Electrochimica Acta最新文献_第10页

Corrosion protection performance of poly(PyM-co-GMA)/SWCNT nanocomposites coating on mild steel 聚(PyM-co-GMA)/SWCNT 纳米复合材料涂层对低碳钢的腐蚀防护性能

IF 5.5 3区材料科学 Q1 ELECTROCHEMISTRY

Electrochimica Acta

Pub Date : 2024-10-23 DOI: 10.1016/j.electacta.2024.145272

Patnam Mohamed Ashfaque, Kottur Anver Basha, Sakvai Mohammed Safiullah

Recently, there has been significant emphasis on developing electroactive functional methacrylate polymers for anticorrosive applications. In this context, we have synthesized Poly[(3,5-dimethyl-1H-pyrazole-1-yl) methyl methacrylate-co-glycidyl methacrylate] [Poly(PyM-co-GMA)] and its nanocomposite with single- walled carbon nanotubes (SWCNTs) [Poly(PyM-co-GMA)/SWCNT]. The resulting materials were characterized using Fourier Transform Infrared spectroscopy (FT-IR) and X-ray Diffraction analysis (XRD). Morphological changes due to the incorporation of SWCNTs were examined using field-emission scanning electron microscopy (FE-SEM) and high-resolution transmission electron microscopy (HR-TEM). The optical properties of Poly(PyM-co-GMA) and Poly(PyM-co-GMA)/SWCNT (0.5, 1.0, and 1.5 wt. %) were investigated. The thermal behavior of Poly(PyM-co-GMA) and its SWCNT nanocomposites was analyzed through thermogravimetric analysis (TGA). The anticorrosive performance of the prepared materials was evaluated on a mild steel substrate (MS) in a 3.5% (w/v) NaCl medium using electrochemical techniques. Results from potentiodynamic polarization and electrochemical impedance spectroscopy indicate that the Poly(PyM-co-GMA) and Poly(PyM- co-GMA)/SWCNT coatings (0.5, 1.0, and 1.5 wt. %) provide effective barrier protection for mild steel against marine environments.

最近，开发用于防腐应用的电活性功能性甲基丙烯酸酯聚合物受到了极大重视。为此，我们合成了聚[(3,5-二甲基-1H-吡唑-1-基) 甲基丙烯酸甲酯-甲基丙烯酸缩水甘油酯] [Poly(PyM-co-GMA)] 及其与单壁碳纳米管 (SWCNT) 的纳米复合材料 [Poly(PyM-co-GMA)/SWCNT]。使用傅立叶变换红外光谱（FT-IR）和 X 射线衍射分析（XRD）对所得材料进行了表征。使用场发射扫描电子显微镜（FE-SEM）和高分辨率透射电子显微镜（HR-TEM）研究了加入 SWCNT 后的形态变化。研究了 Poly(PyM-co-GMA)和 Poly(PyM-co-GMA)/SWCNT（0.5、1.0 和 1.5 wt.%）的光学特性。通过热重分析 (TGA) 分析了聚(PyM-co-GMA)及其 SWCNT 纳米复合材料的热行为。利用电化学技术评估了所制备材料在 3.5% (w/v) NaCl 介质中对低碳钢基材 (MS) 的防腐性能。电位极化和电化学阻抗光谱的结果表明，Poly(PyM- co-GMA)和 Poly(PyM- co-GMA)/SWCNT涂层（0.5、1.0 和 1.5 wt.%）能有效阻隔海洋环境对低碳钢的腐蚀。

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引用次数: 0

Fluorescence switching of triarylamine-based polyamides with pendant pyrene units and its application in electrochromic smart displays 带有芘单元的三芳基胺基聚酰胺的荧光转换及其在电致变色智能显示器中的应用

