Rational Design of Molecular Catalysts for Efficient Electrocatalytic Hydrogenation

Motivated by the urgent need to address climate change and to transition from fossil fuel-based chemical production toward sustainable, renewable- driven processes, RIDE-ECH aims to generate enduring fundamental knowledge on the parameters governing electrocatalytic hydrogenation (ECH) of unsaturated organic substrates. Hydrogenation is a cornerstone transformation in the chemical industry, enabling the large-scale production of chemicals in the manufacturing of pharmaceuticals, polymers, agrochemicals, and fine chemicals, yet its reliance on fossil-derived H₂ and noble-metal catalysts underscores the urgent need for sustainable, decarbonized hydrogenation technologies powered by renewable electricity. RIDE-ECH will contribute to this objective by developing molecular electrocatalysts based on earth-abundant transition metals, functionalized to modulate second- coordination-sphere and electronic effects, with the aim of elucidating their structure-activity-selectivity relationships, revealing powerful electrocatalysts. Pushing beyond the state of the art, the project will also implement strategies to immobilize these catalysts, transferring their solution-phase activity to surfaces, which is essential for practical applications. Finally, the project will utilize a comprehensive spectroscopic toolkit to characterize key reaction intermediates using steady-state and operando spectroscopic techniques, providing fundamental mechanistic insights to optimize these systems for efficient electrochemical hydrogenation of organic substrates. To achieve this, RIDE-ECH employs a multidisciplinary approach and integrates a diverse group of researchers, including members from UAB and international collaborators, whose expertise is crucial to achieving the objectives of this project. Furthermore, the research plan is structured in a systematic and circular manner, allowing iterative feedback and redesign of the prepared complexes and materials. The research is organized across four work packages: 1) Synthesis and characterization of molecular catalysts; 2) Immobilization of catalysts and preparation of cathodes; 3) Evaluation of catalytic performance toward hydrogenation of organic substrates; 4) Mechanistic studies using ex situ and operando spectroscopy. RIDE-ECH represents a unique opportunity for the PI to establish an independent and pioneering research program at the forefront of the emerging field of sustainable chemistry based on rational molecular catalyst design. This project not only aims to advance the development of next-generation materials for a cleaner generation of chemicals but also provides an exceptional platform for the multidisciplinary training of early-career researchers in the expanding domain of sustainable chemistry. By addressing key scientific and technological challenges, RIDE-ECH will drive innovation at both Spanish and European levels while significantly enhancing the PIs profile and competitiveness within the global academic community.