Zhang Zhenzhen, Si Wenqin, Wu Baohua, Wang Wei, Li Yawen, Ma Wei, Lin Yuze
Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Organic Solids, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, China.
University of Chinese Academy of Sciences, Beijing, 100049, China.
Angew Chem Int Ed Engl. 2022 Mar 1;61(10):e202114234. doi: 10.1002/anie.202114234. Epub 2022 Jan 17.
Typical organic semiconductors show a high trap density of states (10 -10 cm ), 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 2.3×10 cm , 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 g under AM1.5G sunlight (100 mW cm ), and 72.75 mmol h g under 330-1100 nm illumination (198 mW cm ) higher than that of the control NPs based on typical PM6 : Y6 (62.67 mmol h g ).
典型的有机半导体具有较高的陷阱态密度(10-10 cm),为电荷载流子复合提供了大量中心,从而阻碍了光催化析氢的发展。在此,我们设计并合成了一种二维多环光伏材料,命名为TPP,将陷阱密度降低至低至2.3×10 cm,比典型有机半导体低1-3个数量级。此外,TPP表现出宽泛且强烈的吸收、具有大晶体相干长度的有序分子堆积以及增强的电子迁移率。然后,基于聚合物给体(PM6)和TPP混合物的本体异质结纳米颗粒(BHJ-NPs)在AM1.5G太阳光(100 mW cm)下的平均析氢速率(HER)为64.31 mmol h g,在330-1100 nm光照(198 mW cm)下为72.75 mmol h g,高于基于典型PM6 : Y6(62.67 mmol h g)的对照纳米颗粒。