Abundant use of aluminum cookware and treatment of high fluoride-containing water with aluminum salts results in the discharge of aluminum ions into water bodies and food items, causing harmful effects on human health. Herein, an electrochemical sensor for sensing the Al (III) ions by modification of glassy carbon electrode (GCE) with Schiff’s base ligand as an electrocatalyst and activated charcoal as an electro-conductive material is being reported. The response is recorded via Square wave voltammetry (SWV) for the modified GCE, resulting in a characteristic peak at potential 0.4 V due to the interaction of the Al (III) ions with the electrocatalyst. The peak current intensity increases linearly in the concentration range from 0.1 – 50 µM (R2 = 0.994), and the detection limit of 45 nM (S/N = 3) was calculated. DFT calculation reveals that the energy gap between the HOMO and LUMO decreases from 0.551 eV to 0.303 eV after the complexation of the ligand with the Al (III) ions indicating the stability enhancement after complex formation. Common interfering agents do not significantly change in the peak current intensity, demonstrating excellent selectivity. Spiking Al (III) ions in tap and river water checked practical applicability, which gave satisfactory recovery results.
Graphical Abstract
铝制炊具的大量使用和用铝盐处理含氟量高的水会导致铝离子排入水体和食品中，对人体健康造成危害。本文报告了一种电化学传感器，它以希夫碱配体为电催化剂，以活性炭为导电材料，对玻璃碳电极（GCE）进行改性，从而感测铝（III）离子。通过方波伏安法（SWV）记录了改性 GCE 的反应，由于 Al (III) 离子与电催化剂的相互作用，在 0.4 V 电位处产生了一个特征峰。峰值电流强度在 0.1 - 50 µM 的浓度范围内线性增加（R2 = 0.994），计算得出检测限为 45 nM（S/N = 3）。DFT 计算显示，配体与 Al (III) 离子络合后，HOMO 和 LUMO 之间的能隙从 0.551 eV 减小到 0.303 eV，表明络合物形成后稳定性增强。普通干扰剂不会明显改变峰值电流强度，这表明了极佳的选择性。在自来水和河水中添加铝（III）离子检验了该方法的实用性，结果令人满意。
{"title":"Selective And Sensitive Electrochemical Detection of Trace Level Al (III) Ions in Water by Antipyrine Schiff’s Base-Modified Glassy Carbon Electrode","authors":"Md Zainul Abedeen, Priya Yadav, Manish Sharma, Lalita Yadav, Priya Sharma, Himmat Singh Kushwaha, Ragini Gupta","doi":"10.1007/s12678-024-00899-2","DOIUrl":"10.1007/s12678-024-00899-2","url":null,"abstract":"<div><p>Abundant use of aluminum cookware and treatment of high fluoride-containing water with aluminum salts results in the discharge of aluminum ions into water bodies and food items, causing harmful effects on human health. Herein, an electrochemical sensor for sensing the Al (III) ions by modification of glassy carbon electrode (GCE) with Schiff’s base ligand as an electrocatalyst and activated charcoal as an electro-conductive material is being reported. The response is recorded via Square wave voltammetry (SWV) for the modified GCE, resulting in a characteristic peak at potential 0.4 V due to the interaction of the Al (III) ions with the electrocatalyst. The peak current intensity increases linearly in the concentration range from 0.1 – 50 µM (R<sup>2</sup> = 0.994), and the detection limit of 45 nM (S/N = 3) was calculated. DFT calculation reveals that the energy gap between the HOMO and LUMO decreases from 0.551 eV to 0.303 eV after the complexation of the ligand with the Al (III) ions indicating the stability enhancement after complex formation. Common interfering agents do not significantly change in the peak current intensity, demonstrating excellent selectivity. Spiking Al (III) ions in tap and river water checked practical applicability, which gave satisfactory recovery results.</p><h3>Graphical Abstract</h3><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":535,"journal":{"name":"Electrocatalysis","volume":"16 1","pages":"67 - 77"},"PeriodicalIF":2.7,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142859579","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-11DOI: 10.1007/s12678-024-00901-x
Eleilde de Sousa Oliveira, Adolfo Lopes Figueredo, Maitê Lippel Gothe, Pedro Vidinha, Auro Atsushi Tanaka, Marco Aurélio Suller Garcia
Developing efficient and cost-effective oxygen reduction reaction (ORR) catalysts is critical for advancing fuel cell technologies. Based on this, we propose a metal-free reduced graphene oxide (rGO) catalyst produced from graphite as a base material for electrode modification. Nevertheless, by using phenanthroline as a nitrogen precursor, we investigated different synthesis conditions to adjust the electrocatalytic characteristics of the material precisely, aiming for a four-electron mechanism with low onset potential. A comprehensive experimental design revealed that specific preparation parameters (75 mg of phenanthroline, 1079 °C, and 1.73 h) significantly influenced the catalyst’s performance: the optimized catalyst had an increase in current density and a positive shift in the half-wave potential compared to other materials that underwent not optimized synthetic conditions. Morphological and physicochemical characterizations, including SEM and XPS analyses, provided insights into the material’s structure and composition, correlating the observed catalytic performance with graphitic nitrogen and an optimized degree of deoxygenation. Crucially, our study demonstrated a method for achieving varied levels of nitrogen species with the same nitrogen precursor, revealing that, under optimized conditions, the same precursor can yield diverse outcomes. Importantly, the optimized catalyst demonstrated impressive performance, showing only a 0.1 V difference in onset potential compared to the commercial Pt/C catalyst and a limiting current density of 2.1 mA cm−2. Thus, this study underscores the importance of systematic experimental design and optimization in developing high-performance, metal-free electrocatalysts for energy conversion applications.
