Pub Date : 2025-02-01DOI: 10.1016/j.jelechem.2024.118884
Yan-Ping Liu , Ji-Huan He
A variety of nonlinear differential models exist for reaction kinetics. Although exact or approximate solutions might not be the main focus in practical applications, the slope at a specific point holds great physical significance and an accurate estimate is crucial. This paper introduces two novel concepts: the point solution and the point slope. These are based on the idea that the accuracy of a particular point is notably higher than that of other points within the solution domain. The paper uses non-Michaelis-Menten kinetics as an example to explain the methodology for obtaining an accurate point slope for the amperometric current response. Moreover, the main factors influencing the response are clearly shown through a closed and simple mathematical formulation. The effectiveness and advantages of this technique are demonstrated by comparing the results with those in existing literature. For the chemistry field to leverage the potential of this approach, this article can serve as a model for practical applications.
{"title":"A fast and accurate estimation of amperometric current response in reaction kinetics","authors":"Yan-Ping Liu , Ji-Huan He","doi":"10.1016/j.jelechem.2024.118884","DOIUrl":"10.1016/j.jelechem.2024.118884","url":null,"abstract":"<div><div>A variety of nonlinear differential models exist for reaction kinetics. Although exact or approximate solutions might not be the main focus in practical applications, the slope at a specific point holds great physical significance and an accurate estimate is crucial. This paper introduces two novel concepts: the point solution and the point slope. These are based on the idea that the accuracy of a particular point is notably higher than that of other points within the solution domain. The paper uses non-Michaelis-Menten kinetics as an example to explain the methodology for obtaining an accurate point slope for the amperometric current response. Moreover, the main factors influencing the response are clearly shown through a closed and simple mathematical formulation. The effectiveness and advantages of this technique are demonstrated by comparing the results with those in existing literature. For the chemistry field to leverage the potential of this approach, this article can serve as a model for practical applications.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"978 ","pages":"Article 118884"},"PeriodicalIF":4.1,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143093022","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 : 2025-02-01DOI: 10.1016/j.jelechem.2024.118852
Saule Gizatova, Ayça Demirel Özel
This study represents the first investigation into the fabrication of paper-based thiocyanate-selective potentiometric nanosensor, employing a palladium(II) complex as an ionophore. The construction of a new disposable, environmentally friendly and cost-effective sensing platform and the optimization of both nanocomposite ink suspension containing multi-walled carbon nanotubes (MWCNTs) and NiO nanoparticles (NiONPs) used to achieve conductive paper and thiocyanate-selective membrane cocktail deposited onto the paper substrate using a drop-casting technique were described. Electrochemical impedance spectroscopy (EIS) and potentiometric measurements were examined to identify the appropriate ink and selective membrane compositions resulting in best analytical performances such as Nernstian slope of 59.0 ± 0.8 mV/pSCN with 6.7 nM limit of detection (LOD) in linear range of 1.0 × 10−6- 1.0 × 10−1 M at pH = 2.0. EIS was also used for characterization of membrane-solution interface to confirm interaction between analyte and the ionophore in the organic membrane phase. Water-layer test was performed to evaluate membrane adherence to the conductive paper substrate by chronopotentiometric method. Assessment of the selectivity coefficients determined through the separate solution methodology indicated that the developed nanosensor displayed a highly selective interaction with thiocyanate in comparison to the other anions that were tested. Finally, the repeatability, reproducibility and analytical applicability of the proposed sensor were studied. Artificial saliva, mustard seed and veterinary drug were selected as real sample examples to prove its successful use as an indicator electrode.