IF 5.5 3区材料科学 Q1 ELECTROCHEMISTRY

Electrochimica Acta

Pub Date : 2024-10-23 DOI: 10.1016/j.electacta.2024.145277

Dongxu Li , Xiaoqi Shi , Wanan Cai , Haijun Niu

The pyrene group was directly connected to the triarylamine (TAA) unit through a benzene bridge via the Suzuki reaction to successfully prepare the diamine monomer. A series of new polyamides (PAs) based on TAA units were prepared by polycondensation. The PAs exhibited good solution processability and high thermal stability with the char yield in excess of 53 % at 800 °C in air atmosphere. In solvents with different polarities, these PAs showed solvatochromic effect and large stokes shift. Strongly photoluminescent PAs have a sensitive stimulus response to explosive and hazardous gas, and its fluorescence is easily turned off by the addition of trinitrophenol (TNP) and hydrogen chloride (HCl). And achieve fluorescence switching between exposure to HCl and ammonia (NH₃) gas. The PAs exhibited a reversible color response in the electrochemical oxidation process, with no significant degradation in current and transmittance after 200 cycles. The sandwich structure multicolor electrochromic device can achieve electrochromic performance applied by different voltages.

通过铃木反应，芘基通过苯桥与三芳基胺（TAA）单元直接连接，成功制备出二元胺单体。通过缩聚反应，制备出了一系列基于 TAA 单元的新型聚酰胺（PAs）。这些聚酰胺具有良好的溶液加工性和较高的热稳定性，在 800°C 的空气环境中，炭化率超过 53%。在不同极性的溶剂中，这些聚酰胺表现出溶解变色效应和较大的斯托克斯偏移。强光致发光 PA 对爆炸性有害气体具有灵敏的刺激响应，加入三硝基苯酚（TNP）和氯化氢（HCl）后，其荧光很容易熄灭。并在暴露于 HCl 和氨（NH3）气体之间实现荧光切换。PAs 在电化学氧化过程中表现出可逆的颜色响应，200 次循环后电流和透射率均无明显衰减。这种三明治结构的多色电致变色器件可在不同电压下实现电致变色性能。

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引用次数: 0

Comparative study of zinc sulfide, tin selenide, and their composite electrocatalysts for oxygen evolution reaction: Towards efficient and stable water splitting 硫化锌、硒化锡及其复合电催化剂在氧进化反应中的比较研究：实现高效稳定的水分离

IF 5.5 3区材料科学 Q1 ELECTROCHEMISTRY

Electrochimica Acta

Pub Date : 2024-10-23 DOI: 10.1016/j.electacta.2024.145279

Rida Fatima , Kareem Yusuf , Muhammad Shuaib Khan , Mehar Un Nisa

Oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) are critical processes in electrochemical water splitting, driving demand for efficient and durable electrocatalysts. This study presents a comprehensive evaluation of water splitting performance of ZnS@SnSe₂ nano–composite in 1.0 M KOH solution. With ZnS nanoparticles decorated on SnSe₂, exhibited remarkable catalytic activity for both HER and OER. ZnS@SnSe₂ composite demonstrated an low overpotential of 22 mV to reach a current density of 10 mA cm^-2, outperforming ZnS (245 mV) and SnSe₂ (280 mV). Furthermore, it achieved a Tafel slope of 25 mV dec^‑1 and a charge transfer resistance (Rct) of 5.2 Ω, reflecting its enhanced kinetics compared to ZnS (101 mV dec^‑1, Rct = 35 Ω) and SnSe₂ (230 mV dec^‑1, Rct = 7.5 Ω). These results are even competitive with benchmark Pt/C catalyst (30 mV overpotential, 46 mV dec^‑1, and 2.2 Ω Rct), highlighting efficiency of composite for hydrogen production. For OER, ZnS@SnSe₂ composite required an overpotential of 234 mV to reach 10 mA cm⁻², a substantial improvement over ZnS (361 mV) and SnSe₂ (375 mV). Composite showcased a low Tafel slope of 48 mV dec^‑1 and an Rct of 1.5 Ω, comparable to commercial RuO₂ catalyst (44 mV dec^‑1, Rct = 2.2 Ω), further underscoring its superior oxygen evolution capabilities. In practical device configuration, ZnS@SnSe₂/NF electrode achieved a Tafel slope of 21.335 mV dec^‑1 for HER and 58.028 mV dec^‑1 for OER, demonstrating its bifunctional efficiency in a two-electrode system. The device exhibited exceptional long-term stability over 50 h of continuous operation, highlighting its potential for scalable and sustainable water splitting applications.

