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Integrating theoretical and experimental insights into nanoporous gold electrochemistry for enhanced baicalein sensing performance 将理论和实验见解融入纳米多孔金电化学,提高黄芩素传感性能
IF 5.5 3区 材料科学 Q1 ELECTROCHEMISTRY Pub Date : 2024-11-04 DOI: 10.1016/j.electacta.2024.145316
Antonio Gomes dos Santos Neto , Jose Antonio de Oliveira Junior , Glaucio Régis Nagurniak , Shuai Zhang , Marcelo Eduardo Huguenin Maia da Costa , Liying Liu , Marco Aurélio Suller Garcia , Sergio Yesid Gómez González , Maurício Jeomar Piotrowski , Cristiane Luisa Jost
We introduce an innovative electrochemical sensing method for the sensitive detection of Baicalein (BAI), emphasizing a simple surface modification process. The study encompasses both practical and theoretical investigations into the electrochemical behavior of nanoporous gold. Our theoretical analysis, based on advanced quantum-mechanical calculations, demonstrates that the adsorption of BAI molecule on gold-based substrates is energetically favorable, with adsorption energy increasing from an unmodified surface to a more porous substrate. BAI physisorbs on unmodified regions in a horizontal alignment, while it chemisorbs more strongly on nanoporous regions by penetrating the pores. On less modified surfaces, interaction energy predominates, whereas on heavily modified surfaces, distortion energies become more significant due to increased substrate reactivity. These results align with physicochemical characterizations, which reveal that nanoscale modifications, induced by different anodization times, explain the variations in electrode performance. Experimentally, cyclic voltammetry (CV) and differential pulse voltammetry (DPV) were employed using both a gold electrode (GE) and a nanoporous gold electrode (NPGE). The GE was subjected to surface treatment by immersion in H2SO4 and potential control at ca. +2.0 V for 40 seconds, resulting in a nanoporous configuration. Following optimizations, Adsorptive Stripping Voltammetry (AdSV) was used to determine BAI. The method achieved detection (LOD) and quantification (LOQ) limits of 0.015 µmol L-1 and 0.045 µmol L-1, respectively (Edeposition=-0.25 V; tdeposition=50 s). Additionally, the standard addition method was applied to the NPGE for recovering BAI from spiked synthetic human plasma and urine, with success rates ranging from 93.4% to 106%. This approach exhibited excellent stability, precision, and accuracy, with minimal interference from other substances. Moreover, the theoretical findings provided deeper insights into the selective electrochemical detection of BAI on nanoporous gold surfaces, offering new perspectives on this field.
我们介绍了一种用于灵敏检测黄芩素(BAI)的创新电化学传感方法,强调了一种简单的表面改性工艺。这项研究包括对纳米多孔金电化学行为的实践和理论研究。我们基于先进量子力学计算的理论分析表明,BAI 分子在金基基底上的吸附在能量上是有利的,从未修改的表面到多孔基底,吸附能不断增加。BAI 在未改性区域以水平排列的方式进行物理吸附,而在纳米多孔区域则通过穿透孔隙进行更强的化学吸附。在改性程度较低的表面上,相互作用能占主导地位,而在改性程度较高的表面上,由于基底反应活性的增加,畸变能变得更加重要。这些结果与物理化学特征相吻合,表明不同阳极氧化时间引起的纳米级改性解释了电极性能的变化。实验中,使用金电极 (GE) 和纳米多孔金电极 (NPGE) 进行了循环伏安法 (CV) 和差分脉冲伏安法 (DPV)。金电极在 H2SO4 中浸泡后进行表面处理,电位控制在约 +2.0 V,持续 40 秒。+2.0V,持续 40 秒,从而形成纳米多孔结构。经过优化后,采用吸附剥离伏安法(AdSV)测定 BAI。该方法的检出限(LOD)和定量限(LOQ)分别为 0.015 µmol L-1 和 0.045 µmol L-1(沉积电压=-0.25 V;沉积时间=50 秒)。此外,还将标准添加法应用于 NPGE,从添加的合成人血浆和尿液中回收 BAI,成功率在 93.4% 至 106% 之间。这种方法具有极佳的稳定性、精确性和准确性,受其他物质的干扰极小。此外,理论研究结果为纳米多孔金表面选择性电化学检测 BAI 提供了更深入的见解,为这一领域提供了新的视角。
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引用次数: 0
Exploring the impact of ionomer content and distribution on inkjet printed cathodes for anion exchange membrane fuel cells 探索离子聚合物含量和分布对阴离子交换膜燃料电池喷墨打印阴极的影响
IF 5.5 3区 材料科学 Q1 ELECTROCHEMISTRY Pub Date : 2024-11-03 DOI: 10.1016/j.electacta.2024.145293
Jiafei Liu, Marc Secanell
