Journal of Electroanalytical Chemistry最新文献_第9页

Alkali-induced zinc vacancies boost charge transfer in porous ZnCo2O4 Nanoflakes for ultrahigh-energy supercapacitors 碱诱导的锌空位促进了用于超高能超级电容器的多孔ZnCo2O4纳米片中的电荷转移

IF 4.1 3区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Electroanalytical Chemistry

Pub Date : 2025-12-27 DOI: 10.1016/j.jelechem.2025.119771

YaQi Wang, XiaoQian Wang, XiongZhi Li, WangTing Luo, Chao Yu, FanBin Meng, YuJie Zhang

Supercapacitors with high energy and power densities are crucial for next-generation energy storage. Herein, we report a strategy that simultaneously engineers nanoarchitecture and electronic structure to overcome the intrinsic limitations of spinel ZnCo₂O₄. Porous lamellar ZnCo₂O₄ nanoflakes were synthesized on nickel foam via hydrothermal growth and calcination, followed by controlled alkali etching. This process not only constructs permeable networks but also induces zinc vacancies. First-principles calculations reveal that these intentionally introduced Zn vacancies effectively modulate electronic interactions by lowering charge transfer barriers, thereby accelerating electrochemical reaction kinetics. The optimized electrode delivers a high specific capacity of 1653.1 F g⁻¹ at 1 A g⁻¹ and maintains 94.4 % capacity retention from 0.5 to 5 A g⁻¹, showcasing superior rate capability. It also exhibits excellent cycling stability with 93.3 % capacity retention over 5000 cycles. Furthermore, an assembled ZnCo₂O₄//AC hybrid supercapacitor achieves an energy density of 63.8 Wh kg⁻¹ at a power density of 850 W kg⁻¹. Remarkably, it retains 46.5 Wh kg⁻¹ (73 % retention) at an ultrahigh power density of 4249.6 W kg⁻¹, outperforming many reported ZnCo-based devices. This work highlights the synergy of morphological and defect engineering in designing advanced electrode materials.

具有高能量和功率密度的超级电容器对下一代储能至关重要。在此，我们报告了一种同时设计纳米结构和电子结构的策略，以克服尖晶石ZnCo2O4的固有局限性。通过水热生长和煅烧，在泡沫镍表面合成了多孔片状ZnCo2O4纳米片，并进行了控制碱腐蚀。这一过程不仅构建了可渗透网络，而且引起了锌空位。第一性原理计算表明，这些有意引入的Zn空位通过降低电荷转移势垒有效地调节电子相互作用，从而加速电化学反应动力学。优化后的电极在1 a g−1时具有1653.1 F g−1的高比容量，在0.5 ~ 5 a g−1范围内保持94.4%的容量保持率，显示出优越的倍率能力。它还表现出优异的循环稳定性，在5000次循环中保持93.3%的容量。此外，组装的ZnCo2O4//AC混合超级电容器在850 W kg - 1的功率密度下获得了63.8 Wh kg - 1的能量密度。值得注意的是，它在4249.6 W kg−1的超高功率密度下保持了46.5 Wh kg−1（73%的保留率），优于许多报道的znco基器件。这项工作突出了形态学和缺陷工程在设计先进电极材料中的协同作用。

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引用次数: 0

Dual crystal fields synergistic catalytic oxygen reduction reaction regulated via Ba doping in Sm1-xBaxMn2O5 Ba掺杂调控Sm1-xBaxMn2O5双晶场协同催化氧还原反应

IF 4.1 3区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Electroanalytical Chemistry

