Pub Date : 2025-01-06DOI: 10.1016/j.electacta.2025.145659
Minal A. Bhatt, Ashish R. Tanna
The Li-ion doping in V₂O₅ leads to structural distortion, which results in modifications to the optical and electrical properties of the material. The X-ray diffractometer (XRD) measurement reveals orthorhombic and monoclinic structures for the present system. There is a significant change in the optical energy band which decreases from 3.37 eV to 2.44 eV, evaluated from Tauc extrapolation. The relation between energy band gap and refractive index is derived using different theoretical fitting formulas. The Reflectivity, reflection loss, and transmission coefficient values gradually decrease as Li-ion content increases. The molar refractive index (Rm) and molar electronic polarizability (αe) decrease from 29.99 cm3/mol to 28.54 cm3/mol and 11.893Å3 to 11.318Å3, respectively. The complex impedance and modulus spectra evaluate the electrical and dielectric properties of the vanadium pentoxide. The equivalent circuits have been analyzed for the complex dielectric parameters using Cole-Cole plots, and the electrical modulus shows the non-Debye type relaxation process. The analysis demonstrates the vital role of these materials in future electrochromic smart window devices (EC-SM) and optoelectronic applications.
{"title":"Ramification of Li-ion array on structural, optical and electrical properties of vanadium pentoxide for energy-efficient material","authors":"Minal A. Bhatt, Ashish R. Tanna","doi":"10.1016/j.electacta.2025.145659","DOIUrl":"https://doi.org/10.1016/j.electacta.2025.145659","url":null,"abstract":"The Li-ion doping in V₂O₅ leads to structural distortion, which results in modifications to the optical and electrical properties of the material. The X-ray diffractometer (XRD) measurement reveals orthorhombic and monoclinic structures for the present system. There is a significant change in the optical energy band which decreases from 3.37 eV to 2.44 eV, evaluated from Tauc extrapolation. The relation between energy band gap and refractive index is derived using different theoretical fitting formulas. The Reflectivity, reflection loss, and transmission coefficient values gradually decrease as Li-ion content increases. The molar refractive index (R<sub>m</sub>) and molar electronic polarizability (α<sub>e</sub>) decrease from 29.99 cm<sup>3</sup>/mol to 28.54 cm<sup>3</sup>/mol and 11.893Å<sup>3</sup> to 11.318Å<sup>3</sup>, respectively. The complex impedance and modulus spectra evaluate the electrical and dielectric properties of the vanadium pentoxide. The equivalent circuits have been analyzed for the complex dielectric parameters using Cole-Cole plots, and the electrical modulus shows the non-Debye type relaxation process. The analysis demonstrates the vital role of these materials in future electrochromic smart window devices (EC-SM) and optoelectronic applications.","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"131 1","pages":""},"PeriodicalIF":6.6,"publicationDate":"2025-01-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142929795","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-06DOI: 10.1016/j.electacta.2024.145619
E. Dehnari, Z. Jamshidi, D. Taherinia
Herein, we report the synthesis and electrochemical characterization of seven ferrocene-terminated self-assembled monolayers (SAMs) on fluorine-doped tin oxide (FTO). The ferrocene surface coverage (ΓFc) of SAMs was systematically varied and its impact on the kinetics of interfacial electron transfer (ET) was investigated by cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS). It was found that as ΓFc gradually declined from ∼8.0 molecules/nm2 (its maximum value) to ∼2.4 molecules/nm2, the standard ET rate constant (, extracted from CV data) slowly declined from 4.9 s-1 to 4.1 s-1. However, with a further decrease in ΓFc, abruptly dropped by ∼2.0 s-1 and remained in the range of 2.2-2.7 s-1. The charge transfer resistance (Rct) of SAMs (determined from EIS data) was also found to follow a trend consistent with the one observed for . Density functional theory (DFT) calculations confirmed that the observed behavior of ET kinetics as a function of ΓFc can be attributed to the favorable interaction between adjacent Fc and Ph groups and the stabilization of the Fc HOMO. Besides exploring ET kinetics, ΓFc data was also employed to evaluate the kinetics of imine condensation reaction at the surface. The corresponding bimolecular rate constant for PhCHO () was found to be ∼6.2 times greater than that of FcCHO ().
