Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 61, Issue 10, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202114234
Keywords
Bulk Heterojunction Nanoparticle; Photocatalytic Hydrogen Evolution; Solar Hydrogen; Trap Density; Two-Dimensional Polycyclic Material
Categories
Funding
- National Natural Science Foundation of China [52173189, 21704082, 21875182]
- Key Scientific and Technological Innovation Team Project of Shaanxi Province [2020TD-002]
- China Postdoctoral Science Foundation [2017M623162]
- 111 project 2.0 [BP2018008]
- Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231]
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The study successfully designed and synthesized a two-dimensional polycyclic photovoltaic material named TPP, which exhibits a low trap density and excellent light absorption, leading to improved photocatalytic hydrogen evolution rate.
Typical organic semiconductors show a high trap density of states (10(16)-10(18) cm(-3)), providing a large number of centers for charge-carrier recombination, thus hindering the development of photocatalytic hydrogen evolution. Here, we design and synthesize a two-dimensional polycyclic photovoltaic material, named as TPP, to reduce the trap density to as low as 2.3x10(15) cm(-3), which is 1-3 orders of magnitude lower than those of typical organic semiconductors. Moreover, TPP exhibits a broad and strong absorption, ordered molecular packing with a large crystalline coherence length and enhanced electron mobility. Then, the bulk heterojunction nanoparticles (BHJ-NPs) based on a blend of polymer donor (PM6) and TPP exhibit an average hydrogen evolution rate (HER) of 64.31 mmol h(-1) g(-1) under AM1.5G sunlight (100 mW cm(-2)), and 72.75 mmol h(-1) g(-1) under 330-1100 nm illumination (198 mW cm(-2)) higher than that of the control NPs based on typical PM6 : Y6 (62.67 mmol h(-1) g(-1)).
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