Nanospatial Charge Modulation of Monodispersed Polymeric Microsphere Photocatalysts for Exceptional Hydrogen Peroxide Production

Photocatalysis offers a sustainable strategy for hydrogen peroxide (H 2 O 2 ) production, which is an essential oxidant and emerging energy carrier in modern chemical industry. The development of polymer‐based photocatalysts to produce H 2 O 2 has great potential but is limited by lower efficiency due to the limitation of light utilization and the low charge separation efficiency. Herein, a series of monodispersed mesoporous resorcinol‐formaldehyde resin spheres (MRFS) are reported with a rational designed spatial charge distribution, exhibiting wide light absorption with a solar‐to‐chemical conversion (SCC) efficiency of 1.1%. Surface photovoltage microscopy (SPVM) measurements unraveled the charge separation in nanospace with uneven distribution of donor (D) and acceptor (A) sites. A density functional theory (DFT) calculation elucidated the origin of photogenerated electrons and holes. Moreover, MRFS demonstrates photocatalytic water oxidation ability. The findings in this work open a new avenue for the development of porous polymeric photocatalysts toward highly efficient solar energy conversion.