{"title":"Electron Transfer Kinetics in Ferrocene-Terminated Self-Assembled Monolayers: The Effect of Ferrocene Surface Coverage Variation","authors":"E. Dehnari, Z. Jamshidi, D. Taherinia","doi":"10.1016/j.electacta.2024.145619","DOIUrl":"https://doi.org/10.1016/j.electacta.2024.145619","url":null,"abstract":"Herein, we report the synthesis and electrochemical characterization of seven ferrocene-terminated self-assembled monolayers (SAMs) on fluorine-doped tin oxide (FTO). The ferrocene surface coverage (Γ<sub>Fc</sub>) of SAMs was systematically varied and its impact on the kinetics of interfacial electron transfer (ET) was investigated by cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS). It was found that as Γ<sub>Fc</sub> gradually declined from ∼8.0 molecules/nm<sup>2</sup> (its maximum value) to ∼2.4 molecules/nm<sup>2</sup>, the standard ET rate constant (<span><span><math><msubsup is=\"true\"><mi is=\"true\">k</mi><mrow is=\"true\"><mtext is=\"true\">ET</mtext></mrow><mn is=\"true\">0</mn></msubsup></math></span><script type=\"math/mml\"><math><msubsup is=\"true\"><mi is=\"true\">k</mi><mrow is=\"true\"><mtext is=\"true\">ET</mtext></mrow><mn is=\"true\">0</mn></msubsup></math></script></span>, extracted from CV data) slowly declined from 4.9 s<sup>-1</sup> to 4.1 s<sup>-1</sup>. However, with a further decrease in Γ<sub>Fc</sub>, <span><span><math><msubsup is=\"true\"><mi is=\"true\">k</mi><mrow is=\"true\"><mtext is=\"true\">ET</mtext></mrow><mn is=\"true\">0</mn></msubsup></math></span><script type=\"math/mml\"><math><msubsup is=\"true\"><mi is=\"true\">k</mi><mrow is=\"true\"><mtext is=\"true\">ET</mtext></mrow><mn is=\"true\">0</mn></msubsup></math></script></span> abruptly dropped by ∼2.0 s<sup>-1</sup> and remained in the range of 2.2-2.7 s<sup>-1</sup>. The charge transfer resistance (<em>R</em><sub>ct</sub>) of SAMs (determined from EIS data) was also found to follow a trend consistent with the one observed for <span><span><math><msubsup is=\"true\"><mi is=\"true\">k</mi><mrow is=\"true\"><mtext is=\"true\">ET</mtext></mrow><mn is=\"true\">0</mn></msubsup></math></span><script type=\"math/mml\"><math><msubsup is=\"true\"><mi is=\"true\">k</mi><mrow is=\"true\"><mtext is=\"true\">ET</mtext></mrow><mn is=\"true\">0</mn></msubsup></math></script></span>. Density functional theory (DFT) calculations confirmed that the observed behavior of ET kinetics as a function of Γ<sub>Fc</sub> can be attributed to the favorable interaction between adjacent Fc and Ph groups and the stabilization of the Fc HOMO. Besides exploring ET kinetics, Γ<sub>Fc</sub> data was also employed to evaluate the kinetics of imine condensation reaction at the surface. The corresponding bimolecular rate constant for PhCHO (<span><span><math><msub is=\"true\"><mi is=\"true\">k</mi><mtext is=\"true\">PhCHO</mtext></msub></math></span><script type=\"math/mml\"><math><msub is=\"true\"><mi is=\"true\">k</mi><mtext is=\"true\">PhCHO</mtext></msub></math></script></span>) was found to be ∼6.2 times greater than that of FcCHO (<span><span><math><msub is=\"true\"><mi is=\"true\">k</mi><mtext is=\"true\">FcCHO</mtext></msub></math></span><script type=\"math/mml\"><math><msub is=\"true\"><mi is=\"true\">k</mi><mtext is=\"true\">FcCHO</mtext></msub></math></script></span>).","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"96 1","pages":""},"PeriodicalIF":6.6,"publicationDate":"2025-01-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142929506","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Creatinine is a product of muscle metabolism in the body, it's normally filtered out by the glomeruli. However, creatinine values will deviate from normal when renal function is disturbed. Therefore, it is of great significance to develop an accurate and sensitive creatinine detection method for the preliminary diagnosis of chronic kidney disease(CKD). In this study, Using 1,3, 5-Benzenetricarboxylic acid as ligand, a bimetallic organic framework ZnNiMOF with large specific surface area was prepared, and composite them with carbon nanotubes (CNT). The ratio of the two metals in the bimetal and the ratio of ZnNiMOF to CNT were also optimized. Finally, the optimal proportion was used as the electrode material for molecular imprinting. A molecularly imprinted electrochemical sensor for the accurate and sensitive detection of creatinine was obtained. The obtained sensor has good sensitivity, detection limit of 0.009 μM, and wide detection range (0.03–400 μM). It also shows excellent performance in the detection of actual urine and sweat samples. This study on the molecular imprinted electrochemical sensor provides a new strategy for the subsequent detection of creatinine.
