Pub Date : 2024-10-11DOI: 10.1016/j.jelechem.2024.118711
Yanna Hu , Xian Cao , Kai Zhang , Shichao Chen , Lingzhi Wei , Chun Ye , Guoxing Pan , Lin Hu
CO2 electrochemical reduction reaction (CO2RR) to formic acid (HCOOH) is beneficial for the recycling of carbon resources, which needs the highly selective catalysts with long-term stability for HCOOH production. In this study, the coupling of In nanoclusters (Inclus) and Bi nanoparticles (Binps) in nitrogen-doped carbon was designed by the thermal decomposition of the mixture of bimetallic MOFs and dicyanamide. When the In/Bi molar ratio was 1:2 (Inclus/Binps-1:2), the hybrid catalyst achieved a HCOOH Faradaic efficiency (FEHCOOH) of 94.5 % at −1.1 V vs reversible hydrogen electrode (RHE) in an H-type electrolysis cell, superior to that of single metal counterparts. Moreover, the Inclus/Binps-1:2 can maintain high stability of structures during the catalytic process, leading to no significant decay of FEHCOOH over 32 h. The enhanced performance of Inclus/Binps-1:2 is attributed to the strong electron interactions induced by the charge transfer between the In and Bi sites in Inclus/Binps-1:2 catalyst. The tuned electronic structure results in an offset effect that optimizes the binding energy to HCOO* intermediate, thus accelerating the CO2 to HCOOH conversion, as proven by the in-situ ATR-SEIRAS and density functional theory (DFT) calculations.
CO2 电化学还原反应（CO2RR）制取甲酸（HCOOH）有利于碳资源的循环利用，而 HCOOH 的制取需要具有长期稳定性的高选择性催化剂。本研究通过双金属 MOFs 和双氰胺混合物的热分解，设计了氮掺杂碳中 In 纳米团簇（Inclus）和 Bi 纳米颗粒（Binps）的耦合。当 In/Bi 摩尔比为 1:2 时（Inclus/Binps-1:2），混合催化剂在 H 型电解池中与可逆氢电极（RHE）的电压为 -1.1 V 时的 HCOOH 法拉第效率（FEHCOOH）达到 94.5%，优于单一金属催化剂。此外，Inclus/Binps-1:2 还能在催化过程中保持较高的结构稳定性，使 FEHCOOH 在 32 小时内无明显衰减。Inclus/Binps-1:2 性能的提高归因于 Inclus/Binps-1:2 催化剂中 In 和 Bi 位点之间的电荷转移引起的强电子相互作用。原位 ATR-SEIRAS 和密度泛函理论 (DFT) 计算证明，调整后的电子结构产生了偏移效应，优化了与 HCOO* 中间体的结合能，从而加速了 CO2 到 HCOOH 的转化。
{"title":"Coupling In nanoclusters and Bi nanoparticles in nitrogen-doped carbon for enhanced CO2 electroreduction to HCOOH","authors":"Yanna Hu , Xian Cao , Kai Zhang , Shichao Chen , Lingzhi Wei , Chun Ye , Guoxing Pan , Lin Hu","doi":"10.1016/j.jelechem.2024.118711","DOIUrl":"10.1016/j.jelechem.2024.118711","url":null,"abstract":"<div><div>CO<sub>2</sub> electrochemical reduction reaction (CO<sub>2</sub>RR) to formic acid (HCOOH) is beneficial for the recycling of carbon resources, which needs the highly selective catalysts with long-term stability for HCOOH production. In this study, the coupling of In nanoclusters (In<sub>clus</sub>) and Bi nanoparticles (Bi<sub>nps</sub>) in nitrogen-doped carbon was designed by the thermal decomposition of the mixture of bimetallic MOFs and dicyanamide. When the In/Bi molar ratio was 1:2 (In<sub>clus</sub>/Bi<sub>nps</sub>-1:2), the hybrid catalyst achieved a HCOOH Faradaic efficiency (FE<sub>HCOOH</sub>) of 94.5 % at −1.1 V vs reversible hydrogen electrode (RHE) in an H-type electrolysis cell, superior to that of single metal counterparts. Moreover, the In<sub>clus</sub>/Bi<sub>nps</sub>-1:2 can maintain high stability of structures during the catalytic process, leading to no significant decay of FE<sub>HCOOH</sub> over 32 h. The enhanced performance of In<sub>clus</sub>/Bi<sub>nps</sub>-1:2 is attributed to the strong electron interactions induced by the charge transfer between the In and Bi sites in In<sub>clus</sub>/Bi<sub>nps</sub>-1:2 catalyst. The tuned electronic structure results in an offset effect that optimizes the binding energy to HCOO* intermediate, thus accelerating the CO<sub>2</sub> to HCOOH conversion, as proven by the in-situ ATR-SEIRAS and density functional theory (DFT) calculations.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"974 ","pages":"Article 118711"},"PeriodicalIF":4.1,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142432784","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 : 2024-10-11DOI: 10.1016/j.jelechem.2024.118698
Romas Baronas
