Electrochimica Acta最新文献_第6页

Repurposing discarded porphyrin waste as electrocatalysts for the oxygen reduction reaction 将废弃的卟啉废料重新用作氧还原反应的电催化剂

IF 5.5 3区材料科学 Q1 ELECTROCHEMISTRY

Electrochimica Acta

Pub Date : 2024-09-22 DOI: 10.1016/j.electacta.2024.145113

The oxygen reduction reaction (ORR), presently known as the key bottleneck in the mass-scale implementation of fuel cells (FCs), typically relies on the exploitation of scarce and expensive platinum group metals (PGMs). Meanwhile, as a substitute for PGMs, transition metal-nitrogen carbons (TM-N_x-C) are proving to be reliable electrocatalysts (ECs) in which atomically dispersed TMs coordinated with nitrogen are integrated into the carbon matrix. Such TM-N_x coordination already exists in metal-porphyrins making them suitable precursors for TM-N_x-C. Adler-Longo method is the standard recipe for meso‑tetraphenyl porphyrin realizes ca. 20 % yield whereas the residual polypyrromethenes, structurally resembling open porphyrin rings, are often wasted. Herein, the possibility of upcycling waste polypyrromethenes into efficient TM-N_x-C for ORR is demonstrated. A comprehensive structural and morphological characterization is provided, and the electrocatalytic activity towards ORR in an alkaline environment is discussed using Fe and Mn as TMs. The EC synthesized from pure porphyrin precursor at 600 °C (FeTPP_600) had the best performance recording 0.972 and 0.852 V vs RHE for E_onset and E_1/2. Mixing porphyrins with their synthetic waste (ratio of 1:4) and pyrolyzing it at 800 °C (FeTPP/Waste(1:4)_800) still exhibits appreciable kinetics with similar results (0.977 and 0.853 V vs RHE for E_onset and E_1/2).

氧还原反应（ORR）是目前燃料电池（FC）大规模应用的关键瓶颈，通常依赖于稀缺而昂贵的铂族金属（PGM）的利用。与此同时，作为铂族金属的替代品，过渡金属氮碳（TM-Nx-C）被证明是一种可靠的电催化剂（EC），其中原子分散的 TM 与氮配位集成在碳基体中。这种 TM-Nx 配位已经存在于金属卟啉中，使它们成为 TM-Nx-C 的合适前体。Adler-Longo 方法是生产中四苯基卟啉的标准配方，产率约为 20%，而残留的多吡咯烷酮（结构上类似于开放的卟啉环）通常会被浪费掉。在此，我们证明了将废弃的多吡咯烷酮升级循环为用于 ORR 的高效 TM-Nx-C 的可能性。本文提供了全面的结构和形态特征，并讨论了以铁和锰为 TMs 在碱性环境中对 ORR 的电催化活性。由纯卟啉前体在 600 °C 下合成的 EC（FeTPP_600）具有最佳性能，其 Eonset 和 E1/2 对 RHE 的记录分别为 0.972 V 和 0.852 V。将卟啉与其合成废料（比例为 1:4）混合并在 800 ℃ 高温下热解（FeTPP/Waste(1:4)_800），仍然可以显示出类似的动力学结果（Eonset 和 E1/2 对 RHE 的比值分别为 0.977 和 0.853 V）。

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引用次数: 0

Grain boundary defect passivation and iodine migration inhibition for efficient and stable perovskite solar cells 晶界缺陷钝化和碘迁移抑制，实现高效稳定的过氧化物太阳能电池

