On-Surface Decarboxylation Coupling Facilitated by Lock-to-Unlock Variation of Molecules upon the Reaction.

decarboxylation coupling high energy barrier intramolecular charge redistribution on-surface synthesis

Journal

Angewandte Chemie (International ed. in English)
ISSN: 1521-3773
Titre abrégé: Angew Chem Int Ed Engl
Pays: Germany
ID NLM: 0370543

Informations de publication

Date de publication:
02 Aug 2021
Historique:
received: 14 05 2021
pubmed: 4 6 2021
medline: 4 6 2021
entrez: 3 6 2021
Statut: ppublish

Résumé

On-surface synthesis (OSS) involving relatively high energy barriers remains challenging due to a typical dilemma: firm molecular anchor is required to prevent molecular desorption upon the reaction, whereas sufficient lateral mobility is crucial for subsequent coupling and assembly. By locking the molecular precursors on the substrate then unlocking them during the reaction, we present a strategy to address this challenge. High-yield synthesis based on well-defined decarboxylation, intermediate transition, and hexamerization is demonstrated, resulting in an extended and ordered network exclusively composed of the newly synthesized macrocyclic compound. Thanks to the steric hindrance of its maleimide group, we attain a preferential selection of the coupling. This work unlocks a promising path to enrich the reaction types and improve the coupling selectivity hence the structual homogeneity of the final product for OSS.

Identifiants

pubmed: 34080274
doi: 10.1002/anie.202106477
doi:

Types de publication

Journal Article

Langues

eng

Sous-ensembles de citation

IM

Pagination

17435-17439

Subventions

Organisme : National Natural Science Foundation of China
ID : 21473045
Organisme : National Natural Science Foundation of China
ID : 51772066

Informations de copyright

© 2021 Wiley-VCH GmbH.

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Auteurs

Shaoshan Wang (S)

School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, 150001, China.
Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China.

Zhuo Li (Z)

School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, 150001, China.
Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China.

Pengcheng Ding (P)

School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, 150001, China.

Cristina Mattioli (C)

CEMES-CNRS, 31055, Toulouse, France.

Wujun Huang (W)

Department of Chemistry, Xiamen University, Xiamen, 361005, China.

Yang Wang (Y)

School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, 150001, China.

André Gourdon (A)

CEMES-CNRS, 31055, Toulouse, France.

Ye Sun (Y)

Condensed Matter Science and Technology Institute, Harbin Institute of Technology, Harbin, 150001, China.

Mingshu Chen (M)

Department of Chemistry, Xiamen University, Xiamen, 361005, China.

Lev Kantorovich (L)

Department of Physics, King's College London, The Strand, London, WC2R 2LS, UK.

Xueming Yang (X)

Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China.

Federico Rosei (F)

INRS Centre for Energy, Materials and Telecommunications, Varennes Quebec, J3X 1S2, Canada.

Miao Yu (M)

School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, 150001, China.
Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China.

Classifications MeSH