Journal of Electroanalytical Chemistry最新文献

英文中文

Synthesis and sodium storage performance of MxSy@N, C composites derived from l-methionine-based MOFs

IF 4.1 3区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Electroanalytical Chemistry

Pub Date : 2025-01-15 DOI: 10.1016/j.jelechem.2024.118850

Na Xin , Kangjia Zhao , Zijian Shao , Kui Wang , Huanhuan Li , Lei Yuan , Yaping Wang

Transition metal sulfides (TMSs), celebrated for their elevated theoretical capacities, are prospective anode candidates for sodium-ion batteries (SIBs). However, the conventional synthesis of TMSs is marred by intricate, multi-stage procedures and reliance on external sulfur precursors. Herein, we present a novel one-pot synthesis strategy utilizing l-methionine within a metal–organic framework (MOF) to incorporate carbon, nitrogen, and sulfur sources, thereby enabling the direct synthesis of carbon, nitrogen-doped sulfides (M_xS_y@N, C) without the need for external sulfurization agents. By altering the metal ions, we synthesized a series of M_xS_y@N, C composites characterized by co-doping with nitrogen and carbon. Among these, Co₉S₈@N, C demonstrated an impressive reversible sodium ion capacity of 592.7 mAh/g at a current density of 200 mA/g, along with stable cycling performance over 150 cycles and superior rate capability. These findings underscore the potential of this material as a high-performance anode for SIBs. Our research signifies a significant advancement in the synthesis of transition metal sulfides for energy storage applications, laying the groundwork for the development of high-capacity, long-lasting anode materials. This work contributes to the progress of energy storage technologies and supports the expansion of SIBs.

{"title":"Synthesis and sodium storage performance of MxSy@N, C composites derived from l-methionine-based MOFs","authors":"Na Xin , Kangjia Zhao , Zijian Shao , Kui Wang , Huanhuan Li , Lei Yuan , Yaping Wang","doi":"10.1016/j.jelechem.2024.118850","DOIUrl":"10.1016/j.jelechem.2024.118850","url":null,"abstract":"<div><div>Transition metal sulfides (TMSs), celebrated for their elevated theoretical capacities, are prospective anode candidates for sodium-ion batteries (SIBs). However, the conventional synthesis of TMSs is marred by intricate, multi-stage procedures and reliance on external sulfur precursors. Herein, we present a novel one-pot synthesis strategy utilizing <span>l</span>-methionine within a metal–organic framework (MOF) to incorporate carbon, nitrogen, and sulfur sources, thereby enabling the direct synthesis of carbon, nitrogen-doped sulfides (M<sub>x</sub>S<sub>y</sub>@N, C) without the need for external sulfurization agents. By altering the metal ions, we synthesized a series of M<sub>x</sub>S<sub>y</sub>@N, C composites characterized by co-doping with nitrogen and carbon. Among these, Co<sub>9</sub>S<sub>8</sub>@N, C demonstrated an impressive reversible sodium ion capacity of 592.7 mAh/g at a current density of 200 mA/g, along with stable cycling performance over 150 cycles and superior rate capability. These findings underscore the potential of this material as a high-performance anode for SIBs. Our research signifies a significant advancement in the synthesis of transition metal sulfides for energy storage applications, laying the groundwork for the development of high-capacity, long-lasting anode materials. This work contributes to the progress of energy storage technologies and supports the expansion of SIBs.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"977 ","pages":"Article 118850"},"PeriodicalIF":4.1,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143132447","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}

引用次数: 0

Selectivity and activity trends of single-phase copper-tin foam electrocatalysts in CO2 electroreduction reaction

IF 4.1 3区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Electroanalytical Chemistry

Pub Date : 2025-01-15 DOI: 10.1016/j.jelechem.2024.118854

Ruslan Z. Faizullin , Margarita I. Guskova , Alexander V. Rudnev , Eduard E. Levin , Victoria A. Nikitina , Sergey Y. Istomin

