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Dual-Type Polarization-Triggered Spontaneous Exciton Dissociation in Conjugated Polymers for Enhanced Photocatalytic
Peiyan Chen1, Chongliang Li1, Haobin Huang1
1School of Advanced Energy, IGCME, Shenzhen Campus of Sun Yat-sen University, Shenzhen, 518107, China.
None:
Severe exciton effect significantly hinders free-charge-involved water redox reactions, limiting the improvement of photocatalytic performance. Herein, a dual polarization strategy was proposed to achieve spontaneous exciton dissociation while lowering exciton binding energy by introducing B←N bonds and triazine as the dual-type polarization unit into the alkynyl-linked conjugated backbone. Dual-type polarization centers can induce spontaneous exciton dissociation (exciton activation energy <25 meV) to generate more free charges that participate in water oxidation reactions. Triazine as the second polarization unit, lowers the energy barrier of the H2O oxidation reaction and serves as the active site of the O2 reduction reaction to accelerate H2O2-evolution. The H2O2-evolution performance of the dual-polarization photocatalyst reaches up to 4261 µmol g-1 h-1 with a superb apparent quantum yield of 25.84% at 420 nm and solar-to-chemical energy conversion up to 1.20% in pure water, surpassing most of the H2O2-evolution organic photocatalysts ever reported. Furthermore, the dual-polarization photocatalyst exhibits strong universality in complex water bodies (lake water, river water, and seawater), while achieving higher H2O2-evolution performance than that in pure water.
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