{"title":"Cost-effective and highly selective paper-based potentiometric thiocyanate nanosensor employing nanocomposite for substrate preparation","authors":"Saule Gizatova, Ayça Demirel Özel","doi":"10.1016/j.jelechem.2024.118852","DOIUrl":"10.1016/j.jelechem.2024.118852","url":null,"abstract":"<div><div>This study represents the first investigation into the fabrication of paper-based thiocyanate-selective potentiometric nanosensor, employing a palladium(II) complex as an ionophore. The construction of a new disposable, environmentally friendly and cost-effective sensing platform and the optimization of both nanocomposite ink suspension containing multi-walled carbon nanotubes (MWCNTs) and NiO nanoparticles (NiONPs) used to achieve conductive paper and thiocyanate-selective membrane cocktail deposited onto the paper substrate using a drop-casting technique were described. Electrochemical impedance spectroscopy (EIS) and potentiometric measurements were examined to identify the appropriate ink and selective membrane compositions resulting in best analytical performances such as Nernstian slope of 59.0 ± 0.8 mV/pSCN<!--> <!-->with 6.7 nM limit of detection (LOD) in linear range of 1.0 × 10<sup>−6</sup>- 1.0 × 10<sup>−1</sup> M at pH = 2.0. EIS was also used for characterization of membrane-solution interface to confirm interaction between analyte and the ionophore in the organic membrane phase. Water-layer test was performed to evaluate membrane adherence to the conductive paper substrate by chronopotentiometric method. Assessment of the selectivity coefficients determined through the separate solution methodology indicated that the developed nanosensor displayed a highly selective interaction with thiocyanate in comparison to the other anions that were tested. Finally, the repeatability, reproducibility and analytical applicability of the proposed sensor were studied. Artificial saliva,<!--> <!-->mustard seed and veterinary drug were selected as real sample examples to prove its successful use as an indicator electrode.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"978 ","pages":"Article 118852"},"PeriodicalIF":4.1,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143092100","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}
The quest for highly effective and durable electrocatalysts for methanol oxidation remains a contemporary research endeavour in the direct methanol fuel cells (DMFC) domain. Pt-based electrocatalysts remain the front-runner in DMFC due to their exceptional catalytic performance and stability irrespective of cost. In this regard, the present investigation delves into tuning the inherent synergy of the Au/Pt bi-metallic catalytic system by switching the gold (Au) and platinum (Pt) nanocatalyst layers toward boosting methanol electro-oxidation. The sequential electrodeposition strategy was adopted to form distinct catalyst models; Pt on Au (Au/Pt), Au on Pt (Pt/Au), and Au–Pt alloy. Interestingly, switching the outer layer of Au into Pt nanostructures via changing the order of electrodeposition (Pt/Au to Au/Pt), the resulting Au/Pt electrocatalyst exhibits remarkable efficiency and long-term durability regarding methanol oxidation reaction in comparison with mono-metallic Pt and commercial Pt–C. The synergistic effect attained by tuning Au/Pt catalyst layers arises from the following fact that the top Pt layer favours the direct methanol adsorption and its oxidation, while the underlying Au assists the transformation of electroformed CO-like intermediate species into CO2 and protects the Pt surface from the CO surface poisoning, which makes present catalyst perform better for long duration.
{"title":"Exploring the synergistic impact of switched gold and platinum nanocatalyst layers towards methanol electrooxidation reaction","authors":"Raman Kumar , Perumal Viswanathan , Kyuwon Kim , Shanmugam Manivannan","doi":"10.1016/j.jelechem.2024.118905","DOIUrl":"10.1016/j.jelechem.2024.118905","url":null,"abstract":"<div><div>The quest for highly effective and durable electrocatalysts for methanol oxidation remains a contemporary research endeavour in the direct methanol fuel cells (DMFC) domain. Pt-based electrocatalysts remain the front-runner in DMFC due to their exceptional catalytic performance and stability irrespective of cost. In this regard, the present investigation delves into tuning the inherent synergy of the Au/Pt bi-metallic catalytic system by switching the gold (Au) and platinum (Pt) nanocatalyst layers toward boosting methanol electro-oxidation. The sequential electrodeposition strategy was adopted to form distinct catalyst models; Pt on Au (Au/Pt), Au on Pt (Pt/Au), and Au–Pt alloy. Interestingly, switching the outer layer of Au into Pt nanostructures via changing the order of electrodeposition (Pt/Au to Au/Pt), the resulting Au/Pt electrocatalyst exhibits remarkable efficiency and long-term durability regarding methanol oxidation reaction in comparison with mono-metallic Pt and commercial Pt–C. The synergistic effect attained by tuning Au/Pt catalyst layers arises from the following fact that the top Pt layer favours the direct methanol adsorption and its oxidation, while the underlying Au assists the transformation of electroformed CO-like intermediate species into CO<sub>2</sub> and protects the Pt surface from the CO surface poisoning, which makes present catalyst perform better for long duration.