The quest for active, selective, and stable electrocatalysts to convert CO₂ into valuable products like carbon monoxide and formate has garnered significant attention in recent years, driven by both fundamental research and practical applications. Recent findings on copper-tin electrocatalysts reveal an intriguing shift in selectivity of CO₂ reduction − from producing CO at low Sn concentrations to generating formate with nearly unity selectivity when the Sn content is increased. This shift raises important questions about the factors influencing the dramatic changes in CO₂ reduction product distribution as the Cu-Sn material composition varies. However, existing experimental data primarily derive from multiphase Cu-Sn materials, which typically undergo phase changes under CO₂ reduction conditions, which introduces interpretation uncertainties. In this study, we developed stable single-phase Cu-Sn materials, specifically a tin solid solution in Cu with the composition of Cu₉₇Sn₃ and the intermetallic Cu₆Sn₅, which were fabricated as dispersed foams to facilitate kinetic measurements. Our findings indicate that the high activity and selectivity of the Cu-Sn solid solution in the CO₂-to-CO conversion process are likely due to more favorable kinetics for the formation of the *COOH intermediate, and not due to easier carbon monoxide desorption, as was previously suggested. In contrast, the formate production kinetics for the HCOO-selective Cu₆Sn₅ phase are significantly inhibited compared to pure copper. We hope our results will motivate further investigation into the nature of the active sites in Cu-Sn electrocatalysts, providing a deeper mechanistic understanding of the observed selectivity/activity trends.

{"title":"Selectivity and activity trends of single-phase copper-tin foam electrocatalysts in CO2 electroreduction reaction","authors":"Ruslan Z. Faizullin , Margarita I. Guskova , Alexander V. Rudnev , Eduard E. Levin , Victoria A. Nikitina , Sergey Y. Istomin","doi":"10.1016/j.jelechem.2024.118854","DOIUrl":"10.1016/j.jelechem.2024.118854","url":null,"abstract":"<div><div>The quest for active, selective, and stable electrocatalysts to convert CO<sub>2</sub> into valuable products like carbon monoxide and formate has garnered significant attention in recent years, driven by both fundamental research and practical applications. Recent findings on copper-tin electrocatalysts reveal an intriguing shift in selectivity of CO<sub>2</sub> reduction − from producing CO at low Sn concentrations to generating formate with nearly unity selectivity when the Sn content is increased. This shift raises important questions about the factors influencing the dramatic changes in CO<sub>2</sub> reduction product distribution as the Cu-Sn material composition varies. However, existing experimental data primarily derive from multiphase Cu-Sn materials, which typically undergo phase changes under CO<sub>2</sub> reduction conditions, which introduces interpretation uncertainties. In this study, we developed stable single-phase Cu-Sn materials, specifically a tin solid solution in Cu with the composition of Cu<sub>97</sub>Sn<sub>3</sub> and the intermetallic Cu<sub>6</sub>Sn<sub>5</sub>, which were fabricated as dispersed foams to facilitate kinetic measurements. Our findings indicate that the high activity and selectivity of the Cu-Sn solid solution in the CO<sub>2</sub>-to-CO conversion process are likely due to more favorable kinetics for the formation of the *COOH intermediate, and not due to easier carbon monoxide desorption, as was previously suggested. In contrast, the formate production kinetics for the HCOO-selective Cu<sub>6</sub>Sn<sub>5</sub> phase are significantly inhibited compared to pure copper. We hope our results will motivate further investigation into the nature of the active sites in Cu-Sn electrocatalysts, providing a deeper mechanistic understanding of the observed selectivity/activity trends.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"977 ","pages":"Article 118854"},"PeriodicalIF":4.1,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143132521","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}

引用次数: 0

Insight into organic electrolytes for rechargeable Zn-air battery

IF 4.1 3区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Electroanalytical Chemistry