Electrode composition optimization is critical to achieving high and stable anion exchange membrane fuel cell (AEMFC) performance. In this article, inkjet printing is pioneered as a method to fabricate AEMFC electrodes with varying and graded cathode ionomer loading in order to assess its impact on electrode electrochemical properties, cell performance and stability. Inkjet printed catalyst layers (CLs) exhibited decreasing porosity with increasing ionomer content, maintaining a constant active area at 50 °C under fully humidified conditions. The increase in active area and ionic conductivity with increasing ionomer content was detectable only at higher temperatures. At 60 °C with 90% relative humidity inlet gases, the AEMFCs with cathode electrodes with optimal 20 wt% uniform ionomer content achieved a highly repeatable and stable performance of 0.53 W/cm2 with a total loading of 0.3 mgPt/cmCL2. Grading the cathode ionomer content, with higher concentration near the membrane and lower near the gas diffusion layer (GDL), does not improve cell performance, indicating neither cathode conductivity nor mass transport limits performance. When tested at 80 °C, AEMFCs with a graded cathode ionomer structure (30 wt% near the membrane and 20 wt% near the GDL) demonstrated improved stability compared to those with a uniform 20 wt% ionomer content. This stability improvement is attributed to better water retention with more cathode ionomer content, as evidenced by the cell’s ability to maintain low resistance.
电极成分的优化对于实现阴离子交换膜燃料电池(AEMFC)的高性能和稳定性至关重要。本文开创性地采用喷墨打印的方法来制造具有不同分级阴极离子膜负载的 AEMFC 电极,以评估其对电极电化学特性、电池性能和稳定性的影响。喷墨打印催化剂层(CL)的孔隙率随着离子聚合物含量的增加而降低,在完全加湿条件下,50 °C°C 的温度下保持活性面积不变。只有在较高温度下,才能检测到活性面积和离子导电率随离子聚合物含量增加而增加。在相对湿度为 90% 的入口气体条件下,温度为 60°C 时,阴极电极离子聚合物含量均为 20 wt%的 AEMFC 达到了 0.53 W/cm2W/cm2,总负载量为 0.3 mgPt/cmCL2mgPt/cmCL2,性能重复性高且稳定。对阴极离子聚合物含量进行分级,膜附近的浓度较高,而气体扩散层(GDL)附近的浓度较低,但这并不能提高电池的性能,这表明阴极导电性和质量传输都没有限制电池的性能。在 80 °C°C 下进行测试时,采用分级阴极离子膜结构(膜附近为 30 wt%,GDL 附近为 20 wt%)的 AEMFC 比离子膜含量均为 20 wt% 的 AEMFC 具有更高的稳定性。这种稳定性的提高归因于阴极离子膜含量越高,保水性越好,电池保持低电阻的能力也证明了这一点。
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引用次数: 0
Fabrication of high-efficiency perovskite solar cells using benzodithiophene-based random copolymeric hole transport material 使用苯并二噻吩基无规共聚物空穴传输材料制造高效率 Perovskite 太阳能电池
IF 5.5 3区 材料科学 Q1 ELECTROCHEMISTRY Pub Date : 2024-11-03 DOI: 10.1016/j.electacta.2024.145315
Vijay Srinivasan Murugesan , Michael Ruby Raj , Hock Beng Lee , Neetesh Kumar
The design of donor-acceptor (D-A)-based random copolymers-type hole transporting materials (HTMs) are important for achieving superior performance of perovskite solar cells (PSCs) with high durability. In this work, a 2-alkylthienyl-substituted benzodithiophene (BDTT)-based random copolymer (denoted as RCP-BDTTPD), containing 2-ethylhexylthiophene-substituted benzo[1,2-b:4,5-b′]dithiophene (BDTT as an electron-donor; M1) and two different side-chain functionalized thieno[3,4-c]-pyrrole-4,6‑dione as the electron-acceptors (M2 and M3), is prepared and applied as an efficient interfacial HTM for PSCs. The optical, electrochemical, and electronic properties of RCP-BDTTPD are shown to be structurally and energetically viable to serve as HTM for PSCs. The RCP-BDTTPD has deeper highest occupied molecular orbitals (HOMO; −5.53 eV) and lowest unoccupied molecular orbitals (LUMO; −3.57 eV) energy levels. This is shown to be energetically suitable for realizing better compatibility with Cs-containing formamidinium/methylammonium (FAMA) mixed-cation perovskite as light absorber having HOMO energy level (−5.85 eV). The RCP-BDTTPD possessing gradient band alignment with perovskite, which is shown to be highly significant for the extraction of charge carriers, resulting in higher hole mobility of PSCs. RCP-BDTTPD delivered a reasonably good Voc of 1.10 V and higher Jsc of 19.01 mAcm−2 and, champion power conversion efficiency (PCE) up to 15.30 % with hole mobility (1.34×10−3 cm2V−1s−1) and high durability (Encapsulated cell retention of its PCE about 98 % over 16 h under harsh environment: Temp. ∼85 °C, RH∼85 %). This work demonstrating a potential application of RCP-BDTTPD based HTMs for the fabrication of high-performance PSCs with high durability as well as low cost.
