Journal of Electroanalytical Chemistry最新文献

Heteroatom doped MoO3 as efficient electrocatalyst towards hydrogen evolution reaction in acidic as well as alkaline medium 掺杂杂原子的 MoO3 作为高效电催化剂在酸性和碱性介质中进行氢进化反应

IF 4.1 3区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Electroanalytical Chemistry

Pub Date : 2024-11-26 DOI: 10.1016/j.jelechem.2024.118827

Arti Maurya, Nidhi Pradhan, Mahendra Yadav

In general, slow kinetics and cost concern impede the development of electrocatalyst for water splitting. For practical application, the design and development of an inexpensive catalyst efficient towards hydrogen evolution reaction (HER) in acidic as well as alkaline medium is crucial. Here, Ruthenium (Ru) and MoO₃ alone are not efficient for HER in the alkaline medium but, Ni and Ru doped MoO₃ nanosphere shaped material (Ni-Ru-MoO₃₎ prepared by the facile two-step synthesis process, acts as efficient electrocatalyst towards HER in acidic as well as alkaline medium. The low cost of the prepared catalyst and comparable activity with costly noble metal catalyst is novelty of this work. Due to the synergistic effect of Ni and Ru doping on the MoO₃ and enhanced porosity Ni-Ru-MoO₃ acts as efficient catalyst. It merely requires 59 and 151 mV overpotential to reach 10 mA/cm² of current density and exhibits small Tafel slope values as 64 and 68 mV/dec for HER in 1 M KOH and 0.5 M H₂SO₄ solution, respectively, which are comparable to the respective values obtained for benchmark costly catalyst Pt/C. In addition, this catalyst shows remarkable stability even at high current density of 50 mA/cm² and time 24 h, low value of charge transfer resistance and high value of electrochemically active surface area, suggesting its substantial electronic conductivity and high electrocatalytic activity. This work presents a good strategy for tuning the electronic structure of MoO₃ to make it an efficient catalyst for HER by simply doping it with hetero elements.

一般来说，缓慢的动力学和成本问题阻碍了水分离电催化剂的开发。在实际应用中，设计和开发一种在酸性和碱性介质中都能有效进行氢进化反应（HER）的廉价催化剂至关重要。在这里，钌（Ru）和氧化钼（MoO3）本身在碱性介质中不能有效地进行氢进化反应，但通过简单的两步合成工艺制备的掺杂镍和钌的氧化钼（MoO3）纳米球状材料（Ni-Ru-MoO3）在酸性和碱性介质中均可作为高效的氢进化反应电催化剂。所制备的催化剂成本低廉，活性可与昂贵的贵金属催化剂媲美，这是该研究的新颖之处。由于 MoO3 上掺杂的 Ni 和 Ru 的协同效应以及 Ni-Ru-MoO3 孔隙率的提高，使其成为一种高效催化剂。它只需要 59 和 151 mV 的过电位就能达到 10 mA/cm2 的电流密度，并且在 1 M KOH 和 0.5 M H2SO4 溶液中对 HER 的 Tafel 斜坡值分别为 64 和 68 mV/dec，与基准昂贵催化剂 Pt/C 的相应值相当。此外，这种催化剂即使在 50 mA/cm2 的高电流密度和 24 小时的时间内也表现出显著的稳定性、低电荷转移电阻值和高电化学活性表面积值，这表明它具有很强的电子导电性和很高的电催化活性。这项研究提出了一种良好的策略，即通过简单地掺杂杂质元素来调整 MoO3 的电子结构，使其成为一种高效的 HER 催化剂。

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引用次数: 0

Tailoring Pd-Co/PPD/NS composite electrode for efficient electrocatalytic dechlorination of 4-chlorophenol 定制 Pd-Co/PPD/NS 复合电极，实现 4-氯苯酚的高效电催化脱氯

IF 4.1 3区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Electroanalytical Chemistry