氧进化反应（OER）和氢进化反应（HER）是电化学水分离的关键过程，因此需要高效耐用的电催化剂。本研究全面评估了 ZnS@SnSe2 纳米复合材料在 1.0 M KOH 溶液中的分水性能。在 SnSe2 上装饰了 ZnS 纳米颗粒后，ZnS@SnSe2 纳米复合材料在 HER 和 OER 中都表现出了显著的催化活性。ZnS@SnSe₂ 复合材料的过电位低至 22 mV，电流密度达到 10 mA cm-2，优于 ZnS（245 mV）和 SnSe2（280 mV）。此外，与 ZnS（101 mV dec-1，Rct = 35 Ω）和 SnSe2（230 mV dec-1，Rct = 7.5 Ω）相比，它的塔菲尔斜率（Tafel slope）为 25 mV dec-1，电荷转移电阻（Rct）为 5.2 Ω，反映了其更强的动力学性能。这些结果甚至可以与基准 Pt/C 催化剂（30 mV 过电位、46 mV dec-1 和 2.2 Ω Rct）相媲美，从而凸显了复合催化剂的制氢效率。就 OER 而言，ZnS@SnSe2 复合材料需要 234 mV 的过电位才能达到 10 mA cm-²，与 ZnS（361 mV）和 SnSe2（375 mV）相比有了大幅提高。复合材料的塔菲尔斜率较低，为 48 mV dec-1，Rct 为 1.5 Ω，与商用 RuO2 催化剂（44 mV dec-1，Rct = 2.2 Ω）相当，进一步突出了其卓越的氧进化能力。在实际器件配置中，ZnS@SnSe₂/NF 电极在 HER 和 OER 的塔菲尔斜率分别为 21.335 mV dec-1 和 58.028 mV dec-1，显示了其在双电极系统中的双功能效率。该装置在 50 小时的连续运行中表现出卓越的长期稳定性，突显了其在可扩展和可持续水分离应用方面的潜力。

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引用次数: 0

An assessment of electroneutrality implementations for accurate electrochemical ion transport models 评估精确电化学离子传输模型的电中性实施情况

IF 5.5 3区材料科学 Q1 ELECTROCHEMISTRY

Electrochimica Acta

Pub Date : 2024-10-23 DOI: 10.1016/j.electacta.2024.145280

Benjamin Janotta , Maximilian Schalenbach , Hermann Tempel , Rüdiger-A. Eichel

During the diffusion and migration of ions in electrolytes, the electrodynamic ion-ion interactions prevent charge separation despite different ionic mobilities, ultimately enforcing electroneutrality in the bulk electrolyte. To model ion transport accurately, a method to enforce electroneutrality must be implemented. In this study, four strategies to implement electroneutrality are discussed and evaluated. The ion distributions that result from a transport model with the different electroneutrality implementations are calculated, considering various electrolytes and sets of electrochemical parameters. The meaningfulness and applicability of each implementation are assessed through spatial charge accumulations, transference numbers, and experimental data from the literature. Combining the electrochemical ion transport models with the electroneutrality constraint for all ions is shown to result in an overdetermined system of equations if the driving forces are calculated under neglection of diffusion potentials. The often-reported model simplification of using the electroneutrality constraint to resolve the transport of one specific species explicitly results in non-physically correct mass transport. A practical approach to precisely describe the measured physicochemical ion movements is obtained by equilibrating spatial charges with the ion conduction for every time step in the ion transport model, which is reasonably applicable to multi-ion systems in three-dimensional frameworks. This comprehensive assessment aims to guide readers in selecting an appropriate electroneutrality implementation framework for ion transport models.

