Pub Date : 2025-11-07DOI: 10.1016/j.jelechem.2025.119638
Zhen Guan , Yu Zhong , Lingchen Kong , Bin Chen , Wenjie Li , Zhou Shi , Rui Zhang , Jiang Wu , Zaiguo Fu
The Earth's plentiful seawater resources make direct seawater electrolysis for hydrogen generation an optimal approach to realize large-scale industrial hydrogen production. Nevertheless, the presence of complex organic compounds in seawater leads to not just competitive chlorine evolution reactions (ClER) induced by chloride ions during electrolysis, but also catalyst corrosion due to high chloride ion concentrations. These many problems have restricted the large-scale and efficient decomposition of seawater for hydrogen production. The development of cost-effective electrocatalysts exhibiting exceptional activity, long-term stability, and excellent corrosion resistance is crucial for realizing sustainable large-scale hydrogen generation. In this context, transition metal-based catalysts have gained significant research attention for water electrolysis applications due to their outstanding catalytic performance and operational robustness. This review initially clarifies the basic principles of seawater electrolysis, followed by a comprehensive analysis of recent progress in transition metal electrocatalysts for marine water splitting. The work further identifies key challenges in seawater electrolysis processes, proposes mitigation strategies, and concludes with future perspectives on electrocatalytic seawater splitting for hydrogen generation.
{"title":"Research progress and prospects of electrocatalytic seawater electrolysis for hydrogen production","authors":"Zhen Guan , Yu Zhong , Lingchen Kong , Bin Chen , Wenjie Li , Zhou Shi , Rui Zhang , Jiang Wu , Zaiguo Fu","doi":"10.1016/j.jelechem.2025.119638","DOIUrl":"10.1016/j.jelechem.2025.119638","url":null,"abstract":"<div><div>The Earth's plentiful seawater resources make direct seawater electrolysis for hydrogen generation an optimal approach to realize large-scale industrial hydrogen production. Nevertheless, the presence of complex organic compounds in seawater leads to not just competitive chlorine evolution reactions (ClER) induced by chloride ions during electrolysis, but also catalyst corrosion due to high chloride ion concentrations. These many problems have restricted the large-scale and efficient decomposition of seawater for hydrogen production. The development of cost-effective electrocatalysts exhibiting exceptional activity, long-term stability, and excellent corrosion resistance is crucial for realizing sustainable large-scale hydrogen generation. In this context, transition metal-based catalysts have gained significant research attention for water electrolysis applications due to their outstanding catalytic performance and operational robustness. This review initially clarifies the basic principles of seawater electrolysis, followed by a comprehensive analysis of recent progress in transition metal electrocatalysts for marine water splitting. The work further identifies key challenges in seawater electrolysis processes, proposes mitigation strategies, and concludes with future perspectives on electrocatalytic seawater splitting for hydrogen generation.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"1000 ","pages":"Article 119638"},"PeriodicalIF":4.1,"publicationDate":"2025-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145526677","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-11-07DOI: 10.1016/j.jelechem.2025.119643
Muhammad Ishfaq Ghori , Dure Najaf Iqbal , Muhammad Fahad Saeed , Aleeza Sattar , Syed Imran Abbas Shah , Nadeem Raza , Anis Ahmad Chaudhary , Muhammad Naeem Ashiq
The escalating global energy demands necessitate pursuit of next-generation and sustainable energy storage solutions. Supercapacitors are increasingly being researched due to their short charge-discharge time and prolonged cycling life. Halide perovskites' outstanding electrochemical versatility is significant in overcoming current energy storage problems, especially when utilized as a supercapacitor electrode. This paper reports design and evaluation of novel Alkali-transition metal-based Perovskite halide (NaCoCl3) composite with biochar. This heterogeneous structure combines Faradaic behavior of NaCoCl3 with conductive and high-surfaced biochar matrix to overcome shortcomings of pristine materials. Electrochemical analysis such as cyclic voltammetry (CV) reveals pseudocapacitive characteristics of produced materials. GCD analysis shows that nanocomposite exhibit a superior specific capacitance (Csp) 705.1 F g−1, specific power (225 W kg−1) and specific energy (19.8 Wh kg−1) at 1 A g−1 current density. EIS investigation corroborated these findings, whereby Nyquist plot indicated a narrower semicircle, signifying a reduced resistance to charge transfer (2 Ω) of NaCoCl3/biochar nanocomposite. Moreover, Chronoamperometric analysis showed steady current density of 201 mA cm−2 during a 50-h time. The findings suggest that halide perovskite compound (NaCoCl3/biochar) has great potential in development of energy storage systems, especially in formation of high-performance supercapacitors.