{"title":"Development of a ZnNiMOF@CNT-based MIP electrochemical sensor: Toward the selective detection of creatinine in urine and saliva","authors":"Shuang Yang, Haifeng Gao, Yukui Tong, Fang Chai, Miaomiao Tian","doi":"10.1016/j.electacta.2025.145665","DOIUrl":"https://doi.org/10.1016/j.electacta.2025.145665","url":null,"abstract":"Creatinine is a product of muscle metabolism in the body, it's normally filtered out by the glomeruli. However, creatinine values will deviate from normal when renal function is disturbed. Therefore, it is of great significance to develop an accurate and sensitive creatinine detection method for the preliminary diagnosis of chronic kidney disease(CKD). In this study, Using 1,3, 5-Benzenetricarboxylic acid as ligand, a bimetallic organic framework ZnNiMOF with large specific surface area was prepared, and composite them with carbon nanotubes (CNT). The ratio of the two metals in the bimetal and the ratio of ZnNiMOF to CNT were also optimized. Finally, the optimal proportion was used as the electrode material for molecular imprinting. A molecularly imprinted electrochemical sensor for the accurate and sensitive detection of creatinine was obtained. The obtained sensor has good sensitivity, detection limit of 0.009 μM, and wide detection range (0.03–400 μM). It also shows excellent performance in the detection of actual urine and sweat samples. This study on the molecular imprinted electrochemical sensor provides a new strategy for the subsequent detection of creatinine.","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"72 1","pages":""},"PeriodicalIF":6.6,"publicationDate":"2025-01-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142925163","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Electroreduction of gas-phase CO2 (CO2RR) to CO is an attractive way to promote sustainable and carbon-neutral economic development. The Ag-based catalysts have demonstrated great potential for CO2RR to CO reaction. Herein, we showed that the Co-doping into Ag catalyst significantly enhanced the performance of CO2RR. Compared with pure Ag catalyst, the FECO for Ag-Co bimetallic catalyst was increased by nearly 30%, reaching 95.3% with high stability at the full-cell potential of −2.1 V in the gas-phase electroreduction system. Based on physicochemical characterizations, we confirmed that the specific Ag-Co bimetallic structure was formed, the interaction between Ag and Co metals increased the electrochemically active surface area and exposed more adsorption and reactive sites. Combined with the DFT calculation results, we revealed that the Co doping regulated the electronic structure around Ag sites, and more electrons transferred from Co to Ag sites, promoting the CO2 adsorption and the formation of key intermediates (*COOH) on catalyst surface, therefore leading to a higher performance for CO2RR to CO.
