RT Journal Article T1 Orthogonal cation and anion template-directed synthesis of a heteroditopic [3]catenane for ionpair recognition A1 Tay, Hui Min A1 Docker, Andrew A1 Martínez Martínez, Antonio Jesús A1 Beer, Paul D. AB The first orthogonal template strategy for the synthesis of higher order interlocked structures is described. Orthogonal cation and anion templates were employed in a stepwise fashion to construct a hetero[3] catenane composed of structurally distinct macrocyclic components. Importantly, the [3]catenane contains two interlocked binding cavities tailored for cation and anion binding, enabling it to function as a heteroditopic ion-pair receptor. The co-conformational dynamics and cation/anion binding properties of the [3]catenane were investigated by 1H NMR studies, which displayed temperature-dependent and guest-induced changes in chemical shift and linewidth. The potent ion-pair binding capability of the [3] catenane was confirmed by single-crystal X-ray diffraction studies, which showed the [3]catenane to recognise a sodium chloride ion-pair in a mechanically bonded receptor-separated ion-pair binding mode, wherein the two guest ions are encapsulated within their respective interlocked host cavities. PB Royal Society of Chemistry SN 2041-6520 SN 2041-6539 (electrónico) YR 2026 FD 2026 LK https://hdl.handle.net/10272/28457 UL https://hdl.handle.net/10272/28457 LA eng NO Tay, H. M., Docker, A., Martínez-Martínez, A. J., & Beer, P. D. (2026). Orthogonal cation and anion template-directed synthesis of a heteroditopic [3]catenane for ion-pair recognition. Chemical Science, 17(21), 10581–10588. https://doi.org/10.1039/d5sc05942a NO H. M. T. acknowledges the Clarendon Fund and the Oxford Australia Scholarships Fund for a postgraduate research scholarship. A. D. would like to thank Gonville and Caius College, University of Cambridge for a Research Fellowship and funding. A. J. M.-M. acknowledges Financial support from the Spanish Ministerio de Ciencia, Innovación y Universidades MICIN/AEI/10.13039/501100011033 (PID2022-142270OB-I00), MICIN/NextGenerationEU/PRTR (CNS2022-136087), the European Research and Development Fund (ERDF) and the University of Huelva (EPIT1442023). DS Repositorio Institucional de la Universidad de Huelva RD 13 jul 2026