A Two-Dimensional Polyimide-Graphene Heterostructure with Ultra-fast Interlayer Charge Transfer

Kejun Liu; Jiang Li; Haoyuan Qi; Mike Hambsch; Jonathan Rawle; Adrián Romaní Vázquez; Ali Shaygan Nia; Alexej Pashkin; Harald Schneider; Mirosllav Polozij; Thomas Heine; Manfred Helm; Stefan C.B. Mannsfeld; Ute Kaiser; Renhao Dong; Xinliang Feng

doi:10.1002/anie.202102984

A Two-Dimensional Polyimide-Graphene Heterostructure with Ultra-fast Interlayer Charge Transfer

Kejun Liu, Jiang Li, Haoyuan Qi, Mike Hambsch, Jonathan Rawle, Adrián Romaní Vázquez, Ali Shaygan Nia, Alexej Pashkin, Harald Schneider, Mirosllav Polozij, Thomas Heine, Manfred Helm, Stefan C.B. Mannsfeld, Ute Kaiser, Renhao Dong, Xinliang Feng

Department of Chemistry

Research output: Contribution to journal › Article › peer-review

8 Citations (Scopus)

Abstract

Two-dimensional polymers (2DPs) are a class of atomically/molecularly thin crystalline organic 2D materials. They are intriguing candidates for the development of unprecedented organic–inorganic 2D van der Waals heterostructures (vdWHs) with exotic physicochemical properties. In this work, we demonstrate the on-water surface synthesis of large-area (cm²), monolayer 2D polyimide (2DPI) with 3.1-nm lattice. Such 2DPI comprises metal-free porphyrin and perylene units linked by imide bonds. We further achieve a scalable synthesis of 2DPI-graphene (2DPI-G) vdWHs via a face-to-face co-assembly of graphene and 2DPI on the water surface. Remarkably, femtosecond transient absorption spectroscopy reveals an ultra-fast interlayer charge transfer (ca. 60 fs) in the resultant 2DPI-G vdWH upon protonation by acid, which is equivalent to that of the fastest reports among inorganic 2D vdWHs. Such large interlayer electronic coupling is ascribed to the interlayer cation–π interaction between 2DP and graphene.

Original language	English
Pages (from-to)	13859-13864
Number of pages	6
Journal	Angewandte Chemie - International Edition
Volume	60
Issue number	25
DOIs	https://doi.org/10.1002/anie.202102984
Publication status	Published - 2021 Jun 14

Bibliographical note

Funding Information:
We acknowledge financial support from EU Graphene Flagship (Core3, No. 881603), ERC Grants on T2DCP and FC2DMOF (No. 852909) and DFG projects (SFB‐1415, No. 417590517; SPP 2244, 2DMP) as well as the German Science Council, Centre of Advancing Electronics Dresden, EXC1056 (Center for Advancing Electronics Dresden) and OR 349/1. We thank Prof. Xiaodong Zhuang (Shanghai Jiao Tong University) and Prof. Zhikun Zheng (Sun Yat‐sen University) for fruitful discussions. We acknowledge Dresden Center for Nanoanalysis (DCN) for scanning electron microscopy and Dr. Petr Formanek (Leibniz Institute for Polymer Research, IPF, Dresden) for the use of facilities. We acknowledge Diamond Light Source for time on Beamline I07 under Proposal SI25070. Open access funding enabled and organized by Projekt DEAL.

Funding Information:
We acknowledge financial support from EU Graphene Flagship (Core3, No. 881603), ERC Grants on T2DCP and FC2DMOF (No. 852909) and DFG projects (SFB-1415, No. 417590517; SPP 2244, 2DMP) as well as the German Science Council, Centre of Advancing Electronics Dresden, EXC1056 (Center for Advancing Electronics Dresden) and OR 349/1. We thank Prof. Xiaodong Zhuang (Shanghai Jiao Tong University) and Prof. Zhikun Zheng (Sun Yat-sen University) for fruitful discussions. We acknowledge Dresden Center for Nanoanalysis (DCN) for scanning electron microscopy and Dr. Petr Formanek (Leibniz Institute for Polymer Research, IPF, Dresden) for the use of facilities. We acknowledge Diamond Light Source for time on Beamline I07 under Proposal SI25070. Open access funding enabled and organized by Projekt DEAL.