不断增长的全球能源需求使下一代可持续能源存储解决方案成为必要。超级电容器因其充放电时间短、循环寿命长而受到越来越多的研究。卤化物钙钛矿突出的电化学通用性对于克服当前的能量存储问题具有重要意义,特别是当用作超级电容器电极时。本文报道了新型碱过渡金属钙钛矿卤化物(NaCoCl3)与生物炭复合材料的设计与评价。这种非均相结构结合了NaCoCl3的法拉第性质和导电的高表面生物炭基质,克服了原始材料的缺点。循环伏安法(CV)等电化学分析揭示了所制备材料的赝电容特性。GCD分析表明,在1 a g−1电流密度下,纳米复合材料具有优异的比电容(Csp) 705.1 F g−1,比功率(225 W kg−1)和比能量(19.8 Wh kg−1)。EIS研究证实了这些发现,Nyquist图显示一个更窄的半圆,表明NaCoCl3/生物炭纳米复合材料的电荷转移阻力降低(2 Ω)。此外,计时安培分析显示,在50小时的时间内,电流密度稳定在201 mA cm−2。研究结果表明,卤化物钙钛矿化合物(NaCoCl3/生物炭)在储能系统,特别是高性能超级电容器的形成方面具有很大的发展潜力。
{"title":"Perovskite halide (NaCoCl3)/biochar composite for energy storage applications","authors":"Muhammad Ishfaq Ghori , Dure Najaf Iqbal , Muhammad Fahad Saeed , Aleeza Sattar , Syed Imran Abbas Shah , Nadeem Raza , Anis Ahmad Chaudhary , Muhammad Naeem Ashiq","doi":"10.1016/j.jelechem.2025.119643","DOIUrl":"10.1016/j.jelechem.2025.119643","url":null,"abstract":"<div><div>The escalating global energy demands necessitate pursuit of next-generation and sustainable energy storage solutions. Supercapacitors are increasingly being researched due to their short charge-discharge time and prolonged cycling life. Halide perovskites' outstanding electrochemical versatility is significant in overcoming current energy storage problems, especially when utilized as a supercapacitor electrode. This paper reports design and evaluation of novel Alkali-transition metal-based Perovskite halide (NaCoCl<sub>3</sub>) composite with biochar. This heterogeneous structure combines Faradaic behavior of NaCoCl<sub>3</sub> with conductive and high-surfaced biochar matrix to overcome shortcomings of pristine materials. Electrochemical analysis such as cyclic voltammetry (CV) reveals pseudocapacitive characteristics of produced materials. GCD analysis shows that nanocomposite exhibit a superior specific capacitance (Csp) 705.1 F g<sup>−1</sup>, specific power (225 W kg<sup>−1</sup>) and specific energy (19.8 Wh kg<sup>−1</sup>) at 1 A g<sup>−1</sup> current density. EIS investigation corroborated these findings, whereby Nyquist plot indicated a narrower semicircle, signifying a reduced resistance to charge transfer (2 Ω) of NaCoCl<sub>3</sub>/biochar nanocomposite. Moreover, Chronoamperometric analysis showed steady current density of 201 mA cm<sup>−2</sup> during a 50-h time. The findings suggest that halide perovskite compound (NaCoCl<sub>3</sub>/biochar) has great potential in development of energy storage systems, especially in formation of high-performance supercapacitors.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"1000 ","pages":"Article 119643"},"PeriodicalIF":4.1,"publicationDate":"2025-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145526742","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Developing highly efficient, stable, non-noble, environment-friendly, and inexpensive research on the conversion and storage of renewable energy heavily relies on electrocatalysts. The oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER) extant substantial challenges. Herein, we efficiently developed zinc oxide (ZnO) nanoparticles as electrocatalysts by using plant extract. Green synthesis is a sustainable technique due to its benefits, ease of manufacturing, eco-friendly nature, and low cost. An efficient, sustainable green synthesis of zinc oxide material has been developed, using organic compounds of Andrographis echioides (L.f.) Nees leaves. The produced electrocatalyst materials were examined using X-ray diffraction (XRD) and Field-Emission Scanning Electron Microscopy (FESEM) techniques. As the pH value increases the shape of the synthesized materials also changes. ZnO electrocatalyst (pH -12) demonstrated better OER and HER catalytic activity with overpotential performance of 197 and 307 mV, respectively, at a current density of ±10 mA/cm2 in 1 M KOH. Furthermore, the ZnO electrocatalyst demonstrated a robust kinetic response with 24-h cycle stabilities at ±10 mA/cm2 constant current densities, according to the chronopotentiometry (CP) data for OER and HER. This work presents a new technique for creating non-noble catalyst materials with high OER and HER activity for the production of oxygen and hydrogen.
