{"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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