在电解质中离子的扩散和迁移过程中，尽管离子的迁移率不同，但电动离子间的相互作用阻止了电荷分离，最终在大体积电解质中实现了电中性。为了准确地模拟离子传输，必须采用一种方法来实现电中性。本研究讨论并评估了实现电中性的四种策略。考虑到各种电解质和电化学参数集，计算了采用不同电中性实施方法的传输模型所产生的离子分布。通过空间电荷累积、转移数和文献中的实验数据，对每种实现方式的意义和适用性进行了评估。将电化学离子输运模型与所有离子的电中性约束相结合，如果在负选择扩散电位下计算驱动力，则会导致过确定方程组。经常报道的使用电中性约束来解决某一特定物种迁移的模型简化会导致非物理正确的质量迁移。在离子输运模型中，通过平衡每一个时间步的空间电荷与离子传导，可以获得精确描述测量到的物理化学离子运动的实用方法，该方法合理地适用于三维框架中的多离子系统。本综合评估旨在指导读者为离子输运模型选择合适的电中性实施框架。

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引用次数: 0

Enhanced ammonia yield rate from nitrogen on collapsed dodecahedral-shaped Co/NC electrocatalyst 在塌陷十二面形 Co/NC 电催化剂上提高氮气产氨率

IF 5.5 3区材料科学 Q1 ELECTROCHEMISTRY

Electrochimica Acta

Pub Date : 2024-10-23 DOI: 10.1016/j.electacta.2024.145278

Bohui Wei , Yaodong Liang , Yuangang Li , Xudong Yang , Chenzhong Yao

Nowadays, multi-component non-precious metal catalysts have been considered as a significant strategy for enhancing the yield of synthesizing NH₃ by electrocatalytic nitrogen reduction reaction (E-NRR). In the present work, carbon composites doped with well-dispersed Co and N (Co/NC) were prepared by pyrolyzing zeolitic imidazolate framework-67 (ZIF-67) at various temperatures protected under a N₂ flow. Co/NC exhibits a collapsed dodecahedral morphology with a mesoporous structure (3.5–4 nm). The chemical states of Co/N and the structural defects of C are closely related to the carbonization temperature. In a N₂-saturated 0.1 M KOH electrolyte, the as-prepared catalysts exhibit an NH₃ yield rate (Y(NH₃)) of 60.57 μg h^-1 mg_cat.^-1 and a Faradaic efficiency (FE) of 23.3 % at -0.1 V (vs the reversible hydrogen electrode, RHE) at ambient conditions. The enhanced E-NRR activity of Co/NC may primarily originate from an associative distal pathway on the Co-N₃C sites and the carbon defects in an alkaline electrolyte. Specifically, this work presents a three-component E-NRR catalyst with excellent stability and great activity based on Co/NC.

如今，多组分非贵金属催化剂已被视为通过电催化氮还原反应（ERR）提高合成 NH3 产率的重要策略。在本研究中，通过在不同温度下热解沸石咪唑盐酸盐框架-67（ZIF-67），并在氮气流保护下制备了掺杂了良好分散的 Co 和 N 的碳复合材料（Co/NC）。Co/NC 呈十二面体塌缩形态，具有介孔结构（3.5-4 nm）。Co/N 的化学状态和 C 的结构缺陷与碳化温度密切相关。在 N2 饱和的 0.1 M KOH 电解液中，所制备的催化剂在环境条件下的 NH3 产率（Y(NH3)）为 60.57 μg h-1 mgcat.-1，在 -0.1 V 下的法拉第效率（FE）为 23.3%（相对于可逆氢电极，RHE）。Co/NC 增强的ERR 活性可能主要源于 Co-N3-C 位点和碱性电解质中碳缺陷的关联远端途径。具体而言，本研究提出了一种基于 Co/NC 的三组份 E-NRR 催化剂，该催化剂具有优异的稳定性和极高的活性。