Pub Date : 2024-11-24 DOI: 10.1016/j.jelechem.2024.118825

Yuanjie Liang , Xia Li , Qiang Xu , Zikang Hou

To address the challenges of slow bio-degradation and high toxicity of organic chlorophenols, some high-efficiency treatment strategies have been proposed. In this study, a high-performance palladium-cobalt/poly-(phenylenediamine)/nickel sponge (Pd-Co/PPD/NS) composite electrode was fabricated and utilized for electrocatalytic dechlorination of chlorophenol. Surface micromorphology, elemental distribution, and structural features of the electrodes were thoroughly investigated. Furthermore, effects of p-phenylenediamine concentration, chlorophenol concentration, cathode potential, and electrolyte content on electrocatalytic dechlorination efficiency were comprehensively studied. The presence of polyphenylene diamine greatly improved interfacial compatibility, thus promoting more Pd-Co particles deposition and creating additional catalytic active sites. Moreover, the larger conjugated structure in polyphenylene diamine facilitated electron transfer between electrode surface and electrolyte, resulting in high conductivity and substantially reducing charge transfer resistance. These enhancements greatly increased the electrocatalytic dechlorination efficiency. Under optimal reaction conditions, the dechlorination efficiency of the electrode reached 93.4 % with a mass activity of 25.3 min⁻¹g_pd⁻¹. Besides, the corresponding current efficiency also achieved about 24.6 %. Consequently, the Pd-Co/PPD/NS composite electrode we prepared also exhibited excellent recycling stability and high resistance to interference from negative ions.

为了解决有机氯酚生物降解慢、毒性大的难题，人们提出了一些高效处理策略。本研究制备了高性能钯钴/聚苯二胺/海绵镍（Pd-Co/PPD/NS）复合电极，并将其用于氯酚的电催化脱氯。对电极的表面微观形态、元素分布和结构特征进行了深入研究。此外，还全面研究了对苯二胺浓度、氯酚浓度、阴极电位和电解质含量对电催化脱氯效率的影响。聚对苯二胺的存在大大提高了界面相容性，从而促进了更多钯钴粒子的沉积，并创造了更多的催化活性位点。此外，聚苯二胺中较大的共轭结构促进了电极表面与电解质之间的电子转移，从而产生了较高的导电性，并大大降低了电荷转移电阻。这些改进大大提高了电催化脱氯效率。在最佳反应条件下，电极的脱氯效率达到 93.4%，质量活性为 25.3 min-1gpd-1。此外，相应的电流效率也达到了约 24.6%。因此，我们制备的 Pd-Co/PPD/NS 复合电极还具有出色的循环稳定性和较高的抗负离子干扰能力。

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引用次数: 0

Solvent effect on facile in situ precipitation of nickel–iron hydroxide for enhanced overall water splitting 溶剂对氢氧化镍-铁原位沉淀促进整体水分解的影响

IF 4.1 3区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Electroanalytical Chemistry

Pub Date : 2024-11-23 DOI: 10.1016/j.jelechem.2024.118826

Giljung Kim , Yujin Son , Yunji Jeong, Moonsu Kim, Gibaek Lee

Efficient and economical electrocatalysts are essential for addressing the high overpotential challenges of the oxygen evolution reaction (OER) in electrochemical water splitting. This study explores the synthesis of nickel–iron hydroxide (NiFeOH) catalysts via in situ precipitation, focusing on the impact of the solvent composition on the morphology and catalytic performance of the material. The volumetric ratio of H₂O to ethanol in the solvent mixture was systematically varied, revealing that higher proportions of H₂O promoted the formation of thicker and larger needle-like NiFeOH structures. In contrast with the common preference for thin needle-shaped morphologies, our findings reveal that these thicker structures exhibit superior electrocatalytic activity. This enhanced performance is attributed to the higher iron content and faster reaction kinetics promoted by the increased permittivity of water-rich environments. The optimized NiFeOH catalysts, particularly those with higher water content, exhibit excellent OER and hydrogen evolution reaction (HER) activities, achieving low overpotentials of 288 mV at 100 mA cm⁻² for OER and 131 mV at 10 mA cm⁻² for HER. Furthermore, long-term stability tests confirmed the robustness of the catalysts, with minimal morphological degradation and consistent performance in overall water splitting. This work highlights the significance of solvent effects in tailoring the morphology and catalytic properties of NiFeOH, providing valuable insights for the design of effective water-splitting electrocatalysts.

