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A Synergistic Photocatalysis-Electrocatalysis System for Efficient Hydrogen Generation and Energy-Saving Benzylamine
Shengchang Hong1, Qianqian Zhang1, Xiaolei Liu2
1State Key Laboratory of Crystal Materials, Shandong University, Jinan, 250100, China.
Abstract:
Photocatalytic hydrogen iodide (HI) splitting represents a promising tactic for H2 generation, but the light-shielding effect induced by the generated I3 - greatly impedes subsequent reactions. A critical challenge in this field lies in achieving the timely reduction of I3 - while avoiding the use of additional sacrificial agents, such as H3PO2. Herein, we develop a synergistic photocatalysis-electrocatalysis system to address this challenge and achieve efficient H2 generation and benzylamine oxidative upgrading. The photocatalytic component features a Re0.5Mo0.5S2 cocatalyst-modified MAPbI3 with efficient charge separation and ample active sites, achieving a remarkable H2 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 I3 - and oxidize benzylamine to value-added chemicals. After the electrolysis, the regenerated HI solution can be recycled for subsequent photocatalytic H2 generation. The synergistic system establishes a sustainable catalytic cycle mediated by I-/I3 - redox couples, enabling continuous photocatalytic H2 generation from HI splitting and energy-saving electrocatalytic benzylamine oxidative upgrading.
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