开展高效、稳定、非贵金属、环保、廉价的可再生能源转化和储存研究,在很大程度上依赖于电催化剂。析氧反应(OER)和析氢反应(HER)存在很大的挑战。本文以植物提取物为原料,制备了氧化锌纳米颗粒作为电催化剂。绿色合成是一种可持续发展的技术,因为它的优点,易于制造,生态友好的性质,和低成本。利用穿心莲的有机化合物,开发了一种高效、可持续的绿色合成氧化锌材料。需要雇树叶。采用x射线衍射(XRD)和场发射扫描电镜(FESEM)技术对制备的电催化剂材料进行了表征。随着pH值的增加,合成材料的形状也发生了变化。ZnO电催化剂(pH -12)在1 M KOH电流密度为±10 mA/cm2时表现出较好的OER和HER催化活性,过电位性能分别为197和307 mV。此外,根据OER和HER的时间电位(CP)数据,ZnO电催化剂在±10 mA/cm2恒定电流密度下表现出强大的动力学响应,具有24小时循环稳定性。本文提出了一种制备具有高OER和HER活性的非贵金属催化剂材料的新技术,用于生产氧和氢。
{"title":"Bio-derived zinc oxide nanorod architectures as a bifunctional electrocatalyst for the oxygen evolution reaction and hydrogen evolution reaction","authors":"Meenakshamma Ambapuram , Obula Reddy Ankinapalli , Ramakrishna Reddy Ayyaluri , Phaneendra Reddy Guddeti , Kavyashree Nagappa Kummur , Supriya Athuru , Vasudeva Reddy Minnam Reddy","doi":"10.1016/j.jelechem.2025.119637","DOIUrl":"10.1016/j.jelechem.2025.119637","url":null,"abstract":"<div><div>Developing highly efficient, stable, non-noble, environment-friendly, and inexpensive research on the conversion and storage of renewable energy heavily relies on electrocatalysts. The oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER) extant substantial challenges. Herein, we efficiently developed zinc oxide (ZnO) nanoparticles as electrocatalysts by using plant extract. Green synthesis is a sustainable technique due to its benefits, ease of manufacturing, eco-friendly nature, and low cost. An efficient, sustainable green synthesis of zinc oxide material has been developed, using organic compounds of <em>Andrographis echioides</em> (L.f.) Nees leaves. The produced electrocatalyst materials were examined using X-ray diffraction (XRD) and Field-Emission Scanning Electron Microscopy (FESEM) techniques. As the pH value increases the shape of the synthesized materials also changes. ZnO electrocatalyst (pH -12) demonstrated better OER and HER catalytic activity with overpotential performance of 197 and 307 mV, respectively, at a current density of ±10 mA/cm<sup>2</sup> in 1 M KOH. Furthermore, the ZnO electrocatalyst demonstrated a robust kinetic response with 24-h cycle stabilities at ±10 mA/cm<sup>2</sup> constant current densities, according to the chronopotentiometry (CP) data for OER and HER. This work presents a new technique for creating non-noble catalyst materials with high OER and HER activity for the production of oxygen and hydrogen.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"1000 ","pages":"Article 119637"},"PeriodicalIF":4.1,"publicationDate":"2025-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145576685","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-11-07DOI: 10.1016/j.jelechem.2025.119640
Amir Hatamie , Saba Mohammadlou , Shima Kamran Haghighi , Shohreh Madani , Shayan Angizi
In modern analytical science, the development of low-cost, simple, and rapid detection tools is advancing quickly, particularly in the field of clinical diagnostics. In this study, we introduce a miniaturized user-friendly, and wearable ring-based voltammetric sensor for the detection of nitrite ions (NO2−)—a key biomarker used to diagnose urinary tract infections (UTIs), which are common bacterial infections of the urinary system. The miniaturized electrochemical cell was developed by integrating nanoelectronics with wearable accessory design. First, a simple nano-ink was synthesized by mixing graphite, copper nanoparticles (average diameter: 40 ± 20 nm), and nail polish, which serves as an effective binder and film-forming agent. This ink was used to fabricate film electrodes, combining both working and reference electrodes, on paper strips. These strips were then inserted into a newly designed hollow ring, forming a compact electrochemical cell suitable for on-site analysis. A key feature of this design is the replaceable electrode system, allowing for easy maintenance and extended usability. The “lab-on-a-ring” device can be connected to a portable potentiostat for nitrite sensing. It requires only a microsample of urine or other fluids (approximately 5.0–100.0 μL) and demonstrated detection ranges of 3.0–66.7 μM and 66.7–130.0 μM, with a detection limit as low as 1.53 μM. Additionally, the mini-sensor exhibited acceptable repeatability and precision, with a relative standard deviation (RSD) of approximately 8.6 % (n = 8), good stability after 20 repeated continuous nitrite measurements, the sensor exhibited approximately 3.66 % error, and showed satisfactory performance in real urine sample analysis within just a few minutes (around 4 min). Moreover, the sensor's response was confirmed by parallel measurements using a gold electrode, with a confidence level of 95 %. In conclusion, by merging nano-ink technology with wearable design, this new sensor is significantly faster than conventional clinical methods such as traditional urine culture, which can take several days. The wearable sensor provides rapid results, simplifying and accelerating the diagnostic process. Furthermore, beyond clinical diagnostics, this nitrite mini-sensor is inexpensive (approximately $4), lightweight, and well-suited for on-site analysis. It holds strong potential for broader applications in chemical monitoring, including environmental, forensic, and military settings, offering a promising alternative to conventional analytical instruments.