The nonlinear effects of the partitioning and diffusion limitation on the efficiency of enzyme-based bioreactors and potentiometric biosensors are investigated analytically and numerically using a three-layer mathematical model involving the Michaelis–Menten type reaction in the transient and steady states. Analytical expressions of the steady state substrate and reaction product concentrations and the bioreactor effectiveness as well as biosensor output potential are presented for the first and zero-order reaction rates. Mathematical modelling of the diffusion limiting membrane and the conditions under which the same values of the steady state characteristics are obtained when simulating the treated system at different values of the diffusion and distribution coefficients are investigated. The effective diffusion coefficients in the total diffusion layer consisting of the diffusion limiting membrane and the outer diffusion (Nernst) layer are applied to reduce the three-layer model to the corresponding two-layer model. The dynamics and behaviour of the substrate consumption rate, product emission rate, effectiveness factor and the output potential are numerically investigated.
{"title":"Nonlinear effects of partitioning and diffusion limitation on the efficiency of three-layer enzyme bioreactors and potentiometric biosensors","authors":"Romas Baronas","doi":"10.1016/j.jelechem.2024.118698","DOIUrl":"10.1016/j.jelechem.2024.118698","url":null,"abstract":"<div><div>The nonlinear effects of the partitioning and diffusion limitation on the efficiency of enzyme-based bioreactors and potentiometric biosensors are investigated analytically and numerically using a three-layer mathematical model involving the Michaelis–Menten type reaction in the transient and steady states. Analytical expressions of the steady state substrate and reaction product concentrations and the bioreactor effectiveness as well as biosensor output potential are presented for the first and zero-order reaction rates. Mathematical modelling of the diffusion limiting membrane and the conditions under which the same values of the steady state characteristics are obtained when simulating the treated system at different values of the diffusion and distribution coefficients are investigated. The effective diffusion coefficients in the total diffusion layer consisting of the diffusion limiting membrane and the outer diffusion (Nernst) layer are applied to reduce the three-layer model to the corresponding two-layer model. The dynamics and behaviour of the substrate consumption rate, product emission rate, effectiveness factor and the output potential are numerically investigated.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"974 ","pages":"Article 118698"},"PeriodicalIF":4.1,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142441614","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 : 2024-10-11DOI: 10.1016/j.jelechem.2024.118713
Hualan Luo , Shenqi Wei , Pingxing Xing , Yuanyuan Wang , Liyi Dai
The development of efficient non-precious metal electrocatalysts for electrochemical water splitting is still a huge challenge. In this study, we designed and synthesized an efficient electrocatalyst for Ni-doped cobalt sulfide supported on 3D RGO (Ni-CoS2/3D RGO) using a simple one-step solvent-thermal method. Ni doping adjusted the charge distribution on the surface of the material, significantly improved the catalytic activity, and then accelerated the reaction kinetics. The high specific surface area and high stability of 3D RGO greatly improved the intrinsic activity of the material, making Ni-CoS2/3D RGO exhibit superior catalytic activity in both electrochemical hydrogen evolution and oxygen evolution. We evaluated the morphology and properties of the catalysts through a series of characterization methods and electrochemical performance tests. When the current density is 10 mA cm−2, the HER overpotential of Ni-CoS2/3D RGO under acidic condition reaches 138 mV, and the Tafel slope is 61 mV dec−1. Under alkaline conditions, the OER overpotential reaches 286 mV, and the Tafel slope is only 48 mV dec−1. And the OWS overpotential of the catalyst is 1.41 V and 1.82 V under acidic and alkaline conditions, respectively, indicating that the catalyst has ideal water splitting performance. This work provides a new idea for the application of 3D reduced graphene oxide in electrochemical direction, and also provides a new strategy for the design and preparation of non-precious metal catalysts for the efficient electrochemical water splitting.