Graphical Abstract
开发高效、经济的氧还原反应（ORR）催化剂是推进燃料电池技术发展的关键。基于此，我们提出了一种由石墨作为电极修饰的基础材料制备的无金属还原氧化石墨烯（rGO）催化剂。然而，我们以菲罗啉为氮前驱体，研究了不同的合成条件，以精确调整材料的电催化特性，旨在实现低起始电位的四电子机制。综合实验设计表明，特定的制备参数（75 mg菲罗啉，1079°C, 1.73 h）对催化剂的性能有显著影响：与未经优化合成条件的其他材料相比，优化后的催化剂电流密度增加，半波电位正偏移。形态学和物理化学表征，包括SEM和XPS分析，提供了对材料结构和组成的深入了解，将观察到的催化性能与石墨氮和优化的脱氧程度联系起来。重要的是，我们的研究展示了一种用相同的氮前体获得不同水平氮的方法，揭示了在优化条件下，相同的前体可以产生不同的结果。重要的是，优化后的催化剂表现出令人印象深刻的性能，与商用Pt/C催化剂相比，起始电位仅相差0.1 V，极限电流密度为2.1 mA cm−2。因此，这项研究强调了系统实验设计和优化在开发高性能、无金属的能量转换电催化剂中的重要性。图形抽象
{"title":"Optimizing Metal-free Phenanthroline-assisted Nitrogen-doped Reduced Graphene Oxide for Enhanced Oxygen Reduction Reaction: An Experimental Design and Performance Study","authors":"Eleilde de Sousa Oliveira, Adolfo Lopes Figueredo, Maitê Lippel Gothe, Pedro Vidinha, Auro Atsushi Tanaka, Marco Aurélio Suller Garcia","doi":"10.1007/s12678-024-00901-x","DOIUrl":"10.1007/s12678-024-00901-x","url":null,"abstract":"<div><p>Developing efficient and cost-effective oxygen reduction reaction (ORR) catalysts is critical for advancing fuel cell technologies. Based on this, we propose a metal-free reduced graphene oxide (rGO) catalyst produced from graphite as a base material for electrode modification. Nevertheless, by using phenanthroline as a nitrogen precursor, we investigated different synthesis conditions to adjust the electrocatalytic characteristics of the material precisely, aiming for a four-electron mechanism with low onset potential. A comprehensive experimental design revealed that specific preparation parameters (75 mg of phenanthroline, 1079 °C, and 1.73 h) significantly influenced the catalyst’s performance: the optimized catalyst had an increase in current density and a positive shift in the half-wave potential compared to other materials that underwent not optimized synthetic conditions. Morphological and physicochemical characterizations, including SEM and XPS analyses, provided insights into the material’s structure and composition, correlating the observed catalytic performance with graphitic nitrogen and an optimized degree of deoxygenation. Crucially, our study demonstrated a method for achieving varied levels of nitrogen species with the same nitrogen precursor, revealing that, under optimized conditions, the same precursor can yield diverse outcomes. Importantly, the optimized catalyst demonstrated impressive performance, showing only a 0.1 V difference in onset potential compared to the commercial Pt/C catalyst and a limiting current density of 2.1 mA cm<sup>−2</sup>. Thus, this study underscores the importance of systematic experimental design and optimization in developing high-performance, metal-free electrocatalysts for energy conversion applications.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":535,"journal":{"name":"Electrocatalysis","volume":"16 1","pages":"54 - 66"},"PeriodicalIF":2.7,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142858599","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-11DOI: 10.1007/s12678-024-00897-4
Meng Yu, Wenzheng Wang, Pengjie Wu, Hongyu Wen
The inherent disadvantages of carbon-based anodes, including their low hydrophilicity, significant charge transfer resistance, and limited power density, hinder their widespread commercial utilization in microbial fuel cells (MFC). Addressing these challenges, this study involved the surface modification of a carbon-based anode. To improve the adhesion of electroactive microorganisms (EAM) on the anode surface and increase the extracellular electron transfer rate, CNT@Ti3C2TxMXene was applied to the surface of carbon cloth (CC) using drip coating. Initially, we conducted a comprehensive investigation on the optimal amount of modification required. To achieve this, we designed four distinct groups of modified electrodes. Through electrochemical analysis and phase characterization, it was determined that a modification dosage of 1.5 mg/cm2 for CNT@Ti3C2TxMXene/CC electrodes yielded the most optimal electrical conductivity and the highest capacitance. The Rs of CC is reduced from 1.48 to 0.55 Ω and the Rct from 2.62 to 2.09 Ω, and the capacitance is increased from 3.98 10−07F to 9.11 10−06F. Subsequently, the CNT@Ti3C2TxMXene/CC with a modification of 1.5 mg/cm2 was used as the anode of the microbial fuel cell. The modification of CNT@Ti3C2TxMXene improved the power generation performance. The maximum output voltage of the MFC was increased from 546 to 709 mv, and the power density was increased from 44.9 to 101.8 mW/m2. The underlying factor lies in the ability of CNT@Ti3C2TxMXene/CC to significantly lower the internal resistance within the microbial fuel cell, thereby fostering the development of biofilm. Notably, our observations revealed that the biofilm formation was particularly facilitated on the anode surface of CNT@Ti3C2TxMXene/CC. In essence, the CNT@Ti3C2TxMXene-modified carbon cloth not only minimizes internal resistance but also enhances the electroactive surface area, exhibiting superior electrical conductivity. These attributes make it an advantageous material for biological applications.
