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.
| Identifer | oai:union.ndltd.org:DRESDEN/oai:qucosa:de:qucosa:84378 |
| Date | 29 March 2023 |
| Creators | Lu, Yang, Zhang, Yingying, Yang, Chi-Yuan, Revuelta, Sergio, Qi, Haoyuan, Huang, Chuanhui, Jin, Wenlong, Li, Zichao, Vega-Mayoral, Victor, Liu, Yannan, Huang, Xing, Pohl, Darius, Položij, Miroslav, Zhou, Shengqiang, Cánovas, Enrique, Heine, Thomas, Fabiano, Simone, Feng, Xinliang, Dong, Renhao |
| Publisher | Nature Publishing |
| Source Sets | Hochschulschriftenserver (HSSS) der SLUB Dresden |
| Language | English |
| Detected Language | English |
| Type | info:eu-repo/semantics/publishedVersion, doc-type:article, info:eu-repo/semantics/article, doc-type:Text |
| Rights | info:eu-repo/semantics/openAccess |
| Relation | 2041-1723, 7240, 10.1038/s41467-022-34820-6, info:eu-repo/grantAgreement/European Commission/H2020 | ERC | ERC-STG/852909//Development of Functional Conjugated Two-Dimensional Metal-Organic Frameworks/FC2DMOF, info:eu-repo/grantAgreement/European Commission/H2020 | SGA-RIA/881603//Graphene Flagship Core Project 3/GrapheneCore3, info:eu-repo/grantAgreement/European Commission/H2020 | ERC | ERC-COG/819698//Development of Thiophene Based Conjugated Polymers in Two Dimensions/T2DCP, info:eu-repo/grantAgreement/Deutsche Forschungsgemeinschaft/Sonderforschungsbereiche/417590517//Chemie der synthetischen zweidimensionalen Materialien/SFB 1415, info:eu-repo/grantAgreement/Deutsche Forschungsgemeinschaft/Schwerpunktprogramme/273920491//Koordinationsnetzwerke als Bausteine für Funktionssysteme/SPP 1928, info:eu-repo/grantAgreement/European Commission/H2020 | MSCA-ITN-ETN/813036//Bottom-Up generation of atomicalLy precise syntheTIc 2D MATerials for high performance in energy and Electronic applications – A multi-site innovative training action/ULTIMATE, info:eu-repo/grantAgreement/European Commission/H2020 | RIA/899205//Proto-Opto-Electro-Mechanical Hybrid Systems for Generation-Next Bionic Devices/PROGENY, info:eu-repo/grantAgreement/Deutsche Forschungsgemeinschaft/Exzellenzcluster/194636624//Zentrum für Perspektiven in der Elektronik Dresden/EXC 1056 |
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