{"title":"Enhanced ammonia yield rate from nitrogen on collapsed dodecahedral-shaped Co/NC electrocatalyst","authors":"Bohui Wei , Yaodong Liang , Yuangang Li , Xudong Yang , Chenzhong Yao","doi":"10.1016/j.electacta.2024.145278","DOIUrl":"10.1016/j.electacta.2024.145278","url":null,"abstract":"<div><div>Nowadays, multi-component non-precious metal catalysts have been considered as a significant strategy for enhancing the yield of synthesizing NH<sub>3</sub> by electrocatalytic nitrogen reduction reaction (E-NRR). In the present work, carbon composites doped with well-dispersed Co and N (Co/NC) were prepared by pyrolyzing zeolitic imidazolate framework-67 (ZIF-67) at various temperatures protected under a N<sub>2</sub> flow. Co/NC exhibits a collapsed dodecahedral morphology with a mesoporous structure (3.5–4 nm). The chemical states of Co/N and the structural defects of C are closely related to the carbonization temperature. In a N<sub>2</sub>-saturated 0.1 M KOH electrolyte, the as-prepared catalysts exhibit an NH<sub>3</sub> yield rate (<em>Y</em>(NH<sub>3</sub>)) of 60.57 μg h<sup>-1</sup> mg<sub>cat.</sub><sup>-1</sup> and a Faradaic efficiency (FE) of 23.3 % at -0.1 V (<em>vs</em> the reversible hydrogen electrode, RHE) at ambient conditions. The enhanced E-NRR activity of Co/NC may primarily originate from an associative distal pathway on the Co-N<sub>3<img></sub>C sites and the carbon defects in an alkaline electrolyte. Specifically, this work presents a three-component E-NRR catalyst with excellent stability and great activity based on Co/NC.</div></div>","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"508 ","pages":"Article 145278"},"PeriodicalIF":5.5,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142487543","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Novel pseudocapacitive one-dimensional copper pyrophosphate (Cu2P2O7) nanofibers for asymmetric supercapacitor 用于不对称超级电容器的新型伪电容一维焦磷酸铜（Cu2P2O7）纳米纤维

IF 5.5 3区材料科学 Q1 ELECTROCHEMISTRY

Electrochimica Acta

Pub Date : 2024-10-23 DOI: 10.1016/j.electacta.2024.145275

Nutan V. Mangate , Sushama M. Giripunje , Subhash B. Kondawar

The redox activity of a supercapacitor electrode can be significantly compromised by irregular, non-uniform, and agglomerated morphologies of the material. The preparation of a one-dimensional fibrous morphology not only ensures a consistent, continuous, and well-separated network of fibers but also results in an increased surface area compared to higher-dimensional structures. In this study, the fabrication of a continuous network of one-dimensional copper pyrophosphate (Cu₂P₂O₇) nanofibers through a straightforward polymer-based electrospinning method followed by calcination at 900 °C is reported. The resulting Cu₂P₂O₇ monoclinic nanofibers exhibited an average diameter of 95 nm, highlighting the enhanced surface area of the material. By employing nickel foam (NF) as a current collector, the Cu₂P₂O₇/NF electrode demonstrated a remarkable specific capacitance of 567.31 F g^-1 (357.4 C g^-1) at 2 A g^-1 in 1 M LiOH electrolyte, surpassing performances in 1 M KOH and 1 M NaOH electrolytes. Furthermore, we designed an asymmetric supercapacitor (ASC) device configuration by incorporating carbon nanofibers (CNFs) as the negative electrode. Cu₂P₂O₇//CNFs asymmetric supercapacitor showcases an exceptional specific capacitance, reaching 143.73 F g^-1 (244.34 C g^-1) at a current density of 0.4 A g^-1. This remarkable performance is complemented by a notable energy density of 57.69 Wh kg^-1 and power density of 1104.7 W kg^-1. Furthermore, even at an elevated power density of 5132.25 W kg^-1, the device maintained a considerable energy density of 22.81 Wh kg^-1. These findings underscore the viability of Cu₂P₂O₇ nanofibers as a compelling choice for energy storage devices.

超级电容器电极的氧化还原活性会因材料的不规则、不均匀和团聚形态而大打折扣。制备一维纤维形态不仅能确保纤维网络的一致性、连续性和良好的分离性，而且与高维结构相比，还能增加表面积。本研究报告采用基于聚合物的电纺丝方法，在 900°C 煅烧后制备出连续的一维焦磷酸铜（Cu2P2O7）纳米纤维网络。所制备的 Cu2P2O7 单晶纳米纤维的平均直径为 95 nm，凸显了该材料表面积的增大。通过采用泡沫镍（NF）作为集流体，Cu2P2O7/NF 电极在 1 M LiOH 电解液中的比电容达到了显著的 567.31 F g-1（357.4 C g-1）（2 A g-1），超过了在 1 M KOH 和 1 M NaOH 电解液中的表现。此外，我们还设计了一种非对称超级电容器（ASC）装置配置，将碳纳米纤维（CNF）作为负极。Cu2P2O7//CNFs 不对称超级电容器展示了非凡的比电容，在电流密度为 0.4 A g-1 时达到 143.73 F g-1（244.34 C g-1）。除了这一卓越性能外，它还具有 57.69 Wh kg-1 的能量密度和 1104.7 W kg-1 的功率密度。此外，即使在功率密度高达 5132.25 W kg-1 的情况下，该器件仍能保持 22.81 Wh kg-1 的可观能量密度。这些发现强调了 Cu2P2O7 纳米纤维作为储能装置的一种令人信服的选择的可行性。