Pub Date : 2025-01-15 DOI: 10.1016/j.jelechem.2024.118855

Mohammad Ziauddin Chowdhury

In rechargeable zinc-air batteries (RZABs) use of aqueous electrolytes is prevalent, but this approach introduces several challenges, such as hydrogen evolution, lower electrochemical stability window, corrosion and passivation of the Zn electrodes. In this regard, the suitability of zinc organic electrolytes is explored to resolve the technical challenges associated with the aqueous electrolytes. In order to address the current challenges and research gaps, suitability of the addressed zinc organic electrolytes was investigated through analyzing their – physicochemical properties and mass transport; compositional analyses (decomposition screening), formed discharge product and reversibility during redox kinetics; corrosion and passivation phenomena of zinc metal as well as the cathodic oxygen reduction reaction (ORR) performance. Notably, this study is the first to investigate the passivation and corrosion phenomena of Zn metal anodes in organic electrolytes, establishing the correlation between cathodic ORR activity and electrolyte medium, and the decomposition process of organic electrolytes in air environment through saturating the electrolyte medium with dissolved oxygen. The study revealed that zinc triflate/DMF (Dimethylformamide) organic electrolyte has excellent reversibility, charge and mass transport, ORR activity, and minimum passivation than the zinc nitrate/DMF and zinc nitrate/DMSO (Dimethylsufoxide) organic electrolytes.

{"title":"Insight into organic electrolytes for rechargeable Zn-air battery","authors":"Mohammad Ziauddin Chowdhury","doi":"10.1016/j.jelechem.2024.118855","DOIUrl":"10.1016/j.jelechem.2024.118855","url":null,"abstract":"<div><div>In rechargeable zinc-air batteries (RZABs) use of aqueous electrolytes is prevalent, but this approach introduces several challenges, such as hydrogen evolution, lower electrochemical stability window, corrosion and passivation of the Zn electrodes. In this regard, the suitability of zinc organic electrolytes is explored to resolve the technical challenges associated with the aqueous electrolytes. In order to address the current challenges and research gaps, suitability of the addressed zinc organic electrolytes was investigated through analyzing their – physicochemical properties and mass transport; compositional analyses (decomposition screening), formed discharge product and reversibility during redox kinetics; corrosion and passivation phenomena of zinc metal as well as the cathodic oxygen reduction reaction (ORR) performance. Notably, this study is the first to investigate the passivation and corrosion phenomena of Zn metal anodes in organic electrolytes, establishing the correlation between cathodic ORR activity and electrolyte medium, and the decomposition process of organic electrolytes in air environment through saturating the electrolyte medium with dissolved oxygen. The study revealed that zinc triflate/DMF (Dimethylformamide) organic electrolyte has excellent reversibility, charge and mass transport, ORR activity, and minimum passivation than the zinc nitrate/DMF and zinc nitrate/DMSO (Dimethylsufoxide) organic electrolytes.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"977 ","pages":"Article 118855"},"PeriodicalIF":4.1,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143132446","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Anodic and cathodic dual-mode cysteine detection utilizing a glassy carbon electrode co-activated by electrochemical pretreatment and fully fluorinated cobalt phthalocyanine

IF 4.1 3区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Electroanalytical Chemistry

Pub Date : 2025-01-15 DOI: 10.1016/j.jelechem.2024.118861

Ming Qin , Jinqiu Zhu , Jiaqi Zhao, Baiqing Yuan, Sixian Liu, Tingting Cai, Chunying Xu

l-cysteine (Cys), a fundamental amino acid within the human body, is crucial for a variety of biological processes. Its concentration levels offer valuable insights into an individual’s health status and are instrumental in the early diagnosis of various conditions. Traditional electrochemical detection techniques for Cys, primarily based on anodic oxidation, require complex and time-consuming steps including the creation of electrocatalysts and subsequent electrode modifications. This method is also prone to inaccuracies due to interference from other easily oxidized electroactive substances. To address these challenges, we present an innovative dual-mode detection strategy for Cys, leveraging both anodic and cathodic responses on a glassy carbon electrode. This electrode is dual-activated by electrochemical pretreatment and fully fluorinated cobalt phthalocyanine, facilitating a robust and reversible transformation between cystine and Cys. Remarkably, this method enables Cys detection at negative potential range, significantly reducing interference from prevalent biological and electroactive compounds like ascorbic acid and uric acid. Moreover, the process for modifying the electrode is remarkably simple, efficient, and eco-friendly.

