Understanding structure-property relationships in coordination polymers: a comparative study of the copper() and zinc() coordination mechanism
Coordination polymers (CPs) are an interesting class of materials due to their tunable structures and electrical properties where, however, the correlation between the former and latter is still not fully understood. Here we compare the structures and properties of CPs derived from copper( ii ) and...
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| Published in | Nanoscale Vol. 17; no. 24; pp. 14816 - 14826 |
|---|---|
| Main Authors | , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
England
Royal Society of Chemistry
19.06.2025
|
| Subjects | |
| Online Access | Get full text |
| ISSN | 2040-3364 2040-3372 2040-3372 |
| DOI | 10.1039/d5nr01087j |
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| Abstract | Coordination polymers (CPs) are an interesting class of materials due to their tunable structures and electrical properties where, however, the correlation between the former and latter is still not fully understood. Here we compare the structures and properties of CPs derived from copper(
ii
) and zinc(
ii
) ions coordinating a triphenylene derivative (OHPTP). To focus on the effect of the coordinating ion used and avoid possible differences due to the processing method, we synthesized different CPs using a novel two-step technique, potentially scalable for applications in transistors, sensors, and photovoltaics: first, the organic ligand is deposited using a shear-coating technique which ensures uniform deposition on the macroscopic scale. Then, in the second step, the sample is exposed to solutions of the metal ions, which can penetrate in the organic layer to coordinate with the ligand. Density functional theory (DFT) calculations show that Cu ions have a higher affinity for the ligand and form square-planar CP structures due to their d
9
electronic configuration. Conversely, Zn ions can coordinate with the chelating ligands using only their empty 4s and 4p orbitals to achieve sp
3
hybridisation, thus preferring to adopt a tetrahedral geometry and leading to less ordered structures with significantly hampered conductivity. FT-IR and UV-vis spectra, XPS and conductive atomic force microscopy confirm the distinct coordination behaviour of Cu and Zn ions. Thermal stability analysis further shows that Zn-based CPs retain their structural integrity at temperatures up to 300 °C, whereas Cu-based CPs degrade earlier. These results show how metal-ligand interactions impact the properties of CPs, enhancing the understanding of structure-property relationships, and provide practical insights for designing CPs with desired electronic and thermal properties by varying the coordinating metal ions.
In metal-organic coordination polymers, metal ions can adopt square-planar or tetrahedral geometries, affecting electronic properties. These configurations are studied
via
AFM, XPS, and DFT modelling to compare structural and electronic differences. |
|---|---|
| AbstractList | Coordination polymers (CPs) are an interesting class of materials due to their tunable structures and electrical properties where, however, the correlation between the former and latter is still not fully understood. Here we compare the structures and properties of CPs derived from copper(II) and zinc(II) ions coordinating a triphenylene derivative (OHPTP). To focus on the effect of the coordinating ion used and avoid possible differences due to the processing method, we synthesized different CPs using a novel two-step technique, potentially scalable for applications in transistors, sensors, and photovoltaics: first, the organic ligand is deposited using a shear-coating technique which ensures uniform deposition on the macroscopic scale. Then, in the second step, the sample is exposed to solutions of the metal ions, which can penetrate in the organic layer to coordinate with the ligand. Density functional theory (DFT) calculations show that Cu ions have a higher affinity for the ligand and form square-planar CP structures due to their d9 electronic configuration. Conversely, Zn ions can coordinate with the chelating ligands using only their empty 4s and 4p orbitals to achieve sp3 hybridisation, thus preferring to adopt a tetrahedral geometry and leading to less ordered structures with significantly hampered conductivity. FT-IR and UV-vis spectra, XPS and conductive atomic force microscopy confirm the distinct coordination behaviour of Cu and Zn ions. Thermal stability analysis further shows that Zn-based CPs retain their