{"title":"Ni-CoS2 nanoparticles loaded on 3D RGO for efficient electrochemical hydrogen and oxygen evolution reaction","authors":"Hualan Luo , Shenqi Wei , Pingxing Xing , Yuanyuan Wang , Liyi Dai","doi":"10.1016/j.jelechem.2024.118713","DOIUrl":"10.1016/j.jelechem.2024.118713","url":null,"abstract":"<div><div>The development of efficient non-precious metal electrocatalysts for electrochemical water splitting is still a huge challenge. In this study, we designed and synthesized an efficient electrocatalyst for Ni-doped cobalt sulfide supported on 3D RGO (Ni-CoS<sub>2</sub>/3D RGO) using a simple one-step solvent-thermal method. Ni doping adjusted the charge distribution on the surface of the material, significantly improved the catalytic activity, and then accelerated the reaction kinetics. The high specific surface area and high stability of 3D RGO greatly improved the intrinsic activity of the material, making Ni-CoS<sub>2</sub>/3D RGO exhibit superior catalytic activity in both electrochemical hydrogen evolution and oxygen evolution. We evaluated the morphology and properties of the catalysts through a series of characterization methods and electrochemical performance tests. When the current density is 10 mA cm<sup>−2</sup>, the HER overpotential of Ni-CoS<sub>2</sub>/3D RGO under acidic condition reaches 138 mV, and the Tafel slope is 61 mV dec<sup>−1</sup>. Under alkaline conditions, the OER overpotential reaches 286 mV, and the Tafel slope is only 48 mV dec<sup>−1</sup>. And the OWS overpotential of the catalyst is 1.41 V and 1.82 V under acidic and alkaline conditions, respectively, indicating that the catalyst has ideal water splitting performance. This work provides a new idea for the application of 3D reduced graphene oxide in electrochemical direction, and also provides a new strategy for the design and preparation of non-precious metal catalysts for the efficient electrochemical water splitting.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"974 ","pages":"Article 118713"},"PeriodicalIF":4.1,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142527489","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 : 2024-10-10DOI: 10.1016/j.jelechem.2024.118692
Dazhi Zhang , Yaqi Wang , Maosheng Yang , Jiajia Zhang , Ju Wu , Honglai Liu , Jianjun Wu , Peipei Li
The development of multicomponent electrodes incorporating diverse capacitive materials has become a viable strategy for engineering high-performance supercapacitors. In this paper, a sandwich-structured ternary composite consisting of polyaniline (PANI), manganese dioxide (MnO2), and porous carbon-derived from waste tires (PCDWT) has been synthesized via in-situ chemical oxidative polymerization of aniline. The composite features worm-like PANI tightly and uniformly coated on pompon-like PCDWT/MnO2 surfaces, facilitated by MnO2 serving as a reactive template during polymerization. The ternary nanocomposite PCDWT/MnO2/PANI-3 g exhibited exceptional electrochemical performance, achieving a specific capacitance of 369.6F/g at 1.0 A/g in three-electrode configuration. Remarkably, it retained 95.5 % of its initial capacitance after 6,000 charge–discharge cycles at 10 A/g. Moreover, an asymmetric supercapacitor fabricated with PCDWT/MnO2/PANI-3 g and PCDWT electrodes exhibited a specific capacitance of 91.34F/g at 0.5 A/g. The device delivered a maximum energy density of 36.66 Wh kg−1 at a power density of 424.99 W kg−1 and maintained capacitance holdings of 87.72 % after 10,000 cycles at 10 A/g. This superior electrochemical performance can be attributed to the synergistic effects of the PCDWT/MnO2 scaffold, which enhances charge transfer and electron transport, and the outer PANI layer, which improves the electrical conductivity of MnO2, protects against dissolution, and increases electroactive sites.
