Issue 4, 2024

Ruthenium nanoparticles on covalent triazine frameworks incorporating thiophene for the electrocatalytic hydrogen evolution reaction

Abstract

In this study, 2 to 4 nm ruthenium nanoparticles (Ru-NPs) were loaded (21 to 33 wt%) by decomposition of triruthenium dodecacarbonyl, Ru3(CO)12, through microwave heating on the prototypal CTF-1 and on thiophene-containing CTFs to access the influence of the thiophene content on the electrocatalytic properties in the hydrogen evolution reaction (HER). The CTFs were synthesized ionothermally with heating at 400 °C and 600 °C (CTF_400/600) using thiophene- (Th-CTF), phenylthiophene- (PhTh-CTF), bithiophene- (BTh-CTF) or quaterthiophene- (QTh-CTF) dinitrile precursors. The homogenous nature of the Ru/CTF composite materials was confirmed by transmission electron microscopy (TEM) and scanning electron microscopy (SEM) combined with energy-dispersive X-ray spectroscopy (EDX). X-ray photoelectron spectroscopy (XPS) revealed the successful introduction of thiophene units and the deposition of Ru-NPs. The Ru/CTF composite materials retained their porosity with calculated Brunauer–Emmett–Teller (BET) surface areas being between 540 to 1326 m2 g−1. Low overpotentials and Tafel slopes towards HER down to 30 mV at 10 mA cm−2 and 55 mV dec−1 were recorded in 0.5 mol L−1 H2SO4 with the lowest (i.e. best) value observed for Ru/BTh-CTF_600. Notably, Ru/CTF composite materials based on CTFs synthesized at 600 °C are generally superior compared to the ones at 400 °C by exhibiting lower overpotentials due to more pronounced carbonization during synthesis. In 1 mol L−1 KOH the Ru/CTFs demonstrate even lower overpotentials down to 3 mV with Ru/PhTh-CTF_600 and Ru/QTh-CTF_600 as the two best materials. Tafel slopes down to 39 mV dec−1 indicate fast kinetics. Durability tests of Ru/BTh-CTF_600, Ru/PhTh-CTF_600 and Ru/QTh-CTF_600 with 2000 voltammetry cycles show minor to no alterations in the electrocatalytic performances.

Graphical abstract: Ruthenium nanoparticles on covalent triazine frameworks incorporating thiophene for the electrocatalytic hydrogen evolution reaction

Supplementary files

Article information

Article type
Paper
Submitted
14 Sep 2023
Accepted
15 Dec 2023
First published
15 Dec 2023
This article is Open Access
Creative Commons BY-NC license

J. Mater. Chem. A, 2024,12, 2093-2109

Ruthenium nanoparticles on covalent triazine frameworks incorporating thiophene for the electrocatalytic hydrogen evolution reaction

L. Rademacher, T. H. Y. Beglau, B. Ali, L. Sondermann, T. Strothmann, I. Boldog, J. Barthel and C. Janiak, J. Mater. Chem. A, 2024, 12, 2093 DOI: 10.1039/D3TA05597C

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