{"title":"Anodic and cathodic dual-mode cysteine detection utilizing a glassy carbon electrode co-activated by electrochemical pretreatment and fully fluorinated cobalt phthalocyanine","authors":"Ming Qin , Jinqiu Zhu , Jiaqi Zhao, Baiqing Yuan, Sixian Liu, Tingting Cai, Chunying Xu","doi":"10.1016/j.jelechem.2024.118861","DOIUrl":"10.1016/j.jelechem.2024.118861","url":null,"abstract":"<div><div><span>l</span>-cysteine (Cys), a fundamental amino acid within the human body, is crucial for a variety of biological processes. Its concentration levels offer valuable insights into an individual’s health status and are instrumental in the early diagnosis of various conditions. Traditional electrochemical detection techniques for Cys, primarily based on anodic oxidation, require complex and time-consuming steps including the creation of electrocatalysts and subsequent electrode modifications. This method is also prone to inaccuracies due to interference from other easily oxidized electroactive substances. To address these challenges, we present an innovative dual-mode detection strategy for Cys, leveraging both anodic and cathodic responses on a glassy carbon electrode. This electrode is dual-activated by electrochemical pretreatment and fully fluorinated cobalt phthalocyanine, facilitating a robust and reversible transformation between cystine and Cys. Remarkably, this method enables Cys detection at negative potential range, significantly reducing interference from prevalent biological and electroactive compounds like ascorbic acid and uric acid. Moreover, the process for modifying the electrode is remarkably simple, efficient, and eco-friendly.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"977 ","pages":"Article 118861"},"PeriodicalIF":4.1,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143132463","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}

引用次数: 0

Helical carbon nanofibers-supported MnSiO3 for high-performance lithium-ion battery anode materials

IF 4.1 3区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Electroanalytical Chemistry

Pub Date : 2025-01-15 DOI: 10.1016/j.jelechem.2024.118849

Dongwei Jiang , Yongzhong Jin , Wenjun Zhang , Xu Li , Ge Chen , Yonghong Liu

Metal silicates are regarded as promising candidates for lithium-ion batteries due to their high capacity, ease of synthesis, and environmental friendliness. Unfortunately, the challenge of enhancing the electrical conductivity of metal silicates represents a significant obstacle in this field. In this study, a simple and controllable two-step method was used to design and prepare the novel helical carbon nanofibers@manganese silicate (HCNFs@MnSiO₃) anode composite, in which the size of MnSiO₃ nanoparticles are about 20 nm. After 200 cycles at 200 mA g⁻¹, the HCNFs@MnSiO₃ anode exhibits an excellent reversible specific capacity of 878.1 mA h/g, which is 158 % higher than that of the MnSiO₃ anode. The synergistic interaction of HCNFs and MnSiO₃ is primarily responsible for the enhanced electrochemical performance of HCNFs@MnSiO₃. A robust supportive network space is offered by the three-dimensional helical structure of HCNFs to allow for the volume expansion of MnSiO₃ during charging and discharging. Furthermore, MnSiO₃′s low electrical conductivity is enhanced by HCNFs’ high electrical conductivity. The development of high-performance lithium-ion batteries using metal silicate-based anode materials is aided by the useful reference provided by this study.

{"title":"Helical carbon nanofibers-supported MnSiO3 for high-performance lithium-ion battery anode materials","authors":"Dongwei Jiang , Yongzhong Jin , Wenjun Zhang , Xu Li , Ge Chen , Yonghong Liu","doi":"10.1016/j.jelechem.2024.118849","DOIUrl":"10.1016/j.jelechem.2024.118849","url":null,"abstract":"<div><div>Metal silicates are regarded as promising candidates for lithium-ion batteries due to their high capacity, ease of synthesis, and environmental friendliness. Unfortunately, the challenge of enhancing the electrical conductivity of metal silicates represents a significant obstacle in this field. In this study, a simple and controllable two-step method was used to design and prepare the novel helical carbon nanofibers@manganese silicate (HCNFs@MnSiO<sub>3</sub>) anode composite, in which the size of MnSiO<sub>3</sub> nanoparticles are about 20 nm. After 200 cycles at 200 mA g<sup>−1</sup>, the HCNFs@MnSiO<sub>3</sub> anode exhibits an excellent reversible specific capacity of 878.1 mA h/g, which is 158 % higher than that of the MnSiO<sub>3</sub> anode. The synergistic interaction of HCNFs and MnSiO<sub>3</sub> is primarily responsible for the enhanced electrochemical performance of HCNFs@MnSiO<sub>3</sub>. A robust supportive network space is offered by the three-dimensional helical structure of HCNFs to allow for the volume expansion of MnSiO<sub>3</sub> during charging and discharging. Furthermore, MnSiO<sub>3</sub>′s low electrical conductivity is enhanced by HCNFs’ high electrical conductivity. The development of high-performance lithium-ion batteries using metal silicate-based anode materials is aided by the useful reference provided by this study.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"977 ","pages":"Article 118849"},"PeriodicalIF":4.1,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143132485","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}