{"title":"Cobalt doping regulated Ag electronic structure for boosting electroreduction of CO2 to CO at gas-solid interface","authors":"Yu Qin, Weiming Qian, Jianghao Zhang, Xueyan Chen, Min Chen, Xiaoxiao Qin, Changbin Zhang","doi":"10.1016/j.electacta.2024.145637","DOIUrl":"https://doi.org/10.1016/j.electacta.2024.145637","url":null,"abstract":"Electroreduction of gas-phase CO<sub>2</sub> (CO<sub>2</sub>RR) to CO is an attractive way to promote sustainable and carbon-neutral economic development. The Ag-based catalysts have demonstrated great potential for CO<sub>2</sub>RR to CO reaction. Herein, we showed that the Co-doping into Ag catalyst significantly enhanced the performance of CO<sub>2</sub>RR. Compared with pure Ag catalyst, the FE<sub>CO</sub> for Ag-Co bimetallic catalyst was increased by nearly 30%, reaching 95.3% with high stability at the full-cell potential of −2.1 V in the gas-phase electroreduction system. Based on physicochemical characterizations, we confirmed that the specific Ag-Co bimetallic structure was formed, the interaction between Ag and Co metals increased the electrochemically active surface area and exposed more adsorption and reactive sites. Combined with the DFT calculation results, we revealed that the Co doping regulated the electronic structure around Ag sites, and more electrons transferred from Co to Ag sites, promoting the CO<sub>2</sub> adsorption and the formation of key intermediates (*COOH) on catalyst surface, therefore leading to a higher performance for CO<sub>2</sub>RR to CO.","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"126 1","pages":""},"PeriodicalIF":6.6,"publicationDate":"2025-01-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142925137","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-05DOI: 10.1016/j.electacta.2024.145636
Xue Bai, Liyin Bu, Yongqiang Du, Quan Wang
Owing to the internal correction function and good resistance to complex factors, dual-signal electrochemical sensors have abilities to avoid false positives. In this work, Cu-MOF and MnCO3 were combined and further prepared the Cu2+ and Hg2+ dual-signal electrochemical sensor for ultra-sensitive detection of Hg2+. Notably, beyond the commonness of the general MOFs, Cu-MOF could undergo oxidation-reduction to provide an internal reference signal. MnCO3, a porous structure with good electrocatalysis, exhibits an obvious signal amplification effect on the detection of Hg2+. Differential pulse voltammetry was applied for the detection of Hg2+. The current signal of Cu2+ and Hg2+ reduced regularly with Hg2+ concentration decreased. Under optimized conditions, the LOD of Hg2+ was calculated around 6.82 nM with a linear range of 0.10 ∼ 2.50 μM. The proposed sensor was proven to show satisfactory anti-interference, stability, and reliability, which is promising for the ultra-sensitive detection of Hg2+ in real life.
{"title":"Dual-signal electrochemical sensor based on Cu-MOF and MnCO₃ for ultra-sensitive detection of mercury ions in water","authors":"Xue Bai, Liyin Bu, Yongqiang Du, Quan Wang","doi":"10.1016/j.electacta.2024.145636","DOIUrl":"https://doi.org/10.1016/j.electacta.2024.145636","url":null,"abstract":"Owing to the internal correction function and good resistance to complex factors, dual-signal electrochemical sensors have abilities to avoid false positives. In this work, Cu-MOF and MnCO<sub>3</sub> were combined and further prepared the Cu<sup>2+</sup> and Hg<sup>2+</sup> dual-signal electrochemical sensor for ultra-sensitive detection of Hg<sup>2+</sup>. Notably, beyond the commonness of the general MOFs, Cu-MOF could undergo oxidation-reduction to provide an internal reference signal. MnCO<sub>3</sub>, a porous structure with good electrocatalysis, exhibits an obvious signal amplification effect on the detection of Hg<sup>2+</sup>. Differential pulse voltammetry was applied for the detection of Hg<sup>2+</sup>. The current signal of Cu<sup>2+</sup> and Hg<sup>2+</sup> reduced regularly with Hg<sup>2+</sup> concentration decreased. Under optimized conditions, the LOD of Hg<sup>2+</sup> was calculated around 6.82 nM with a linear range of 0.10 ∼ 2.50 μM. The proposed sensor was proven to show satisfactory anti-interference, stability, and reliability, which is promising for the ultra-sensitive detection of Hg<sup>2+</sup> in real life.","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"37 1","pages":""},"PeriodicalIF":6.6,"publicationDate":"2025-01-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142925152","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-05DOI: 10.1016/j.electacta.2025.145664
Jiawen Yin, Shengkang Lu, Hanyang Tong, Jianqian Li, Rentao Cao, Shouhong Li, Wanlei Gao, Jie Zou, Qinghui Jin