高效、经济的电催化剂是解决电化学水分解过程中析氧反应（OER）高过电位问题的关键。本研究探索了原位沉淀法合成氢氧化镍铁（NiFeOH）催化剂，重点研究了溶剂组成对材料形貌和催化性能的影响。溶剂混合物中H2O与乙醇的体积比有系统地变化，表明较高的H2O比例有利于形成更粗、更大的针状NiFeOH结构。与通常偏好的细针状结构相反，我们的研究结果表明，这些较厚的结构具有优越的电催化活性。这种增强的性能是由于富水环境中更高的铁含量和更高的介电常数促进的更快的反应动力学。优化后的NiFeOH催化剂，特别是高含水量的NiFeOH催化剂，表现出优异的OER和析氢反应（HER）活性，OER在100 mA cm−2时达到288 mV， HER在10 mA cm−2时达到131 mV。此外，长期稳定性测试证实了催化剂的稳健性，具有最小的形态降解和一致的整体水分解性能。这项工作强调了溶剂效应在调整NiFeOH的形态和催化性能方面的重要性，为设计有效的水分解电催化剂提供了有价值的见解。

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引用次数: 0

Enhancing catalytic efficiency: InSe quantum dots’ role in hydrogen evolution reaction 提高催化效率：铟硒量子点在氢进化反应中的作用

IF 4.1 3区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Electroanalytical Chemistry

Pub Date : 2024-11-21 DOI: 10.1016/j.jelechem.2024.118806

Mahmoud A.S. Sakr , Hazem Abdelsalam , Ghada M Abdelrazek , Nahed H. Teleb , Omar H. Abd-Elkader , Yushen Liu , Qinfang Zhang

This study investigates the structural, electronic, and adsorption properties of InSe quantum dots. We focus on hydrogen atom adsorption and its implications on quantum stability chemical parameters and the hydrogen evolution reaction (HER). Optimized structures reveal distinct atomic interactions post-H adsorption, affecting bond lengths, dihedral angles, and bond angles. Adsorption energies confirm spontaneous H-adsorption across various sites, highlighting preferences for specific interactions. Electronic properties analysis showcases significant shifts in energy levels, energy gaps, and chemical parameters following H-atom adsorption, indicating a transition towards more insulating states. The catalytic performance for HER is assessed through calculated free energy changes (ΔG), demonstrating superior catalytic activity. Comparison with a Pt catalyst underscores the potential of these quantum dots as efficient HER catalysts. For instance, the ΔG value decreases to 0.005 eV in InSe-quantum dots passivated with F- and H-atoms at the edges. These findings contribute to understanding the role of InSe quantum dots in enhancing the HER reaction, offering insights for potential application in electrocatalysis and energy conversion.

本研究探讨了 InSe 量子点的结构、电子和吸附特性。我们重点关注氢原子吸附及其对量子稳定性化学参数和氢进化反应（HER）的影响。优化后的结构揭示了氢吸附后独特的原子相互作用，影响了键长、二面角和键角。吸附能证实了不同位点的自发氢吸附，突出了对特定相互作用的偏好。电子特性分析表明，H 原子吸附后，能级、能隙和化学参数发生了显著变化，表明向更绝缘的状态过渡。通过计算自由能变化 (ΔG)，对 HER 的催化性能进行了评估，结果表明该催化剂具有卓越的催化活性。与铂催化剂的比较凸显了这些量子点作为高效 HER 催化剂的潜力。例如，在边缘用 F 原子和 H 原子钝化的 InSe 量子点中，ΔG 值降至 0.005 eV。这些发现有助于理解 InSe 量子点在增强 HER 反应中的作用，为其在电催化和能量转换中的潜在应用提供了启示。

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引用次数: 0

Developing efficient anodic electrocatalyst: Three-dimensional interconnected network of bimetallic Pd–Ni aerogel for advanced electrocatalysis of ethanol 开发高效阳极电催化剂：用于乙醇高级电催化的双金属钯镍气凝胶三维互连网络

IF 4.1 3区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Electroanalytical Chemistry