引用次数: 0

Electrocatalytic oxidation of formaldehyde using pencil graphite electrode modified with layer-by-layer electrodeposition of carbon dots/polypectin/cobalt nanoparticles

IF 4.1 3区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Electroanalytical Chemistry

Pub Date : 2025-01-15 DOI: 10.1016/j.jelechem.2024.118859

Elnaz Minaie , Khalil Farhadi , Biuck Habibi

The development of non-noble metal-based catalysts with high electrocatalytic activity and minimal poisoning for the oxidation of small organic molecules is of vital importance in the energy world. In the present work, carbon dots (CDs) and polypectin (PPC) were electrochemically synthesized and deposited on pencil graphite electrodes (PGE) to create unique multifunctional PPC/CD/PGE. Co nanoparticles (CoNPs) were subsequently electrodeposited on PPC/CDs, leading to the fabrication of CoNPs/PPC/CDs/PGE. The nanostructure nature of electrode modifier was characterized by various techniques. The electrocatalytic performance of CoNPs/PPC/CDs/PGE for the electrooxidation of formaldehyde in alkaline medium was investigated using different electrochemical methods. Based on the electrochemical results, the modified electrode showed excellent electrocatalytic activity for formaldehyde oxidation with minimum onset potential (−0.020 V/SCE) and high current density (35 mA cm⁻²) compared to other reported nanocatalysts based on noble (platinum group) and non-noble metals through an electrochemical-chemical (EC′) pathway. The electrochemical behavior of CoNPs/PPC/CDs/PGE in the presence of formaldehyde showed that the incorporation of CoNPs in the PPC/CD nanocomposite prepared on PGE significantly increases the electrocatalytic activity of the direct oxidation of formaldehyde, which can promise a new strategy in order to design cobalt-based high performance nanoelectrocatalysts for formaldehyde fuel cells.

{"title":"Electrocatalytic oxidation of formaldehyde using pencil graphite electrode modified with layer-by-layer electrodeposition of carbon dots/polypectin/cobalt nanoparticles","authors":"Elnaz Minaie , Khalil Farhadi , Biuck Habibi","doi":"10.1016/j.jelechem.2024.118859","DOIUrl":"10.1016/j.jelechem.2024.118859","url":null,"abstract":"<div><div>The development of non-noble metal-based catalysts with high electrocatalytic activity and minimal poisoning for the oxidation of small organic molecules is of vital importance in the energy world. In the present work, carbon dots (CDs) and polypectin (PPC) were electrochemically synthesized and deposited on pencil graphite electrodes (PGE) to create unique multifunctional PPC/CD/PGE. Co nanoparticles (CoNPs) were subsequently electrodeposited on PPC/CDs, leading to the fabrication of CoNPs/PPC/CDs/PGE. The nanostructure nature of electrode modifier was characterized by various techniques. The electrocatalytic performance of CoNPs/PPC/CDs/PGE for the electrooxidation of formaldehyde in alkaline medium was investigated using different electrochemical methods. Based on the electrochemical results, the modified electrode showed excellent electrocatalytic activity for formaldehyde oxidation with minimum onset potential (−0.020 V/SCE) and high current density (35 mA cm<sup>−2</sup>) compared to other reported nanocatalysts based on noble (platinum group) and non-noble metals through an electrochemical-chemical (EC′) pathway. The electrochemical behavior of CoNPs/PPC/CDs/PGE in the presence of formaldehyde showed that the incorporation of CoNPs in the PPC/CD nanocomposite prepared on PGE significantly increases the electrocatalytic activity of the direct oxidation of formaldehyde, which can promise a new strategy in order to design cobalt-based high performance nanoelectrocatalysts for formaldehyde fuel cells.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"977 ","pages":"Article 118859"},"PeriodicalIF":4.1,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143132522","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}