The safety of drinking water is the most basic safeguard for the human survival. In-situ and on-line monitoring of tap water is considered an effective method to reduce the harm of tap water pollution, caused by pipeline rupture or leakage. However, a sensing device of the quality of tap water with the characteristic of anti-cross interference, in-situ, batch-fabrication always is a challenge issue. In this paper, a multi-parameter integrated micro-nano sensor, monitoring six key daily inspection indicators, is designed and prepared by MEMS technology on silicon substrate. By fabricating an all solid thin-film Ag/AgCl reference electrode, employing electrochemical stable/active Pt/Au/PbO2/IrO2 as the working/counter electrode and verified the effectiveness of as-fabricated sensor by pH/COD/Free Chlorine/Conductivity/Temperature detection, the sensor demonstrates acceptable limit of detection, desirable linearity and competitive accuracy. In addition, a miniature turbidity sensor is fixed on another side of the substrate, which can accurately distinguish turbidity changes of 0.1 NTU in the range of 0-1 NTU in dark environments. Particularly, a flow velocity detection unit is fabricated to avoid the data deviation by water flow fluctuation. By placing the electrode array in a tiny area (17*19*0.6 mm), a significant improvement in data accuracy is discovered for 9% after cross interference compensation. Finally, a circuit system is developed to assist as-proposed sensor in online and continuous monitoring of the tap water in pipeline. So, the interesting sensing behavior indicate that this work developed a competitive device for tap water online monitoring in pipeline.
{"title":"Batch Preparation of Multi-parameter Sensor for Online and In-situ Monitoring of Tap Water","authors":"Jiawen Yin, Shengkang Lu, Hanyang Tong, Jianqian Li, Rentao Cao, Shouhong Li, Wanlei Gao, Jie Zou, Qinghui Jin","doi":"10.1016/j.electacta.2025.145664","DOIUrl":"https://doi.org/10.1016/j.electacta.2025.145664","url":null,"abstract":"The safety of drinking water is the most basic safeguard for the human survival. In-situ and on-line monitoring of tap water is considered an effective method to reduce the harm of tap water pollution, caused by pipeline rupture or leakage. However, a sensing device of the quality of tap water with the characteristic of anti-cross interference, in-situ, batch-fabrication always is a challenge issue. In this paper, a multi-parameter integrated micro-nano sensor, monitoring six key daily inspection indicators, is designed and prepared by MEMS technology on silicon substrate. By fabricating an all solid thin-film Ag/AgCl reference electrode, employing electrochemical stable/active Pt/Au/PbO<sub>2</sub>/IrO<sub>2</sub> as the working/counter electrode and verified the effectiveness of as-fabricated sensor by pH/COD/Free Chlorine/Conductivity/Temperature detection, the sensor demonstrates acceptable limit of detection, desirable linearity and competitive accuracy. In addition, a miniature turbidity sensor is fixed on another side of the substrate, which can accurately distinguish turbidity changes of 0.1 NTU in the range of 0-1 NTU in dark environments. Particularly, a flow velocity detection unit is fabricated to avoid the data deviation by water flow fluctuation. By placing the electrode array in a tiny area (17*19*0.6 mm), a significant improvement in data accuracy is discovered for 9% after cross interference compensation. Finally, a circuit system is developed to assist as-proposed sensor in online and continuous monitoring of the tap water in pipeline. So, the interesting sensing behavior indicate that this work developed a competitive device for tap water online monitoring in pipeline.","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"34 1","pages":""},"PeriodicalIF":6.6,"publicationDate":"2025-01-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142925178","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Coal tar-based pores carbon (PC) is a widely studied electrode material for supercapacitors. However, coal tar-based PC has fewer oxygen-containing groups on the surface, less developed pores, and poor wettability limits its electrochemical performance. Therefore, it is necessary to modulate the structural characteristics of PC by changing the activation conditions, which in turn improves their electrochemical properties, and to explore the applicable environments for PC electrode materials. Here in the paper, coal tar-based PC was prepared by low-temperature solvothermal and activation methods using microcrystalline cellulose-HCl as an additive, based on single-factor results as a basis for designing response optimization experiments. The optimized PC was characterized by SEM, TEM, FT-IR, XPS, XRD, and nitrogen adsorption and detestation tests for its morphology and structure, and oxygen-rich, hierarchical PC with larger layer spacing was obtained. Meanwhile, three-electrode and two-electrode performance tests were performed on different electrolytes. Among them, the three-electrode system in an alkaline environment has good electrochemical performance. The current was increased from 0.3 A g−1 to 10 A g−1, the specific capacitance was decreased from 317 F g−1 to 220 F g−1, and the capacitance retention was as high as 95.2% after 10,000 cycles at 5 A g−1. In the two-electrode system in a neutral environment, the energy density was 23.4 Wh kg−1 at an output power of 296.0 W kg−1. The capacity retention was 68.7% after 5000 cycles at 2 A g−1. The results demonstrated that coal tar-based PC has some application value in supercapacitor electrode materials.