Publisher Copyright:
© 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH

All Science Journal Classification (ASJC) codes

Catalysis
Chemistry(all)

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10.1002/anie.202102984

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Liu, K., Li, J., Qi, H., Hambsch, M., Rawle, J., Vázquez, A. R., Nia, A. S., Pashkin, A., Schneider, H., Polozij, M., Heine, T., Helm, M., Mannsfeld, S. C. B., Kaiser, U., Dong, R., & Feng, X. (2021). A Two-Dimensional Polyimide-Graphene Heterostructure with Ultra-fast Interlayer Charge Transfer. Angewandte Chemie - International Edition, 60(25), 13859-13864. https://doi.org/10.1002/anie.202102984

@article{2d1733247dc9420086dde3b8bf52f643,

title = "A Two-Dimensional Polyimide-Graphene Heterostructure with Ultra-fast Interlayer Charge Transfer",

abstract = "Two-dimensional polymers (2DPs) are a class of atomically/molecularly thin crystalline organic 2D materials. They are intriguing candidates for the development of unprecedented organic–inorganic 2D van der Waals heterostructures (vdWHs) with exotic physicochemical properties. In this work, we demonstrate the on-water surface synthesis of large-area (cm2), monolayer 2D polyimide (2DPI) with 3.1-nm lattice. Such 2DPI comprises metal-free porphyrin and perylene units linked by imide bonds. We further achieve a scalable synthesis of 2DPI-graphene (2DPI-G) vdWHs via a face-to-face co-assembly of graphene and 2DPI on the water surface. Remarkably, femtosecond transient absorption spectroscopy reveals an ultra-fast interlayer charge transfer (ca. 60 fs) in the resultant 2DPI-G vdWH upon protonation by acid, which is equivalent to that of the fastest reports among inorganic 2D vdWHs. Such large interlayer electronic coupling is ascribed to the interlayer cation–π interaction between 2DP and graphene.",

author = "Kejun Liu and Jiang Li and Haoyuan Qi and Mike Hambsch and Jonathan Rawle and V{\'a}zquez, {Adri{\'a}n Roman{\'i}} and Nia, {Ali Shaygan} and Alexej Pashkin and Harald Schneider and Mirosllav Polozij and Thomas Heine and Manfred Helm and Mannsfeld, {Stefan C.B.} and Ute Kaiser and Renhao Dong and Xinliang Feng",

note = "Funding Information: We acknowledge financial support from EU Graphene Flagship (Core3, No. 881603), ERC Grants on T2DCP and FC2DMOF (No. 852909) and DFG projects (SFB‐1415, No. 417590517; SPP 2244, 2DMP) as well as the German Science Council, Centre of Advancing Electronics Dresden, EXC1056 (Center for Advancing Electronics Dresden) and OR 349/1. We thank Prof. Xiaodong Zhuang (Shanghai Jiao Tong University) and Prof. Zhikun Zheng (Sun Yat‐sen University) for fruitful discussions. We acknowledge Dresden Center for Nanoanalysis (DCN) for scanning electron microscopy and Dr. Petr Formanek (Leibniz Institute for Polymer Research, IPF, Dresden) for the use of facilities. We acknowledge Diamond Light Source for time on Beamline I07 under Proposal SI25070. Open access funding enabled and organized by Projekt DEAL. Funding Information: We acknowledge financial support from EU Graphene Flagship (Core3, No. 881603), ERC Grants on T2DCP and FC2DMOF (No. 852909) and DFG projects (SFB-1415, No. 417590517; SPP 2244, 2DMP) as well as the German Science Council, Centre of Advancing Electronics Dresden, EXC1056 (Center for Advancing Electronics Dresden) and OR 349/1. We thank Prof. Xiaodong Zhuang (Shanghai Jiao Tong University) and Prof. Zhikun Zheng (Sun Yat-sen University) for fruitful discussions. We acknowledge Dresden Center for Nanoanalysis (DCN) for scanning electron microscopy and Dr. Petr Formanek (Leibniz Institute for Polymer Research, IPF, Dresden) for the use of facilities. We acknowledge Diamond Light Source for time on Beamline I07 under Proposal SI25070. Open access funding enabled and organized by Projekt DEAL. Publisher Copyright: {\textcopyright} 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH",

year = "2021",

month = jun,

day = "14",

doi = "10.1002/anie.202102984",

language = "English",

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Liu, K, Li, J, Qi, H, Hambsch, M, Rawle, J, Vázquez, AR, Nia, AS, Pashkin, A, Schneider, H, Polozij, M, Heine, T, Helm, M, Mannsfeld, SCB, Kaiser, U, Dong, R & Feng, X 2021, 'A Two-Dimensional Polyimide-Graphene Heterostructure with Ultra-fast Interlayer Charge Transfer', Angewandte Chemie - International Edition, vol. 60, no. 25, pp. 13859-13864. https://doi.org/10.1002/anie.202102984

TY - JOUR

T1 - A Two-Dimensional Polyimide-Graphene Heterostructure with Ultra-fast Interlayer Charge Transfer

AU - Liu, Kejun

AU - Li, Jiang

AU - Qi, Haoyuan

AU - Hambsch, Mike

AU - Rawle, Jonathan

AU - Vázquez, Adrián Romaní

AU - Nia, Ali Shaygan

AU - Pashkin, Alexej

AU - Schneider, Harald

AU - Polozij, Mirosllav

AU - Heine, Thomas

AU - Helm, Manfred

AU - Mannsfeld, Stefan C.B.

