Dual‐Pronged Strategy for Practical H 2 O 2 Electrosynthesis: Cross‐Scale Engineering of Nanocarbon Catalysts

ABSTRACT Both the atomic‐/molecular‐scale active sites and the mesoscopic mass transfer properties jointly govern the overall performance of catalytic materials. In this work, we propose a dual‐pronged strategy that integrates heteroatom doping with micro/nano‐scale structural design, thereby optimizing surface carbonaceous active sites and mesoscale mass transport, ultimately enabling the development of a mesoporous carbon‐based catalyst for practical electrochemical H 2 O 2 synthesis. Impressively, the optimized nanocatalyst exhibits high electrocatalytic activity and selectivity (> 95% at pH 13 and > 90% at pH 7) toward H 2 O 2 , facilitating the production of H 2 O 2 solution at industrial‐related current densities in flow‐cell systems and making it suitable for applications such as pulp bleaching and medical‐grade disinfection. Mechanistically, we propose that sulfur heteroatoms modulate the binding energy of *OOH intermediates on the carbonaceous surface, thereby enhancing H 2 O 2 formation; besides, the mesoscopic geometric structure with a hollow interior and mesoporous channels ensures sufficient O 2 supply and a hydrated environment, supporting mass transfer‐enhanced H 2 O 2 generation. The dual‐pronged strategy presented here offers a new framework for designing catalytic platforms aimed at cross‐scale process intensification in the electrocatalytic small molecule conversion.