{"title":"Nanoelectronic accessory integration: A finger-worn wearable platform for rapid nitrite detection","authors":"Amir Hatamie , Saba Mohammadlou , Shima Kamran Haghighi , Shohreh Madani , Shayan Angizi","doi":"10.1016/j.jelechem.2025.119640","DOIUrl":"10.1016/j.jelechem.2025.119640","url":null,"abstract":"<div><div>In modern analytical science, the development of low-cost, simple, and rapid detection tools is advancing quickly, particularly in the field of clinical diagnostics. In this study, we introduce a miniaturized user-friendly, and wearable ring-based voltammetric sensor for the detection of nitrite ions (NO<sub>2</sub><sup>−</sup>)—a key biomarker used to diagnose urinary tract infections (UTIs), which are common bacterial infections of the urinary system. The miniaturized electrochemical cell was developed by integrating nanoelectronics with wearable accessory design. First, a simple nano-ink was synthesized by mixing graphite, copper nanoparticles (average diameter: 40 ± 20 nm), and nail polish, which serves as an effective binder and film-forming agent. This ink was used to fabricate film electrodes, combining both working and reference electrodes, on paper strips. These strips were then inserted into a newly designed hollow ring, forming a compact electrochemical cell suitable for on-site analysis. A key feature of this design is the replaceable electrode system, allowing for easy maintenance and extended usability. The “lab-on-a-ring” device can be connected to a portable potentiostat for nitrite sensing. It requires only a microsample of urine or other fluids (approximately 5.0–100.0 μL) and demonstrated detection ranges of 3.0–66.7 μM and 66.7–130.0 μM, with a detection limit as low as 1.53 μM. Additionally, the mini-sensor exhibited acceptable repeatability and precision, with a relative standard deviation (RSD) of approximately 8.6 % (<em>n</em> = 8), good stability after 20 repeated continuous nitrite measurements, the sensor exhibited approximately 3.66 % error, and showed satisfactory performance in real urine sample analysis within just a few minutes (around 4 min). Moreover, the sensor's response was confirmed by parallel measurements using a gold electrode, with a confidence level of 95 %. In conclusion, by merging nano-ink technology with wearable design, this new sensor is significantly faster than conventional clinical methods such as traditional urine culture, which can take several days. The wearable sensor provides rapid results, simplifying and accelerating the diagnostic process. Furthermore, beyond clinical diagnostics, this nitrite mini-sensor is inexpensive (approximately $4), lightweight, and well-suited for on-site analysis. It holds strong potential for broader applications in chemical monitoring, including environmental, forensic, and military settings, offering a promising alternative to conventional analytical instruments.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"1000 ","pages":"Article 119640"},"PeriodicalIF":4.1,"publicationDate":"2025-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145463962","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-11-07DOI: 10.1016/j.jelechem.2025.119639
Sajeeda Shaikh , Sarfaraz Kamangar , Irfan Anjum Badruddin , Amir Ibrahim Ali Arabi
The emergence of ultra-thin electronic devices and the growing demand for human-centric designs have propelled the development of wearable flexible micro-devices. However, the technology for applying electrode materials to flexible substrates remains in its infancy. In today's landscape of zero-pollution energy devices, lightweight formulations and adaptable shapes are crucial for meeting the current needs of wearables. Flexible supercapacitors are particularly attractive for many new devices, offering advantages over traditional supercapacitors, such as improved safety, reduced weight, compact size, and environmental sustainability. As a result, flexible supercapacitors hold significant potential for smart, wearable, and portable electronic devices. In this review, we explore recent advancements in the fabrication of flexible, self-sustaining supercapacitors, including innovations in materials—from conventional carbons to newly developed nanomaterials for lightweight, stretchable active components in flexible wearable supercapacitors. We also discuss fabrication techniques and new flexible substrates, as well as the challenges and benefits of developing flexible, self-supporting electrodes for supercapacitors and other electronic devices.