IF 5.5 3区材料科学 Q1 ELECTROCHEMISTRY

Electrochimica Acta

Pub Date : 2024-09-22 DOI: 10.1016/j.electacta.2024.145129

To inhibit the I⁻migration and passivate the uncoordinated Pb²⁺ on perovskite grain boundary (GB), 3-methyl-(1,1′-biphenyl)-4,4′-diformaldehyde (BPDA-Me) and 3-chlorine-(1,1′-biphenyl)-4,4′-diformaldehyde (BPDA-Cl) were synthesized and incorporated into perovskite films, respectively. The C = O groups in both additives can strongly interact with the uncoordinated Pb²⁺, allowing them to be anchored in perovskite GB. At the same time, the benzene ring skeleton in these two molecular structures can interact with the migrating I⁻ in GB. The Cl atom in the BPDA-Cl molecule delocalize electrons into the C = O group due to the conjugation effect of the benzene ring, so that the C = O group can provide stronger electronegativity, thus enhancing the interaction with the uncoordinated Pb²⁺. Meanwhile, Cl atom can coordinate with Pb²⁺ to synergically passivate the I vacancy defect on GB and enhance the lattice strength of PbI₆. This cooperative passivation further effectively inhibited the I⁻migration occurring at the perovskite GB. The functional group electron density regulation and cooperative passivation of Cl and C = O in BPDA-Cl make the passivation effect better than BPDA-Me. Consequently, the BPDA-Cl based perovskite solar cell achieved the highest power conversion efficiency of 24.96 % and stability with 92.1 % of the initial performance retained after 500 h of operation under continuous lighting and maximum power point tracking conditions.

为了抑制I迁移并钝化包晶晶界（GB）上未配位的Pb2+，合成了3-甲基-（1,1′-联苯）-4,4′-二甲醛（BPDA-Me）和3-氯-（1,1′-联苯）-4,4′-二甲醛（BPDA-Cl），并分别将其加入到包晶薄膜中。这两种添加剂中的 C = O 基团都能与未配位的 Pb2+ 发生强烈的相互作用，使它们能够锚定在包晶 GB 中。同时，这两种分子结构中的苯环骨架还能与 GB 中迁移的 I- 相互作用。由于苯环的共轭效应，BPDA-Cl 分子中的 Cl 原子会将电子析出到 C = O 基团中，这样 C = O 基团就能提供更强的电负性，从而增强与未配位 Pb2+ 的相互作用。同时，Cl 原子能与 Pb2+ 配位，协同钝化 GB 上的 I 空位缺陷，增强 PbI6 的晶格强度。这种协同钝化作用进一步有效地抑制了包晶 GB 上发生的 I 迁移。BPDA-Cl 中的官能团电子密度调节和 Cl 与 C = O 的协同钝化使其钝化效果优于 BPDA-Me。因此，在连续照明和最大功率点跟踪条件下，基于 BPDA-Cl 的过氧化物太阳能电池实现了最高的功率转换效率（24.96%）和稳定性，在运行 500 小时后，其初始性能仍能保持 92.1%。

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引用次数: 0

A composite electrocatalytic poly(3,4-ethylenedioxythiophene) film incorporated with silver nanowires for bifacial dye-sensitized solar cells 用于双面染料敏化太阳能电池的含银纳米线的复合电催化聚（3,4-亚乙二氧基噻吩）薄膜

IF 5.5 3区材料科学 Q1 ELECTROCHEMISTRY

Electrochimica Acta

Pub Date : 2024-09-22 DOI: 10.1016/j.electacta.2024.145132

Poly(3,4-ethylenedioxythiophene) (PEDOT) is a superior electrocatalyst for dye-sensitized solar cells (DSSCs). The porous PEDOT film, however, lacks directional conduction paths, resulting in slower electron transfer and lower cell efficiency. In this study, silver nanowires (Ag NWs) are incorporated into a PEDOT film to construct a PEDOT-coated Ag NW composite film, wherein the Ag NWs serve as highways for charge transport. The composite film is constructed by spreading Ag NWs on tin-doped indium oxide (ITO) glass via a three-step process (dip coating, brush painting, and thermal compression), followed by coating a PEDOT film via electropolymerization. The DSSC catalyzed by the PEDOT-coated Ag NW exhibited an efficiency of 9.22 % under one-sun illumination, outperforming platinum (9.09 % efficiency) and PEDOT (8.33 % efficiency) by increasing the short-circuit current density. Chemical state analyses were performed to determine the interactions between the Ag NWs and PEDOT. Impedance measurements and quantum chemical calculations were conducted to rationalize the functionality of the PEDOT-coated Ag NWs. Owing to its high transparency, the resulting DSSC achieves an efficiency of 6.74 % under rear illumination, demonstrating its high feasibility as a bifacial DSSC. The DSSC also exhibited high efficiencies ranging from 14.05 % to 19.69 % under front-side illumination at low intensities of 300–1000 lux.

