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Electrocatalyst for hydrogen evolution and H2O2 recognition on composite carbon paste electrodes with three new Ag(I) MOFs
•Three new Ag(Ⅰ) MOFs were synthesized and characterized.•Electrodes composited by Ag(Ⅰ) MOFs show effective HER activity.•The highest HER activity of Ag-MOF-2@CPE may be attributed to coordinated water.•Three Ag-MOF-1∼3@CPE have good H2O2-sensing and exhibit good anti-interference. Three new Ag(I)...
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Published in: | Journal of molecular structure 2024-09, Vol.1311, p.138448, Article 138448 |
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Main Authors: | , , , , , |
Format: | Article |
Language: | English |
Subjects: | |
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Online Access: | Get full text |
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Summary: | •Three new Ag(Ⅰ) MOFs were synthesized and characterized.•Electrodes composited by Ag(Ⅰ) MOFs show effective HER activity.•The highest HER activity of Ag-MOF-2@CPE may be attributed to coordinated water.•Three Ag-MOF-1∼3@CPE have good H2O2-sensing and exhibit good anti-interference.
Three new Ag(I) metal-organic frameworks (Ag-MOFs) containing bisbenzimidazole-derived ligand, namely, {[Ag2(L)(TP)](H2O)}n (1), {[Ag2(L)(HBTC))(H2O)](CH3CH2OH)(H2O)}n (2) and {[Ag4(L)2(IP)2](CH3CN)3(H2O)16}n (3) (L = bis(1-(pyridin-4-ylmethyl)-benzimidazol-2-yl methyl) ether, TP = Terephthalate, BTC = Benzenetricarboxylate, IP = Isophthalate), have been synthesized by volatilization method and systematic adjustment of solvent and aromatic polyacid co-ligand. Single crystal structural analysis showed that although three Ag-MOFs have a three-dimensional (3D) network backbone structure, their topological structures are different. Electrocatalytic hydrogen evolution reaction (HER) of carbon paste composite electrodes (Ag-MOF-1∼3@CPE) prepared by mixing graphite powder with Ag-MOFs were investigated in 0.5 M H2SO4 electrolyte. The HER measurements show that the overpotential η10293K of Ag-MOF-1∼3@CPE are -634, -533 and -615 mV compared with sCPCE (blank electrode, -966 mV), and the Tafel slope of sCPCE and Ag-MOF-1∼3@CPE were 276, 251, 123 and 220 mV dec−1, respectively. The results prove that Ag-MOF-1∼3@CPE could effectively catalyze and accelerate the HER behavior, with electrocatalytic activity order being Ag-MOF-2@CPE > Ag-MOF-3@CPE > Ag-MOF-1@CPE > sCPE. The highest HER activity of Ag-MOF-2@CPE can be attributed to the fact that Ag-MOF-2 contains coordination water molecule, while the higher activity of Ag-MOF-3@CPE than Ag-MOF-1@CPE is due to steric hindrance. Furthermore, the recognition performance of Ag-MOF-1∼3@CPE for H2O2 was further studied by chronoamperometry in 0.2 M phosphate buffer solution (PBS, pH = 6). The three sensors can detect H2O2 in a linear range from 0.5 μM to 4 mM with sensitivities of 103, 34.5 and 138 μA·mM−1·cm−2, and also revealed long-term stability and good selectivity. Our study provides a new approach for designing efficient, non-precious metal electrochemical catalysts.
Three new Ag(Ⅰ) MOFs have been synthesized by systematically tuning the solvent and aromatic polyacid co-ligand. Crystallographic analysis revealed that the three Ag(I)-MOFs exhibit different topological channel structures. The Ag-MOF-1∼3@CPE have more positive overpotentials (η |
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ISSN: | 0022-2860 1872-8014 |
DOI: | 10.1016/j.molstruc.2024.138448 |