{"title":"Towards sustainable electronics: Advances in flexible supercapacitors for energy storage applications","authors":"Sajeeda Shaikh , Sarfaraz Kamangar , Irfan Anjum Badruddin , Amir Ibrahim Ali Arabi","doi":"10.1016/j.jelechem.2025.119639","DOIUrl":"10.1016/j.jelechem.2025.119639","url":null,"abstract":"<div><div>The emergence of ultra-thin electronic devices and the growing demand for human-centric designs have propelled the development of wearable flexible micro-devices. However, the technology for applying electrode materials to flexible substrates remains in its infancy. In today's landscape of zero-pollution energy devices, lightweight formulations and adaptable shapes are crucial for meeting the current needs of wearables. Flexible supercapacitors are particularly attractive for many new devices, offering advantages over traditional supercapacitors, such as improved safety, reduced weight, compact size, and environmental sustainability. As a result, flexible supercapacitors hold significant potential for smart, wearable, and portable electronic devices. In this review, we explore recent advancements in the fabrication of flexible, self-sustaining supercapacitors, including innovations in materials—from conventional carbons to newly developed nanomaterials for lightweight, stretchable active components in flexible wearable supercapacitors. We also discuss fabrication techniques and new flexible substrates, as well as the challenges and benefits of developing flexible, self-supporting electrodes for supercapacitors and other electronic devices.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"1000 ","pages":"Article 119639"},"PeriodicalIF":4.1,"publicationDate":"2025-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145526671","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-11-05DOI: 10.1016/j.jelechem.2025.119624
Ziyu Lu , Siwu Li , Liang Ming , Ziling Jiang , Lin Li , Qiyue Luo , Miao Deng , Chen Liu , Chuang Yu
Despite the exceptional Na+ conductivity enabled by its three-dimensional diffusion pathways, Na11Sn2PS12 (NSPS) sulfide electrolytes face critical challenges in intrinsic stability and practical all-solid-state battery performance. This study systematically investigates the NSPS solid electrolyte synthesized via high-energy ball milling and optimized annealing. Rietveld refinement reveals that annealing at 500 °C yields minimized lattice parameters and dense atomic packing, achieving optimal ionic conductivity (0.59 mS cm−1) and low activation energy (0.33 eV) through 3D Na+ diffusion pathways, while higher temperatures induce detrimental lattice distortions. Air exposure studies demonstrate moisture-induced degradation, with secondary phase formation and lattice contraction reducing conductivity by ∼66 % (to 0.2 mS cm−1) and increasing activation energy by 30 %. A pelletilizing and thermal treatment protocol effectively restores 92 % of the original conductivity while recovering electrochemical stability. Electrochemical analyses reveal superior interfacial compatibility of NSPS with Na3Sn alloy anodes versus Na metal, attributed to suppressed interfacial impedance growth. The FeS2/NSPS/Na3Sn battery delivers 530.0 mAh g−1 initial capacity with 62.3 % retention (80 cycles), vastly outperforming the Na-metal counterpart (96.4 mAh g−1, 6.5 %). Cathode stability tests using NSPS@VGCF (vapor-grown carbon fiber) composite identify electrolyte phase transitions as capacity contributors (51.8 mAh g−1 initial discharge at 0.1 A g−1), with limited oxidative stability traced to NSPS's narrow electrochemical window. This work provides fundamental insights into structure-property relationships and interfacial challenges in sulfide-based sodium-ion solid electrolytes, guiding future development of stable all-solid-state batteries.
尽管Na11Sn2PS12 (NSPS)硫化物电解质通过其三维扩散途径实现了优异的Na+导电性,但在固有稳定性和全固态电池性能方面面临着严峻的挑战。本文系统地研究了高能球磨和优化退火法制备的NSPS固体电解质。Rietveld细化表明,在500°C退火时,晶格参数最小,原子堆积致密,通过3D Na+扩散途径获得最佳离子电导率(0.59 mS cm−1)和低活化能(0.33 eV),而高温会导致有害的晶格扭曲。空气暴露研究表明,水分引起的降解,二次相的形成和晶格收缩使电导率降低~ 66%(至0.2 mS cm - 1),使活化能增加30%。球团和热处理方案有效地恢复了92%的原始电导率,同时恢复了电化学稳定性。电化学分析表明,NSPS与Na3Sn合金阳极的界面相容性优于Na金属阳极,这是由于抑制了界面阻抗的增长。FeS2/NSPS/Na3Sn电池的初始容量为530.0 mAh g−1,保留率为62.3%(80次循环),大大优于na金属电池(96.4 mAh g−1,6.5%)。使用NSPS@VGCF(气相生长碳纤维)复合材料进行阴极稳定性测试,确定电解质相变是容量贡献者(0.1 A g−1初始放电51.8 mAh g−1),有限的氧化稳定性可追溯到NSPS的狭窄电化学窗口。这项工作为硫化物基钠离子固体电解质的结构-性能关系和界面挑战提供了基本的见解,指导未来稳定的全固态电池的发展。
{"title":"Annealing-tuned sodium-ion transport in Na11Sn2PS12: Interfacial stabilization and degradation mechanisms for all-solid-state sodium batteries","authors":"Ziyu Lu , Siwu Li , Liang Ming , Ziling Jiang , Lin Li , Qiyue Luo , Miao Deng , Chen Liu , Chuang Yu","doi":"10.1016/j.jelechem.2025.119624","DOIUrl":"10.1016/j.jelechem.2025.119624","url":null,"abstract":"<div><div>Despite the exceptional Na<sup>+</sup> conductivity enabled by its three-dimensional diffusion pathways, Na<sub>11</sub>Sn<sub>2</sub>PS<sub>12</sub> (NSPS) sulfide electrolytes face critical challenges in intrinsic stability and practical all-solid-state battery performance. This study systematically investigates the NSPS solid electrolyte synthesized via high-energy ball milling and optimized annealing. Rietveld refinement reveals that annealing at 500 °C yields minimized lattice parameters and dense atomic packing, achieving optimal ionic conductivity (0.59 mS cm<sup>−1</sup>) and low activation energy (0.33 eV) through 3D Na<sup>+</sup> diffusion pathways, while higher temperatures induce detrimental lattice distortions. Air exposure studies demonstrate moisture-induced degradation, with secondary phase formation and lattice contraction reducing conductivity by ∼66 % (to 0.2 mS cm<sup>−1</sup>) and increasing activation energy by 30 %. A pelletilizing and thermal treatment protocol effectively restores 92 % of the original conductivity