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引用次数: 0

Facile synthesis of monoclinic (NH4)2V4O9 nanosheets for zinc-ion batteries 用于锌-离子电池的单斜 (NH4)2V4O9 纳米片的简单合成

IF 5.5 3区材料科学 Q1 ELECTROCHEMISTRY

Electrochimica Acta

Pub Date : 2024-10-23 DOI: 10.1016/j.electacta.2024.145264

Chongchong Li , Changyu Zhou , Jiangyong Xiong , Xinying Li

Aqueous zinc-ion batteries (ZIBs) are increasingly popular due to their low cost and high safety. However, the quest for cathode materials with robust internal structures and efficient ion transport pathways remains critical. In this study, we introduce a simple hydrothermal method to synthesize monoclinic (NH₄)₂V₄O₉ nanosheets, serving as a advanced cathode for ZIBs. This material demonstrates outstanding electrochemical properties, with a high specific capacity of 389 mAh g⁻¹ at 0.1 A g⁻¹, and retains 78.9 % capacity after 3000 cycles at 1 A g⁻¹ and 77.3 % after 15,000 cycles at 5 A g⁻¹. Additionally, it achieves an energy density of 325 Wh kg⁻¹ at 101 W kg⁻¹. In-depth electrochemical analysis reveals the structural stability during reversible Zn²⁺ ion intercalation/de-intercalation, underscoring the potential of (NH₄)₂V₄O₉ as a high-performance material for ZIBs.

锌离子水电池（ZIB）因其低成本和高安全性而越来越受欢迎。然而，寻找具有坚固内部结构和高效离子传输途径的阴极材料仍然至关重要。在本研究中，我们介绍了一种简单的水热法合成单斜 (NH4)2V4O9 纳米片，作为 ZIB 的先进阴极材料。这种材料具有出色的电化学性能，在 0.1 A g-1 条件下，比容量高达 389 mAh g-1，在 1 A g-1 条件下循环 3000 次后，容量保持率为 78.9%，在 5 A g-1 条件下循环 15000 次后，容量保持率为 77.3%。此外，在 101 W kg-1 的条件下，它的能量密度达到 325 Wh kg-1。深入的电化学分析揭示了 Zn2+ 离子可逆插层/去插层过程中的结构稳定性，凸显了 (NH4)2V4O9 作为 ZIB 高性能材料的潜力。

引用次数: 0

Effect of high-boiling point solvents on inkjet printing of catalyst layers for proton exchange membrane fuel cells 高沸点溶剂对质子交换膜燃料电池催化剂层喷墨打印的影响

IF 5.5 3区材料科学 Q1 ELECTROCHEMISTRY

Electrochimica Acta

Pub Date : 2024-10-22 DOI: 10.1016/j.electacta.2024.145273

Qingying Zhao , Tobias Morawietz , Pawel Gazdzicki , K. Andreas Friedrich

Inkjet printing (IJP) is considered as a promising and flexible method for low cost and drop-on-demand pattern formation in proton exchange membrane (PEM) fuel cells. Although significant advancements have been made in inkjet-printed electrodes, identifying the optimal ink formulations remains challenging due to severe restrictions on the ink properties. Generally, the catalyst layer prepared by IJP using low boiling point solvents (water/alcohol) show reasonable electrochemical performance. However, low boiling point solvents lead to clogging of the printhead nozzle due to fast evaporation of the solvent in the inkjet print head. In this study, high boiling point solvents (propylene glycol (PG) or ethylene glycol (EG)) were used as additives to reduce nozzle clogging and improve printing efficiency. In this context, the relationship between catalyst ink properties, CL microstructure, and electrochemical performance of the MEA is investigated. Results show that printing time is significantly reduced with adding high boiling point solvents in the ink (66.67% reduction of time with 30 wt% PG). However, an increased amount of additive is detrimental in terms of electrochemical performance due to formation of larger agglomerates, lower porosity of the catalyst layer, and reduced ECSA. The results of this work can be used to develop a strategy to adjust the trade-off between printing time and electrochemical performance of electrodes prepared using IJP.

