Pyridine polymer tubular structures connected with polyoxometalates as bifunctional electrocatalysts for water splitting†

IF 3.3 3区化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR

Dalton Transactions Pub Date : 2024-12-31 DOI:10.1039/D4DT02612H

Jihua Wang, Hui Li, Lige Gong, Limin Dong, Yunhao Gu, Meijia Wang and BingHe Yang

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Abstract

In this work, we successfully prepared four POM-based organic–inorganic hybrids, namely, [(C₅H₆N)₂(C₄H₅N₂)][PMo₁₂O₄₀] (1), [(C₅H₆N)₃(C₅H₅N)][PMo₁₂O₄₀] (2), [(C₃H₆N₈)₃][PMo₁₂O₄₀]·4H₂O (3), and [(C₂H₅N₄)₃][PMo₁₂O₄₀] (4) (where C₅H₆N = pyridine, C₄H₅N₂ = pyrazine, C₃H₆N₈ = 2,7-diamino-1,3,4,6,8,9-hexaazaspiro[4.4] nonane, and C₂H₅N₄ = 3-amino-1,2,4-triazole), using a hydrothermal method. Compounds 1 and 2 exhibited a lamellar three-dimensional structure. Compared to compound 1, compound 2 contained only one ligand, pyridine, which formed a pyridine polymer tubular structure that was further connected to a [PMo₁₂O₄₀]³⁻ anion, creating a pyridine-PMo₁₂-pyridine stacking-like structure. Compounds 3 and 4 showed a stereostructure, where organic ligands were wrapped around polyacid spheres. Unlike compound 3, compound 4 maintained a similar three-dimensional structure but had a hexagonal astral ligand configuration. However, ligands formed hexagonal boxes that were smaller than those in compound 3, with shorter distances between the ligands. The overpotential values for compound 2 were 143 mV (HER) and 136 mV (OER) at 10 mA cm⁻², which were significantly lower than those of the other compounds, the H₃[PMo₁₂O₄₀] precursor, and the organic ligands. Given the relatively outstanding HER/OER catalytic properties of compound 2, a dual-electrode water-splitting device was assembled. The compound 2/CC∥compound 2/NF system achieved a low cell voltage of 1.48 V at 10 mA cm⁻², which was significantly lower than that of the commercial Pt/C/CC∥RuO₂/NF setup (1.5 V). In addition, compound 2/CC∥compound 2/NF exhibited rapid response capabilities and showed no significant increase in voltage after 6000 s of operation.

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吡啶聚合物管与多金属氧酸酯连接作为水裂解双功能电催化剂

在这项工作中，我们成功地用水热法制备了四个pom基有机无机杂化物，[(C5H6N) 2(C4H5N2)][PMo12O40](1),[(C5H6N)3(C5H5N)][PMo12O40](2),[(C3H6N8)3][PMo12O40] (4)（C5H6N=吡啶，C4H5N2=吡嗪，C3H6N8=2,7-二氨基-1,3,4,6,8,9- 6氮杂灵[4.4]壬烷，C2H5N4= 3-氨基-1,2,4-三唑）。化合物1和化合物2均呈片层状三维结构。与化合物1相比，化合物2只有一个配体吡啶，并且吡啶配体呈吡啶聚合物管状结构，与[PMo12O40]3-阴离子进一步连接，形成吡啶- pmo12 -吡啶堆叠状结构。化合物3和4均呈有机配体包裹聚酸球的立体结构。与化合物3相比，化合物4具有相似的三维结构，是一个六角形星光配体。然而，配体形成的六边形盒子比化合物3小，配体之间的距离也更小。在10 mA cm-2下，化合物2的过电位值为143 mV （HER）和136 mV (OER)，低于其他化合物、H3[PMo12O40]前体和有机配体。鉴于化合物2具有较为突出的HER/OER催化性能，我们组装了双电极水分解装置。在10 mA cm−2条件下，Compound2/CC∥Compound2/ NF可获得1.48 V的低电池电压，显著低于商用Pt/C/CC∥RuO2/NF (1.5 V)，且复方2/CC∥复方2/NF具有快速响应能力，且在6000s后无显著升高。

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来源期刊

Dalton Transactions 化学-无机化学与核化学

CiteScore

6.60

自引率

7.50%

发文量

1832

审稿时长

1.5 months

期刊介绍： Dalton Transactions is a journal for all areas of inorganic chemistry, which encompasses the organometallic, bioinorganic and materials chemistry of the elements, with applications including synthesis, catalysis, energy conversion/storage, electrical devices and medicine. Dalton Transactions welcomes high-quality, original submissions in all of these areas and more, where the advancement of knowledge in inorganic chemistry is significant.