structural integrity at temperatures up to 300 °C, whereas Cu-based CPs degrade earlier. These results show how metal-ligand interactions impact the properties of CPs, enhancing the understanding of structure-property relationships, and provide practical insights for designing CPs with desired electronic and thermal properties by varying the coordinating metal ions.Coordination polymers (CPs) are an interesting class of materials due to their tunable structures and electrical properties where, however, the correlation between the former and latter is still not fully understood. Here we compare the structures and properties of CPs derived from copper(II) and zinc(II) ions coordinating a triphenylene derivative (OHPTP). To focus on the effect of the coordinating ion used and avoid possible differences due to the processing method, we synthesized different CPs using a novel two-step technique, potentially scalable for applications in transistors, sensors, and photovoltaics: first, the organic ligand is deposited using a shear-coating technique which ensures uniform deposition on the macroscopic scale. Then, in the second step, the sample is exposed to solutions of the metal ions, which can penetrate in the organic layer to coordinate with the ligand. Density functional theory (DFT) calculations show that Cu ions have a higher affinity for the ligand and form square-planar CP structures due to their d9 electronic configuration. Conversely, Zn ions can coordinate with the chelating ligands using only their empty 4s and 4p orbitals to achieve sp3 hybridisation, thus preferring to adopt a tetrahedral geometry and leading to less ordered structures with significantly hampered conductivity. FT-IR and UV-vis spectra, XPS and conductive atomic force microscopy confirm the distinct coordination behaviour of Cu and Zn ions. Thermal stability analysis further shows that Zn-based CPs retain their structural integrity at temperatures up to 300 °C, whereas Cu-based CPs degrade earlier. These results show how metal-ligand interactions impact the properties of CPs, enhancing the understanding of structure-property relationships, and provide practical insights for designing CPs with desired electronic and thermal properties by varying the coordinating metal ions. Coordination polymers (CPs) are an interesting class of materials due to their tunable structures and electrical properties where, however, the correlation between the former and latter is still not fully understood. Here we compare the structures and properties of CPs derived from copper( ii ) and zinc( ii ) ions coordinating a triphenylene derivative (OHPTP). To focus on the effect of the coordinating ion used and avoid possible differences due to the processing method, we synthesized different CPs using a novel two-step technique, potentially scalable for applications in transistors, sensors, and photovoltaics: first, the organic ligand is deposited using a shear-coating technique which ensures uniform deposition on the macroscopic scale. Then, in the second step, the sample is exposed to solutions of the metal ions, which can penetrate in the organic layer to coordinate with the ligand. Density functional theory (DFT) calculations show that Cu ions have a higher affinity for the ligand and form square-planar CP structures due to their d 9 electronic configuration. Conversely, Zn ions can coordinate with the chelating ligands using only their empty 4s and 4p orbitals to achieve sp 3 hybridisation, thus preferring to adopt a tetrahedral geometry and leading to less ordered structures with significantly hampered conductivity. FT-IR and UV-vis spectra, XPS and conductive atomic force microscopy confirm the distinct coordination behaviour of Cu and Zn ions. Thermal stability analysis further shows that Zn-based CPs retain their structural integrity at temperatures up to 300 °C, whereas Cu-based CPs degrade earlier. These results show how metal-ligand interactions impact the properties of CPs, enhancing the understanding of structure-property relationships, and provide practical insights for designing CPs with desired electronic and thermal properties by varying the coordinating metal ions. In metal-organic coordination polymers, metal ions can adopt square-planar or tetrahedral geometries, affecting electronic properties. These configurations are studied via AFM, XPS, and DFT modelling to compare structural and electronic differences. Coordination polymers (CPs) are an interesting class of materials due to their tunable structures and electrical properties where, however, the correlation between the former