Photocatalytic hydrogen production (PHP) from water is a promising solution for environmental pollution due to its high energy density and the abundant availability of water and solar energy on Earth. 1,1-dicyanomethylene-3-indanone (IC) has been widely used as an end group in organic photovoltaics owing to its strong electron-withdrawing ability and planarity. However, research on the application of IC structures in PHP is limited due to synthesis challenges. In this study, we designed a series of novel IC-based monomers incorporating a dibenzothiophene-S,S-dioxide unit through Suzuki coupling. These monomers were used to synthesize polymers with varying degrees of malononitrile substitution, referred to as ICFTDB, ICTDB, and IDMTDB. We investigated the correlation between the optical, electrochemical, and hydrogen evolution performances of these polymers. Through transient absorption spectroscopy, we demonstrated that ICTDB exhibited enhanced capabilities for ultrafast electron transfer and reduced recombination effects. As a result, ICTDB, photocatalysts with IC-containing structures achieved a hydrogen evolution rate of 30.0 mmol g-1 h-1, which was 11.5 times higher than that of ICFTDB, the polymer with no malononitrile substitution. This study provides valuable insights into the potential of IC-based conjugated polymers for photocatalytic hydrogen evolution.
Our study underscores that ICTDB, a polymer with one malononitrile substitution, outperforms in the HER and displays enhanced ultrafast charge transfer capabilities.
- Indanone-based conjugated polymers enabling ultrafast electron transfer for visible light-driven hydrogen evolution from water
- Tse-Fu Huang - Natl Tsing Hua Univ, Dept Chem Engn, Hsinchu 300044, TaiwanYing-Rang Zhuang - Natl Tsing Hua Univ, Dept Chem Engn, Hsinchu 300044, TaiwanChih-Li Chang - Natl Tsing Hua Univ, Dept Chem Engn, Hsinchu 300044, TaiwanChing-Li Huang - National Yang Ming Chiao Tung UniversityWei-Cheng Lin - Natl Tsing Hua Univ, Dept Chem Engn, Hsinchu 300044, TaiwanZi-Cheng Jiang - National Tsing Hua UniversityLi-Yu Ting - Natl Tsing Hua Univ, Dept Chem Engn, Hsinchu 300044, TaiwanIslam M. A. Mekhemer - National Tsing Hua UniversityYu-En Sun - National Tsing Hua UniversityPinit Kidkhunthod - Synchrotron Light Research InstituteJeng-Lung Chen - Natl Synchrotron Radiat Res Ctr, Hsinchu 30076, TaiwanYi-Chan Huang - National Tsing Hua UniversityHung-Kai Hsu - Natl Tsing Hua Univ, Inst Photon Technol, Hsinchu 300044, TaiwanYuan-Ting Tseng - Natl Tsing Hua Univ, Dept Chem Engn, Hsinchu 300044, TaiwanYi-Hsiang Wu - Natl Tsing Hua Univ, Dept Chem Engn, Hsinchu 300044, TaiwanBing-Heng Li - Natl Tsing Hua Univ, Dept Chem Engn, Hsinchu 300044, TaiwanShang-Da Yang - National Tsing Hua University, College of Semiconductor ResearchYen-Ju Cheng - National Yang Ming Chiao Tung UniversityHo-Hsiu Chou - National Tsing Hua University, College of Semiconductor Research
- Royal Society of Chemistry
- 11
- NSTC-112-2223-E-007-006-MY3; NSTC-112-2221-E-007-081; NSTC-112-2622-E-007-032; NSTC-112-2823-8-007-001 / National Science and Technology Council National Science and Technology Council, Taiwan Instrumentation Center at NTHU
- Journal article
- 06/02/2024
- Journal of materials chemistry. A, Materials for energy and sustainability, Vol.12(6), pp.3633-3643
- English