while recovering electrochemical stability. Electrochemical analyses reveal superior interfacial compatibility of NSPS with Na<sub>3</sub>Sn alloy anodes versus Na metal, attributed to suppressed interfacial impedance growth. The FeS<sub>2</sub>/NSPS/Na<sub>3</sub>Sn battery delivers 530.0 mAh g<sup>−1</sup> initial capacity with 62.3 % retention (80 cycles), vastly outperforming the Na-metal counterpart (96.4 mAh g<sup>−1</sup>, 6.5 %). Cathode stability tests using NSPS@VGCF (vapor-grown carbon fiber) composite identify electrolyte phase transitions as capacity contributors (51.8 mAh g<sup>−1</sup> initial discharge at 0.1 A g<sup>−1</sup>), with limited oxidative stability traced to NSPS's narrow electrochemical window. This work provides fundamental insights into structure-property relationships and interfacial challenges in sulfide-based sodium-ion solid electrolytes, guiding future development of stable all-solid-state batteries.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"1000 ","pages":"Article 119624"},"PeriodicalIF":4.1,"publicationDate":"2025-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145463964","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-11-05DOI: 10.1016/j.jelechem.2025.119622
Prerna Chaturvedi , Smruti Medha Mishra , Daniel S. Choi
Silicon-based anodes are promising for lithium-ion batteries (LIBs) due to their high capacity and low voltage plateau but suffer from poor conductivity, volume expansion, and unstable solid electrolyte interphase (SEI) growth, causing rapid capacity loss. To overcome these challenges, this work fabricates a novel bilayer-coating of MnO and N-doped carbon (NC) on SiO2 microspheres. The MnO layer enhances electrochemical kinetics, while the outer carbon coating improves conductivity and structural stability, reducing volume changes during cycling. This unique SiO2@MnO-NC composite structure effectively suppresses volume expansion and stabilizes the electrode. A full cell employing SiO2@MnO-NC as anode and nickel‑cobalt‑aluminum oxide (NCA) as cathode displayed excellent rate capability and long-term cycling, delivering a high capacity (157 mAh/g) with ∼73 % capacity retention and ∼ 99 % Coulombic efficiency over 250 cycles. SiO2@MnO-NC//NCA full cell achieves an energy density of 619 Wh/kg and power density of 556 W/kg. These findings demonstrate the strong potential of SiO2@MnO-NC composite as a high-performance anode material for next-generation LIBs.
{"title":"Bilayer-coating of MnO and N-doped carbon on SiO2 microspheres as a high-performance anode for flexible li-ion batteries","authors":"Prerna Chaturvedi , Smruti Medha Mishra , Daniel S. Choi","doi":"10.1016/j.jelechem.2025.119622","DOIUrl":"10.1016/j.jelechem.2025.119622","url":null,"abstract":"<div><div>Silicon-based anodes are promising for lithium-ion batteries (LIBs) due to their high capacity and low voltage plateau but suffer from poor conductivity, volume expansion, and unstable solid electrolyte interphase (SEI) growth, causing rapid capacity loss. To overcome these challenges, this work fabricates a novel bilayer-coating of MnO and N-doped carbon (NC) on SiO<sub>2</sub> microspheres. The MnO layer enhances electrochemical kinetics, while the outer carbon coating improves conductivity and structural stability, reducing volume changes during cycling. This unique SiO<sub>2</sub>@MnO-NC composite structure effectively suppresses volume expansion and stabilizes the electrode. A full cell employing SiO<sub>2</sub>@MnO-NC as anode and nickel‑cobalt‑aluminum oxide (NCA) as cathode displayed excellent rate capability and long-term cycling, delivering a high capacity (157 mAh/g) with ∼73 % capacity retention and ∼ 99 % Coulombic efficiency over 250 cycles. SiO<sub>2</sub>@MnO-NC//NCA full cell achieves an energy density of 619 Wh/kg and power density of 556 W/kg. These findings demonstrate the strong potential of SiO<sub>2</sub>@MnO-NC composite as a high-performance anode material for next-generation LIBs.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"1000 ","pages":"Article 119622"},"PeriodicalIF":4.1,"publicationDate":"2025-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145463960","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Designing sustainable and surface-active carbon catalysts for efficient two-electron oxygen reduction (2e− ORR) requires precise control over interfacial chemistry and defect architecture. Current methods, however, rely on corrosive chemical oxidation or complex multi-step processes that degrade structural integrity. Herein, we propose a folic acid assisted surface reconstruction strategy to engineer oxygen/nitrogen co-functionalized carbon nanotubes (O-CNTs) through one-step green pyrolysis. Unlike conventional acid treatments, this approach leverages folic acid's thermally stable heterocyclic framework to synchronously graft oxygen functional groups (C=O/C–OH) and N dopants onto defective CNT surfaces, achieving defect property balance between catalytic activity and conductivity. The resulting O-CNTs exhibit an exceptional H₂O₂ selectivity (89 % at 0.5 V vs. RHE) and durability (95 % current retention over 50 h) in alkaline media, outperforming analogues crafted by HNO₃ oxidation or plasma etching. Systematic characterization reveals that enhancing H₂O₂ selectivity correlates with folic acid-derived N/O co-doping, specifically through synergistic modulation of pyrrolic-N content (57.6 %) and electrophilic CO groups (32.1 %). While multiple defect types coexist, our control experiments using non-functionalized templates and molecular analogues (e.g., glucose/citric acid) indicate that O/N co-doping dominates the activity enhancement, contributing >85 % selectivity gains. This synergistic mechanism provides a versatile design strategy for sustainable H₂O₂ electrosynthesis.