and latter is still not fully understood. Here we compare the structures and properties of CPs derived from copper(ii) and zinc(ii) ions coordinating a triphenylene derivative (OHPTP). To focus on the effect of the coordinating ion used and avoid possible differences due to the processing method, we synthesized different CPs using a novel two-step technique, potentially scalable for applications in transistors, sensors, and photovoltaics: first, the organic ligand is deposited using a shear-coating technique which ensures uniform deposition on the macroscopic scale. Then, in the second step, the sample is exposed to solutions of the metal ions, which can penetrate in the organic layer to coordinate with the ligand. Density functional theory (DFT) calculations show that Cu ions have a higher affinity for the ligand and form square-planar CP structures due to their d9 electronic configuration. Conversely, Zn ions can coordinate with the chelating ligands using only their empty 4s and 4p orbitals to achieve sp3 hybridisation, thus preferring to adopt a tetrahedral geometry and leading to less ordered structures with significantly hampered conductivity. FT-IR and UV-vis spectra, XPS and conductive atomic force microscopy confirm the distinct coordination behaviour of Cu and Zn ions. Thermal stability analysis further shows that Zn-based CPs retain their structural integrity at temperatures up to 300 °C, whereas Cu-based CPs degrade earlier. These results show how metal–ligand interactions impact the properties of CPs, enhancing the understanding of structure–property relationships, and provide practical insights for designing CPs with desired electronic and thermal properties by varying the coordinating metal ions. Coordination polymers (CPs) are an interesting class of materials due to their tunable structures and electrical properties where, however, the correlation between the former and latter is still not fully understood. Here we compare the structures and properties of CPs derived from copper(ii) and zinc(ii) ions coordinating a triphenylene derivative (OHPTP). To focus on the effect of the coordinating ion used and avoid possible differences due to the processing method, we synthesized different CPs using a novel two-step technique, potentially scalable for applications in transistors, sensors, and photovoltaics: first, the organic ligand is deposited using a shear-coating technique which ensures uniform deposition on the macroscopic scale. Then, in the second step, the sample is exposed to solutions of the metal ions, which can penetrate in the organic layer to coordinate with the ligand. Density functional theory (DFT) calculations show that Cu ions have a higher affinity for the ligand and form square-planar CP structures due to their d 9 electronic configuration. Conversely, Zn ions can coordinate with the chelating ligands using only their empty 4s and 4p orbitals to achieve sp 3 hybridisation, thus preferring to adopt a tetrahedral geometry and leading to less ordered structures with significantly hampered conductivity. FT-IR and UV-vis spectra, XPS and conductive atomic force microscopy confirm the distinct coordination behaviour of Cu and Zn ions. Thermal stability analysis further shows that Zn-based CPs retain their structural integrity at temperatures up to 300 °C, whereas Cu-based CPs degrade earlier. These results show how metal-ligand interactions impact the properties of CPs, enhancing the understanding of structure-property relationships, and provide practical insights for designing CPs with desired electronic and thermal properties by varying the coordinating metal ions. Coordination polymers (CPs) are an interesting class of materials due to their tunable structures and electrical properties where, however, the correlation between the former and latter is still not fully understood. Here we compare the structures and properties of CPs derived from copper(II) and zinc(II) ions coordinating a triphenylene derivative (OHPTP). To focus on the effect of the coordinating ion used and avoid possible differences due to the processing method, we synthesized different CPs using a novel two-step technique, potentially scalable for applications in transistors, sensors, and photovoltaics: first, the organic ligand is deposited using a shear-coating technique which ensures uniform deposition on the macroscopic scale. Then, in the second step, the sample is exposed to solutions of the metal ions, which can penetrate in the organic layer to coordinate with the ligand. Density functional theory (DFT) calculations show that Cu ions have a