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Prof. Se­bas­ti­an Henke’s Group Develops Novel Responsive Materials

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Portrait of a man © Nikolas Golsch​/​TU Dort­mund
Prof. Se­bas­ti­an Henke teaches and conducts re­search in the Department of Chem­is­try and Chemical Biology at TU Dort­mund Uni­ver­sity.

A re­search team associated with Prof. Se­bas­ti­an Henke’s group in the Department of Chem­is­try and Chemical Biology at TU Dort­mund Uni­ver­sity, in cooperation with partners at Ruhr Uni­ver­si­tät Bochum, has investigated the extraordinarily responsive behavior of porous metal-organic frame­work compounds. These can, depending on conditions of their physical environment, crumple up like a piece of paper and unfold again. The findings, which are highly re­le­vant for applications such as energy storage or molecular se­pa­ra­tion, were re­cent­ly published in the re­nowned scientific journal Nature Com­mu­ni­ca­tions.

Metal-organic frameworks, MOFs for short, are synthetic materials. Composed of organic and inorganic mol­ecules, they have a porous, open structure. Some MOFs have responsive properties; that is, they change their crystal structure depending on conditions of their physical environment. Thus the size and shape of the pores can change, for example, if one varies the chemical composition of the ambient atmosphere or exerts mechanical pressure. Among other things, this responsiveness enables MOFs to store gases very efficiently or to separate mol­ecules from one another.

Doctoral candidate Roman Pallach from Prof. Se­bas­ti­an Henke’s group has now discovered a new form of responsiveness in MOFs: Through targeted chemical modification of the organic MOF building blocks, the networks of pores no longer switch back and forth between two ordered, crystalline states, but rather between an ordered state and one that is very complex and disordered. The modified building blocks generate competing interactions within the network structures, so that the disordered state is preferred when guest mol­ecules – stored gases, for example – are absent in the pores.

Graphic of metal-organic frameworks © Arbeits­gruppe Henke​/​TU Dort­mund
If the organic MOF building blocks are chemically modified, the networks change to a disordered state.

“When we remove the guest mol­ecules from the pores, the network is, in a sense, frustrated, and it can only fold up in a disordered manner,” says Prof. Se­bas­ti­an Henke. “With these MOFs, folding up while maintaining the order is not possible.”

Investigation with X-ray scattering methods

In cooperation with Dr. Julian Keupp from Prof. Rochus Schmid’s re­search group at Ruhr Uni­ver­si­tät Bochum and mem­bers of Physical Chem­is­try Prof. Rasmus Linser’s group at TU Dort­mund Uni­ver­sity, the sci­en­tists conducted theoretical and experimental studies of the MOFs’ responsive behavior and were able to gain deep insights into the structure and temperature-dependent dynamics of the disordered state. In addition to computer simulations and spectroscopic techniques, they used sophisticated X-ray scattering methods at Dort­mund’s synchrotron radiation source DELTA, at the German Electron Synchrotron DESY in Hamburg, and at the Diamond Light Source near Oxford, UK.

The findings of the interdiscplinary re­search team were re­cent­ly published in the re­nowned scientific journal Nature Com­mu­ni­ca­tions. The proj­ect was funded in part within the frame­work of the joint Excellence Cluster RESOLV of Ruhr Uni­ver­si­tät Bochum and TU Dort­mund Uni­ver­sity.

R. Pallach, J. Keupp, K. Terlinden, L. Frentzel-Beyme, M. Kloß, A. Machalica, J. Kotschy, S. K. Vasa, P. A. Chater, C. Sternemann, M. T. Wharmby, R. Linser, R. Schmid, S. Henke, Nat. Commun. 2021, 12, 4097: Frustrated Flexibility in Metal-Organic Frameworks. DOI: 10.1038/s41467-021-24188-4

Frustrated flexibility in metal-organic frameworks

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