A Synergistic Photocatalysis–Electrocatalysis System for Efficient Hydrogen Generation and Energy‐Saving Benzylamine Oxidative Upgrading
Shengchang Hong, Qianqian Zhang, Xiaolei Liu, Zeyan Wang, Yuanyuan Liu, Zhaoke Zheng, Hefeng Cheng, Baibiao Huang, Peng Wang
Abstract
Abstract Photocatalytic hydrogen iodide (HI) splitting represents a promising tactic for H 2 generation, but the light‐shielding effect induced by the generated I 3 − greatly impedes subsequent reactions. A critical challenge in this field lies in achieving the timely reduction of I 3 − while avoiding the use of additional sacrificial agents, such as H 3 PO 2 . Herein, we develop a synergistic photocatalysis–electrocatalysis system to address this challenge and achieve efficient H 2 generation and benzylamine oxidative upgrading. The photocatalytic component features a Re 0.5 Mo 0.5 S 2 cocatalyst‐modified MAPbI 3 with efficient charge separation and ample active sites, achieving a remarkable H 2 generation of 875.4 µmol within 4 h through HI splitting. The subsequent electrocatalytic module can operate at a low potential (only 0.44 V to reach 10 mA cm −2 ) to reduce the generated I 3 − and oxidize benzylamine to value‐added chemicals. After the electrolysis, the regenerated HI solution can be recycled for subsequent photocatalytic H 2 generation. The synergistic system establishes a sustainable catalytic cycle mediated by I − /I 3 − redox couples, enabling continuous photocatalytic H 2 generation from HI splitting and energy‐saving electrocatalytic benzylamine oxidative upgrading.