设计基于供体-受体的无规共聚物型空穴传输材料(HTMs)对于实现性能优越、耐用性高的过氧化物太阳能电池(PSCs)非常重要。在这项研究中,一种基于 2-烷基噻吩基取代苯并二噻吩(BDTT)的无规共聚物(称为 RCP-BDTTPD)含有 2-乙基己基噻吩基取代苯并[1,2-b:M1)和两种不同侧链官能化的噻吩并[3,4-c]吡咯-4,6-二酮(M2 和 M3)作为电子受体。RCP-BDTTPD 的光学、电化学和电子特性表明,它在结构上和能量上都可以用作 PSC 的 HTM。RCP-BDTTPD 具有较深的最高占位分子轨道(HOMO;-5.53 eV)和最低未占位分子轨道(LUMO;-3.57 eV)能级。这表明,RCP-BDTTPD 在能量上适合与具有 HOMO 能级(-5.85 eV)的含铯甲脒/甲铵(FAMA)混合阳离子包晶实现更好的兼容性。RCP-BDTTPD 与过氧化物具有梯度带排列,这对电荷载流子的萃取非常重要,从而提高了 PSC 的空穴迁移率。RCP-BDTTPD 的 Voc 值为 1.10 V,Jsc 值为 19.01 mAcm-2,功率转换效率(PCE)高达 15.30%,空穴迁移率为 1.34×10-3 cm2V-1s-1,并且具有很高的耐用性(封装电池在恶劣环境下 16 小时的 PCE 保持率约为 98%):温度∼85 °C,相对湿度∼85%)。这项研究表明,基于 RCP-BDTTPD 的 HTMs 有可能用于制造具有高耐用性和低成本的高性能 PSC。
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引用次数: 0
Selective electrooxidation of glucose towards gluconic acid on Ni@Au foam electrodes 镍@金泡沫电极上葡萄糖对葡萄糖酸的选择性电氧化作用
IF 5.5 3区 材料科学 Q1 ELECTROCHEMISTRY Pub Date : 2024-11-02 DOI: 10.1016/j.electacta.2024.145307
Erwann Ginoux , Thibault Rafaïdeen , Patrick Cognet , Laure Latapie , Christophe Coutanceau
Ni@Au electrodes are prepared by galvanic replacement of Ni atoms of a commercial Ni foam by Au atoms. The physicochemical characterizations indicate gold atomic ratios of ca. 6 %, independently on the galvanic replacement time (1, 2 and 3 min), but differences in the structure of the deposited gold layers. The shapes of the cyclic voltammograms recorded in a 0.1 M NaOH aqueous electrolyte indicate that both Au and Ni sites are accessible. In the presence of 0.1 M glucose, the same oxidation onset potential of ca. 0.3 V vs RHE and a comparable activity in terms of achieved geometric current densities were recorded for all the Ni@Au electrodes. The long term electrolyses of 0.1 M glucose in 0.1 M aqueous KOH electrolyte on the Ni@Au electrodes performed at cell voltages corresponding to anode potentials of 0.575 V, 0.675 V and 0.775 V vs RHE show a surprising excellent stability over 5 h, which is explained by the presence of a Ni(OH)2 layer on the surface of the Ni foam in contact with the deposited gold layers. Conversions up to 60 % are obtained after 5 h electrolyses with the Ni-Au electrode obtained after 3 min deposition, with 100 % selectivity and faradaic efficiency towards gluconic acid for all the electrodes and for the lower potential of 0.575 V vs RHE. Increasing the glucose and KOH initial concentrations decreases the conversion rate, selectivity and faradaic efficiency.
