From electronic descriptors to durable design: a multi-scale review of catalysts for LOHC dehydrogenation

Liquid organic hydrogen carriers offer a dense platform for hydrogen storage, yet their deployment is hindered by catalyst deactivation and energy demand. This review provides a mechanism-focused synthesis connecting atomic-scale electronic descriptors to catalyst formulation and reactor performance. We revisit Brønsted–Evans–Polanyi relationships, volcano trends, and electronic modulation as conditional tools for interpreting C-H activation. These principles rationalize alloying strategies: Pt-Sn illustrates activity–stability trade-offs; Pt-Pd tailors adsorption energetics; supported Pt-Ir illustrates preparation-dependent dispersion. We also examine metal–support interactions on oxides, mesoporous silicas, and carbon matrices that enable confinement and spillover. Integrating these insights, we outline a multi-scale design perspective linking electronic descriptors to surface kinetics, framing durability as a central criterion. The review concludes with opportunities in data-driven discovery, operando deactivation mapping, and process optimization, emphasizing green-chemistry priorities of efficiency, selectivity, reduced critical-metal use, and long-term stability.