{"title":"基于咪唑二羧酸的 Ni(II) 复合物有望成为氢气进化反应和 H2O2 传感的电催化剂","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":"{\"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}","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
摘要
确定络合物结构有助于探索其反应机理，并为指导合成高性能氢进化反应（HER）电催化剂提供设计策略。在溶热条件下，由 p-MOPh3IDC（2-(4-甲氧基苯基)-1 H-咪唑-4,5-二羧酸）和 Ni(NO3)2-6H2O 反应合成了一种新的单核 Ni(II) 复合物 [Ni(p-MOPh2IDC)2(H2O)2]，并通过单晶 X 射线衍射、元素分析、红外光谱和紫外可见光谱对其进行了表征。结构分析表明，镍中心为六配位八面体配位几何。在 0.5 M H2SO4 电解液中，通过循环伏安法（CV）、线性扫描伏安法（LSV）和电化学阻抗谱法（EIS）研究了掺杂镍（II）络合物的碳浆电极（Ni-CPE）的电化学特性。HER 测量结果表明，镍-CPE 的 η10298K（过电位，10 mA cm-2）与裸-CPE（不含复合物）相比正移了 265 mv。Ni-CPE 的塔菲尔斜率为 187 mV dec-1。这表明 Ni-CPE 对 HER 电催化反应非常有效。此外，Ni-CPE 对 H2O2 的电化学传感性能在 0.5 µM 至 4.0 mM 之间呈线性响应，检测限为 0.036 µM。上述研究证明，镍（II）配合物可作为一种有效的双功能分子电催化剂用于 HER 和 H2O2 的传感，并为设计高效的非贵金属电化学催化剂提供了一种新方法。研究了掺杂镍（II）配合物的碳浆电极（Ni-CPE）的电化学性能。在氢反应研究中，与裸碳糊电极相比，Ni-CPE 在氢反应过程中具有更正的过电位（η10293K）、更小的塔菲尔斜率和更低的活化能，这表明 Ni-CPE 具有有效的电催化氢进化活性。此外，电化学传感性能表明，Ni-CPE 对 H2O2 具有良好的检测能力，并表现出良好的稳定性和抗干扰性。因此，Ni-CPE 可用作一种有效的双功能电催化剂。
Ni(II) Complex Based on Imidazole Dicarboxylic Acid as a Promising Electrocatalyst for Hydrogen Evolution Reaction and H2O2-Sensing
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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