Ni@Au 电极是通过金原子电化学置换商用泡沫镍中的镍原子而制备的。理化特性表明,金原子比率约为 6%,与电化学置换时间(1、2 和 3 分钟)无关,但沉积金层的结构存在差异。在 0.1 M NaOH 水溶液电解液中记录的循环伏安图的形状表明,金和镍的位点都是可接触的。在 0.1 M 葡萄糖存在下,所有 Ni@Au 电极都记录到了相同的氧化起始电位(与 RHE 相比约为 0.3 V),在达到的几何电流密度方面也具有相似的活性。在 Ni@Au 电极上对 0.1 M KOH 电解液中的 0.1 M 葡萄糖进行长期电解,电解槽电压分别为 0.575 V、0.675 V 和 0.775 V(相对于 RHE),结果表明在 5 小时内具有令人惊讶的出色稳定性,这是因为在与沉积金层接触的镍泡沫表面存在镍(OH)2 层。在 3 分钟沉积后获得的镍金电极上进行 5 小时电解后,转化率高达 60%,所有电极和 0.575 V 对 RHE 的较低电位对葡萄糖酸的选择性和远红外效率均为 100%。增加葡萄糖和 KOH 的初始浓度会降低转化率、选择性和法拉第效率。
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引用次数: 0
Electrochemical carboxylation: Green synthesis of atrolactic acid using boron-doped diamond electrodes 电化学羧化:使用掺硼金刚石电极绿色合成阿曲酸
IF 5.5 3区 材料科学 Q1 ELECTROCHEMISTRY Pub Date : 2024-11-02 DOI: 10.1016/j.electacta.2024.145310
Yuvaraj M. Hunge , Toya Inaba , Keizo Ishihara , Kai Takagi , Ryoya Okamura , Hiroshi Uetsuka , Chiaki Terashima
Electrochemical CO2 fixation is vital for sustainability in the chemical industry, yet the selective synthesis of multi-carbon products remains challenging. Organic electrosynthesis offers promise by enabling precise control over reaction conditions and facilitating novel reactivity patterns. One such technique, electrochemical carboxylation, involves coupling CO2 with organic molecules to produce carboxylic acids. Specifically, electro-carboxylation of acetophenone yields atrolactic acid, a valuable precursor for nonsteroidal anti-inflammatory drugs, providing a greener alternative to traditional production methods. This study focuses on the synthesis and characterization of boron-doped diamond (BDD) films using the microwave plasma-assisted chemical vapor deposition (MP-CVD) method and synthesized BDD electrodes were then used for the electrolytic carboxylation of acetophenone. Various analytical techniques, including X-ray diffraction (XRD), Raman spectroscopy, and laser microscopy, etc. were employed to characterize the BDD films. Various BDD films synthesized for different durations were utilized in the electrolytic carboxylation of acetophenone, with the highest yield of atrolactic acid (25 %) achieved using a BDD film synthesized over 6 h. Also, the effect of BDD surface modification i.e. oxygen and hydrogen terminated BDD on the synthesis of atrolactic acid was studied. Additionally, different electrolytes were employed in the synthesis process of atrolactic acid. A comparative study between Pt and BDD electrodes for the electrolytic carboxylation of acetophenone was conducted, and a mechanism for the formation of atrolactic acid was proposed.