{"title":"CNT@Ti3C2TxMXene Nanocomposite Catalysts as Anodes to Improve the Electricity Production Performance of Microbial Fuel Cells","authors":"Meng Yu, Wenzheng Wang, Pengjie Wu, Hongyu Wen","doi":"10.1007/s12678-024-00897-4","DOIUrl":"10.1007/s12678-024-00897-4","url":null,"abstract":"<div><p>The inherent disadvantages of carbon-based anodes, including their low hydrophilicity, significant charge transfer resistance, and limited power density, hinder their widespread commercial utilization in microbial fuel cells (MFC). Addressing these challenges, this study involved the surface modification of a carbon-based anode. To improve the adhesion of electroactive microorganisms (EAM) on the anode surface and increase the extracellular electron transfer rate, CNT@Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>MXene was applied to the surface of carbon cloth (CC) using drip coating. Initially, we conducted a comprehensive investigation on the optimal amount of modification required. To achieve this, we designed four distinct groups of modified electrodes. Through electrochemical analysis and phase characterization, it was determined that a modification dosage of 1.5 mg/cm<sup>2</sup> for CNT@Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>MXene/CC electrodes yielded the most optimal electrical conductivity and the highest capacitance. The Rs of CC is reduced from 1.48 to 0.55 Ω and the Rct from 2.62 to 2.09 Ω, and the capacitance is increased from 3.98 10<sup>−07</sup><i>F</i> to 9.11 10<sup>−06</sup><i>F</i>. Subsequently, the CNT@Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>MXene/CC with a modification of 1.5 mg/cm<sup>2</sup> was used as the anode of the microbial fuel cell. The modification of CNT@Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>MXene improved the power generation performance. The maximum output voltage of the MFC was increased from 546 to 709 mv, and the power density was increased from 44.9 to 101.8 mW/m<sup>2</sup>. The underlying factor lies in the ability of CNT@Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>MXene/CC to significantly lower the internal resistance within the microbial fuel cell, thereby fostering the development of biofilm. Notably, our observations revealed that the biofilm formation was particularly facilitated on the anode surface of CNT@Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>MXene/CC. In essence, the CNT@Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>MXene-modified carbon cloth not only minimizes internal resistance but also enhances the electroactive surface area, exhibiting superior electrical conductivity. These attributes make it an advantageous material for biological applications.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":535,"journal":{"name":"Electrocatalysis","volume":"16 1","pages":"42 - 53"},"PeriodicalIF":2.7,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142858596","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-09DOI: 10.1007/s12678-024-00900-y
Kusumita Dutta, S. Pushpavanam
A novel electrochemical molecularly imprinted composite (MIC)-based sensor for detection of triclosan was developed. MIC was synthesized from o-phenylenediamine (o–PD), -COOH functionalized multiwalled carbon nanotube (cf-MWCNT), and triclosan by cyclic voltammetry on molybdenum nanoparticle (Mo-NP) embedded cf-MWCNT (Mo-cf-MWCNT) coated glassy carbon (GC) electrode, following removal of surface triclosan to form MIC/Mo-cf-MWCNT/GC. In our earlier work, two novel electrodes MIC/cf-MWCNT/GC and MIC/GC were fabricated. The presence of cf-MWCNT coating substrate on GC in MIC/cf-MWCNT/GC had improved the sensing performance than MIC/GC since presence of this substrate had decreased the electrochemical band gap (Eg) and increased Debye length (λd), Gibb’s free energy of adsorption (− ΔGads), electrochemical surface area (Ae), and surface redox site concentration (C*). Therefore, further improvement in sensing performance can be carried out by utilizing Mo-NP in the cf-MWCNT coating substrate using MIC to be the sensing material. This novel electrode (MIC/Mo-cf-MWCNT/GC) provided a limit of detection (LOD) of 900 ppt of triclosan, which was lower than the LOD achieved by using MIC/cf-MWCNT/GC (10 ppb) and MIC/GC (40 ppb). Adsorption isotherm was constructed for MIC/Mo-cf-MWCNT/GC delivering − ΔGads value of 59.049 kJ/mol indicating stronger chemisorption. To understand the role of Mo-cf-MWCNT in detection of triclosan, cyclic voltammetry, electrochemical impedance spectroscopy, and electrochemical band gap studies were conducted. This MIC/Mo-cf-MWCNT/GC showed good selectivity towards triclosan in presence of interfering ions.