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"978 ","pages":"Article 118905"},"PeriodicalIF":4.1,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143092102","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 : 2025-02-01DOI: 10.1016/j.jelechem.2024.118889
Haoming Xiao , Fujian Wang , Jun Peng , Junhui Luo , Hongquan Li , Ziheng Wang , Xianyou Luo , Yong Chen
Hard carbon is recognized as a highly promising anode material for sodium-ion batteries (SIBs), with its microstructure playing a critical role in determining Na+ storage performance. Despite recent advancements in improving the Na+ storage capabilities of hard carbon, significant challenges remain in optimizing these materials. In this study, zinc-modified hard carbon was synthesized using coconut shells as the carbon source and ZnCl2 as a modifier. The introduction of ZnCl2 effectively expanded the graphite interlayer spacing, reduced microcrystal size, and created closed pores, leading to significantly enhanced Na+ storage performance. Consequently, the ZnCl2-modified hard carbon exhibited a high reversible capacity of 352.0 mAh/g, with a plateau capacity of 242.6 mAh/g, outperforming the unmodified hard carbon (294.4 mAh/g and 199.8 mAh/g, respectively). Additionally, the modified material showed superior rate performance and cycling stability. The Na+ storage mechanism in the ZnCl2-modified carbon aligns with the “adsorption-intercalation-filling” model. This study highlights the effectiveness of ZnCl2 modification in enhancing Na+ storage, providing a promising strategy for the development of high-performance hard carbon anodes in SIBs.
{"title":"Zinc-assisted modification of hard carbon for enhanced sodium-ion storage","authors":"Haoming Xiao , Fujian Wang , Jun Peng , Junhui Luo , Hongquan Li , Ziheng Wang , Xianyou Luo , Yong Chen","doi":"10.1016/j.jelechem.2024.118889","DOIUrl":"10.1016/j.jelechem.2024.118889","url":null,"abstract":"<div><div>Hard carbon is recognized as a highly promising anode material for sodium-ion batteries (SIBs), with its microstructure playing a critical role in determining Na<sup>+</sup> storage performance. Despite recent advancements in improving the Na<sup>+</sup> storage capabilities of hard carbon, significant challenges remain in optimizing these materials. In this study, zinc-modified hard carbon was synthesized using coconut shells as the carbon source and ZnCl<sub>2</sub> as a modifier. The introduction of ZnCl<sub>2</sub> effectively expanded the graphite interlayer spacing, reduced microcrystal size, and created closed pores, leading to significantly enhanced Na<sup>+</sup> storage performance. Consequently, the ZnCl<sub>2</sub>-modified hard carbon exhibited a high reversible capacity of 352.0 mAh/g, with a plateau capacity of 242.6 mAh/g, outperforming the unmodified hard carbon (294.4 mAh/g and 199.8 mAh/g, respectively). Additionally, the modified material showed superior rate performance and cycling stability. The Na<sup>+</sup> storage mechanism in the ZnCl<sub>2</sub>-modified carbon aligns with the “adsorption-intercalation-filling” model. This study highlights the effectiveness of ZnCl<sub>2</sub> modification in enhancing Na<sup>+</sup> storage, providing a promising strategy for the development of high-performance hard carbon anodes in SIBs.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"978 ","pages":"Article 118889"},"PeriodicalIF":4.1,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143101466","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 : 2025-02-01DOI: 10.1016/j.jelechem.2024.118887
Elena B. Molodkina, Alexander V. Rudnev, Maria R. Ehrenburg