{"title":"Preparation of sandwich-structured ternary nanocomposites porous carbon-derived from waste tires/manganese dioxide/polyaniline as electrode for supercapacitor","authors":"Dazhi Zhang , Yaqi Wang , Maosheng Yang , Jiajia Zhang , Ju Wu , Honglai Liu , Jianjun Wu , Peipei Li","doi":"10.1016/j.jelechem.2024.118692","DOIUrl":"10.1016/j.jelechem.2024.118692","url":null,"abstract":"<div><div>The development of multicomponent electrodes incorporating diverse capacitive materials has become a viable strategy for engineering high-performance supercapacitors. In this paper, a sandwich-structured ternary composite consisting of polyaniline (PANI), manganese dioxide (MnO<sub>2</sub>), and porous carbon-derived from waste tires (PCDWT) has been synthesized via in-situ chemical oxidative polymerization of aniline. The composite features worm-like PANI tightly and uniformly coated on pompon-like PCDWT/MnO<sub>2</sub> surfaces, facilitated by MnO<sub>2</sub> serving as a reactive template during polymerization. The ternary nanocomposite PCDWT/MnO<sub>2</sub>/PANI-3 g exhibited exceptional electrochemical performance, achieving a specific capacitance of 369.6F/g at 1.0 A/g in three-electrode configuration. Remarkably, it retained 95.5 % of its initial capacitance after 6,000 charge–discharge cycles at 10 A/g. Moreover, an asymmetric supercapacitor fabricated with PCDWT/MnO<sub>2</sub>/PANI-3 g and PCDWT electrodes exhibited a specific capacitance of 91.34F/g at 0.5 A/g. The device delivered a maximum energy density of 36.66 Wh kg<sup>−1</sup> at a power density of 424.99 W kg<sup>−1</sup> and maintained capacitance holdings of 87.72 % after 10,000 cycles at 10 A/g. This superior electrochemical performance can be attributed to the synergistic effects of the PCDWT/MnO<sub>2</sub> scaffold, which enhances charge transfer and electron transport, and the outer PANI layer, which improves the electrical conductivity of MnO<sub>2</sub>, protects against dissolution, and increases electroactive sites.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"974 ","pages":"Article 118692"},"PeriodicalIF":4.1,"publicationDate":"2024-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142441505","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 : 2024-10-10DOI: 10.1016/j.jelechem.2024.118708
Vitaliy A. Kislenko, Sergey V. Pavlov, Sergey A. Kislenko
Nitrogen-doped carbon materials (NCMs) are widely regarded as promising alternatives to expensive platinum-based electrocatalysts for the oxygen reduction reaction (ORR). While NCMs exhibit considerable electrochemical activity in alkaline media, their performance in acidic environments remains a significant challenge. However, acidic conditions are commercially desirable for ORR’s catalysis in proton-exchange membrane fuel cells (PEMFCs). The dramatic pH dependence of NCM effectiveness has sparked ongoing debate, with several factors under consideration, including surface protonation, variations in hydrogen binding energy, differences in proton donors, and interface structure. In this work, we present a grand canonical density functional theory (GCDFT) study of the chemisorption step on pristine and nitrogen-doped graphene. Through nudged elastic band (NEB) calculations at various electrode potentials, we propose a potential-dependent (and thus pH-dependent) mechanism of oxygen chemisorption at graphitic nitrogen () defects, offering new insights into the pH dependency of the onset potential in NCM catalysts.