{"title":"A Molecularly Imprinted Composite-based Novel Electrochemical Sensor Using o-Phenylenediamine, Molybdenum Nanoparticle, and Multiwalled Carbon Nanotube for Triclosan Detection from Water","authors":"Kusumita Dutta, S. Pushpavanam","doi":"10.1007/s12678-024-00900-y","DOIUrl":"10.1007/s12678-024-00900-y","url":null,"abstract":"<div><p>A novel electrochemical molecularly imprinted composite (MIC)-based sensor for detection of triclosan was developed. MIC was synthesized from o-phenylenediamine (o–PD), -COOH functionalized multiwalled carbon nanotube (<i>cf</i>-MWCNT), and triclosan by cyclic voltammetry on molybdenum nanoparticle (Mo-NP) embedded <i>cf</i>-MWCNT (Mo-<i>cf</i>-MWCNT) coated glassy carbon (GC) electrode, following removal of surface triclosan to form MIC/Mo-<i>cf</i>-MWCNT/GC. In our earlier work, two novel electrodes MIC/<i>cf</i>-MWCNT/GC and MIC/GC were fabricated. The presence of <i>cf</i>-MWCNT coating substrate on GC in MIC/<i>cf</i>-MWCNT/GC had improved the sensing performance than MIC/GC since presence of this substrate had decreased the electrochemical band gap (<i>E</i><sub><i>g</i></sub>) and increased Debye length (<i>λ</i><sub><i>d</i></sub>), Gibb’s free energy of adsorption (− <i>ΔG</i><sub>ads</sub>), electrochemical surface area (<i>A</i><sub><i>e</i></sub>), and surface redox site concentration (<i>C</i>*). Therefore, further improvement in sensing performance can be carried out by utilizing Mo-NP in the <i>cf</i>-MWCNT coating substrate using MIC to be the sensing material. This novel electrode (MIC/Mo-<i>cf</i>-MWCNT/GC) provided a limit of detection (LOD) of 900 ppt of triclosan, which was lower than the LOD achieved by using MIC/<i>cf-</i>MWCNT/GC (10 ppb) and MIC/GC (40 ppb). Adsorption isotherm was constructed for MIC/Mo-<i>cf</i>-MWCNT/GC delivering − <i>ΔG</i><sub>ads</sub> value of 59.049 kJ/mol indicating stronger chemisorption. To understand the role of Mo-<i>cf</i>-MWCNT in detection of triclosan, cyclic voltammetry, electrochemical impedance spectroscopy, and electrochemical band gap studies were conducted. This MIC/Mo-<i>cf</i>-MWCNT/GC showed good selectivity towards triclosan in presence of interfering ions.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":535,"journal":{"name":"Electrocatalysis","volume":"15 6","pages":"529 - 540"},"PeriodicalIF":2.7,"publicationDate":"2024-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142438708","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-05DOI: 10.1007/s12678-024-00891-w
Aswathi Mechoor, K. S. Lavanya Shri, Sheela Berchmans, V. Ganesh
In this work, a peroxidase enzyme mimic is demonstrated using Mo-incorporated Cu@ZIF-8 and showed the electrochemical detection of hydrogen peroxide. Further, TMB, a chromogenic substrate, is introduced to enhance the kinetics and sensor performance of the resultant enzyme mimic. A significant gain in the overpotential value of 0.2 V and lower KM value is noted for the sensor upon introducing TMB. The characteristic kinetic parameters are determined, and a possible mechanism is elucidated for the proposed hydrogen peroxide sensor.