Pub Date : 2025-12-27 DOI: 10.1016/j.jelechem.2025.119772

Tai-Shen Yang , Jie Wu , Jing Chi , Jin-Chao Cao

To enhance the synergistic catalytic effect of pyramid Mn³⁺ and octahedral Mn⁴⁺ dual crystal fields in SmMn₂O₅ and improve its oxygen reduction reaction (ORR) performance, Ba-doped Sm_1-xBa_xMn₂O₅ (x = 0.1–0.5) catalysts were prepared by hydrothermal method. The substitution of partial Sm³⁺ in SmMn₂O₅ by Ba²⁺ leads to the increase in the ratios of Mn⁴⁺/Mn³⁺ and surface adsorbed oxygen/lattice oxygen on the surfaces of Sm_1-xBa_xMn₂O₅. The increase in surface adsorbed oxygen content indicates stronger oxygen adsorption capacity, while the increase in Mn⁴⁺ content facilitates synergistic catalysis of the dual crystal fields. Pyramid Mn³⁺ acts as the active site to catalyze ORR, while the increase in octahedral Mn⁴⁺ content enhances the catalytic activity of Mn³⁺ by reducing the binding energy between Mn³⁺ and oxygen-containing intermediates, weakening the Mn³⁺-O bond, and accelerating the decomposition of hydrogen peroxide generated by Mn³⁺ during the ORR process. Sm_0.6Ba_0.4Mn₂O₅ exhibits excellent ORR performance owing to the suitable Mn⁴⁺/Mn³⁺ ratio on its surface, the half-wave potential reaches 0.77 V, higher than the 0.72 V of SmMn₂O₅, and the diffusion-limited current density increases from 3.50 mA·cm⁻² for SmMn₂O₅ to 5.03 mA·cm⁻². Moreover, the synergistic catalytic mechanism of the dual crystal fields was well discussed.

为了增强金字塔型Mn3+和八面体Mn4+双晶场在SmMn2O5中的协同催化作用，提高其氧还原反应（ORR）性能，采用水热法制备了掺杂钡的Sm1-xBaxMn2O5 （x = 0.1 ~ 0.5）催化剂。Ba2+取代SmMn2O5中的部分Sm3+导致Sm1-xBaxMn2O5表面Mn4+/Mn3+和表面吸附氧/晶格氧的比值增加。表面吸附氧含量的增加表明氧吸附能力增强，而Mn4+含量的增加有利于双晶场的协同催化。金字塔形Mn3+作为催化ORR的活性位点，而八面体Mn4+含量的增加通过降低Mn3+与含氧中间体之间的结合能，减弱Mn3+-O键，加速ORR过程中Mn3+生成的过氧化氢的分解，增强了Mn3+的催化活性。Sm0.6Ba0.4Mn2O5由于其表面合适的Mn4+/Mn3+比例而表现出优异的ORR性能，其半波电位达到0.77 V，高于SmMn2O5的0.72 V，扩散限制电流密度由SmMn2O5的3.50 mA·cm−2提高到5.03 mA·cm−2。并对双晶场的协同催化机理进行了深入探讨。

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引用次数: 0

Hollow-structured ZIF-derived CoS2/nitrogen doped carbon hybrid integrated with layered ReS2 Heterostructures as advanced Electrocatalysts for alkaline water splitting 空心结构zif衍生CoS2/氮掺杂碳杂化物与层状ReS2异质结构集成作为碱性水裂解的高级电催化剂

IF 4.1 3区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Electroanalytical Chemistry

Pub Date : 2025-12-26 DOI: 10.1016/j.jelechem.2025.119769

Yanhui Lu , Zhengqiang Zhao , Zhiqiang Liang , Qing Liu , Ho Seok Park , Jung Kyu Kim , Donglei Guo , Xu Yu

The development of efficient and robust bifunctional electrocatalysts for both oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) is crucial for cleaner hydrogen production. Herein, we report a sophisticated core-shell electrocatalyst by hydrothermal and calcination methods using metal-organic frameworks (MOFs) as precursors. The derivation of MOF features cobalt disulfide (CoS₂) as cores seamlessly integrated with a nitrogen-doped carbon matrix, which further supports an outer shell of rhenium disulfide (ReS₂) nanosheets (CoS₂-NC@ReS₂). Hollow core-shell architecture synergistically combines the high conductivity and stability of the N-doped carbon, the favorable catalytic activity of CoS₂ and ReS₂. Abundant heterointerfaces between CoS₂ and ReS₂ and tunable local charge distributions not only provide abundant surface active sites but also facilitate electrolyte penetration and release of generated H₂/O₂ bubbles. These synergistic effects significantly promote water dissociation and accelerate the electrocatalytic reaction kinetics. When evaluated for overall water splitting, the catalyst demonstrates exceptional bifunctional performance, requiring low overpotentials of 145 and 279 mV for both HER and OER to drive 10 mA cm⁻² with a total water-splitting voltage of 1.65 V. Furthermore, the robust core-shell structure endows the catalyst with remarkable long-term electrochemical stability and negligible performance decay. This work provides a viable MOF-derived strategy for constructing advanced heterostructured electrocatalysts for renewable energy applications.