{"title":"Response surface optimization of coal tar-based porous carbon and its supercapacitor performance analysis","authors":"Peng Wu, XinYuan Xu, Yuanmeng Xue, Qiang Dou, Haibin Luo, Chunru Zhou, Wencheng Li, Yuting Lv","doi":"10.1016/j.electacta.2025.145660","DOIUrl":"https://doi.org/10.1016/j.electacta.2025.145660","url":null,"abstract":"Coal tar-based pores carbon (PC) is a widely studied electrode material for supercapacitors. However, coal tar-based PC has fewer oxygen-containing groups on the surface, less developed pores, and poor wettability limits its electrochemical performance. Therefore, it is necessary to modulate the structural characteristics of PC by changing the activation conditions, which in turn improves their electrochemical properties, and to explore the applicable environments for PC electrode materials. Here in the paper, coal tar-based PC was prepared by low-temperature solvothermal and activation methods using microcrystalline cellulose-HCl as an additive, based on single-factor results as a basis for designing response optimization experiments. The optimized PC was characterized by SEM, TEM, FT-IR, XPS, XRD, and nitrogen adsorption and detestation tests for its morphology and structure, and oxygen-rich, hierarchical PC with larger layer spacing was obtained. Meanwhile, three-electrode and two-electrode performance tests were performed on different electrolytes. Among them, the three-electrode system in an alkaline environment has good electrochemical performance. The current was increased from 0.3 A g<sup>−1</sup> to 10 A g<sup>−1</sup>, the specific capacitance was decreased from 317 F g<sup>−1</sup> to 220 F g<sup>−1</sup>, and the capacitance retention was as high as 95.2% after 10,000 cycles at 5 A g<sup>−1</sup>. In the two-electrode system in a neutral environment, the energy density was 23.4 Wh kg<sup>−1</sup> at an output power of 296.0 W kg<sup>−1</sup>. The capacity retention was 68.7% after 5000 cycles at 2 A g<sup>−1</sup>. The results demonstrated that coal tar-based PC has some application value in supercapacitor electrode materials.","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"16 1","pages":""},"PeriodicalIF":6.6,"publicationDate":"2025-01-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142925162","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-04DOI: 10.1016/j.electacta.2025.145645
Qisong Lv, Yan Liu, Fei Han, Haitao Xia, Qinan Zhou, Zhijian Zhang, Bi Xu, Haochen Shi
Integrating negative thermal expansion (NTE) materials into high TEC cathodes minimizes thermal expansion mismatches in SOFCs. This also boosts their electrochemical performance. Therefore, we chose to prepare the composite cathode material with the negative thermal expansion material Y2W3O12 (YWO) and Sm0.5Sr0.5CoO3-δ (SSC). XRD tests show no elemental segregation or adverse reactions between SSC, YWO, and SDC. This indicates excellent chemical compatibility, meeting SOFCs material requirements. TEC tests show that higher YWO content improves thermal matching and increases the effective contact area between the composite cathode and SDC electrolyte. At 20 wt.% YWO, the TEC value is 10.05 × 10-6 K-1, closely matching SDC. The minimum polarization resistance (Rp) of 0.092 Ω cm2 is achieved for SSC-20YWO at an operating temperature of 800 °C. Oxygen partial pressure tests demonstrate a gradual decrease in Rp as oxygen content increased. Moreover, it is observed that the change in the arc is more pronounced at low-frequency, indicating that the oxygen content has a significant impact on the low-frequency process. For the SSC sample, surface oxygen adsorption is rate-limiting step below 0.05 atm O2 partial pressure, while the further ionization process of oxygen ion is rate-limiting step above this threshold. For SSC-20YWO, the further ionization process of oxygen ion is consistently rate-limiting step across the entire O2 partial pressure range (0.01 atm to 1 atm), indicating accelerated surface oxygen adsorption. This is due to the increased length of the triple phase boundary results in a greater number of oxygen active sites, which further enhances the electrochemical performance. These results show that adding YWO to the SOFCs cathode effectively improves both performance and compatibility.