{"title":"Mo-Incorporated Bimetallic Metal–Organic Framework for Electrochemical Detection of Hydrogen Peroxide: A Potential Biomimic System","authors":"Aswathi Mechoor, K. S. Lavanya Shri, Sheela Berchmans, V. Ganesh","doi":"10.1007/s12678-024-00891-w","DOIUrl":"10.1007/s12678-024-00891-w","url":null,"abstract":"<div><p>In this work, a peroxidase enzyme mimic is demonstrated using Mo-incorporated Cu@ZIF-8 and showed the electrochemical detection of hydrogen peroxide. Further, TMB, a chromogenic substrate, is introduced to enhance the kinetics and sensor performance of the resultant enzyme mimic. A significant gain in the overpotential value of 0.2 V and lower <i>K</i><sub>M</sub> value is noted for the sensor upon introducing TMB. The characteristic kinetic parameters are determined, and a possible mechanism is elucidated for the proposed hydrogen peroxide sensor.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":535,"journal":{"name":"Electrocatalysis","volume":"16 1","pages":"28 - 41"},"PeriodicalIF":2.7,"publicationDate":"2024-10-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142859676","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-01DOI: 10.1007/s12678-024-00896-5
Faiq Saeed, Samia, Mushtaq Ahmad, Waheed Rehman, Yasir Sana, Somavia Ameen, A. S. Altowyan, Amir Zada
A mixed sulfur-doped zinc oxide-nickel oxide (S@ZnO-NiO) nanocomposite electrocatalyst for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) was prepared by hydrothermal method; we prepared a high-efficiency bifunctional electrocatalyst S@ZnO-NiO. By applying different characterizations, the material was proven as a new phase of (S-doped-ZnO-NiO). S@ZnO-NiO showed excellent performance at 10 mA cm−2, the generation potential of OER is 1.45 V, and that of HER is − 0.04 V. Furthermore, when applied for water splitting electrocatalysis, a current density of 10 mA cm−2 was achieved at 1.49 V with excellent stability for 10 h. S@ZnO-NiO bifunctional catalysts offer great potential for electrochemical devices due to their low cost and high activity. We have successfully constructed an electrocatalyst with the dual functions of HER and OER, which can achieve efficient water splitting.
Graphical Abstract
采用水热法制备了一种用于析氧反应（OER）和析氢反应（HER）的混合掺硫氧化锌-氧化镍纳米复合电催化剂（S@ZnO-NiO）；制备了一种高效双功能电催化剂S@ZnO-NiO。通过不同的表征，证明了该材料是一种新的（s掺杂zno - nio）相。S@ZnO-NiO在10 mA cm−2下表现优异，OER的产生电位为1.45 V， HER的产生电位为- 0.04 V。此外，当应用于水分解电催化时，在1.49 V下获得了10 mA cm−2的电流密度，并且在10 h内具有优异的稳定性S@ZnO-NiO双功能催化剂由于其低成本和高活性而在电化学器件中具有很大的潜力。我们成功构建了一种具有HER和OER双重功能的电催化剂，可以实现高效的水分解。图形抽象
{"title":"Sulfur-Doped Zinc Oxide-Nikel Oxide as Efficient Bifunctional Electrocatalyst for Overall Water Splitting","authors":"Faiq Saeed, Samia, Mushtaq Ahmad, Waheed Rehman, Yasir Sana, Somavia Ameen, A. S. Altowyan, Amir Zada","doi":"10.1007/s12678-024-00896-5","DOIUrl":"10.1007/s12678-024-00896-5","url":null,"abstract":"<div><p>A mixed sulfur-doped zinc oxide-nickel oxide (S@ZnO-NiO) nanocomposite electrocatalyst for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) was prepared by hydrothermal method; we prepared a high-efficiency bifunctional electrocatalyst S@ZnO-NiO. By applying different characterizations, the material was proven as a new phase of (S-doped-ZnO-NiO). S@ZnO-NiO showed excellent performance at 10 mA cm<sup>−2</sup>, the generation potential of OER is 1.45 V, and that of HER is − 0.04 V. Furthermore, when applied for water splitting electrocatalysis, a current density of 10 mA cm<sup>−2</sup> was achieved at 1.49 V with excellent stability for 10 h. S@ZnO-NiO bifunctional catalysts offer great potential for electrochemical devices due to their low cost and high activity. We have successfully constructed an electrocatalyst with the dual functions of HER and OER, which can achieve efficient water splitting.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":535,"journal":{"name":"Electrocatalysis","volume":"16 1","pages":"15 - 27"},"PeriodicalIF":2.7,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142859474","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Hydrogen production from water splitting is considered the most environment-friendly and sustainable method to acquire energy. Alkaline water electrolysis has been widely employed for hydrogen production, but it is still challenging to prepare non-precious metals electrocatalysts to replace the noble-metal-based catalysts. Here we proposed electroless method to prepare a NiCoP nanocrystalline thin flim as efficient electrocatalysts. The morphology and mechanisms of the 45-minute alloy films deposited on Cu substrate were characterized by SEM, XRD, and XPS techniques, moreover, LSV, EIS, and CP were applied to analyze the electrochemical behavior. The nanocrystalline NiCoP45min alloy exhibits higher hydrogen evolution reaction (HER) activity than platinum sheet. An overpotential of -98 mV and a Tafel slope of 47.94 mV·dec−1 at 10 mA·cm−2 was achieved with the catalyst during HER in an alkaline medium. Additionally, its excellent catalytic activity is confirmed by a low Rt value 2.48 Ω. Remarkably, this catalyst also exhibits high HER stability for about 45 h in an alkaline electrolysic solution.