higher affinity for the ligand and form square-planar CP structures due to their d electronic configuration. Conversely, Zn ions can coordinate with the chelating ligands using only their empty 4s and 4p orbitals to achieve sp hybridisation, thus preferring to adopt a tetrahedral geometry and leading to less ordered structures with significantly hampered conductivity. FT-IR and UV-vis spectra, XPS and conductive atomic force microscopy confirm the distinct coordination behaviour of Cu and Zn ions. Thermal stability analysis further shows that Zn-based CPs retain their structural integrity at temperatures up to 300 °C, whereas Cu-based CPs degrade earlier. These results show how metal-ligand interactions impact the properties of CPs, enhancing the understanding of structure-property relationships, and provide practical insights for designing CPs with desired electronic and thermal properties by varying the coordinating metal ions. |
| Author | Benekou, Vasiliki Candini, Andrea Liscio, Fabiola Mannsfeld, Stefan C. B Feng, Xinliang Sporrer, Lukas Zhang, Zhe Kovtun, Alessandro Monti, Filippo Palermo, Vincenzo Dong, Renhao |
| AuthorAffiliation | Department of Chemistry The University of Hong Kong Institute of Nanostructured Materials Chair of Molecular Functional Materials Department of Industrial and Materials Science National Research Council of Italy Faculty of Chemistry and Food Chemistry Technische Universität Dresden HKU-SIRI Chalmers University of Technology Materials Innovation Institute for Life Sciences and Energy (MILES) Institute for Organic Synthesis and Photoreactivity |
| AuthorAffiliation_xml | – name: Chalmers University of Technology – name: Materials Innovation Institute for Life Sciences and Energy (MILES) – name: Department of Chemistry – name: National Research Council of Italy – name: Faculty of Chemistry and Food Chemistry Technische Universität Dresden – name: HKU-SIRI – name: Institute for Organic Synthesis and Photoreactivity – name: Institute of Nanostructured Materials – name: The University of Hong Kong – name: Department of Industrial and Materials Science – name: Chair of Molecular Functional Materials |
| Author_xml | – sequence: 1 givenname: Vasiliki surname: Benekou fullname: Benekou, Vasiliki – sequence: 2 givenname: Zhe surname: Zhang fullname: Zhang, Zhe – sequence: 3 givenname: Lukas surname: Sporrer fullname: Sporrer, Lukas – sequence: 4 givenname: Andrea surname: Candini fullname: Candini, Andrea – sequence: 5 givenname: Filippo surname: Monti fullname: Monti, Filippo – sequence: 6 givenname: Alessandro surname: Kovtun fullname: Kovtun, Alessandro – sequence: 7 givenname: Fabiola surname: Liscio fullname: Liscio, Fabiola – sequence: 8 givenname: Stefan C. B surname: Mannsfeld fullname: Mannsfeld, Stefan C. B – sequence: 9 givenname: Xinliang surname: Feng fullname: Feng, Xinliang – sequence: 10 givenname: Renhao surname: Dong fullname: Dong, Renhao – sequence: 11 givenname: Vincenzo surname: Palermo fullname: Palermo, Vincenzo |
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| Cites_doi | 10.1002/adma.201903762 10.1016/j.ccr.2020.213388 10.1002/admi.202100308 10.1038/s41467-022-34139-2 10.1021/acs.chemmater.9b01996 10.1002/anie.202111519 10.1002/smtd.202300842 10.1007/978-0-387-28668-6 10.1039/c0sm01113d 10.1016/j.mattod.2014.05.010 10.1002/adfm.200600122 10.1021/j150579a011 10.1021/acsami.9b07832 10.1002/anie.200300610 10.1351/PAC-REC-12-11-20 10.1002/anie.202300186 10.1021/acs.accounts.4c00305 10.1002/(SICI)1096-9918(19960916)24:9<620::AID-SIA151>3.0.CO;2-Y 10.1021/ja507179d 10.1002/aelm.201900067 10.1039/b900317g 10.1016/S1359-0286(00)00031-0 10.1016/B978-0-444-53599-3.10010-1 10.1021/cm402136z 10.1002/adma.200501394 10.1002/anie.202212797 10.1016/j.inoche.2020.108354 10.3390/polym13091435 10.1002/adma.201002215 10.1038/nature01650 10.3390/nano11092239 |
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| Snippet | Coordination polymers (CPs) are an interesting class of materials due to their tunable structures and electrical properties where, however, the correlation... |
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| SubjectTerms | Chelation Comparative studies Coordination polymers Copper Density functional theory Electrical properties Ligands Metal ions Photovoltaic cells Stability analysis Structural integrity Thermal stability Thermodynamic properties Zinc Zinc coordination |
| Title | Understanding structure-property relationships in coordination polymers: a comparative study of the copper() and zinc() coordination mechanism |
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