开发高效、稳健的析氧反应和析氢反应双功能电催化剂是实现清洁制氢的关键。在此，我们报告了一种复杂的核壳电催化剂，通过水热和煅烧的方法，以金属有机框架（MOFs）为前驱体。衍生的MOF将二硫化钴（CoS2）作为核心与氮掺杂碳基体无缝集成，进一步支持二硫化铼（ReS2）纳米片的外壳（CoS2-NC@ReS2）。空心核壳结构协同结合了n掺杂碳的高导电性和稳定性，以及CoS2和ReS2良好的催化活性。CoS2和ReS2之间丰富的异质界面和可调节的局部电荷分布不仅提供了丰富的表面活性位点，而且促进了电解质的渗透和生成的H2/O2气泡的释放。这些协同效应显著地促进了水的解离，加速了电催化反应动力学。当对整体水分解进行评估时，该催化剂表现出优异的双功能性能，HER和OER都需要145和279 mV的低过电位，以1.65 V的总水分解电压驱动10 mA cm - 2。此外，坚固的核壳结构使催化剂具有显著的长期电化学稳定性和可忽略的性能衰减。这项工作为构建可再生能源应用的先进异质结构电催化剂提供了一种可行的mof衍生策略。

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引用次数: 0

Effect of cathodic potential on the electrochemical and stress corrosion cracking behavior of ER8C wheel steel 阴极电位对ER8C车轮钢电化学及应力腐蚀开裂行为的影响

IF 4.1 3区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Electroanalytical Chemistry

Pub Date : 2025-12-26 DOI: 10.1016/j.jelechem.2025.119767

Tonghan Guo , Shiyu Huang , Bendi Wu , Yuqin Feng , Ni Ao , Wei Wu

Train wheels endure harsh external environments and complex loads during long-term operation, leading to a high stress corrosion cracking (SCC) risk. Currently, research on the SCC mechanisms remains insufficient. This study investigated the effect of cathodic polarization on SCC of ER8C steel in 3.5 % NaCl solution. The results showed that in the potential range of OCP ∼ −850 mV _{vs SCE}, the R_ct and R_p of ER8C steel decreased initially and then increased. The fracture surfaces exhibited quasi-cleavage characteristics, accompanied by shallow dimples and microcracks initiating from the pits bottom. Accordingly, the SCC mechanism was primarily controlled by anodic dissolution, with a gradual reduction in susceptibility. In the potential range of −850 mV _{vs SCE} ∼ −1200 mV _{vs SCE}, both R_ct and R_p continued to diminish as the potential decreased. The SCC susceptibility of ER8C steel increased. Particularly at potentials below −1000 mV _{vs SCE}, the steel exhibited typical brittle fracture characteristics. Cracks propagated preferentially along grain boundaries or pearlite lamellae, indicating that the SCC process was primarily dominated by a hydrogen embrittlement mechanism.

列车车轮在长期运行过程中承受恶劣的外部环境和复杂的载荷，导致高应力腐蚀开裂（SCC）风险。目前，对SCC机制的研究还不够充分。研究了阴极极化对ER8C钢在3.5% NaCl溶液中SCC的影响。结果表明，在OCP ~ - 850 mV vs SCE电位范围内，ER8C钢的Rct和Rp先减小后增大。断口表面呈现准解理特征，并伴有浅韧窝和从坑底开始的微裂纹。因此，SCC机制主要由阳极溶解控制，磁化率逐渐降低。在- 850 mV vs SCE ~ - 1200 mV vs SCE的电位范围内，Rct和Rp都随着电位的降低而继续减小。ER8C钢的SCC敏感性增加。特别是在低于- 1000 mV vs SCE的电位下，钢表现出典型的脆性断裂特征。裂纹优先沿晶界或珠光体片扩展，表明SCC过程主要以氢脆机制为主。

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引用次数: 0

Construction of defective nickel terephthalate nanosheets through modulating the ratio of Ni(II) to ligand for ultra-sensitive glucose detection 通过调节Ni（II）与配体的比例构建用于超灵敏葡萄糖检测的缺陷对苯二甲酸镍纳米片

IF 4.1 3区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Electroanalytical Chemistry

