Heteroatom Dopants Promote Two‐Electron O 2 Reduction for Photocatalytic Production of H 2 O 2 on Polymeric Carbon Nitride

Abstract Polymeric carbon nitride modified with selected heteroatom dopants was prepared and used as a model photocatalyst to identify and understand the key mechanisms required for efficient photoproduction of H 2 O 2 via selective oxygen reduction reaction (ORR). The photochemical production of H 2 O 2 was achieved at a millimolar level per hour under visible‐light irradiation along with 100 % apparent quantum yield (in 360–450 nm region) and 96 % selectivity in an electrochemical system (0.1 V vs. RHE). Spectroscopic analysis in spatiotemporal resolution and theoretical calculations revealed that the synergistic association of alkali and sulfur dopants in the polymeric matrix promoted the interlayer charge…