{"title":"Potential-dependent kinetics of oxygen chemisorption as the crucial step of oxygen reduction reaction: GCDFT study","authors":"Vitaliy A. Kislenko, Sergey V. Pavlov, Sergey A. Kislenko","doi":"10.1016/j.jelechem.2024.118708","DOIUrl":"10.1016/j.jelechem.2024.118708","url":null,"abstract":"<div><div>Nitrogen-doped carbon materials (NCMs) are widely regarded as promising alternatives to expensive platinum-based electrocatalysts for the oxygen reduction reaction (ORR). While NCMs exhibit considerable electrochemical activity in alkaline media, their performance in acidic environments remains a significant challenge. However, acidic conditions are commercially desirable for ORR’s catalysis in proton-exchange membrane fuel cells (PEMFCs). The dramatic pH dependence of NCM effectiveness has sparked ongoing debate, with several factors under consideration, including surface protonation, variations in hydrogen binding energy, differences in proton donors, and interface structure. In this work, we present a grand canonical density functional theory (GCDFT) study of the chemisorption step on pristine and nitrogen-doped graphene. Through nudged elastic band (NEB) calculations at various electrode potentials, we propose a potential-dependent (and thus pH-dependent) mechanism of oxygen chemisorption at graphitic nitrogen (<span><math><msub><mrow><mi>N</mi></mrow><mrow><mi>gr</mi></mrow></msub></math></span>) defects, offering new insights into the pH dependency of the onset potential in NCM catalysts.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"974 ","pages":"Article 118708"},"PeriodicalIF":4.1,"publicationDate":"2024-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142441508","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 : 2024-10-10DOI: 10.1016/j.jelechem.2024.118710
Şehriban Düzmen, Tuğçe Teker, Mehmet Aslanoglu
Yohimbine is a natural supplement to improve symptoms of erectile dysfunction. Yohimbine supplementations are also used for body composition and weight loss. Yohimbine may cause several complications including nausea, abdominal pain, dizziness, nervousness, anxiety and severe acute intoxication. Thus, a sensitive method of analysis is of requirement since many yohimbine-containing supplements are reported to be inaccurately labelled. For this purpose, a novel sensor was constructed by modifying a glassy carbon electrode (GCE) with ultrasonication-assisted preparation of erbium oxide nanoparticles and carbon nanofibers (GCE/CNFs@Er2O3) for the measurement of yohimbine. An electro-active surface area of 0.054, 0.196 and 0.330 cm2 was calculated for GCE, GCE/CNFs and GCE/CNFs@Er2O3, respectively. The impact of nanoparticles of Er2O3 resulted in a good synergistic effect, leading to a large increase in the peak response and a remarkable change in the oxidation potential (Epa) of yohimbine. The novel platform exhibited a linear range of 2.0 × 10-8 ∼ 1.6 × 10-5 M and a detection limit of 8.0 × 10-9 M. GCE/CNFs@Er2O3 exhibited high accuracy and excellent precision for the analysis of yohimbine capsule and urine. In addition, a standard Gibbs free-energy change (ΔG0) of –22.7 kJ/mol at 25 ℃ reveals that the interaction of yohimbine with DNA occurs spontaneously.
{"title":"A nanostructure based voltammetric platform constructed with carbon nanofibers and erbium nanoparticles for the determination of yohimbine and its DNA binding","authors":"Şehriban Düzmen, Tuğçe Teker, Mehmet Aslanoglu","doi":"10.1016/j.jelechem.2024.118710","DOIUrl":"10.1016/j.jelechem.2024.118710","url":null,"abstract":"<div><div>Yohimbine is a natural supplement to improve symptoms of erectile dysfunction. Yohimbine supplementations are also used for body composition and weight loss. Yohimbine may cause several complications including nausea, abdominal pain, dizziness, nervousness, anxiety and severe acute intoxication. Thus, a sensitive method of analysis is of requirement since many yohimbine-containing supplements are reported to be inaccurately labelled. For this purpose, a novel sensor was constructed by modifying a glassy carbon electrode (GCE) with ultrasonication-assisted preparation of erbium oxide nanoparticles and carbon nanofibers (GCE/CNFs@Er<sub>2</sub>O<sub>3</sub>) for the measurement of yohimbine. An electro-active surface area of 0.054, 0.196 and 0.330 cm<sup>2</sup> was calculated for GCE, GCE/CNFs and GCE/CNFs@Er<sub>2</sub>O<sub>3</sub>, respectively. The impact of nanoparticles of Er<sub>2</sub>O<sub>3</sub> resulted in a good synergistic effect, leading to a large increase in the peak response and a remarkable change in the oxidation potential (Epa) of yohimbine. The novel platform exhibited a linear range of 2.0 × 10<sup>-8</sup> ∼ 1.6 × 10<sup>-5</sup> M and a detection limit of 8.0 × 10<sup>-9</sup> M. GCE/CNFs@Er<sub>2</sub>O<sub>3</sub> exhibited high accuracy and excellent precision for the analysis of yohimbine capsule and urine. In addition, a standard Gibbs free-energy change (ΔG<sup>0</sup>) of –22.7 kJ/mol at 25 ℃ reveals that the interaction of yohimbine with DNA occurs spontaneously.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"974 ","pages":"Article 118710"},"PeriodicalIF":4.1,"publicationDate":"2024-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142432791","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 : 2024-10-10DOI: 10.1016/j.jelechem.2024.118699