引用次数: 0

Charge injection dynamics in oxygen-functionalized and heteroatom-doped reduced graphene oxide and their impact on supercapacitor performance: An experimental and DFT investigation

IF 4.1 3区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Electroanalytical Chemistry

Pub Date : 2025-01-15 DOI: 10.1016/j.jelechem.2024.118848

Karthick Raja K , Umamaheswari Rajaji , Ting-Yu Liu , Vivek Kumar

To elucidate the synergistic effects of oxygen functional groups (OFGs) and heteroatoms (HAs) on charge injection dynamics and the electrochemical performance of reduced graphene oxide (rGO), a combination of experimental techniques and density functional theory (DFT) analyses were employed. GO was synthesized using a modified Hummers method and the sample reduced hydrothermally at 150 °C demonstrated the highest areal capacitance of 817 mF/cm². To understand the diffusion and charge transfer characteristics, the diffusion coefficient and distribution of relaxation time studied using the Electrochemical Impedance Spectroscopy data. Further the X-ray photoelectron spectroscopy (XPS) confirmed the incorporation of OFGs and HAs in the rGO. A partially oxygen-functionalized, nitrogen, and sulfur-doped graphene (NS-POG) model was constructed based on the XPS data and analyzed using DFT. The projected density of states analysis revealed a Fermi level shift, indicating the introduction of excess electrons due to incorporating OFGs and HAs in graphene, thereby improving the charge carrier concentration in the partially reduced or oxidized systems. The NS-POG system exhibited a quantum capacitance of 85.92 μF/cm². Additionally, potassium ion (K⁺) adsorption studies indicated that the adsorption energy was highest near sulfur atoms, suggesting that electrolyte ions exhibit enhanced electrochemical activity in proximity to sulfur. These findings provide insight into the mechanisms by which OFGs and HAs enhance the performance of rGO and highlighting the potential of NS-rGO in supercapacitor applications.

{"title":"Charge injection dynamics in oxygen-functionalized and heteroatom-doped reduced graphene oxide and their impact on supercapacitor performance: An experimental and DFT investigation","authors":"Karthick Raja K , Umamaheswari Rajaji , Ting-Yu Liu , Vivek Kumar","doi":"10.1016/j.jelechem.2024.118848","DOIUrl":"10.1016/j.jelechem.2024.118848","url":null,"abstract":"<div><div>To elucidate the synergistic effects of oxygen functional groups (OFGs) and heteroatoms (HAs) on charge injection dynamics and the electrochemical performance of reduced graphene oxide (rGO), a combination of experimental techniques and density functional theory (DFT) analyses were employed. GO was synthesized using a modified Hummers method and the sample reduced hydrothermally at 150 °C demonstrated the highest areal capacitance of 817 mF/cm<sup>2</sup>. To understand the diffusion and charge transfer characteristics, the diffusion coefficient and distribution of relaxation time studied using the Electrochemical Impedance Spectroscopy data. Further the X-ray photoelectron spectroscopy (XPS) confirmed the incorporation of OFGs and HAs in the rGO. A partially oxygen-functionalized, nitrogen, and sulfur-doped graphene (NS-POG) model was constructed based on the XPS data and analyzed using DFT. The projected density of states analysis revealed a Fermi level shift, indicating the introduction of excess electrons due to incorporating OFGs and HAs in graphene, thereby improving the charge carrier concentration in the partially reduced or oxidized systems. The NS-POG system exhibited a quantum capacitance of 85.92 μF/cm<sup>2</sup>. Additionally, potassium ion (K<sup>+</sup>) adsorption studies indicated that the adsorption energy was highest near sulfur atoms, suggesting that electrolyte ions exhibit enhanced electrochemical activity in proximity to sulfur. These findings provide insight into the mechanisms by which OFGs and HAs enhance the performance of rGO and highlighting the potential of NS-rGO in supercapacitor applications.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"977 ","pages":"Article 118848"},"PeriodicalIF":4.1,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143132524","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}

引用次数: 0

Measurement of potential of zero charge at a renewable pencil electrode

IF 4.1 3区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Electroanalytical Chemistry