聚（3,4-亚乙二氧基噻吩）（PEDOT）是染料敏化太阳能电池（DSSC）的优质电催化剂。然而，多孔 PEDOT 薄膜缺乏定向传导路径，导致电子传输速度较慢，电池效率较低。在本研究中，银纳米线（Ag NWs）被加入到 PEDOT 薄膜中，从而构建出一种 PEDOT 涂层 Ag NW 复合薄膜，其中的 Ag NWs 可作为电荷传输的高速公路。这种复合薄膜是通过三步法（浸涂、刷涂和热压）在掺锡氧化铟（ITO）玻璃上铺展银纳米粒子，然后通过电聚合涂覆 PEDOT 薄膜而制成的。通过提高短路电流密度，由 PEDOT 涂层 Ag NW 催化的 DSSC 在一太阳光照下的效率达到了 9.22%，优于铂（效率 9.09%）和 PEDOT（效率 8.33%）。为确定 Ag NWs 和 PEDOT 之间的相互作用，进行了化学状态分析。此外，还进行了阻抗测量和量子化学计算，以合理解释 PEDOT 涂层 Ag NWs 的功能。由于其透明度高，所产生的 DSSC 在背光照明下的效率达到了 6.74%，证明了其作为双面 DSSC 的高度可行性。在 300-1000 勒克斯的低强度正面照明下，该 DSSC 还表现出 14.05% 至 19.69% 的高效率。

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引用次数: 0

Synergistic Schottky contacts & diatomic doping in Cr/P-MoS2@Ti3C2Tx with boosted energy storage performance Cr/P-MoS2@Ti3C2Tx中的肖特基接触与硅原子掺杂协同作用可提高储能性能

IF 5.5 3区材料科学 Q1 ELECTROCHEMISTRY

Electrochimica Acta

Pub Date : 2024-09-22 DOI: 10.1016/j.electacta.2024.145128

Molybdenum disulfide (MoS₂), despite its promising attributes, suffers from low conductivity and aggregation. Herein, we introduce a novel approach that integrates Schottky contacts with Cr/P diatomic doping in MoS₂@Ti₃C₂T_x, significantly enhancing its performance. The Schottky contacts effectively suppress aggregation and accelerate interfacial charge transfer, while Cr/P doping boosts conductivity, active sites, and stability. As a result, the Cr/P-MoS₂@Ti₃C₂T_x electrode exhibits a specific capacitance of 650 F g^-1 at 1 A g^-1, which is fourfold higher than that of pristine MoS₂. When assembled into an asymmetric supercapacitor (Cr/P-MoS₂@Ti₃C₂T_x//AC ASC), the device achieves a peak energy density of 32 Wh kg^-1 at 303 W kg^-1, maintaining 85% capacitance retention after 10,000 cycles with an impressive coulombic efficiency of 97%. Furthermore, the density functional theory (DFT) calculations validate the beneficial effects of Schottky contacts and diatomic doping on the improved energy storage performance of Cr/P-MoS₂@Ti₃C₂T_x. This work demonstrates the promising potential of the material for applications in high-performance supercapacitors (SCs).

二硫化钼（MoS2）尽管具有良好的特性，但却存在导电率低和聚集的问题。在本文中，我们介绍了一种新方法，即在 MoS2@Ti3C2Tx 中整合肖特基接触和 Cr/P 双原子掺杂，从而显著提高其性能。肖特基接触有效抑制了聚集并加速了界面电荷转移，而 Cr/P 掺杂则提高了导电性、活性位点和稳定性。因此，Cr/P-MoS2@Ti3C2Tx 电极在 1 A g-1 时的比电容为 650 F g-1，是原始 MoS2 的四倍。当组装成不对称超级电容器（Cr/P-MoS2@Ti3C2Tx//AC ASC）时，该器件在 303 W kg-1 的条件下实现了 32 Wh kg-1 的峰值能量密度，在 10,000 次循环后仍能保持 85% 的电容保持率，库仑效率高达 97%。此外，密度泛函理论（DFT）计算验证了肖特基接触和二原子掺杂对提高 Cr/P-MoS2@Ti3C2Tx 储能性能的有利影响。这项工作证明了该材料在高性能超级电容器（SC）中的应用潜力。

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引用次数: 0

Metal to metal electron transfer in {111} faceted rice-grain like nanoparticles of Mn-wolframite for oxygen reduction reaction 用于氧还原反应的锰钨矿{111}面米粒状纳米粒子中的金属对金属电子转移