Pub Date : 2025-12-26 DOI: 10.1016/j.jelechem.2025.119768

Lili Xiao , Zishuang Yong , Jin Jiang

In this work, nickel terephthalate coordination polymer (termed as NiPTA) with nanosheet-like structure was in-situ grown on nickel foam (NF) through a one-step solvothermal process. The defective sites of NiPTA were created by facilely modulating the ratio of Ni(II) to ligand. The rich unsaturated metal sites and good conductivity of NiPTA nanosheets (D-NiPTA-NS) significantly facilitated electrocatalytic oxidation of glucose with a sensitivity of 27, 000 μA mM⁻¹ cm⁻² that surpassed that most of recently reported glucose sensors. In addition, the proposed NF/D-NiPTA-NS sensor had some other conspicuous properties including a low limit of detection (0.33 μM), and high repeatability and reproducibility with low RSDs of 4.5 %, and 2.3 %, respectively. Moreover, the current response to 0.05 mM glucose at NF/D-NiPTA-NS retained its 94.5 % initial current value after being stored for 14 days. Most importantly, NF/D-NiPTA-NS was successfully applied to detect glucose in fetal calf serum with satisfactory recoveries (89–100 %).

在这项工作中，通过一步溶剂热法在泡沫镍（NF）上原位生长了具有纳米片状结构的对苯二甲酸镍配位聚合物（NiPTA）。通过调节Ni（II）与配体的比例，可以产生NiPTA的缺陷位点。NiPTA纳米片（D-NiPTA-NS）丰富的不饱和金属位点和良好的导电性显著促进了葡萄糖的电催化氧化，其灵敏度为27000 μA mM−1 cm−2，超过了最近报道的大多数葡萄糖传感器。此外，所提出的NF/D-NiPTA-NS传感器具有检测限低（0.33 μM）、重复性和再现性高（rsd分别为4.5%和2.3%）等显著特性。此外，NF/D-NiPTA-NS对0.05 mM葡萄糖的电流响应在储存14天后仍保持其94.5%的初始电流值。最重要的是，NF/D-NiPTA-NS成功地用于检测胎牛血清中的葡萄糖，回收率令人满意（89 - 100%）。

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引用次数: 0

Construction of defect-engineered ZnS/BP to form S-vacancy heterojunction catalyst for the electrocatalytic reduction of N2 to NH3 构建缺陷工程ZnS/BP形成s -空位异质结催化剂用于电催化还原N2制NH3

IF 4.1 3区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Electroanalytical Chemistry

Pub Date : 2025-12-25 DOI: 10.1016/j.jelechem.2025.119758

Shaona Chen , Tianwei Liang , Demiao Fang , Jie Qin , Rengui Weng , Zhongxu Dai

This paper successfully synthesized a new type of heterojunction material (Vs-ZnS/BP), which is composed of black phosphorus nanosheets and S vacancy defective ZnS nanoparticles. The results show that this material directly possesses a heterojunction, which can effectively enhance the electrocatalytic activity. In 0.1 M Na₂SO₄, the ammonia production rate of the newly prepared catalyst reaches 48.2 μgh⁻¹mgcat⁻¹ at −0.5 V (vs. RHE), and the Faraday efficiency reaches 33.39% at −0.2 V (vs. RHE). Through DFT calculations, it is proved that the introduction of S vacancies provides reaction sites for the N₂-NH₃ conversion and can also activate the N₂ molecule. Compared with black phosphorus, the heterojunction composite material significantly improves the ammonia synthesis yield and Faraday efficiency.

本文成功地合成了一种新型异质结材料（Vs-ZnS/BP），该材料由黑磷纳米片和S空位缺陷ZnS纳米颗粒组成。结果表明，该材料直接具有异质结，可以有效地提高电催化活性。在0.1 M Na2SO4条件下，在- 0.5 V （vs. RHE）下，新制备的催化剂制氨率达到48.2 μgh−1mgcat−1，在- 0.2 V （vs. RHE）下，法拉第效率达到33.39%。通过DFT计算，证明了S空位的引入为N2- nh3转化提供了反应位点，也可以激活N2分子。与黑磷相比，该异质结复合材料显著提高了合成氨收率和法拉第效率。

引用次数: 0

Keggin-type potassium phosphomolybdate-functionalized carbon nanotube composite-modified separator for advanced Lithium-Sulfur battery keggin型磷钼酸钾功能化碳纳米管复合改性锂硫电池隔膜

