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Abstract Designing effective electrocatalysts tailored for targeted reactions requires fundamental insights into the structure dependence of the reaction microenvironment. Herein, inspired by finite element simulations, N,O co‐doped carbon nanosheets featuring a hierarchical micro/mesoporous structure to form an oxygen‐rich and local alkaline‐like microenvironment for the two‐electron oxygen reduction reaction (2e − ORR) in a neutral medium are designed. The in situ and ex situ test results confirmed that the micro/mesoporous carbon architecture can elevate the local pH and accelerate the generation of intermediates (*O 2 , *OOH), leading to high‐efficiency H 2 O 2 production. Utilizing this favorable microenvironment, N,O‐CNS 0.5 demonstrated exceptional H 2 O 2 electrosynthesis performance in neutral media, achieving a superior H 2 O 2 yield rate (6705 mmol g catalyst −1 h −1 in a flow cell). Additionally, comparative experiments and density‐functional theory calculations provided confirmation of the bi‐doping of N and O as the active origin responsible for the electrochemical 2e − ORR. This study synergistically manipulates the reaction microenvironment and active sites, providing an opportunity for efficient H 2 O 2 electro‐production in a neutral medium.
Jing et al. (Wed,) studied this question.