IF 5.5 3区材料科学 Q1 ELECTROCHEMISTRY

Electrochimica Acta

Pub Date : 2024-09-22 DOI: 10.1016/j.electacta.2024.145125

Commercial interest in Pt and Pt-based catalysts is hindered by their high cost. Herein, we have synthesized {111} faceted rice-grain like nanoparticles of p-MnWO₄ with wolframite structure by a polyol method, and applied as catalysts for the ORR in alkaline electrolyte. It enabled a transfer of electron from t_2g orbital of Mn 3d to the empty antibonding orbital of W 5d, producing plentiful Mn³⁺ states towards ORR. Moreover, it showed superior ORR activity to CoWO₄ and FeWO₄ prepared similarly, and to a h-MnWO₄ prepared by a hydrothermal procedure. p-MnWO₄ exhibited lowest negative onset potential (0.92 V vs RHE) and smallest Tafel slope (50 mV dec^‑1). Moreover, it achieved highest redox reaction mediated current density (-4.2 mA cm^-2), attributable to Mn³⁺ to Mn²⁺ reduction and promising stability (96.6 %) over 6 h Excellent performance of p-MnWO₄ is associated with optimal O₂ adsorption energies caused by metal to metal charge transfer and {111} faceted rice-grain like p-MnWO₄ nanoparticles.

铂和铂基催化剂的高成本阻碍了其商业应用。在此，我们采用多元醇法合成了具有黑钨矿结构的{111}面米粒状 p-MnWO4 纳米颗粒，并将其用作碱性电解液中 ORR 的催化剂。它使电子从 Mn 3d 的 t2g 轨道转移到 W 5d 的空反键轨道，从而产生大量的 Mn3+ 态，实现 ORR。p-MnWO4 的负起始电位（0.92 V vs RHE）最低，塔菲尔斜率（50 mV dec-1）最小。此外，p-MnWO4 的氧化还原反应介导电流密度（-4.2 mA cm-2）最高，这归功于 Mn3+ 对 Mn2+ 的还原作用以及 6 小时的稳定性（96.6 %）。 p-MnWO4 的优异性能与金属对金属电荷转移产生的最佳氧气吸附能以及类似 p-MnWO4 纳米颗粒的{111}面米粒有关。

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引用次数: 0

Solvothermal synthesis and enhanced electrochromic properties of coal-based reduced graphene oxide and covalent organic framework electrochromic composite films containing triphenylamine unit 含有三苯胺单元的煤基还原氧化石墨烯和共价有机框架电致变色复合薄膜的溶热合成及其增强的电致变色性能

IF 5.5 3区材料科学 Q1 ELECTROCHEMISTRY

Electrochimica Acta

Pub Date : 2024-09-22 DOI: 10.1016/j.electacta.2024.145112

Two-dimension covalent frameworks (2D COFs) with reversible redox units show the potential in the field of photo-electronic functional materials because of their rich electron transport path and reversible redox characteristic. However, the pure organic conjugated system of COF results in poor electrical conductivity and weak cyclic performance. In this work, tris (4-aminophenyl) amine and 4,4-biphenyldiformaldehyde (TABP) COF electrochromic film with triphenylamine (TPA) active unit was synthesized by a solvothermal method in Teflon-lined reactor. And then the TABP-COF/coal-based reduced graphene oxide (C-rGO) film was prepared by the one pot method. C-rGO provides the growth substrate and electron transport path for COF. Taixi anthracite with a high degree of graphitization also contributes to the preparation of GO. The electrochemical and electrochromic properties of TABP-COF and TABP-COF/C-rGO were studied and they could be switched reversibly from yellow and brown. Relative to TABP-COF, the impedance and response time of composite decrease and the contrast of composite increases. Moreover, TABP-COF/C-rGO exhibits the excellent stability, which can remain 80.1 % initial contrast after 5000 s cycle.