IF 4.1 3区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Electroanalytical Chemistry

Pub Date : 2025-12-24 DOI: 10.1016/j.jelechem.2025.119765

Shuang Wang , Rongrong Wang , Yaqi Chen , Zhiyuan Shi , Jianli Wang , Shanshan Yao

Lithium sulfur batteries are regarded as attractive candidates for next-generation energy storage systems due to their high theoretical energy density. Nevertheless, their commercialization is obstructed by the polysulfide shuttle and sluggish redox reactions. To address these limitations, we introduce a multifunctional separator coating constructed from Keggin-type potassium phosphomolybdate (K₃PMo₁₂O₄₀, KPM) nanospheres combined with functionalized carbon nanotubes (FCNTs). The interconnected one-dimensional FCNTs establish a conductive pathway that accelerates both ion/electron transport, while their oxygen-containing functional groups anchoring polysulfides and inhibiting diffusion. Meanwhile, KPM nanospheres contribute abundant active sites for polysulfides chemisorption, and their Mo⁶⁺/Mo⁵⁺ redox couples act as catalytic centers to accelerate the reversible electrochemical transformation between soluble polysulfides and solid-phase lithium sulfide during cycling. Performance evaluation demonstrates that when the sulfur cathode possesses an area loading of 3.5 mg cm⁻², the functional separator of cell delivers the first discharge capacity of 973.7 mAh g⁻¹ at 0.5C and maintains 589.5 mAh g⁻¹ over 300 cycles. Furthermore, the cell with KPM@FCNTs retains 528.3 mAh g-1 even at −10 °C with stable cycling behavior. This study demonstrates the cooperative action of KPM and FCNTs in mitigating shuttle effects and boosting redox conversion, providing an effective design strategy for advanced lithium sulfur batteries.

锂硫电池由于具有较高的理论能量密度，被认为是下一代储能系统的有吸引力的候选者。然而，它们的商业化受到多硫化物穿梭和缓慢的氧化还原反应的阻碍。为了解决这些限制，我们引入了一种由keggin型磷钼酸钾（K3PMo12O40， KPM）纳米球结合功能化碳纳米管（FCNTs）构建的多功能隔膜涂层。相互连接的一维FCNTs建立了导电途径，加速了离子/电子的传递，而其含氧官能团锚定了多硫化物并抑制了扩散。同时，KPM纳米球为多硫化物的化学吸附提供了丰富的活性位点，其Mo6+/Mo5+氧化还原偶对作为催化中心，加速了循环过程中可溶性多硫化物与固相硫化锂之间的可逆电化学转化。性能评价表明，当硫阴极的面积负载为3.5 mg cm−2时，电池的功能隔板在0.5℃下可提供973.7 mAh g−1的首次放电容量，并在300次循环中保持589.5 mAh g−1。此外，含有KPM@FCNTs的电池即使在−10°C下也能保持528.3 mAh g-1，并且具有稳定的循环行为。本研究证明了KPM和FCNTs在减轻穿梭效应和促进氧化还原转化方面的协同作用，为先进锂硫电池的设计提供了有效的策略。

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引用次数: 0

Vanadium-induced structure reconfiguration of MnO2 and energy storage performance improvement in aqueous zinc ion batteries 钒诱导MnO2结构重构及水锌离子电池储能性能改善

IF 4.1 3区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Electroanalytical Chemistry

Pub Date : 2025-12-24 DOI: 10.1016/j.jelechem.2025.119763

Junjian Zhou , Jiaxin Sun , Tianzhen Jian , Xianhong Li , Haiyang Gao , Jianping Ma , Jiasheng Xu , Yuyan Wang , Wenqing Ma , Lishan Yang