Pub Date : 2024-11-21 DOI: 10.1016/j.jelechem.2024.118810

Masoud Rafigh Esmaeilzaei, Hamideh Saravani, Ahmad Reza Abbasian

This paper introduces a valuable and easy strategy for connecting metallic nanoparticles to assemble a three-dimensional (3D) network of bimetallic palladium-nickel aerogel. This research provides several unique advantages (e.g., facile, surfactant-free, one-pot, and fast) without any chemical destabilizer compounds. The 3D metallic superstructure is formed during the reduction of Ni²⁺ and Pd²⁺ ions by adding NaBH₄, followed by CO₂ supercritical drying. Additionally, the gelation kinetics are explored by raising the temperature to create an efficient anisotropic atmosphere to assemble the 3D Pd-Ni hydrogels. This study demonstrated that the alteration in anisotropic conditions affects the formation of a 3D hydrogel. The production of a 3D network assembled by the extended nanowires with high porosity and plenty of open pores is confirmed by various analyses. The Pd-Ni aerogel is employed as a self-supported electrocatalyst for decomposing EtOH fuel and reflects the more prominent electrocatalytic activity relative to Pd/C. The existence of nickel will facilitate the adsorption of hydroxyl groups on the surface of the resulting aerogel. These adsorbed hydroxyls react with the generated intermediates and release the blocked active sites by carbonaceous intermediates, thereby affecting efficiently the ethanol oxidation.

本文介绍了一种既有价值又简便的金属纳米粒子连接策略，用于组装双金属钯镍气凝胶三维（3D）网络。这项研究具有一些独特的优势（如简便、无表面活性剂、一锅制、快速），且不含任何化学失稳化合物。在加入 NaBH4 还原 Ni2+ 和 Pd2+ 离子的过程中形成三维金属上层结构，然后进行二氧化碳超临界干燥。此外，还通过升高温度探索了凝胶化动力学，以创造一种高效的各向异性气氛来组装三维钯镍水凝胶。这项研究表明，各向异性条件的改变会影响三维水凝胶的形成。各种分析证实，延伸纳米线组装的三维网络具有高孔隙率和大量开放孔隙。钯镍气凝胶被用作分解乙醇燃料的自支撑电催化剂，与钯/镍相比，其电催化活性更为突出。镍的存在将促进羟基在气凝胶表面的吸附。这些被吸附的羟基会与生成的中间产物发生反应，释放被碳质中间产物阻塞的活性位点，从而有效地影响乙醇氧化。

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引用次数: 0

Chemically grown Bi2MoX6 (X = O, S, and Se) nanostructures for efficient electrochemical hydrogen evolution reaction 用于高效电化学氢进化反应的化学生长 Bi2MoX6（X = O、S 和 Se）纳米结构

IF 4.1 3区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Electroanalytical Chemistry

Pub Date : 2024-11-20 DOI: 10.1016/j.jelechem.2024.118823

Sandesh H. Narwade , Balaji G. Ghule , Nanasaheb M. Shinde , Rushikesh R. Suryawanshi , Kyeongnam Kang , Ji-Hyun Jang , Arvind H. Jadhav , Rajaram S. Mane

Here, we present the fabrication of an effective and chemical bath deposition (CBD) of Bi₂MoX₆ (X = O, S, and Se) electrocatalyst for efficient electrochemical hydrogen evolution reaction (HER) activity. To enhance the electrochemical activity of Bi₂MoO₆ (BMO) electrode, the influence of sulfurization and selenization on the wet chemically synthesized BMO has been extensively studied here. These BMO, Bi₂MoS₆ (BMS), and Bi₂MoSe₆ (BMSe) nanostructured developed on nickel-foam are synthesized by a mild two-stage reaction process; a CBD following a sulfo-selenization procedure on BMO. Compared to BMO and BMS electrocatalysts, the BMSe has shown a higher HER activity through a lower overpotential about 120 mV at 10 mA cm⁻² and a lower value of Tafel slope (57 mV dec⁻¹). Surface morphology analysis endows hydrangea flower-type petals, nanosheets, and E. coli bacteria-type surface morphologies for BMO, BMS, and BMSe electrocatalysts, respectively. Thus, this article gives an easy tactic for enhancing the electrochemical HER activity of the BMO through the process of sulfurization/selenization at room temperature (25–27 °C).

