{"title":"Bisbenzimidazole silver(I) complexes regulated by aromatic polycarboxylates as electrocatalysts for hydrogen evolution reaction","authors":"Nannan Huang, Yueyue Xie, Quanlong Cai, Yuanyue Ma, Junjie Teng, Huilu Wu","doi":"10.1016/j.ica.2025.122693","DOIUrl":null,"url":null,"abstract":"<div><div>In this study, two new silver(I) complexes with different structures of [Ag<sub>2</sub>(3Py-bbs)<sub>2</sub>(BDC)]·2H<sub>2</sub>O (<strong>1</strong>), {[Ag<sub>2</sub>(3Py-bbs)<sub>2</sub>](HBTC)·4CH<sub>3</sub>CN·H<sub>2</sub>O}<sub>n</sub> (<strong>2</strong>) (3Py-bbs = bis[1-(pyridin-3-ylmethyl)-benzimidazol-2-ylmethyl] sulfane, H<sub>2</sub>BDC = terephthalic acid, H<sub>3</sub>BTC = trimesic acid) were synthesized by the regulation of aromatic polycarboxylic acids. The single-crystal X-ray diffraction analysis shows that the complex <strong>1</strong> is a binuclear structure, while the complex <strong>2</strong> is a one-dimensional ring-chain structure. The electrocatalytic hydrogen evolution reaction (HER) performance of silver(I) complexes <strong>1</strong> and <strong>2</strong> modified glassy carbon electrodes (1-GCE and 2-GCE) were investigated in 0.5 M H<sub>2</sub>SO<sub>4</sub>. The overpotential (<em>η</em><sub>10</sub><sup>298K</sup>) and Tafel slope (<em>b</em> <sup>298K</sup>) are −941 mV and 278 mV·dec<sup>−1</sup> for bare-GCE, −763 mV and 267 mV·dec<sup>−1</sup> for 1-GCE, −741 mV and 182 mV·dec<sup>−1</sup> for 2-GCE, respectively. The <em>η</em><sub>10</sub><sup>298K</sup> and <em>b</em><sup>298K</sup> of 1–2-GCE were significantly positive shifted and decreased compared with the bare-GCE, indicating that 1–2-GCE have good electrocatalytic HER activity and activity order is 2-GCE > 1-GCE, which is attributed to the difference in the skeleton structure of silver(I) complexes, that is, because of the well-dispersed metal center of the coordination polymer <strong>2</strong>. The present work provides new ideas into the development of non-precious metal complexes as modified electrode materials in electrocatalysis.</div></div>","PeriodicalId":13599,"journal":{"name":"Inorganica Chimica Acta","volume":"583 ","pages":"Article 122693"},"PeriodicalIF":2.7000,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Inorganica Chimica Acta","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0020169325001598","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, INORGANIC & NUCLEAR","Score":null,"Total":0}
Bisbenzimidazole silver(I) complexes regulated by aromatic polycarboxylates as electrocatalysts for hydrogen evolution reaction
In this study, two new silver(I) complexes with different structures of [Ag2(3Py-bbs)2(BDC)]·2H2O (1), {[Ag2(3Py-bbs)2](HBTC)·4CH3CN·H2O}n (2) (3Py-bbs = bis[1-(pyridin-3-ylmethyl)-benzimidazol-2-ylmethyl] sulfane, H2BDC = terephthalic acid, H3BTC = trimesic acid) were synthesized by the regulation of aromatic polycarboxylic acids. The single-crystal X-ray diffraction analysis shows that the complex 1 is a binuclear structure, while the complex 2 is a one-dimensional ring-chain structure. The electrocatalytic hydrogen evolution reaction (HER) performance of silver(I) complexes 1 and 2 modified glassy carbon electrodes (1-GCE and 2-GCE) were investigated in 0.5 M H2SO4. The overpotential (η10298K) and Tafel slope (b298K) are −941 mV and 278 mV·dec−1 for bare-GCE, −763 mV and 267 mV·dec−1 for 1-GCE, −741 mV and 182 mV·dec−1 for 2-GCE, respectively. The η10298K and b298K of 1–2-GCE were significantly positive shifted and decreased compared with the bare-GCE, indicating that 1–2-GCE have good electrocatalytic HER activity and activity order is 2-GCE > 1-GCE, which is attributed to the difference in the skeleton structure of silver(I) complexes, that is, because of the well-dispersed metal center of the coordination polymer 2. The present work provides new ideas into the development of non-precious metal complexes as modified electrode materials in electrocatalysis.
期刊介绍:
Inorganica Chimica Acta is an established international forum for all aspects of advanced Inorganic Chemistry. Original papers of high scientific level and interest are published in the form of Articles and Reviews.
Topics covered include:
• chemistry of the main group elements and the d- and f-block metals, including the synthesis, characterization and reactivity of coordination, organometallic, biomimetic, supramolecular coordination compounds, including associated computational studies;
• synthesis, physico-chemical properties, applications of molecule-based nano-scaled clusters and nanomaterials designed using the principles of coordination chemistry, as well as coordination polymers (CPs), metal-organic frameworks (MOFs), metal-organic polyhedra (MPOs);
• reaction mechanisms and physico-chemical investigations computational studies of metalloenzymes and their models;
• applications of inorganic compounds, metallodrugs and molecule-based materials.
Papers composed primarily of structural reports will typically not be considered for publication.