喷墨打印（IJP）被认为是质子交换膜（PEM）燃料电池中低成本和按需形成图案的一种有前途的灵活方法。尽管在喷墨打印电极方面取得了重大进展，但由于墨水特性的严格限制，确定最佳墨水配方仍具有挑战性。一般来说，使用低沸点溶剂（水/酒精）通过 IJP 制备的催化剂层具有合理的电化学性能。然而，由于溶剂在喷墨打印头中快速蒸发，低沸点溶剂会导致打印头喷嘴堵塞。本研究使用高沸点溶剂（丙二醇 (PG) 或乙二醇 (EG)）作为添加剂，以减少喷嘴堵塞并提高打印效率。在此背景下，研究了催化剂油墨特性、CL 微结构和 MEA 电化学性能之间的关系。结果表明，在油墨中添加高沸点溶剂可显著缩短印刷时间（30 wt% PG 可缩短 66.67 % 的时间）。然而，添加剂量的增加对电化学性能不利，因为会形成较大的团聚体，降低催化剂层的孔隙率，并降低 ECSA。这项工作的结果可用于制定一种策略，以调整使用 IJP 制备的电极的印刷时间和电化学性能之间的权衡。

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引用次数: 0

Electrolytic conversion of CO2 to proportionally tunable syngas using nickel-nitrogen doped carbon materials derived from Chlorella sp. 使用从小球藻提取的掺镍氮碳材料电解转化二氧化碳为比例可调的合成气

IF 5.5 3区材料科学 Q1 ELECTROCHEMISTRY

Electrochimica Acta

Pub Date : 2024-10-21 DOI: 10.1016/j.electacta.2024.145271

Ziwei Mei, Wei Liu, Wenxuan Zhou, Liang Li, Shiqi Chen, Siyu Xie, Xinle Liu, Siting Yang, Hong Tao

Chlorella sp., a common type of algae found in global surface waters, is prone to causing "blooms" and can accumulate significant amounts of nutrients such as nitrogen, phosphorus, and carbon. While carbon materials derived from Chlorella sp. are widely used in the field of adsorption, there are relatively few reports focused on electrocatalysis. This study utilized Chlorella sp. as a raw material to synthesize functional carbon materials, and prepared nitrogen-doped (CN), nickel-doped (CNi), and nitrogen-nickel co-doped (CNNi) carbon-based catalysts with both metal and non-metal elements. The results showed that the CN, CNi and CNNi catalysts possessed certain electrocatalytic properties, among which the CNNi material had the best electrocatalytic activity towards CO₂ reduction (CO₂RR). In 1.0 M KHCO_3, the CNNi catalyst exhibited an instantaneous current density of 15.4 mA/cm² under the potential of -0.82 V (vs. RHE). In terms of product selectivity, the Faraday efficiency of CO on the CNNi electrode was up to 90 % when the electrode potential was -0.62 V (vs. RHE), while the selectivity of the CN and CNi catalysts for CO was only 59 % under the optimal conditions. The co-doping of nitrogen and nickel significantly enhanced the electrocatalytic activity and the selectivity towards CO of Chlorella-based carbon materials.