在此，我们介绍了一种有效的化学浴沉积（CBD）Bi2MoX6（X = O、S 和 Se）电催化剂的制备方法，以实现高效的电化学氢进化反应（HER）活性。为了提高 Bi2MoO6（BMO）电极的电化学活性，本文广泛研究了硫化和硒化对湿化学合成 BMO 的影响。这些在镍泡沫上开发的 BMO、Bi2MoS6 (BMS) 和 Bi2MoSe6 (BMSe) 纳米结构是通过温和的两阶段反应过程合成的；在 BMO 的硫化-硒化过程之后是 CBD。与 BMO 和 BMS 电催化剂相比，BMSe 具有更高的 HER 活性，在 10 mA cm-2 时过电位更低，约为 120 mV，塔菲尔斜率值（57 mV dec-1）也更低。通过表面形态分析，BMO、BMS 和 BMSe 电催化剂分别呈现出绣球花型花瓣、纳米片和大肠杆菌型表面形态。因此，本文给出了在室温（25-27 °C）下通过硫化/软化过程提高 BMO 的电化学 HER 活性的简便方法。

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引用次数: 0

Low-Cost and Eco-Friendly method for activating carbon felt using hypochlorite for electrochemical applications 在电化学应用中使用次氯酸盐活化碳毡的低成本环保方法

IF 4.1 3区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Electroanalytical Chemistry

Pub Date : 2024-11-19 DOI: 10.1016/j.jelechem.2024.118816

Branimir N. Grgur , Vuk V. Radmilović , Houcheng Zhang , Lazar Rakočević , Aleksandra S. Popović

Pristine carbon felt is activated and functionalized through a cost-effective, eco-friendly method by immersion in a commercial 5 wt% hypochlorite solution. Electrochemical analyses, including cyclic voltammetry, galvanostatic charge–discharge tests, capacitance, and impedance measurements at 1 Hz, reveal that the activated carbon felt exhibits a twenty-fold enhancement in performance compared to its pristine counterpart. Pristine and activated carbon felt are characterized using scanning electron microscopy, X-ray photoelectron spectroscopy, contact angle measurement, and water uptake tests confirming the significant changes in material properties. To further validate the activation process, polypyrrole is galvanostatically electrodeposited on both pristine and activated carbon felts, with their electrochemical behaviors serving as a model system. The findings indicate a substantial improvement of activated carbon felt, with fourth times increase in capacity, highlighting the potential for advanced applications.

通过将原始碳毡浸泡在 5 wt% 的商用次氯酸盐溶液中，采用一种具有成本效益的环保方法对其进行活化和功能化。电化学分析（包括循环伏安法、电静态充放电试验、电容和 1 Hz 阻抗测量）表明，与原始碳毡相比，活化碳毡的性能提高了 20 倍。使用扫描电子显微镜、X 射线光电子能谱、接触角测量和吸水测试对原始碳毡和活性碳毡进行了表征，证实了材料性能的显著变化。为了进一步验证活化过程，在原始碳毡和活化碳毡上对聚吡咯进行了静电电沉积，并将它们的电化学行为作为模型系统。研究结果表明，活性碳毡的性能有了大幅提高，容量增加了四倍，这凸显了其在先进应用领域的潜力。

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引用次数: 0

Microwave-Assisted synthesis of interconnected holey nanosheets of zinc vanadate for High-Performance supercapacitor 微波辅助合成用于高性能超级电容器的孔状钒酸锌纳米片

IF 4.1 3区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Electroanalytical Chemistry

Pub Date : 2024-11-19 DOI: 10.1016/j.jelechem.2024.118809

A.T. Avatare , R.S. Redekar , J.L. Chouhan , Sunny Yadav , I.H. Lee , S.B. Patil , N.L. Tarwal

