Abstract

Water splitting to generate green H2 fuel and O2 is essential for global CO2 reductions toward net-zero emissions. In this process, however, O2 generation at the anode through the oxygen evolution reaction (OER) is inherently slower by orders of magnitude than H2 generation at the cathode. Thus, improving OER efficiency has been a major effort in electrolysis. Ni-based and Co-based layered hydroxides are among the most active and studied non-previous catalysts in alkaline electrolytes. Although tremendous advances have been made toward improving the activity and the stability of the catalysts over the past decade, there is still a lack of fundamental insights into active sites and reaction mechanisms, which has hindered the establishment of structure-property relationships.This talk will first provide fundamental insights into reaction centers and catalytic mechanisms of classic Ni oxyhydroxides and Co oxyhydroxides with and without ligand intercalation. We will further discuss the multiple-site synergy in Ni- and Co-based layered double hydroxides (LDH) and ternary hydroxides. We will show that the OER proceeds via a Mars van Krevelen mechanism, starting with the oxidation of bridge OH at the reaction centers with dual metal sites, i.e., M1-OH-M2. We will demonstrate that, to approach the minimum overpotential dictated by a specific OH-OOH scaling relationship, the key is to break the OH-O scaling relationship. A possible route is to form binary metal oxyhydroxides with dual metal sites at the reaction centers or introduce a third element into NiFe LDH or CoFe LDH. If time permits, We will further discuss the role of the non-covalent interaction and polaron-like electronic states in promoting OER at M1-OH-M2 centers.

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