小球藻是全球地表水中常见的一种藻类，容易引起 "水华"，并能积累大量营养物质，如氮、磷和碳。虽然从小球藻中提取的碳材料被广泛应用于吸附领域，但有关电催化的报道却相对较少。本研究以小球藻为原料合成功能碳材料，制备了掺氮 (CN)、掺镍 (CNi) 和掺氮镍共 (CNNi) 金属和非金属元素的碳基催化剂。结果表明，CN、CNi 和 CNNi 催化剂都具有一定的电催化特性，其中 CNNi 材料对二氧化碳还原（CO2RR）的电催化活性最好。在 1.0 M KHCO3 中，CNNi 催化剂在电位为 -0.82V 时的瞬时电流密度为 15.4 mA/cm2（相对于 RHE）。就产物选择性而言，当电极电位为 -0.62 V（相对于 RHE）时，CNNi 电极上 CO 的法拉第效率高达 90%，而在最佳条件下，CN 和 CNi 催化剂对 CO 的选择性仅为 59%。氮和镍的共掺杂显著提高了小球藻基碳材料的电催化活性和对 CO 的选择性。

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引用次数: 0

Intercalation of g-C3N4/Ag2S heterostructure on boronized Ni-MOF for enhanced water splitting and energy storage applications 在硼化 Ni-MOF 上夹杂 g-C3N4/Ag2S 异质结构以增强水分离和储能应用

IF 5.5 3区材料科学 Q1 ELECTROCHEMISTRY

Electrochimica Acta

Pub Date : 2024-10-20 DOI: 10.1016/j.electacta.2024.145258

G. John , T. Susikumar , M. Navaneethan , P. Justin Jesuraj

The increasing global demand for energy conversion and storage technologies including water electrolysis, fuel cells, batteries & supercapacitors depend critically on the performance of their electrode components. Metal Organic Frameworks (MOFs), particularly Nickel Zeolite Imidazole Frameworks (Ni-ZIF) have drawn significant attention due to their greater electrocatalytic performance. Still, their restricted active sites & stability hinder their broader implementation in alkaline/saline water electrolysis & supercapacitor applications. Here, we are reporting the intercalation of heterostructure consisting of silver sulfide (Ag₂S)/graphitic carbon nitride (g-C₃N₄) on Boronized Ni-ZIF (B:NZ) for empowered alkaline/saline water splitting and supercapacitor applications. These heterostructure addition over Boronized Ni-ZIF demonstrated minimal overpotentials for the oxygen evolution reaction (OER) (324 mV at 10.0 mA cm^-2) and the hydrogen evolution reaction (HER) (78 mV at 10.0 mA cm^-2) in alkaline medium (1 M KOH). The observed improvement in activity is ascribed to the decreased charge transfer resistance (R_ct) & the augmented electrochemical active surface area (ECSA). Furthermore, Ag₂S/g-C₃N₄/Boronized Ni-ZIF exhibited high specific capacitances of 1076.6 F/g and areal capacitance of 2584 F/cm² at 0.50 A g^-1 in supercapacitor applications. The incorporation of the g-C₃N₄ layer has enhanced the surface area and roughness facilitating stronger adhesion between hybrid layers which in turn resulted in prolonged stability exceeding 20 h in water splitting and 86 % retention in supercapacitor application.

全球对电解水、燃料电池、电池和超级电容器等能源转换和储存技术的需求日益增长，这主要取决于其电极元件的性能。金属有机框架（MOFs），尤其是镍沸石咪唑框架（Ni-ZIF）因其较高的电催化性能而备受关注。然而，它们有限的活性位点和稳定性阻碍了它们在碱性/盐水电解和超级电容器应用中的广泛应用。在此，我们报告了在硼化镍-ZIF（B:NZ）上插层硫化银（Ag2S）/石墨化氮化碳（g-C3N4）组成的异质结构，以增强碱性/盐水电解和超级电容器的应用。在碱性介质（1 M KOH）中，这些添加在硼化镍-ZIF 上的异质结构在氧进化反应（OER）（10.0 mA cm-2 时为 324 mV）和氢进化反应（HER）（10.0 mA cm-2 时为 78 mV）中的过电位极低。观察到的活性提高归因于电荷转移电阻（Rct）的降低和电化学活性表面积（ECSA）的增加。此外，在超级电容器应用中，Ag2S/g-C3N4/硼化镍-ZIF 在 0.50 A/g 时表现出 1076.6 F/g 的高比电容和 2584 F/cm2 的等面积电容。g-C3N4 层的加入增大了表面积和粗糙度，有利于增强混合层之间的粘合力，进而使其在分水应用中的稳定性超过 20 小时，在超级电容器应用中的保持率达到 86%。

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