The importance of hydrogen peroxide (H 2 O 2 ) continues to grow globally. Deriving the oxygen reduction reaction (ORR) toward the 2epathway to form H 2 O 2 is crucial for high H 2 O 2 productivity. However, most selective electrocatalysts following the 2epathway comprise carbon-containing organic materials with intrinsically low stability, thereby limiting their commercial applicability. Herein, layered double hydroxides (LDHs) are used as inorganic matrices for the first time. The LDH catalyst developed herein exhibits near-100% 2e -ORR selectivity and stably produces H 2 O 2 with a concentration of ≈108.2 mm cm -2 photoanode in 24 h in a two-compartment system (with a photoanode) with a solar-to-chemical conversion efficiency of ≈3.24%, the highest among all reported systems. Density functional theory calculations show that 2e -ORR selectivity is promoted by atomically dispersed cobalt atoms in (012) planes of the LDH catalyst, while a free energy gap between the * O and OOHstates is an important factor.

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Catalyst-support interaction triggering biased electron flows between catalyst and reactant has been studied for electrocatalysis. The interaction was limited to the interfacial region between catalyst and support when nanoparticular catalysts,...

Solar Hydrogen Peroxide Production In article number 2110412, Hu Young Jeong, Changduk Yang, Jun Hee Lee, Ji‐Wook Jang, Seungho Cho, and co‐workers report a highly two‐electron oxygen‐reduction pathway‐selective layered double hydroxide catalyst for hydrogen peroxide production. A bias‐free two‐compartment photoelectrochemi cal system with the catalyst can generate hydrogen peroxide with a solar‐to‐hydrogen peroxide conversion efficiency of 3.24%.