Deep eutectic solvents (DES) are a special class of solvents with specific properties that offer new possibilities for the electroplating of metals and alloys. Ethaline – a mixture of choline chloride and ethylene glycol (EG) – is one of the less viscous DES, which makes it a commonly used medium for studying electrodeposition. The understanding of the metal electrodeposition behavior is much advanced by the data on structural sensitivity obtained with the help of single crystal electrodes. This work is continuation of a previous study on Ag electrosorption and phase deposition on Pt(111) in ethaline. We extend our studies to other basal single crystal surfaces, Pt(100) and Pt(110). Also, with account for the more pronounced sensitivity of these faces to the laboratory atmosphere as compared to Pt(111) and also with regard to the previously obtained data on the possibility of spontaneous EG decomposition on Pt with formation of a CO-like adspecies, we suggest an EG–protection step in the Pt(hkl) pretreatment procedure. We compare the data on Ag electrosorption and phase deposition on the three basal single crystal surfaces pretreated by EG (EG-protected) as opposed to surfaces with no such pretreatment (unprotected). We demonstrate that the EG-protection step results in the surface poisoning by the blocking adspecies. This brings about a significant lowering of the capacitance currents and the currents related to specific adsorption of ethaline components and Ag underpotential deposition (upd) as compared to those on unprotected Pt(hkl). We also show that phase deposition of silver from ethaline on Pt(hkl) starts at almost zero overpotentials on all electrodes except for EG-protected Pt(110), which is probably related to the presence of the already deposited Ag adlayer (for unprotected electrodes) and Ag adlayer patches (for EG-protected ones). In general, Ag deposition occurs via the Stranski–Krastanov mode. Deposition on unprotected electrodes involves simultaneous 2D and 3D deposit formation, while the deposit obtained at moderate overpotentials on all EG-pretreated electrodes contains well-pronounced individual shaped crystallites.
{"title":"Influence of pretreatment conditions on underpotential and phase deposition of silver on Pt(hkl) single crystal substrates in ethaline","authors":"Elena B. Molodkina, Alexander V. Rudnev, Maria R. Ehrenburg","doi":"10.1016/j.jelechem.2024.118887","DOIUrl":"10.1016/j.jelechem.2024.118887","url":null,"abstract":"<div><div>Deep eutectic solvents (DES) are a special class of solvents with specific properties that offer new possibilities for the electroplating of metals and alloys. Ethaline – a mixture of choline chloride and ethylene glycol (EG) – is one of the less viscous DES, which makes it a commonly used medium for studying electrodeposition. The understanding of the metal electrodeposition behavior is much advanced by the data on structural sensitivity obtained with the help of single crystal electrodes. This work is continuation of a previous study on Ag electrosorption and phase deposition on Pt(111) in ethaline. We extend our studies to other basal single crystal surfaces, Pt(100) and Pt(110). Also, with account for the more pronounced sensitivity of these faces to the laboratory atmosphere as compared to Pt(111) and also with regard to the previously obtained data on the possibility of spontaneous EG decomposition on Pt with formation of a CO-like adspecies, we suggest an EG–protection step in the Pt(hkl) pretreatment procedure. We compare the data on Ag electrosorption and phase deposition on the three basal single crystal surfaces pretreated by EG (EG-protected) as opposed to surfaces with no such pretreatment (unprotected). We demonstrate that the EG-protection step results in the surface poisoning by the blocking adspecies. This brings about a significant lowering of the capacitance currents and the currents related to specific adsorption of ethaline components and Ag underpotential deposition (upd) as compared to those on unprotected Pt(hkl). We also show that phase deposition of silver from ethaline on Pt(hkl) starts at almost zero overpotentials on all electrodes except for EG-protected Pt(110), which is probably related to the presence of the already deposited Ag adlayer (for unprotected electrodes) and Ag adlayer patches (for EG-protected ones). In general, Ag deposition occurs via the Stranski–Krastanov mode. Deposition on unprotected electrodes involves simultaneous 2D and 3D deposit formation, while the deposit obtained at moderate overpotentials on all EG-pretreated electrodes contains well-pronounced individual shaped crystallites.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"978 ","pages":"Article 118887"},"PeriodicalIF":4.1,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143101482","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 : 2025-02-01DOI: 10.1016/j.jelechem.2024.118874
Yihan Deng , Zhaoxin Li , Huayi Tan , Shili Zheng , Bingqiang Fan , Yang Zhang