Pub Date : 2025-01-15 DOI: 10.1016/j.jelechem.2024.118853

Hirosuke Tatsumi, Yusuke Kumano , Fumiki Takahashi, Jiye Jin

Potential of zero charge (PZC) was studied by using a renewable pencil lead electrode. A cutting device for the pencil electrode enabled clear observation of the direction of charging current, providing accurate values of PZC. The PZCs of the pencil electrode in aqueous solutions with nine different electrolytes at various concentrations were measured. The positive and negative shifts of the PZC upon the increase of electrolyte concentrations were observed for hydrophobic cations and anions, respectively, suggesting the presence of specific adsorption of the ions onto the electrode surface. An approximately linear relationship was found between the degree of the PZC shift (the Esin–Markov coefficient) and the hydrophobicity parameter of ion (the standard Gibbs energy of transfer of ion at nitrobenzene | water interface), whereas Cs⁺ ion gave practically no shift of PZC in spite of the moderate hydrophobicity.

引用次数: 0

Multidimensional core-shell nanocomposite of iron oxide-carbon tube and graphene nanosheet: A lithium-ion battery anode with enhanced performance through structural optimization

IF 4.1 3区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Electroanalytical Chemistry

Pub Date : 2025-01-15 DOI: 10.1016/j.jelechem.2024.118824

Yohan Jeong , Dae Ung Park , Yong Jae Lee , Sanglim Lee , Weon Ho Shin , Jong-Min Oh , Taek Lee , Chulhwan Park , Anusorn Seubsai , Hiesang Sohn

A novel multidimensional composite of 1D iron oxide (Fe₃O₄)-carbon tube and 2D graphene nanosheet (GNS) was demonstrated to be used as the anode material for lithium-ion batteries (LIBs). Fe₃O₄-carbon tube-GNS manifested a unique core–shell composite structure, where the Fe₃O₄ nanoparticles were embedded in the carbon tube with the GNS. The material characterization confirmed that the Fe₃O₄ nanoparticles were embedded in the highly graphitized carbon tube with the dispersed GNS. Fe₃O₄-carbon tube-GNS exhibited a high porosity (surface area: 62.3 m²/g, pore volume: 0.112 m³/g). It also exhibited an excellent electrochemical performance with a high reversible capacity (900 mAh/g at 1 A/g), a high coulombic efficiency (∼100 % for 100 cycles), and good rate capability (491 mAh/g at 5 A/g). The excellent electrochemical performance of our composite is attributed to the suppressed/accommodated volume expansion of Fe₃O₄ and formation of a stable solid electrolyte interphase (SEI) layer during lithiation/delithiation caused by unique multidimensional composite structure of Fe₃O₄-carbon tube-GNS with a continuous transport path for electrons and Li⁺. In addition, such the enhanced lithium storage of our composite is confirmed with the kinetic characterization at various scan rates by analyzing their storage and capacitive contributions.

{"title":"Multidimensional core-shell nanocomposite of iron oxide-carbon tube and graphene nanosheet: A lithium-ion battery anode with enhanced performance through structural optimization","authors":"Yohan Jeong , Dae Ung Park , Yong Jae Lee , Sanglim Lee , Weon Ho Shin , Jong-Min Oh , Taek Lee , Chulhwan Park , Anusorn Seubsai , Hiesang Sohn","doi":"10.1016/j.jelechem.2024.118824","DOIUrl":"10.1016/j.jelechem.2024.118824","url":null,"abstract":"<div><div>A novel multidimensional composite of 1D iron oxide (Fe<sub>3</sub>O<sub>4</sub>)-carbon tube and 2D graphene nanosheet (GNS) was demonstrated to be used as the anode material for lithium-ion batteries (LIBs). Fe<sub>3</sub>O<sub>4</sub>-carbon tube-GNS manifested a unique core–shell composite structure, where the Fe<sub>3</sub>O<sub>4</sub> nanoparticles were embedded in the carbon tube with the GNS. The material characterization confirmed that the Fe<sub>3</sub>O<sub>4</sub> nanoparticles were embedded in the highly graphitized carbon tube with the dispersed GNS. Fe<sub>3</sub>O<sub>4</sub>-carbon tube-GNS exhibited a high porosity (surface area: 62.3 m<sup>2</sup>/g, pore volume: 0.112 m<sup>3</sup>/g). It also exhibited an excellent electrochemical performance with a high reversible capacity (900 mAh/g at 1 A/g), a high coulombic efficiency (∼100 % for 100 cycles), and good rate capability (491 mAh/g at 5 A/g). The excellent electrochemical performance of our composite is attributed to the suppressed/accommodated volume expansion of Fe<sub>3</sub>O<sub>4</sub> and formation of a stable solid electrolyte interphase (SEI) layer during lithiation/delithiation caused by unique multidimensional composite structure of Fe<sub>3</sub>O<sub>4</sub>-carbon tube-GNS with a continuous transport path for electrons and Li<sup>+</sup>. In addition, such the enhanced lithium storage of our composite is confirmed with the kinetic characterization at various scan rates by analyzing their storage and capacitive contributions.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"977 ","pages":"Article 118824"},"PeriodicalIF":4.1,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143132444","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}