电化学二氧化碳固定法对化学工业的可持续发展至关重要,但选择性合成多碳产品仍具有挑战性。有机电合成技术能够精确控制反应条件,并促进新的反应模式,因此前景广阔。电化学羧化就是这样一种技术,它将二氧化碳与有机分子耦合,生成羧酸。具体来说,对苯乙酮进行电羧化反应可产生阿曲酸,这是一种非甾体抗炎药物的重要前体,为传统生产方法提供了一种更环保的替代方法。本研究的重点是利用微波等离子体辅助化学气相沉积(MP-CVD)方法合成掺硼金刚石(BDD)薄膜并对其进行表征,然后将合成的 BDD 电极用于苯乙酮的电解羧化。在对 BDD 薄膜进行表征时,采用了多种分析技术,包括 X 射线衍射 (XRD)、拉曼光谱和激光显微镜等。在电解羧化苯乙酮的过程中,使用了不同时间合成的 BDD 薄膜,其中使用 6 小时合成的 BDD 薄膜合成的阿曲酸产量最高(25%)。此外,还研究了 BDD 表面改性(即氧和氢终止 BDD)对阿特拉酸合成的影响。此外,在阿特乳酸的合成过程中还采用了不同的电解质。对铂电极和 BDD 电极用于苯乙酮的电解羧化进行了比较研究,并提出了阿特拉酸的形成机理。
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引用次数: 0
The role of cation exchange membrane characteristics in CO2 electrolysis to CO using acid anolyte 阳离子交换膜特性在使用酸性溶解液电解 CO2 到 CO 中的作用
IF 5.5 3区 材料科学 Q1 ELECTROCHEMISTRY Pub Date : 2024-11-02 DOI: 10.1016/j.electacta.2024.145308
Alan M.P. Sakita, Edson A. Ticianelli
Cation exchange membranes are considered a suitable option for zero-gap CO2 electrolysis due to their potential to avoid carbonation and improve carbon efficiency. However, the use of acidic anolytes remains an issue due to high hydrogen production. This study investigates Nafion® membranes (111, 112, 115, 211, and 212) with different thicknesses produced by extrusion or solution-cast processes in a zero-gap cell with an acidic anolyte containing K2SO4. Faradaic efficiencies for CO production (FECO) are higher with thinner membranes, regardless of the manufacturing process, reaching FECO around 75 % at 50 mA cm⁻². Additionally, membranes with similar thicknesses (∼50.8 µm) but produced in different ways displayed flow field carbonation after 3 h of electrolysis at 30 °C and 50 mA cm⁻². Linear sweep voltammetry (LSV) in full and half-cell configurations shows limiting diffusion current (iL) relative to proton transport for all the employed membranes, no matter the thickness. In contrast, the iL for Nafion® 115, the thicker membrane, is suppressed, indicating that proton depletion is fast and the electrode surface alkalinization primarily results from water reduction in this case. A mechanistic analysis was performed to explain the behavior of the limiting currents in the cell with Ar- and CO2-feed, indicating that CO2 reduction aids in the consumption of H+ provided by the membrane, increasing the local pH at less negative potentials. Overall, thinner membranes exhibited higher values of FECO and energy efficiency for CO (EE%CO). However, solution-cast membranes are more prone to provide K+, leading to better performance than those prepared by extrusion.
由于阳离子交换膜具有避免碳化和提高碳效率的潜力,因此被认为是零间隙二氧化碳电解的合适选择。然而,由于制氢量高,使用酸性溶液仍是一个问题。本研究调查了在含有 K2SO4 的酸性溶液的零间隙电池中,通过挤压或溶液浇铸工艺生产的不同厚度的 Nafion® 膜(111、112、115、211 和 212)。无论生产工艺如何,较薄的膜产生二氧化碳的法拉第效率(FECO)较高,在 50 mA cm-² 的条件下,FECO 达到 75% 左右。此外,在 30°C 和 50 mA cm-² 条件下电解 3 小时后,厚度相似(50.8 µm)但制造方法不同的膜会出现流场碳化现象。全电池和半电池配置下的线性扫描伏安法(LSV)显示,无论膜的厚度如何,所有采用的膜都具有相对于质子传输的极限扩散电流(iL)。相比之下,较厚的 Nafion® 115 膜的 iL 被抑制,这表明质子耗竭速度很快,在这种情况下,电极表面碱化主要是由水还原造成的。为解释氩气和二氧化碳馈入电池中的极限电流行为,进行了机理分析,结果表明二氧化碳还原有助于消耗膜提供的 H+,在负电位较低时提高局部 pH 值。总体而言,较薄的膜表现出较高的 FECO 值和 CO 能量效率(EE%CO)。然而,溶液浇铸膜更容易提供 K+,因此比挤压制备的膜性能更好。
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引用次数: 0
Signal amplification platform based on 2D MOF-on-MOF architectures-derived Co-decorated carbon@nitrogen-doped porous carbon for enhanced electrochemical acetaminophen sensing 基于二维 MOF-on-MOF 架构的信号放大平台,用于增强电化学对乙酰氨基酚传感的 Co-decorated carbon@nitrogen-doped 多孔碳