Iron–chromium redox flow batteries (ICRFBs) are attractive potential long-duration energy storage facilities because of their extensive sources and low cost. However, the hydrogen evolution reaction (HER) causes irreversible capacity loss and limits its application. Herein, we explore the influence of organic compounds containing imidazole groups, such as l-histidine (l-his) and 2-methylimidazole (2-mIm), on the performance of negative iron–chromium electrolytes. The results of molecular dynamics and density functional theory calculations revealed that both additives can interact with chromium ions to regulate the solvation shell and that the new complex structures have greater hydrogen evolution barriers. The electrochemical test results show that 2-mIm has a more significant influence than l-his dose. The findings of the single battery tests with two additives indicate that both additives improve the coulombic efficiency (CE) and average decay rate of ICRFB. The capacity decay rate of ICRFB with the electrolyte containing 0.2 M 2-mIm reached 1.79 %. Compared with that of the pure electrolyte, the capacity decay rate is reduced by 76 % in the 0.2 M 2-mIm electrolyte. It achieves a CE of 97.8 % at a current density of 100 mA·cm−2. Furthermore, UV–Vis spectroscopy and long-cycle tests revealed that new complex structures are present and stable during battery operation. Finally, the in situ Raman results show that additives can reduce the amount of water and disrupt the hydrogen bond network around the surface of the electrode during energization. The improvement in the hydrogen evolution barrier and Raman results explain the mechanism by which the HER is suppressed. This study provides a feasible rationale for additive selection.
{"title":"Suppression of the hydrogen evolution reaction of Iron–chromium flow batteries by organic compounds containing the imidazole group","authors":"Yihan Deng , Zhaoxin Li , Huayi Tan , Shili Zheng , Bingqiang Fan , Yang Zhang","doi":"10.1016/j.jelechem.2024.118874","DOIUrl":"10.1016/j.jelechem.2024.118874","url":null,"abstract":"<div><div>Iron–chromium redox flow batteries (ICRFBs) are attractive potential long-duration energy storage facilities because of their extensive sources and low cost. However, the hydrogen evolution reaction (HER) causes irreversible capacity loss and limits its application. Herein, we explore the influence of organic compounds containing imidazole groups, such as <span>l</span>-histidine (<span>l</span>-his) and 2-methylimidazole (2-mIm), on the performance of negative iron–chromium electrolytes. The results of molecular dynamics and density functional theory calculations revealed that both additives can interact with chromium ions to regulate the solvation shell and that the new complex structures have greater hydrogen evolution barriers. The electrochemical test results show that 2-mIm has a more significant influence than <span>l</span>-his dose. The findings of the single battery tests with two additives indicate that both additives improve the coulombic efficiency (CE) and average decay rate of ICRFB. The capacity decay rate of ICRFB with the electrolyte containing 0.2 M 2-mIm reached 1.79 %. Compared with that of the pure electrolyte, the capacity decay rate is reduced by 76 % in the 0.2 M 2-mIm electrolyte. It achieves a CE of 97.8 % at a current density of 100 mA·cm<sup>−2</sup>. Furthermore, UV–Vis spectroscopy and long-cycle tests revealed that new complex structures are present and stable during battery operation. Finally, the in situ Raman results show that additives can reduce the amount of water and disrupt the hydrogen bond network around the surface of the electrode during energization. The improvement in the hydrogen evolution barrier and Raman results explain the mechanism by which the HER is suppressed. This study provides a feasible rationale for additive selection.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"978 ","pages":"Article 118874"},"PeriodicalIF":4.1,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143101485","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 : 2025-02-01DOI: 10.1016/j.jelechem.2024.118885
Lanyang Feng, Yao Xu, Juan Wu, Bencai Lin
In this study, a series of high-performance semi-interpenetrating polymer network (sIPN)-based gel polymer electrolytes (GPEs) were prepared using UV-initiated polymerization of unsaturated-bond-containing ethylene oxide oligomers (specifically poly(ethylene glycol) methyl ether methacrylate(PEGMAMA) and poly(ethylene glycol) diacrylate(PEGDA)), followed by blending with linear poly(vinylidene fluoride-co-hexafluoropropylene)(PVDF-HFP). PEGDA was used as the crosslinking agent to form a crosslinked structure with PEGMAMA. This unique architecture not only provided abundant ethylene oxide chain segments but also disrupted the crystallinity of PVDF-HFP. The sIPNs structure imparts GPEs with high thermal stabilities and robust mechanical properties. Among the sIPN-based GPEs, PP2P3-IL exhibited a high conductivity of 1.05 × 10−3 S cm−1. Owing to the excellent dissociation ability of the sIPNs structure toward Li salts, PP2P3-IL shows a high Li-ion transference number of 0.68. The Li|PP2P3-IL|Li battery maintained a low steady-state overpotential, even after 800 h. Moreover, the discharge capacity of the Li/LiFePO4 battery reached 150 mAh g−1, and its capacity retention higher than 95 % even after 100 cycles, demonstrating its strong potential for application in Li-ion battery.