引用次数: 0

Enhanced oxygen evolution reaction performance of flower-like CoHS @NCDs through in-situ coupling of Nitrogen-Doped carbon dots and cobalt hydroxide nanosheets

IF 4.1 3区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Electroanalytical Chemistry

Pub Date : 2025-01-15 DOI: 10.1016/j.jelechem.2024.118858

Yang Gao , Haiyan Qi , Tao Jing , Jun Li , Siqi Shen , Qingxin Zeng , Hongxu Zhao

Efficient electrocatalytic materials are crucial for enhancing the efficiency of the oxygen evolution reaction (OER) in hydrolysis applications. In this study, we synthesized nitrogen-doped carbon dots (NCDs) via a straightforward one-step hydrothermal method. Subsequently, 3D flower-shaped CoHS@NCDs electrocatalysts were prepared by the integration of NCDs and cobalt hydroxide nanosheets (CoHS) using a solvothermal method. The resulting CoHS@NCDs electrocatalysts demonstrated outstanding catalytic performance for OER under alkaline conditions. Specifically, the CoHS@NCDs-3 electrocatalyst exhibited an overpotential of 280 mV at 10 mA cm⁻²(314 mV at 50 mA cm⁻²), representing an 80 mV improvement compared to CoHS, along with remarkable durability. Through comprehensive characterization, we revealed that the incorporation of NCDs facilitated the creation of numerous exposed active sites on CoHS, forming a unique electron transfer pathway (Co-N), thereby optimizing the kinetics of the OER reaction. This study underscored the significant potential of constructing electrocatalysts with exceptional OER activity based on transition metal hydroxides.

{"title":"Enhanced oxygen evolution reaction performance of flower-like CoHS @NCDs through in-situ coupling of Nitrogen-Doped carbon dots and cobalt hydroxide nanosheets","authors":"Yang Gao , Haiyan Qi , Tao Jing , Jun Li , Siqi Shen , Qingxin Zeng , Hongxu Zhao","doi":"10.1016/j.jelechem.2024.118858","DOIUrl":"10.1016/j.jelechem.2024.118858","url":null,"abstract":"<div><div>Efficient electrocatalytic materials are crucial for enhancing the efficiency of the oxygen evolution reaction (OER) in hydrolysis applications. In this study, we synthesized nitrogen-doped carbon dots (NCDs) via a straightforward one-step hydrothermal method. Subsequently, 3D flower-shaped CoHS@NCDs electrocatalysts were prepared by the integration of NCDs and cobalt hydroxide nanosheets (CoHS) using a solvothermal method. The resulting CoHS@NCDs electrocatalysts demonstrated outstanding catalytic performance for OER under alkaline conditions. Specifically, the CoHS@NCDs-3 electrocatalyst exhibited an overpotential of 280 mV at 10 mA cm<sup>−2</sup>(314 mV at 50 mA cm<sup>−2</sup>), representing an 80 mV improvement compared to CoHS, along with remarkable durability. Through comprehensive characterization, we revealed that the incorporation of NCDs facilitated the creation of numerous exposed active sites on CoHS, forming a unique electron transfer pathway (Co-N), thereby optimizing the kinetics of the OER reaction. This study underscored the significant potential of constructing electrocatalysts with exceptional OER activity based on transition metal hydroxides.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"977 ","pages":"Article 118858"},"PeriodicalIF":4.1,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143132464","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}

引用次数: 0

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