具有可逆氧化还原单元的二维共价框架（2D COFs）因其丰富的电子传输路径和可逆氧化还原特性，在光电功能材料领域展现出巨大潜力。然而，纯有机共轭体系的 COF 导电性差，循环性能弱。本研究在特氟隆衬里反应器中采用溶热法合成了带有三苯胺（TPA）活性单元的三（4-氨基苯基）胺和 4,4-联苯二甲醛（TABP）COF 电致发光薄膜。然后采用一锅法制备了 TABP-COF/ 煤基还原氧化石墨烯（C-rGO）薄膜。C-rGO 为 COF 提供了生长基底和电子传输路径。石墨化程度较高的太西无烟煤也有助于制备 GO。对 TABP-COF 和 TABP-COF/C-rGO 的电化学和电致变色特性进行了研究，结果表明它们可以在黄色和棕色之间进行可逆切换。与 TABP-COF 相比，复合材料的阻抗和响应时间降低，对比度增加。此外，TABP-COF/C-rGO 还具有出色的稳定性，在 5000 秒周期后仍能保持 80.1 % 的初始对比度。

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引用次数: 0

Electrodeposited CoMnS/NiCo2S4 nanocomposite for high performance supercapacitors 用于高性能超级电容器的电沉积 CoMnS/NiCo2S4 纳米复合材料

IF 5.5 3区材料科学 Q1 ELECTROCHEMISTRY

Electrochimica Acta

Pub Date : 2024-09-22 DOI: 10.1016/j.electacta.2024.145133

In this work, we report a facile two-step electrodeposition method to fabricate a CoMnS/NiCo₂S₄/NF (CMS/NCS/NF) composite on nickel foam (NF) for application of supercapacitor electrode. The electrochemical performance of this composite material has been extensively investigated, revealing superior performance compared to individual CMS/NF and NCS/NF materials. The CMS/NCS/NF composite exhibits an exceptionally high specific capacity of 707 C/g at a current density of 1 A/g in a three-electrode system. Remarkably, the material retains 92 % of its specific capacitance after 5000 cycles, indicating excellent cyclic stability and durability. To further explore its practical applications, we constructed a two-electrode symmetric supercapacitor using the CMS/NCS/NF electrode. This symmetric cell demonstrates an outstanding energy density of 97.5 Wh/kg and a peak power density of 12 kW/kg, underscoring its potential for high-performance energy storage applications. These comprehensive studies indicate that the synthesized CMS/NCS/NF is a highly promising candidate for supercapacitor electrodes, offering both high capacity and long-term stability. This work paves the way for the development of efficient and durable energy storage devices.

在这项工作中，我们报告了一种在泡沫镍（NF）上制造 CoMnS/NiCo2S4/NF （CMS/NCS/NF）复合材料的简便两步电沉积方法，该复合材料可用于超级电容器电极。对这种复合材料的电化学性能进行了广泛的研究，结果表明，与单独的 CMS/NF 和 NCS/NF 材料相比，这种复合材料的性能更加优越。在三电极系统中，电流密度为 1 A/g 时，CMS/NCS/NF 复合材料的比容量高达 707 C/g。值得注意的是，该材料在循环使用 5000 次后仍能保持 92% 的比电容，这表明它具有出色的循环稳定性和耐用性。为了进一步探索其实际应用，我们使用 CMS/NCS/NF 电极构建了一个双电极对称超级电容器。这种对称电池的能量密度高达 97.5 Wh/kg，峰值功率密度为 12 kW/kg，显示了其在高性能储能应用方面的潜力。这些综合研究表明，合成的 CMS/NCS/NF 是一种非常有前途的超级电容器电极候选材料，具有高容量和长期稳定性。这项工作为开发高效耐用的储能设备铺平了道路。

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引用次数: 0

Hierarchical MnCo2O4@MnWO4 core-shell nanoarrays on Ni foam as binder-free electrode for asymmetric supercapacitors 泡沫镍上的分层 MnCo2O4@MnWO4 核壳纳米阵列作为不对称超级电容器的无粘结剂电极

IF 5.5 3区材料科学 Q1 ELECTROCHEMISTRY

Electrochimica Acta

Pub Date : 2024-09-22 DOI: 10.1016/j.electacta.2024.145135

Supercapacitors (SCs) are generally perceived as competitive possibilities for portable electronic products due to their exceptionally high power density and extended operational lifespan. Nevertheless, the relatively low energy density remains a crucial obstacle to its widespread application. A hierarchical MnCo₂O₄@MnWO₄ core-shell nanoarrays on nickel foam (NF) was designed and synthesized by utilizing the MnCo₂O₄ nanosheet array as the backbone and the MnWO₄ nanosheet array as the shell via hydrothermal procedure and calcination. The MnCo₂O₄@MnWO₄/NF electrode achieves 1428.5 F g⁻¹ at 1 A g⁻¹ with 97.8 % of its pristine capacity after 4000 cycles. The superior energy storage characteristic is a result of several factors, including the binder-free integrated electrode design, the synergistic effect between MnCo₂O₄ and MnWO₄, and abundant active sites. The assembled asymmetric supercapacitor (ASC) has an energy density of 36.46 Wh kg⁻¹ at 750 W kg⁻¹, and 85.4 % capacity reserved after 5000 cycles.