{"title":"Semi-interpenetrating polymer network-based gel polymer electrolytes for Li-ion batteries applications","authors":"Lanyang Feng, Yao Xu, Juan Wu, Bencai Lin","doi":"10.1016/j.jelechem.2024.118885","DOIUrl":"10.1016/j.jelechem.2024.118885","url":null,"abstract":"<div><div>In this study, a series of high-performance semi-interpenetrating polymer network (sIPN)-based gel polymer electrolytes (GPEs) were prepared using UV-initiated polymerization of unsaturated-bond-containing ethylene oxide oligomers (specifically poly(ethylene glycol) methyl ether methacrylate(PEGMAMA) and poly(ethylene glycol) diacrylate(PEGDA)), followed by blending with linear poly(vinylidene fluoride-<em>co</em>-hexafluoropropylene)(PVDF-HFP). PEGDA was used as the crosslinking agent to form a crosslinked structure with PEGMAMA. This unique architecture not only provided abundant ethylene oxide chain segments but also disrupted the crystallinity of PVDF-HFP. The sIPNs structure imparts GPEs with high thermal stabilities and robust mechanical properties. Among the sIPN-based GPEs, PP<sub>2</sub>P<sub>3</sub>-IL exhibited a high conductivity of 1.05 × 10<sup>−3</sup> S cm<sup>−1</sup>. Owing to the excellent dissociation ability of the sIPNs structure toward Li salts, PP<sub>2</sub>P<sub>3</sub>-IL shows a high Li-ion transference number of 0.68. The Li|PP<sub>2</sub>P<sub>3</sub>-IL|Li battery maintained a low steady-state overpotential, even after 800 h. Moreover, the discharge capacity of the Li/LiFePO<sub>4</sub> battery reached 150 mAh g<sup>−1</sup>, and its capacity retention higher than 95 % even after 100 cycles, demonstrating its strong potential for application in Li-ion battery.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"978 ","pages":"Article 118885"},"PeriodicalIF":4.1,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143101489","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 : 2025-02-01DOI: 10.1016/j.jelechem.2024.118867
Marjorie Montero-Jimenez , Jael R. Neyra Recky , Catalina von Bilderling , Juliana Scotto , Omar Azzaroni , Waldemar A. Marmisollé
We present the development of enzymatic PEDOT-PAH-based (polyethylenedioxythiophene-polyallylamine hydrochloride) organic electrochemical transistors (OECTs) for glucose detection in human urine samples via direct immobilization of glucose oxidase (GOx) onto PEDOT-PAH via electrostatic interactions. An alternative method for recording OECT responses was introduced, involving continuous switching of gate potential and subsequent data processing, which becomes effective for monitoring protein adsorption and reconstructing temporal response curves to analyte injections. Investigation into the sensing mechanism revealed the pivotal role of pH changes induced by enzymatic catalysis in the transistor response. Evaluation of OECT performance in media with higher ionic strength and buffering capacity demonstrated glucose sensing even in complex biological matrices, including promising results in human urine samples with sensitive response up to 2 mM spiked glucose concentration. These findings not only underscore the functionality of the proposed glucose sensor but also highlight the potential of enzymatic OECT-based sensors for biosensing applications in real biological media.
