A Push–Pull Type Electron-Selective Self-Assembled Monolayer in Organic Semiconductor Photoanodes for Solar Water Oxidation
Effective charge extraction in organic semiconductor (OS)-based photoelectrochemical (organic PEC) cells is essential for achieving high-performance while mitigating detrimental charge accumulation. Here, we present a series of 1,8-naphthalimide-derived dipolar molecules as standalone electron-selective self-assembled monolayers (SAMs) in organic PEC cells. The dipole moments of these SAM molecules are significantly adjusted to over 5 D via a push–pull molecular design strategy, enabling effective modulation of the work function of the substrates to facilitate selective electron extraction. Furthermore, we demonstrate that modifying the pendant groups on these SAMs tunes the interfacial dipole, thereby governing electron extraction dynamics. Consequently, organic photoanodes based on a thiophene-substituted SAM (NI-T) achieve efficient solar water oxidation with a photocurrent density up to 7.97 mA cm–2 at 1.23 V vs reversible hydrogen electrode (RHE). Our findings highlight the importance of the push–pull design and interfacial dipole orientation in optimizing charge extraction in organic PEC cells.
Authors
- Inkyoung Cho (ORCID: https://orcid.org/0009-0003-8683-2640)
- Gyu Ho Chae
- Ji‐Youn Seo (ORCID: https://orcid.org/0000-0002-0473-1279)
- Shishou Kang (ORCID: https://orcid.org/0000-0003-4385-0331)
- Jun‐Ho Yum (ORCID: https://orcid.org/0000-0001-8386-2922)
- Euimin Lee (ORCID: https://orcid.org/0009-0004-8913-8539)
- Han‐Hee Cho (ORCID: https://orcid.org/0000-0003-2491-4619)
- Hyuna Kim
- Gyeong-Ho Jeong
- Kevin Sivula (ORCID: https://orcid.org/0000-0002-8458-0270)
- Jong‐Woon Ha (ORCID: https://orcid.org/0000-0003-3753-7947)
- Hoon Kim (ORCID: https://orcid.org/0009-0009-6752-2122)
- Dong-Hyun Lee (ORCID: https://orcid.org/0000-0001-7797-0011)
- Eunsong Jeon
- Jeongyeon Kim (ORCID: https://orcid.org/0000-0002-7106-2773)
- Jin Su Park (ORCID: https://orcid.org/0000-0002-2040-5510)
- Gil-Bok Choi
- Geundoo Jang
Institutions
- ON Semiconductor (United States) (US)
- Gyeongsang National University (KR)
- Nanomaterials Research (United States) (US)
- SiEnergy Systems (United States) (US)
- Korea Research Institute of Chemical Technology (KR)
- Nano Carbon (Poland) (PL)
- Ulsan National Institute of Science and Technology (KR)
- Pusan National University (KR)
- École Polytechnique Fédérale de Lausanne (CH)
Publication Details
- Journal
- ACS Energy Letters
- Published
- 2025-11-11
- DOI
- https://doi.org/10.1021/acsenergylett.5c02848
- Citations
- 1
- Primary Topic
- TiO2 Photocatalysis and Solar Cells
- Type
- article
- Field-Weighted Citation Impact
- 0.36