IF 5.5 3区 材料科学 Q1 ELECTROCHEMISTRY Pub Date : 2024-11-01 DOI: 10.1016/j.electacta.2024.145311
Xue Zhang , Xingpai Cai , Tingting Zhang , Zhuzhen Chen , Wangxing Cheng , Zhenbao Li , Linwei Chen , Nannan Lu
Two-dimensional (2D) carbon-carbon hybrids derived from metal-organic frameworks (MOFs) are regarded as an intriguing type of electrode material in electrochemical sensing. In this work, a Co-decorated carbon@nitrogen-doped porous carbon heterostructure (Co/C@NC) was prepared via the simple calcination of 2D ZIF-L(Co)@ZIF-8. In this MOF-on-MOF precursor, the outer ZIF-8 layer not only prevents the collapse of ZIF-L(Co) during calcination but also endows the outer carbon an extended surface area and porous structure for more accessible active sites and a fast mass transfer process. Meanwhile, the formed CoNPs could facilitate the generation of graphitic carbon layers, which enhances electrocatalytic activity and boosted conductivity. Owing to these merits, the Co/C@NC-based sensor displays high electrochemical activity for acetaminophen (APAP) detection with a wide linear range (4 × 10–7 - 2 × 10–4 M) and a lower detection limit (8.2 × 10–8 M). The constructed sensor has been utilized for the analysis of APAP in real samples, yielding acceptable recovery between 96.6% and 104.0%. This work presents an efficient and convenient method for designing MOF-on-MOF-derived 2D carbon-carbon hybrids, which hold a promising prospect in electrochemical analysis.
由金属有机框架(MOFs)衍生的二维(2D)碳-碳杂化物被认为是电化学传感中一种有趣的电极材料。在这项工作中,通过简单煅烧二维 ZIF-L(Co)@ZIF-8,制备了 Co 装饰碳@氮掺杂多孔碳异质结构(Co/C@NC)。在这种 MOF-on-MOF 前驱体中,外层 ZIF-8 不仅能防止 ZIF-L(Co)在煅烧过程中塌陷,还能赋予外层碳以更大的比表面积和多孔结构,以获得更多的活性位点和更快的传质过程。同时,形成的 CoNPs 可促进石墨碳层的生成,从而提高电催化活性和导电性。由于这些优点,基于 Co/C@NC 的传感器在对乙酰氨基酚(APAP)的检测中显示出较高的电化学活性,具有较宽的线性范围(4 × 10-7 - 2 × 10-4 M)和较低的检测限(8.2 × 10-8 M)。所构建的传感器已被用于分析实际样品中的对乙酰氨基酚,回收率在 96.6% 到 104.0% 之间。这项工作为设计由 MOF-on-MOF 衍生的二维碳碳杂化物提供了一种高效便捷的方法,在电化学分析领域具有广阔的前景。
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引用次数: 0
Corrosion properties and mechanisms of friction stir lap welded TiB2/2024 aluminum matrix composite joint 搅拌摩擦搭接焊接 TiB2/2024 铝基复合材料接头的腐蚀性能和机理
IF 5.5 3区 材料科学 Q1 ELECTROCHEMISTRY Pub Date : 2024-11-01 DOI: 10.1016/j.electacta.2024.145306
Shuai Chen , Pengliang Niu , Yongxian Huang , Yongbing Li , Xurong Fu , Liming Ke , Fencheng Liu , Fenggang Liu
The corrosion properties and mechanisms of friction stir lap welded (FSLWed) TiB2/2024 aluminum matrix composite joint immersed in 3.5 wt.% NaCl solution were deeply investigated. Electron backscatter diffraction (EBSD), transmission electron microscopy (TEM) and high resolution TEM (HRTEM) were conducted to characterize the microstructural evolution of various zones across the joint cross-section. The appearance and penetration depth of the etched surfaces were observed by scanning electron microscopy (SEM). The elements on the etched surface were analyzed by EPMA. Results show that the corrosion properties of the 600/200 (rotational speed 600 r/min, travelling speed 200 mm/min) joint are higher than those of the 400/200 joint. It is noted that the corrosion properties of the stir zone (SZ) are higher than those of base material (BM) and heat affected zone (HAZ) based on the open circuit potential (OCP), the corrosion current icorr, the impedance Rcorr and the corroded appearance after immersion corrosion regardless of the welding parameters.