{"title":"Study of Fabrication and Properties of NiCoP Nanocrystalline Thin Film Electrodes for Hydrogen Evolution Electrocatalysts","authors":"Huibin Yuan, Xiangzhu He, Yuelan Yang, Jiahe Xie, Binjie Wu, Xiangjian Zeng, Shuxun Zeng","doi":"10.1007/s12678-024-00893-8","DOIUrl":"10.1007/s12678-024-00893-8","url":null,"abstract":"<div><p>Hydrogen production from water splitting is considered the most environment-friendly and sustainable method to acquire energy. Alkaline water electrolysis has been widely employed for hydrogen production, but it is still challenging to prepare non-precious metals electrocatalysts to replace the noble-metal-based catalysts. Here we proposed electroless method to prepare a NiCoP nanocrystalline thin flim as efficient electrocatalysts. The morphology and mechanisms of the 45-minute alloy films deposited on Cu substrate were characterized by SEM, XRD, and XPS techniques, moreover, LSV, EIS, and CP were applied to analyze the electrochemical behavior. The nanocrystalline NiCoP<sub>45min</sub> alloy exhibits higher hydrogen evolution reaction (HER) activity than platinum sheet. An overpotential of -98 mV and a Tafel slope of 47.94 mV·dec<sup>−1</sup> at 10 mA·cm<sup>−2</sup> was achieved with the catalyst during HER in an alkaline medium. Additionally, its excellent catalytic activity is confirmed by a low Rt value 2.48 Ω. Remarkably, this catalyst also exhibits high HER stability for about 45 h in an alkaline electrolysic solution.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":535,"journal":{"name":"Electrocatalysis","volume":"15 6","pages":"519 - 528"},"PeriodicalIF":2.7,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142438823","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-27DOI: 10.1007/s12678-024-00895-6
Karuna Korgaonkar, Naveenkumar P. Agadi, J. Seetharamappa
A unique and irregular form distorted Cu2(V2O7) sphere with crumbled sheets of rGO nanocomposite was developed as a sensor over a glassy carbon electrode (GCE). It showed a higher sensitivity for an antipsychotic drug, pimozide (PMZ). Voltammetric techniques were used to investigate the electrochemical behavior of PMZ. The formation of Cu2(V2O7)-rGO nanocomposite was confirmed by X-ray diffraction analysis. Scanning electron microscopy (SEM) and atomic force microscopy (AFM) were used to examine the surface morphology and its properties. Cyclic voltammetric studies revealed that PMZ displayed intense electrocatalytic activity and exhibited an electro-oxidation peak at the modified electrode. The modified electrode possessed unique qualities such as fast electron transfer ability, repeatability, and reproducibility. The proposed differential pulse voltammetric (DPV) and square wave voltammetric (SWV) methods showed linearity in the concentration range of 5.12 × 10−9 M to 3.06 × 10−4 M and 1.02 × 10−9 M to 5.30 × 10−4 M, respectively. The limit of detection (LOD) was calculated to be 1.70 × 10−10 M and 8.52 × 10−11 M, while the limit of quantification (LOQ) was found to be 5.66 × 10−10 M and 2.84 × 10−10 M, respectively, for DPV and SWV methods. The developed methods were successfully applied for the determination of PMZ in pharmaceutical formulations and human urine samples.