超级电容器（SC）因其超高的功率密度和超长的工作寿命，被普遍认为是便携式电子产品中极具竞争力的产品。然而，相对较低的能量密度仍然是其广泛应用的关键障碍。通过水热法和煅烧法，以 MnCo2O4 纳米片阵列为骨架，MnWO4 纳米片阵列为外壳，设计并合成了泡沫镍（NF）上的分层 MnCo2O4@MnWO4 核壳纳米阵列。MnCo2O4@MnWO4/NF 电极在 1 A g-1 电流条件下可达到 1428.5 F g-1，4000 次循环后可达到原始容量的 97.8%。卓越的储能特性是多种因素共同作用的结果，包括无粘结剂的集成电极设计、MnCo2O4 和 MnWO4 之间的协同效应以及丰富的活性位点。组装好的非对称超级电容器（ASC）在 750 W kg-1 的条件下能量密度为 36.46 Wh kg-1，循环 5000 次后容量保留率为 85.4%。

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引用次数: 0

Enhancement of charge storage capacity in two-leg pseudo-spin ladder CaCu2O3 compound through Li-doping 通过掺杂锂提高两脚伪自旋阶梯 CaCu2O3 化合物的电荷存储容量

IF 5.5 3区材料科学 Q1 ELECTROCHEMISTRY

Electrochimica Acta

Pub Date : 2024-09-22 DOI: 10.1016/j.electacta.2024.145119

Nanostructured 2-leg pseudo spin-ladder compound CaCu₂O₃ has been synthesized by chemical co-precipitation method and a significant improvement in its charge storage capacity has been realized through Li-doping. The fabricated electrode based on Li-doped CaCu₂O₃ exhibited higher specific capacitance of 321.26 F/g at 1.5 A g^-1 when compared to that of 205.45 F/g for undoped CaCu₂O₃ system. Moreover, the electrode revealed an excellent cyclic stability (5000 cycles) with capacitance retention of 91.96 % of its initial value. An asymmetric supercapacitor fabricated using nano-flakes shaped Li-CaCu₂O₃ and activated carbon showed a notable energy density of 36.72 Wh/kg and power density of 1406 W/kg which maintains the energy density of 7.81 Wh/kg even at higher power density of 7031.25 W/kg. Among various Li-doped samples, 2.5 wt.% Li-CaCu₂O₃ exhibited the best storage capacity. This improvement has been attributed to the intrinsic off-stoichiometric (Ca_0.86Cu_2.14O_2.93) and spin ladder structure of CaCu₂O₃ which allows Li to intercalate and improve the storage performance. Moreover, higher reactive surface area due to nano-flake morphology and porous structure of Li-CaCu₂O₃ may enhance the permeability of electrolytic ions, thereby improving the performance of the fabricated supercapacitor compared to undoped CaCu₂O₃ with rod-like morphology. These findings underscore the potential of Li-CaCu₂O₃ as a promising candidate material for fabricating supercapacitor devices.

通过化学共沉淀法合成了纳米结构的 2 脚伪自旋梯化合物 CaCu2O3，并通过掺杂锂实现了电荷存储容量的显著提高。与未掺杂 CaCu2O3 体系的 205.45 F/g 相比，基于掺杂锂的 CaCu2O3 制成的电极在 1.5 A g-1 时的比电容高达 321.26 F/g。此外，该电极还具有出色的循环稳定性（5000 次循环），电容保持率为初始值的 91.96%。使用纳米片状锂-CaCu2O3 和活性炭制造的不对称超级电容器显示出显著的能量密度（36.72 Wh/kg）和功率密度（1406 W/kg），即使在更高的功率密度（7031.25 W/kg）下也能保持 7.81 Wh/kg 的能量密度。在各种掺锂样品中，2.5 wt.% Li-CaCu2O3 的存储容量最佳。这种改善归因于 CaCu2O3 固有的非化学计量（Ca0.86Cu2.14O2.93）和自旋梯结构，这种结构允许锂插层并提高了存储性能。此外，与棒状形态的未掺杂 CaCu2O3 相比，Li-CaCu2O3 的纳米片状形态和多孔结构带来的更高反应表面积可提高电解离子的渗透性，从而改善所制造的超级电容器的性能。这些发现凸显了锂钙铜氧化物作为制造超级电容器器件的候选材料的潜力。