深入研究了浸入 3.5 wt.% NaCl 溶液中的搅拌摩擦搭接焊(FSLWed)TiB2/2024 铝基复合材料接头的腐蚀特性和机理。通过电子反向散射衍射 (EBSD)、透射电子显微镜 (TEM) 和高分辨率 TEM (HRTEM) 分析了接头横截面上不同区域的微观结构演变特征。扫描电子显微镜(SEM)观察了蚀刻表面的外观和渗透深度。用 EPMA 分析了蚀刻表面上的元素。结果表明,600/200(转速 600 r/min,移动速度 200 mm/min)接头的腐蚀性能高于 400/200 接头。根据开路电位 (OCP)、腐蚀电流 icorr、阻抗 Rcorr 以及浸泡腐蚀后的腐蚀外观,可以看出无论焊接参数如何,搅拌区 (SZ) 的腐蚀性能都高于母材 (BM) 和热影响区 (HAZ)。
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引用次数: 0
Hierarchical Co3O4 anode for high-performance Na-ion battery 用于高性能钠离子电池的分层 Co3O4 阳极
IF 5.5 3区 材料科学 Q1 ELECTROCHEMISTRY Pub Date : 2024-11-01 DOI: 10.1016/j.electacta.2024.145309
Mewin Vincent , Sandra Sajeev , Monika Srivastava , Ewa Kowalska , Sugarthi Srinivasan , Damian Kowalski
Despite excellent theoretical perditions, sodium-ion batteries have not yet evolved as a reliable replacement of current lithium-ion technology, mostly due to a lack of high capacity-long cycling electrodes. Among the various candidates cobalt(II,III)oxide, Co3O4, is expected to deliver an excellent electrochemical characteristics, owing to its multi-electron conversion type nature, however, usually fails in terms of performance due to the electrode inconsistencies, associated with the poor conductivity and volumetric fluctuations. Herein, we report morphology and crystallinity engineering of the Co3O4 nanostructure to substantially improve the charge storage as well as cycling performance. Largely interconnected hierarchical Co3O4 synthesized via highly reproducible and industrially viable approach demonstrated efficient charge transport kinetics and excellent volume expansion buffering under the de/sodiation cycles. With its unique structural properties hierarchical electrode delivered an excellent reversible capacity (70 % of theoretical limit @25 mAg-1), rate performance (123 mAhg-1 @1Ag-1) and stable cycling (82 % after 250 cycles @1Ag-1). In-situ Raman analysis of the electrode reactions revealed conversion type Na-ion storage in the hierarchical type of electrodes.
尽管钠离子电池的理论熵值极高,但它尚未发展成为当前锂离子技术的可靠替代品,主要原因是缺乏高容量、长循环电极。在各种候选钴(II,III)氧化物(Co3O4)中,Co3O4 因其多电子转换类型的性质而有望提供出色的电化学特性,但由于电极导电性差和体积波动相关的不一致性,其性能通常不尽如人意。在此,我们报告了 Co3O4 纳米结构的形态和结晶度工程,以大幅提高电荷存储和循环性能。通过高度可重复性和工业可行性的方法合成的大面积相互连接的分层 Co3O4 在脱氧/钠化循环中表现出高效的电荷传输动力学和出色的体积膨胀缓冲能力。凭借其独特的结构特性,纳米片电极具有出色的可逆容量(理论极限的 70% @25 mAg-1)、速率性能(123 mAhg-1 @ 1Ag-1)和稳定的循环性能(250 次循环后的 82% @ 1Ag-1)。对电极反应的原位拉曼分析表明,在分层型电极中存在转化型钠离子存储。
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引用次数: 0
Facile fabrication of N-doped RGO decorated CoS2 nanoparticles as advanced integrated electrode for enhanced supercapacitor performance 轻松制备掺杂 N 的 RGO 装饰 CoS2 纳米粒子,作为先进的集成电极提高超级电容器性能
IF 5.5 3区 材料科学 Q1 ELECTROCHEMISTRY Pub Date : 2024-11-01 DOI: 10.1016/j.electacta.2024.145312
Xiaona Li , Weiyang Zhang , Zhengyan Gu , Qingbin Cai , Hongwei Kang , Baocheng Yang , Zhikun Li
Transition metal sulfides (TMSs) are a class of advanced electrode materials for new energy storage devices with superior performance due to their many advantages, such as high specific capacity, good conductivity, low electronegativity, high redox activity, rich variety and low price. Herein, we developed N-doped reduced graphene oxide (N-RGO) decorated CoS2 nanoparticles nanohybrids (N-RGO/CoS2, denoted as NGCS) by a facile hydrothermal method. The doped-N process enriches the specific surface area and porosity of RGO nanosheets, which not only forms rich network nanostructures conducive to rapid charge/ion transport, but also promotes more dispersed anchoring of CoS2, resulting in the formation of smaller-sized CoS2 nanoparticles that can provide rich and exposed electroactive sites. Therefore, such unique hierarchical porous nanostructures help all components in the nanohybrids to “complement each other's strengths”, so that the fabricated NGCS electrode exhibits a high specific capacitance of 797.1 F g−1 at 0.6 A g−1 and an excellent rate capability with 77.5 % retention (20 A g−1). Furthermore, the assembled NGCS//AC hybrid supercapacitor (HSC) delivers excellent energy density of 41.4 Wh kg−1 (at 719.7 W kg−1) and long-term cyclability with 86.02 % capacitance retention after 13,000 cycles, presenting a promising application potential in new high-performance energy storage and conversion devices.
