Hydrogen evolution via hydride transfer by a small organic benzothiadiazole-caffeine electrocatalyst
Year: 2025
Type: article
Abstract: Access to multiple redox states in electrocatalysts is vital to enhance the activity and stability of molecular catalysts toward the production of fuels. In this work, we have developed a catalyst based on two caffeine units covalently linked to a benzothiadiazole core. This catalyst can store three electrons in a fully reversible manner. Under reductive conditions and in the presence of strong acids, this molecule forms an organic hydride donor that is electroactive toward H 2 evolution at mild potentials in DMSO. Faradaic efficiency up to 92% and a turnover number up to 23 were achieved after 4 h of controlled potential electrolysis with no decomposition of the catalyst. A reaction mechanism involving a hydride transfer step is proposed based on the chemical species found under electrocatalytic conditions and density functional theory (DFT) calculations. The development of this small organic molecule is a step forward in the quest to low-cost, active, and long-term stable electrocatalysts for H 2 evolution.
Source: Chem Catalysis
Institution: Uppsala University
Language: English
Field: Energy
Domain: Physical Sciences
Open Access status: hybrid
Estimated APC paid: $9,170
OpenAlex ID: W4416996410