Developing electrode materials with high energy density and cyclic stability is crucial for advanced supercapacitor (SC) devices in the field of green energy technologies. However, the choice of electrode material and its synthesis approaches significantly impact the electrochemical performance of these devices. In this study, the effect of microwave power on the synthesis process, physicochemical properties and electrochemical performance of zinc vanadate (ZVO) is investigated. The interconnected “holey” ZVO nanosheets are synthesized using a microwave-assisted chemical synthesis process with different microwave powers with shorter reaction time (3 min). X-ray diffraction confirmed that the synthesized ZVO has an orthorhombic crystal structure. At lower microwave power (450 W), interconnected holey nanosheets are observed. When the power is increased above 450 W, the nanosheets disintegrated into an interconnected network of nanopebbles. The ZVO nanosheet electrode showed a specific capacity of 145.16 mAh/g and a specific capacitance of 871.01 F/g at 5 A/g, with a capacity retention of 96% after 5000 cycles. Furthermore, an aqueous asymmetric hybrid supercapacitor (AHSC) device with ZVO-1//AC configuration achieved a specific energy density of 32.77 W/kg at a power density of 400 W/kg with a capacity retention of 82.8% after 2000 cycles. These findings strongly indicate that the developed ZVO holey nanosheets can be used as a potential electrode material for high-performance SC devices.

开发具有高能量密度和循环稳定性的电极材料对于绿色能源技术领域的先进超级电容器（SC）设备至关重要。然而，电极材料的选择及其合成方法会对这些设备的电化学性能产生重大影响。本研究探讨了微波功率对钒酸锌（ZVO）的合成过程、理化性质和电化学性能的影响。采用微波辅助化学合成工艺，在较短的反应时间（3 分钟）和不同的微波功率下合成了相互连接的 "孔状 "ZVO 纳米片。X 射线衍射证实合成的 ZVO 具有正方晶系结构。在较低的微波功率（450 W）下，可以观察到相互连接的孔状纳米片。当功率增加到 450 W 以上时，纳米片瓦解成相互连接的纳米卵石网络。在 5 A/g 条件下，ZVO 纳米片电极的比容量为 145.16 mAh/g，比电容为 871.01 F/g，循环 5000 次后容量保持率为 96%。此外，采用 ZVO-1//AC 配置的水基非对称混合超级电容器（AHSC）装置在功率密度为 400 W/kg 时的比能量密度达到了 32.77 W/kg，循环 2000 次后容量保持率为 82.8%。这些发现有力地表明，所开发的 ZVO 孔状纳米片可用作高性能 SC 器件的潜在电极材料。

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引用次数: 0

Beneficial surface defect engineering of MoS2 electrocatalyst for efficient hydrogen evolution reaction 有利于高效氢进化反应的 MoS2 电催化剂表面缺陷工程

IF 4.1 3区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Electroanalytical Chemistry

Pub Date : 2024-11-19 DOI: 10.1016/j.jelechem.2024.118814

Jyoti Ganapati Badiger , Maheswari Arunachalam , Rohini Subhash Kanase , Suzan Abdelfattah Sayed , Kwang-Soon Ahn , Soon Hyung Kang

Hydrogen evolution reaction (HER) is considered the most efficient method for hydrogen production using an effective electrocatalyst. Molybdenum disulfide (MoS₂), with its unique 2D layered structure, is the most promising electrocatalyst. This is attributed to its flexibility, which facilitates the exploration of various MoS₂ phases and properties, closely mirroring those of platinum, particularly its Gibbs energy (ΔG_{H* ̃} 0.08 eV), which makes MoS₂ an excellent electrocatalyst. However, its low electrical conductivity and inert basal planes limit its effectiveness for HER. This study utilized a facile hot-gun approach to successfully introduce sulfur vacancies, simultaneously incorporating oxygen from the air, which partially occupied these vacancies. This process resulted in the formation of an intermediate MoO_xS_y interlayer, yielding a highly effective electrocatalyst. Exposure to the hot gun for a short duration led to several changes, notably expanding the interlayer spacing and altering the atomic S:O ratio from approximately 75 % to 57 %, primarily affecting the MoS₂ structure. The optimal duration for hot-gun treatment was determined to be 30 s, enhancing electrochemical activity for HER, with an overpotential of 486 mV vs. RHE (briefly marked as V_RHE) at a current density of 10 mA·cm⁻² and Tafel slope of 224 mV·dec^-1. The improvement in basal active sites, attributable to the formation of defects from sulfur vacancies and partial passivation by oxygen at these sites, was identified as the key factor for this enhanced performance.