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引用次数: 0

Construction of electrospun multistage ZnO@PMIA gel electrolytes for realizing high performance zinc-ion batteries 构建电纺多级 ZnO@PMIA 凝胶电解质以实现高性能锌离子电池

IF 5.5 3区材料科学 Q1 ELECTROCHEMISTRY

Electrochimica Acta

Pub Date : 2024-09-22 DOI: 10.1016/j.electacta.2024.145124

As an important component of ZIBs, flexible gel electrolytes offer the advantages of solid/liquid electrolytes and good interfacial bonding. However, limited by poor ionic conductivity and mechanical properties, traditional gel electrolytes are still unable to meet realistic applications. To solve the above problems, in this paper, poly(m-phenylene isophthalamide) (PMIA) nanofiber membranes were prepared by electrospinning, and then ordered zinc oxide (ZnO) nanorods were grown on their surfaces by hydrothermal method, and ZnO@PMIA nanofiber membranes were combined with poly(vinyl alcohol) (PVA) gel to obtain ZnO@PMIA-PVA (ZPP) composite electrolytes. On the one hand, thanks to the advantages of large specific surface area and good electrical conductivity of PMIA nanofibers and ZnO nanorods, they can provide continuous and uniform transmission channels for Zn²⁺ .On the other hand, ZPP combines the nanofiber layer with the gel layer, which possesses excellent mechanical properties and produces a well-bonded interface with the electrode, which can effectively reduce the internal resistance and resist the penetration of the dendrimer into the electrolyte during long cycling. The results show that the ZPP composite electrolyte has a high ionic conductivity (18.3 mS·cm^-1) and exhibits obvious advantages in inhibiting hydrogen precipitation and oxidative decomposition of Zn anode, and the Zn/ZPP/Zn symmetric battery can be recycled for >1000 h at 3 mA·cm^-2, and the full battery Zn/ZPP/MnO₂ can still maintain 159.3 mAh·g^-1 residual capacity after 1000 cycles with stable long-cycle performance and high coulombic efficiency (CE) (99 %). This flexible composite electrolyte has high safety, mechanical and electrochemical properties, which can realize high-performance ZIBs, and is expected to provide a new strategy for next-generation wearable energy storage devices.

作为 ZIB 的重要组成部分，柔性凝胶电解质具有固/液电解质和良好界面结合的优点。然而，受限于较差的离子导电性和机械性能，传统的凝胶电解质仍无法满足实际应用的需要。为解决上述问题，本文采用电纺丝法制备了聚间苯二胺（PMIA）纳米纤维膜，然后采用水热法在其表面生长出有序的氧化锌（ZnO）纳米棒，并将ZnO@PMIA纳米纤维膜与聚乙烯醇（PVA）凝胶结合，得到了ZnO@PMIA-PVA（ZPP）复合电解质。一方面，由于 PMIA 纳米纤维和 ZnO 纳米棒具有比表面积大、导电性好等优点，可以为 Zn2+ 提供连续均匀的传输通道；另一方面，ZPP 将纳米纤维层与凝胶层结合在一起，具有优异的机械性能，并与电极产生良好的结合界面，可以有效降低内阻，并在长时间循环过程中防止树枝状聚合物渗透到电解液中。结果表明，ZPP 复合电解液具有较高的离子电导率（18.3 mS-cm-1），在抑制氢析出和锌阳极氧化分解方面具有明显优势，Zn/ZPP/锌对称电池在 3 mA-cm-2 下可循环使用 >1000 h，全电池 Zn/ZPP/MnO2 在循环 1000 次后仍能保持 159.3 mAh-g-1 的剩余容量，具有稳定的长循环性能和较高的库仑效率（CE）（99 %）。这种柔性复合电解质具有很高的安全性、机械性能和电化学性能，可以实现高性能的 ZIB，有望为下一代可穿戴储能设备提供新的策略。

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引用次数: 0