{"title":"Enhanced electrochemical hydrogen peroxide production via functionalized carbon nanotubes with folic acid: A novel route to sustainable and selective 2e− ORR","authors":"Danyang Wu, Yehong Xin, Yu Wang, Dandan Jiang, Xizhen Zhang, Yongze Cao, Baojiu Chen","doi":"10.1016/j.jelechem.2025.119625","DOIUrl":"10.1016/j.jelechem.2025.119625","url":null,"abstract":"<div><div>Designing sustainable and surface-active carbon catalysts for efficient two-electron oxygen reduction (2e<sup>−</sup> ORR) requires precise control over interfacial chemistry and defect architecture. Current methods, however, rely on corrosive chemical oxidation or complex multi-step processes that degrade structural integrity. Herein, we propose a folic acid assisted surface reconstruction strategy to engineer oxygen/nitrogen co-functionalized carbon nanotubes (O-CNTs) through one-step green pyrolysis. Unlike conventional acid treatments, this approach leverages folic acid's thermally stable heterocyclic framework to synchronously graft oxygen functional groups (C=O/C–OH) and N dopants onto defective CNT surfaces, achieving defect property balance between catalytic activity and conductivity. The resulting O-CNTs exhibit an exceptional H₂O₂ selectivity (89 % at 0.5 V vs. RHE) and durability (95 % current retention over 50 h) in alkaline media, outperforming analogues crafted by HNO₃ oxidation or plasma etching. Systematic characterization reveals that enhancing H₂O₂ selectivity correlates with folic acid-derived N/O co-doping, specifically through synergistic modulation of pyrrolic-N content (57.6 %) and electrophilic C<img>O groups (32.1 %). While multiple defect types coexist, our control experiments using non-functionalized templates and molecular analogues (e.g., glucose/citric acid) indicate that O/N co-doping dominates the activity enhancement, contributing >85 % selectivity gains. This synergistic mechanism provides a versatile design strategy for sustainable H₂O₂ electrosynthesis.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"1000 ","pages":"Article 119625"},"PeriodicalIF":4.1,"publicationDate":"2025-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145464328","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-11-05DOI: 10.1016/j.jelechem.2025.119634
Keyan Wei, Suliang Deng, Bingxin Huang
Ca-doped O3-type NaNi1/3Fe1/3Mn1/3-xCaxO2 (x = 0, 0.03, 0.05, 0.10) cathodes were synthesized via co-precipitation and high-temperature sintering to address challenges of Mn3+ Jahn-Teller distortion and irreversible phase transitions in NaNi1/3Fe1/3Mn1/3O2 for sodium-ion batteries. At an optimal doping level (x = 0.05), the doped sample exhibited significantly enhanced electrochemical performance. It delivered an initial discharge capacity of 134.4 mAh g−1 and retained 80.1 % capacity after 100 cycles at 0.5C (2.0–4.3 V), outperforming the undoped cathode (45.6 % retention). The material also achieved 86.2 mAh g−1 at 5C. Ca2+ substitution for Mn stabilized the lattice by reducing Mn3+ content, suppressing Jahn-Teller distortion, expanding interlayer spacing to facilitate Na+ diffusion (DNa+ = 4.99 × 10−8 cm2 s−1), and inhibiting the irreversible P3 → O3′ phase transition above 4.0 V. This work demonstrates transition-metal-site Ca doping as an effective modification strategy.