过渡金属硫化物(TMSs)具有比容量高、导电性好、电负性低、氧化还原活性高、种类丰富、价格低廉等诸多优点,是一类性能优越的新型储能器件用先进电极材料。在此,我们采用简便的水热法开发了掺杂 N 的还原氧化石墨烯(N-RGO)装饰 CoS2 纳米颗粒纳米杂化物(N-RGO/CoS2,简称 NGCS)。掺杂-N过程丰富了RGO纳米片的比表面积和孔隙率,不仅形成了丰富的网络纳米结构,有利于电荷/离子的快速传输,而且促进了CoS2更分散的锚定,从而形成了更小尺寸的CoS2纳米颗粒,可提供丰富的暴露电活性位点。因此,这种独特的分层多孔纳米结构有助于纳米混合体中的所有成分 "优势互补",从而使制造出的 NGCS 电极在 0.6 A g-1 电流条件下具有 797.1 F g-1 的高比电容和 77.5% 的卓越速率保持能力(20 A g-1)。此外,组装后的 NGCS//AC 混合超级电容器(HSC)具有 41.4 Wh kg-1 的出色能量密度(719.7 W kg-1)和长期循环能力,13,000 次循环后电容保持率为 86.02%,在新型高性能能量存储和转换设备中具有广阔的应用前景。
{"title":"Facile fabrication of N-doped RGO decorated CoS2 nanoparticles as advanced integrated electrode for enhanced supercapacitor performance","authors":"Xiaona Li ,&nbsp;Weiyang Zhang ,&nbsp;Zhengyan Gu ,&nbsp;Qingbin Cai ,&nbsp;Hongwei Kang ,&nbsp;Baocheng Yang ,&nbsp;Zhikun Li","doi":"10.1016/j.electacta.2024.145312","DOIUrl":"10.1016/j.electacta.2024.145312","url":null,"abstract":"<div><div>Transition metal sulfides (TMSs) are a class of advanced electrode materials for new energy storage devices with superior performance due to their many advantages, such as high specific capacity, good conductivity, low electronegativity, high redox activity, rich variety and low price. Herein, we developed N-doped reduced graphene oxide (N-RGO) decorated CoS<sub>2</sub> nanoparticles nanohybrids (N-RGO/CoS<sub>2</sub>, denoted as NGCS) by a facile hydrothermal method. The doped-N process enriches the specific surface area and porosity of RGO nanosheets, which not only forms rich network nanostructures conducive to rapid charge/ion transport, but also promotes more dispersed anchoring of CoS<sub>2</sub>, resulting in the formation of smaller-sized CoS<sub>2</sub> nanoparticles that can provide rich and exposed electroactive sites. Therefore, such unique hierarchical porous nanostructures help all components in the nanohybrids to “complement each other's strengths”, so that the fabricated NGCS electrode exhibits a high specific capacitance of 797.1 F <em>g</em><sup>−1</sup> at 0.6 A <em>g</em><sup>−1</sup> and an excellent rate capability with 77.5 % retention (20 A <em>g</em><sup>−1</sup>). Furthermore, the assembled NGCS//AC hybrid supercapacitor (HSC) delivers excellent energy density of 41.4 Wh kg<sup>−1</sup> (at 719.7 W kg<sup>−1</sup>) and long-term cyclability with 86.02 % capacitance retention after 13,000 cycles, presenting a promising application potential in new high-performance energy storage and conversion devices.</div></div>","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"509 ","pages":"Article 145312"},"PeriodicalIF":5.5,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142562302","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}
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Electrochimica Acta
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