{"title":"Performance Analysis of Cathode Materials SSC-xYWO (x = 0-30 wt. %) Based on Thermal Expansion Complementarity for SOFCs","authors":"Qisong Lv, Yan Liu, Fei Han, Haitao Xia, Qinan Zhou, Zhijian Zhang, Bi Xu, Haochen Shi","doi":"10.1016/j.electacta.2025.145645","DOIUrl":"https://doi.org/10.1016/j.electacta.2025.145645","url":null,"abstract":"Integrating negative thermal expansion (NTE) materials into high TEC cathodes minimizes thermal expansion mismatches in SOFCs. This also boosts their electrochemical performance. Therefore, we chose to prepare the composite cathode material with the negative thermal expansion material Y<sub>2</sub>W<sub>3</sub>O<sub>12</sub> (YWO) and Sm<sub>0.5</sub>Sr<sub>0.5</sub>CoO<sub>3-δ</sub> (SSC). XRD tests show no elemental segregation or adverse reactions between SSC, YWO, and SDC. This indicates excellent chemical compatibility, meeting SOFCs material requirements. TEC tests show that higher YWO content improves thermal matching and increases the effective contact area between the composite cathode and SDC electrolyte. At 20 wt.% YWO, the TEC value is 10.05 × 10<sup>-6</sup> K<sup>-1</sup>, closely matching SDC. The minimum polarization resistance (<em>Rp</em>) of 0.092 Ω cm<sup>2</sup> is achieved for SSC-20YWO at an operating temperature of 800 °C. Oxygen partial pressure tests demonstrate a gradual decrease in <em>Rp</em> as oxygen content increased. Moreover, it is observed that the change in the arc is more pronounced at low-frequency, indicating that the oxygen content has a significant impact on the low-frequency process. For the SSC sample, surface oxygen adsorption is rate-limiting step below 0.05 atm O<sub>2</sub> partial pressure, while the further ionization process of oxygen ion is rate-limiting step above this threshold. For SSC-20YWO, the further ionization process of oxygen ion is consistently rate-limiting step across the entire O<sub>2</sub> partial pressure range (0.01 atm to 1 atm), indicating accelerated surface oxygen adsorption. This is due to the increased length of the triple phase boundary results in a greater number of oxygen active sites, which further enhances the electrochemical performance. These results show that adding YWO to the SOFCs cathode effectively improves both performance and compatibility.","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"41 1","pages":""},"PeriodicalIF":6.6,"publicationDate":"2025-01-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142924523","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Polymer electrolyte membranes have been proposed as alternatives to conventional liquid electrolytes to improve the performance and stability of lithium-ion batteries. For past decades, wide varieties of polymer electrolyte membranes have been reported; however, most of the membranes contain critical issues with their ion conductivity and/or stability for practical battery applications. In this study, we aim to develop gel polymer electrolyte membranes with high ion conductivity and sufficient stability by combining solvate ionic liquid and three types of crosslinked network polymers synthesized from multifunctional monomers with vinyl and thiol groups. One of the obtained gel polymer electrolyte membranes, poly(TTT-PEMP)/G4-LiTFSI, showed high ion conductivity close to 10-3 S cm-1 at room temperature and superior electrochemical stability (oxidation stability: >5.0V vs. Li/Li+). The lithium metal batteries using the gel polymer electrolyte membranes achieved continuous stable charge/discharge cycles, promising future lithium metal batteries operated at high voltage for the long term.