The development of high-performance cathode materials for aqueous zinc-ion batteries (AZIBs) is crucial for advancing sustainable energy storage. Manganese dioxide (MnO₂) is a promising candidate but suffers from poor electronic conductivity, structural instability, and sluggish Zn²⁺ diffusion kinetics. In this study, we demonstrate that vanadium (V) doping effectively reconfigures the structure of MnO₂, leading to significantly enhanced electrochemical performance. A series of V-doped MnO₂ samples with controlled doping levels were synthesized via a scalable solvothermal method. We found that V doping induces a morphological transformation from nanowires to nanosheets, expands the lattice spacing, and improves hydrophilicity, thereby facilitating Zn²⁺ diffusion and increasing reversible capacity. Comprehensive structural and electrochemical analyses reveal that an optimal V doping concentration balances the contributions from Zn²⁺ and H⁺ intercalation, while additional redox activity from vanadium further boosts capacity. The optimized medium-V-content MnO₂ cathode exhibits a superior rate capability of 133.1 mAh g⁻¹ at 5 A g⁻¹ and exceptional stability with 87.3 mAh g⁻¹ retained after 2000 cycles at 2 A g⁻¹. This work provides deep insights into the role of V doping in modifying the structure and reaction mechanisms of MnO₂, offering an effective strategy for designing high-performance cathodes for AZIBs.

开发高性能的水性锌离子电池正极材料对于推进可持续储能至关重要。二氧化锰（MnO2）是一种很有前途的候选材料，但其电子导电性差，结构不稳定，Zn2+扩散动力学缓慢。在这项研究中，我们证明了钒(V)的掺杂有效地重新配置了MnO2的结构，从而显著提高了电化学性能。采用可扩展溶剂热法合成了一系列可控掺杂水平的v掺杂MnO2样品。我们发现V掺杂诱导了纳米线到纳米片的形态转变，扩大了晶格间距，提高了亲水性，从而促进了Zn2+的扩散，增加了可逆容量。综合结构和电化学分析表明，最佳V掺杂浓度平衡了Zn2+和H+插入的贡献，而钒的额外氧化还原活性进一步提高了容量。优化后的中v含量MnO2阴极在5 a g−1下具有133.1 mAh g−1的优异倍率性能，在2 a g−1下循环2000次后仍保持87.3 mAh g−1的优异稳定性。该研究深入揭示了V掺杂对MnO2结构和反应机理的影响，为设计高性能azib阴极提供了有效的策略。

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引用次数: 0

Synthesis and electrochemical performance of Al-doped P2-type Na0.67Co0.2−xMn0.8AlxO2 for sodium-ion battery cathodes 钠离子电池负极用掺铝p2型Na0.67Co0.2−xMn0.8AlxO2的合成及电化学性能

IF 4.1 3区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Electroanalytical Chemistry

Pub Date : 2025-12-24 DOI: 10.1016/j.jelechem.2025.119764

Gongqin Yan , Yuxin Hong , Yanchao Qi , Xianghui Fu , Chunbo Lan , Zhijie Fang

To mitigate the challenges of high-voltage phase transitions, increased polarization, and interfacial instability in Co/Mn-based layered oxides, this study synthesized Al-doped P2-type Na_0.67Co_0.2−xMn_0.8Al_xO₂(x = 0, 0.02, 0.05, 0.08) cathodes via a high-temperature solid-state method, and systematically characterized their crystal structure, morphology, and valence evolution via X-ray diffraction (XRD), scanning electron microscopy (SEM), energy-dispersive spectroscopy (EDS), and X-ray photoelectron spectroscopy (XPS). The results indicate that Al³⁺ ions were successfully and uniformly incorporated into the lattice without destroying the P2-type structure, which regulated lattice parameters, modulated Mn valence states, suppressed the Jahn-Teller effect, and enhanced structural stability. Further electrochemical tests revealed that appropriate Al doping effectively suppressed high-voltage phase transitions and reduced charge-transfer resistance, thereby enhancing the electrochemical performance. At a voltage range of 2–4.2 V and a rate of 0.1C, the initial discharge specific capacity of Na_0.67Co_0.15Mn_0.8Al_0.05O₂ was 131.8 mAh·g⁻¹, and the capacity retention rate after 100 cycles was 82.4 %, which was 17.3 % higher than that of the undoped material. Band structure calculations confirmed the optimized electronic structure, demonstrating that Al doping is an effective strategy for improving the electrochemical performance of Co/Mn-based layered oxide cathodes for sodium-ion batteries.

