Electron Release via Internal Polarization Fields for Optimal S‐H Bonding States
Transition metal dichalcogenides (TMDs) have received considerable attention as promising electrocatalysts for the hydrogen evolution reaction (HER), yet their potential is often constrained by the inertness of the basal planes arising from their poor hydrogen adsorption ability. Here, the relationship between the electronic structure of the WS<sub>2</sub> basal plane and HER activity is systemically analyzed to establish a clear insight. The valance state of the sulfur atoms on the basal plane has been tuned to enhance hydrogen adsorption through sequential engineering processes, including direct phase transition and heterostructure that induces work function-difference-induced unidirectional electron transfer. Additionally, an innovative synthetic approach, harnessing the built-in internal polarization field at the W-graphene heterointerface, triggers the in-situ formation of sulfur vacancies in the bottom WS<sub>x</sub> (x < 2) layers. The resultant modulation of the valance state of the sulfur atom stabilizes the W-S bond, while destabilizing the S-H bond. The electronic structural changes are further amplified by the release and transfer of surplus electrons via sulfur vacancies, filling the valance state of W and S atoms. Consequently, this work provides a comprehensive understanding of the interplay between the electronic structure of the WS<sub>2</sub> basal plane and the HER activity, focusing on optimizing S-H bonding state.
Authors
- Jihun Mun (ORCID: https://orcid.org/0000-0002-1070-2095)
- Pil J. Yoo (ORCID: https://orcid.org/0000-0002-5499-6566)
- Vinit Kanade (ORCID: https://orcid.org/0000-0002-3603-7003)
- Hyeong‐U Kim (ORCID: https://orcid.org/0000-0002-0018-9603)
- Muyoung Kim (ORCID: https://orcid.org/0000-0002-1102-8194)
- Jin Kon Kim (ORCID: https://orcid.org/0000-0002-3872-2004)
- Hyunho Seok (ORCID: https://orcid.org/0000-0002-3189-5930)
- Ji Won Suk (ORCID: https://orcid.org/0000-0002-3953-6617)
- Seong Soo Yoo (ORCID: https://orcid.org/0000-0002-2704-1537)
- Keon‐Woo Kim (ORCID: https://orcid.org/0000-0001-5741-8895)
- Sihoon Son (ORCID: https://orcid.org/0009-0002-9052-335X)
- Myeong Gyun Nam
- Kübra Aydın (ORCID: https://orcid.org/0009-0001-9894-1639)
- Yonas Tsegaye Megra (ORCID: https://orcid.org/0000-0002-0386-8193)
- Jinill Cho
- Minjun Kim
- Hyeonjeong Lee (ORCID: https://orcid.org/0000-0003-2028-3557)
- Taesung Kim (ORCID: https://orcid.org/0000-0001-6280-7668)
- Jin-Hyoung Lee (ORCID: https://orcid.org/0009-0003-0679-629X)
Institutions
- Pohang University of Science and Technology (KR)
- Korea Research Institute of Standards and Science (KR)
- Korea Institute of Machinery & Materials (KR)
- Sungkyunkwan University (KR)
- Korea University of Science and Technology (KR)
Publication Details
- Journal
- Advanced Materials
- Published
- 2024-09-09
- DOI
- https://doi.org/10.1002/adma.202411211
- Citations
- 8
- Primary Topic
- Electrocatalysts for Energy Conversion
- Type
- article
- Field-Weighted Citation Impact
- 0.82
Funders
- National Research Foundation
- Ministry of Education
- Ministry of Trade, Industry and Energy
- Korea Institute of Machinery and Materials
- Ministry of Science and ICT, South Korea