{"title":"PEDOT: Tosylate-polyamine-based enzymatic organic electrochemical transistors for high-performance glucose biosensing in human urine samples","authors":"Marjorie Montero-Jimenez , Jael R. Neyra Recky , Catalina von Bilderling , Juliana Scotto , Omar Azzaroni , Waldemar A. Marmisollé","doi":"10.1016/j.jelechem.2024.118867","DOIUrl":"10.1016/j.jelechem.2024.118867","url":null,"abstract":"<div><div>We present the development of enzymatic PEDOT-PAH-based (polyethylenedioxythiophene-polyallylamine hydrochloride) organic electrochemical transistors (OECTs) for glucose detection in human urine samples via direct immobilization of glucose oxidase (GOx) onto PEDOT-PAH via electrostatic interactions. An alternative method for recording OECT responses was introduced, involving continuous switching of gate potential and subsequent data processing, which becomes effective for monitoring protein adsorption and reconstructing temporal response curves to analyte injections. Investigation into the sensing mechanism revealed the pivotal role of pH changes induced by enzymatic catalysis in the transistor response. Evaluation of OECT performance in media with higher ionic strength and buffering capacity demonstrated glucose sensing even in complex biological matrices, including promising results in human urine samples with sensitive response up to 2 mM spiked glucose concentration. These findings not only underscore the functionality of the proposed glucose sensor but also highlight the potential of enzymatic OECT-based sensors for biosensing applications in real biological media.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"978 ","pages":"Article 118867"},"PeriodicalIF":4.1,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143128315","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}
The key to promoting the four-electron pathway towards oxygen reduction reaction (ORR) lies in the design of efficient electrocatalysts. This study elucidated the impact of MnO2 morphology and the combination of MnO2 and N-doped coconut shell charcoal (NCSC) on generation of oxygen vacancies in MnO2, thereby triggering the formation of active sites. The XPS analysis reveals that MnO2-NW/NCSC possesses a higher concentration of oxygen vacancies, which facilitates the formation of surface oxygen adsorption centers. The MnO2-NW/NCSC exhibits remarkable ORR activity with high initial potential (Eonset = 0.92 vs. RHE), half-wave potential (E1/2 = 0.82 vs. RHE), diffusion-limited current density, and long-term durability. Moreover, the introduction of additional oxygen vacancies in MnO2 can facilitate the decomposition of intermediates, thereby intensifying the O2 reaction to OH− and ultimately enhancing the ORR activity of MnO2-NW/NCSC. By analyzing experimental results, this discovery highlights an extremely effective approach for investigating ORR catalysts with enhanced performance and durability.
{"title":"MnO2 nanowires with abundant oxygen vacancies loaded to NCSC for the synergistically enhanced oxygen reduction reaction","authors":"Aiai Zhang , Chunli Li , Zheng Liu, Shisi Yuan, Fengzhen Zhang","doi":"10.1016/j.jelechem.2025.118976","DOIUrl":"10.1016/j.jelechem.2025.118976","url":null,"abstract":"<div><div>The key to promoting the four-electron pathway towards oxygen reduction reaction (ORR) lies in the design of efficient electrocatalysts. This study elucidated the impact of MnO<sub>2</sub> morphology and the combination of MnO<sub>2</sub> and <em>N</em>-doped coconut shell charcoal (NCSC) on generation of oxygen vacancies in MnO<sub>2</sub>, thereby triggering the formation of active sites. The XPS analysis reveals that MnO<sub>2</sub>-NW/NCSC possesses a higher concentration of oxygen vacancies, which facilitates the formation of surface oxygen adsorption centers. The MnO<sub>2</sub>-NW/NCSC exhibits remarkable ORR activity with high initial potential (<em>E</em><sub>onset</sub> = 0.92 <em>vs</em>. RHE), half-wave potential (<em>E</em><sub>1/2</sub> = 0.82 <em>vs</em>. RHE), diffusion-limited current density, and long-term durability. Moreover, the introduction of additional oxygen vacancies in MnO<sub>2</sub> can facilitate the decomposition of intermediates, thereby intensifying the O<sub>2</sub> reaction to OH<sup>−</sup> and ultimately enhancing the ORR activity of MnO<sub>2</sub>-NW/NCSC. By analyzing experimental results, this discovery highlights an extremely effective approach for investigating ORR catalysts with enhanced performance and durability.