{"title":"Gel Polymer Electrolyte Membranes Consisted of Solvate Ionic Liquid and Crosslinked Network Polymers Bearing Different Main Chains: Fabrication and Lithium Battery Application","authors":"Yubing Dong, Xinming Qi, Manabu Tanaka, Hiroyoshi Kawakami","doi":"10.1016/j.electacta.2025.145661","DOIUrl":"https://doi.org/10.1016/j.electacta.2025.145661","url":null,"abstract":"Polymer electrolyte membranes have been proposed as alternatives to conventional liquid electrolytes to improve the performance and stability of lithium-ion batteries. For past decades, wide varieties of polymer electrolyte membranes have been reported; however, most of the membranes contain critical issues with their ion conductivity and/or stability for practical battery applications. In this study, we aim to develop gel polymer electrolyte membranes with high ion conductivity and sufficient stability by combining solvate ionic liquid and three types of crosslinked network polymers synthesized from multifunctional monomers with vinyl and thiol groups. One of the obtained gel polymer electrolyte membranes, poly(TTT-PEMP)/G4-LiTFSI, showed high ion conductivity close to 10<sup>-3</sup> S cm<sup>-1</sup> at room temperature and superior electrochemical stability (oxidation stability: >5.0V <em>vs.</em> Li/Li<sup>+</sup>). The lithium metal batteries using the gel polymer electrolyte membranes achieved continuous stable charge/discharge cycles, promising future lithium metal batteries operated at high voltage for the long term.","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"34 1","pages":""},"PeriodicalIF":6.6,"publicationDate":"2025-01-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142924524","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The study investigates the effects of substituting calcium (Ca) for strontium (Sr) in La₀.₅₈Sr₀.₄Co₀.₂Fe₀.₈O₃−δ (L58CCF) perovskite, evaluating its thermal stability and electrochemical performance as a potential cathode for intermediate-temperature solid oxide fuel cells (IT-SOFCs). Through X-ray diffraction (XRD) and electrochemical impedance spectroscopy (EIS), L58CCF demonstrates superior thermal stability, maintaining its structure up to 1200°C, compared to L58SCF, which undergoes a phase transition above 1000°C. The L58CCF symmetric cell sintered at 950°C has the lowest area-specific resistance (ASR) of 0.99 Ω·cm², offering competitive ASR values compared to L58SCF and L6CCF ones. Additionally, the L58CCF cathode showed an oxygen reduction reaction (ORR) polarization resistance of 0.47 Ω·cm² at 800°C, further indicating its efficiency as a cathode material. The study concludes that while L58CCF presents a promising balance of stability and electrochemical performance, further optimization is needed to address impurity phase issues and enhance long-term durability for IT-SOFC applications.
{"title":"Calcium (Ca) Substitution for Strontium (Sr) in La₀.₅₈Sr₀.₄Co₀.₂Fe₀.₈O₃−δ: Stability and Elechtrochemical Performance in IT-SOFC Cathodes","authors":"Majid Jafari, Fatemeh Yadollahi Farsani, Fabian Grimm","doi":"10.1016/j.electacta.2025.145662","DOIUrl":"https://doi.org/10.1016/j.electacta.2025.145662","url":null,"abstract":"The study investigates the effects of substituting calcium (Ca) for strontium (Sr) in La₀.₅₈Sr₀.₄Co₀.₂Fe₀.₈O₃<sub>−δ</sub> (L58CCF) perovskite, evaluating its thermal stability and electrochemical performance as a potential cathode for intermediate-temperature solid oxide fuel cells (IT-SOFCs). Through X-ray diffraction (XRD) and electrochemical impedance spectroscopy (EIS), L58CCF demonstrates superior thermal stability, maintaining its structure up to 1200°C, compared to L58SCF, which undergoes a phase transition above 1000°C. The L58CCF symmetric cell sintered at 950°C has the lowest area-specific resistance (ASR) of 0.99 Ω·cm², offering competitive ASR values compared to L58SCF and L6CCF ones. Additionally, the L58CCF cathode showed an oxygen reduction reaction (ORR) polarization resistance of 0.47 Ω·cm<sup>²</sup> at 800°C, further indicating its efficiency as a cathode material. The study concludes that while L58CCF presents a promising balance of stability and electrochemical performance, further optimization is needed to address impurity phase issues and enhance long-term durability for IT-SOFC applications.","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"203 1","pages":""},"PeriodicalIF":6.6,"publicationDate":"2025-01-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142924526","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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