N‐Heterocyclic Carbene Functionalization of 2D Transition Metal Dichalcogenides via a Frustrated Lewis Pair Strategy

Gao, Jia; Li, Nachuan; Dai, Bona; Zhou, Xiaojie; Chen, Chaohuang; Fujisawa, Kazunori; Yang, Zhenzhen; Dai, Sheng; Sun, Yifan

doi:10.1002/adfm.202502325

N‐Heterocyclic Carbene Functionalization of 2D Transition Metal Dichalcogenides via a Frustrated Lewis Pair Strategy

Journal Article · Thu May 22 00:00:00 EDT 2025 · Advanced Functional Materials

DOI:https://doi.org/10.1002/adfm.202502325· OSTI ID:2573123

Gao, Jia ^[1]; Li, Nachuan ^[1]; Dai, Bona ^[1]; Zhou, Xiaojie ^[2]; Chen, Chaohuang ^[1]; Fujisawa, Kazunori ^[3]; ^[4]; ^[5]; ^[1]

Shanghai Jiao Tong Univ. (China)
Chinese Academy of Sciences (CAS), Shanghai (China)
Shinshu Univ., Matsumoto, Nagano (Japan)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

Molecular functionalization of 2D transition metal dichalcogenides (TMDs), which unites tailorability of organic molecules and robustness of inorganic solids, is important for tuning their surface properties. While it is common to leverage the electronic effect of organic ligands to functionalize TMDs, the corresponding steric hinderance has remained elusive and underexplored. Herein N‐heterocyclic carbene (NHC) functionalization of WS₂ is demonstrated via a frustrated Lewis pair (FLP) route, which exploits both the electronic and steric effect for TMD functionalization. The Lewis base, 1,3‐bis(2,4,6‐trimethylphenyl)imidazol‐2‐ylidene (IMes), is anchored to the sulfur vacancy sites (Lewis acid) of the WS₂ nanostructures with the hybrid‐interface‐mediated steric hinderance, mimicking the FLP chemistry and enabling dihydrogen cleavage at room temperature and atmospheric pressure. Solid‐state nuclear magnetic resonance (ssNMR) results reveal the local chemical environment of the activated hydrogen species, which can be transferred for room‐temperature hydrogenation reactions. Finally, the insights are useful for designing weak, non‐covalent bonds to modify the 2D surface of TMDs for a broad scope of applications.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2573123

Journal Information:: Advanced Functional Materials, Journal Name: Advanced Functional Materials Vol. 2025; ISSN 1616-301X; ISSN 1616-3028

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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