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

In this work, we successfully prepared four POM-based organic-inorganic hybrids, namely, [(C<sub>5</sub>H<sub>6</sub>N)<sub>2</sub>(C<sub>4</sub>H<sub>5</sub>N<sub>2</sub>)][PMo<sub>12</sub>O<sub>40</sub>] (1), [(C<sub>5</sub>H<sub>6</sub>N)<sub>3</sub>(C<sub>5</sub>H<sub>5</sub>N)][PMo<sub>12</sub>O<sub>40</sub>] (2), [(C<sub>3</sub>H<sub>6</sub>N<sub>8</sub>)<sub>3</sub>][PMo<sub>12</sub>O<sub>40</sub>]·4H<sub>2</sub>O (3), and [(C<sub>2</sub>H<sub>5</sub>N<sub>4</sub>)<sub>3</sub>][PMo<sub>12</sub>O<sub>40</sub>] (4) (where C<sub>5</sub>H<sub>6</sub>N = pyridine, C<sub>4</sub>H<sub>5</sub>N<sub>2</sub> = pyrazine, C<sub>3</sub>H<sub>6</sub>N<sub>8</sub> = 2,7-diamino-1,3,4,6,8,9-hexaazaspiro[4.4] nonane, and C<sub>2</sub>H<sub>5</sub>N<sub>4</sub> = 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 [PMo<sub>12</sub>O<sub>40</sub>]<sup>3-</sup> anion, creating a pyridine-PMo<sub>12</sub>-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<sup>-2</sup>, which were significantly lower than those of the other compounds, the H<sub>3</sub>[PMo<sub>12</sub>O<sub>40</sub>] 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<sup>-2</sup>, which was significantly lower than that of the commercial Pt/C/CC∥RuO<sub>2</sub>/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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Publication Details

Journal
Dalton Transactions
Published
2024-12-31
DOI
https://doi.org/10.1039/d4dt02612h
Citations
3
Primary Topic
Polyoxometalates: Synthesis and Applications
Type
article
Field-Weighted Citation Impact
0.35
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article

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

Bing Yang, M. Wang, Lige Gong, Limin Dong et al.
3 citations
Dalton Transactions
Polyoxometalates: Synthesis and Applications
0.35
article

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

Bing Yang, M. Wang, Lige Gong, Limin Dong, Yingying Gu, Jihua Wang, Hui Li
article en
3 citations

Abstract

In this work, we successfully prepared four POM-based organic-inorganic hybrids, namely, [(C<sub>5</sub>H<sub>6</sub>N)<sub>2</sub>(C<sub>4</sub>H<sub>5</sub>N<sub>2</sub>)][PMo<sub>12</sub>O<sub>40</sub>] (1), [(C<sub>5</sub>H<sub>6</sub>N)<sub>3</sub>(C<sub>5</sub>H<sub>5</sub>N)][PMo<sub>12</sub>O<sub>40</sub>] (2), [(C<sub>3</sub>H<sub>6</sub>N<sub>8</sub>)<sub>3</sub>][PMo<sub>12</sub>O<sub>40</sub>]·4H<sub>2</sub>O (3), and [(C<sub>2</sub>H<sub>5</sub>N<sub>4</sub>)<sub>3</sub>][PMo<sub>12</sub>O<sub>40</sub>] (4) (where C<sub>5</sub>H<sub>6</sub>N = pyridine, C<sub>4</sub>H<sub>5</sub>N<sub>2</sub> = pyrazine, C<sub>3</sub>H<sub>6</sub>N<sub>8</sub> = 2,7-diamino-1,3,4,6,8,9-hexaazaspiro[4.4] nonane, and C<sub>2</sub>H<sub>5</sub>N<sub>4</sub> = 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 [PMo<sub>12</sub>O<sub>40</sub>]<sup>3-</sup> anion, creating a pyridine-PMo<sub>12</sub>-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<sup>-2</sup>, which were significantly lower than those of the other compounds, the H<sub>3</sub>[PMo<sub>12</sub>O<sub>40</sub>] 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<sup>-2</sup>, which was significantly lower than that of the commercial Pt/C/CC∥RuO<sub>2</sub>/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.

Dalton TransactionsVol. 54(8)
Harbin University of Science and Technology (CN)
Clean water and sanitation
Openalex Percentile: Top 42%
Polyoxometalates: Synthesis and Applications
0.35
DOISourceOpenAlex
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