Precise tuning of interlayer electronic coupling in layered conductive metal-organic frameworks

Yang Lu, Yingying Zhang, Chi Yuan Yang, Sergio Revuelta, Haoyuan Qi, Chuanhui Huang, Wenlong Jin, Zichao Li, Victor Vega-Mayoral, Yannan Liu, Xing Huang, Darius Pohl, Miroslav Položij, Shengqiang Zhou, Enrique Cánovas, Thomas Heine, Simone Fabiano, Xinliang Feng, Renhao Dong

Research output: Contribution to journalArticlepeer-review

Abstract

Two-dimensional conjugated metal-organic frameworks (2D c-MOFs) have attracted increasing interests for (opto)-electronics and spintronics. They generally consist of van der Waals stacked layers and exhibit layer-depended electronic properties. While considerable efforts have been made to regulate the charge transport within a layer, precise control of electronic coupling between layers has not yet been achieved. Herein, we report a strategy to precisely tune interlayer charge transport in 2D c-MOFs via side-chain induced control of the layer spacing. We design hexaiminotriindole ligands allowing programmed functionalization with tailored alkyl chains (HATI_CX, X = 1,3,4; X refers to the carbon numbers of the alkyl chains) for the synthesis of semiconducting Ni3(HATI_CX)2. The layer spacing of these MOFs can be precisely varied from 3.40 to 3.70 Å, leading to widened band gap, suppressed carrier mobilities, and significant improvement of the Seebeck coefficient. With this demonstration, we further achieve a record-high thermoelectric power factor of 68 ± 3 nW m−1 K−2 in Ni3(HATI_C3)2, superior to the reported holes-dominated MOFs.

Original languageEnglish
Article number7240
JournalNature communications
Volume13
Issue number1
DOIs
Publication statusPublished - 2022 Dec

Bibliographical note

Funding Information:
The authors acknowledge cfaed and Dresden Center for Nano-analysis (DCN) at TUD. This work is financially supported by ERC starting grant (FC2DMOF, No. 852909), EU Graphene Flagship (Core3, No. 881603), ERC Consolidator Grant (T2DCP), DFG projects (CRC-1415, No. 417590517; SPP-1928, COORNET), H2020-MSCA-ITN (ULTIMATE, No. 813036), EMPIR-20FUN03-COMET, H2020-FETOPEN (PROGENY, 899205) as well as the German Science Council and Center of Advancing Electronics Dresden (cfaed). R.D. thanks Taishan Scholars Program of Shandong Province (tsqn201909047) and the National Natural Science Foundation of China (22272092). E.C. acknowledges MCIN/AEI grant PID2019-107808RA-I00 and Comunidad de Madrid grants 2021-5A/AMB-20942 & P2018/NMT-451. S.F. acknowledges support from the Swedish Research Council (2020-03243) and the Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linköping University (Faculty Grant SFO-Mat-LiU 2009-00971). Y.Z. acknowledges China Scholarship Council. Y.L. and Y.Z. acknowledge ZIH Dresden for computer time.

Funding Information:
The authors acknowledge cfaed and Dresden Center for Nano-analysis (DCN) at TUD. This work is financially supported by ERC starting grant (FC2DMOF, No. 852909), EU Graphene Flagship (Core3, No. 881603), ERC Consolidator Grant (T2DCP), DFG projects (CRC-1415, No. 417590517; SPP-1928, COORNET), H2020-MSCA-ITN (ULTIMATE, No. 813036), EMPIR-20FUN03-COMET, H2020-FETOPEN (PROGENY, 899205) as well as the German Science Council and Center of Advancing Electronics Dresden (cfaed). R.D. thanks Taishan Scholars Program of Shandong Province (tsqn201909047) and the National Natural Science Foundation of China (22272092). E.C. acknowledges MCIN/AEI grant PID2019-107808RA-I00 and Comunidad de Madrid grants 2021-5A/AMB-20942 & P2018/NMT-451. S.F. acknowledges support from the Swedish Research Council (2020-03243) and the Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linköping University (Faculty Grant SFO-Mat-LiU 2009-00971). Y.Z. acknowledges China Scholarship Council. Y.L. and Y.Z. acknowledge ZIH Dresden for computer time.

Publisher Copyright:
© 2022, The Author(s).

All Science Journal Classification (ASJC) codes

  • Chemistry(all)
  • Biochemistry, Genetics and Molecular Biology(all)
  • General
  • Physics and Astronomy(all)

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