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"981 ","pages":"Article 118976"},"PeriodicalIF":4.1,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143096681","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 : 2025-02-01DOI: 10.1016/j.jelechem.2024.118909
Jiuqing Xiong , Yifan Wang , Jingjing Wu , Shihai Yan , Bingping Liu
The electrocatalytic reduction of nitrate (NO3−RR) to ammonia under mild conditions reduces energy consumption and helps to decrease greenhouse gas emissions, thus protecting the ecological environment. However, this reaction faces challenges such as low yield and low Faradaic efficiency (FE). Designing high-performance catalysts to improve ammonia (NH3) yield and FE is an important pathway for NO3−RR. In this paper, a novel catalyst is synthesized by doping amorphous iron onto TiO2/Ti nanosheets, which maintains the morphology of the TiO2/Ti nanosheets while enhancing catalytic performance. The highest FE of this catalyst reaches 97.67 % at −0.4 V (vs. RHE), with an NH3 yield of 23.11 mg h−1 cm−2 at −0.7 V (vs. RHE). Additionally, this catalyst exhibits excellent stability and selectivity, outperforming most currently reported catalysts. Density functional theory calculations indicate that the doping of Fe in TiO2/Ti leads to a lower bandgap, thereby improving the conductivity. In addition, the calculations show that Fe plays a significant role in structural adjustment and charge transfer during the catalytic process, reducing the energy barrier of the reaction and facilitating the NO3−RR. This study suggests that the Fe-doped TiO2/Ti nanosheets has great potential in the fields of NH3 synthesis and wastewater treatment.
{"title":"Amorphous Fe-doped TiO2 nanosheet arrays: A catalyst for efficient nitrate reduction to ammonia","authors":"Jiuqing Xiong , Yifan Wang , Jingjing Wu , Shihai Yan , Bingping Liu","doi":"10.1016/j.jelechem.2024.118909","DOIUrl":"10.1016/j.jelechem.2024.118909","url":null,"abstract":"<div><div>The electrocatalytic reduction of nitrate (NO<sub>3</sub><sup>−</sup>RR) to ammonia under mild conditions reduces energy consumption and helps to decrease greenhouse gas emissions, thus protecting the ecological environment. However, this reaction faces challenges such as low yield and low Faradaic efficiency (FE). Designing high-performance catalysts to improve ammonia (NH<sub>3</sub>) yield and FE is an important pathway for NO<sub>3</sub><sup>−</sup>RR. In this paper, a novel catalyst is synthesized by doping amorphous iron onto TiO<sub>2</sub>/Ti nanosheets, which maintains the morphology of the TiO<sub>2</sub>/Ti nanosheets while enhancing catalytic performance. The highest FE of this catalyst reaches 97.67 % at −0.4 V (vs. RHE), with an NH<sub>3</sub> yield of 23.11 mg h<sup>−1</sup> cm<sup>−2</sup> at −0.7 V (vs. RHE). Additionally, this catalyst exhibits excellent stability and selectivity, outperforming most currently reported catalysts. Density functional theory calculations indicate that the doping of Fe in TiO<sub>2</sub>/Ti leads to a lower bandgap, thereby improving the conductivity. In addition, the calculations show that Fe plays a significant role in structural adjustment and charge transfer during the catalytic process, reducing the energy barrier of the reaction and facilitating the NO<sub>3</sub><sup>−</sup>RR. This study suggests that the Fe-doped TiO<sub>2</sub>/Ti nanosheets has great potential in the fields of NH<sub>3</sub> synthesis and wastewater treatment.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"978 ","pages":"Article 118909"},"PeriodicalIF":4.1,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143092101","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}
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