{"title":"Optimizing electrochemical performance of O3- NaNi1/3Fe1/3Mn1/3O2 cathodes via transition-metal-site calcium doping for sodium-ion batteries","authors":"Keyan Wei, Suliang Deng, Bingxin Huang","doi":"10.1016/j.jelechem.2025.119634","DOIUrl":"10.1016/j.jelechem.2025.119634","url":null,"abstract":"<div><div>Ca-doped O3-type NaNi<sub>1/3</sub>Fe<sub>1/3</sub>Mn<sub>1/3-<em>x</em></sub>Ca<sub><em>x</em></sub>O<sub>2</sub> (<em>x</em> = 0, 0.03, 0.05, 0.10) cathodes were synthesized via co-precipitation and high-temperature sintering to address challenges of Mn<sup>3+</sup> Jahn-Teller distortion and irreversible phase transitions in NaNi<sub>1/3</sub>Fe<sub>1/3</sub>Mn<sub>1/3</sub>O<sub>2</sub> for sodium-ion batteries. At an optimal doping level (<em>x</em> = 0.05), the doped sample exhibited significantly enhanced electrochemical performance. It delivered an initial discharge capacity of 134.4 mAh g<sup>−1</sup> and retained 80.1 % capacity after 100 cycles at 0.5C (2.0–4.3 V), outperforming the undoped cathode (45.6 % retention). The material also achieved 86.2 mAh g<sup>−1</sup> at 5C. Ca<sup>2+</sup> substitution for Mn stabilized the lattice by reducing Mn<sup>3+</sup> content, suppressing Jahn-Teller distortion, expanding interlayer spacing to facilitate Na<sup>+</sup> diffusion (D<sub>Na</sub><sup>+</sup> = 4.99 × 10<sup>−8</sup> cm<sup>2</sup> s<sup>−1</sup>), and inhibiting the irreversible P3 → O3′ phase transition above 4.0 V. This work demonstrates transition-metal-site Ca doping as an effective modification strategy.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"1000 ","pages":"Article 119634"},"PeriodicalIF":4.1,"publicationDate":"2025-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145526673","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-11-05DOI: 10.1016/j.jelechem.2025.119620
Kudakwashe Meki, Shiyu Meng, Shan Qiu, Fengxia Deng
The global transition toward sustainable chemical manufacturing necessitates greener alternatives to the energy-intensive anthraquinone process currently dominating hydrogen peroxide (H₂O₂) production. Electrochemical synthesis via the two-electron oxygen reduction reaction (2e− ORR) in gas diffusion electrodes (GDEs) presents a promising solution. This review explores recent advances in engineering tunable triple-phase interfaces (TPIs) within GDE architectures to enhance H₂O₂ electrosynthesis efficiency and durability. Emphasis is placed on material design strategies that synergistically integrate catalyst activity, pore structure, and interfacial wettability to mitigate challenges such as flooding and poor mass transport. Key developments are examined, including the use of defect-engineered carbon frameworks, single-atom metal–nitrogen–carbon (M–N–C) catalysts, and optimized binder systems such as PTFE and Nafion. The role of fabrication methods—ranging from ink formulation and vacuum infiltration to layer-by-layer deposition—is critically assessed for their influence on TPI robustness and electrochemical performance. Across the literature, H₂O₂ yields exceeding 80 % faradaic efficiency have been demonstrated through such design principles. By bridging material chemistry and electrochemical engineering, this review provides a climate-conscious roadmap for scalable, decentralized H₂O₂ production. The insights discussed are broadly applicable to green oxidant generation for environmental remediation, disinfection, and sustainable chemical processes.
{"title":"Tunable triple-phase interfaces in GDEs: A climate-conscious approach to hydrogen peroxide electrosynthesis","authors":"Kudakwashe Meki, Shiyu Meng, Shan Qiu, Fengxia Deng","doi":"10.1016/j.jelechem.2025.119620","DOIUrl":"10.1016/j.jelechem.2025.119620","url":null,"abstract":"<div><div>The global transition toward sustainable chemical manufacturing necessitates greener alternatives to the energy-intensive anthraquinone process currently dominating hydrogen peroxide (H₂O₂) production. Electrochemical synthesis via the two-electron oxygen reduction reaction (2e<sup>−</sup> ORR) in gas diffusion electrodes (GDEs) presents a promising solution. This review explores recent advances in engineering tunable triple-phase interfaces (TPIs) within GDE architectures to enhance H₂O₂ electrosynthesis efficiency and durability. Emphasis is placed on material design strategies that synergistically integrate catalyst activity, pore structure, and interfacial wettability to mitigate challenges such as flooding and poor mass transport. Key developments are examined, including the use of defect-engineered carbon frameworks, single-atom metal–nitrogen–carbon (M–N–C) catalysts, and optimized binder systems such as PTFE and Nafion. The role of fabrication methods—ranging from ink formulation and vacuum infiltration to layer-by-layer deposition—is critically assessed for their influence on TPI robustness and electrochemical performance. Across the literature, H₂O₂ yields exceeding 80 % faradaic efficiency have been demonstrated through such design principles. By bridging material chemistry and electrochemical engineering, this review provides a climate-conscious roadmap for scalable, decentralized H₂O₂ production. The insights discussed are broadly applicable to green oxidant generation for environmental remediation, disinfection, and sustainable chemical processes.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"1001 ","pages":"Article 119620"},"PeriodicalIF":4.1,"publicationDate":"2025-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145578553","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}