Graphical Abstract
研究人员在玻璃碳电极（GCE）上开发了一种独特的不规则变形 Cu2(V2O7)球体，球体上有碎裂的 rGO 纳米复合材料片，作为传感器。它对抗抑郁药物匹莫齐特（PMZ）具有更高的灵敏度。研究人员采用伏安法研究了匹莫齐（PMZ）的电化学行为。X 射线衍射分析证实了 Cu2(V2O7)-rGO 纳米复合材料的形成。扫描电子显微镜（SEM）和原子力显微镜（AFM）用于研究其表面形貌及其特性。循环伏安研究表明，PMZ 具有很强的电催化活性，并在修饰电极上出现了电氧化峰。改性电极具有快速电子传递能力、可重复性和再现性等独特品质。所提出的微分脉冲伏安法（DPV）和方波伏安法（SWV）分别在 5.12 × 10-9 M 至 3.06 × 10-4 M 和 1.02 × 10-9 M 至 5.30 × 10-4 M 的浓度范围内呈线性关系。经计算，DPV 和 SWV 方法的检出限（LOD）分别为 1.70 × 10-10 M 和 8.52 × 10-11 M，定量限（LOQ）分别为 5.66 × 10-10 M 和 2.84 × 10-10 M。所建立的方法成功地应用于药物制剂和人体尿样中PMZ的测定。 图文摘要
{"title":"Cu2(V2O7)-rGO Engineered Sensor for the Electrochemical Determination of Antipsychotic drug, Pimozide","authors":"Karuna Korgaonkar, Naveenkumar P. Agadi, J. Seetharamappa","doi":"10.1007/s12678-024-00895-6","DOIUrl":"10.1007/s12678-024-00895-6","url":null,"abstract":"<div><p>A unique and irregular form distorted Cu<sub>2</sub>(V<sub>2</sub>O<sub>7</sub>) sphere with crumbled sheets of rGO nanocomposite was developed as a sensor over a glassy carbon electrode (GCE). It showed a higher sensitivity for an antipsychotic drug, pimozide (PMZ). Voltammetric techniques were used to investigate the electrochemical behavior of PMZ. The formation of Cu<sub>2</sub>(V<sub>2</sub>O<sub>7</sub>)-rGO nanocomposite was confirmed by X-ray diffraction analysis. Scanning electron microscopy (SEM) and atomic force microscopy (AFM) were used to examine the surface morphology and its properties. Cyclic voltammetric studies revealed that PMZ displayed intense electrocatalytic activity and exhibited an electro-oxidation peak at the modified electrode. The modified electrode possessed unique qualities such as fast electron transfer ability, repeatability, and reproducibility. The proposed differential pulse voltammetric (DPV) and square wave voltammetric (SWV) methods showed linearity in the concentration range of 5.12 × 10<sup>−9</sup> M to 3.06 × 10<sup>−4</sup> M and 1.02 × 10<sup>−9</sup> M to 5.30 × 10<sup>−4</sup> M, respectively. The limit of detection (LOD) was calculated to be 1.70 × 10<sup>−10</sup> M and 8.52 × 10<sup>−11</sup> M, while the limit of quantification (LOQ) was found to be 5.66 × 10<sup>−10</sup> M and 2.84 × 10<sup>−10</sup> M, respectively, for DPV and SWV methods. The developed methods were successfully applied for the determination of PMZ in pharmaceutical formulations and human urine samples.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":535,"journal":{"name":"Electrocatalysis","volume":"15 6","pages":"507 - 518"},"PeriodicalIF":2.7,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s12678-024-00895-6.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142438822","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-26DOI: 10.1007/s12678-024-00889-4
Mahmoud A. Hefnawy, Rewaida Abdel-Gaber, Sobhi M. Gomha, Magdi E. A. Zaki, Shymaa S. Medany
The Co2O3-Chitosan composite (Co@Chitosan) nanoparticles were synthesized through a green approach. The composite under investigation was characterized by various analytical methods, including scanning electron microscopy (SEM), transmitted electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and atomic force microscope (AFM) confirming the preparation step. The modified composite’s performance was evaluated for its potential applications in nitrite sensing and hydrogen production by utilizing diverse electrochemical methodologies. The Co2O3-Chitosan that has been modified exhibits a linear detection range of 0.25–100 µM and a limit of detection (LOD) of 0.117 µM with a response time of approximately 5 s using the amperometry technique. Furthermore, the utilization of Co2O3-Chitosan composite as a proficient catalyst for hydrogen generation in an alkaline environment was implemented. The electrode exhibited enduring stability in fuel generation and heightened energy safeguarding. The current density of the electrode was observed to attain a value of (upeta)50 at − 0.55 and − 0.43 V (versus RHE) for Co2O3 and Co@Chitosan, respectively. The study investigated the durability of electrodes during extended periods of constant potential chronoamperometry lasting 6 h. The Co2O3 and Co@Chitosan exhibited a reduction in initial current by 11% and 7%, respectively.