AU - Kaiser, Ute

AU - Dong, Renhao

AU - Feng, Xinliang

N1 - Funding Information: We acknowledge financial support from EU Graphene Flagship (Core3, No. 881603), ERC Grants on T2DCP and FC2DMOF (No. 852909) and DFG projects (SFB‐1415, No. 417590517; SPP 2244, 2DMP) as well as the German Science Council, Centre of Advancing Electronics Dresden, EXC1056 (Center for Advancing Electronics Dresden) and OR 349/1. We thank Prof. Xiaodong Zhuang (Shanghai Jiao Tong University) and Prof. Zhikun Zheng (Sun Yat‐sen University) for fruitful discussions. We acknowledge Dresden Center for Nanoanalysis (DCN) for scanning electron microscopy and Dr. Petr Formanek (Leibniz Institute for Polymer Research, IPF, Dresden) for the use of facilities. We acknowledge Diamond Light Source for time on Beamline I07 under Proposal SI25070. Open access funding enabled and organized by Projekt DEAL. Funding Information: We acknowledge financial support from EU Graphene Flagship (Core3, No. 881603), ERC Grants on T2DCP and FC2DMOF (No. 852909) and DFG projects (SFB-1415, No. 417590517; SPP 2244, 2DMP) as well as the German Science Council, Centre of Advancing Electronics Dresden, EXC1056 (Center for Advancing Electronics Dresden) and OR 349/1. We thank Prof. Xiaodong Zhuang (Shanghai Jiao Tong University) and Prof. Zhikun Zheng (Sun Yat-sen University) for fruitful discussions. We acknowledge Dresden Center for Nanoanalysis (DCN) for scanning electron microscopy and Dr. Petr Formanek (Leibniz Institute for Polymer Research, IPF, Dresden) for the use of facilities. We acknowledge Diamond Light Source for time on Beamline I07 under Proposal SI25070. Open access funding enabled and organized by Projekt DEAL. Publisher Copyright: © 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH

PY - 2021/6/14

Y1 - 2021/6/14

N2 - Two-dimensional polymers (2DPs) are a class of atomically/molecularly thin crystalline organic 2D materials. They are intriguing candidates for the development of unprecedented organic–inorganic 2D van der Waals heterostructures (vdWHs) with exotic physicochemical properties. In this work, we demonstrate the on-water surface synthesis of large-area (cm2), monolayer 2D polyimide (2DPI) with 3.1-nm lattice. Such 2DPI comprises metal-free porphyrin and perylene units linked by imide bonds. We further achieve a scalable synthesis of 2DPI-graphene (2DPI-G) vdWHs via a face-to-face co-assembly of graphene and 2DPI on the water surface. Remarkably, femtosecond transient absorption spectroscopy reveals an ultra-fast interlayer charge transfer (ca. 60 fs) in the resultant 2DPI-G vdWH upon protonation by acid, which is equivalent to that of the fastest reports among inorganic 2D vdWHs. Such large interlayer electronic coupling is ascribed to the interlayer cation–π interaction between 2DP and graphene.

AB - Two-dimensional polymers (2DPs) are a class of atomically/molecularly thin crystalline organic 2D materials. They are intriguing candidates for the development of unprecedented organic–inorganic 2D van der Waals heterostructures (vdWHs) with exotic physicochemical properties. In this work, we demonstrate the on-water surface synthesis of large-area (cm2), monolayer 2D polyimide (2DPI) with 3.1-nm lattice. Such 2DPI comprises metal-free porphyrin and perylene units linked by imide bonds. We further achieve a scalable synthesis of 2DPI-graphene (2DPI-G) vdWHs via a face-to-face co-assembly of graphene and 2DPI on the water surface. Remarkably, femtosecond transient absorption spectroscopy reveals an ultra-fast interlayer charge transfer (ca. 60 fs) in the resultant 2DPI-G vdWH upon protonation by acid, which is equivalent to that of the fastest reports among inorganic 2D vdWHs. Such large interlayer electronic coupling is ascribed to the interlayer cation–π interaction between 2DP and graphene.

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A Two-Dimensional Polyimide-Graphene Heterostructure with Ultra-fast Interlayer Charge Transfer

Abstract

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