Atomically engineered triphase nanoreactors for selective hydrogen peroxide photogeneration
Xiaoying Peng, Zongxing Tu, Ke Wang, Bin Lei, Suqin Wu, Jing Wang, Shou‐Ri Sheng, Gangbin Yan, Guiming Peng
Abstract
Overcoming oxygen (O 2 ) mass transport and active site limitations is key to advancing photocatalytic hydrogen peroxide (H 2 O 2 ) production via the two-electron O 2 reduction reaction (2e − ORR). Here, we design liquid/solid/gas triphase nanoreactors based on Pt single-atom-decorated carbon nitride nanotubes (Pt/CNNT), which synergistically integrate confined O 2 storage, efficient mass transfer, and highly active atomic sites. The hollow nanotube architecture facilitates continuous O 2 delivery, while atomically dispersed Pt sites modulate the electronic structure to enhance O 2 adsorption and *OOH intermediate formation. As a result, the Pt/CNNT nanoreactors exhibit a seven-fold increase in H 2 O 2 yield compared to the bulk CN diphase system, reaching 232 μmol g −1 h −1 with apparent quantum yields of 5.1 % and 4.2 % at 400 and 420 nm, respectively. DFT calculations and electrochemical studies confirm the enhanced 2e − ORR selectivity via a sequential two-step 1e − pathway. This work highlights the power of nanoreactor engineering combined with atomic-level catalytic tuning for efficient and selective photocatalytic H 2 O 2 synthesis.