材料科学
光催化
分解水
半导体
带隙
聚合物
聚合
量子效率
光诱导电荷分离
光化学
化学工程
光电子学
纳米技术
人工光合作用
催化作用
有机化学
复合材料
化学
工程类
作者
Yiou Wang,Fabrizio Silveri,Mustafa K. Bayazit,Qiushi Ruan,Yaomin Li,Jijia Xie,C. Richard A. Catlow,Junwang Tang
标识
DOI:10.1002/aenm.201801084
摘要
Abstract The bandgap engineering of semiconductors, in particular low‐cost organic/polymeric photocatalysts could directly influence their behavior in visible photon harvesting. However, an effective and rational pathway to stepwise change of the bandgap of an organic/polymeric photocatalyst is still very challenging. An efficient strategy is demonstrated to tailor the bandgap from 2.7 eV to 1.9 eV of organic photocatalysts by carefully manipulating the linker/terminal atoms in the chains via innovatively designed polymerization. These polymers work in a stable and efficient manner for both H 2 and O 2 evolution at ambient conditions (420 nm < λ < 710 nm), exhibiting up to 18 times higher hydrogen evolution rate (HER) than a reference photocatalyst g‐C 3 N 4 and leading to high apparent quantum yields (AQYs) of 8.6%/2.5% at 420/500 nm, respectively. For the oxygen evolution rate (OER), the optimal polymer shows 19 times higher activity compared to g‐C 3 N 4 with excellent AQYs of 4.3%/1.0% at 420/500 nm. Both theoretical modeling and spectroscopic results indicate that such remarkable enhancement is due to the increased light harvesting and improved charge separation. This strategy thus paves a novel avenue to fabricate highly efficient organic/polymeric photocatalysts with precisely tunable operation windows and enhanced charge separation.
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