Scholarlink

<p>Today, prioritising the design of a highly active and efficient bifunctional electrocatalyst for water splitting is essential to meet global energy demands. In this study, two acylpyrazolone ligands (HPMBP and HPMTP) were used to form copper complexes {Cu(<b>1</b>) and Cu(<b>2</b>)}. Various analytical techniques and spectroscopic methods have been employed to determine the coordination mode and elucidate the structure and properties of the complexes. Theoretical studies were performed using DFT with the PBE/DNP basis set for calculations on the ligand atoms and their copper complexes. Spectroscopic data showed that the acylpyrazolone ligand acted as an anionic chelating bidentate ligand in copper complexes through the O,O pattern of hydroxyl (C-O-Cu) and carbonyl (C = O-Cu) groups. The geometry of the complexes is assigned as paramagnetic, elongated octahedral around the Cu(II) ion. The DFT study provides a comparative analysis of the reactivity and stability of the synthesised complexes, indicated by their HOMO-LUMO energy gaps, global reactivity, and Fukui descriptors. The high HOMO energy (− 5.754&#xa0;eV), lower LUMO energy (− 5.510&#xa0;eV), and high Fukui descriptors were observed for Cu(<b>2</b>) compared to Cu(<b>1</b>), which has a low HOMO energy of -5.690&#xa0;eV and a high LUMO energy of − 5.520&#xa0;eV. The complexes were screened for their electrocatalytic activity. Cu(<b>2</b>) has shown a low overpotential of 300 mV@10 mAcm<sup>− 2</sup>, a Tafel slope of 50 mV/dec, and an Rct of 2 Ω with excellent stability compared to Cu(<b>1</b>). Investigations of the mechanism revealed that the sulphate and pyrazolone groups participate in the formation of the O–O bond, thus enhancing the catalytic activity of the complexes.</p> Graphical Abstract <p></p>

错误：搜索内容不能为空，请输入英文关键词
错误：关键词超出字数限制，请精简
高级检索

Investigation of Promising Electrocatalytic Activity of Coordinated O,O-acylpyrazolone Copper(II) Complexes for Overall Water Splitting

  • 期刊论文

  • 发表日期：

    2025年8月12日

查看全文
  • Claudelle Sybilline Anensong Djadock,
  • Singaram Vengatesan,
  • kasthuri Annamalai Sami,
  • Emeline Sorelle Mefouegang,
  • Achille Nana,
  • Jean Ngoune,
  • Subbiah Ravichandrana,
  • Subramanyan Vasudevan

摘要

Today, prioritising the design of a highly active and efficient bifunctional electrocatalyst for water splitting is essential to meet global energy demands. In this study, two acylpyrazolone ligands (HPMBP and HPMTP) were used to form copper complexes {Cu(1) and Cu(2)}. Various analytical techniques and spectroscopic methods have been employed to determine the coordination mode and elucidate the structure and properties of the complexes. Theoretical studies were performed using DFT with the PBE/DNP basis set for calculations on the ligand atoms and their copper complexes. Spectroscopic data showed that the acylpyrazolone ligand acted as an anionic chelating bidentate ligand in copper complexes through the O,O pattern of hydroxyl (C-O-Cu) and carbonyl (C = O-Cu) groups. The geometry of the complexes is assigned as paramagnetic, elongated octahedral around the Cu(II) ion. The DFT study provides a comparative analysis of the reactivity and stability of the synthesised complexes, indicated by their HOMO-LUMO energy gaps, global reactivity, and Fukui descriptors. The high HOMO energy (− 5.754 eV), lower LUMO energy (− 5.510 eV), and high Fukui descriptors were observed for Cu(2) compared to Cu(1), which has a low HOMO energy of -5.690 eV and a high LUMO energy of − 5.520 eV. The complexes were screened for their electrocatalytic activity. Cu(2) has shown a low overpotential of 300 mV@10 mAcm− 2, a Tafel slope of 50 mV/dec, and an Rct of 2 Ω with excellent stability compared to Cu(1). Investigations of the mechanism revealed that the sulphate and pyrazolone groups participate in the formation of the O–O bond, thus enhancing the catalytic activity of the complexes.

Graphical Abstract