{"title":"Ni(II) Complex Based on Imidazole Dicarboxylic Acid as a Promising Electrocatalyst for Hydrogen Evolution Reaction and H2O2-Sensing","authors":"Xia Tang, Wei Gao, Zhengwei Wu, Tiantian Wan, Qinqin Shen, Xiaoxia Kong, Kaiyi Li, Huilu Wu","doi":"10.1007/s12678-024-00866-x","DOIUrl":null,"url":null,"abstract":"<div><p>The determination of complex structure helps to explore its reaction mechanism and provides design strategies for guiding synthesis of high-performance hydrogen evolution reaction (HER) electrocatalysts. A new mononuclear Ni(II) complex, [Ni(<i>p</i>-MOPhH<sub>2</sub>IDC)<sub>2</sub>(H<sub>2</sub>O)<sub>2</sub>], was synthesized by the reaction of <i>p</i>-MOPhH<sub>3</sub>IDC (2-(4-methoxyphenyl)-1 H-imidazole-4,5-dicarboxylic acid) and Ni(NO<sub>3</sub>)<sub>2</sub>·6H<sub>2</sub>O under solvothermal conditions and characterized by single-crystal X-ray diffraction, elemental analysis, IR and UV-vis spectroscopy. The structure analysis revealed that the nickel center was six-coordinated octahedron coordination geometry. The electrochemical properties of the Ni(II) complex-doped carbon paste electrode (Ni-CPE) were investigated by cyclic voltammetry (CV), linear sweep voltammetry (LSV) and electrochemical impedance spectroscopy (EIS) in 0.5 M H<sub>2</sub>SO<sub>4</sub> electrolyte. The HER measurements show that the η<sub>10</sub><sup>298K</sup> (overpotential, 10 mA cm<sup>–2</sup>) of the Ni-CPE was positively shifted by 265 mv compared with the bare-CPE (without complex). The Tafel slope of the Ni-CPE was 187 mV dec<sup>− 1</sup>. These indicated that the Ni-CPE was effective for HER electrocatalytic reaction. In addition, the electrochemical sensing performances of the Ni-CPE towards H<sub>2</sub>O<sub>2</sub> were found to have a linear response from 0.5 µM to 4.0 mM with a detection limit of 0.036 µM. The above studies prove that the Ni(II) complex can be used as an effective bi-functional molecular electrocatalyst for HER and H<sub>2</sub>O<sub>2</sub> sensing, and provide a new approach for designing efficient, non-precious metal electrochemical catalysts.</p><h3>Graphical Abstract</h3><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div><p>A new mononuclear Ni(II) complex, [Ni(<i>p</i>-MOPhH<sub>2</sub>IDC)<sub>2</sub>(H<sub>2</sub>O)<sub>2</sub>], was synthesized under solvothermal conditions. The electrochemical properties of the Ni(II) complex-doped carbon paste electrode (Ni-CPE) were investigated. In the HER study, the Ni-CPE has more positive overpotentials (<i>η</i><sub>10</sub><sup>293K</sup>), smaller Tafel slopes and lower activation energies in the HER process compared to the bare-CPE, demonstrating that the Ni-CPE has effective electrocatalytic hydrogen evolution activity. Moreover, electrochemical sensing performance shows that Ni-CPE has good detection ability for H<sub>2</sub>O<sub>2</sub> and exhibit good stability and anti-interference properties. Therefore, the Ni-CPE can be used as an effective bifunctional electrocatalyst.</p></div>","PeriodicalId":535,"journal":{"name":"Electrocatalysis","volume":"15 2-3","pages":""},"PeriodicalIF":2.7000,"publicationDate":"2024-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Electrocatalysis","FirstCategoryId":"92","ListUrlMain":"https://link.springer.com/article/10.1007/s12678-024-00866-x","RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
The determination of complex structure helps to explore its reaction mechanism and provides design strategies for guiding synthesis of high-performance hydrogen evolution reaction (HER) electrocatalysts. A new mononuclear Ni(II) complex, [Ni(p-MOPhH2IDC)2(H2O)2], was synthesized by the reaction of p-MOPhH3IDC (2-(4-methoxyphenyl)-1 H-imidazole-4,5-dicarboxylic acid) and Ni(NO3)2·6H2O under solvothermal conditions and characterized by single-crystal X-ray diffraction, elemental analysis, IR and UV-vis spectroscopy. The structure analysis revealed that the nickel center was six-coordinated octahedron coordination geometry. The electrochemical properties of the Ni(II) complex-doped carbon paste electrode (Ni-CPE) were investigated by cyclic voltammetry (CV), linear sweep voltammetry (LSV) and electrochemical impedance spectroscopy (EIS) in 0.5 M H2SO4 electrolyte. The HER measurements show that the η10298K (overpotential, 10 mA cm–2) of the Ni-CPE was positively shifted by 265 mv compared with the bare-CPE (without complex). The Tafel slope of the Ni-CPE was 187 mV dec− 1. These indicated that the Ni-CPE was effective for HER electrocatalytic reaction. In addition, the electrochemical sensing performances of the Ni-CPE towards H2O2 were found to have a linear response from 0.5 µM to 4.0 mM with a detection limit of 0.036 µM. The above studies prove that the Ni(II) complex can be used as an effective bi-functional molecular electrocatalyst for HER and H2O2 sensing, and provide a new approach for designing efficient, non-precious metal electrochemical catalysts.
Graphical Abstract
A new mononuclear Ni(II) complex, [Ni(p-MOPhH2IDC)2(H2O)2], was synthesized under solvothermal conditions. The electrochemical properties of the Ni(II) complex-doped carbon paste electrode (Ni-CPE) were investigated. In the HER study, the Ni-CPE has more positive overpotentials (η10293K), smaller Tafel slopes and lower activation energies in the HER process compared to the bare-CPE, demonstrating that the Ni-CPE has effective electrocatalytic hydrogen evolution activity. Moreover, electrochemical sensing performance shows that Ni-CPE has good detection ability for H2O2 and exhibit good stability and anti-interference properties. Therefore, the Ni-CPE can be used as an effective bifunctional electrocatalyst.
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Electrocatalysis is cross-disciplinary in nature, and attracts the interest of chemists, physicists, biochemists, surface and materials scientists, and engineers. Electrocatalysis provides the unique international forum solely dedicated to the exchange of novel ideas in electrocatalysis for academic, government, and industrial researchers. Quick publication of new results, concepts, and inventions made involving Electrocatalysis stimulates scientific discoveries and breakthroughs, promotes the scientific and engineering concepts that are critical to the development of novel electrochemical technologies.
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