Bisbenzimidazole silver(I) complexes regulated by aromatic polycarboxylates as electrocatalysts for hydrogen evolution reaction

IF 2.7 3区化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR

Inorganica Chimica Acta Pub Date : 2025-04-11 DOI:10.1016/j.ica.2025.122693

Nannan Huang, Yueyue Xie, Quanlong Cai, Yuanyue Ma, Junjie Teng, Huilu Wu

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Abstract

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 (η₁₀^298K) and Tafel slope (b ^298K) 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 η₁₀^298K and b^298K 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.

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本研究通过芳香族聚羧酸的调节合成了两种新的银（I）配合物，它们具有不同的结构：[Ag2(3Py-bbs)2(BDC)]-2H2O (1)、{[Ag2(3Py-bbs)2](HBTC)-4CH3CN-H2O}n (2) (3Py-bbs = 双[1-(吡啶-3-基甲基)-苯并咪唑-2-基甲基]硫烷、H2BDC=对苯二甲酸，H3BTC=三聚甲酸）由芳香族聚羧酸调节合成。单晶 X 射线衍射分析表明，配合物 1 为双核结构，配合物 2 为一维环链结构。在 0.5 M H2SO4 中，研究了银(I)配合物 1 和 2 修饰的玻璃碳电极（1-GCE 和 2-GCE）的电催化氢进化反应（HER）性能。裸 GCE 的过电位（η10298K）和 Tafel 斜率（b 298K）分别为 -941 mV 和 278 mV-dec-1，1-GCE 为 -763 mV 和 267 mV-dec-1，2-GCE 为 -741 mV 和 182 mV-dec-1。与裸 GCE 相比，1-2-GCE 的 η10298K 和 b298K 显著正移和降低，表明 1-2-GCE 具有良好的电催化 HER 活性，且活性顺序为 2-GCE > 1-GCE，这归因于银（I）配合物骨架结构的不同，即配位聚合物 2 的金属中心分散良好。本研究为开发非贵金属配合物作为电催化改性电极材料提供了新思路。

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来源期刊

Inorganica Chimica Acta 化学-无机化学与核化学

CiteScore

6.00

自引率

3.60%

发文量

440

审稿时长

35 days

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.