-1)。通过一种支持这些优点的模拟方法,发现了 Co-MOFs 的主要扩散特性(3 mV s-1 时为 89.11%)。此外,用 Co-MOFs 和活性炭组装的不对称超级电容器显示出很高的比容量(254.45 C g-1),以及出色的比能量和比功率(分别为 60.07 W h kg-1 和 850 W kg-1)。此外,还观察到了令人满意的速率能力(保留了 58.47% 的比容量和能量,同时比功率提高了 6 倍)和稳定的循环寿命。对实验结果的模拟揭示了该器件的混合性质,在 3 mV s-1 和 100 mV s-1 时,扩散贡献率分别为 80.01%,电容贡献率为 76.72%。研究结果表明,Co-MOFs 是先进储能设备电极材料中一种极佳的定制和环保选择,可推动可持续能源技术的进步。
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引用次数: 0
Cu2NiSnS4/g-C3N4 S-scheme photocatalysts: interfacial surface trap states vs. hydrogen production† Cu2NiSnS4/g-C3N4 S 型光催化剂:界面表面阱态与氢气产生
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-08-16 DOI: 10.1039/D4SE00744A
Rugma T. P., Rishi Krishna B. S., K. Priyanga Kangeyan, Neppolian Bernaurdshaw, Abdullah Saad AlArifi and Sandeep Kumar Lakhera

Graphitic carbon nitride (g-C3N4), a two-dimensional semiconducting material, shows promise in energy conversion but faces challenges such as rapid charge carrier recombination and poor visible-light absorption. To address these issues, we integrated Cu2NiSnS4 (CNTS) with g-C3N4 using an ultrasonication-assisted microwave irradiation method and observed that incorporating g-C3N4 with 5 wt% CNTS produced 4.6 μmol of sacrificial hydrogen under direct sunlight irradiation over 4 h. This presents a significant 38-fold increase in photocatalytic hydrogen production compared to that of bare g-C3N4. However, increasing the CNTS loading beyond 5 wt% gradually decreased hydrogen production. Higher CNTS loading also caused gradual quenching of photoluminescence spectra, which contradicts the hydrogen evolution results. On the other hand, time-resolved photoluminescence measurements indicated a shorter charge carrier lifetime in the composite, suggesting higher non-radiative recombination and/or a faster charge carrier separation rate. The discrepancies between PL spectra, TRPL measurements, and hydrogen production suggest the presence of a higher density of surface trap states at the CNTS/g-C3N4 interface. These trap states likely facilitate faster charge separation at lower CNTS loadings but lead to increased non-radiative recombination at higher loadings, thereby reducing hydrogen production. The CNTS/g-C3N4 photocatalysts showed outstanding stability over a period of ten cycles under a xenon lamp. This work provides new insights into interfacial charge transfer dynamics in heterojunction photocatalysts.

氮化石墨碳(g-C3N4)是一种二维半导体材料,在能量转换方面前景广阔,但面临着电荷载流子快速重组和可见光吸收差等挑战。为了解决这些问题,我们采用超声辅助微波辐照法将 Cu2NiSnS4(CNTS)与 g-C3N4 集成在一起,并观察到在太阳光直射下,加入 5 wt% CNTS 的 g-C3N4 在 4 小时内产生了 4.6 μmol 的牺牲氢,与裸 g-C3N4 相比,光催化产氢量显著增加了 38 倍。然而,将 CNTS 的负载量提高到 5 wt% 以上后,制氢量逐渐减少。更高的 CNTS 含量还会导致光致发光光谱逐渐淬灭,这与氢气进化结果相矛盾。另一方面,时间分辨光致发光测量结果表明,复合材料中的电荷载流子寿命较短,这表明非辐射重组较高和/或电荷载流子分离速率较快。光致发光光谱、TRPL 测量和氢气产生之间的差异表明,CNTS/g-C3N4 界面存在更高密度的表面陷阱态。这些捕获态可能会在较低的 CNTS 负载下加快电荷分离速度,但在较高负载下会导致非辐射重组增加,从而降低氢气产生量。在氙灯照射下,CNTS/g-C3N4 光催化剂在十次循环过程中表现出卓越的稳定性。这项研究为异质结光催化剂的界面电荷转移动力学提供了新的见解。
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Sustainable Energy & Fuels
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