K. Azgaou , W. Ettahiri , E. Ech-chihbi , M. Adardour , Mohammad Azam , M. Benmessaoud , A. Baouid , Kim Min , S. El Hajjaji
Two newly synthesized benzimidazole compounds, 1-(Cyclopent-1-en-1-yl)-3-(prop-2-yn-1-yl)-1H-benzimidazol-2(3H)-one (IMD1) and 1-allyl-3-(cyclopent-1-en-1-yl)-1H-benzimidazol-2(3H)-one (IMD2), were evaluated for corrosion inhibition on mild steel (MS) in 1.0 M HCl solution. Techniques such as potentiodynamic polarization (PDP), electrochemical impedance spectroscopy (EIS), and weight loss (WL) analysis were employed. EIS analysis indicated increased resistance with compound concentration, suggesting the formation of a protective film at the MS/HCl interface. The formation of this protective coating was further confirmed through SEM-EDX analysis. PDP plots suggested a mixed-type inhibition mechanism. At 10−4 M concentration, IMD1 and IMD2 showed significant inhibition efficiencies of 98.1 % and 95.6 %, respectively. DFT gives insights into charge-sharing (donor–acceptor) interactions between inhibitor molecules and metallic surfaces. Monte Carlo simulation (MCS) confirmed these results, indicating that the molecules studied adsorbed almost parallel to the Fe (1 1 0) surface.
{"title":"Experimental and computational study of newly synthesized benzimidazole derivatives as corrosion inhibitors for mild steel in 1.0 M HCl: Electrochemical, surface studies, DFT modeling, and MC simulation","authors":"K. Azgaou , W. Ettahiri , E. Ech-chihbi , M. Adardour , Mohammad Azam , M. Benmessaoud , A. Baouid , Kim Min , S. El Hajjaji","doi":"10.1016/j.jelechem.2024.118699","DOIUrl":"10.1016/j.jelechem.2024.118699","url":null,"abstract":"<div><div>Two newly synthesized benzimidazole compounds, 1-(Cyclopent-1-en-1-yl)-3-(prop-2-yn-1-yl)-1H-benzimidazol-2(3H)-one (<strong>IMD1</strong>) and 1-allyl-3-(cyclopent-1-en-1-yl)-1H-benzimidazol-2(3H)-one (<strong>IMD2</strong>), were evaluated for corrosion inhibition on mild steel (MS) in 1.0 M HCl solution. Techniques such as potentiodynamic polarization (PDP), electrochemical impedance spectroscopy (EIS), and weight loss (WL) analysis were employed. EIS analysis indicated increased resistance with compound concentration, suggesting the formation of a protective film at the MS/HCl interface. The formation of this protective coating was further confirmed through SEM-EDX analysis. PDP plots suggested a mixed-type inhibition mechanism. At 10<sup>−4</sup> M concentration, IMD1 and IMD2 showed significant inhibition efficiencies of 98.1 % and 95.6 %, respectively. DFT gives insights into charge-sharing (donor–acceptor) interactions between inhibitor molecules and metallic surfaces. Monte Carlo simulation (MCS) confirmed these results, indicating that the molecules studied adsorbed almost parallel to the Fe (1 1 0) surface.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"974 ","pages":"Article 118699"},"PeriodicalIF":4.1,"publicationDate":"2024-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142432792","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 : 2024-10-10DOI: 10.1016/j.jelechem.2024.118703
Jingjing Yuan , Wenyong Xi , Yifan Qiao , Yan Zhou , Yuan Ruan , Hui Xu , Yifan Li , Junjie He , Guangyu He , Haiqun Chen
ZnMn2O4 spinel is considered a promising cathode material for zinc-ion batteries due to its superior Zn2+ storage capability. However, the widespread utilization of ZnMn2O4 spinel as a high-capacity cathode material is impeded by its insufficient electrical conductivity. To tackle this limitation, we have employed a sulfur doping approach by substituting sulfur for oxygen atoms within the ZnMn2O4 lattice structure. After theoretical calculation, the charge exchange between metal Zn/Mn and surrounding coordinated atoms is enhanced after sulfur doping. The sulfur-doped ZnMn2O4 spinel effectively enhances the electrical conductivity, improving its electrochemical discharge capacity. Furthermore, the results reveals that a doping level of 20 % provided the greatest enhancement in capacitance, achieving a specific capacity of 220.1 mAh/g. This work improves the disadvantages of ZnMn2O4 at the atomic level and can provide ideas for the optimization and modification of spinel cathode materials.