氢进化反应（HER）被认为是使用有效电催化剂制氢的最有效方法。二硫化钼（MoS2）具有独特的二维层状结构，是最有前途的电催化剂。这要归功于它的灵活性，这种灵活性有助于探索 MoS2 的各种相态和特性，这些相态和特性与铂的相态和特性密切相关，特别是它的吉布斯能（ΔGH* ̃ 0.08 eV），这使得 MoS2 成为一种极佳的电催化剂。然而，MoS2 的低导电性和惰性基底面限制了其在 HER 方面的有效性。本研究利用简便的热枪方法成功引入了硫空位，同时从空气中引入了氧，部分占据了这些空位。这一过程形成了中间的 MoOxSy 夹层，产生了一种高效的电催化剂。短时间暴露在热风枪下会导致几种变化，特别是扩大层间间距和改变原子 S:O 比率，从大约 75% 降至 57%，主要影响 MoS2 结构。热枪处理的最佳持续时间为 30 秒，可提高 HER 的电化学活性，在电流密度为 10 mA-cm-2、塔菲尔斜率为 224 mV-dec-1 时，相对于 RHE 的过电位为 486 mV（简要标记为 VRHE）。基底活性位点的改善被认为是性能提高的关键因素，这归因于硫空位形成的缺陷以及这些位点上氧的部分钝化。

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引用次数: 0

Functional Au@Cu/Cu2O/C composites derived from 2D Cu-based metal–organic framework for sensitive label-free electrochemical immunoassay 源自二维铜基金属有机框架的功能性 Au@Cu/Cu2O/C 复合材料用于灵敏的无标记电化学免疫分析

IF 4.1 3区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Electroanalytical Chemistry

Pub Date : 2024-11-19 DOI: 10.1016/j.jelechem.2024.118815

Baojun Han , Shuqin Fang , Yu Wang, Jiajun Ma, Jinling Wu, Xiaoming Ma, Qingchun Lan

Metal-organic frameworks (MOFs) face challenges in electrochemical sensing due to low conductivity and poor stability. Herein, we report the synthesis of MOFs-derived metal/carbon composites (Au@Cu/Cu₂O/C) that exhibit synergistic effects by combining metallic and carbonaceous characteristics due to their hierarchical structures and metal contents. The Au@Cu/Cu₂O/C composites were characterized using electron microscopy, X-ray diffraction, Raman spectroscopy, and X-ray photoelectron spectroscopy. These composites inherit the exceptional properties of the pristine MOFs while exhibiting a large specific surface area, high electrical conductivity and stability. As an excellent electrode material, the Au@Cu/Cu₂O/C composites were biofunctionalized with streptavidin and a biotinylated antibody for use as a highly sensitive, label-free electrochemical immunosensor for the detection of the tumor marker prostate specific antigen (PSA). The fabricated immunosensor successfully detected PSA concentrations ranging from 0.05 to 60 ng/mL, with a detection limit of 0.01 ng/mL, showcasing high sensitivity comparable to other existing methods. This research provides a versatile and promising platform for developing advanced biosensors for disease diagnostics and further expanding the application of MOFs.

金属有机框架（MOFs）由于电导率低、稳定性差，在电化学传感领域面临挑战。在此，我们报告了由 MOFs 衍生的金属/碳复合材料（Au@Cu/Cu2O/C）的合成过程，由于其分层结构和金属含量，这些复合材料结合了金属和碳的特性，从而表现出协同效应。利用电子显微镜、X 射线衍射、拉曼光谱和 X 射线光电子能谱对 Au@Cu/Cu2O/C 复合材料进行了表征。这些复合材料继承了原始 MOFs 的优异特性，同时具有大比表面积、高导电性和稳定性。作为一种优良的电极材料，Au@Cu/Cu2O/C 复合材料与链霉亲和素和生物素化抗体进行了生物功能化，可用作一种高灵敏度、无标记的电化学免疫传感器，用于检测肿瘤标志物前列腺特异性抗原（PSA）。制备的免疫传感器成功检测了 0.05 至 60 纳克/毫升的前列腺特异性抗原浓度，检测限为 0.01 纳克/毫升，显示出与其他现有方法相当的高灵敏度。这项研究为开发用于疾病诊断的先进生物传感器提供了一个多功能且前景广阔的平台，并进一步拓展了 MOFs 的应用领域。

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引用次数: 0