为了减轻Co/ mn基层状氧化物中高压相变、极化加剧和界面不稳定性的挑战，本研究通过高温固相法合成了al掺杂的p2型Na0.67Co0.2−xMn0.8AlxO2（x = 0,0.02, 0.05, 0.08）阴极，并通过x射线衍射（XRD）、扫描电子显微镜（SEM）、能谱（EDS）、和x射线光电子能谱（XPS）。结果表明，在不破坏p2型结构的情况下，Al3+离子成功且均匀地掺入到晶格中，从而调节晶格参数，调制Mn价态，抑制Jahn-Teller效应，增强结构稳定性。进一步的电化学测试表明，适当的Al掺杂可以有效地抑制高压相变，降低电荷转移电阻，从而提高电化学性能。在2 ~ 4.2 V电压范围和0.1C倍率下，Na0.67Co0.15Mn0.8Al0.05O2的初始放电比容量为131.8 mAh·g−1,100次循环后的容量保持率为82.4%，比未掺杂材料提高了17.3%。带结构计算证实了优化后的电子结构，表明Al掺杂是提高钠离子电池Co/ mn基层状氧化物阴极电化学性能的有效策略。

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引用次数: 0

Tuning the oxygen concentrations in perovskite oxide thin films for improved double-exchange interaction and enhanced electrocatalytic oxygen evolution reaction 调整钙钛矿氧化物薄膜中的氧浓度以改善双交换相互作用和增强电催化析氧反应

IF 4.1 3区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Electroanalytical Chemistry

Pub Date : 2025-12-23 DOI: 10.1016/j.jelechem.2025.119762

Ji Qi , Kaixin Zhu , Weiguang Ma , Hefeng Zhang , Ming Feng , Xu Zong

Double-exchange interaction has been identified as a crucial factor in tuning oxygen evolution reaction (OER) activity of perovskite-type transition metal oxides (ABO₃-TMOs). The double-exchange interaction is an electron transfer mechanism mediated by bridging atoms (typically oxygen) and governed by spin alignment. However, the influence of oxygen concentration on the double-exchange interaction and the OER activity of different types of ABO₃-TMOs remains unclarified. Herein, a series of ABO₃-TMOs thin films with controllable oxygen concentration, including LaNiO₃ (LNO), La_2/3Sr_1/3CoO₃ (LSCO), La_2/3Sr_1/3MnO₃ (LSMO), LaFeO₃ (LFO) and SrMnO₃ (SMO) were prepared on SrTiO₃ (STO) substrate with pulsed laser deposition (PLD) under different growth oxygen pressures, yielding epitaxial single-crystal ABO₃-TMOs thin films with high (H) or low (L) oxygen concentrations. We showed that by modulating the oxygen concentration, the double-exchange interaction in ABO₃-TMOs thin films was regulated, thereby changing the e_g electron hopping behavior. Moreover, LNO-H, LSCO-H, LSMO-H, LFO-L and SMO-L demonstrated higher OER activity than LNO-L, LSCO-L, LSMO-L, LFO-H and SMO-H thin films, indicating a strong correlation with the strength of the double-exchange interaction. This study underscores the significance of rationally modulating the double-exchange interaction in ABO₃-TMOs thin films via tuning oxygen concentration to enhance OER activity.

双交换相互作用是调节钙钛矿型过渡金属氧化物（ABO3-TMOs）析氧反应（OER）活性的关键因素。双交换相互作用是一种由桥接原子（通常是氧）介导并由自旋排列控制的电子传递机制。然而，氧浓度对不同类型ABO3-TMOs的双交换相互作用和OER活性的影响尚不清楚。本文采用脉冲激光沉积（PLD）技术，在不同生长氧压下，在SrTiO3 （STO）衬底上制备了一系列氧浓度可控的ABO3-TMOs薄膜，包括LaNiO3 （LNO）、La2/3Sr1/3CoO3 （LSCO）、La2/3Sr1/3MnO3 （LSMO）、LaFeO3 （LFO）和SrMnO3 (SMO)，得到了高(H)或低(L)氧浓度的外延单晶ABO3-TMOs薄膜。我们发现，通过调节氧浓度，ABO3-TMOs薄膜中的双交换相互作用被调节，从而改变了eg电子跳变行为。此外，LNO-H、LSCO-H、lsmoo - h、LFO-L和smoo - l薄膜的OER活性高于LNO-L、LSCO-L、lsmoo - l、LFO-H和smoo - h薄膜，这与双交换作用强度有很强的相关性。本研究强调了通过调节氧浓度来合理调节ABO3-TMOs薄膜中双交换相互作用以提高OER活性的重要性。

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引用次数: 0