{"title":"Sulfur-doped enhanced ZnMn2O4 spinel for high-capacity zinc-ion batteries: Facilitating charge transfer","authors":"Jingjing Yuan , Wenyong Xi , Yifan Qiao , Yan Zhou , Yuan Ruan , Hui Xu , Yifan Li , Junjie He , Guangyu He , Haiqun Chen","doi":"10.1016/j.jelechem.2024.118703","DOIUrl":"10.1016/j.jelechem.2024.118703","url":null,"abstract":"<div><div>ZnMn<sub>2</sub>O<sub>4</sub> spinel is considered a promising cathode material for zinc-ion batteries due to its superior Zn<sup>2+</sup> storage capability. However, the widespread utilization of ZnMn<sub>2</sub>O<sub>4</sub> spinel as a high-capacity cathode material is impeded by its insufficient electrical conductivity. To tackle this limitation, we have employed a sulfur doping approach by substituting sulfur for oxygen atoms within the ZnMn<sub>2</sub>O<sub>4</sub> lattice structure. After theoretical calculation, the charge exchange between metal Zn/Mn and surrounding coordinated atoms is enhanced after sulfur doping. The sulfur-doped ZnMn<sub>2</sub>O<sub>4</sub> spinel effectively enhances the electrical conductivity, improving its electrochemical discharge capacity. Furthermore, the results reveals that a doping level of 20 % provided the greatest enhancement in capacitance, achieving a specific capacity of 220.1 mAh/g. This work improves the disadvantages of ZnMn<sub>2</sub>O<sub>4</sub> at the atomic level and can provide ideas for the optimization and modification of spinel cathode materials.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"974 ","pages":"Article 118703"},"PeriodicalIF":4.1,"publicationDate":"2024-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142432793","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 : 2024-10-09DOI: 10.1016/j.jelechem.2024.118704
Linwei Xie, Jiao Hou, Chenglong Xia, Xiaoguang Liu, Ling Li
An effective method to improve the catalytic performance of electrocatalytic alcohol oxidation by establishing strong interfacial interactions through novel carrier materials and polymetallic alloys. In this paper, novel polyhedral metal–organic framework Al-based [Al(OH)(mBDC)] (CAU-10) composites with PdPbBi trimetallic particles embedded in folded graphene oxide (rGO) modified by a simple hydrothermal reaction were prepared and applied to the electrocatalytic oxidation reaction of ethylene glycol. The results of electrochemical tests showed that the trimetallic catalysts exhibited excellent electrocatalytic activity compared to commercial Pd/C. In particular, PdPbBi@rGO/CAU-10 has the highest peak current density of 241.82 mA cm−2, which is 8.97 times higher than that of Pd/C (26.92 mA cm−2), and the largest electrochemical active area (ECSA) value of 88.12 mA cm−2, which is 2.40 times higher than that of Pd/C (36.75 mA cm−2). This outstanding electrocatalytic activity is mainly attributed to the polyhedral structure of CAU-10 composite carriers and the abundance of oxygen-containing atoms, which is conducive to the homogeneous loading of metals, at the same time, the strong electronic effect between Pd, Pb and Bi and the abundance of oxygen-containing species provide significant enhancement of electrocatalytic activity and stability, which provides an important reference for the development of electrocatalysts for ethylene glycol fuel cells.