{"title":"Green Synthesis of Cobalt Oxide Decorated Chitosan Substrates for Electrochemical Detection of Nitrite and Hydrogen Evolution Reactions","authors":"Mahmoud A. Hefnawy, Rewaida Abdel-Gaber, Sobhi M. Gomha, Magdi E. A. Zaki, Shymaa S. Medany","doi":"10.1007/s12678-024-00889-4","DOIUrl":"10.1007/s12678-024-00889-4","url":null,"abstract":"<div><p>The Co<sub>2</sub>O<sub>3</sub>-Chitosan composite (Co@Chitosan) nanoparticles were synthesized through a green approach. The composite under investigation was characterized by various analytical methods, including scanning electron microscopy (SEM), transmitted electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and atomic force microscope (AFM) confirming the preparation step. The modified composite’s performance was evaluated for its potential applications in nitrite sensing and hydrogen production by utilizing diverse electrochemical methodologies. The Co<sub>2</sub>O<sub>3</sub>-Chitosan that has been modified exhibits a linear detection range of 0.25–100 µM and a limit of detection (LOD) of 0.117 µM with a response time of approximately 5 s using the amperometry technique. Furthermore, the utilization of Co<sub>2</sub>O<sub>3</sub>-Chitosan composite as a proficient catalyst for hydrogen generation in an alkaline environment was implemented. The electrode exhibited enduring stability in fuel generation and heightened energy safeguarding. The current density of the electrode was observed to attain a value of <span>(upeta)</span> <sub>50</sub> at − 0.55 and − 0.43 V (versus RHE) for Co<sub>2</sub>O<sub>3</sub> and Co@Chitosan, respectively. The study investigated the durability of electrodes during extended periods of constant potential chronoamperometry lasting 6 h. The Co<sub>2</sub>O<sub>3</sub> and Co@Chitosan exhibited a reduction in initial current by 11% and 7%, respectively.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":535,"journal":{"name":"Electrocatalysis","volume":"15 6","pages":"496 - 506"},"PeriodicalIF":2.7,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142438820","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-25DOI: 10.1007/s12678-024-00890-x
Pheladi L. Mokaba, Nolwazi T. Gazu, Marang L. Makinita, Nomcebo H. Mthombeni, Pinkie Ntola, Usisipho Feleni
In recent years, the development of highly sensitive and selective electrochemical sensors has been a pivotal area of research, driven by the growing demand for environmental monitoring and industrial process control. Among various materials investigated for sensor applications, manganese oxide (MnO2) nanoparticles have garnered significant attention due to their excellent electrochemical properties, environmental friendliness, and natural abundance. Critical analyses of the synthesis of MnO2 using different techniques such as hydrothermal method, chemical precipitation, and sol–gel process which allows for the fine-tuning of particle size and morphology while enhancing the electrochemical sensing capabilities have been reviewed. The review also provides a comprehensive overview of the recent advancement evaluation of manganese oxide-based electrodes for detecting sulfonamides and other analytes in water across diverse matrices. This paper sets the stage for a comprehensive exploration of the synthesis methods and application areas of MnO2 nanoparticles in electrochemical sensors, highlighting their role in advancing sensor technology and their impact on various sectors.
{"title":"Manganese Oxide Applications in Sulfonamides Electrochemical, Thermal and Optical Sensors: A Short Review","authors":"Pheladi L. Mokaba, Nolwazi T. Gazu, Marang L. Makinita, Nomcebo H. Mthombeni, Pinkie Ntola, Usisipho Feleni","doi":"10.1007/s12678-024-00890-x","DOIUrl":"10.1007/s12678-024-00890-x","url":null,"abstract":"<div><p>In recent years, the development of highly sensitive and selective electrochemical sensors has been a pivotal area of research, driven by the growing demand for environmental monitoring and industrial process control. Among various materials investigated for sensor applications, manganese oxide (MnO<sub>2</sub>) nanoparticles have garnered significant attention due to their excellent electrochemical properties, environmental friendliness, and natural abundance. Critical analyses of the synthesis of MnO<sub>2</sub> using different techniques such as hydrothermal method, chemical precipitation, and sol–gel process which allows for the fine-tuning of particle size and morphology while enhancing the electrochemical sensing capabilities have been reviewed. The review also provides a comprehensive overview of the recent advancement evaluation of manganese oxide-based electrodes for detecting sulfonamides and other analytes in water across diverse matrices. This paper sets the stage for a comprehensive exploration of the synthesis methods and application areas of MnO<sub>2</sub> nanoparticles in electrochemical sensors, highlighting their role in advancing sensor technology and their impact on various sectors.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":535,"journal":{"name":"Electrocatalysis","volume":"15 6","pages":"421 - 437"},"PeriodicalIF":2.7,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s12678-024-00890-x.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142438756","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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