通过新型载体材料和多金属合金建立强界面相互作用，是提高电催化醇氧化催化性能的有效方法。本文制备了新型多面体金属有机框架铝基[Al(OH)(mBDC)]（CAU-10）复合材料，其PdPbBi三金属粒子嵌入折叠氧化石墨烯（rGO）中，并通过简单的水热反应进行修饰，将其应用于乙二醇的电催化氧化反应。电化学测试结果表明，与商用 Pd/C 相比，三金属催化剂具有优异的电催化活性。其中，PdPbBi@rGO/CAU-10 的峰值电流密度最高，为 241.82 mA cm-2，是 Pd/C （26.92 mA cm-2）的 8.97 倍；电化学活性面积（ECSA）值最大，为 88.12 mA cm-2，是 Pd/C （36.75 mA cm-2）的 2.40 倍。这种突出的电催化活性主要得益于CAU-10复合载体的多面体结构和含氧原子的丰富性，有利于金属的均匀负载，同时Pd、Pb和Bi之间的强电子效应和含氧物种的丰富性也显著增强了电催化活性和稳定性，为乙二醇燃料电池电催化剂的开发提供了重要参考。
{"title":"Preparation of rGO/CAU-10 anchored PdPbBi composites and their electrocatalytic ethylene glycol properties","authors":"Linwei Xie, Jiao Hou, Chenglong Xia, Xiaoguang Liu, Ling Li","doi":"10.1016/j.jelechem.2024.118704","DOIUrl":"10.1016/j.jelechem.2024.118704","url":null,"abstract":"<div><div>An effective method to improve the catalytic performance of electrocatalytic alcohol oxidation by establishing strong interfacial interactions through novel carrier materials and polymetallic alloys. In this paper, novel polyhedral metal–organic framework Al-based [Al(OH)(mBDC)] (CAU-10) composites with PdPbBi trimetallic particles embedded in folded graphene oxide (rGO) modified by a simple hydrothermal reaction were prepared and applied to the electrocatalytic oxidation reaction of ethylene glycol. The results of electrochemical tests showed that the trimetallic catalysts exhibited excellent electrocatalytic activity compared to commercial Pd/C. In particular, PdPbBi@rGO/CAU-10 has the highest peak current density of 241.82 mA cm<sup>−2</sup>, which is 8.97 times higher than that of Pd/C (26.92 mA cm<sup>−2</sup>), and the largest electrochemical active area (ECSA) value of 88.12 mA cm<sup>−2</sup>, which is 2.40 times higher than that of Pd/C (36.75 mA cm<sup>−2</sup>). This outstanding electrocatalytic activity is mainly attributed to the polyhedral structure of CAU-10 composite carriers and the abundance of oxygen-containing atoms, which is conducive to the homogeneous loading of metals, at the same time, the strong electronic effect between Pd, Pb and Bi and the abundance of oxygen-containing species provide significant enhancement of electrocatalytic activity and stability, which provides an important reference for the development of electrocatalysts for ethylene glycol fuel cells.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"974 ","pages":"Article 118704"},"PeriodicalIF":4.1,"publicationDate":"2024-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142432789","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 : 2024-10-09DOI: 10.1016/j.jelechem.2024.118705
Liyan Wang , Jiahan Li , Fei Xie, Dan Wang, Ming Wu
Sulfate-reducing bacteria (SRB) present in sea mud pose a challenge to the safe operation of subsea pipelines. Chlorides and sulfates in sea mud promote the microbial corrosion of subsea pipelines by SRB. This study investigates the effects of sulfate and chloride on the microbial corrosion of X80 pipeline steel in the sea mud environment. The results indicate that sulfate serves as an electron acceptor, promoting the growth of SRB, while chloride regulates the osmotic pressure of SRB cells, affecting their bioactivity. SRB exhibit more aggressive corrosion behavior in sea mud with high concentrations of both chloride and sulfate.
{"title":"Anions exacerbate microbial corrosion of X80 pipeline steel induced by sulfate-reducing bacteria in the sea mud environment","authors":"Liyan Wang , Jiahan Li , Fei Xie, Dan Wang, Ming Wu","doi":"10.1016/j.jelechem.2024.118705","DOIUrl":"10.1016/j.jelechem.2024.118705","url":null,"abstract":"<div><div>Sulfate-reducing bacteria (SRB) present in sea mud pose a challenge to the safe operation of subsea pipelines. Chlorides and sulfates in sea mud promote the microbial corrosion of subsea pipelines by SRB. This study investigates the effects of sulfate and chloride on the microbial corrosion of X80 pipeline steel in the sea mud environment. The results indicate that sulfate serves as an electron acceptor, promoting the growth of SRB, while chloride regulates the osmotic pressure of SRB cells, affecting their bioactivity. SRB exhibit more aggressive corrosion behavior in sea mud with high concentrations of both chloride and sulfate.</div></div>","PeriodicalId":355,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"973 ","pages":"Article 118705"},"PeriodicalIF":4.1,"publicationDate":"2024-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142422852","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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